proceedings of econos 2016 gothenburg, sweden

Proceedings of ECONOS 2016Gothenburg, Sweden

Hosted by Chalmers University

April 24-27, 2016

Published by:ECONOS Local Organizing CommitteeCombustion DivisionDepartment of Applied MechanicsChalmers University, Gothenburg, Swedenhttp://www.chalmers.se/en/conference/econos2016

Credits:LATEX editor: David Sedarsky

Printed in Gothenburg by TeknologTryck — April 2016.

http://www.chalmers.se/en/conference/econos2016

ECONOS GOLD SPONSORS

ECONOS PARTNERS

CONFERENCE PROGRAM

ECONOS GOLD SPONSORS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . iii

ECONOS PARTNERS . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . iv

ECONOS 2016 Schedule . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ix

Sunday, April 24th 3

Zhongshan Li — Mid-infrared Combustion Diagnostics 33 Zhongshan Li

Mid-infrared nonlinear optical diagnostics for combustion applications

Monday, April 25th 7

Ammar Hideur — Ultrafast fiber lasers 77 H. Wang, M. Tang, H. Puwar, E. Silaeva, M. Baumgartl, C. Lecaplain, T. Schreiber, J. Limpert, A. Tünnermann,

J. Houard, A. Vella, S. Idlahcen, C. Rozé, J.-B. Blaisot, T. Godin, A. HideurUltrafast fiber lasers for material analysis and dense media metrology

High Resolution Spectroscopy 99 Rasmus Lyngbye Pedersen, Peter Tidemand-Lichtenberg, Lasse Høgstedt

Tunable 1.9m Laser System for Intracavity Mid-IR Upconversion Detection

11 D. Bermejo, R.Z. Martínez, G. Di Lonardo, L. FusinaHigh resolution stimulated Raman spectroscopy from collisionally populated states after optical pumping.Acetyleneisotopologues in the 3800-3900 cm−1 and 5800-5900 cm−1 regions.

13 A.D. Kudryavtseva, H.V. Ehrlich, G.V. Lisichkin, N.V. Tcherniega, K.I. Zemskov, M.P. ZhilenkoStimulated low-frequency Raman scattering in sodium chloride nanoparticles ensemble

15 D. Hot, A.-L. Sahlberg, J. Kiefer, M. Aldén, Z.S. LiMid-infrared laser-induced thermal grating spectroscopy for detection of small hydrocarbons

Steve Baldelli — SFG microscopy of surfaces 1717 Steven Baldelli

Sum frequency generation microscopy of surfaces

Microscopy and Imaging 1919 Ahmed Abdelmonem, Ellen H.G. Backus, Thomas Leisner, Mischa Bonn

Probing ice nucleation abilities of atmospheric aerosol particles using sum frequency generation spectroscopy

21 Juha Koivistoinen, Jukka Aumanen, Vesa-Matti Hiltunen, Pasi Myllyperkiö, Andreas Johansson, Mika PetterssonImaging of graphene with wide-field four-wave mixing microscopy

23 K.-L. Liu, T. De Wit, C. Steuwe, M.B.J. RoeffaersRationalizing catalyst performance using stimulated Raman microscopy

25 A. D’Arco, N. Brancati, M.A. Ferrara, M. Indolfi, M. Frucci, L. SirletoStimulated Raman scattering in between nano and biophotonics applications

Tuesday, April 26th 29

Jürgen Popp — Imaging with multimodal CARS/SHG/TPEF 2929 Jürgen Popp

Non-linear optical histopathology utilizing multimodal CARS/SHG/TPEF imaging

CARS – Session I 3131 E. Nordström, A. Hosseinnia, C. Brackmann, J. Bood, P.-E. Bengtsson

Raman linewidth measurements using time-resolved hybrid picosecond/nanosecond rotational CARS

33 A.K. Vereshchagin 1 , K.A. Vereshchagin, V.B. Morozov, V.G. Tunkin, Kh. KhasanovCharacterization of bi-spiral twisted supersonic gas flow using time-resolved picosecond pure rotational coherentanti-Stokes Raman spectroscopy

35 A. Aybush, F. Gostev, V. Nadtochenko, K.A. VereshchaginChirped CARS for microspectroscopy and visualization of oocytes and embryonic stem cells: merits and demerits

37 Michele MarroccoClosed-form solutions to time model for hybrid fs/ps coherent anti-Stokes Raman scattering

Sean Kearney — Hybrid fs/ps Rotational CARS 3939 Sean Kearney

Temperature and Major Species Detection in Particle-Laden Flames by fs/ps Rotational CARS

CARS – Session II 4141 A. Hosseinnia, E. Nordström, J. Bood, P.-E. Bengtsson

Ethane thermometry using rotational coherent anti-Stokes Raman scattering (CARS)

43 L. Brückner, T. Buckup, M. MotzkusOptimizing spectral focusing CARS by tailored probing

45 H.U. Stauffer, P.J. Wrzesinski, J.B. Schmidt, D.R. Richardson, S. Roy, J.R. GordSimultaneous single-shot thermometry and detection of minor species via femtosecond, fully resonant electron-ically enhanced CARS (FREE-CARS)

Wednesday, April 27th 49

Michael Scherman — New laser architecture for hybrid fs-ps/CARS 4949 M. Scherman, M. Nafa, A. Bresson, H. Danvy, A. Godard, T. Schmid, B. Attal-Tretout, P. Joubert

New laser architecture for hybrid fs-ps/CARS applied to thermometry and molecular probing

Novel Methods 5151 A.-L. Sahlberg, D. Hot, R.L. Pedersen, J. Zhou, M. Aldén, Z.S. Li

Spatially resolved, in situ, non-intrusive detection of hydrocarbon intermediate species in a rich low-pressuredimethyl-ether/oxygen/argon premixed flame

53 A. Materny, P. Donfack, T.Z. Khan, M.M. Kazemi, F. Mohaghegh, A.M. TehraniMetal-molecule interactions investigated in frequency and time domain

55 B. Visser, M. Beck, P. Bornhauser, G. Knopp, T. Gerber, R. Abela, J.A. van Bokhoven, P.P. RadiUnravelling the complex electronic structure of transition metal dimers using four-wave mixing techniques

57 Christian Steuwe, Hannelore Bové, Maarten Roeffaers, Marcel AmelootLabel-free detection mechanism for carbon nanoparticles using femtosecond pulsed illumination

Commercial Systems 5959 H-C. Becker, I. Rimke

Low noise picosecond fiber laser pumped OPO for improved sensitivity in coherent Raman microscopy

Poster Presentations 6363 K. Becker, J. Kiefer

Simultaneous vibrational Raman and CARS spectroscopy for gas temperature and composition65 J. Tröger, C. Meißner, F. Beyrau, T. Seeger

Comparison of different Raman crystals as a narrowband light source for a vibrational CARS system applied tosooting flames

67 F. Berthillier, B. Barviau, F. GrischDevelopment of CPP femtosecond CARS for 1kHz single-shot thermometry

69 A. RaeEvaluation of a parabolic scan unit for stimulated Raman scattering microscopy

71 A. Kouzov, P. Radi, N. EgorovaLine space theory of resonant four-wave mixing by rotationally anisotropic photofragments

73 M. Rahm, D. Sedarsky, M. LinneKerr lensing effects in time-gated imaging of atomizing sprays

75 H. Purwar, S. Idlahcen, J.-B. Blaisot, C. RozéApproach for volumetric spray measurements using Mueller calculus

77 M. Nafa, M. Scherman, H. Danvy, A. Bresson, A. Godard, T. Schmid, B. Attal-Tretout, P. JoubertN2 thermometry in hybrid fs/ps CARS

List of Authors 79

3

3

3

3 Conference Schedule

Sunday, April 24th15:00—17:00 Registration at Chalmerska Huset

17:00—17:15 Opening of ECONOS 2016

17:15—18:00 “Mid-infrared nonlinear optical diagnostics for combustion applications”Zhongshan Li, Combustion Physics, Lund University, Sweden

18:00—20:00 Welcome reception at Chalmerska Huset

Monday, April 25th09:00—09:45 “Ultrafast fiber lasers for material analysis and dense media metrology”

Amar Hideur, CNRS-Université et INSA de Rouen, France

09:45—10:20 Coffee Break

10:20—12:20 Session I: High resolution spectroscopy

12:20—14:20 Lunch at Chalmerska Huset

14:20—15:05 “Sum frequency generation microscopy of surfaces”Steven Baldelli, University of Houston, United States

15:05—16:25 Session II: Microscopy and imaging


17:00—18:00 Poster Session

Tuesday, April 26th09:00—09:45 “Non-linear optical histopathology utilizing multimodal CARS/SHG/TPEF imaging”

Jürgen Popp, Friedrich-Schiller University Jena, Germany


10:20—12:00 Session I: Coherent Anti-Stokes Raman Scattering


14:00—14:45 “Temperature and major species detection in particle-laden flames by fs/ps rotational CARS”Sean Kearney, Sandia National Laboratories, Albuquerque, United States

14:45—16:25 Session II: Coherent Anti-Stokes Raman Scattering


17:00—18:00 Poster Session

19:00—21:00 Conference Dinner at Chalmerska Huset

Wednesday, April 27th09:00—09:45 “New laser architecture for hybrid fs-ps/CARS applied to thermometry and molecular probing”

Michael Scherman, ONERA, Palaiseau, France


10:20—12:00 Session I: Novel Methods


13:00—13:45 Session II: Commercial Systems

13:45—14:00 Closing of ECONOS 2016

14:00—16:00 Post-conference fika at Chalmerska Huset

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Sunday, April 24th

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Mid-infrared nonlinear optical diagnostics for combustion applications

Z. Li1 Combustion Physics, Department of Physics, Lund University

P.O. Box 118, SE-221 00 Lund, Sweden e-mail: [email protected]

URL: http://www.forbrf.lth.se/ KEY WORDS: thermal gratings, degenerate four-wave mixing, polarization spectroscopy

Nonlinear optical diagnostics employing four-wave mixing techniques have been developed in

the last decades, which have demonstrated substantial advantages in combustion applications

based on the following facts. Firstly, by probing molecular ro-vibrational transitions, many

molecular species, e.g. methane, ethane, acetylene, HCl, HCN, HF, which do not easy

accessible electronic transitions to be probed, can be detected. Secondly, sensitive detection

down to ppm level in harsh environments even in 2D can be achieved based on the fact of the

fully resonant enhancement from the strong fundamental transitions. Thirdly, the coherent

feature of the generated nonlinear signal allows efficient discrimination from the strong thermal

radiation from flames which otherwise will be serious problem. Techniques will be discussed

include Polarization Spectroscopy, Degenerated Four-Wave Mixing and Laser-induced

Thermal Grating Spectroscopy.

PROCEEDINGS OF ECONOS 24–27 April, 2016

— 3 —

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Monday, April 25th

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Ultrafast fiber lasers for material analysis and dense media

metrology

H. Wang1, M. Tang1, H. Puwar1, E. Silaeva2, M. Baumgartl3, C. Lecaplain1, T. Schreiber4, J. Limpert3,4, A.

Tünnermann3,4, J. Houard2, A. Vella2, S; Idlahcen1, C. Rozé1, J.-B. Blaisot1, T. Godin1, A. Hideur1 1CORIA UMR 6614, Normandie Université, CNRS-Université et INSA de Rouen, 76800 Saint Etienne du Rouvray, France

2GPM UMR 6634, Normandie Université, CNRS-Université et INSA de Rouen, 76800 Saint Etienne du Rouvray, France 3Institute of Applied Physics, Friedrich-Schiller-Universität Jena, Albert-Einstein-Strasse 15, 07745 Jena, Germany

4Fraunhofer IOF, Albert-Einstein-Strasse 7, D-07745 Jena, Germany

[email protected]

High-power femtosecond laser sources are versatile tools for numerous applications ranging from material

processing on a sub-micrometer scale to high-field physics. The proliferation of these sources outside a laboratory

environment relies on the development of robust powerful sources. Ultra-short pulse generation in rare-earth-doped

fibers is considered to be the most promising approach to fulfill these requirements. Their advantages arise from the

light propagation in waveguide-structures, and hence, inherent stability and immunity against thermo-optical issues.

The fundamental challenge for ultrafast fiber lasers relies on the control of the excessive nonlinearity caused by the

tight confinement of the laser radiation in small sections. During the past decade, significant progress has been

realized by applying the well-known CPA technique with large-mode-area fiber designs. Using LMA fiber

amplifiers, femtosecond pulses with energies in excess of 1 mJ have been generated. The second approach is based

on energy scaling in passively mode-mode-locked oscillators. Compared to bulk-based technologies such as thin-

disks, fiber lasers are the most promising concept for extremely short pulse generation (<<100fs) at highest average

powers. To circumvent pump limitations diode-pumped Ytterbium-doped gain media are predominantly used

whenever it comes to high power operation. The active waveguide offers superior thermal properties, an enormous

single-pass gain and an excellent beam quality. Moreover, Yb-fiber lasers support the generation of pulse durations

below 30 fs due to their large amplification bandwidth and due to the nonlinear spectral broadening inside the

cavity, which can extend the pulse spectrum even beyond the gain bandwidth. At the same time, however, the

accumulation of excessive nonlinear phase leads to pulse breakup. Recently, novel pulse shaping mechanisms in

normal group-velocity-dispersion (GVD) cavity designs [1-4] in conjunction with the development and use of large-

mode-area (LMA) fibers [5-11] brought rapid progress, reaching several tens of watts average power with sub-100

fs pulses. We review the current state-of-the-art of high-power mode-locked fiber lasers and discuss their potential

to drive real-world applications [12-13].

References [1] A. Chong, W. Renninger, and F. Wise, “All-normal-dispersion femtosecond fiber laser with pulse energy above 20 nJ,” Opt. Lett. 32, 2408-

2410 (2007). [2] A. Chong, W. Renninger, and F. Wise, "Properties of normal-dispersion femtosecond fiber lasers," J. Opt. Soc. Am. B 25, 140-148 (2008).

[3] C. Lecaplain, M. Baumgartl, T. Schreiber, and A. Hideur, "On the mode-locking mechanism of a dissipative- soliton fiber oscillator," Opt.

Express 19, 26742-26751 (2011). [4] M. Tang, H. Wang, A. Becheker, D. Gaponov, J-L. Oudar, T. Godin and A. Hideur, “High-energy dissipative solitons generation from a large

normal dispersion Er-fiber laser”, Opt. Lett. 40, 1414-1417 (2015).

[5] B. Ortaç, M. Baumgartl, J. Limpert, and A. Tünnermann, "Approaching microjoule-level pulse energy with mode-locked femtosecond fiber lasers," Opt. Lett. 34, 1585-1587 (2009).

[6] C. Lecaplain, B. Ortaç, G. Machinet, J. Boullet, M. Baumgartl, T. Schreiber, E. Cormier, and A. Hideur, "High-energy femtosecond photonic

crystal fiber laser," Opt. Lett. 35, 3156-3158 (2010).

[7] M. Baumgartl, B. Ortaç, C. Lecaplain, A. Hideur, J. Limpert, and A. Tünnermann, "Sub-80 fs dissipative soliton large-mode-area fiber laser,"

Opt. Lett. 35, 2311-2313 (2010).

[8] M. Baumgartl, F. Jansen, F. Stutzki, C. Jauregui, B. Ortaç, J. Limpert, and A. Tünnermann, "High average and peak power femtosecond large-pitch photonic-crystal-fiber laser," Opt. Lett. 36, 244-246 (2011).

[9] N. B. Chichkov, C. Hapke, J. Neumann, D. Kracht, D. Wandt, and U. Morgner, "Pulse duration and energy scaling of femtosecond all-normal

dispersion fiber oscillators," Opt. Express 20, 3844-3852 (2012). [10] M. Baumgartl, C. Lecaplain, A. Hideur, J. Limpert, and A. Tünnermann, "66 W average power from a microjoule-class sub-100 fs fiber

oscillator," Opt. Lett. 37, 1640-1642 (2012)

[11] S. Lefrancois, C-H Liu, M. L. Stock, T. S. Sosnowski, A. Galvanauskas, and F. W. Wise, "High-energy similariton fiber laser using chirally coupled core fiber," Opt. Lett. 38, 43-45 (2013).

[12] H. Wang, J. Houard, L. Arnoldi, A. Hideur, E. P. Silaeva, B. Deconihout, A. Vella, “Effect of the laser pulse width on the field evaporation

behavior of metals and oxides”, Ultramicroscopy 160, 18-24 (2016). [13] H. Purwar, H. Wang, M. Tang, S. Idlahcen, A. Hideur, C. Rozé, J.-B. Blaisot, T. Godin, “Development of Picosecond Fiber Laser for High

Repetition Diesel Spray Imaging,” ICLASS’2015, Taiwan, August 23-27 (2015).


— 7 —

Tunable 1.9µm Laser System for Intracavity Mid-IR Upconversion

Detection

Rasmus Lyngbye Pedersen, Peter Tidemand-Lichtenberg*, Lasse Høgstedt* Lund University, Combustion Physics Department, Professorsgatan 1

SE-223 63 Lund *Technical University of Denmark, Frederiksborgvej 399, 4000 Roskilde, Denmark

[email protected]

[email protected]

KEY WORDS: Infra-red, upconversion, Tm:YLF

Sum Frequency Generation (SFG) can be used to combine a weak signal wavelength in the

infrared (IR) with a more powerful mixing laser to generate a signal at shorter wavelengths.

This will move the IR signal from a region with inherently noisy detectors to the visible

regime or near IR, where low noise silicon based detectors can be used, which allows for

more sensitive quantitative spectroscopy. Upconversion for IR detection has been

demonstrated earlier in a short wavelength pump scheme 1 and using longer wavelength

mixing fields for pumping in waveguides2.

A tunable 1.9µm Tm:YLF laser was built as shown in Figure 1 for low-noise infrared

upconversion imaging and spectroscopy. The purpose of this system was low-noise

upconversion of the 1572nm and 1643nm light for sensitive detection of CO2 and CH4. The

system was tested using a 1064nm source, and with this, we achieved a stable upconverted

signal. As far as we are aware, this is the first demonstration of an intracavity upconversion

system using a Tm:YLF crystal as the laser crystal.

For 1-2µm light upconversion detection is competing mainly with InGaAs diodes, and we

expect only minor noise improvements over these. However, a long term goal is to replace the

periodically poled Lithium Niobate (PPLN) crystal with an AGS crystal, to allow

upconversion in the 5-10µm range, where thermal noise is a much larger problem. We expect

an upconversion system to improve the possible signal-to-noise ratio by orders of magnitude.

Figure 1: M1: Plane mirror, M2: concave mirror, r = 150, M6-M7 Plane protected silver mirrors, M8:

concave mirror, r =150, PPLN: Periodically Poled Lithium Niobate, L6: 250mm focal length lens,

1 Dam, Jeppe Seidelin, Peter Tidemand-Lichtenberg, and Christian Pedersen. “Room-Temperature Mid-Infrared

Single-Photon Spectral Imaging.” NATURE PHOTONICS 6.11 (2012): 788–793. Web. 2 Pelc, J. S. et al. Long-Wavelength-Pumped Upconversion Single-Photon Detector at 1550 Nm: Performance

and Noise Analysis. OPTICS EXPRESS 19.22 (2011): 21445–21456. Web.


— 9 —

High resolution stimulated Raman spectroscopy from collisionally

populated states after optical pumping. Acetylene isotopologues in the

3800-3900 cm-1 and 5800-5900 cm-1 regions.

D. Bermejo

1, R.Z. Martínez

1, G. Di Lonardo

2 and L. Fusina

2

1. Instituto de Estructura de la Materia (CSIC), Serrano 123, 28006-Madrid, Spain

2. Dipartimento di Chimica Fisica e Inorgánica, Università di Bologna, Viale Risorgimento 4, I-40136 Bologna, Italy [email protected]

KEY WORDS: Stimulated Raman Spectroscopy, High Resolution, Gas Phase

Optical population of vibrationally excited states by Stimulated Raman pumping as a

means for high resolution investigation of excited states at low temperatures has been

widely demonstrated1. In the present communication we show the feasibility of

collisionally populating excited states others than the ones optically pumped, keeping

pressure at levels low enough to allow for the observation of fully resolved Q branches of

light molecules.

We present some results for 12

C2H2, 13

C12

CH2 and 13

C2H2. In all cases, one single

rotational level of the state v2=1 is populated by means of a doubly pulsed stimulated

Raman process. After a delay of about 500ns, a second stimulated Raman process, in this

case quasi-CW, is used to record the high resolution stimulated Raman spectra from the

collisionally populated levels to upper levels differing by a quantum of v2. It is worth

pointing out that after this delay, not only other vibrational states are populated, but also

the distribution among the rotational levels has achieved a thermal equilibrium.

In all cases, the pressure has been kept between 5 and 12 mbar at a temperature of 150K.

After the optical pumping, the main collisional processes involved are:

C2H2 (v2=1) + C2H2 (v2=0) → C2H2 (v2=0) + C2H2 (v4=2, v5=1) + E

C2H2 (v2=1) + C2H2 (v2=1) → C2H2 (v2=0) + C2H2 (v2=2) + E

C2H2 (v2=1) + C2H2 (v2=1) → C2H2 (v2=0) + C2H2 (v2=2, v4=2, v5=1) + E

Where E corresponds to the conversion of a small fraction of vibrational energy into

rotational or translational energy in order to keep the energy balance. In the present case,

E is < 10cm-1

). The observed transitions are: 32-22 and (2+24+5) – (24+5) of

symmetry ← and ← respectively.

As an example, figure 1 shows the 32-22 and [2+24(2)+5(-1)] – [24(2)+5(-1)]

Q-branches of 13

C2H2.

1881.0 1881.5 1882.0 1882.5 1883.0 1883.5 1884.0

0

R a

m a

n

l o s

s ( a

. u

. )

Wavenumber (cm-1)

13C

2H

2

150K, 12 mbar

(2+2

2

4+

-1

5) - (2

2

4+

-1

5) ()

32-2

2 ()

2, O(7)

Figure 1. Stimulated Raman Spectrum of 13

C2H2 from collisionally populated states.

1 R. Z. Martínez and D. Bermejo. J. Raman Spectrosc. 44, 727 (2013)


— 11 —

Stimulated Low-Frequency Raman Scattering in Sodium Chloride

Nanoparticles Ensemble

A.D. Kudryavtseva1, H.V. Ehrlich

2, G.V. Lisichkin

2, N.V.Tcherniega

1, K.I. Zemskov

1, M.P. Zhilenko

2

1P.N. Lebedev Physical Institute of the RAS, Leninskii pr., 53, 119991, Moscow, Russia 2M.V. Lomonosov Moscow State University, Vorob’evy Gory, 119991, Moscow, Russia

E-mail addres: [email protected]

KEY WORDS: stimulated scattering, nanoparticles, spectrum

One of the methods of the nanomaterials investigations is low-frequency Raman scattering

(LFRS). LFRS is inelastic light scattering on the localized acoustic phonons. It is observed in

dielectric, semiconductor and metal nanoparticles and gives important information about their

vibration dynamic. Under laser pulses two light fields interaction (laser and spontaneous

LFRS) can lead to the appearance and strong amplification of the stimulated low-frequency

Raman scattering (SLFRS). Previously we observed SLFRS in nanomaterials with different

composition, morphology and nanoparticles dimensions both in high-ordered and random

materials1,2

. In this work we studied SLFRS in NaCl nanoparticles suspensions in ethanol and

acetone, which practically do not solve NaCl. It allowed us to study pure nanoparticles

containing no water.

The images of sodium chloride samples were obtained with the LEO912 AB OMEGA

transmission electron microscope. To determine average size of elementary particles of NaCl

the X-ray phase analysis was used.

Vibrations of NaCl nanoparticles in suspension were excited by single 20 ns pulses of ruby

laser. SLFRS spectra have been registered with the help of Fabri-Perot interferometers.

Scattering was excited with high conversion efficiency of the exciting light into SLFRS (near

10 %), which is evidence of strong acoustic vibrations of nanoparticles. SLFRS frequency

shifts are determined by the eigenfrequencies of nanoparticles vibrations lying in the

gigahertz range. Frequency shifts were shown to be proportional to 1/D, where D is

nanoparticle diameter (see Figure 1).

Figure 1. Frequency shift of the SLFRS components in NaCl nanoparticles in ethanol.

SLFRS gives possibility to create a source of biharmonic pumping, which may be used in

basic research and for many applications in nonlinear spectroscopy, laser physics, in biology

and medicine. Due to short pulse duration SLFRS can be applied for determination of

nanoparticles size in real time, for instance, in aerosols.

_______________________ 1 A.D. Kudryavtseva, N.V. Tcherniega, M.I. Samoylovich, and A.S. Shevchuk, International Journal of

Thermophysics, 33 (2012) 2194-2202. 2 N.V.Tcherniega, K.I.Zemskov, V.V.Savranskii, A.D.Kudryavtseva, A.Yu.Olenin, and G.V.Lisichkin, Optics

Letters, 38 (2013) 824-826.


— 13 —

Mid-infrared laser-induced thermal grating spectroscopy for detection of

small hydrocarbons

D. Hot1,*

, A.-L. Sahlberg1, J. Kiefer

2,3,4, M. Aldén

1 and Z.S. Li

1

1Division of Combustion Physics, Lund University, P.O. Box 118, S221 00 Lund, Sweden

2Technische Thermodynamik, Universität Bremen, Badgasteiner Str. 1, 28359 Bremen, Germany 3School of Engineering, University of Aberdeen, Aberdeen AB24 3UE, UK

4Erlangen Graduate School in Advanced Optical Technologies, Universität Erlangen-Nürnberg, Erlangen, Germany

*Corresponding author: [email protected], http://www.forbrf.lth.se/english/staff/phd-students/dina-hot/

KEY WORDS: laser-induced thermal grating spectroscopy, mid-infrared, hydrocarbons

We demonstrate mid-infrared laser-induced thermal grating spectroscopy (LITGS) for

detection of the combustion relevant hydrocarbon species CH4, C2H6, C2H2, C2H4 and

CH3OH. The investigated hydrocarbons were diluted in nitrogen gas flows at 296 K and

atmospheric pressure. The two coherent pump beams provided by a pulsed infrared laser

(generated by difference frequency mixing of a dye laser beam with the fundamental output

from an Nd:YAG laser) were tuned to resonant transitions around 3-3.4 μm and crossed in the

measurement point to create an interference pattern. The subsequent thermalization of the

excited hydrocarbon species resulted in a transient density pattern and thus a refractive index

spatial modulation, i.e. a laser-induced grating (LIG). A cw laser (457 nm) was used to probe

the dynamics of the LIG. The probe laser beam was Bragg diffracted by the LIG, forming the

signal. This setup has the advantage of performing spectroscopy in the mid-infrared to give

access to plenty of interesting molecules combined with signal detection in the visible region,

thus being able to take advantage of the more sensitive detectors available for visible light.

The time-resolved LITGS signals, which are rich in information regarding temperature and

chemical composition of the gas flows, were recorded for all investigated hydrocarbon

species. There is a clear difference in the LITGS signal between different hydrocarbons,

which reflects the time scale of the different energy transfer mechanisms. In addition, LITGS

excitation scans were recorded, to investigate the mid-infrared spectral structure of the

hydrocarbons. Figure 1 shows an example of a time-resolved LITGS signal from C2H4 diluted

in N2 at room temperature, together with the LITGS excitation scan of C2H4 in the spectral

region 3200-3240 cm-1

.

Figure 1. LITGS temporal shape at 3200 cm-1

in a gas flow of 2.6 % C2H4 diluted in N2 at 296 K. The red curve

shows the timing of the pump laser pulses. Inset: LITGS excitation scan 3200-3240 cm-1

.


— 15 —

Sum frequency generation microscopy of surfaces

Steven Baldelli Department of Chemistry, University of Houston,

Houston, Texas 77204-5003, United States

KEY WORDS: thermal gratings, degenerate four-wave mixing, polarization spectroscopy

Sum frequency generation spectroscopy (SFG) is a useful technique to study molecular

properties of surfaces. As a second-order technique it is uniquely sensitive to the average

organization of molecules at the surface. However, as most surfaces are spatially

heterogeneous, it is difficult to interpret the spectrum as single domain. The development of

SFG into a microscopy has allow a more detailed and accurate analysis of the spatio-spectro-

temporal evolution of the surface chemistry. The SFG microscope development will be

presented, as well as the use of compressive sensing and the application toward corrosion

inhibition and self-assembled monolayers.


— 17 —

Probing Ice Nucleation abilities of Atmospheric Aerosol Particles using Sum Frequency Generation Spectroscopy

Ahmed Abdelmonem1*, Ellen H.G. Backus2, Thomas Leisner1 and Mischa Bonn2

1Institute of Meteorology and Climate Research – Atmospheric Aerosol Research (IMKAAF), Karlsruhe Institute of Technology (KIT), 76344 Eggenstein-Leopoldshafen, Germany

2 Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany

*Correspondence to: [email protected], https://www.imk-aaf.kit.edu/44_165.php

Key words: Heterogeneous ice nucleation, SFG, Water/Sapphire interface

Heterogeneous ice nucleation on the surface of an atmospheric aerosol particle is important for precipitation formation in mixed phase clouds and for the formation of cirrus clouds. The structural and chemical characteristics of the surface of an ice nucleation particle (INP) play a major role in the ice nucleation ability of that INP. Nevertheless this role is not well explored in terms of surface-surface interactions.

We apply Sum Frequency Generation spectroscopy to study the ice freezing at the water/Sapphire interface on the molecular level. Previous SHG experiments with neutral water have shown that the neat sapphire surface is not a good ice nucleating surface1. Therefore this surface can be used to study the structure of water at the surface upon cooling down to the temperature of heterogeneous freezing. We compare the freezing process of water on a sapphire surface at different surface charges and ions in solution. For the pH9 NaOH sample rapid fluctuations in the SFG intensity of some bands were observed which could be related to transient crystallizations.

1 A. Abdelmonem, J. Lützenkirchen, and T. Leisner (2015). Probing ice-nucleation processes on the molecular level using second harmonic generation spectroscopy. Atmos. Meas. Tech., 8, 3519–3526, 2015

Mica

SFG

Sapphire

T °C10 -30-200

IceWater


— 19 —

Imaging of Graphene with Wide-Field Four-Wave Mixing Microscopy

Juha Koivistoinen1, Jukka Aumanen1, Vesa-Matti Hiltunen2, Pasi Myllyperkiö1, Andreas Johansson1,2 and

Mika Pettersson1* 1Nanoscience Center, Department of Chemistry, P.O. Box 35, FI-40014, University of Jyväskylä, Finland 2Nanoscience Center, Department of Physics, P.O. Box 35, FI-40014, University of Jyväskylä, Finland.

Corresponding Author e-mail address and URL: (8-point type, centered, italicized)

KEY WORDS: Four-wave mixing, Wide-field imaging, online oxidation The single atom thick two dimensional graphene is a promising material for various applications due to its extraordinary electronic, optical, optoelectronic and mechanical properties. The demand for developing graphene based applications has entailed requirement for development of methods for fast imaging techniques for graphene. We developed a method for imaging graphene with femtosecond wide-field four-wave mixing (FWM) microscopy providing sensitive, non-destructive approach for large area imaging of air-suspended graphene. The method is suitable for real-time following of a laser patterning oxidation process0F

1 on single-layer graphene and within sub-second timescale. Also, the wide-field FWM imaging is capable of monitoring large areas of single-layer graphene with proficiency to distinguish sub-micrometer patterned structures. The next step of developing the method is imaging graphene samples on Si/SiO2 substrate using backscattering measurement geometry, hence opening possibility to image dynamics of graphene in different temperatures and, in the future, online following graphene during synthesis.

Nine snap shots of FWM wide-field online imaging of laser patterning1 of suspended-graphene. The gray signal is originated from single layer suspended graphene, the brighter areas are due to inhomogeneities, and the yellow is the laser spot patterning the graphene. In time, the leftmost and the rightmost images are the first and the last, respectively. A square-shaped pattern, which is seen as depletion of the FWM signal, is clearly formed during the process.

1Aumanen, J. Johansson, A., Koivistoinen, J., Myllyperkiö P., Pettersson M. Patterning and tuning of electrical and optical properties of graphene by laser induced two-photon oxidation. Nanoscale, 7 (2015) 2851-2855.


— 21 —

Rationalizing catalyst performance using stimulated Raman microscopy

K.-L. Liu1, T. De Wit1, C. Steuwe1, M.B.J. Roeffaers1

Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, B-3001 Heverlee, Belgium [email protected]

KEY WORDS: SRS, imaging, materials science Solid catalysts are widely used in chemical research as well as in large scale (petro)chemical processes. The catalytic performance is determined by several catalysts properties and molecular processes. So far catalysis research has focused largely on characterizing the inorganic catalyst properties, in this research we applied for the first time simulated Raman scattering (SRS) microscopy to get detailed understanding of catalytic site distribution and the molecular accessibility. Rather than looking at the inorganic compositions, as in electron and X-ray microscopy, SRS microscopy with organic probes molecules enables visualizing the 3D acid site distribution in acid zeolite catalysts.1 Unlike the more commonly used coherent anti-Stokes Raman scattering (CARS), the SRS signal is free from non-resonant background, which allows straightforward quantitative and qualitative analyses. The highly sensitive chemical imaging with sub-micrometer spatial resolution make SRS microscopy a promising tool to investigate catalytic materials. In this presentation the detailed information from SRS microscopy will be complemented by single molecule fluorescence microscopy to give a detailed picture of working zeolite catalysts at the single particle level; as example we will mainly focus on acid mordenites. The presented approach enables unraveling the complex interplay between diffusion, catalytic site distribution and reactions at the single particle level. Furthermore, next to significant intraparticle heterogeneities, the data also reveal important interparticle heterogeneities which have often been overlooked so far. Acknowledgement Financial support from European Research Council for financial support (ERC Starting Grant 307523) is gratefully acknowledged.

1 K.-L. Liu, A. Kubarev et al., ACS Nano 2014, 8(12), 12650.


— 23 —

Stimulated Raman scattering in between nano and biophotonics applications

A.D’Arco1,2, N. Brancati3, M. A. Ferrara1, M. Indolfi1, M. Frucci3, L. Sirleto1* 1 National Research Council(CNR) - Institute for Microelectronics and Microsystems, I-80131 Napoli, Italy

2 Second University of Naples (SUN), Department of Information Engineering, I-81031 Aversa, Italy 3 National Research Council (CNR), Institute for High-Performance Computing and Networking, , I-80131 Napoli, Italy

[email protected] KEY WORDS: Stimulated Raman Scattering; nanolaser; nonlinear microscopy.

Stimulated Raman Scatttering has important connections with nanophotonics and biophotonics. Concerning nanophotonics, one of the most recent challenges is the investigation of ‘nonlinear optical phenomena at nanoscale’. Among them, stimulated Raman scattering is one of the most interesting, due to its significant implications from both fundamental and applicative point of view. Being the essence of SRS phenomena a ‘light amplification’, one of the most important application is the realization of amplifiers or laser sources in bulk materials, in fiber and in integrated optics format as well. In this talk we investigate the possibility of obtaining new materials with both large Raman gain coefficients and spectral bandwidth, taking advantage of optical properties of nanostructures[1]. Concerning biophotonics, a subject of wide interest in the physical and life sciences is the noninvasive characterization of microscopic objects within a complex heterogeneous system through nonlinear optical microscopy. Computational approaches to bioimaging analysis are increasingly used to extract quantitative information about both the structure and dynamics of biological systems at the single-cell level. In this talk, a methodology for delineating subcellular morphology with chemical specificity, combining stimulated Raman microscopy and image analysis technique, will be presented and discussed. 1. L. Sirleto, M. A. Ferrara, T. Nikitin, S. Novikov, and L. Khriachtchev, “Giant Raman gain in silicon nanocrystals”, Nat. Commun.

3,1220 (2012).


— 25 —

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Tuesday, April 26th

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Non-linearopticalhistopathologyutilizingmultimodalCARS/SHG/TPEFimaging

JürgenPopp

LeibnizInstituteofPhotonicTechnology,Albert-Einstein-Str.9,D-07744Jena,GermanyInstituteofPhysicalChemistry,Friedrich-SchillerUniversityJena,Helmholtzweg4,D-07743Jena,

Germany

Newapproachesforafastandreliableinvivoandnearinvivotissuecharacterizationtosupplementroutine pathological diagnostics are needed. This presentation highlights the great potential ofmultimodal nonlinear microscopy combining coherent anti-Stokes Raman scattering (CARS), twophoton excited fluorescence (TPEF) and second harmonic generation (SHG) to complementestablished clinical pathological diagnostic tools and to augment standard intraoperative clinicalassessmentwithmultimodalimagestohighlightfunctionalactivityandtumorboundaries.Acompactand portable multimodal nonlinear microscope for use in clinics together with novel fiber lasersourceswillbeintroduced.Tofacilitatehandlingandinterpretationoftheimagedatacharacteristicpropertiescanbeautomaticallyextractedbyadvancedimageprocessingalgorithms.

Acknowledgements:WethanktheEU,the”ThüringerMinisteriumfürWirtschaft,WissenschaftundDigitale Gesellschaft”, the ”Thüringer Aufbaubank (TAB)”, the Federal Ministry of Education andResearch, Germany (BMBF), the German Science Foundation, the Carl Zeiss Foundation and theFondsderChemischenIndustrieforFinancialsupport.


— 29 —

Raman linewidth measurements using time-resolved hybrid

picosecond/nanosecond rotational CARS

E. Nordström, A. Hosseinnia, C. Brackmann, J. Bood, P.-E. Bengtsson

Combustion Physics, Department of Physics, Lund University

P.O. Box 118, SE-221 00 Lund, Sweden

e-mail: [email protected]

URL: http://www.forbrf.lth.se/

KEY WORDS: rotational CARS, Raman linewidths, streak camera

Coherent anti-Stokes Raman spectroscopy (CARS) is commonly used for gas-phase

thermometry in reactive flows [1]. In order to achieve high thermometric accuracy, knowledge

on Raman linewidths for the probed molecule and its collision partners is often crucial. In recent

years various methods have been developed to measure Raman linewidths using short pulse

lasers, see for example [2,3].

In this work, we report a novel approach for time-domain measurements of S-branch Raman

linewidths using hybrid picosecond/nanosecond pure-rotational Coherent Anti-Stokes Raman

Spectroscopy (RCARS) [4]. The Raman

coherences are created by two

picosecond excitation pulses and probed

using a narrow-band nanosecond pulse.

This generates an RCARS signal

containing the entire coherence decay in

a single pulse and detection with a streak

camera at the output of a spectrograph

provides data with temporal as well as

spectral resolution, see Fig. 1. By

extracting the decay times of the

individual transitions, the J-dependent

Raman linewidths can be calculated. We

report self-broadened S-branch

linewidths for nitrogen (J”=2-18) and

oxygen (N’’=5-27) at 293 K and

ambient pressure, which are in good

agreement with previous time-domain

measurements. Experimental con-

siderations of the approach are discussed

along with its merits and limitations. The

approach can be extended to a wide

range of pressures and temperatures and

has potential for simultaneous single-

shot thermometry and linewidth deter-

mination.

1 S. Roy, J. R. Gord, and A. K. Patnaik, Prog. Energy and Combustion Science 36, 280 (2010). 2 J. D. Miller, S. Roy, J. R. Gord, and T. R. Meyer, J. of Chemical Physics 135, 201104 (2011). 3 A. Bohlin, E. Nordström, B. Patterson, P.-E. Bengtsson, and C. Kliewer, J. of Chemical Physics 137, 074302 (2012). 4 E. Nordström, A. Hosseinnia, C. Brackmann, J. Bood, and P.-E. Bengtsson, Opt. Letters 40(24), 5718-5721 (2015).

Figure 1. Averaged image (a) of the time- and frequency-

resolved RCARS spectrum of N2. The three colored regions

represent the data used to plot the correspondingly colored

signal decays for J=4, 10 and 16 in (b) where a time-resolved

non-resonant signal (measured in argon) is also shown

(crosses). The time constants for the exponential fits to the

decays are indicated in the figure legend. The RCARS

spectrum of the image in (a) is shown in (c) with the same

colored regions indicated [4].


— 31 —

Characterization of bi-spiral twisted supersonic gas flow using time-

resolved picosecond pure rotational coherent anti-Stokes Raman

spectroscopy

A.K.Vereshchagin1, K.A.Vereshchagin

1, V.B.Morozov

2, V.G.Tunkin

2, Kh. Khasanov

3

1 General Physics Institute of RAS, Vavilov Str.38, 119991, Moscow, Russia; 2Lomonosov Moscow State University and International Laser Center, Leninskie Gori,1, 119991, Moscow,Russia

2Lomonosov Moscow State University, Gas and Wave Dynamics Department, Leninskie Gori,1, 119991, Moscow,Russia

Corresponding Author: [email protected]

KEY WORDS: picosecond RCARS, supersonic gas flow

Time-resolved pure-rotational coherent anti-Stokes Raman spectroscopy using picosecond

broadband CARS-spectrometer1 is implemented for mapping of submerged under- expanded

supersonic spiral-twisted gaseous jets2 during its flowing from the annular nozzle with a

central cone (see Fig.1). We have investigated the regular unusual axial symmetric vortex

structures of body rotation and chain structures of jets in nitrogen and air. The type of

structure depends on geometry of nozzle and pressure in pre-chamber. Strong density gradient

appears discretely in mentioned jets.

Figure 1. Submerged under- expanded supersonic spiral-twisted gaseous jet while central conic body

outside the nozzle cut for 3 mm (visualized by direct shadow method).

1 A. Vereschagin, K. Vereschagin, V.Morozov, V.Tunkin, The 13th European Conference on Nonlinear Optical

Spectroscopy (ECONOS). Book of abstracts, p.44. 2 Kh. Khasanov, Physics Letters A, 5 (2012), Vol.376, pp.25-27.


— 33 —

Chirped CARS for microspectroscopy and visualization of oocytes

and embryonic stem cells: merits and demerits

A. Aybush1, F. Gostev

1, V. Nadtochenko

1, K.A.Vereshchagin

2

1 N.N. Semenov Institute of Chemical Physics of RAS, Kosygina st., 4, 117977, Moscow, Russia; 2 A.M. Prokhorov General Physics Institute of RAS, Vavilov Str.38, 119991, Moscow, Russia;


KEY WORDS: CARS-microscopy, Chirped CARS, oocyte, embryonic stem cells

For microspectroscopy of oocytes and chemically-selective 3-D cell imaging and

determination of a chemical composition of organelles in structure of a cell/embryo,

femtosecond CARS-microscopy based on chirped CARS technique1 with scanning of

collinear interacting light beams was used2. Advantages and drawbacks of c-CARS approach

for such a task have been analyzed and reported.

1 K.P. Knutsen, J.C. Johnson, A.E. Miller, P.B. Petersen, R.J. Saykally. Chem. Phys. Let., 387, (2004), 436–441

2 Konstantin A. Vereschagin, E. Shashkov, A. Aybush, F. Gostev, A. Astaf’ev , A. Shakhov, A. Titov, A.

Zalessky, V. Nadtochenko. The 13th European Conference on Nonlinear Optical Spectroscopy (ECONOS).

Book of abstracts, p.40.


— 35 —

Closed-Form Solutions to Time Model for Hybrid fs/ps Coherent Anti-

Stokes Raman Scattering

M. Marrocco ENEA, via Anguillarese 301, Rome, 00123 Italy

[email protected]

KEY WORDS: CARS, spectral analysis, time model

Hybrid fs/ps coherent anti-Stokes Raman scattering (CARS)1, realized with simultaneous

femtosecond pump and Stokes pulses (i.e. impulsive Raman excitation) followed by

picosecond probing, is usually studied by using numerical methods based on the conventional

time-dependent model of Raman coherence1, 2

.

Here, we prove that, in place of numerical solutions, the time model can be treated to a great

extent despite the complications arising from probe pulses of non-trivial profiles. Indeed,

time-symmetric and -asymmetric probes do not hinder signal interpretation via analytical

tools and results are given for a variety of known pulses (Gaussian, square of hyperbolic

secant, rect, sinc, exponential, asymmetric Gaussian, asymmetric square of hyperbolic

secant). Thanks to these achievements, some of the numerical efforts that are common in the

conventional approach to time-resolved CARS can be avoided and the advantages resulting

from fast calculation become evident in spectral imaging. Examples are provided in the figure

where probes with rect (or square) and sinc time profiles are used to simulate known

experimental results for benzonitrile3 and nitrogen

1.

Two examples of simulated delay-dependent spectra of hybrid fs/ps CARS of benzonitrile and nitrogen probed

respectively by means of rect (or square) and sinc pulses. The images reproduce experimental results found by

Selm et al.3 for benzonitrile and Satuffer et al.

1 for nitrogen. The laser parameters used in the simulations

corresponds to those employed in the cited experiments.

1 H. U. Stauffer, J. D. Miller, M. N. Slipchenko, T. R. Meyer, B. D. Prince, S. Roy, and J. R. Gord, J. Chem.

Phys., 140 (2014) 024316. 2 S. Mukamel, Principles of nonlinear optical spectroscopy (Oxford University Press, Oxford, 1995).

3 R. Selm, M. Winterhalder, A. Zumbusch, G. Krauss, T. Hanke, A. Sell, and A. Leitenstorfer, Opt. Lett. 35

(2010) 3282-3284.


— 37 —

Temperature and Major Species Detection in Particle-Laden Flames by

fs/ps Rotational CARS

Sean Kearney Engineering Sciences Center, 9100,

Sandia National Laboratories, P.O. Box 5800, MS 0834,

Albuquerque, NM 87185-0834


KEY WORDS: CARS, combustion diagnostics

A hybrid CARS instrument with broadband femtosecond Raman preparation and a frequency

narrow, picosecond probe generated by second-harmonic bandwidth compression (SHBC) is

presented. The high probe-beam energies provided by SHBC enable acquisition of good quality

pure-rotational CARS spectra at flame temperatures in excess of 3000 K on a single laser shot.

Our instrument is demonstrated in a variety of hostile, particle-laden flames including a sooting

turbulent C2H4 jet flame and the high-temperature plume emanating from a burning aluminized

propellant. The system is capable of temperature and relative O2 measurements in the presence

of significant amounts of soot and large-scale aluminum particles.


— 39 —

Ethane thermometry using rotational

coherent anti-Stokes Raman scattering (CARS)

A. Hosseinnia, E. Nordström, J. Bood, P.-E. Bengtsson

Combustion Physics, Department of Physics, Lund University

P.O. Box 118, SE-221 00 Lund, Sweden


URL: http://www.forbrf.lth.se/

KEY WORDS: rotational CARS, thermometry, ethane

Coherent anti-Stokes Raman scattering (CARS) has during the last decades been an essential

tool for combustion diagnostics, most importantly for accurate thermometry. Diatomics and

triatomics of high abundance in combustion have been probed using rotational as well as ro-

vibrational transitions. These species include oxygen (O2), nitrogen (N2), and the products

carbon dioxide (CO2), water (H2O), carbon monoxide (CO), and hydrogen (H2). For these

molecules highly resolved spectra have been recorded and fitted to theoretical models, and

subsequently used for thermometry and species concentration measurements. Less attention

has been paid to high-resolution CARS of fuel

molecules, motivating the present study of

rotational CARS on ethane.

The complete rotational CARS (coherent anti-

Stokes Raman scattering) spectrum of ethane

(C2H6) has for the first time been recorded

instantaneously under high spectral resolution, and

the potential for thermometry has been investigated

[1]. Experiments were performed in the temperature

range 292 – 650 K in pure ethane and in binary

mixtures with nitrogen. Experimentally recorded

spectra at different temperatures are shown in Fig.

1. A polarization technique was used to suppress the

non-resonant contribution to the CARS signal [2].

The ethane RCARS spectra show both S- and R-

branch lines, which are more closely spaced than for

the well-known nitrogen spectrum and located at

much smaller Raman shifts. The peak signal

strength was found to be around 240 times lower for

ethane than for nitrogen (at 292 K). Two main

approaches for ethane thermometry are evaluated,

which both show high potential. The first is a

method in which a spectrum with unknown

temperature is fitted using a library of experimental

spectra recorded at various temperatures. The

second is a method based on ratios of integrated

signals in different spectral regions. A theoretical

model that fairly well can reproduce the

experimental spectra is under development.

1 A. Hosseinnia, E. Nordström, J. Bood, P.-E. Bengtsson, Ethane thermometry using rotational coherent anti-Stokes Raman

scattering (CARS), submitted to the 36th Int. Symp. on Combustion (2016.). 2 F. Vestin, M. Afzelius, P.-E. Bengtsson, Proc. Comb. Inst. 31, 833-840 (2007).

Figure 1. Rotational CARS spectra of ethane

averaged over 1500 shots recorded at

atmospheric pressure at a temperature of a)

292 K, b) 500 K, and c) 650 K.


— 41 —

Optimizing spectral focusing CARS by tailored probing

L. Brückner, T. Buckup, M. Motzkus Physikalisch-Chemisches Institut, Im Neuenheimer Feld 229, 69120 Heidelberg, Germany


KEY WORDS: Coherent anti-Stokes Raman microscopy; pulse shaping; coherent control.

We present a novel scheme for spectral focusing using a broadband sub-10 fs oscillator in

combination with a pulse shaper controlling the spectral phase and amplitude of the laser.

Applying equal amounts of chirp to the pump and Stokes frequencies focuses the spectral

amplitude into a specific Raman line. The achieved constant instantaneous frequency

difference (IFD) induces a coherence and signal is generated by interaction with the probe. In

typical spectral focusing setups, the chirp is applied by dispersive elements like glass and the

highly chirped pump acts as probe. We show that using a shaper offers many advantages,

especially due to the fact that the phase of the probe frequencies can be controlled

independently.

By identifying the role of the different spectral regions, the flexibility of the pulse shaper can

be exploited in order to variably adjust the instantaneous bandwidth of pump and Stokes to

the linewidth of different Raman modes while independently tailoring the phase of the probe.

A significant increase in signal intensity in comparison with usual spectral focusing schemes

is readily obtained by time-delaying the probe frequencies, allowing the build-up of the

coherence. Additional delay and the knowledge of the region of probing frequencies in

combination with the addressed Raman line determines the detection window for the

generated background-free signal. The resulting signal enhancement and improved contrast is

demonstrated by imaging the CH-resonance around 2850 cm-1 of lipid cells in human skin

tissue. Furthermore, the transform-limited nature of the delayed probe greatly increases TPEF

and SHG signal intensities, which is beneficial for simultaneous multimodal imaging.

In addition, due to the high degree of control using the pulse shaper, spectral focusing can be

applied in a broad spectral range. By scanning the IFD of the chirped pump and Stokes

frequencies, microspectroscopy in the fingerprint region can be performed and is shown

exemplarily on the Raman line of toluene at 1004 cm-1.1,2

L. Brückner, T. Buckup and M. Motzkus, Opt. Lett. 40, (2015) 5204-5207.

J. Rehbinder, L. Brückner, A. Wipfler, T. Buckup, and M. Motzkus, Opt. Express 22, (2014) 28790.

pump

probe

Stokes

Left: Spectrum and time-frequency plot for tailored spectral focusing. The IFD is set to the CH-

resonance of lipids at 2850 cm-1. The frequencies acting solely as probe are delayed in time in order

to maximize the signal by probing after the build-up of the coherence. Right: Obtained spectral

focusing CARS image of lipid cells in human skin tissue (200 µm x 200 µm).


— 43 —

Simultaneous Single-Shot Thermometry and Detection of Minor

Species via Femtosecond, Fully Resonant Electronically Enhanced CARS

(FREE-CARS)

H. U. Stauffer1,*

, P. J. Wrzesinski2, J. B. Schmidt

1, D. R. Richardson

1, S. Roy

1, and J. R. Gord

2

1Spectral Energies, LLC, 5100 Springfield St., Suite 301 Dayton, OH 45431 2Aerospace Systems Directorate, Air Force Research Laboratory, Wright-Patterson Air Force Base, Ohio 45433

*Corresponding Author e-mail address: [email protected]

KEY WORDS: Fully resonant CARS, femtosecond gas-phase diagnostics, minor-species

detection

Femtosecond time-resolved, fully resonant electronically enhanced coherent anti-Stokes

Raman scattering (FREE-CARS) spectroscopy is used to demonstrate selective and sensitive

detection of gas-phase species. This approach, incorporating a two-color ultraviolet excitation

scheme, is applied toward nitric oxide (NO) and the hydroxyl (OH) radical. The observed

time-dependent spectrally resolved CARS signal (Fig. 1) contains rich structure that depends

on both a) the rovibronic states accessed within the bandwidth of the initial (pump) excitation

pulse; and b) the Raman-active rovibrational levels within the vibrationally excited ground

electronic state that are accessed following interaction with the second (Stokes) excitation

pulse. For OH radical detected in a laminar ethylene–air flame, spectral resolution of the

emitted FREE-CARS signal allows simultaneous detection of relative OH mole-fraction and

temperature under single-laser-shot conditions. High-precision (1-σ standard deviation <3%)

temperature measurements with simultaneous determination of OH concentration are

observed under single-shot conditions for fuel–air equivalence ratios (φ) ranging from

φ = 0.45 to φ = 1.6.

Fig. 1. a) Example FREE-CARS signal from gas-phase NO when probe pulse arrives

1.0 ps after time-overlapped pump/Stokes pulses. b) Contour plot depicting beat

frequencies observed during Stokes/probe evolution period.


— 45 —

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Wednesday, April 27th

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New laser architecture for hybrid fs-ps/CARS applied to thermometry and molecular probing

M. Scherman1, M. Nafa1, A. Bresson1, H. Danvy1, A. Godard1, T. Schmid1, B. Attal-

Tretout1 and P. Joubert² 1 ONERA, The French Aerospace Lab, F-91123 Palaiseau Cedex, France 2 Institut UTINAM, UMR CNRS 6213, Université de Franche-Comté, 25030 Besançon Cedex, France

High speed laser diagnostic techniques have proven to be very powerful for the study of the combustion in real turbulent media [1]. Among other techniques, hybrid femto-picosecond CARS [2] is showing great potential and has been successfully applied in gaseous media. It allows to retrieve point information of temperature or chemical composition at high repetition rate (kHz) [3], 2D hyperspectral images [4] and ultra-broadband spectra [5] in single shot.

An original laser architecture was built at ONERA in order to produce the exciting beams, namely broadband Pump and Stokes pulses, combined to a narrowband picosecond probe pulse out of a single Yb:KGW laser chosen and tested in that regards. Pulse shaping is achieved thanks to a volume Bragg grating (VBG). It is a monolithic element that acts as an ultra-narrow band filter. We have shown that VBG provides a good enough spectral resolution (0.7 cm-1) In order to properly resolve the fine structure of N2 Q-branch from which temperature is extracted. The compact and mobile CARS system was designed and tested so as to operate in combustion facility with robust fiability.

Using that CARS setup, the spectro-temporal ro-vibrational response [6] of nitrogen molecule was recorded in ambient air and in a CH4-air flame. Good performances are obtained as regards to signal intensity, non resonant rejection, shot to shot fluctuation and other critical parameters both in cold and hot gases. Following recent suggestion [7], we studied particular pump/probe delay windows that better investigate either cold or hot gases in order to propose optimal measurement strategies mainly adapted to turbulent experimental situations. Spectroscopic properties of the apparatus were also demonstrated on other molecules of interest for combustion sensing.

[1] S. Roy, J. Gord, and A. Patnaik, "Recent advances in coherent antistokes Raman scattering spectroscopy : Fundamental developments and applications in reacting flows", Prog. in Energy and Combustion Science 36, 280 (2010). [2] B.D. Prince, A. Chakraborty, B.M. Prince, and H.U. Stauffer, "Development of simultaneous frequency- and time-resolved coherent antistokes raman scattering for ultrafast detection of molecular raman spectra", J. Chem. Phys. 125, 044502 (2006) [3] J. D. Miller, M. N. Slipchenko, T. Meyer, H. U. Stauffer, J. Gord, "Hybrid femtoseconde/picosecond coherent anti-Stokes Raman scattering for high speed gas phase thermometry", Optics Letters 35, 2430-2432 (2010). [4] A. Bohlin and C. Kliewer, "Two-dimensional gas-phase coherent antistokes Raman spectroscopy (2d-cars): Simultaneous planar imaging and multiplex spectroscopy in a single laser shot", J. Chem. Phys. 138, 221101 (2013) [5] A. Bohlin, C. Kliewer, "Two-beam ultrabroadband coherent anti-Stokes Raman spectroscopy for high resolution gas-phase multiplex imaging", Applied Physics Letters 104, 031107 (2014) [6] H. Stauffer, J. Miller, M. Slipchenko, T. Meyer, B. Prince, S. Roy, and J. Gord, "Time- and frequency-dependent model of time-resolved coherent anti-stokes raman scattering (cars) with a picosecond-duration probe pulse", J. Chem. Phys. 140, 024316 (2014). [7] J. Miller, C. Dedic, and T. Meyer, “Vibrational femtosecond/picosecond coherent anti-stokes raman scattering with enhanced temperature sensitivity for flame thermometry from 300 to 2400k,” J. Raman Spectrosc. 46, 702 (2015).


— 49 —

Spatially resolved, in situ, non-intrusive detection of hydrocarbon

intermediate species in a rich low-pressure dimethyl-ether/oxygen/argon

premixed flame

A.-L. Sahlberg1, D. Hot1, R. L. Pedersen1, J. Zhou1, M. Aldén1, Z.S. Li1

1Division of Combustion Physics, Lund University, P.O. Box 118, S-221 00 Lund, Sweden

[email protected], http://www.forbrf.lth.se/english/staff/phd-students/anna-lena-sahlberg/

KEY WORDS: polarization spectroscopy, low pressure flame, dimethyl ether

Low pressure laminar flames have been widely employed for the investigation of combustion

chemistry of different fuels. The distributions of different combustion intermediates species in

laminar flames as the key information are commonly measured with probing techniques, such

as molecular beam mass spectroscopy (MBMS). While MBMS is useful for studying many

species at the same time, it is also an intrusive probing technique, which may affect the flame

chemistry. It is thus of crucial importance to check the potential intrusiveness of these probing

techniques with nonintrusive optical techniques.

Dimethyl ether (DME) has been widely studied as a potential alternative to diesel and

biodiesel, but it is still a relatively new fuel and measurements of the chemistry are very

interesting. A detailed study of dimethyl ether/oxygen/argon flames at many different flame

conditions using MBMS was recently performed by Wang et al.1 In this work, we have

studied a similar rich flame as presented by Wang et al., to demonstrate the measurement

capability of infrared polarization spectroscopy (IRPS) as a diagnostic tool to validate MBMS

measurements.

IRPS is useful for studies of species that don’t have easily accessible electronic transitions.

Specifically, many important hydrocarbon species can be studied through the asymmetric C-H

vibration bands around 3 μm. We demonstrate non-intrusive, in situ detection of CH4, C2H2

and C2H6 in low pressure rich dimethyl ether/oxygen /argon flat flames using IRPS, by

probing the asymmetric C-H stretching vibration bands in the respective molecules. CH4,

C2H2 and C2H6 absorption lines are identified in the IRPS spectra through comparison with

the HITRAN and HITEMP databases. The flames were stabilized on a McKenna-type porous

plug burner. The temperature was measured using the line ratio of H2O lines, and was

compared with CHEMKIN simulations. These measurements prove the possibilities of IRPS

as a sensitive, non-intrusive technique for detection of many small hydrocarbons in low

pressure flames, and the possibility of using this technique to validate probe measurements in

flames.

1J. Wang, M. Chaos, B. Yang, T. A. Cool, F. L. Dryer, T. Kasper, N. Hansen, P. Osswald, K. Kohse-Hoinghaus,

P. R. Westmorelande, Phys. Chem. Chem. Phys. 11 (2009) 1328-1339


— 51 —

Metal-Molecule Interactions Investigated in Frequency and Time Domain

A. Materny*, P. Donfack, T. Z. Khan, M. M. Kazemi, F. Mohaghegh, A. M. Tehrani Department of Physics and Earth Sciences, Jacobs University Bremen, Campus Ring 1, 27759 Bremen, Germany

* [email protected], www.jacobs-university.de

KEY WORDS: Linear and nonlinear Raman, surface enhancement, plasmon-molecule

interactions

Vibrational and electronic properties of molecules adsorbed to metals can be strongly

influenced by the interaction between metal electrons and the electronic system of the

molecules. This is well known from the surface-enhancement (SE) observed for Raman

scattering when nanoparticles of coin metals are added to a sample containing a low

concentration of specific molecules. There, besides the pure enhancement of the Raman

scattering also changes in the Raman spectra can be observed. For a better understanding of

this so-called chemical or electronic SE mechanism of the SE Raman scattering (SERS),

different experiments have been performed, which try to combine the energetic with the

dynamic picture of this mechanism.

The investigations starting from linear Raman spectroscopy to femtosecond time-resolved

nonlinear Raman and pump-probe spectroscopy will be discussed. In order to create well-

defined conditions for the interaction of metal-plasmons and the electronic system of

molecules, a Kretschmann setup has been chosen, which allows for a phase-matched

excitation of surface polaritons in a flat silver layer. Additionally, scanning near-field optical

microscopy (SNOM) has been combined with ultrafast spectroscopy to access the dynamics

in a range of few nanometers at the interface between a molecular layer and a thin gold

coating.

Figure: Scanning near-field microscopy combined with a tip-enhancement effect allow for accessing

interfaces between an organic semiconductor layer and a gold coating, yielding changed exciton

dynamics compared to bulk values.

The experiments show that the electronic coupling strongly influences the response of the

molecules to the exciting laser fields in the SERS process. This is a highly mode-specific

mechanism, which yields drastically different response for different vibrational modes.

Additionally, a nonlinear dependence of the Raman scattering of the incoming light intensity

can be observed. In time domain it can be demonstrated that the dynamics of excited

electronic molecule states is clearly changed when the molecules are in contact with metal.


— 53 —

Unravelling the Complex Electronic Structure of Transition Metal Dimers

using Four-Wave Mixing Techniques

B. Visser1, M. Beck

1, P. Bornhauser

1, G. Knopp

1, T. Gerber

1, R. Abela

1, J. A. van Bokhoven

1,2 and P. P.

Radi1

1Paul Scherrer Institut, 5232 Villigen, Switzerland

2ETH Zürich, 8093 Zürich, Switzerland [email protected]

KEY WORDS: four-wave mixing, transition metals, copper dimer

Two-color resonant four-wave mixing is a form of non-linear optical spectroscopy that results

in the creation of a laser-like signal beam. It has numerous advantages over standard

spectroscopic techniques, such as background free detection of a spatially separated signal,

spectral selectivity due to double resonance restrictions and does not require fluorescent

coupling to known electronic states.

Gas phase spectroscopy of transition metal dimers, clusters and metal containing complexes is

complicated by the presence of numerous additional atomic and molecular species resulting

from the typical sources used. The experimental techniques that can effectively separate

spectra from individual spectral carriers (e.g. REMPI) run into difficulties with the sheer

number of low-lying excited electronic states that result from the open d shell electronic

configurations.

We have recently built a laser vaporization source for the stable production of transition metal

dimers and small metal clusters for use with four-wave mixing techniques. Initial experiments

on the copper dimer have shown the power of these techniques to selectively excite and thus

simplify the spectra of this species in a molecular beam environment.1 Our recent

identification of the A′ state in Cu2 resolves a long standing mystery and provides further

insight into the coupling of ‘d-hole’ excited states.

In this contribution we will show the application of four-wave mixing techniques to transition

metal species in molecular beam environments using the example of the copper dimer.

Furthermore, the future use of these techniques to disentangle the complex electronic

structure of transition metals and extend the achievements of single-resonance studies will be

discussed.

An example TC-RFWM isotopologue and J selective spectrum of the A′-X (0,0) transition in Cu2.

B. Visser, M. Beck, P. Bornhauser, G. Knopp, T. Gerber, R. Abela, J. A. van Bokhoven, P. P. Radi, J. Raman

Spec., Published online (2015) DOI: 10.1002/jrs.4841.


— 55 —

Label-free detection mechanism for carbon nanoparticles using femtosecond pulsed

illumination

Christian Steuwe‡1,2, Hannelore Bové‡1,2, Maarten Roeffaers1, and Marcel Ameloot2

1 Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, 3001 Leuven, Belgium 2 Biomedical Research Institute, Hasselt University, Agoralaan Building C, 3590 Diepenbeek, Belgium

‡ These authors contributed equally to this work

Contact: [email protected]

While adverse health effects of particulate matter exposure are a generally accepted concern, locating

and tracking these nanometer sized particles is not straight forward. Measurements1-3 in polluted air

such as absorption photometry and laser induced incandescence (LII) have so far been used to

determine particle concentrations, alternatively labeling methods4-6 have been applied in

epidemiological and toxicology research such as the technetium-99-m radionuclide marker. In this

paper we present a direct, label-free optical contrast mechanism to detect carbon nanoparticles in fluids

and cells. The mechanism is non-incandescence related and demonstrated with dry and suspended

carbon black particles (CB), a widely used model compound for soot7,8, under illumination with

femtosecond pulsed near-infrared light (780 nm - 950 nm, 150 fs, 80 MHz). Four different, strongly

absorbing CB species with diameters ranging from 13 to 500 nm have been scrutinized, all showing

similar detection possibilities. Consequently, the described WL emission allows optical detection and

unequivocal localization of CB particles in fluids and in cellular environments. The experiments are

performed on a typical multiphoton laser-scanning microscopy platform, a system commonly available

in research laboratories.

1. Chow, J. C.; Watson, J. G.; Doraiswamy, P.; Chen, L.-W. A.; Sodeman, D. A.; Lowenthal, D. H.; Park, K.; Arnott,

W. P.; Motallebi, N. Atmos. Res. 2009, 93, (4), 874-887.

2. OECD. Methods of Measuring Air Pollution: Report of the Working Party on Methods of Measuring Air Pollution

and Survey Techniques; Organization for Economic Co-operation and Development: Paris, France, 1964.

3. Schulz, C.; Kock, B. F.; Hofmann, M.; Michelsen, H.; Will, S.; Bougie, B.; Suntz, R.; Smallwood, G. Appl. Phys.

B 2006, 83, (3), 333-354.

4. Kong, H.; Zhang, Y.; Li, Y.; Cui, Z.; Xia, K.; Sun, Y.; Zhao, Q.; Zhu, Y. Int. J. Mol. Sci. 2013, 14, (11), 22529-

22543.

5. Wang, H.-f.; Troxler, T.; Yeh, A.-g.; Dai, H.-l. J. Phys. Chem. C 2007, 111, (25), 8708-8715.

6. Nemmar, A.; Hoet, P. M.; Vanquickenborne, B.; Dinsdale, D.; Thomeer, M.; Hoylaerts, M.; Vanbilloen, H.;

Mortelmans, L.; Nemery, B. Circulation 2002, 105, (4), 411-414.

7. Arnal, C.; Alzueta, M.; Millera, A.; Bilbao, R. Combust. Sci. Technol. 2012, 184, (7-8), 1191-1206.

8. Tankersley, C. G.; Bierman, A.; Rabold, R. Inhal. Toxicol. 2007, 19, (8), 621-9.


— 57 —

Low noise picosecond fiber laser pumped OPO for improved sensitivity in

coherent Raman microscopy

H-C. Becker1*, Ingo Rimke2 1 Gammadata Instrument AB,Uppsala, Sweden

2 A.P.E. Berlin GmbH

Corresponding Author e-mail address: [email protected]

KEY WORDS: CARS, Raman spectroscopy

We describe a picosecond OPO light source and its application for Raman spectroscopy. In

particular, we focus on how to improve CARS and SRS signal to noise and sensitivity.

Experimental data showing the improvement is shown along with the technical development

done to achieve the desired performance. In summary, using 2 ps, 10 cm-1 bandwidth pulses

we obtain 2.5x higher signal in SRS, and 10x higher signal in CARS compared to standard,

solid-state-pumped OPO systems. Furthermore, the 2 ps pulse length and high output energy

of the OPO is also usable for multiphoton absorption and SHG imaging. We also show how a

sensitive lock-in amplifier and detector unit can be integrated into standard microscopes.

Furthermore, we show how modulation of the output beam can be used for video-rate imaging

of live cells and other specimens.


— 59 —

qpqpqp Poster Presentations qpqpqp

Simultaneous Vibrational Raman and CARS Spectroscopy for Gas

Temperature and Composition

K. Becker1, J. Kiefer1* Technische Thermodynamik, Universität Bremen, Badgasteiner Str. 1, 28359 Bremen, Germany

Corresponding Author e-mail address and URL: [email protected], www.thermo.uni-bremen.de

KEY WORDS: CARS, Raman, Optimization

The temperature and the chemical composition are key parameters in the characterization of

combustion systems. While coherent anti-Stokes Raman scattering (CARS) spectroscopy is a

well-established thermometry tool, its capability for multispecies measurements is limited. On

the other hand, spontaneous Raman scattering spectroscopy is well suited for detecting all

major species in a gas simultaneously. Therefore, it is very attractive to combine both

techniques.

In the past, pure rotational CARS was combined with Raman spectroscopy in order to

investigate the evaporation in a liquid fuel spray.1 At high temperature, however, rotational

CARS exhibits less sensitivity and hence vibrational CARS is better suited. Unfortunately,

combining vibrational CARS with vibrational Raman spectroscopy is not as straightforward

as rotational CARS. Selecting an appropriate combination of laser sources in order to obtain

sufficient signal intensities for both techniques while minimizing cross interferences is

important.

The present work reports a systematic analysis of the different possibilities for combining

vibrational CARS with vibrational Raman spectroscopy, where a dual-pump CARS approach

allows to use one CARS pump laser as the excitation source for Raman scattering. A

simplified approach for the evaluation of relative signal intensities is demonstrated. In

addition, a computational method for estimating the probe volume size and length is shown.

The results indicate that there is not THE optimal configuration, but approaches to maximize

the intensities of the different signals or to optimize the spatial resolution can be derived from

the present work.

Fig. 1. Energy level diagrams of dual-pump CARS and spontaneous Stokes Raman scattering.

1 M.C. Weikl, F. Beyrau, J. Kiefer, T. Seeger, and A. Leipertz, Optics Letters, 31 (2006) 1908-1910.


— 63 —

- POSTER -

Comparison of Different Raman Crystals as a Narrowband Light Source

for a Vibrational CARS System Applied to Sooting Flames

Johannes W. Tröger1,2, Christian Meißner1, Frank Beyrau3, Thomas Seeger1,2,4 1Engenieering Thermodynamics, University of Siegen, Paul-Bonatz-Str. 9-11, 57076 Siegen, Germany

2Erlangen Graduated School in Advanced Optical Technologies (SAOT), University of Erlangen Nuremberg, Paul-Gordan-Str. 6, 91052 Erlangen Germany

3Technical Thermodynamics, Otto-von-Guericke University Magdeburg,Universitätsplatz 2, 39106 Magdeburg, Germany 4ITMO University Saint Petersburg, Kronverkskiy prospect 49, 197101 Saint Petersburg, Russia

Corresponding Author e-mail address and URL: [email protected], www.mb.uni-siegen.de/tts

KEY WORDS: dual-pump CARS, Raman crystal, thermometry

Standard vibrational coherent anti-Stokes Raman spectroscopy (CARS) is using two frequency

doubled Nd:YAG laser beams as pump and probe beams together with a broadband dye-laser

for the Stokes beam. This is a well established tool for temperature measurements in various

combustion processes. However, its application to sooting flames faces some drawbacks since

the N2 CARS signal appears at about 473 nm, which is the same spectral region as the C2 Swan

band. This leads to falsification of measurement results and a significant error in the

temperature determination when standard vibrational CARS is used for N2-thermometry1.

Different approaches have been proposed in the past to overcome this problem. One option is

to use a rather complex dual-pump vibrational CARS setup including an additional expensive

narrowband dye laser2. Another approach called shifted vibrational CARS is also using an

additional expensive narrowband dye laser3. In this work, we propose a novel method using a

Nd:YAG laser-pumped Raman crystal as narrowband light source. Two Raman crystals, a

Barium Nitrate (Ba(NO3)2) and an undoped potassium gadolinium tungstate (KGd(WO4)2) are

investigated in respect of their suitability for their application in a vibrational CARS system for

sooting flames.

Conversion efficiency of the KGd(WO4)2 Raman crystal for different pump energies using a picosecond pulsed

frequency-doubled Nd:YAG laser as light source

1 P.-E. Bengtsson, M. Aldén, S. Kröll, D. Nilsson, Combust. Flame, 5, (1990), 25. 2 A. Malarski, F. Beyrau, A. Leipertz, J. Raman Spectrosc., 36, (2005), 102. 3 M.S. Tsurikov, K.P. Geigle, V. Krüger, Y. Schneider-Kühnle, W. Stricker, R. Lückerath, R. Hadef, M. Aigner,

Combust. Sci. Technol., 177, (2005), 1835.


— 65 —

Development of CPP femtosecond CARS for 1kHz single-shot thermometry

F. Berthillier, B. Barviau, F. Grisch CORIA-UMR 6614- Normandie Université - CNRS-Université et INSA de Rouen

Campus Universitaire du Madrillet - 76800 Saint Etienne du Rouvray, France. Corresponding Author: [email protected]

KEY WORDS: CPP fs CARS, high-repetition rate thermometry, CARS modelling.

For nearly four decades, considerable efforts have been devoted to improve the design

and the optimization of high performance aircraft and rocket combustors. Most of the

experimental studies aim at a better understanding of the underlying physical phenomena and

rely on advanced optical diagnostics, which feed numerical solvers with measurements of

scalar parameters. Among the optical diagnostics available thus far, coherent anti-Stokes

Raman scattering (CARS) is recognized as a powerful laser diagnostic for detailed study of

combustion chemistry and physics with high spatial and temporal resolutions, even in harsh

conditions. The availability of commercial high-repetition rate femtosecond lasers made this

temporal resolution thermometry possible and permitted detailed investigations on turbulent

flows dynamics1,2,3.

Chirped-probe-pulse (CPP) fs CARS is one of the techniques providing time-resolved single-

shot measurements4. In this way, the investigation of nitrogen Raman transitions (2330 cm-1)

is developed by using a high-energy 1kHz Ti:Sapphire laser, 12mJ/pulse, 100fs full width at

half maximum (Legend Elite Duo HE+III from Coherent). A 55% part of this 800nm laser

output is directed into an OPA (TOPAS Prime Plus from Light Conversion) to form the probe

and pump pulses at 675nm. The 45% remaining part is dedicated to the Stokes pulse. Chirped

probe pulse is generated by passing through a 30-cm dispersive glass rod. The spatial overlap

of the three pulses at the probe volume is then achieved using the well-known folded

BOXCARS5 configuration. The CARS signal generated is finally collected on a spectrograph

and a CCD camera (Princeton ProEM-HS 512x512).

First experimental results are compared to numerical computation, which provides time-

resolved CPP fs CARS spectra for our setup parameters. Temperature determination is

performed by fitting theoretical spectrum with experimental data minimizing the associated

least-square function. This investigation is carried out for a temperature range from 300 K to

600 K at atmospheric pressure by heating a non-reactive gas flow. Accuracy of the

temperature measurement is evaluated by comparison with the data obtained by

thermocouple. The effect of the probe time delay on the experimental CARS signal and its

similarity with the numerical behavior is also investigated. Probe time delay is a parameter

easy to change experimentally compare to other parametric variables (chirp, pulse

duration…). Other numerical parametric investigations are presented in order to establish

guidelines for improving the experimental setup.

1 S. Roy, J.R. Gord, A.K. Patnaik, Progress in Energy and Combustion Science, 36 (2010) 280-306. 2 A. Bohlin, M. Mann, B.D. Patterson, A. Dreizler, C.J. Kliewer, Proceeding of the Combustion Institute, 35

(2015) 3723-3730. 3 C.N. Dennis, C.D. Slabaugh, I.G. Boxx, W. Meier and R.P. Lucht, Proceeding of the Combustion Institute, 35

(2015) 3731-3738. 4 D.R. Richardson, R.P. Lucht, W.D. Kulatilaka, S. Roy and J.R. Gord, Applied Physics B, 104 (2011) 699-714. 5 S.A.J. Druet and J.P.E. Taran, Progress in Quantum Electronics, 7 (1981) 1-72.


— 67 —

Evaluation of a Parabolic Scan Unit for Stimulated Raman Scattering

Microscopy

A. Rae1

National Physical Laboratory, Teddington, London, TW11 0LW

[email protected]

KEY WORDS: SRS, Metrology, Optical Aberration

The wide wavelength range utilized for coherent Raman microscopy makes the design of scan

relay optics a challenging task. Typical laser scanning confocal setups utilize two galvanometric

mirrors and achromatic relay optics. However, most standard achromatic lenses introduce

significant optical aberrations, even at small scan angles. The amplification of these aberrations

through the following optics, including the objective, significantly reduce the performance of

the system from the diffraction limit. Additionally, axial chromatic aberrations introduced by

intermediate scan optics lead to an appreciable reduction in signal intensity in multi-wavelength

techniques such as SRS and CARS.

We present a parabolic mirror based scan relay unit optimized for coherent Raman microscopy.

The performance of this scan unit is evaluated and compared against the typical achromatic

relay setup.

Cross section of the 100 nm polystyrene bead reference sample used to characterize the performance of the

parabolic scan unit.


— 69 —

Line Space Theory of Resonant Four-Wave Mixing by Rotationally

Anisotropic Photofragments

A. Kouzov

1,*, P. Radi

2, N. Egorova

3

1Saint-Petersburg State University, Ulianovskaya str. 3, Petrodvoretz, Saint-Petersburg 198504, Russia 2Paul Scherrer Institute, 5232 Villigen, Switzerland

3Saint-Petersburg University of State Fire Service of EMERCOM, Moskovsky pr. 149, Saint-Petersburg 196105, Russia *Corresponding Author. E-mail: [email protected]

KEY WORDS: Resonant four-wave mixing, rotational and translational anisotropies of

photofragment states

Based on the line-space (Liouville) quantum formalism, the potential of Resonant Four-Wave

Mixing spectroscopy as a new tool to study rotational and translational anisotropy of

photofragments produced by absorption of plane-polarized photons is theoretically addressed.

Due to synergy of the flexible polarization setup, fine quantum state resolution and of the

possibility to study translational recoil distributions, the tool is unsurpassed among the all-

optical means to interrogate the photofragment states. It furnishes a direct way to separate

signals induced by the rotational anisotropy which remain silent in laser-induced fluorescence

spectra and, as such, constitutes a promising approach to study rotational helicity, one of the

crucial signatures of the photolytic bond rupture mechanism. A Fortran code to calculate a set

of irreducible polarization tensors appearing in the case of collinear RFWM geometry is

also reported.


— 71 —

Kerr lensing effects in time-gated imaging of atomizing sprays

M. Rahm,1 D. Sedarsky,1 and M. Linne2 1Division of Combustion, Department of Applied Mechanic, Chalmers University of Technology, Gothenburg, Sweden.

2School of Engineering, University of Edinburgh, Edinburgh, UK. Corresponding Author: [email protected]

KEY WORDS: Optical Kerr effect, imaging through turbid media.

In modern compression ignition engines liquid fuel is converted into fuel vapor using

vigorously atomizing sprays. The spray formation process, starting with the flow inside the

injector nozzle and ending with a developed spray is, however, not fully understood. Among

other experimental challenges, the adverse conditions for optical techniques imposes

limitations in this region; larger liquid structures undergoing breakup can be shielded from

direct view by a very dense cloud of fuel droplets. To address this challenge, various

specialized techniques have been developed in order to penetrate this dense cloud of

scattering droplets. Time-gating schemes based on ultrafast optical Kerr effect (OKE) gates

such as ballistic imaging (BI) and time-gated optical sectioning are examples on such

techniques.

Commonly the time-gated techniques are using femtosecond laser systems as the source light,

and the OKE is used to induce a transient birefringence Kerr active media. This transient

birefringence can be used to filter image pulses in the time domain. In this way image noise

from multiply scattered light can be reduced. The OKE, however, induces other effects in

addition to time gating.

In this work Kerr lensing effects in OKE-gated BI-setups were investigated. The investigation

showed that Kerr lensing can occur in the OKE-gates as used. This lensing can induce

aberrations in the image pulse, thereby degrade the quality of the ballistic images. The

investigation, however, indicated that the choice of imaging setup affects the image

aberrations that are induced by the Kerr effect. Two setups previously used for BI spray

studies were investigated, and it was shown that they responded differently to variations in the

OKE-gate setup.


— 73 —

Approach for volumetric spray measurements using Mueller calculus

H. Purwar*, S. Idlahcen, J.-B. Blaisot, C. Rozé UMR-6614 CORIA, CNRS, Université de Rouen Normandie, INSA de Rouen, 76800 Saint-Étienne-du-Rouvray, France

*Corresponding Author: [email protected]

KEY WORDS: Sprays, birefringence, Mueller matrices

Volumetric spray measurements are extremely important for the very basic understanding of

liquid fuel atomization and could help in improving the efficiency of automobile engines and

thereby reduce the emitted pollutants. Such measurements could also be useful to validate

various high-fidelity numerical methods for fuel spray simulations.

Our approach for volumetric spray measurements is based on the accurate measurement of

linear retardance of the birefringent liquid fuel (birefringence in fuel could be introduced by

mixing small quantities of other birefringent liquids, like liquid carbon disulfide). In general,

a significant amount of birefringence could be induced in certain liquids by using the high-

power laser pulses for a duration depending on the incident pump pulse’s duration and

relaxation time of the medium. This transient birefringence induced in the medium would

change the polarization of any light (linearly polarized probe) passing through it. The change

in the polarization properties of light passing through an active birefringent medium depends

on the optical path length of light in the medium and can be quantified accurately by

measuring its Mueller matrix (MM). We aim at exploring this approach to obtain volumetric

measurements for fuel sprays.

Following is the optical setup for measurement of MM for a birefringent liquid (or Kerr

medium) using the dual rotating-retarder approach1. On the right, an estimate of the linear

retardance (δ) obtained by decomposing the measured MM using a scheme proposed by Lu

and Chipman2, for 1 mm thick CS2 with different delays between pump and probe beams.

D = -1.0 ps D = -0.67 ps

D = -0.33 ps D = 0 ps

Left: Optical setup for Mueller matrix measurement for a birefringent liquid using dual rotating-retarder

approach. Right: Polar decomposition derived linear retardance for different relative time delays (D) between the

pump and probe beams in 1.0 mm thick CS2 cell.

Further details about the MM measurements, preliminary results for retardance measurement

in pure liquid carbon disulfide and how these results could help in obtaining volumetric

measurements for fuel sprays, will be discussed at the conference.

1 J. Soni, H. Purwar, H. Lakhotia, et al., Optics Express, 21 (2013) 15475. 2 S. Lu and R. A. Chipman, Journal of the Optical Society of America A 13 (1996) 1106.


— 75 —

N2 thermometry in hybrid fs/ps CARS: resonant and non-resonant

interferences influencing measurement accuracy

M. Nafa

1, M. Scherman

1, H. Danvy

1, A. Bresson

1, A. Godard

1, T. Schmid

1, B. Attal-Tretout

1, P. Joubert

2

1. ONERA, Chemin de la Hunière et des Joncherettes 91123 Palaiseau Cedex

2. Institut UTINAM - UMR CNRS 6213 UFR Sciences et Techniques, 16, Route de Gray 25030 BESANCON Cedex Corresponding Author e-mail address : [email protected]

KEY WORDS: CARS, Thermometry, Femtosecond lasers

Hybrid femto-picosecond CARS is a spectroscopic technique that can be used in gases

to retrieve point information of temperature. Indeed, accurate temperature information is

required in reactive and turbulent media encountered in combustion chambers or plasmas.

The technique was recently used to demonstrate high repetition rate1,2

(kHz) point, and 10 Hz

2D- temperature measurements in laboratory flames3.

An original laser architecture was built at ONERA using a single Yb:KGW laser to

produce the broadband exciting beams, so called Pump and Stokes pulses, and the

narrowband picosecond probe pulse. Spectroscopy could be performed with 0.7 cm-1

resolution, allowing to resolve N2 ro-vibrational lines. In that manner, simultaneous

information on both rotational and vibrational distributions is obtained, as previously done in

ns-CARS4. Spectra could be recorded at 1 kHz in ambient air, and integrated over 100 shots

in CH4/air flames5.

Temperature information is obtained by comparing spectral profiles to computed ones.

Various contributions to the signal have to be taken into account, such as non-resonant

background amplitude, coherent dephasing between ro-vibrational lines, and spectral

distribution of the coherences excitation. They can be monitored by playing with optical

pulses arrangement, polarization or synchronization. Thus non resonant background

contribution could be efficiently rejected and measurement range be increased. Other

parameters such as pulse to pulse laser amplitude, and spectrum fluctuations, were also

monitored, and confirmed the reliability of the laser source. The influence of these various

parameters on the experimental spectral profile and on the accuracy of the thermometry will

be discussed.

(a) (b) (c)

CARS experimental spectra in ambient air and in CH4/flame, obtained with : (a) ns-CARS, (b) fs/ps-

CARS (1.8 cm-1

), (c) fs/ps-CARS (0.7 cm-1

)

1. Miller et al. “Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman

scattering”, Optics Express 19, n°16 (2011) : 15627

2. Kearney et al. “Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering at flame temperatures using a second-harmonic bandwidth-compressed probe”, Optics Letters 38, n°6 (2010) : 833

3. Bohlin et al. “Two-dimensional gas-phase coherent anti-Stokes Raman spectroscopy (2d-cars): Simultaneous planar imaging and

multiplex spectroscopy in a single laser shot”, J. Chem. Phys. 138, 221101 (2013) 4. Messina et al. “Study of a Non-Equilibrium Pulsed Nanosecond Discharge at Atmospheric Pressure Using Coherent Anti-Stokes Raman

Scattering”, Proceedings of the Combustion Institute 31, n°1 (2007) : 825

5. Scherman et al. “Rovibrational Hybrid fs/ps-CARS Using a Volume Bragg Grating for N2 Thermometry”. Optics Letters 41 (2016): 488


— 77 —

List of Authors

——/ A /——Abdelmonem, Ahmed . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19Abela, R. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56Aldén, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .52Ameloot, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 58Attal-Tretout, B. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50, 78Aumanen, J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22Aybush, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36

——/ B /——Backus, E.H.G. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20Baldelli, Steven . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17Barviau, B. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 68Baumgartl, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Beck, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56Becker, K. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 64Becker, Hans-Christian . . . . . . . . . . . . . . . . . . . . . . . . . . . 59Bengtsson, P.-E. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .32, 42Bermejo, Dionisio . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11Berthiller, Frédéric . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 67Beyrau, F. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .66Blaisot, J.-B. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8, 76Bonn, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20Bood, J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32, 42Bornhauser, P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56Bové, H. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 58Brackmann, C. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32Brancati, N. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26Bresson, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50, 78Brückner, Lukas . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43Buckup, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 44

——/ D /——D’Arco, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .26Danvy, H. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50, 78De Wit, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24Di Lonardo, G. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12Donfack, P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54

——/ E /——Egorova, N. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 72Ehrlich, H.V. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14

——/ F /——Ferrara, M.A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26Frucci, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26Fusina, L. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12

——/ G /——Gerber, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56

Godard, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50, 78Godin, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Gord, J.R. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46Gostev, F. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36Grisch, F. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 68

——/ H /——Hideur, Amar . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7Hiltunen, V.-M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22Hosseinnia, Ali . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41Hosseinnia, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32Hot, Dina . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15Hot, D. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52Houard, J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .8Høgstedt, L. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .10

——/ I /——Idlahcen, Saïd . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75Idlahcen, S. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8, 76Indolfi, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26

——/ J /——Johansson, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22Joubert, P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50, 78

——/ K /——Kazemi, M.M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54Kearney, Sean . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 39Khan, T.Z. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54Khasanov, Kh. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34Kiefer, Johannes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 63Knopp, G. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56Koivistoinen, Juha . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21Kouzov, Alexander . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71Kudryavtseva, Anna . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13

——/ L /——Lecaplain, C. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Leisner, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20Li, Zhongshan . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3Li, Z.S. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52Limpert, J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Linne, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 74Lisichkin, G.V. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14Liu, K.-L. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24

——/ M /——Marrocco, Michele . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37Martínez, R.Z. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12Materny, Arnulf . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 53

Meißner, C. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 66Mohaghegh, F. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54Morozov, V.B. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .34Motzkus, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 44Myllyperkiö, P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22

——/ N /——Nadtochenko, V. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 36Nafa, Malik . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77Nafa, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50Nordström, Emil . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31Nordström, E. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42

——/ P /——Pedersen, Rasmus . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9Pedersen, R.L. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52Pettersson, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22Popp, Jürgen . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29Puwar, H. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

——/ R /——Radi, P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 72Radi, P.P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56Rae, Ali . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 69Rahm, Mattias . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73Richardson, D.R. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46Rimke, I. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 60Roeffaers, M.B.J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24, 58Roy, S. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46Rozé, C. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76Rozé, C. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

——/ S /——Sahlberg, Anna-Lena . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 51Scherman, Michael . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49

Scherman, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78Schmid, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .50, 78Schmidt, J.B. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46Schreiber, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Sedarsky, D. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 74Seeger, T. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 66Silaeva, E. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Sirleto, Luigi . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25Stauffer, Hans . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45Steuwe, Christian . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23, 57

——/ T /——Tang, M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Tcherneiga, N.V. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14Tehrani, A.M. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54Tidemand-Lichtenberg, P. . . . . . . . . . . . . . . . . . . . . . . . . . . 10Tröger, Johannes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 65Tunkin, V.G. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34Tünnermann, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

——/ V /——van Bokhoven, J.A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56Vella, A. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Vereshchagin, A.K. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34Vereshchagin, Konstantin . . . . . . . . . . . . . . . . . . . . . 33, 35Visser, Bradley . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 55

——/ W /——Wang, H. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8Wrzesinski, P.J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 46

——/ Z /——Zemskov, K.I. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14Zhilenko, M.P. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14Zhou, J. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52

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