A. M. Munshi

Position-Controlled Uniform GaAs Nanowires on Silicon using Nanoimprint Lithography

We report on the epitaxial growth of large-area position-controlled self-catalyzed GaAs nanowires (NWs) directly on Si by molecular beam epitaxy (MBE). Nanohole patterns are defined in a SiO2 mask on 2 in. Si wafers using nanoimprint lithography (NIL) for the growth of positioned GaAs NWs. To optimize the yield of vertical NWs the MBE growth parameter space is tuned, including Ga predeposition time, Ga and As fluxes, growth temperature, and annealing treatment prior to NW growth. In addition, a non-negligible radial growth is observed with increasing growth time and is found to be independent of the As species (i.e., As2 or As4) and the growth temperatures studied. Cross-sectional transmission electron microscopy analysis of the GaAs NW/Si substrate heterointerface reveals an epitaxial growth where NW base fills the oxide hole opening and eventually extends over the oxide mask. These findings have important implications for NW-based device designs with axial and radial p-n junctions. Finally, NIL positioned GaAs/AlGaAs core-shell heterostructured NWs are grown on Si to study the optical properties of the NWs. Room-temperature photoluminescence spectroscopy of ensembles of as-grown core-shell NWs reveals uniform and high optical quality, as required for the subsequent device applications. The combination of NIL and MBE thereby demonstrates the successful heterogeneous integration of highly uniform GaAs NWs on Si, important for fabricating high throughput, large-area position-controlled NW arrays for various optoelectronic device applications.

Controlling crystal phases in GaAs nanowires grown by Au-assisted molecular beam epitaxy.

Control of the crystal phases of GaAs nanowires (NWs) is essential to eliminate the formation of stacking faults which deteriorate the optical and electronic properties of the NWs. In addition, the ability to control the crystal phase of NWs provides an opportunity to engineer the band gap without changing the crystal material. We show that the crystal phase of GaAs NWs grown on GaAs(111)B substrates by molecular beam epitaxy using the Au-assisted vapor-liquid-solid growth mechanism can be tuned between wurtzite (WZ) and zinc blende (ZB) by changing the V/III flux ratio. As an example we demonstrate the realization of WZ GaAs NWs with a ZB GaAs insert that has been grown without changing the substrate temperature.

Compositional characterization of GaAs/GaAsSb nanowires by quantitative HAADF-STEM.

The Sb concentration in axial GaAs(1-x)Sb(x) inserts of otherwise pure GaAs nanowires has been investigated with quantitative high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). The Sb concentration was quantified by comparing the experimental image intensities normalized to the incident beam intensity with intensities simulated with a frozen lattice multislice approach. Including static atomic displacements in the simulations was found to be crucial for correct compositional analysis of GaAs(1-x)Sb(x). HAADF intensities of individual nanowires were analysed both across the nanowires, exploiting their hexagonal cross-sectional shape, and along the evenly thick central part of the nanowires. From the cross-sectional intensity profiles, a decrease in the Sb concentration towards the nanowire outer surfaces was found. The longitudinal intensity profiles revealed a gradual build-up of Sb in the insert. The decrease of the Sb concentration towards the upper interface was either gradual or abrupt, depending on the growth routine chosen. The compositional analysis with quantitative HAADF-STEM was verified by energy dispersive X-ray spectroscopy.

Compositional analysis of GaAs/AlGaAs heterostructures using quantitative scanning transmission electron microscopy

We demonstrate a method for compositional mapping of AlxGa1–xAs heterostructures with high accuracy and unit cell spatial resolution using quantitative high angle annular dark field scanning transmission electron microscopy. The method is low dose relative to spectroscopic methods and insensitive to the effective source size and higher order lens aberrations. We apply the method to study the spatial variation in Al concentration in cross-sectioned GaAs/AlGaAs core-shell nanowires and quantify the concentration in the Al-rich radial band and the AlGaAs shell segments.

Near-surface depletion of antimony during the growth of GaAsSb and GaAs/GaAsSb nanowires

The near-surface reduction of the Sb mole fraction during the growth of GaAsSb nanowires (NWs) and GaAs NWs with GaAsSb inserts has been studied using quantitative high-angle annular dark field scanning transmission electron microscopy (STEM). A model for diffusion of Sb in the hexagonal NWs was developed and employed in combination with the quantitative STEM analysis. GaAsSb NWs grown by Ga-assisted molecular beam epitaxy (MBE) and GaAs/GaAsSb NWs grown by Ga- and Au-assisted MBE were investigated. At the high temperatures employed in the NW growth, As-Sb exchange at and outward diffusion of Sb towards the surface take place, resulting in reduction of the Sb concentration at and near the surface in the GaAsSb NWs and the GaAsSb inserts. In GaAsSb NWs, an increasing near-surface depletion of Sb was observed towards the bottom of the NW due to longer exposure to the As beam flux. In GaAsSb inserts, an increasing change in the Sb concentration profile was observed with increasing post-insert axial GaAs grow...

Effect of V/III ratio on the structural and optical properties of self-catalysed GaAs nanowires

The performance of GaAs nanowire (NW) devices depends critically on the presence of crystallographic defects in the NWs such as twinning planes and stacking faults, and considerable effort has been devoted to understanding and preventing the occurrence of these. For self-catalysed GaAs NWs grown by molecular beam epitaxy (MBE) in particular, there are in addition other types of defects that may be just as important for NW-based optoelectronic devices. These are the point defects such as the As vacancy and the Ga antisite occurring due to the inherently Ga-rich conditions of the self-catalysed growth. Here we demonstrate experimentally the effects of these point defects on the optical properties of GaAs/AlGaAs core-shell NWs grown by self-catalysed MBE. The present results enable insight into the role of the point defects both on their own and in conjunction with crystallographic planar defects.

In situ electronic probing of semiconducting nanowires in an electron microscope

For the development of electronic nanoscale structures, feedback on its electronic properties is crucial, but challenging. Here, we present a comparison of various in situ methods for electronically probing single, p‐doped GaAs nanowires inside a scanning electron microscope. The methods used include (i) directly probing individual as‐grown nanowires with a sharp nano‐manipulator, (ii) contacting dispersed nanowires with two metal contacts and (iii) contacting dispersed nanowires with four metal contacts. For the last two cases, we compare the results obtained using conventional ex situ litho‐graphy contacting techniques and by in situ, direct‐write electron beam induced deposition of a metal (Pt). The comparison shows that 2‐probe measurements gives consistent results also with contacts made by electron beam induced deposition, but that for 4‐probe, stray deposition can be a problem for shorter nanowires. This comparative study demonstrates that the preferred in situ method depends on the required throughput and reliability.

In-situ electrical and structural characterization of individual GaAs nanowires

A method for probing the electrical and structural characteristics of individual as-grown III-V nanowires was studied. In-situ electrical characterization was performed in a focused ion beam / scanning electron microscopy system by using a fine nano-manipulator and ion beam assisted deposition. Transmission electron microscopy specimens of probed nanowires are prepared afterwards. This method would potentially allow the correlation of electrical and structural characteristics (e.g. crystal faults such as twinning) of the nanowire-substrate system. The challenge is in contacting the nanowires so that the electrical characteristics of the nanowire-substrate system can be extracted correctly.

Determination of GaAs zinc blende/wurtzite band offsets utilizing GaAs nanowires with an axial GaAsSb insert

By applying a correlated micro-photoluminescence spectroscopy and transmission electron microscopy (TEM) approach, we have utilized molecular beam epitaxy grown self-catalysed GaAs nanowires (NWs) with an axial GaAsSb insert to determine the band offsets at the crystal phase heterojunction between zinc blende (ZB) and wurtzite (WZ) GaAs. Two distinct PL emission bands originating from the ZB GaAsSb insert were identified. The lower energy PL emission allowed an independent verification of the maximum Sb molar fraction to be ∼30%, in agreement with quantitative high-angle annular dark field scanning TEM performed on the same single NW. The higher energy PL emission revealed a low temperature ZB/WZ band offset of 120 meV at the interface between the two GaAs crystal phases occurring at the upper boundary of the insert. Separate conduction and valence band offsets develop at a higher temperature due to the different temperature dependence of the ZB and WZ GaAs band gaps, but both offset values show a relativ...

Radial composition variations in the shells of GaAs/AlGaAs core-shell nanowires

GaAs nanowires (NWs) are seen as promising building blocks for future optoelectronic devices. To ensure reproducible properties, a high NW uniformity is required. Here, a substantial number of both position-controlled and randomly grown self-catalyzed GaAs/AlGaAs core-shell NWs are compared. Single NWs are characterized by correlated microphotoluminescence (µ-PL) spectroscopy and transmission electron microscopy (TEM). TEM is done in the 〈110〉- and 〈112〉-projections, and on the 〈111〉-cross-section of the NWs. The position-control grown NWs showed a higher degree of uniformity in morphology. All NWs on both samples had a predominantly stacking fault free zinc blende structure, with a main optical response around the GaAs free exciton energy. However, NW-to-NW structural variations in the tip region and radial compositional variations in the shell are present in both samples. These structural features could be the origin of variations in the optical response just below and above the free exciton energy. This correlated study demonstrates that the observed distinct, sharp PL peaks in the 1.6 - 1.8 eV energy range present in several NWs, are possibly related to radial compositional variations in the AlGaAs shell rather than the structural defects in the tip region.