Semicand. Sci. Technal. 8 (1993) 67M74.

Printed in the UK

Centre-of-mass quantization of excitons in GaAs quantum boxes

S Jaziritx?G Bastards and R Bennaceurt 7 Laboratoire de Physique de la Matiere Condensbe, Facult6 des Sciences de Tunis, Campus Universitaire, Belvedkre.1060 Tunis, Tunisia Dkpartment de Physique de L'Ecole Normale Superieure d e Bizerte, Jarzouna 7021, Bizerte, Tunisia 9Laboratoire de Physique de la Matikre Condensee d e I'Ecole Normale Sup&rieure,24 rue Lhomond, F-75005 Paris, France

Received 4 December 1992, accepted for publication 20 January 1993

Abstract. By using

a variational-perturbative method, we have studied the excitons confined in wide quantum boxes, i.e. the size quantization of the exciton centre-ofmass. The exciton energies are significantlyshifted to high energy. The oscillator strength is enhanced with decreasing box size.

1. Introduction

2. Determinationof energy levels and wavefunctions

Recently nanofabncation technology has attracted great interest, and it has become possible to confine carriers in all three spatial dimensions, thereby creating quantum boxes and quantum dots [l-131. The optical properties of confined systems have been shown to be strongly influencedby the carrier confinement, leading to a significant enhancement of the excitonic binding energy and oscillator strength, as in two-dimensional structures (quantum we& QW)[14] and in one-dimensional systems (quantum well wire, QW) [l5] and probably in zerodimensional systems (quantum box, QB) [S, 16J To our knowledge the transitions between the different dimensional systems are not well known. The transition from 3D bulk-like excitons to 2D quantum well excitons is characterized by the quantization of the centre-of-mass motion of the exciton [17-191. Recently [ZO] the transition from the 2D quantum well regime to the ID quantum well wire exciton regime was also shown to be dominated by the quantization of the centre-ofmass motion, Here, we shall study the excitons in a large quantum box the volume of which is significantly larger than U:, where a, is the exciton Bohr radius. This corresponds to the dimensions of the boxes currently being fabricated. In these wide boxes, the Coulomb interaction correlates the relative motion of electronhole pair while the confinement influences the centre-ofmass motion of the pair. We shall show that the exciton levels follow the centre-of-mass quantization like a 'single particle' and not the separate electron-hole quantization. We present the theoretical framework in section 2, the results for exciton binding energies and oscillator strengths in a quantum box in section 3 and our conclusions in 4.
0268-1242/93/050670

We consider a rectangular GaAs quantum box (Lx, L,, Lz) embedded in Ga,-Al,As barriers, with the condiL,, L, are the well widths along tion Lx > L, > L, (Lx, the x, y and z directions respectively). The Hamiltonian or the exciton in this quantum box, within the effectivemass approximation, is given by

- -E 2mLi (E) az: + V,(Xi,y;, 2;)

(3) O(x) is the step function, E, is the bulk bandgap energy and E is the dielectric constant for GaAs; the distortion due to the image potential effect is neglected. K=c, is the potential of the finite well in one direction determined by the energy discontinuity between well and barrier materials. In the GaAs/Ga,-&As system this discontinuity (ev) at 300 K and can be expressed as AEG = 1.247~ x 50 . 4 5 , where x represents the mole fraction of A l in the alloy. In our calculation x is'equal to 0.32. This discontinuity is then split between conduction and valence bands. A splitting ratio of 0.65/0.35 was used in this work. The effectivemass in the directions (x, y) is m,,,, and inLiis the effective mass in the perpendicular direction (2). At the

+ 05 $07.50 @ 1993 IOP Publishing Ltd

Quantization of excitons in GaAs quantum boxes

. . c

n.. . A . : . . * . c ..__. ,... . . .11. L . _ . : . _ . -7.. lor v a n s . n t inc inierrdces oetween wcus m u uamcrs tile discontinuity in effective masses was taken into account.
^__I

band edge, the effective masses are mi/, = m,, = 0.665m0; the heavy hole has miihb= mo/(yl y Z ) , mlhh = mo/(y, - Zy,), and for the light hole m,,lh = mo/(yl - y2), mLlh = mo/(y, + 2y,), where m is the free electron mass and y1 = 6.85 and y 2 = 2.1 are the Luttinger parameters

.,..

The Hamiltonian H,(R, A) is the unperturbed part which can he solved exactly. H,(R, r, A) is the perturbation term and the parameter A is a variational parameter. This method combines the variational method with the perturbation one and its validity can be assessed immediaieiy ,Decause creates own smdd p a r ~ e i e r ,iising the quasidecoupling approximation [22] to solve the Hamiltonian H2(R, I.), which is valid because we consider a large quantum box with the condition L, > L y > Lz, the calculation is processed from the motion along
2

Using the centre-of-mass and relative coordinates (R, r) of the electron-hole. pair with the corresponding total masses ( M / / , M,) and reduced masses (,u/,, pi), the iiamiiionian caR.De iew.riiien ag

axis io

motion

. + e obtain the

envelope function and the energy level for the centre-ofmass (CM)motion along the z axis by the following equations:

+ V(R, + E ,
P)

(4)
hcUh)

with the potential given by

v(R U) = ve(re) f

(5)
(6)

H = Hl(r) + H2(R)+ V(R,r).

V,(Z, A) = lAEG@ 2 --

( ?)

VZO Z 2 - -

7)
.

(14)

H,(r) represents the relative motion of the electron-hole pair and characterizes the Coulomb correlation between the two particles. As a first simplifying step we can approximate the reduced masses in H,(r) by

21 1 1 P 3 P// 3 Pl The Hamiltonian HI@)becomes

- = _ _ +--,

(7)

By the same calculation as that in a conventional quanis a simple trigotum well [14] the wavefunction nometric function in the well and exponential outside the well in the case of the bound states. At the interface between the weU and the barrier, the discontinuity in effective masses is taken into account and the energy level E, is determined by

@ , ( a

and the solutions for H,(r) are the well known hydrogenic wavefunctions. The Hm.i!tonian li12(11) + V(R, r ) describes the centre-of-mass motion, like a single-particle system conlined in a box with barriers characterized by the potential V(R, r). To solve this Hamiltonian we introduce a parameter 1, by adding and subtracting the potential AV@): in order to be able to split this Hamiltonian into two terms [Zl]:
HLR) +

In a second step, we obtain the envelope function a,(?) and the energy ievei E , along the y axis by tine same procedure, with the harrier potential given by

W,
O2

= HLR, 1 . )
-1
\

+ HAR,

F,

A)

(9)

with
H2(R, 1 . )= hZ -2M,,X : 2 (

5)

Finally we obtain the envelope function (X) and the energy level E,, in the x direction with the barrier potential.

- ?-(E) 2 ~ , azz + AV(R)

where

xo

. ( ?)
x2--

1Y(R) = 1AE&

(X 2 -):

We thus obtain the total wavefunctions of the CM in the quantum box as

Y,,,(X, x 2, I.) = W Z , A)@,(E: They correspond to the energies

%MN(~)

A)@,(X, I.). (18)

and

H,(R, r, A) = V(R,r ) - IV(R).

(12)

(1% These solutions, which still depend on the parameter A, are for the unperturbed part of the CM Hamiltonian. To
= EL@)
671

+ EM@) + EN@).

S Jaziri et a/

obtain the actual CM energies and wavefunctions, we determine the best choice of 1 as the one which ensures the fastest convergence of the perturbation series. Under these circumstances we shall write

R = re = r,. According to equation (27) the oscillator

strength for a 3D bulk-like exciton is

ELMN= E h N ( 4 + A E W " 4 (20) where AELMN(A) is approximated by the first-order energy matrix correction calculated by perturbation method AE!&

where E , is the exciton energy given by E., = E , - R, in the bulk, 2 ! is the sample volume and ]91s(0)12 is equal to 1/naz. Substituting C in equation (28) we find

" ( 4

(X.~,,,,,,~~(R, r, A)lH3(R,r, L ) ) I X ~ ~ ~ , L M NV, (R A, ) (211 where x~~~.LM Y, N 4( = R> Rni(r)YX&~ Y L M N 4( R = Cp,dr, W L M ~ (4. RI (22) Finally, the energy levels of the exciton in a quantum box are given by
RY E n i m ,=~EG ~~i N &,,,,LMN n + E ~ M+

I
In the following we will present the calculated oscillator strength of the exciton ground state in the box normalized to that of a free exciton in a bulk material with volume C2 = LxL,Lz. In the large C2 limit f/f., becomes independent of C2 and converges towards 2'/n6 = 0.53, a limit obtained by assuming an infinite confinement for the CM coordinates along x, y and z. It is troublesome that one does not recover lim (f/f,,) = 1. This point has already been noticed by Kayanuma [16] (who studied the case of cylindrical confinement) and directly results from the assumed even distribution of the free exciton CM in the volume a, i.e. disregarding any edge effect. One may, however, remark that the infinite L limit is to a large extent unreachable in actual materials. Indeed, if the box size is very large, the scattering phenomena will unavoidably limit the coherence of the exciton wave function to a volume V,,, thereby preventing the infinite L limit being meaningful.
3 . Numerical results

(23)

where R, is the effective Rydberg of the 3D exciton. The best solution, which no longer depends explicitly on the parameter A, is determined by minimization of the total energy value by the principle of minimal sensitivity [21,23]. This condition is satisfied by requiring

with respect to L. If AEnlm,LMdA) is approximated by AE,$A,LMN(%)of equation (21), the condition (24) can be satisfied by requiring

AEL;A,LMdl) = 0 (25) yielding the L value. In order to calculate the exciton ground state relative to the heavy-hole exciton (E-HH) and light-hole (E-LH), we numerically evaluate the first-order perturbation energy; the optimum condition requires AE\i!lll(J.) = 0 and thus determines the best variational parameter Lo. Hence the exciton ground state determined by the perturbative variational criterion is E E , - R y E11l(do). (26) We also calculate the oscillator strength for the exciton ground state using the normalized wavefunction given by (22); the oscillator strength for the ground state is [24]

where C is a constant of proportionality which includes the electric dipole matrix element and E is the exciton energy in the box given by (26). The oscillator strength is proportional to the probability amplitude of finding an electron and a hole at the same site, as is well known in the case of the bulk [26] corresponding to Y = 0 and
672

We have numerically evaluated the expressions derived CM energy levels for heavy-hole exciton (E-HH) and light-hole exciton (E-LH) for several values o f the box dimensions. In figure 1 we plot the CM energies of the two quantum states as a function of the length Lz, keeping L, = 500 & . and Lx = 1000 8, to show the importance of the CM size quantization. We see that the energies decrease with increasing Lz, a feature reminiscent of quantum well behaviour (the size quantization for the x and y motion in negligible compared with that of the z motion in figure 1). At large Lz the exciton energies converge to the respective bulk Rydbergs. Note that in this limit the model of CM quantization provides a lower exciton energy than the one which assumes an independent confinement for the electron and the hole (since l/(m, mh) < l/m, + l/mh). It is not easy to find a lower limit on Lzwhere the CM quantization model becomes worse than the model of independent particle quantization. A qualitative criterion would be to consider the CM quantization meaningful if the CM confinement were smaller than or equal to the energy separation between the 1s and 2s states, i.e. if

i n section 2 and minimized the

(30)

Quantization of excitons in GaAs quantum boxes

150

125

;::\
v I

h G E

50~

25 ~

00 0

Figure 1. Excitonic CM energies as a function of L, for t h e ground state of heavy-hole excitons (E-HH) and light-hole
excitons (E-LH).

LY=500

%.

I uu=innn =1000%.

:E-HH - . .,,
I .

, particle quantization.

behaviour as in figure 1. The heavy-hole CM is lower in energy than the light-hole CM because of its heavier mass along the z axis. Figures 3 and 4 show plots of the reduced exciton oscillator strength f / f . , versus Lz (at fixed Lx, Ly) or versus L, (at fixed L,, Lz). In these plots the change of f/f., -with Lz or L, is dominated by that of I~YlI1(R)d3RIZ while the CM energy-dependent term displays negligible variation. In the strong confinement regime, our calculated increase of f/f,. is less important than the ones found by Bryant [SI or Kayanuma [16] who used models of separate confinement for the electron and the hole. In the intermediate regime (Lz 2 200 A), however, our model of CM quantization leads to a gent1e.r . l , : -'t , ' . ___:It. r . L e . . & I . ":--IUCUIUC UI J Jer W l U l fiz W61l LUG UllC5 d>>UUUUgS L U p G ^^^^

100
1

do

200 200

400 400

500 500

c-IUI

a Way the effectiveHamiltonian acting on the exciton CM can

a
VlIC-UUUCU>IUIldl
blLG q U l U ~ t l U l l . Ill b U U I

.-, :

_I_^ -2--<-..

TA

_ . . _ I .

safely be taken as scalar, and the effective potential energy is the actual one weighed by the 1s probability density for the reduced motion. The criterion quantitatively means Lz 2 200 A for GaAs-like parameters. In materials with a wider bandgap or more polar materials the CM quantization model should work down to lower thicknesses than in GaAs-Ga(A1)As. We show in figure 2 the CM ground state energy versus L, for the (E-HH)and the (E-LH) excitons for Lz = 250 8, and Lx = 2000 A. One finds the same kind of

.-I
s
0

I
--- E-HH
LY=500 A. U=2000 A E-LH

2-

Figure 3 . The normalized oscillator strength of the exciton ground state per unit volume as a function of the length Lz.

2 ,

---

I7-nEn Y-LJY

A. LX=2000 A E-HH

E-LH

Figure 2. Excitonic CM energies as a function o f L, for the

ground state o f heavy-hole excitons (E-HH) and light-hole excitons (SLH).

Figure 4. The normalized oscillator strength of the exciton ground state per unit volume as a function o f the length L,.

673

S Jaziri et a/

4. Conclusion

[ q Gilliot P, Merle J C, Levy R, Robino M and Honerlage

B 1989 Phvs. status Solidi b 153 403 Gilliot P, Honerlage B, Levy R and Grun J B 1990 Phys Starus Solidi b 159 259 [7J Hu Y Z , Koch S W, Lindberg M and Peygahambarian N 1990 Phys. status Solidi b 159 249 [SI Bryant G W 1988 Phys. Reu. B 37 8763 [9] Belleguie Land Banyai L 1991 Phys. Rev B 44 8785 [lo] Pollock E L and Koch S W 1991 J. Chem. Phys. 94
fi7-X ",

We have studied the size quantization of the exciton centre of mass in quantum boxes by combining variational and perturbation methods. Our calculations should work relatively well in wide boxes (with dimensions 2 2-3 Bohr r a d i i ) but are not expected to be better than the models which assume independent size quantizations for the electron and the hole in narrow boxes. The transition from the CM quantization to the singleparticle independent quantizations remains to be more quantitatively studied.

[Ill Tran Thoai D B, Hu Y 2 and Koch S W 1990 Phys. Rev. B 42 11261 r121 Sakaki H .Kat0 K and Yoshimura H 1990 ADD[. Phvs. Lett. SI 2800 [13] Ye Q Y, Tsu Rand Nicollian E H 1991 Phys. Reu. B 44

.-

- _

. 1

1806
hd...nu.l.%Anm.%nt.=

-"R'."...'~J.."..."

[I41 Basiaid G 1988 Wave Mechapics Applied to Semiconductor Heterostructures (Les Ulis: Les Editions de Physique) [l5] Hirayama Y and Okamoto H 1988 Physics and

The Laboratoire de Physique de la MatiLre Condende de l'Ecole Normale SupCrieure is Laboratoire associk au CNRS (UA 1437) et aux UniversitCs Paris 6 et Paris 7. This work has been partially supported by the Commission of the European Communities (Esprit Project

[la

6719)

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