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Article Biasiol1998
Article Biasiol1998
Two- or three-dimensionally quantum-confined semi- The formation of surface patterns during growth relies
conductor structures have attracted much attention because on lateral gradients in the surface chemical potential m.
of their interesting physical properties and potential device Considering, for simplicity, variations in only one dimen-
applications [1]. To overcome limitations in size and inter- sion (j), m of the component i of an alloy at a growth
face quality related to traditional lithography techniques, temperature T is written as
many efforts have been devoted to study their formation mi m0 1 V0 fst sjdg2 y2E 1 V0 fgsud 1 g 00 sudgksjd
during the epitaxial process [2]. This can be accomplished
if a suitable driving force is introduced to yield the desired 1 kB T ln xi sjd , (1)
lateral heterostructure patterning. A widely used approach where xi is the mole fraction. In (1), the second term is
in this direction is to exploit self-ordering processes on pla- related to the tangential surface stress st , E being the elas-
nar surfaces, as for strained-induced Stranski-Krastanow tic modulus [4], the third one is due to the surface cur-
growth of quantum dots (QDs) [3,4]. Such techniques vature k and involves the (orientation-dependent) surface
have the advantage that self-ordering is achieved without free energy gsud [12] (with V0 the atomic volume), and the
any surface patterning prior to growth; however, they suf- fourth one is a contribution due to the entropy of mixing
fer from a limited control on uniformity and deposition [13]. Self-ordering driven by lateral gradients of stress has
site due to the intrinsic random nature of the nucleation been discussed for the InAsyGaAs system [4]. In what fol-
process. lows, we consider self-ordering of lattice-matched, strain-
Self-ordering of nanostructures on nonplanar sur- free structures, and hence drop the strain-related term.
faces has the potential for solving these problems, as For faceted surface profiles, such as the one shown in
the corrugated surface can provide a template for the Fig. 1, the curvature-related contribution to m in (1) can
nucleation sites. In fact, organometallic chemical vapor be expressed as [12,14]
deposition (OMCVD) and molecular beam epitaxy mt,b m0 6 gV0 ylt,b ; m s m0 , (2)
(MBE) on substrates patterned with corrugations (see
Fig. 1) [5,6] or with pyramidal patterns [7] have been
successfully employed to fabricate uniform arrays of
quantum wires (QWRs) and QDs. Despite the accurate
structural control demonstrated with this approach, the
understanding of the self-limiting growth mechanism
on such corrugated surfaces has been essentially phe-
nomenological [8]. Existing models can, in fact, predict
only constant growth rates of thick layers on mm-sized
facets, depending on their orientation and environment,
as a result of gas-phase and surface diffusion [9,10].
The growth behavior of facets in the 10-nm scale,
relevant to the self-ordering of quantum nanostructures,
cannot be explained with such models, since facet-size
dependent surface diffusion fluxes should be invoked to
account for the self-limiting growth [11].
In this Letter we address the self-limiting growth of
FIG. 1. Schematic groove profiles, composed of three facets
a corrugated surface, and establish a model that quan- (not to scale). (a) Evolution of the growth front as commonly
titatively describes the self-ordering of quantum wells observed in OMCVD. (b) The same for MBE. (c) Chemical
(QWs), QWRs, and QDs on such patterned substrates. potential at each facet.
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VOLUME 81, NUMBER 14 PHYSICAL REVIEW LETTERS 5 OCTOBER 1998
sl sl
where lb,A and lb,G denote the self-limiting facet widths for barrier on the sidewalls perpendicular to the groove
the binary AlAs and GaAs composition, respectively. The axis, (4) predicts a dependence essentially of the form
self-limiting profile of an alloy is therefore determined by exps2EB y3kB Td for lbsl in a binary. For Alx Ga12x As,
the interplay among the effects of capillarity sad, entropy the T dependence of lbsl , given by (6), derives from the
of mixing sbd, and growth rate anisotropy fDrsxdg. Arrhenius form of lb,A sl sl
, lb,G , LAs , and LGs . The measured
The self-limiting widths lbsl of Alx Ga12x As grooves sl
variation of lb with T is shown in Fig. 3(b) for x 0,
grown by low pressure OMCVD were measured from 0.19, 0.29, and 0.47 and for 600 , T , 750 ±C. As
TEM data for a wide range of growth parameters [18]. the bottom facets could not be readily resolved for very
Figure 3(a) shows the measured self-limiting widths versus narrow s,10 nmd profiles, we have characterized the
sl
x for T 700 ±C. Using the measured parameters lb,G groove width in that case by the radius of curvature rsl
sl
129 6 3 nm, lb,A 9.1 6 0.1 nm, and Dr 0.22 6 G
for a hyperbola tangent to the surface [8]; rsl is related
0.05 [19], we fitted the experimental values with the to lbsl via a simple geometrical factor. The Arrhenius
solution of (6), leaving LG s as the only fit parameter fit for GaAs gives EBG 1.9 6 0.3 eV. This parameter
[20], and finding LG s 175 6 20 nm. This value is is then employed in (6) to fit the Alx Ga12x As profiles,
lower than the one estimated on (100) surfaces [21], as sl
as a function of lb,A only. As before, we have assumed
expected for a densely stepped, high-index facet. To sLs d ¿ sLs d , Dr G 0.22 6 0.05 (this value does
G 2 A 2
estimate the importance of the entropy effects, we also not vary significantly with T , in the range considered),
represent by the shaded area in Fig. 3(a) the best fits and verified the insensitivity of the fit to the value of
for lbsl neglecting the term sbd in (6) and setting Dr G Dr A . Least squares fits of the Alx Ga12x As profiles
0.22, with the boundaries corresponding to the extreme [Fig. 3(b)] yield, consistently for the three composi-
cases Dr A 1 (long-dashed line) or Dr A 0 (short- tions, EBA 2.3 6 0.2 eV. This difference between
dashed line). The measured alloy self-limiting widths are the GaAs and AlAs diffusion barriers is consistent with
systematically smaller than the ones predicted neglecting stronger Al-As bonds, as compared with Ga-As ones [22].
the entropy term. The evolution of the surface profile towards a self-
Assuming an Arrhenius temperature dependence limiting shape can be evaluated by relating the variation
of Ds D0 exps2EB ykB T d, with EB the diffusion in the facet width to the difference in growth rates at the
bottom facet and the sidewalls as dlb psdzb 2 dzs d [2],
where p is a factor dependent on the facet orientations
( p 3.75 for our geometry). The evolution of lb is
obtained by combining (3) and (4) for a binary, or (5) and
(6) for a ternary, yielding, respectively,
"√ !3 #
dlb lbsl
pDr 21 , (7a)
dzn lb
( "√ !3 # )
dlb lbsl b
p Drsxd 2 1 1 3 slb 2 lb d , (7b)
sl
dzn lb lb
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VOLUME 81, NUMBER 14 PHYSICAL REVIEW LETTERS 5 OCTOBER 1998
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