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K.G.Lagoudakis*,K.A.Fischer,T.Sarmiento,P.L.McMahon,M.Radulaski,J.L.Zhang,

Y.Kelaita,C.Dory,K.Mller&J.Vukovi

E. L. Ginzton Laboratory, Stanford University, Stanford, California 94305, United States

Althoughindividualspinsinquantumdotshavebeenstudiedextensivelyasqubits,theirinvestigationunderstrongresonant

drivingin thescopeofaccessingMollowphysicsisstillanopenquestion.Here,wehavegrown highqualitypositively

chargedquantumdotsembeddedinaplanarmicrocavitythatenableenhancedlight-matterinteractions.UnderastrongmagneticfieldintheVoigtconfiguration,individualpositivelychargedquantumdotsprovideadouble-lambdalevelstructure.

Using a combination of above-band and resonant excitation, we observe the formation of Mollow triplets on all optical

transitions.WefindthatwhenthestrongresonantdrivepowerisusedtotunetheMollowtripletlinesthrougheachother,we

observeanticrossings.Wealsodemonstratethattheinteractionthatgivesrisetotheanticrossingscanbecontrolledinstrength

bytuningthepolarizationoftheresonantlaserdrive.Quantum-opticalmodelingofoursystemfullycapturestheexperimentally observed spectra and provides insight on the complicated level structure that results from the strong driving of the

double-lambdasystem.

systemshasbeenthesubjectofintenseinvestigationsoverthe

past40yearsforbothitsfascinatingphysicsandthepotential

for a variety of applications. Strongly-driven two-level

systems are known to exhibit a fluorescence spectrum that

comprisesatriplet as wasfirstpredictedbyMollow[1]and

demonstrated in a variety of physical systems ranging from

atoms[2]andmolecules[3]tosuperconductingqubits[4]and

hybridnanomechanicalsystems[5].

Another prominent system for the study of strong lightmatter interactions in the solid state is the platform of

semiconductor quantum dots (QDs). The atom-like behavior

of quantum dots along with the simultaneous existence of

excitonicandbiexcitonicstates,givethemaveryinteresting

cascaded-Vlevelstructurethathasbeenstudiedextensively

understrongresonantdriving[6]-[20].

ChargedQDshaveaspectralstructureverysimilartothat

of neutral QDs, but applying a strong magnetic field in the

Voigt configuration (magnetic field perpendicular to growth

axisofQD)Zeemansplitsthegroundandexcitedstates,lifting

thedegeneracyandresultinginadouble-levelstructure.

InthisLetter,wedemonstratetheobservationofMollow

tripletswithtunableanticrossingsinadouble-system,which

originatesfromtheresonantdrivingofanindividualholespin

trappedinanInAsquantumdotunderastrongmagneticfield

intheVoigtconfiguration.

Stronginteractionoftheresonantlaserwiththequantum

dotisenabledbyembeddingtheQDsinaplanarmicrocavity.

The microcavity was grown with Molecular Beam Epitaxy

(MBE) and consists of a 25-pair AlAs/GaAs bottom

DistributedBraggReflector(DBR),a1-GaAscavityand5-

pairAlAs/GaAstopDBR.ChargingoftheQDsisensuredby

aberyllium(p-type)-dopinglayer,located10nmbelowthe

QDs.TheQDlayerispositionedatthecenterofthecavity,on

anantinodeoftheelectricfieldtoenhancetheinteractionof

theQDswiththeresonantlaserlight.Theresultingstructure

has an experimentally-estimated quality factor of Q~65 and

showsstrongdirectionalemissionfromtheasymmetriccavity.

ThesamplestructureisshownintheinsetofFig.1(b).

Thequantumdotunderinvestigationisspectrallylocated

closetothepeakofthecavityreflectionspectra,at917.190nm

(1.351782 eV) and features a 9.81.7 eV linewidth under

above-bandexcitationat780nm.Thephotoluminescence(PL)

spectra have a linear power dependence as shown by the

detectedphotoncountsusingasinglephotoncountingmodule

(SPCM)inFig.1(a).Time-resolvedPLmeasurementsunder

weak, pulsed wetting-layer excitation at ~850 nm show a

radiative lifetime of 5972 ps yielding a Fourier-limited

linewidthof6.93eV,which isingood agreement withthe

observed PL linewidths. Applying a magnetic field in the

Voigt configuration Zeeman splits the ground and excited

statesofthepositivelychargedQDintoaquadrupletasshown

inFig.1(c).ForthisQDwefindgh=0.356andge=0.416,which

aretypicalvaluesforthissample[21],whilethediamagnetic

shift factor was fitted to 3.450.02 eV/T. We further

investigatethisquadrupletwithapolarizationanalysisofthe

PL spectra at maximum magnetic field (Bmax=5 T), which

exhibits crossed polarizations between the inner and outer

transitionsasshowninFig.1(d).Theresultinglevelstructure

isthereforeadouble-system,asshownintheinsetofFig.

1(c). The wavy downward arrows depict the allowed

transitions and their polarizations (blue-vertical and red-

FIG.1(a)Above-bandexcitationpowerdependenceoftheemission

fromtheinvestigatedquantumdot.Saturationoccurs at1.250.05

W driving power. (b) Time resolved QD emissionunder wetting

layerexcitationgivingalifetimeof5972ps.Theinsetdepictsthe

samplesstructure.(c)Zeemansplittingofthechargedquantumdot.

TheinsetshowsthefourlevelstructureofthepositivelychargedQD

underahighmagneticfieldintheVoigtconfiguration,alongwith

theallowedtransitionsandthedrivingschemesinvestigatedinthis

work.(d)PolarizationanalysisofPLspectrumat5Tmagneticfield.

excitationschemesthat willbe discussedlater. Inparticular,

theyellow(violet)arrowcorrespondstoresonantexcitationof

theouterhighest(lowest)energytransitions(at112eVin

Fig. 1(d)) whereas the two light-blue arrows depict the

excitationschemewherebythelaserissetin-betweenthetwo

innertransitions(at0eVinFig.1(d)).

Inordertostudythefour-levelsystemunderstrongresonantexcitation,wepumpitwithacombinationoftwolasers:

anabove-bandlaseratsaturationandavariablepowerresonantlaserthatweinitiallytunein-betweenthetwoinnertransitions(lightbluearrowsininsetofFig.1(c)and0eVinFig.

1(d)).Thisexcitationschemesharessimilaritieswithasinglelaser pumping and repumping scheme [22], yet here the

repumping effect is almost negligible because of the abovebandexcitationatsaturation.Theabove-bandlaserhasadual

role:firstitenablesPLmeasurements,andsecond,itisusedto

stabilizethechargesintheQD.Whenthesystemisdrivenusingonlyresonantexcitation,thereiscompletesuppressionof

thepositivelychargedexcitonstates.Theadditionofnon-resonant light charges the QD and therefore enables resonant

drivingoftheQD[23],[24].Here,weusethisfeaturetoour

advantagefortheacquisitionofdifferentialspectra thatprovide additional suppression of the unwanted resonant laser

light[21],beyond thesuppression wegetthroughthecrosspolarizeddetectionscheme.Fig.2showstheexperimentally

observedspectraasafunctionoftheresonantdrivingpower

forfourdifferentexcitationpolarizationangles.Inparticular,

Fig. 2 corresponds to (a) 94 (4), (b) 100 (10) , (c) 110

(20) and (d) 120 (30) excitation (detection) angles. Note

thattheseanglesarequotedwithrespecttotheQDmainpolarizations,asshowninFig.1(d).Asthedetectionisalways

cross-polarized to the excitation polarization, for the lowest

detectionangles,thetwoinnertransitionsandtheirsidebands

arebarelyvisible,whileforlargeranglestheyareeasiertoperceive.

Themost-strikingelementinallfourpowerdependences

ofFig.2isthatforincreasingpowerstheoutertransitionssplit

intotripletstheMollowtripletsandshowlineardependence

ofthespectralsplittingasafunctionoftheexcitationdriving

fieldupto610-3W.IncontrasttoMollowtripletsgenerated

bystandardtwo-levelsystems,theobservedtripletsgenerated

bythefour-levelsystemarecenteredondifferentenergiesthan

thelaserphotons.Beyondthelow-powerregime,theMollow

triplet splitting becomes comparable to the Zeeman splitting

andanevenmorestrikingphenomenonbecomesapparent:the

Mollow sidebands of the inner transitions spectrally overlap

withtheoutertransitions oftheQDand instead ofcrossing,

they show a clear anticrossing. The interaction strength betweentheunsplitoutertransitionsandtheMollowsidebands

oftheinnertransitionscanbetunedbychangingthepolarizationoftheexcitationlaserasshowninFigs.2(b)-(d).

Inordertounderstandthissurprisingbehavior,wehaveto

takeintoaccounttheeffectofthestrongresonantlaseronthe

levelstructureofthechargedQDintheVoigtmagneticfield.

Inthelaboratoryframe,thestrongresonantdrivingleadstothe

dressingofboththetwogroundandtwoexcitedstatescreating

an8-levelsystemwherealltransitionsareallowed.Alessintuitiveyetmoreappropriatewayofdescribingsuchastrongly

drivensystemisintherotatingframe,wherethesystemisstill

described as a four-level structure and its time independent

Hamiltonianreads

de 2

0

cos i sin

0

de 2

i sin cos

H

(1)

cos i sin d h 2

0

d h 2

i sin cos

inthe , , , basiswhere de and dh aretheexcitedandgroundstateZeemansplittings, isthedrivingfield

strengthand isthelaserpolarizationwithrespecttotheQD

mainpolarizationaxis. o L with o theunsplitexciton energy for zero magnetic field, and L the laser frequency.

TheeigenvaluesofthisHamiltonianprovideasetofquasienergies of the system, whose difference reproduces the observedPLenergiesalongwiththeanticrossingbehavior.The

reddottedlinesontopoftheexperimentaldatainFig.2(a)-(d)

bandsoftheinnertransitionsspectrallyoverlapwiththeMollowsidebandsoftheoutertransitionsshowingaclearcrossing

forallexcitationangles.

Inordertofullycapturetheobservedphenomenologywe

use quantum optical modelling, here implemented using the

quantumtoolboxinPython(QuTiP)[25].Wesolvethequantum-opticalmasterequationofthedensitymatrix

d

i

H ,

dt

cn

(2)

superoperatorofthecollapseoperator cn .

Here, cn

13 , 14 , 23 , 24 isthe sponta-

neousemission,whiletheabove-bandincoherentpumpingis

represented by cn

Pab 13

, Pab 14

, Pab 23

, Pab 24

eV),and Pab 5 theabove-banddrivingpowerextracted

fromfitting.

Similar to polarizing the in-coupling by adjusting the

Hamiltonian, the cross-polarized out-coupling is represented

withoperator Xpol cos 13 14 sin 23 24

thatisaweightedlinearcombinationofallfourofthedoublesystemsdipole operators.Thespectra arethencalculated

withthisnewoperatorastheinputtothestandardcorrelator

1

S

t Xpol ei d available in

2 Xpol

QuTiP.Themodelfullycapturestheobservedphenomenology

asshowninFig.2(e)-(h).

Additionally,wenoteaninterestingfeatureoftheMollow

spectraatlowpowerthatwebelieveisusefulasageneraltechniqueforchargedQDspectroscopy.Forapositively-charged

QD, when the outer Mollow sidebands are brighter than the

innersidebands,e.g.around0.5W,thenge>gh;thiscanbe

mostclearlyseeninFig.2(d)and(h).Ontheotherhand,ifge

<gh,thentheinnersidebandswouldbebrighterthantheouter

sidebands. Thus through the Mollow luminescence spectra,

onecangaininsightintowhichgfactor,georgh,isthelarger

ofthetwo.

Tofurtherinvestigatetheeffectofthestronglaseronthe

four-levelsystemofourpositivelychargedQD,weresonantly

pumpthetwooutertransitions,asshowninFig.3.InFig.3(a)

wedrivethehighest,whereasinFig.3(b)wedrivethelowest

energytransition.Thestronglaserdrivingleadstothedressing

ofthegroundandexcitedstatesofthetransitionbeingdriven,

whichinturngivesrisetoaMollowtriplet,similartothatofa

regulartwo-levelsystem.However,thisdressingalsoaffects

thetwoinnertransitionsaseachofthemdevelopsintoadoublet.WenotethattheMollowsidebandsofthedriventransitionshowasimplecrossingwiththeinnertransitiondoublets.

FIG. 2(a)-(d)PowerdependentexperimentalPLspectraforaQD

stronglydrivenwithalaserspectrallypositionedin-betweenthetwo

innertransitions(0 eV),forfourdifferentexcitation(detection)angles.Theplotsareshowninlinearcolorscaleandhavetheeigenenergiesofeq.(1)superposedinreddottedline.(e)-(h)Calculatedspectrafromquantumopticalmodelingforthesamepolarizationsettings

asin(a)-(d)respectively.

correspondtotheeigenvaluescalculatedfromHamiltonianin

Eq.(1).Superimposingtheeigenenergiesontheexperimental

datainFigs.2(a)-(d)enablesustofurtheridentifyanotherinteresting anticrossing, between the Mollow sidebands of the

twooutertransitions.Themodelsuggeststhattheanticrossing

splittingbetweenthetwoouter-transitionMollowsidebandsis

twicethesplittingbetweentheinner-transitionMollowsidebandandtheouter-QDtransition.Thetwoaforementionedanticrossingsareinstarkcontrasttothebehaviorseenforlower

drivingpowers.At~4.510-3W,wheretheMollowsideband

splittingisabouthalftheZeemansplitting,theMollowside-

*lagous@stanford.edu

[1]

[2]

[3]

[4]

[5]

[6]

[7]

[8]

[9]

FIG.3(a)Powerdependentspectrawhenthelaserisinresonance

withthehighestenergytransitionofthefourlevelsystem(transition

1-4oryellowarrowinFig.1(c))at112eV.Thecolorscaleishere

logarithmictohighlighttheghostbranchesofthetwoinnertransitionswhichappearatenergieshigherthananyoftheQDstatesthat

exist in the lab frame. (b) PL spectrum when pumping the lowest

energytransition(transition2-3orvioletarrowinFig.1(c))at-112

eV.ThereddottedlinesaretheeigenenergiescalculatedfromEq.

(1).(c),(d)Modeledspectrawithparametersthatcorrespondtothe

experimentalconditionsof(a)and(b)respectively.

emissionatenergiesbeyondthefourtransitionsthatexistin

the laboratory frame. These ghost transitions are a consequenceofthedressing(transitionsbetweendifferentdressedstatemanifolds),andarefullycapturedbyourrotatingframe

modelasshownbythesuperposedeigenvaluesandthecalculatedspectra.

Insummary,wehaveinvestigatedMollowphysicsbeyond

asimpletwo-levelsystembystudyingthefirst-ordercorrelationsoftheMollow-tripletemission(theluminescencespectra)inamoreintricatefour-levelsystem.Webelievethatour

workwillpavethewayforfuturestudiesofnonclassicallight

emissionthatwillshowstrongcorrelationsintheoutputstatisticsofthesidebands.Tothisend,lightcontainedinMollow

tripletshasrecentlybecomeofincreasinginteresttothecommunityduetoitsabilitytocomprisetailorednonclassicalstatisticsthroughspectralfiltering[26].Wethusexpectthatour

morecomplexandinteractingMollowsystemwillprovidea

richsetoffrequency-filteredstatisticstoexploreinthefuture

and might prove extremely valuable in building future nonclassicallightsources.

TheauthorsacknowledgefinancialsupportfromtheArmyResearchOffice(ARO)(W911NF1310309)andtheNationalScienceFoundation(NSF)(1503759).

[10]

[11]

[12]

[13]

[14]

[15]

[16]

[17]

[18]

[19]

[20]

[21]

[22]

[23]

[24]

[25]

[26]

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Observation of Mollow Triplets with Tunable Interactions

in Double Lambda Systems of Individual Hole Spins

K. G. Lagoudakis*, K. A. Fischer, T. Sarmiento, P. L. McMahon, M. Radulaski, J. L. Zhang,

Y. Kelaita, C. Dory, K. Mller & J. Vukovi

E. L. Ginzton Laboratory, Stanford University, Stanford, California 94305, United States

This document provides supplemental material for the Letter Observation of Mollow Triplets with Tunable Interactions in

Double Lambda Systems of Individual Hole Spins. In particular, we provide more detailed information on the magnetic

spectroscopy of the QD studied in this work as well as statistics for the charged quantum dot g factors. In addition we explain

in detail the differential spectroscopy method that we used for the observation of Mollow triplets with tunable interactions.

charged quantum dots we perform standard magnetospectroscopy combined with above-band excitation. The

quantum dot (QD) studied in this Letter is centered at 1.351782

eV, and features a 9.8 1.7 eV linewidth as shown by the fit

in Fig. S1(a). This linewidth is very close to the resolution of

our custom monochromator which is ~9 eV. The energy

difference between the two main orthogonal polarizations of

this QD is fitted to 0.40 0.05 eV yielding a 0.2 eV fine

structure splitting. Application of a magnetic field

perpendicular to the growth axis (Voigt configuration) splits

the ground and excited states of the charged quantum dot

leading to the gradual transformation of the initial doublet into

fitting for each of the two polarizations to extract the peak

locations, as is shown in Fig. S1(c). For the extraction of the

linear-in-field Zeeman splitting, one has to subtract the

quadratic-in-field diamagnetic shift. This is done by

calculating the center of mass energy of the two outer

transitions, which is shown in Fig. S1(d). A quadratic fit allows

estimation of the diamagnetic shift factor, here fitted to 3.45

0.02 eV/T2. Any deviation of the data from this quadratic

behavior is due to thermal drifts, and as can be seen from the

data in Fig. S1(d), we have taken great care to maintain a

constant sample temperature (8.92 0.02 K) during the

adjustment of the magnetic field. To better characterize the

QDs of our sample, we also performed spectroscopic studies

on multiple QDs at maximum magnetic field (5T) in order to

have an overview of the g-factors of the quantum dots. The

distribution of g-factors is shown in Fig. S2, and is color coded

according to the center wavelengths of the QD PL emission

spectra.

Differential Spectroscopy. For the acquisition of the

power dependencies that are presented in the main part of the

FIG. S1. (a) PL spectra of the QD studied in this Letter under zero

magnetic field. (b) Waterfall plot of PL spectra for increasing

magnetic field. (c) Raw peak locations for the two inner and two

outer transitions extracted from multi peak fitting. (d) Center-ofmass energy of the two outer transitions. A quadratic fit allows

estimation of the diamagnetic shift factor.

studied. The electron g-factors are centered around 0.43 with a

narrow distribution, whereas the hole g-factors are distributed

between 0.1 and 0.45.

this section. The system under investigation is driven with two

lasers; an above band laser of fixed power close to saturation

(~ 1.25 W) and a resonant laser of variable power. The aboveband laser has a dual role: it is used to stabilize the charges in

the QD and is used for PL emission. When the above-band

laser is turned off, there is complete suppression of the charged

exciton states and therefore only photons from the scattered

laser are detected (due to the incomplete cross-polarized

suppression). Fig. S3(a) shows the raw acquired spectra with

both lasers on, while the raw spectra with only the resonant

laser applied are shown in (b). A pixel by pixel subtraction of

the spectra in Fig. S3(b) from those in Fig. S3(a), leaves only

the PL coming from the strongly driven four level system of

the positively charged QD studied in this Letter. In particular,

here we show the raw data from the acquisition done with

120/30 excitation/detection as shown in Fig. 2 (d) in the main

manuscript. This method is independent of the resonant laser

excitation frequency and therefore was used for the acquisition

of the spectra in Figs. 2 and 3 of the manuscript.

FIG. S3. (a) Raw power dependent experimental PL spectra for the

QD studied in this Letter when it is driven with a combination of an

above-band laser of fixed power and a resonant laser with variable

power, spectrally positioned in-between the two inner transitions (0

eV), for 120/30 excitation/detection angles. (b) Raw power

dependent spectra with only resonant laser on. Subtraction of (b)

from (a) results in the data presented in the manuscript (in particular

Fig. 2(d)). Note that both graphs are presented in log colorscale to

enable the reader to identify the lines coming from the strongly

driven four-level system.

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