rixs-hxes @ xfels - international centre for theoretical
TRANSCRIPT
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RIXS-hXES @ XFELsMARTINA DELL’ANGELA
CNR-IOM, TRIESTE
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. RIXS @FLASH: Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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I. Exp. Techniques
hXES
RIXS Photon-in/Photon-out
Core level spectroscopies
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X-ray absorption spectroscopy (XAS)
A photon is absorbed and a core electronis excited to an unoccupied state
XAS is element-specificCore level
Valence states
Empty states
Fermi level
hv
𝑃𝑖→𝑓 ∝ < 𝑓 𝐻′|𝑖 > |2𝜚𝑓
𝐻′ = 𝒑 ∙ 𝒆exp(𝑖𝒌𝒓) 𝑑𝑖𝑝𝑜𝑙𝑒 𝑎𝑝𝑝𝑟𝑜𝑥𝑖𝑚𝑎𝑡𝑖𝑜𝑛
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Decay of core holes
Core level
Valence states
Empty states
Fermi level
Auger Electron Emission
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X-ray emission spectroscopy (XES)
Core level
Valence states
Empty states
Fermi level
hv
P. Glatzel, bergmann U., Coord. Chem. Rev. 249 (2005) 65
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Resonant Inelastic X-ray Scattering (RIXS)
Inelastic scattering cross section (Kramers-Heisenberg formula):
𝐹 𝜔,𝜔𝑖 = σ𝑓 σ𝑚<𝑓 𝐷 𝑚><𝑚 𝐷 𝑔>
𝐸𝑔+ℏ𝜔 −𝐸𝑚−𝑖Γ𝑚
2
𝛿(𝐸𝑔 + ℏ𝜔 − 𝐸𝑓 − ℏ𝜔′)
i. Site selectivityii. Simmetry selectivityiii. Probe low energy excitationsiv. Sub-natural width spectrav. Ultrafast dynamicsvi. Bulk and buried structuresvii. Band dispersion
J. Nordgren et al., in Handbook of Solid State Spectroscopy, Springer 2006, Ed. W.R. Wij
Core level
Valence states
Empty states
Fermi level
hv
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Low energy excitations in materials
L.J.P. Ament, et al., Rev. Mod. Phys., 83, No.2 (2011)
Ground state
Core states
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. RIXS@ FLASH: Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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Requirements
1. Photon Detection System (energy resolution)
2. Tunable and brilliant photon source (VUV and X-ray)
Monochromatic synchrotron beamlines
Photon hungry
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X-ray Spectrometers ...history
Nordgren, J., Bray, G., Cramm, S., Nyholm, R., Rubensson, J.-
E. & Wassdahl, N. (1989). Rev. Sci. Instrum. 60, 1690–1696.
VG Scienta, XES 350 Grace
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https://www.bnl.gov/ps/userguide/lectures/Lecture-8-Jarrige.pdf
I. Jarrige, BNL
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RIXS resolution
A. Fohlisch, XFEL hRIXS
L3 Cu Edge
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Examples of X-ray spectrometers
Rowland geometry (Monochromatic; spherical mirror)
von Hamos (Dispersive)
M. Czarnota et al., Phys. Rev. A 88, 052505 (2013)
Hettrick-Underwood(qRIXS, MERLIN(ALS))
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Lab based RIXS/XES ....future developments
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RIXS projects @FELs ...(soft X-rays)XFEL Heisenberg RIXS (A. Fohlisch)
Yi de Chuang et al. Review of
Scientific Instruments 88, 013110
(2017); https://doi.org/10.1063/1.4974356
LCLS qRIXS
PAL-XFEL, ....https://www.xfel.eu/sites/sites_custom/site_xfel/content/e51499/e60513/e63567/e63600/9_XFUM2017-SASE3_Satellite_Neppl_hRIXS_eng.pdf
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. RIXS@FLASH: Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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Tr-XES on Silicon
M. Beye et al., PNAS 107, 16772 (2010)
Liquid-liquid transition in silicon
Transient ‘’low density ‘’state accessibleat short timescales
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. RIXS@FLASH: Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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II. RIXS@LCLS: Femtochemistry
LCLS (Stanford)
https://lcls.slac.stanford.edu/overview
SXR Instrument
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X-ray Spectrometer
Surface Science Endstation(prof. A. Nilsson)
https://lcls.slac.stanford.edu/instruments/sxr/specifications
T. Katayama, et al. J. Elect. Spec. Rel Phen 187 (2013) 9
Spectrometer (Rowland type):
Elliptical grating (Ni coated)
Negative Diffraction Order
No entrance slit
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FemtochemistryP
ote
nti
al
E
ne
rgy A + B
Surface
AB
AB
Without Catalyst
With Catalyst
Reaction coordinate
Challenge: Understand reaction mechanism
and dynamics
Case study:
H.-J.Freund, G. Meijer, M. Scheffler, R. Schlogl, M. Wolf, Angew. Chem. Int. Ed. 2011, 50, 10064 – 1009 (and ref therein)
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CO RIXS @synchrotron
A. Nilsson et al., Chem Phys Lett, 675 (2017) 145 A. Föhlisch et al., J. Chem Phys, 121 (2004) 4848
Ruthenium
Carbon
Oxygen
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Tr-RIXS in catalysisM. Bonn et al, Science 285, 1042 (1999)
Create HOT ELECTRONS that trigger reactions
THERMAL vs ULTRAFAST laser induced heating
LCLS set up
60 Hz
533eV
(100 l/mm grating)
100fs
12 J/m2
50x1800 μm2
Scienta R3000
Electron
Spectrometer
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FE
L B
an
dw
idth
M. Dell’Angela, et al. Science 339, 1302 (2013)
CO/Ru(0001)
RIXS MAP
A. Fohlisch et al., J. Chem Phys 121 (2004) 4848
FEL vs Synchrotron ‘’static’’ data
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Co desoprtion from Ru(0001)
M. Dell’Angela, et al. Science 339, 1302 (2013)
Bond Weakening towards gas phase
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FIT = Chemisorbed + Gas Phase Resonant
P. Skytt et al, PRA 55 (1997) 134
Spectator shifts
due to 2π*
70% Unpumped + 30 % “Gas phase”
Spectator shifts: 1π 0.1eV less
4σ 0.3eV less
Participator: -0.5eV and x0.5
Are the molecules in the gas phase?
Literature Our data
Not really! …PRECURSOR?
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Free-energy curve
DFT+BEEF-vdW Wellendorff L. et al PRB 85, 235149 (2012)
TWO MINIMA!
Chemisorbed
Precursor
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Conclusion II
We have been able to measure for the first time molecules in the precursor state upon desorption.
Review of FEL femtochemistry experiments:
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Ultrafast Surface Chemistry and Catalysis Collaboration
Toyli Anniyev (1)
Martin Beye (1,4)
Ryan Coffee (1)
Martina Dell'Angela (2)
Alexander Foehlisch (4)
Jorgen Gladh (3)
Florian Hieke (2)
Markus Hantschmann (5)
Tetsuo Katayama (1)
Sarp Kaya (1)
Oleg Krupin (1)
Jerry LaRue (1)
Giuseppe Mercurio (2)
Ankush Mitra (1)
Stefan Moeller (1)
Andreas Moegelhoej (1)
Anders R. Nilsson (1)
May Ling Ng (1)
Dennis Nordlund (1)
(1) SLAC National Accelerator Laboratory, USA;
(2) Institut für Experimentalphysik, Universität Hamburg
and Center for Free Electron Laser, Hamburg, Germany;
(3) Department of Physics, Stockholm University,
Sweden;
(4) Methods and Instrumentation in Synchrotron
Radiation, Helmholtz-Zentrum Berlin, Berlin, Germany;
(5) Department of Physical Chemistry, Fritz-Haber-Institut,
Berlin, Germany.
(6) Surface Science Research Centre, Department of
Chemistry, University of Liverpool, United Kingdom
Jens Norskov (1)
Henrik Oberg (3)
Hirohito Ogasawara (1)
Henrik Ostrom (3)
Frank Abild-Pedersen (1)
Lars Pettersson (3)
Mats Persson (6)
William F. Schlotter(1)
Jonas A. Sellberg (1)
Florian Sorgenfrei (2)
Joshua J. Turner (1)
Hongliang Xin (1)
Martin Wolf (5)
Wilfried Wurth (2)
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. RIXS@FLASH: Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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III. RIXS@LCLS: Liquids (next lecture by Ph. Wernet)
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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Tr-RIXS on Sr2IO4
Strongly correlated system
hv = 11.22 keV (L3 Ir)
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Tr-RIXS on Sr2IO4
magnetic
orbital
Magnons or spin waves
Bragg peak
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Outline
I. Techniques1. X-ray absorption (XAS)
2. X-ray emission (XES) /High resolution X-ray Emission (hXES)
3. Resonant Inelastic X-ray Scattering (RIXS)
II. Instruments
III. Selected RIXS-hXES applications @ XFELsI. RIXS@FLASH: Phase Transitions
II. RIXS@LCLS: Femtochemistry
III. RIXS@LCLS: Liquids
IV. RIXS@SACLA: Magnetism
V. RIXS@FERMI: dd excitations
RIXS-hXES@ XFELs
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V. RIXS@FERMI: dd excitations
FERMI (Elettra Sincrotrone Trieste)
FERMI = M 2,3 Edges of Cu, Ni, Co
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M-edge vs L-edge50 eV -100 eV 500 eV -1 keV
100 eV/10 meV = 10^4 1 keV/ 10 meV = 10^5
Energy
Resolving Power
Small machineLarger throughput
butStrong elastic peak
More branching
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Nordgren Spectrometer @ SLS
MERIXS/MERLIN @ ALS (Worlwide Record)
Z. Hussain, CORPES 07
Y.D. Chuang, Synchrotron Radiation News, 25 (4), 22 (2012)
M-edge RIXS
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Set-up for RIXS @FERMI
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First experiment: KCoF3MERIXS Beamline @ALS
-Perovskite
-114K Neel Temperature (small thetragonal distortion)
A. Caretta et al., PRB 96, 184420 (2017)
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KCoF3 M-edge RIXS
The onset of magnetic
ordering, which quenches the
spin-flip excitation channel,
affects the overall energy of dd
excitations.
A. Caretta et al., PRB 96, 184420 (2017)
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High resolution RIXS at FERMI: KCoF3
NEXAFS is feasible
RIXS is also feasible
M. Dell’Angela et al., Scientific Reports 6, 38796 (2016)
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High resolution RIXS at FERMI: KCoF3
M. Dell’Angela et al., Scientific Reports 6, 38796 (2016)
Resolution is not limited by FERMI
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NiO: FEL vs SynchrotronCollaboration with
G. GhiringhelliA. ScherzJ. Schlappa
S. G. Chiuzbaian et al. PRL 95, 197402 (2005)
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Time resolved reflectivity of CuGeO3Giannetti et al. PRB 80 (2009) 235129
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High resolution RIXS on CuGeO3
MERIXS Beamline @ALS
Unpublished data
D4h
x2-y2
xy
xz,yz
z2
1.56 eV
1.73 eV
10Dq=1.56; Ds=0.306; Dt=0.145
1.95 eV
CTM4XAS, CTM4RIXS (only crystal field, no CT)
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High resolution RIXS on CuGeO3
xyx2-y2
xz,yzz2
x2-y2
xyxz,yzz2
De Graaf, Broer PRB 62 (2000) 705
Giannetti et al. PRB 80 (2009) 235129
x2-y2
xyz2
xz,yz
Unpublished data
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Pump Probe M-edge RIXS of CuGeO3
We observe dynamics in dd transitions !
Unpublished data
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Conclusions IV
We measured high resolution M-edge RIXS spectra at FERMI
We measured a femtosecond dynamics in the dd-trasitions in a pump-probe RIXS experiment
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RIXS@TIMEX:
Wilfried Wurth (CFEL/DESY)
Florian Hieke
Sasa Bait
Fulvio Parmigiani
Marco Malvestuto
Antonio Caretta
Luca Sturari
Measurements @ ALS:
Yi De Chuang
Lewis A. Wray (NYU)
NiO measurements
Giacomo Ghiringhelli (PoliMi)
Andreas Scherz (XFEL)
Justine Schlappa
TIMEX staff:
Emiliano Principi
Riccardo Mincigrucci
Laura Foglia
Alberto Simoncig
Acknowlegments RIXS@FERMI