High Purcell Factor Due To Coupling of a Single Emitter to aDielectric Slot WaveguidePavel Kolchin,† Nitipat Pholchai,†,‡ Maiken H. Mikkelsen,† Jinyong Oh,§ Sadao Ota,† M. Saif Islam,§

Xiaobo Yin,† and Xiang Zhang*,†,‡,∥

†NSF Nanoscale Science and Engineering Center (NSEC), University of California, 3112 Etcheverry Hall, Berkeley, California 94720,United States‡Applied Science and Technology Graduate Group, University of California, Berkeley, California 94720, United States§Department of Electrical and Computer EngineeringUniversity of California, 2064 Kemper Hall, Davis, California 95616, UnitedStates∥Materials Science Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States

*S Supporting Information

ABSTRACT: We demonstrate an all-dielectric quantum electrodynamicalnanowire-slab system with a single emitter that concentrates the extremelyintense light at the scale of 10 × 75 nm2. The quantum dot exhibits a recordhigh 31-fold spontaneous decay rate enhancement, its optical saturation andblinking are strongly suppressed, and 80% of emission couples into awaveguide mode.

KEYWORDS: Nanophotonics, quantum dot, field enhancement, emission coupling, all-dielectric waveguide,deep subwavelength light confinement, waveguide QED

Strong light-matter interactions at the single emitter-photonlevel are of fundamental importance for quantum

information science and constitute the basis of such importantapplications as quantum memories, switches and gates,1−8 long-range coupling of single emitters and novel entanglementschemes.9,10 While narrow microcavity resonances weretraditionally used for strong optical interactions,11,12 subwave-length plasmonic nanostructures have been recently introducedto improve emission directivity and coupling to tightly confinedelectromagnetic modes,13−16 enabling strong interaction regimein broadband cavity-free nanoscale one-dimensional environ-ment2−5 and therefore making it promising as a building blockfor quantum nanodevices. However, despite significantadvances demonstrated by merging plasmonics with quantumoptics,14−16 stronger interaction, high coupling efficiency, andemission rate enhancement have yet to be observed.We demonstrate here strong optical interactions and

emission coupling at single photon and single emitter levelusing an all-dielectric nanoscale waveguide that exibits a deepsubwavelength field confinement of λ2/50. The confinement iscreated by squeezing light in the low index gap region betweena high index dielectric nanowire and a slab, where the largediscontinuity in the refraction indices concentrates the electricfield in the nanometer scale gap region along the nanowire,

constituting a deeply confined one-dimensional waveguidemode. Alternative approaches using high-index contrastbetween dielectric interfaces to overcome the diffraction limithas recently been investigated19,20 and light concentration at100 nm scale was demonstrated in a slot waveguide.20−22

However, incorporating single quantum emitters into such awaveguide while squeezing the active region in order to achievestrong coupling regime remains a challenge.20

By placing a single CdSe/ZnS quantum dot (QD) at anoptimal position in the system with nanometer precision,enabled by atomic force microscope (AFM) manipulation, weobtain strong spontaneous decay rate enhancement of 31 andstrong emission coupling from a single QD into the deeplyconfined waveguide mode. We observe a high emissioncoupling efficiency of about 80%. Moreover, we observe thatsuch a strong coupling modifies the emission dynamics: the QDbecomes brighter, and its blinking behavior and opticalsaturation are strongly suppressed. The demonstrated all-dielectric nano-QED system not only achieves simultaneously

Received: October 1, 2014Revised: November 20, 2014Published: November 28, 2014

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strong field confinement, efficient emission channeling, andenhanced light-matter interactions, but also provides a compact,broad-band, low loss and readily scalable photonic platform forclassical and quantum information processing in a one-dimensional continuum.2−5

Figure 1a shows the schematic of the all-dielectric nano-QEDsystem that consists of the nanowire-slab waveguide and a

single QD strongly coupled to the waveguide mode. In theexperiment, the dielectric waveguide is formed by a high-indexSi nanowire (refractive index n1 = 3.7120 + 0.0085i, 260−280nm in diameter) on top of a 90 nm ZnS film (refractive indexn2 = 2.3). Colloidal CdSe/ZnS core−shell QDs (800 nm peakemission) are spin-coated on the sample to form a dispersemonolayer prior to nanowire transfer. The AFM is used forselection and positioning of the nanowires such that a QD isprecisely placed right underneath the nanowire. Given thephysical size of ∼8 nm of the QDs along with ZnS surfaceroughness of 6.6 nm (P−V), one creates a nanometer-sized airgap between the nanowires and ZnS film (inset of Figure 1a).Such a narrow nanoscale air gap region along the nanowiresupports a deeply confined one-dimensional guided mode.Because of large refactive index contrast the electric fieldnormal to the boundaries jumps up inside the air gap, resultingin high electric energy density concentration in the gap region.Alternatively such a confined mode can be viewed as a cross-coupling between the nanowire waveguide mode and slab

mode, resulting in capacitor-like in-phase polarization chargeoscillations at the gap boundaries. Because of its capacitor-likeelectric field distribution inside the gap region, the mode areascales generally as (refractive index)−4.19 Therefore, it is criticalto use high index materials in order to increase confinementand Purcell emission rate enhancement.24 The experimentalsetup consists of the fluorescence imaging and single photoncounting systems with an integrated AFM that allows precisioncontrol over the position of individual QDs and nanowires, amajor advantage over conventional lithographic approacheswith limited lateral resolution. The AFM is operated in tappingmode for topographic imaging while in contact mode forpositioning the nanowire on top of the desired QD. At roomtemperature, the QDs are excited by a 532 nm continuous wave(cw) laser and their fluorescent emission is imaged on a charge-coupled device (CCD) camera (Hamamatsu EM-CCD,C9100). When the QD is placed in the region of large fieldenhancement, its emission scatters directionally into thewaveguide mode and propagates along the waveguide beforeit scatters out at the ends, indicating the strong interactionbetween the confined mode and emitter. If necessary, thenanowire is repeatedly repositioned until spatially optimalcoupling is observed. A complete description of theexperimental setup and AFM manipulation procedures areavailable in the Supporting Information.Figure 1b shows the fluorescence image of a single QD that

is strongly coupled to the waveguide averaged over 200 sduration. The quantum dot (QD1) is placed underneath thenanowire and the bright glowing ends of the waveguide signifythe strong interaction. The intensity time traces from the twoends and from QD1 position reveals fluorescence blinking thatis characteristic to a colloidal QD, as shown in Figure 1c. Theblinking signal in these three traces are simultaneous (withcorrelation values higher than 0.9), indicating that the lightscattered out at the ends of the waveguide is coming from thesame coupled quantum dot (QD1). For comparison, anyisolated QD nearby blinks independently (correlation <0.1)from one another and from the coupled QD1.QD strong interaction with the deeply confined photonic

mode is evident as the emission from each nanowire end isabout twice as strong as that at QD1 position. The ratio of thefluorescence signals from the two nanowire ends to the sum ofall the three spots yields an apparent emission coupling factorof about 80%, which is in good agreement with theoreticalprediction of 80% for a Si nanowire on ZnS slab (see Figure3b). In the meantime, as shown in the final trace (shaded) inFigure 1c, the strong confinement significantly enhances thetotal photon flux and more than 4 times more photons arecollected from coupled QD1 than that of the uncoupledscenario. Moreover, the deep subwavelength confinement isstrong enough to achieve near unity emission couplingfactor23,25,26 despite the fact that the colloidal quantum dotsare two-dimensional isotropic emitters with random orientationof their crystalline axis.27

In order to verify that the emission originates from a singleQD emitter, we perform two-photon intensity autocorrelationmeasurements using a pair of single photon counting modules(SPCMs). Figure 2b shows normalized two-photon intensitycorrelation g(2)(τ) of QD2 for both coupled and uncoupledcases. When the emission of the QD is strongly coupled to thewaveguide mode, as shown in Figure 2b, the autocorrelationsshow identical narrow dips measured at the QD position (redcurve) and nanowire end (green curve). When uncoupled from

Figure 1. The deep subwavelength all-dielectric QED system with ananoscale gap. (a) The dielectric nano-QED system consists of thenanowire-slab waveguide and a single quantum emitter stronglycoupled to the waveguide mode. Light is confined in the gap regiondue to the high index contrast for optical modes with dominantelectric field components normal to the interfaces. (b) The averagedfluorescence image of a single QD coupled to a nanowire-slabwaveguide. The inset shows the AFM scan image of the nanowire. (c)Fluorescence time traces detected at the nanowire ends and at positionof the coupled QD1 on the same time axis. Simultaneous blinking oftwo nanowire ends and coupled QD1 indicates that light from thethree spots comes from the same coupled QD1. Time trace of thesame QD1 when uncoupled at a different location away from wire isincluded (shaded) for comparison.

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the nanowire, a much wider dip is measured from the same QD(blue curve). In all three cases g(2)(0) < 0.5 verifies that theemission is indeed from a single QD and its single photon statepurity is excellently preserved after coupling. Slightly highervalue of g(2)(0) for the coupled case is due to spuriousuncorrelated fluorescence from the nanowire, finite histogramtime-bin size, and dark background photon count rate.Both lifetime measurements with pulsed excitation and

intensity autocorrelation measurement under cw excitationreveal a striking difference in the recombination lifetimes of thecoupled and uncoupled QD. Because the emission lifetimevaries among different QDs, measurements on the same QDbefore and after coupling provides unambiguous determinationof the Purcell enhancement factor. The pulsed excitationmeasurements reveal a multiexponential decay curve, character-istic of colloidal QDs (Figure 2a) with a longer time constantcorresponding to the radiative recombination lifetime of thebright state.29 The inset shows the fluorescence image of thestrongly coupled QD. A long lifetime of 120−180 ns is typicallyobserved for uncoupled CdSe/ZnS QDs.30 Extracted fromFigure 2a, the recombination lifetimes are 5.4 ± 0.1 ns for thecoupled and 170 ± 2 ns for the uncoupled QD, resulting in astrong Purcell enhancement factor of 31 due to the strong field

confinement in the deeply confined photonic mode, muchgreater than observed in plasmonic waveguides and nano-particles.14−18,28 This enhancement factor agrees well with thetheoretical prediction for a gap of 9 ± 1 nm and corresponds toa field confinement of at least λ2/50. Meanwhile, the width ofthe antibunching dip in intensity autocorrelations (Figure 2b) isdetermined by the overall emission rates, the sum of theintrinsic decay rate (k21) and the excitation rate (k12), the latterof which is proportional to the pump power. As shown inFigure 2c, extrapolation of the measured emission rates to zeropump power yields the intrinsic lifetimes of 5.2 ± 0.4 and 160± 22 ns for the coupled and uncoupled cases, which is in goodagreement with the lifetime values directly measured underpulsed excitation.Importantly, we observe that strong Purcell enhancement

tremendously reduces the saturation of the QD bright stateemission that is favorable for implementation of high brightnesssingle photon sources. Figure 2d shows peak intensitysaturation curves for coupled and uncoupled QD2. Theintensity saturation occurs under typical excitation conditionsfor uncoupled QDs when the excitation rate is higher than thespontaneous emission rate k12 > k21. However, when QD iscoupled to the nanowire the radiative decay rate is significantlyenhanced. As a result, the intensity curve shows almost lineardependence on the pump power, indicating the absence ofsaturation (k12 ≪ k21). The intensity saturation can be alsoindependently determined from the autocorrelation measure-ments: the relative slope steepness of the rate (k12 + k21) curve[Figure 2c] indicates the degree of the intensity saturation. Flatcurve for the coupled QD indicates that the saturation istremendously suppressed. For example, under the sameexcitation power of 0.45 mW, k12/k21 = 0.1 and 1.7 for thecoupled and uncoupled QD2, respectively. This indicates thatfor the coupled QD the saturation point (k12 = k21) should bereached at the pump power of 4.5 mW, 17 times higher thanthat of the uncoupled QD (0.27 mW). During the period ofbright state manifold, the peak photon emission rate (R) of thequantum dot is described by the simple emission model underincoherent pumping R = χk12 k21/(k12+ k21).

33−35 The factor χcan be expressed using the emission outcoupling efficiency (γ)into the single mode fiber and the emission quenching factor(kr/k21) as χ = γkr/k21. Here kr is the radiative decay rate fromthe upper state. By fitting peak intensity saturation curves tothis emission model with χ as the only free scaling parameter,we obtain that the saturated peak photon count rate should be12 times higher for the coupled QD as compared to that of theuncoupled QD. The difference in the saturation photon countfactor of 12 and decay enhancement factor of 31 is due todifferent photon out-coupling efficiencies from QD to micro-scope objective for coupled (27%) and uncoupled QD (63%)and emission quenching factor of 0.9 for the coupled QD,explained below (see also Supporting Information).Unambiguous measurements of Purcell effect performed on

the same QDs before and after interacting with the deeplyconfined photonic mode quantitatively confirm the dramaticoptical confinement in this waveguide QED system. Theoreticalcalculation in Figure 3a,b shows how the electric field of thedeeply confined photonic modes for 150 and 270 nmdiameters, particularly the normal component to the slab, ishighly concentrated in the gap region. For 270 nm diameter, alateral confinement is 75 nm (fwhm), corresponding to aneffective mode area of λ2/50 at 10 nm gap. As the diameterincreases, the second deeply confined photonic mode replaces

Figure 2. Purcell emission enhancement of a single QD stronglyinteracting with the deeply confined photonic mode. (a) Directlifetime measurements of another QD-nanowire system (inset) underpulsed laser excitation shows drastic 31-fold difference from the sameQD2 decoupled from the nanowire. (b) Two photon intensityautocorrelation measurements (at pump power 0.45 mW) showantibunching dips confirming single photon emission from theindividual quantum emitter. A clear difference in the dip width isobserved between the coupled and uncoupled QD, showing a stronglyreduced recombination lifetime of the coupled QD. (c) A plot ofphoton circulation rate is linearly dependent on the pump power.Extrapolation to zero pump value yields the intrinsic lifetime of about5.2 ± 0.4 ns and 160 ± 22 ns, respectively for the coupled anduncoupled cases, which is in good agreement with the lifetime directlymeasured under pulsed excitation. (d) Measured total fluorescencepeak intensities versus pump power for coupled and uncoupled QD.Dashed lines are fitted to a saturation model. Within the illuminationrange of the experiment, coupled QD emission remains linear andunsaturated, whereas uncoupled QD clearly saturates at higher pumppower.

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the first one. These modes have different field topology. At 150and 270 nm, the modes are HE11 and HE21 circular dielectricwaveguide modes,36 respectively, altered in the proximity of thehigh index slab. The simulations are performed under theexperimental conditions. The theoretical Purcell factor FP andcorresponding coupling factor β for a Si nanowire with 270 nmdiameter are shown in Figure 3c with respect to gap size, wherean optimally placed linear vertical dipole at the center of thegap region is assumed in the calculation. A tiny gap (below 40nm) is crucial for observing the emission enhancement effect.Simulation of Purcell effect with varying diameter (Figure 3d)at a fixed gap = 10 nm shows modal structure of the deeplyconfined photonic modes and confirms that interaction withthe second order mode is dominant in our experimentalconfiguration. In particular, because the dipole moment of acolloidal QD is randomly oriented in the plane perpendicular toits crystalline c-axis27 we expect to observe experimentally aPurcell enhancement of at most FP/2 under an optimalcondition where the QD c-axis is horizontal. The measuredPurcell factor of 31 for QD2 therefore corresponds to atheoretical value of 62 or higher at the gap of 9 ± 1 nmconsistent with actual geometry of the structure. We alsoestimate an apparent emission coupling efficiency as 72% forQD2.More accurate coupling factor estimation takes into account

the propagation losses, emission quenching in the nanowire,difference in collection efficiencies at the waveguide ends and atQD position due to different radiation patterns. The objectivecollection efficiencies, computed from the simulated radiationpatterns are 31% for the nanowire end and 40% for the QD outof total out-coupled radiation over full solid angle. Thepropagation length is estimated as 5.8 ± 2.2 um. Thenonradiative rate contribution corresponding to the emissionquenching due to ohmic loss in the nanowire is estimated as

10% from fitting intensity saturation curves to the emissionmodel with incoherent pumping (see Supporting Information).With these numbers, the coupling efficiency for QD1 and QD2of Figures 1-2 become 78% and 71% respectively. Thesenumbers are consistent with 80% value from theory and arehardly affected by 2D orientation averaging due to dominantemission enhancement for y dipole component and outperformthose for previously reported plasmonic waveguides withcoupled single QDs.14−16 We also note that our waveguideconfiguration should allow for higher field confinement ifhigher index materials are used both for the nanowire and slab.For example, for a more ideal Si or transparent GaP nanowireand Si or GaP slab material system and further reduction of gapsize to 5 nm the confinement is predicted to be as high as λ2/300, corresponding to 91% coupling efficiency (see SupportingInformation).The demonstrated waveguide also substantially improves the

QD emission dynamics. Strongly suppressed blinking behaviorand enhanced brightness of the QD is observed when coupledto the waveguide. Figure 4 shows fluorescence time traces of

the QD measured at SPCMs with 100 ms resolution.Fluorescence blinking is associated with carrier trapping atsurface defects of the QD shell.31,32 When coupled, the QD isin the bright state 90% of the time, whereas only 63% whenuncoupled. The strongly confined waveguide mode acceleratesthe radiative decay that then competes effectively against thenonradiative transition into the dark state, thereby suppressingthe blinking.32 This blinking suppression, along with thereduction of intensity saturation, results in an increase in totalfluorescence.In conclusion, we demonstrated an all-dielectric waveguide

QED system with light concentration at the tens of nanometerscale resulting from a high index contrast dielectrics. Thestrongly enhanced interaction between the single emitter anddeeply confined photonic mode and its effect on the emissiondynamics has been observed experimentally with a record highPurcell enhancement factor of 31 in nonresonant photonicsystems that is broadband in nature. Such a strong interactionresults in strong suppression of QD blinking and opticalsaturation. The small footprint and broad-band nature of thissimple but efficient dielectric system suggests a broader use for

Figure 3. Simulation of Purcell effect. (a,b) The simulated |E|-fielddistribution of the two deeply confined photonic modes shows stronglight confinement in the gap region between the nanowire and slab.Arrows indicate E-field vectors. The slab thickness is optimized to 90nm for strongest field confinement. (c) Theoretical total Purcellemission enhancement factor (FP) and emission coupling factor (β)versus gap size at 270 nm diameter. The curves show strongdependence on the gap size, indicating a tiny gap is crucial forobserving the emission enhancement effect. (d) Modal Purcell factor(FM) at varying nanowire diameter for a fixed 10 nm gap, together withits corresponding coupling factor, reveals the modal structure.

Figure 4. Observation of blinking suppression of the QD coupled tothe deeply confined photonic mode. Fluorescence time traces of theQD (left panel) measured at the single photon counters with 100 msresolution with their corresponding histograms of count rate (rightpanel). The blinking behavior of coupled QD1 (bottom panel) isstrongly suppressed compared to the same QD1 when uncoupled (toppanel). The QD is in the bright state 90% of the time when coupledwhereas only 63% of the time when uncoupled. This is manifested in asharp increase in the fraction of bright state emission to the dark stateemission in the bottom histogram.

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efficient on-chip optical components and networks both atclassical and quantum level.

■ ASSOCIATED CONTENT*S Supporting InformationExperimental setup, procedure of optical coupling via AFMmanipulation, characterization of a single emitter using intensityauto-correlation, intensity saturation suppression of thequantum dot coupled to the nanowire, effect of strong emissionenhancement on the photon flux, estimation of out-couplingefficiencies, measurement of propagation length of thewaveguide, estimation of emission quenching, Estimation ofemission coupling factor β, deeply confined photonic modes ofthe nanowire-slab waveguide, multiemitter interaction regime inthe deeply confined photonic waveguide, all localized modes ofthe nanowire-slab waveguide, effect of waveguide slab thicknesson the emission enhancement and confinement, effect of thenanowire background fluorescence on QD intensity saturation,sample preparation method, additional figures, table, andreferences. This material is available free of charge via theInternet at http://pubs.acs.org.

■ AUTHOR INFORMATIONCorresponding Author*E-mail: xiang@berkeley.edu.Author ContributionsP.K., N.P., and M.H.M. contributed equally to this work.NotesThe authors declare no competing financial interest.

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