Effects of the Thickness of GaAs Spacer Layers on the Structure of Multi Layer

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Effects of the thickness of GaAs spacer layers on the structure of multilayerstacked InAs quantum dots

Hyung Seok Kim

, Ju Hyung Suh

, Chan Gyung Park

, Sang Jun Lee

, Sam Kyu Noh

, Jin Dong Song

,Yong Ju Park

, Won Jun Choi

, Jung Il Lee

Department of Materials Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, Kyungbuk 790-784, Republic of Korea

Quantum Dot Technology Laboratory, Korea Research Institute of Standards and Science (KRISS), Daejeon 305-600, Republic of Korea

Nano Device Research Center, Korea Institute of Science and Technology (KIST), Seoul 136-791, Republic of Korea

a r t i c l e i n f o

Article history:

Received 13 September 2005Received in revised form13 October 2008Accepted 20 October 2008Communicated by K.H. PloogAvailable online 1 November 2008

PACS:

68.37.Lp68.43.Hn68.55.Jk68.65.Hb

Keywords:

A1. Microstructure characterizationA1. Quantum dotsA1. Transmission electron microscopy(TEM)B1. Multilayer InAs/GaAs

a b s t r a c t

The effects of the thickness of GaAs spacer layers on the structure of multilayer stacked InAs quantumdots (QDs) grown by molecular-beam epitaxy were studied using transmission electron microscopy. Toinvestigate QD structure depending on spacer layer growth, first uncapped free-standing QDs weregrown and their structure compared with that of multilayer stacked QDs. In addition, verticallynonaligned and aligned stacked QDs were grown by adjusting the thickness of GaAs spacer layers. Theuncapped QDs were found to form a lens-shaped structure with side facets. Upon capping with a GaAsspacer, the apexof nonaligned QDs flattened by In diffusion. However, the aligned QDs maintained theirlens-shaped structure with round apex after capping. It is believed that their apex did not flattenbecause the chemical potential gradient of In was relatively low due to the adjacent InAs QD layers. Theresults demonstrate the possibility of controlling QD structure by adjusting the thickness of spacerlayers.

2008 Published by Elsevier B.V.

1. Introduction

Recently self-assembled heteroepitaxial quantum dots (QDs)have been grown in Stranski-Krastanow mode[1]and consider-able effort has been devoted to fabricating laser devices[2],photodetectors[3]and advanced memory[4]by using self- assembled QDs. To understand and control the optoelectronicproperties of QD devices, the shape and size of QDs have to bemeasured exactly because their optoelectronic properties aresigniﬁcantly dependent on their structural properties such asshape, size, uniformity and density. In addition, the study of thedetailed structure of QDs provides new insight into understandingthe growth characteristics of QDs and controlling their growthparameters.There are many important growth parameters such as growthtemperature, deposition rate, growth interruption and the growthcondition of cap layers, which affect the QD structures and theiroptoelectronic properties. In particular, the growth procedure of acap layer plays a crucial role in determining QD structure andvarious QD shapes, depending on cap layer growth have beenreported including truncation[5], ride-valley transition[6]and dissolution of QDs[7]. Typical analysis of the effect of cap layergrowth on the QD structure was performed using atomic forcemicroscopy (AFM) in uncapped or partially capped QDs andshowed an important material redistribution during cap layergrowth[8,9]. However, the AFM investigation is not capable of resolving QD structure owing to the well-known tip convolutioneffect, and it is impossible to investigate the structure of fullycapped QDs. Transmission electron microscopy (TEM) is a uniqueanalysis technique for investigating QD structures capped with anoverlayer and atomic scale analyses are also possible by high-resolution electron microscopy (HREM).In the present study, multilayer stacked InAs QDs were grownon GaAs by molecular-beam epitaxy (MBE) and their structuralproperties were investigated by ﬁeld emission gun-TEM (FEG-TEM)and high-voltage electron microscopy (HVEM) depending on thethickness of spacer cap layers. The uncapped QDs were found to

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Contents lists available atScienceDirectjournal homepage:www.elsevier.com/locate/jcrysgro

Journal of Crystal Growth

0022-0248/$-see front matter

2008 Published by Elsevier B.V.doi:10.1016/j.jcrysgro.2008.10.054

Corresponding author. Tel.: +82542792139; fax: +82542792399.

E-mail addresses:

kuku@postech.ac.kr (H.S. Kim).cgpark@postech.ac.kr (C.G. Park). Journal of Crystal Growth 311 (2009) 258–262

form a lens-shaped structure with side facets. In addition,vertically nonaligned and aligned stacked QDs were grown byadjusting the thickness of GaAs spacer layers. Upon capping byGaAs, the apex of nonaligned QDs ﬂattened by In diffusionalthough the aligned QDs maintained their lens-shaped structurewith round apex.

2. Experimental procedure

The InAs QDs were grown on semi-insulating GaAs(001)substrates using the MBE system (RIBER32P). In order toinvestigate the effects of GaAs spacer growth on the QD structure,uncapped QDs were grown and their structures were investigatedby AFM and HREM. In addition, two different samples, onevertically aligned and the other nonaligned along the growthdirection, were grown by varying the thickness of GaAs spacerlayers.Fig. 1shows the schematic diagram of ﬁve-period stackedInAs/GaAs QDs heterostructures. The GaAs buffer layer with athickness of 250nm was deposited on the substrate at 560

C. TheInAs QDs with an equivalent thickness of 2.5 monolayers (ML)were formed and GaAs overlayers were deposited at 480

C. Forthe growth of vertically nonaligned and aligned QDs, 49 and 9nmthick GaAs spacers were deposited, respectively. The growth of InAs QDs and GaAs spacers was repeated five times with growthrates of 1.4 and 12.4nm/min, respectively.The structural properties of QDs were studied using AFM(Dimension 3100, Digital Instruments) in tapping mode and200kV HR-TEM (JEM-2010F, JEOL). In addition, scanning-TEM(STEM; JEM2100F, JEOL) with energy dispersive X-ray spectro-scopy (EDS) and 1.25MV HVEM (JEM-ARM1300S, JEOL) locatedat the Korea Basic Science Institute (KBSI) were used for theobservation of QD structures on an atomic-length scale. TEMinvestigations were performed by conventional bright field (BF)TEM and HREM techniques. TEM images were recorded on animage plateand their resolutionwas improvedenough tomeasureQD size using digital intensity profiling through fast Fouriertransformation (FFT) and the inverse FFT processes.

3. Results and discussion

Fig. 2(a) shows an AFM height image of uncapped InAs QDsmeasured in tapping mode. The QDs were lens-shaped and theiraverage height and diameter were 3.5 and 35nm, respectively.The QDs were distributed randomly and had a tendency to growtogether in twos or threes. The QDs density was 7.7

.Fig. 2(b) is an AFM height proﬁle of single QD indicated in theFig. 2(a) by the dotted line A–B. The section proﬁle shows that theQD has symmetrical dimensions and QD height and diameterwere measured as 3.75 and 36nm, hence the aspect ratio wasabout 0.1.However, the cross-sectional HREM of uncapped QDs revealedthat the lateral dimension measured by AFM was enlarged byabouttwotimes although the QDs height byAFM nearlycoincidedwith the result by TEM.Fig. 2(c) shows the HREM image of uncapped QD on [110] zone. The QD height and the diameterof base were measured as

4.2 and

18.5nm, respectively, andhence the aspect ratio was 0.23 which is more than twice as largeas the result by AFM. The resolution of AFM is limited by thesharpness and shape of the tip whose normal radius of curvatureis 20–60nm[10]. In particular, lateral resolution is much moredependent on the dimension of the tip than vertical resolution innanometer-sized samples because of the measuring geometrybetween the tip and sample[11]. Considering the QD structure byTEM, it is believed that the lateral dimension of QDs measured byAFM is not reliable although their vertical dimension by AFM isreasonable. The HREM also shows that the QDs are coherentislands without any defects such as dislocations or stacking faults.The uncapped QDs were lens-shaped with side facets whosewetting angles were about 26

. The phenomenon of equilibriumfaceting plays a crucial role in determining the QD shape[12]. Thefacets with high Miller indices such as (136), (137), (125) and(2511) were reported in many studies using scanning tunnelingmicroscopy, AFM and reﬂection high-energy electron diffraction.The facet angle was measured as 23–28

and the main facet anglewas 26

which coincides with the (137) facet[12].We have investigated the structure of uncapped InAs QDsbefore GaAs spacer growth. However, the QDs have to be coveredwith a cap layer which is needed for the passivation of the QDsfor device application. In addition, multilayer stacked QDs arerequired to increase the QD density and the optoelectronicefficiency of QD devices[13]. In the present study, therefore,five-period stacked QD structures were grown with varying thethickness of spacer layers, after which the effects of GaAs spaceroverlayer on the QD structures were investigated.Fig. 3shows a cross-sectional TEM BF image of five-periodstacked InAs QDs with 49nm thick GaAs spacer layers and the[110] zone HREM image (b). The five-period stacked QDs weresuccessively grown and randomly distributed along the growthdirection. A lens-shaped very dark contrast was observed on andbeneath the wetting layers under the

004

two beam condition.The InAs/GaAs heteroepitaxy has a 7.2% lattice misfit and themisfit strain induces a dark contrast in TEM observations usingphase contrast as well as diffraction contrast. The QD height anddiameter were measured as 3.5–4.5 and 15–20nm, respectively.In particular, the BF and HREM images show that QD apexesflattened after capping with a spacer layer. The effects of elasticenergy and surface energy can explain the QD apex flattening[6,14]. The increase of the elastic energy and surface energy of InAs QDs by depositing a GaAs overlayer induces the diffusion of In from the QDs[14]. Therefore, QD apex flattening is possible duetothe In diffusion induced by the compressive strain from GaAs toQDs and the chemical potential gradient of In during overlayergrowth at high temperature. The QD height and base diameterwere measured as

4.6 and

23.2nm in the HREM. However,exact determination of the shape and size of capped QDs wasdifﬁcult because of the indistinct boundary between InAs andGaAs as shown inFig. 3(b). In the BF image under dynamical twobeam and the HREM on-zone axis multi beam conditions, thediffraction contrast image of QDs can be observed largely by strain

ARTICLE IN PRESS

Fig. 1.

Schematic diagram of ﬁve-period stacked InAs QDs grown on GaAs.

H.S. Kim et al. / Journal of Crystal Growth 311 (2009) 258–262

259

ARTICLE IN PRESS

Fig. 2.

AFM height image of a free-standing uncapped InAs QDs in tapping mode (a), section height proﬁle indicated by dotted line A–B in (a), and a [110] zone cross-sectional HREM image of a single QD showing lens-shaped structure.

Fig. 3.

Cross-sectional BF image of ﬁve-period stacked InAs QDs with 49nm thick GaAs spacers in

004

two beam condition (a) and the [110] HREM image of the QDshowing ﬂat QD apex (b).

Fig. 4.

Annular dark ﬁeld (ADF) STEM image of capped QD with FFT pattern (a) and EDS line-scan proﬁle for In along the denoted line in the ADF image (b).

H.S. Kim et al. / Journal of Crystal Growth 311 (2009) 258–262

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