Self-assembling InAs and InP quantum dots for optoelectronic devices

Stranski–Krastanov growth in molecular beam epitaxy allows the preparation of self assembling InAs and InP quantum dots on GaAs and Ga_0.52In_0.48P buffer layers, respectively. InAs dots in GaAs prepared by slow growth rates and low temperature overgrowth provide intense photoluminescence at the technologically important wavelength of 1.3 μm at room temperature. Strain induced vertical alignment, size modification and material interdiffusion for stacked dot layers are studied. A blue shift of the ground state transition energy is observed for the slowly deposited stacked InAs dots. This is ascribed to enhanced strain driven intermixing in vertically aligned islands. For very small densely stacked InP and InAs dots the reduced confinement shift causes a red shift of the ground state emission. The InP quantum dots show intense and narrow photoluminescence at room temperature in the visible red spectral range. First InP/Ga_0.52In_0.48P quantum dot injection lasers are prepared using threefold stacked InP dots. We observe lasing at room temperature in the wavelength range between 690–705 nm depending on the size of the stacked InP dots.     

张应变GaAs层引入使InAs/InP量子点有序化排列的机理研究

采用ＬＰ－ＭＯＶＰＥ技术,在（００１）ＩｎＰ衬底上生长的ＩｎＡｓ／ＩｎＰ自组装量子点是无序的。为了解决这个问题,在ＩｎＰ衬底上先生长张应变的ＧａＡｓ层,然后再生长ＩｎＡｓ层,可得到有序化排列的量子点。本文对张应变ＧａＡｓ层引入使量子点有序化排列的机理进行了分析,为生长有序化、高密度,均匀性好自组装量子点提供了依据。     

Focused ion beam creation and templating of InAs and InAs/InP nanospikes

Ion beam irradiation has been examined as a method for creating nanoscale semiconductor pillar and cone structures, but has the drawback of inaccurate nanostructure placement. We report on a method for creating and templating nanoscale InAs spikes by focused ion beam (FIB) irradiation of both homoepitaxial InAs films and heteroepitaxial InAs on InP substrates. These 'nanospikes' are created as In droplets, formed due to FIB irradiation, act as etch masks for the underlying InAs. By pre-patterning the InAs to influence In droplet movement, nanospike locations on homoepitaxial InAs may be controlled with limited accuracy. Creating nanospikes using an InAs/InP heterostructure provides an additional measure of control over where the spikes form because nanospikes will not form on exposed regions of InP. This effect may be exploited to accurately control nanospike placement by pre-patterning an InAs/InP heterostructure to control the location of the InAs/InP interface. Using this heterostructure templating method it is possible to accurately place nanospikes into regular arrays that may be useful for a variety of applications.     

Mechanisms of molecular beam epitaxy growth in InAs/InP nanowire heterostructures

InAs/InP axial nanowire heterostructures were grown by the Au-assisted vapour-liquid-solid method in a gas source molecular beam epitaxy system. The nanowire crystal structure and morphology were investigated by transmission electron microscopy for various growth conditions (temperature, growth rate, V/III flux ratio). Growth mechanisms were inferred from the InAs and InP segment lengths as a function of the nanowire diameter. Short InAs segment lengths were found to grow by depletion of In from the Au particle as well as by direct impingement, while longer segments of InAs and InP grew by diffusive transport of adatoms from the nanowire sidewalls. The present study offers a way to control the lengths of InAs quantum dots embedded in InP barriers.     

Photovoltaic Laser-Power Converters Based on LPE-Grown InP(GaAs)/InP Heterostructures

We have studied the possibility of creating laser-power converters based on LPE-grown InP(GaAs)/InP heterostructures intended for wireless power transmission via a laser beam channel at wavelengths λ ≈ 1.06–1.2 μm.     

Determination of the strain generated in InAs/InP quantum wires: prediction of nucleation sites

The compositional distribution in a self-assembled InAs(P) quantum wire grown by molecular beam epitaxy on an InP(001) substrate has been determined by electron energy loss spectrum imaging. We have determined the strain and stress fields generated in and around this wire capped with a 5?nm InP layer by finite element calculations using as input the compositional map experimentally obtained. Preferential sites for nucleation of wires grown on the surface of this InP capping layer are predicted, based on chemical potential minimization, from the determined strain and stress fields on this surface. The determined preferential sites for wire nucleation agree with their experimentally measured locations. The method used in this paper, which combines electron energy loss spectroscopy, high-resolution Z contrast imaging, and elastic theory finite element calculations, is believed to be a valuable technique of wide applicability for predicting the preferential nucleation sites of epitaxial self-assembled nano-objects.     

Shape and size control of InAs/InP (113)B quantum dots by Sb deposition during the capping procedure

The role of Sb atoms present on the growth front during capping of InAs/InP (113)B quantum dots (QDs) is investigated by cross-sectional scanning tunnelling microscopy, atomic force microscopy, and photoluminescence spectroscopy. Direct capping of InAs QDs by InP results in partial disassembly of InAs QDs due to the As/P exchange occurring at the surface. However, when Sb atoms are supplied to the growth surface before InP capping layer overgrowth, the QDs preserve their uncapped shape, indicating that QD decomposition is suppressed. When GaAs(0.51)Sb(0.49) layers are deposited on the QDs, conformal growth is observed, despite the strain inhomogeneity existing at the growth front. This indicates that kinetics rather than the strain plays the major role during QD capping with Sb compounds. Thus Sb opens up a new way to control the shape of InAs QDs.     

Spatial carrier distribution in InP/GaAs type II quantum dots and quantum posts

We performed a detailed investigation of the structural and optical properties of multi-layers of InP/GaAs quantum dots, which present a type II interface arrangement. Transmission electronic microscopy analysis has revealed relatively large dots that coalesce forming so-called quantum posts when the GaAs layer between the InP layers is thin. We observed that the structural properties and morphology affect the resulting radiative lifetime of the carriers in our systems. The carrier lifetimes are relatively long, as expected for type II systems, as compared to those observed for single layer InP/GaAs quantum dots. The interface intermixing effect has been pointed out as a limiting factor for obtaining an effective spatial separation of electrons and holes in the case of single layer InP/GaAs quantum-dot samples. In the present case this effect seems to be less critical due to the particular carrier wavefunction distribution along the structures.     

Melting of Ni and Fe nanoparticles: a molecular dynamics study with application to carbon nanotube synthesis

Molecular dynamics simulations with many-body interatomic potentials are used to study melting of Ni and Fe nanoparticles with diameters that range between 2 and 12 nm. Two different embedded-atom method interatomic potentials are used for each element. The capability of each interatomic potential to model (i) size-dependent melting in nanoparticles and (ii) the bulk melting temperature of Ni or Fe is explored. In agreement with existing theory, molecular dynamics simulations show that the melting temperature of non-supported nanoparticles decreases with decreasing nanoparticle size, displaying a linear relationship with the inverse of nanoparticle diameter. However, molecular dynamics simulations using the interatomic potentials considered in this work provide a lower estimate than existing theory for the sensitivity of the melting temperature to nanoparticle size (slope of linear relationship). Molecular dynamics simulations demonstrate that melting is surface initiated and that a finite temperature range exists in which partial melting of the nanoparticle occurs. This observation is very important in the development of advanced vapor-liquid-solid models for catalyst-assisted single-walled carbon nanotube synthesis.     

Designing spatial correlation of quantum dots: towards self-assembled three-dimensional structures

Buried two-dimensional arrays of InP dots were used as a template for the lateral ordering of self-assembled quantum dots. The template strain field can laterally organize compressive (InAs) as well as tensile (GaP) self-assembled nanostructures in a highly ordered square lattice. High-resolution transmission electron microscopy measurements show that the InAs dots are vertically correlated to the InP template, while the GaP dots are vertically anti-correlated, nucleating in the position between two buried InP dots. Finite InP dot size effects are observed to originate InAs clustering but do not affect GaP dot nucleation. The possibility of bilayer formation with different vertical correlations suggests a new path for obtaining three-dimensional pseudocrystals.     

Remote p-doping of InAs nanowires

We report on remote p-type doping of InAs nanowires by a p-doped InP shell grown epitaxially on the core nanowire. This approach addresses the challenge of obtaining quantitative control of doping levels in nanowires grown by the vapor-liquid-solid (VLS) mechanism. Remote doping of III-V nanowires is demonstrated here with the InAs/InP system. It is especially challenging to make p-type InAs wires because of Fermi level pinning around 0.1 eV above the conduction band. We demonstrate that shielding with a p-doped InP shell compensates for the built-in potential and donates free holes to the InAs core. Moreover, the off-current in field-effect devices can be reduced up to 6 orders of magnitude. The effect of shielding critically depends on the thickness of the InP capping layer and the dopant concentration in the shell.     

Analytic bond-order potentials for modelling the growth of semiconductor thin films

Interatomic potentials for modelling the vapour phase growth of semiconductor thin films must be able to describe the breaking and making of covalent bonds in an efficient format so that molecular dynamics simulations of thousands or millions of atoms may be performed. We review the derivation of such potentials, focusing upon the emerging role of the bond-based analytic bond-order potential (BOP). The BOP is derived through systematic coarse graining from the electronic to the atomistic modelling hierarchies. In a first step, the density functional theory (DFT) electronic structure is simplified by introducing the tight-binding (TB) bond model whose parameters are determined directly from DFT results. In a second step, the electronic structure of the TB model is coarse grained through atom-centered moments and bond-centered interference paths, thereby deriving the analytic form of the interatomic BOP. The resultant σ and π bond orders quantify the concept of single, double, triple and conjugate bonds in hydrocarbon systems and lead to a good treatment of radical formation. We show that the analytic BOP is able to predict accurately structural energy differences in quantitative agreement with TB calculations. The current development of these potentials for simulating the growth of Si and GaAs thin films is discussed.     

Theoretical prediction on the local structure and transport properties of molten alkali chlorides by deep potentials

In this work,the local structure and transport properties of three typical alkali chlorides(LiCl,NaCl,and KCl)were investigated by our newly trained deep potentials(DPs).We extracted datasets from ab initio molecular dynamics(AIMD)calculations and used these to train and validate the DPs.Large-scale and long-time molecular dynamics simulations were performed over a wider range of temperatures than AIMD to confirm the reliability and generality of the DPs.We demonstrated that the generated DPs can serve as a powerful tool for simulating alkali chlorides;the DPs also provide results with accuracy that is comparable to that of AIMD and efficiency that is similar to that of empirical potentials.The partial radial distribution functions and angle distribution functions predicted using the DPs are in close agreement with those derived from AIMD.The estimated densities,self-diffusion coefficients,shear viscosities,and electrical conductivities also matched well with the AIMD and experimental data.This work provides confidence that DPs can be used to explore other systems,including mixtures of chlorides or entirely different salts.     

Site-controlled self-organization of InAs quantum dots

In situ site-control techniques for self-organized InAs quantum dots (QDs) have been developed using an electron beam (EB) and a scanning tunneling microscope (STM) probe combined with molecular beam epitaxy. In the in situ EB-assisted process, InAs dots are preferentially formed in shallow, sub-μm-size GaAs holes with the InAs supply. We find that the specific slope of a hole acts as a favorable site for dot formation. In the in situ STM probe-assisted process, the size and pitch of the holes are considerably reduced into nanoscale. InAs QDs are then self-organized only at the hole sites due to strain-induced selective nucleation. Using this process, two- and three-dimensional QD arrays are fabricated with nanometer precision.     

InAs/InP radial nanowire heterostructures as high electron mobility devices

Radial core/shell nanowires (NWs) represent an important class of one-dimensional (1D) systems with substantial potential for exploring fundamental materials electronic and photonic properties. Here, we report the rational design and synthesis of InAs/InP core/shell NW heterostructures with quantum-confined, high-mobility electron carriers. Transmission electron microscopy studies revealed single-crystal InAs cores with epitaxial InP shells 2-3 nm in thickness, and energy-dispersive X-ray spectroscopy analysis further confirmed the composition of the designed heterostructure. Room-temperature electrical measurements on InAs/InP NW field-effect transistors (NWFETs) showed significant improvement in the on-current and transconductance compared to InAs NWFETs fabricated in parallel, with a room-temperature electron mobility, 11,500 cm(2)/Vs, substantially higher than other synthesized 1D nanostructures. In addition, NWFET devices configured with integral high dielectric constant gate oxide and top-gate structure yielded scaled on-currents up to 3.2 mA/microm, which are larger than values reported for other n-channel FETs. The design and realization of high electron mobility InAs/InP NWs extends our toolbox of nanoscale building blocks and opens up opportunities for fundamental and applied studies of quantum coherent transport and high-speed, low-power nanoelectronic circuits.     

Engineering molecular mechanics: an efficient static high temperature molecular simulation technique

Inspired by the need for an efficient molecular simulation technique, we have developed engineering molecular mechanics (EMM) as an alternative molecular simulation technique to model high temperature (T>0?K) phenomena. EMM simulations are significantly more computationally efficient than conventional techniques such as molecular dynamics simulations. The advantage of EMM is achieved by converting the dynamic atomistic system at high temperature (T>0?K) into an equivalent static system. Fundamentals of the EMM methodology are derived using thermal expansion to modify the interatomic potential. Temperature dependent interatomic potentials are developed to account for the temperature effect. The efficiency of EMM simulations is demonstrated by simulating the temperature dependence of elastic constants of copper and nickel and the thermal stress developed in a confined copper system.     

Numerical simulation of electronic properties of coupled quantum dots on wetting layers

Self-assembled quantum dots are grown on wetting layers and frequently in an array-like assembly of many similar but not exactly equal dots. Nevertheless, most simulations disregard these structural conditions and restrict themselves to simulating a pure single quantum dot. For reasons of numerical efficiency we advocate the effective one-band Hamiltonian with energy-?and position-dependent effective mass approximation and a finite height hard-wall 3D confinement potential for computation of the energy levels of the electrons in the conduction band. Within this model we investigate the geometrical effects mentioned above on the electronic structure of a pyramidal InAs quantum dot embedded in a GaAs matrix. We find that the presence of a wetting layer may affect the electronic structure noticeably. Furthermore, we establish that, in spite of the large bandgap of the InAs/GaAs heterostructure, if the dots in a vertically aligned array are sufficiently close stacked there is considerable interaction between their eigenfunctions. Moreover, the eigenfunctions of such an array are quite sensitive to certain structural perturbations.