InAs quantum dots on GaAs()B

T. Suzuki, Y. Temko, M. C. Xu, and K. Jacobi Citation: J. Appl. Phys. 96, 6398 (2004); doi: 10.1063/1.1811387 View online: http://dx.doi.org/10.1063/1.1811387 View Table of Contents: http://jap.aip.org/resource/1/JAPIAU/v96/i11 Published by the American Institute of Physics.

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JOURNAL OF APPLIED PHYSICS

VOLUME 96, NUMBER 11

1 DECEMBER 2004

InAs quantum dots on GaAs112B

T. Suzuki, Y. Temko, M. C. Xu, and K. Jacobia)
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany

(Received 4 August 2004; accepted 7 September 2004) InAs quantum dots (QDs) were prepared by molecular beam epitaxy on GaAs B substrates. 112 Shape and size distribution of the QDs were investigated using in situ scanning tunneling microscopy as function of preparation temperature between 435 and 550 C. The wetting layer is not at but undulated in submicrometer scale in a similar way as the bare substrate. The atomic structure of the wetting layer is the same as found for the at base of InAs QDs grown on 111 143 GaAs B substrates. The shape of the QDs is given by {110}, B, and B bounding 113 facets and a round vicinal 001 region. Unexpectedly, the number density increases and the size distribution sharpens, when the growth temperature is increased from 435 to 470 C, which is attributed to lattice defects incorporated into the QDs during growth at 435 C. 2004 American Institute of Physics. [DOI: 10.1063/1.1811387]
I. INTRODUCTION

used in situ scanning tunneling microscopy (STM) for analysis.

II. EXPERIMENTAL METHODS

High-index GaAs and InAs surfaces have attracted much interest in connection with quantum dot (QD) preparation. A recently reported high-index GaAs 2 5 1 1 A surface14 and its 137 A subunit form bounding facets on InAs QDs grown on the GaAs(001),5,6 GaAs 113 A,69 GaAs 114 A,10 and GaAs B.11 Another high-index GaAs B surface has 135 135 been discovered recently, which is facetted into vicinal 11 B surfaces for the bare surface, but becomes at by 25 deposition of a small amount of InAs, accompanied by a 135 c 2 2 reconstruction.12 The B facet forms a at base of InAs QDs grown on GaAs B13,14 and 113 11 B.15 GaAs 25 The GaAs B surface, which we use as substrate 112 here, has also interesting properties. It contributes to the at base of the InAs QDs on GaAs B, although its surface 113 13 InAs or InGaAs deposition structure is rather disordered. on this surface has been reported to induce QDs or quantum dashes formation.1619 The bare surface structures of the GaAs B have been already investigated in our previous 112 studies.2024 There are two surface structures, depending on the preparation temperature. A Ga-rich structure forms above 520 C with an interesting self-organized surface corrugation: 12 nm wide stripes form with two {110} side facets. An As-rich structure forms below 520 C that exhibits locally a highly disordered 2 1 reconstruction and some undulation on a submicrometer scale.24 Moreover, a complex faceted structure has been reported near the transition temperature.2023 In the present study, we investigated shape and size distribution of the InAs QDs grown on GaAs B. We pre112 pared our samples by molecular beam epitaxy (MBE) and
a)

The experiments were carried out in a multichamber ultrahigh vacuum system consisting of a surface-analysis, a MBE- and an STM-chamber (Park Scientic Instruments, VP2).25 STM tips were clipped from a tungsten wire and cleaned by electron bombardment in the STM chamber. Samples with a typical size of about 5 10 mm2 were cut from a GaAs B wafer (n type, Si doped, carrier concen112 tration 6.3 34.0 1017 cm3, wafer technology). The samples were cleaned by several ion bombardment and annealing cycles. Afterwards a GaAs buffer layer about 50 nm thick was deposited using MBE at 500 550 C. After the growth, the samples were kept under As2 ux for about 10 min. Then the samples were cooled down to 435 500 C, and kept at these temperatures for about 10 min under As2 ux. Then InAs was deposited. The sample heater and the In- and As-Knudsen cells were shut off, as soon as the reection high-energy electron diffraction (RHEED) pattern changed from streaky to spotty indicating QD formation. Then the samples were transferred to the STM chamber within one minute without breaking vacuum. All STM images were taken at room temperature. The nominal amount of InAs deposited onto the substrate was 0.71 0.02 nm, 0.64 0.02 nm, and 0.56 0.12 nm for 435 C, 470 C, and 500 C, respectively, at a growth rate of about 0.004 0.007 nm/ s. Beam equivalent pressure ratio 4.5 of As2 to In was 4050 at an As2 pressure of 107 mbar.
III. RESULTS AND DISCUSSION A. Structure determination during growth

Author to whom the correspondence should be addressed; electronic mail: Jacobi@fhiberlin.mpg.de 6398

RHEED patterns from the GaAs B substrate surface 112 are shown in Figs. 1(a) and 1(b) before and in Figs. 1(a ) and 1(b ) after InAs deposition at 470 C. The electron beam
2004 American Institute of Physics

0021-8979/2004/96(11)/6398/7/$22.00

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FIG. 1. RHEED patterns of the GaAs B surface, before (a, b) and after a , b 112

InAs deposition at 470 C.

was directed along 1 for Figs. 1(a) and 1(a ) and along 11 0 for Figs. 1(b) and 1(b ). Periodic reections are seen in 11 Fig. 1(a) as indicated by arrowheads. The distance between them corresponds to 0.41 nm in real space, which agrees with the unit-cell vector length 0.40 nm of the 11 GaAs B surface perpendicular to 1 . In addition, 112 weak half-order reections are seenas noted by 1 / 2 , 0 in Fig. 1(a)which indicate that the surface has a twofold periodicity in this direction. The reections are more diffuse in the 110 direction, as shown in Fig. 1(b), which indicates that the surface structure (in real space) is disordered perpen dicular to 110 . These RHEED patterns agree with our previous, atomically resolved STM images that exhibited a disordered 2 1 reconstruction under As-rich preparation conditions.24 At about 520 C a phase transition occurs between the As rich, disordered 2 1 reconstruction below and a Ga rich, corrugated structure above 520 C.24 Thus, all InAs QDs discussed in this contribution were grown on the As rich, disordered, and 2 1 reconstructed surface at temperatures between 430 and 500 C. After InAs deposition, the RHEED pattern changed from streaky to spotty as shown in Figs. 1(a ) and 1(b ), which indicates the formation of QDs in the Stranski-Krastanov growth mode. The InAs deposition was stopped as soon as this change was recognized by eye on the RHEED screen. Fundamental reections remain, but half-order reections disappear after this transition, as shown in Fig. 1(a ). A socalled chevron structure is not seen both in Figs. 1(a ) and 1(b ). A chevron structure is due to electron reections from facets tilted around an axis, that is an intersection line between the substrate plane and the electron scattering plane, and has been observed for the (137) facets for InAs QDs on GaAs(001).26

B. Overview STM images and size distribution

Figure 2 shows overview STM images after the InAs growth at sample temperatures of (a) 435, (b) 470, and (c) 500 C. QDs form at all growth temperatures. The number densities are 4 109, 3 1010, and 2 109 cm2 for 435, 470, and 500 C, respectively. The QD formation varies quite unexpectedly with growth temperature. There is a wellknown empirical rule that the size of the QDs increases with growth temperature and the number density of the QDs decreases.14,27 The results presented here do not comply with this rule: By raising the temperature from 435 C to 470 C the number density increases. Another interesting observation can be made from overview images such as those presented in Fig. 2: The wetting layer is not at but undulated on a submicrometer scale. The maximum corrugation is about 4 nm. The undulation seems to reproduce the initial bare surface that is also undulated on a submicrometer scale.24 The atomic structure of the wetting layer is described later in detail when presenting Fig. 7. Although there are some reports that InAs deposition on the B surface induces InAs quantum-dash (QDH) 112 formation,16,19 we could not nd any evidence for QDHs. Even for growth temperatures up to 550 C, that is, above the transition temperature between the As-rich and the Garich structures of the bare surface, no QDHs but large InAs clusters with ill-dened shapes are formed (not shown here). Figure 3 shows the size distributions of QDs grown at various temperatures. The size is measured at the foot of the QDs along 111 . The QDs show an unexpected behavior with the growth temperature as already mentioned during presentation of the overview STM images in Fig. 2. The size of the QDs in Fig. 3(a) ranges from 10 to 50 nm with a peak at 20 nm. The sizes are not as small as expected for the low preparation temperature of 435 C. Also, the distribution

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FIG. 3. Size distribution of InAs QDs grown on GaAs B at 435 C (a), 112 470 C (b), and 500 C (c).

FIG. 2. Overview STM images after InAs growth at (a) 435 C, (b) 470 C, and (c) 500 C. The sample bias is V = 3 V and the tunneling current is I = 0.1 nA. The size of the images is 500 500 nm2.

is broad with many relatively large QDs, one of which is indicated by an arrowhead in Fig. 2(a). Moreover, the number density is not large. As the growth temperature increases from 435 C in Fig. 3(a) to 470 C in Fig. 3(b), the mean

size of the QDs does not increase. The size distribution becomes much sharperloosing the tail to larger sizesand the number density increases by more than one order of magnitude. The remaining very weak tail between 35 and 90 nm is attributed to the relatively small number of the large dots, of which one is marked by an arrowhead in Fig. 2(b). A small number of such large QDs have been observed for all QD assembles, which have been studied in our laboratory on GaAs substrates of different orientation so far, and are attributed to dislocated QDs which grow larger due to reduced strain. The dislocations are thought to be created to reduce the strain.11 As the growth temperature is increased from 470 C in Fig. 3(b) to 500 C in Fig. 3(c), the changes in size distribution complies with the general rule: The QD size

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increases with the size distribution ranging from 30 to 55 nm and a peak at 35 nm. The number density decreases by nearly one order of magnitude.
C. Atomically resolved shape of InAs quantum dots on GaAs112B

In Fig. 2 it can be seen already that the QDs are of different size but of a typical shape at least with respect to their lateral connement at the wetting layer. It is very interesting to zoom in and to determine the three dimensional (3D) shape of a typical QD. 3D STM images of two QDs of slightly different shape, both grown at 435 C, are shown in Figs. 4(a) and 4(b). The azimuthal orientation of the QDs could be exactly determined from the atomically resolved structure of the wetting layer that is shown below in Fig. 8. The QDs are mirror symmetric with respect to the 110 plane normal to the surface, which reects the symmetry of the substrate. This proofs epitaxial growth. Interestingly, some QDs [see Fig. 4(b)] are elongated along 111 . In the case of the 113 A substrate we could correlate a similar elongation with a faceting of the round part 4 which obviously slowed down the growth speed of the round part along this direction.7 The QDs in Fig. 4 are terminated by four facets numbered 14 in Fig. 4(a) The QDs grown at 470 C exhibit quite a similar shape and are not shown separately. In Fig. 5 three QDs of different size are shown which were grown at 500 C. These QDs differ from those shown in Fig. 4 by the additional facets 5 and 6. Also in this case elongation into different directions is observed. Typical bounding facets of the QDs of Figs. 4 and 5 are depicted in Fig. 6. The individual facets were atomically resolved by STM, which allowed determining the orientation and surface structure of each facet. A high-resolution STM image of the facet 1 in Fig. 4 is shown in Fig. 6(a). White lines mark a rectangular unit cell on the facet. The facet is inclined to the substrate by 29 2 ; the lengths of the unitcell vectors and the angle between them are u1 = 0.54 0.04 nm, u2 = 0.41 0.02 nm, and 98 3 , respectively. The geometric values are 30, u1 = 0.55 0.52 nm, u2 = 0.41 0.38 nm, and 98. Thus, the facet 1 is identied as 1 01 and facet 2 as 01 . This assignment is also valid for 1 the 500 C QDs in Fig. 5. The facet 3 exhibits two different structures as shown in Figs. 6(b) and 6(c). The rst structure shown in 6(b) is identied as B-2 2 reconstruction from the following 111 data: The facet is inclined to the substrate by 19 2 and exhibits a rhombic unit cell as marked in Fig. 6(b). The lengths of the unit-cell vectors and the angle between them are v1 = 0.87 0.07 nm, v2 = 0.78 0.04 nm, and 57 3 , respectively. [Geometric values: 19, v1 = 0.86 0.80 nm, v2 = 0.83 0.77 nm, 59] The second structure is shown in Fig. 19 reconstruction 6(c) and is identied as B- 19 111 from the ringlike structures on the facet that are 0.93 0.07 nm in diameter. The same ringlike structures have been observed on the B facets of InAs QDs grown on 111 B13 and B11 substrates. It is known that the GaAs 113 135

FIG. 4. 3D STM images of InAs QDs grown at 435 C (V = 3 V, I = 0.1 nA). The size at the base along 111 is noted.

the 2 2 reconstruction is stabilized at lower temperature and the less As-rich 19 19 reconstruction at higher temperature.28,29 This agrees with our observation here that the B facet is 2 2 reconstructed for QDs prepared at 111 435 C [Fig. 4 and Fig. 6(b)] and 19 19 reconstructed for QDs prepared at 500 C [Fig. 5 and Fig. 6(c)]. Remarkably, only the smallest QD in Fig. 5(b) is completely 19 19 reconstructed whereas for the larger QDs this reconstruction exists only near to the wetting layer. For the assumption of a temperature gradient across the QD its size is certainly too small. However, it may also be connected with a reduced ux of In arriving from the wetting layer by diffusion at the top. A high-resolution STM image of the facet 6 of the 500 C QD in Fig. 5 is shown in Fig. 6(d). The facet is inclined to the substrate by 27 2 . The lengths of the unitcell vectors and the angle between them are w1 = 0.87 0.03 nm, w2 = 0.93 0.04 nm, and 119 8 , re-

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FIG. 5. 3D STM images of InAs QDs grown at 500 C (V = 3 V, I = 0.1 nA). The size at the base along 111 is noted.

spectively. (Geometric values: 28, w1 = 0.93 0.86 nm, w2 = 0.95 0.89 nm, 110) Thus, the facet 6 is identied as B and correspondingly the facet 5 as B. This is 143 413 B may be a stable surface on an the rst indication that 134 InAs QD. The areas 4 in Figs. 4 and 5 do not exhibit any ordered surface structure (not shown here in detail) but are rounded as obvious from both gures. From pure geometrical consid erations, the rounded area should consist of 001 and its B by 35. The area vicinals which are inclined to 112 4lying opposite to Bis disordered for the QDs on 111 nearly all high-index surfaces we have studied. The reason for this is not clear yet and is hoped to be given by future simulations of the QD growth. Finally, a schematic drawing of the QD shape is depicted in Fig. 6(e). The QD exhibits the 110 plane normal to the substrate as the only plane of (mirror) symmetry. This demonstrates perfect epitaxial growth as it sustains the symmetry of the substrate surface. A large part of the QD is terminated by the facets tilted to the substrate by up to 30, i.e., the QD is a rather at entity in line with our earlier results on different substrates.6
D. Observation of lattice defects in InAs quantum dots on GaAs112B

1 appearing on a 01 facet is shown in Fig. 7(a). Rows of bright humps that correspond to As dangling bonds of the typical Ga-As zigzag rows run along 011 . In the upper and the right-hand side of Fig. 7(a) areas are marked by arrowheads, in which the rows are shifted aside along [100] by about 2 / 3 row spacings. Quite obviously, the observed defects are stacking faults in {111} planes. The stacking-faults penetrate the QD perfectly along 111 and 111 planes, respectively, i.e., establish area defects. In addition, another lattice defect is seen in the lower side of the gure marked by a large arrowhead: An additional single step emerges near the crossing point of the two stacking faults. Thus, the defect is a screw dislocation. The screw dislocation penetrates the 1 QDs along 01 establishing a line defect. The same lattice defects have been observed on the InAs QDs grown on GaAs B recently, and have been discussed in detail pre135 senting atomic structure models.11 A similar lattice defect is observed on the B-2 2 facet, as shown in Fig. 7(b) 111 where an additional single step emerges near the middle of the facet as marked by an arrowhead. Thus, the defect is a screw dislocation again, but the screw dislocation penetrates 1 the QD along in this case, instead of along 01 . It is 111 noted that the squarelike unit cell, marked by dotted lines in the right-hand side of Fig. 7(b), is related to an out-of-phase boundary of the B-2 2 reconstruction (see also Fig. 111 1(b) in Ref. 28), and is not related to any lattice defect penetrating the bulk crystal.

Interestingly, about 50%, 20%, and 0% of the observed QDs, grown at 435 C, 470 C, and 500 C, respectively, exhibit lattice defects observable on the bounding facets by STM. A high-resolution STM image of such a lattice defect

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FIG. 6. High-resolution STM images of (a) facet 1, (b),(c) facet 3 and (d) facet 6 (V = 3 V, I = 0.1 nA). (e) A schematic drawing of the 3D shape of the QD.

1 FIG. 7. High-resolution STM images of lattice defects on (a) 01 and (b) B facets (V = 3 V, I = 0.1 nA). The sizes of the images are (a) 30 111 30 nm2 and (b) 13 13 nm2.

The unexpected variation of the QD ensembles when the temperature changes from 435 C to 470 C as reported in Figs. 2 and 3 can be explained by the lattice defects of the QDs. As the temperature increases, many QDs change from a disordered to the well ordered coherent state, i.e., during growth at the higher temperature most defects can heal out already during growth. The coherent QDs are strained and hence the size distribution becomes sharper. Moreover, when the number of incoherent QDs decreases, many coherent QDs do not have incoherent QDs in their neighborhood, and therefore are not incorporated into the incoherent QD during the anticipated ripening process. Hence, the number density stays high, instead of being reduced. Broad size distribution and occurrence of lattice defects are experimentally correlated here again.
E. InAs wetting layer on GaAs112B

The wetting layer is very important for the QD growth since it is the template for the diffusion of the incoming In atoms and As2 molecules to the growing QDs. The STM

images in Fig. 8 show the morphology and structure of the wetting layer on the GaAs B substrate. Many at ter112 races can be seen in Fig. 8(a). The terraces are not very wide and are frequently interrupted by steps. This gives rise to the undulated morphology, as shown in Fig. 2. An enlarged STM image in Fig. 8(b) shows the surface structure on a terrace. Although it is difcult to recognize the exact unit cell, rows of bright humps are seen which can be connected by lines at a given separation x = 0.98 0.06 nm, in accordance with the periodicity length along 111 of 1.05 0.98 nm at a InAs GaAs B surface. Moreover, at the side wall of step 112 315 bunches along 312 , the B facets form. Thus, the structure of the wetting layer is exactly the same to that of the at base on the InAs QDs grown on the GaAs B.17 The 113 B surface has been discovered recently; it is facGaAs 135 etted into vicinal B surfaces for the bare surface, but 2511 becomes at by deposition of a small amount of InAs, accompanied by a c 2 2 reconstruction.12

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increase, but the size distribution drastically becomes sharp, and the number density increases. This phenomenon is attributed to lattice defects incorporated in the QDs at the lower growth temperature. A wide size distribution is correlated here again with incorporation of lattice defects. The wetting layer is not at but undulated on a submicrometer scale and reects the structure of the bare substrate surface. The atomic structure of the wetting layer is exactly the same to that of the at base of InAs QDs grown on the GaAs B substrate. 113
ACKNOWLEDGMENTS

The authors thank G. Ertl for support and P. Geng and M. Richard for technical assistance.
L. Geelhaar, J. Mrquez, P. Kratzer, and K. Jacobi, Phys. Rev. Lett. 86, 3815 (2001). 2 L. Geelhaar, Y. Temko, J. Mrquez, P. Kratzer, and K. Jacobi, Phys. Rev. B 65, 155308 (2002). 3 K. Jacobi, L. Geelhaar, and J. Mrquez, Appl. Phys. A: Mater. Sci. Process. 75, 113 (2002). 4 Y. Temko, L. Geelhaar, T. Suzuki, and K. Jacobi, Surf. Sci. 513, 328 (2002). 5 J. Mrquez, L. Geelhaar, and K. Jacobi, Appl. Phys. Lett. 78, 2309 (2001). 6 K. Jacobi, Prog. Surf. Sci. 71, 185 (2003). 7 Y. Temko, T. Suzuki, and K. Jacobi, Appl. Phys. Lett. 82, 2142 (2003). 8 Y. Temko, T. Suzuki, P. Kratzer, and K. Jacobi, Phys. Rev. B 68, 165310 (2003). 9 Z. M. Wang, H. Wen, V. R. Yazdanpanah, J. L. Shultz, and G. J. Salamo, Appl. Phys. Lett. 82, 1688 (2003). 10 M. C. Xu, Y. Temko, T. Suzuki, and K. Jacobi, Appl. Phys. Lett. 84, 2283 (2004). 11 T. Suzuki, Y. Temko, M. C. Xu, and K. Jacobi, Phys. Rev. B 69, 235302 (2004). 12 T. Suzuki, Y. Temko, M. C. Xu, and K. Jacobi, Surf. Sci. 548, 333 (2004). 13 T. Suzuki, Y. Temko, and K. Jacobi, Appl. Phys. Lett. 80, 4744 (2002). 14 T. Suzuki, Y. Temko, and K. Jacobi, Phys. Rev. B 67, 045315 (2003). 15 Y. Temko, T. Suzuki, M. C. Xu, and K. Jacobi, Appl. Phys. Lett. 83, 3680 (2003). 16 S. P. Guo, H. Ohno, A. Shen, F. Matsukura, and Y. Ohno, Appl. Phys. Lett. 70, 2738 (1997). 17 S. C. Fortina, S. Sanguinetti, E. Grilli, M. Guzzi, M. Henini, A. Polimeni, and L. Eaves, J. Cryst. Growth 187, 126 (1998). 18 J. S. Lee, S. Sugou, and Y. Masumoto, J. Cryst. Growth 205, 467 (1999). 19 H. Yasuda, F. Matsukura, Y. Ohno, and H. Ohne, Appl. Surf. Sci. 166, 413 (2000). 20 J. Platen, C. Setzer, P. Geng, W. Ranke, and K. Jacobi, Microelectron. J. 28, 969 (1997). 21 L. Geelhaar, J. Mrquez, K. Jacobi, A. Kley, P. Ruggerone, and M. Schefer, Microelectron. J. 30, 393 (1999). 22 J. Platen, A. Kley, C. Setzer, K. Jacobi, P. Ruggerone, and M. Schefer, J. Appl. Phys. 85, 3597 (1999). 23 K. Jacobi et al., Surf. Sci. 59, 439 (1999). 24 T. Suzuki, Y. Temko, M. C. Xu, and K. Jacobi, Surf. Sci.(in press). 25 P. Geng, J. Mrquez, L. Geelhaar, J. Platen, C. Setzer, and K. Jacobi, Rev. Sci. Instrum. 71, 504 (2000). 26 See, e.g., H. Lee, R. Lowe-Webb, W. Yang, and P. C. Sercel, Appl. Phys. Lett. 72, 812 (1998). 27 M. Meixner, E. Schll, V. A. Shchukin, and D. Bimberg, Phys. Rev. Lett. 87, 236101 (2001). 28 D. K. Biegelsen, R. D. Bringans, J. E. Northrup, and L.-E. Swartz, Phys. Rev. Lett. 65, 452 (1990). 29 M. C. Thornton, D. A. Woolf, and P. Weightman, Appl. Surf. Sci. 123/ 124, 115 (1998).
1

FIG. 8. STM images of the wetting layer (V = 3 V, I = 0.1 nA). The sizes of the images are (a) 100 100 nm2 and (b) 27 27 nm2.

IV. CONCLUSIONS

Shape and size distribution of the InAs QDs grown on the GaAs B by MBE were investigated using in situ 112 STM. The shape of the QDs is given by {110}, B, and 111 B bounding facets and a rounded vicinal 001 region. 143 The QDs exhibit the 110 plane normal to the substrate as the only plane of (mirror) symmetry. This demonstrates perfect epitaxial growth as it mirrors the symmetry of the substrate surface. A large part of the QD is terminated by facets tilted to the substrate by up to 30: The QDs are rather at entities. This is the rst indication that B may be a 134 stable surface on the InAs QDs. The QDs show an unexpected behavior for growth temperatures changing between 435 C and 470 C. As growth temperature increases, the size of the QDs does not simply

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