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Fine structure of excited excitonic states in quantum disks M. M. Glazov,1 E. L. Ivchenko,1 R. v. Baltz,2 and E. G. Tsitsishvili2 1A.F. Ioffe Physico-Technical Institute RAS, 194021 St.-Petersburg, Russia 2Universit¨at Karlsruhe, 76128 Karlsruhe, Germany 5 Wereportonatheoreticalstudyofthefinestructureofexcitedexcitoniclevelsinsemiconductor 0 quantum disks. A particular attention is paid to the effect of electron-hole long-range exchange 0 interaction. We demonstrate that, even in the axisymmetric quantum disks, the exciton P-shell is 2 split into three sublevels. The analytical results are obtained in the limiting cases of strong and n weak confinement. A possibility of exciton spin relaxation dueto theresonant LO-phonon-assisted a coupling between the P and S shells is discussed. J 6 2 I. INTRODUCTION similarly to4 if one includes an admixture of light-hole states into the heavy-hole exciton wave function. ] Weconsideraquantumdiskformedbya2Dharmonic In the envelope-function approximation, the excitonic l al states in semiconductors and semiconductor quantum potential V(ρe,ρh) = Aeρ2e +Ahρ2h in a quantum well grown along the z-axis. Here the 2D vector ρ deter- h dots can be classified by referring to the orbital shape e,h - of the exciton envelope function (S-, P-, D-like)and the mines the in-plane position of an electron or a hole, and s A are positive constants. Assuming that the confine- e characteroftheelectronandholeBlochfunctions(bright e,h m and dark states). For example, the state P y means a ment along the growth direction is stronger than both x | i the quantum-disk and Coulomb potentials the envelope brightP -shell exciton with the electron-hole dipole mo- . x t for the electron-holepair wavefunctioncanbe written as a ment directed along the y axis. Theoretically, the fine m structureofexcitedstates ofzero-dimensional(0D)exci- - tonshasbeenstudiedforexcitonslocalized,respectively, Ψ(re,rh)=ψ(ρe,ρh)ϕe(ze)ϕe(zh), (1) d by rectangular islands in a quantum-well structure1, n quantum disks with a Gaussian lateral potential2 and where ϕe,h(ze,h) are the respective z-envelopes of elec- o lens-shaped quantum dots3. However, up to now the tronandhole, and ψ(ρe,ρh) is anin-plane wavefunction c splitting of excited-exciton levels has been analyzed for of exciton calculated with allowance for both Coulomb [ a fixed orbital shell, e.g., the P shell, which is valid in interaction and quantum disk potential. The form of x 1 the case of strongly anisotropic confinement so that the the function ψ(ρe,ρh) depends on the relationship be- v orbitalsplittingoftheP-likeshellsP andP exceedsby tween the potential radius and 2D-exciton Bohr radius, 5 x y 3 far the exchange-interaction energy. Here we show that, aB. In the weak confinement regime, i.e. in a quantum 6 foraxiallysymmetricorsquarequantumdots,onehas,in diskwiththediameterexceedingaB,thetwo-particleen- 1 addition, to take into account the exchange-interaction- velope probe function ψ(ρe,ρh) is a product F(R)f(ρ) 0 induced mixing between the excitonic states P y and oftwofunctionsdescribing,respectively,thein-planemo- x 5 P x . Moreover, for the first time we focus o|n thie in- tion of the exciton center of mass R = (X,Y) and the y 0 |terpliaybetweentheexchangeinteractionandanisotropic relativeelectron-holemotion,ρ=ρe ρh. Onthe other t/ shape of the dot and develop an analytic theory in the hand, in small quantum disks with −strong confinement a particularcasewhere the orbitalandexchangesplittings where single-particle lateral confinement dominates over m are comparable. the Coulomb interaction, the pair envelope can also be - presented as a product of two functions, ψ (ρ )ψ (ρ ), d e e h h butheretheydescribetheindependentin-planelocaliza- n o II. ELECTRON-HOLE EXCHANGE tion of an electron and a hole. c INTERACTION IN QUANTUM DISKS For the exciton envelope functions presented in the v: form (1), the matrix element Hn(l′onng) of long-range ex-′ i change interaction taken between the exciton states n X The two-particle excitonic wave function can be writ- and n is written as follows ten as a linear combination of products Ψ (r ,r )s,j , ar wfuhnecrteio|nss,,jsi aisnda jpraordeutchteoefletchteroenleactnrdonhoalsnejdspheinolehinBd|ilcoecsih, 2π1κ∞ (cid:18)me~0|pE0g|(cid:19)2Z dKKαKKα′ψn∗′(K)ψn(K), (2) Ψ(r ,r ) is the envelope function, and r is the elec- e h e,h e e tron (hole) 3D radius-vector. In the following, for the where the exciton-state index n includes the dipole mo- sakeofsimplicity, we concentrateonheavy-holeexcitons mentα,κ∞ isthehigh-frequencydielectricconstant,m0 withj = 3/2andthelong-rangemechanismofelectron- isthefreeelectronmass,Eg isthebandgap,p0 isthein- holeexcha±ngeinteractionwhichallowstodiscussonlythe terband matrix element of the momentum operator,and brightexcitonicstates s,j withs+j = 1ortheirlinear we introduced the 2D Fourier-transform | i ± combinations α with the dipole moment α=x,y. The | i ψ(K)= dRe−iKRψ(R,R) short-range mechanism may be taken into consideration Z e 2 of the function ψ(ρ ,ρ ) at the coinciding coordinates, to introduce, as a parameter describing the anisotropy, e h ρ =ρ R. a half of the P -P splitting, E , calculated neglecting e h x y anis ≡ theexchangeinteraction. Itsvaluedependsonthemodel of exciton quantization. If an electron and a hole are III. P-ORBITAL EXCITONS IN quantized independently (a a ) then, for the P ,S B e h AXIALLY-SYMMETRIC DISKS excited state, we have ≪ | i We startwith anaxially-symmetricquantum disk and d 2~ E = (6) calculate the fine structure of the P-orbital exciton level anis am a2 e and then proceed to a slightly anisotropic disk. The straightforwardcalculationshowsthatthelong-rangeex- and, for the Se,Ph state, Eanis differs from Eq. (6) | i changeHamiltonian(2)hasthefollowingnon-zeromatrix by the replacement me mh. Here Se,Ph means → | i elements an exciton formed by a Se-shell electron and a Ph-shell hole. If exciton is quantized as a whole then in Eq. (6) hPxx|H(long)|Pxxi=hPyy|H(long)|Pyyi=λ , (3) one should replace me by the exciton translational mass M =m +m and a by a =a(µ/M)1/4. e h exc Figure 1 shows splitting of the P-shell bright-exciton P y (long) P y = P x (long) P x =η , h x |H | x i h y |H | y i level as a function the ratio ξ = Eanis/∆. For small valuesofξ thesplittingofthedoublet 2isproportional ± hPyx|H(long)|Pxyi=hPxy|H(long)|Pyxi=µ , ttoheξP2.-shIenlltehxecitliomnitstaotfesstfroornmgtawnoisdootruobpleyt,s,EaPnis,α≫an∆d, x | i where λ = 3η = 3µ. According to Eq. (3) and in agree- P ,α (α=x,y), separated by 2E and each split by y anis | i ment with the angular-momentum considerations, the ∆. P-shell of the bright exciton in an axisymmetric quan- tum disk is split into three sublevels, see Fig. 1. The (P , x) 4 x outermost sublevels labelled 0U, 0L are nondegenerate and characterized by a zero total angular-momentum z- 2 (P , y) component. The central doubly-degenerate sublevel cor- 0U x respondstothe angular-momentumcomponent±2. The D / 0 +2 intersublevel energy spacing, ∆, equals to 2η =2µ. E -2 The splitting ∆ depends on the character of exciton -2 0L (P , y) confinementinadisk. LetusassumeA =~2/2m a4, y e,h e,h where ais the disk effective radius,m arethe electron e,h -4 and hole effective masses. It follows then that in the (P , y) y strong confinement regime, a aB, one has 0.0 0.5 1.0 1.5 2.0 2.5 3.0 ≪ 3√2π e~p 2 x=E /D ∆= | 0| . (4) anis 16a3κ (cid:18)m E (cid:19) b 0 g FIG. 1: Interplay between the in-plane anisotropy and ex- In the opposite limiting case a aB where the exciton changeinteraction. Theexciton sublevelenergyE isreferred ≫ is quantized as a whole we obtain to theenergy of theuniaxial exciton ±2. 3√π e~p 2 0 ∆= | | (5) 2a a2κ (cid:18)m E (cid:19) exc B b 0 g with a = a(µ/M)1/4 being the radius of exciton in- V. RESONANT P-S EXCITONIC POLARONS exc plane confinement, M =m +m and µ=m m /M. e h e h Finally, we briefly discuss the P-S excitonic polaron which is formed as a result of the resonant coupling of IV. P-SHELL EXCITONS IN ANISOTROPIC the P- and S-like levels by a longitudinal optical (LO) QUANTUM DISKS phonon5. We use an approachdeveloped in Ref.6 to cal- culatetheLO-assistedresonantcouplingbetweenS-and We introduce a slightly elliptical lateral potential re- P-shell electron states confined in a quantum dot. For placingthediskradiusabytheeffectiveradiia =a d, the Fr¨olich interaction, the constant of exciton-phonon x − a = a+d along the x and y axes, respectively, and as- P-S coupling is given by y suming d a. At zero d the exciton P-states are par- ≪ tially split by the exchange interaction. The anisotropy 2πe2~Ω (q) 2 of a quantum disk results in a full removal of the degen- γ =v I . (7) u Vκ∗ (cid:12) q (cid:12) eracy and formation of four sublevels. It is convenient u Xq (cid:12) (cid:12) t (cid:12) (cid:12) (cid:12) (cid:12) 3 HereΩistheLO-phononfrequency,V isthe 3Dnormal- tial linear polarization is being rapidly lost and the ex- ization volume, κ∗−1 =κ−1 κ−1, and citon photoluminescence is practically depolarized. On ∞ − 0 the contrary, if ∆ γ then the polarization relaxes on ≪| | (q)= dr dr Ψ (r ,r )Ψ (r ,r ) eiqre eiqrh . a much longer time scale and can be well preserved. e h p e h s e h I Z − (cid:0) (cid:1) The work is supported by RFBR, “Dynasty” founda- Depolarization of the linearly-polarized P-S excitonic tion–ICFPM,theCenterforFunctionalNanostructures polaronexcitedviatheP-shellisdeterminedbytheratio of the Deutsche Forschungsgemeinschaft within project of γ and the exchange splitting ∆. If ∆ γ the ini- A2 and by the programs of Russian Academy of Sci. ≫ | | 1 S. V. Goupalov, E. L. Ivchenko and A. V. Kavokin, JETP 77, 609 (1993). 86, 388 (1998). 5 O. Verzelen, R. Ferreira and G. Bastard, Phys. Rev. Lett. 2 T. Takagahara, Phys. Rev. B62, 16 840 (2000). 88, 146803 (2002). 3 G. Bester, S. Nair and A. Zunger, Phys. Rev. B 67, 6 T. Stauber, R. Zimmerman and H. Castella, Phys. Rev. B 161306(R) (2003). 62, 7336 (2000). 4 E. L. Ivchenko, A.Yu. Kaminskii and I.L. Aleiner, JETP

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