We calculate the Overhauser frequency shifts in semiconductor nanostructures resulting from the hyperfine interaction between nonequilibrium electronic spins and nuclear spins. The frequency shifts depend on the electronic local density of states and spin polarization as well as the electronic and nuclear spin relaxation mechanisms. Unlike previous calculations, our method accounts for the electron confinement in low dimensional semiconductor nanostructures, resulting in both nuclear spin polarizations and Overhauser shifts that are strongly dependent on position. Our results explain previously puzzling measurements of Overhauser shifts in an Al$_x$Ga$_{1-x}$As parabolic quantum well by showing the connection between the electron spin lifetime and the frequency shifts.
We investigate the dynamic nuclear polarization from the hyperfine interaction between nonequilibrium electronic spins and nuclear spins coupled to them in semiconductor nanostructures. We derive the time and position dependence of the induced nuclear spin polarization and dipolar magnetic fields. In GaAs/AlGaAs parabolic quantum wells the nuclear spin polarization can be as high as 80% and the induced nuclear magnetic fields can approach a few gauss with an associated nuclear resonance shift of the order of kHz when the electronic system is 100% spin polarized. These fields and shifts can be …
We derive interatomic potentials for zinc blende InAs, InP, GaAs and GaP semiconductors with possible applications in the realm of nanostructures. The potentials include bond stretching interaction between the nearest and next-nearest neighbors, a three body term and a long-range Coulomb interaction. The optimized potential parameters are obtained by (i) fitting to bulk phonon dispersions and elastic properties and (ii) constraining the parameter space to deliver well behaved potentials for the structural relaxation and vibrational properties of nanostructure clusters. The targets are thereby …
We propose an efficient reduced-order technique for electronic structure calculations of semiconductor nanostructures, suited for inclusion in full-band quantum transport simulators. The model is based on the linear combination of bulk bands obtained by the empirical pseudopotential method, combined with the use of problem-matched basis functions numerically generated from the singular value decomposition. The efficiency and accuracy of the proposed approach are demonstrated in the case of the dispersion relation of hole subbands in an unstrained GaN layer.
Excitonic contributions to absorption and photocurrent generation in semiconductor nanostructures are described theoretically and simulated numerically using steady-state non-equilibrium Green's function theory. In a first approach, the coherent interband polarization including Coulomb corrections is determined from a Bethe-Salpeter-type equation for the equal time interband single-particle charge carrier Green's function. The effects of excitonic absorption on photocurrent generation are considered on the same level of approximation via the derivation of the corresponding corrections to the e…
Anharmonicity of the inter-atomic potential is taken into account for the quantitative simulation of the conduction and valence band offsets for highly-strained semiconductor heterostructures. The anharmonicity leads to a weaker compressive hydrostatic strain than that obtained with the commonly used quasi-harmonic approximation of the Keating model. Inclusion of the anharmonicity in the simulation of strained InAs/GaAs nanostructures results in an improvement of the electron band offset computed on an atomistic level by up to 100 meV compared to experiment.
We present experimental coherent two-dimensional Fourier transform spectra of the exciton resonances in semiconductor quantum wells for a pulse sequence that isolates two-quantum coherences. By measuring the real part of the spectra, we can determine that the spectra are dominated by two quantum coherences due to many-body interactions, not bound biexcitons. Simulations performed using dynamics controlled truncation agree well with the experiments.
An extension of the original Overhauser effect to a more general nonequilibrium state was proposed by G. Feher, and demonstrated by Clark and Feher some forty years ago. It is suggested here that it might be possible to produce excess electron spin polarization by allowing the role of the nuclei to be played by other magnetic entities, such as paramagnetic impurities or adjacent magnetically ordered structures.
We propose a technique for achieving large improvements in carrier mobilities in 2- and 1-dimensional semiconductor nanostructures by modifying their dielectric environments. We show that by coating the nanostructures with high-$κ$ dielectrics, scattering from Coulombic impurities can be strongly damped. Though screening is also weakened, the damping of Coulombic scattering is much larger, and the resulting improvement in mobilities of carriers can be as much as an order of magnitude for thin 2D semiconductor membranes, and more for semiconductor nanowires.
The interpretation of the electronic kinetic processes in the quantum zero dimensional nanostructures is considered. The main mechanism of the processes is supposed to be the interaction of electrons with the optical phonons. An emphasis is put on the recently measured effect of the long-time photoluminescence of quantum dot samples, which is observed to occur after an illumination of the sample by a laser pulse. In addition to this, an attention is devoted to the possible origin of the optical effect of the blinking (intermittence) of the optical emission of certain quantum dot samples under …
We investigate the optical control possibilities of spin-valley qubit carried by single electrons localized in nanostructures of monolayer TMDs, including small quantum dots formed by lateral heterojunction and charged impurities. The quantum controls are discussed when the confinement induces valley hybridization and when the valley hybridization is absent. We show that the bulk valley and spin optical selection rules can be inherited in different forms in the two scenarios, both of which allow the definition of spin-valley qubit with desired optical controllability. We also investigate nucle…
The modification of acoustic phonons in semiconductor nanostructures embedded in a host crystal is investigated including corrections due to strain within continuum elasticity theory. Effective elastic constants are calculated employing {\em ab initio} density functional theory. For a spherical InAs quantum dot embedded in GaAs barrier material, the electron-phonon coupling is calculated. Its strength is shown to be suppressed compared to the assumption of bulk phonons.
The modeling of finite-extent semiconductor nanostructures that are embedded in a host material requires the numerical treatment of the boundary in a finite simulation domain. For the study of a self-assembled InAs dot embedded in GaAs, three kinds of boundary conditions are examined within the empirical tight-binding model: (i) the periodic boundary condition, (ii) raising the orbital energies of surface atoms, and (iii) raising the energies of dangling bonds at the surface. The periodic boundary condition requires a smooth boundary and consequently a larger GaAs buffer than the two nonperiod…
Effective conduction-band model for zincblende III-V semiconductors in the presence of strain: tuning the properties of bulk crystals and nanostructures
Highly polarized nuclear spins within a semiconductor quantum dot (QD) induce effective magnetic (Overhauser) fields of up to several Tesla acting on the electron spin or up to a few hundred mT for the hole spin. Recently this has been recognized as a resource for intrinsic control of QD-based spin quantum bits. However, only static long-lived Overhauser fields could be used. Here we demonstrate fast redirection on the microsecond time-scale of Overhauser fields of the order of 0.5 T experienced by a single electron spin in an optically pumped GaAs quantum dot. This has been achieved using ful…
An overview of recent studies on ferromagnetism in Cr- and Mn-based II-VI diluted magnetic semiconductors is presented emphasizing differences in underlying exchange mechanisms. Examples of manipulations with spin ordering by carrier density, dimensionality, light, and electric field are given.
We propose the 14-band $\mathbf k \cdot \mathbf p$ model to calculate spin-orbit splittings of the valence subbands in semiconductor quantum wells. The reduced symmetry of quantum well interfaces is incorporated by means of additional terms in the boundary conditions which mix the $Γ_{15}$ conduction and valence Bloch functions at the interfaces. It is demonstrated that the interface-induced effect makes the dominating contribution to the heavy-hole spin splitting. A simple analytical expression for the interface contribution is derived. In contrast to the 4$\times$4 effective Hamiltonian mode…
We review our theoretical investigation on the spin relaxation/dephasing in spin precession and spin diffusion/transport in semiconductor nanostructures based on the kinetic spin Bloch equation approach.
A short overview is given of recent advances in the field of nanosemiconductors, which are suitable as materials for spin polarized transport of charge carriers. On the basis of last theoretical and experimental achievements it is shown that development of diluted and wide forbidden zone semiconductors with controlled disorders as well as their molecular structures is the very prospective way for magnetic semiconductors preparation.
We find that spin-polarized ground states emerge in nanofacets which are self-organized on SiC (0001) surfaces. Our large-scale density-functional calculations reveal that the nanofacet formed by bunching of single bilayer steps generates peculiar carbon dangling bond states localized at but extended along step edges. The flat-band characteristics of those C states cause either ferromagnetic or anti-ferromagnetic chains on covalent semiconductors.
A multi-band effective-mass Hamiltonian is derived for lattice-matched semiconductor nanostructures in a slowly varying external magnetic field. The theory is derived from the first-principles magnetic-field coupling Hamiltonian of Pickard and Mauri, which is applicable to nonlocal norm-conserving pseudopotentials in the local density approximation to density functional theory. The pseudopotential of the nanostructure is treated as a perturbation of a bulk reference crystal, with linear and quadratic response terms included in k.p perturbation theory. The resulting Hamiltonian contains several…
The near field scanning optical microscopy (NSOM) is not only a tool for imaging of objects in the sub wavelength limit but also a prominent characteristic tool for understanding the intrinsic properties of the nanostructures. The effect of strong localized surface plasmon resonance absorption of excitation laser in the NSOM images for Au nanoparticles is observed. The role of electronic transitions from different native defect related energy states of AlGaN are also discussed in understanding the NSOM images for the semiconductor nanowire.
We have shown that bilinear conformal mapping can be used to transform 4-lead internally shunted EMR semiconductor-metal hybrid structures to galvanomagnetically equivalent externally shunted 4 lead structures. The latter are compatible with the fabrication of nanoscale EMR devices while the former are not. Mapped rectangular EMR van der Pauw plate exhibit very large EMR values in both macroscopic and nanoscopic form. We have also shown that the mapping procedure applied in the case of EMR will also be applicable to other generalized EXX structures.
We present a detailed microscopic study of quasi-ballistic transport in deep submicron semiconductor channels. In particular, we study the crossover between the diffusive and ballistic regimes of transport and identify signatures in the electrostatic response, electron density, and nonequilibrium electron distribution function that are due to ballistic and diffusive transport, respectively. Our theoretical and computational approach is based on the Boltzmann transport equation for a nondegenerate electron system, together with the Poisson equation, from which we obtain the nonequilibrium elect…
A general density-matrix formulation of quantum-transport phenomena in semiconductor nanostructures is presented. More specifically, contrary to the conventional single-particle correlation expansion, we shall investigate separately the effects of the adiabatic or Markov limit and of the reduction procedure. Our fully operatorial approach allows us to better identify the general properties of the scattering superoperators entering our effective quantum-transport theory at various description levels, e.g., N electrons-plus-quasiparticles, N electrons only, and single-particle picture. In additi…
We present a unified model of compound semiconductor growth based on kinetic Monte Carlo simulations in tandem with new experimental results that can describe and predict the mechanisms for the formation of various types of nanostructures observed during droplet epitaxy. The crucial features of the model include the explicit and independent representation of atoms with different species and the ability to treat solid and liquid phases independently. Using this model, we examine nanostructural evolution in droplet epitaxy. The model faithfully captures several of the experimentally observed str…
We present a theory of highly excited interacting carriers confined in a semiconductor nanostructure, incorporating Auger coupling between excited states with different number of excitations. The Coulomb matrix elements connecting exciton, bi-exciton and tri-exciton complexes are derived and an intuitive picture of breaking neutral multi-exction complexes into positively and negatively charged multi-exciton complexes is given. The general approach is illustrated by analyzing the coupling of biexciton and exciton in CdSe spherical nanocrystals. The electron and hole states are computed using at…
The structural inversion asymmetry-induced spin-orbit interaction of conduction band electrons in zinc-blende and wurtzite semiconductor structures is analysed allowing for a three-dimensional (3D) character of the external electric field and variation of the chemical composition. The interaction, taking into account all remote bands perturbatively, is presented with two contributions: a heterointerface term and a term caused by the external electric field. They have generally comparable strength and can be written in a unified manner only for 2D systems, where they can partially cancel each o…
The near-field Coulomb interaction between a nano-emitter and a graphene monolayer results in strong Förster-type resonant energy transfer and subsequent fluorescence quenching. Here, we investigate the distance dependence of the energy transfer rate from individual, i) zero-dimensional CdSe/CdS nanocrystals and ii) two-dimensional CdSe/CdS/ZnS nanoplatelets to a graphene monolayer. For increasing distances $d$, the energy transfer rate from individual nanocrystals to graphene decays as $1/d^4$. In contrast, the distance dependence of the energy transfer rate from a two-dimensional nanoplatele…
We present a theoretical analysis of the effect of dielectric confinement on the Coulomb interaction in dielectrically modulated quantum structures. We discuss the implications of the strong enhancement of the electron-hole and electron-electron coupling for two specific examples: (i) GaAs-based quantum wires with remote oxide barriers, where combined quantum and dielectric confinements are predicted to lead to room temperature exciton binding, and (ii) semiconductor quantum dots in colloidal environments, where the many-body ground states and the addition spectra are predicted to be drastical…
Theoretical prediction of phonon transport in modern semiconductor nanodevices requires atomic resolution of device features and quantum transport models covering coherent and incoherent effects. The nonequilibrium Green's function method (NEGF) is known to serve this purpose very well, but is numerically very expensive. This work extends the very efficient Büttiker probe concept to phonon NEGF and discusses all implications of this method. Büttiker probe parameters are presented that reproduce within NEGF experimental phonon conductances of Si and Ge between 10K and 1000K. Results of this met…
We present a theoretical approach to calculate the {\it local} absorption spectrum of excitons confined in a semiconductor nanostructure. Using the density-matrix formalism, we derive a microscopic expression for the non-local susceptibility, both in the linear and non-linear regimes, which includes a three-dimensional description of electronic quantum states and their Coulomb interaction. The knowledge of the non-local susceptibility allows us to calculate a properly defined local absorbed power, that depends on the electro-magnetic field distribution. We report on explicit calculations of th…
We account for lateral orderings of III-V nanostructures resulting from a GaAs/InAs/InGaAs/GaAs sequence grown on GaAs by metallorganic vapour phase epitaxy at two different temperatures. For both samples, the ordering is induced by the stress field of a periodic dislocation network (DN) shallowly buried and parallel to the surface. This DN is a grain boundary (GB) that forms, between a thinGaAs layer (onwhich growthwas performed) and aGaAs substrate joined together by wafer bonding, in order to accommodate a tilt and a twist between these two crystals; both these misorientations are imposed i…
Understanding the electronic structure of semiconductor nanostructures is not complete without a detailed description of their corresponding spin-related properties. Here we explore the response of the shell structure of InAs self-assembled quantum dots to magnetic fields oriented in several directions, allowing the mapping of the g-tensor modulus for the s and p shells. We found that the g-tensors for the s and p shells show a very different behavior. The s-state in being more localized allows the probing of the confining potential details by sweeping the magnetic field orientation from the g…
Vanadium is a transition metal with multiple oxidation states and V2O5 is the most stable form among them. Besides catalysis, chemical sensing and photo-chromatic applications, V2O5 is also reported to exhibit a semiconductor to metal transition (SMT) at a temperature range of 530-560K. Even though, there are debates in using the term 'SMT' for V2O5, the metallic behavior above transition temperature and its origin are of great interests in the scientific community. In this study, V2O5 nanostructures were deposited on SiO2/Si substrate by vapour transport method using Au as catalyst. Temperatu…
We have studied the influence of intrinsic and extrinsic defects in the magnetic and electrical transport properties of Co-doped ZnO thin films. X ray absorption measurements show that Co substitute Zn in the ZnO structure and it is in the 2+ oxidation state. Magnetization (M) measurements show that doped samples are mainly paramagnetic. From M vs. H loops measured at 5 K we found that the values of the orbital L and spin S numbers are between 1 and 1.3 for L and S = 3/2, in agreement with the representative values for isolated Co 2+. The obtained negative values of the Curie-Weiss temperature…
We first report a detailed transmission electron microscopy study of dislocation networks (DNs) formed at shallowly buried interfaces obtained by bonding two GaAs crystals between which we establish in a controlled manner a twist and a tilt around a k110l direction. For large enough twists, the DN consists of a twodimensional network of screw dislocations accommodating mainly the twist and of a one-dimensional network of mixed dislocations accommodating mainly the tilt. We show that in addition the mixed dislocations accommodate part of the twist and we observe and explain slight unexpected di…
Quadratic-response theory is shown to provide a conceptually simple but accurate approximation for the self-consistent one-electron potential of semiconductor nanostructures. Numerical examples are presented for GaAs/AlAs and InGaAs/InP (001) superlattices using the local-density approximation to density-functional theory and norm-conserving pseudopotentials without spin-orbit coupling. When the reference crystal is chosen to be the virtual-crystal average of the two bulk constituents, the absolute error in the quadratic-response potential for Gamma(15) valence electrons is about 2 meV for GaA…
Theoretical predictions have lead to the experimental synthesis of new low dimensional layered structures. Herein we show for the very first time that compounds of carbon monosulfide exhibit a great variety of layered nanostructures, such as chains arrays, monolayers, and thin films. We find that the chains arrays are the most stable because they are mainly dimensionality-driven by the $sp^2$ hybridization of sulfur and carbon orbitals. Furthermore, the chains arrays are direct gap semiconductors. In contrast to thin films, the monolayers are stable at room temperature with a semiconductor pha…
A blueprint for producing scalable digital graphene electronics has remained elusive. Current methods to produce semiconducting-metallic graphene networks all suffer from either stringent lithographic demands that prevent reproducibility, process-induced disorder in the graphene, or scalability issues. Using angle resolved photoemission, we have discovered a unique one dimensional metallic-semiconducting-metallic junction made entirely from graphene, and produced without chemical functionalization or finite size patterning. The junction is produced by taking advantage of the inherent, atomical…
Self-assembled, semimetallic ErSb single crystal nanostructures, grown by molecular beam epitaxy, are embedded within a semiconductor GaSb matrix. Formation, evolution and orientation of a variety of nanostructures, including spherical nanoparticles, elongated nanorods, octagonal shaped nanowires oriented along the surface normal and nanowires oriented in the growth plane, are controlled simply by the Er fraction. The plasmonic properties of the semimetal/semiconductor composites are characterized and quantified by three polarization-resolved spectroscopy techniques, spanning more than three o…
Understanding the electron dynamics and transport in metallic and semiconductor nanostructures -- such as metallic nanoparticles, thin films, quantum wells and quantum dots -- represents a considerable challenge for today's condensed matter physics, both fundamental and applied. In this review article, we will describe the collective electron dynamics in metallic and semiconductor nanostructures using different, but complementary, approaches. For small excitations (linear regime), the spectral properties can be investigated via quantum mean-field models of the TDLDA type (time-dependent local …
We have developed an unifying tight-binding Hamiltonian that can account for the electronic properties of recently proposed Si-based nanostructures, namely, Si graphene-like sheets and Si nanotubes. We considered the $sp^3s^*$ and $sp^{3}$ models up to first- and second-nearest neighbors, respectively. Our results show that the Si graphene-like sheets considered here are metals or zero-gap semiconductors, and that the corresponding Si nanotubes follow the so-called Hamada's rule [Phys. Rev. Lett. {\bf 68}, 1579 1992]. Comparison to a recent {\it ab initio} calculation is made.
We study experimentally and theoretically the temperature dependence of transverse magnetic routing of light emission from hybrid plasmonic-semiconductor quantum well structures where the exciton emission from the quantum well is routed into surface plasmon polaritons propagating along a nearby semiconductor-metal interface. In II-VI and III-V direct band semiconductors the magnitude of routing is governed by the circular polarization of exciton optical transitions, that is induced by a magnetic field. For structures comprising a (Cd,Mn)Te/(Cd,Mg)Te diluted magnetic semiconductor quantum well …
The quantitative composition of metal alloy nanowires on InSb(001) semiconductor surface and gold nanostructures on germanium surface is determined by blind source separation (BSS) machine learning (ML) method using non negative matrix factorization (NMF) from energy dispersive X-ray spectroscopy (EDX) spectrum image maps measured in a scanning electron microscope (SEM). The BSS method blindly decomposes the collected EDX spectrum image into three source components, which correspond directly to the X-ray signals coming from the supported metal nanostructures, bulk semiconductor signal and carb…
The long dreamed quantum internet would consist of a network of quantum nodes (solid-state or atomic systems) linked by flying qubits, naturally based on photons, travelling over long distances at the speed of light, with negligible decoherence. A key component is a light source, able to provide single or entangled photon pairs. Among the different platforms, semiconductor quantum dots are very attractive, as they can be integrated with other photonic and electronic components in miniaturized chips. In the early 1990s two approaches were developed to synthetize self-assembled epitaxial semicon…
Here, we demonstrate an approach that provides a precise control of the dimension of InAs from one-dimensional nanowires to wafer-scale free-standing two-dimensional nanosheets, which have a high degree of crystallinity and outstanding electrical and optical properties, using molecular-beam epitaxy by controlling catalyst alloy segregation. In our approach, two-dimensional InAs nanosheets can be obtained directly from one-dimensional InAs nanowires by silver-indium alloy segregation, which is much easier than all previously reported method, such as traditional buffering technique and select ar…
Spectroscopic data demonstrate that impurity D/A levels in doped semiconductor nanostructures are energetically pinned, resulting in variations in D/A binding energies with increasing quantum confinement. Using magnetic circular dichroism spectroscopy, the donor binding energies of Co2+ ions in colloidal ZnSe quantum dots have been measured as a function of quantum confinement and analyzed in conjunction with ab initio density functional theory calculations. The resulting experimental demonstration of pinned impurity levels in quantum dots has far-reaching implications for physical phenomena i…
Junction between metal, superconductor and semiconductor materials seems to be promising for their applications as the electronic devices, microelectronic devices and high power transmission. E-mail shpawar_phy@unishivaji.ac.in.
In a semiconductor heterostructure with type II energy band alignment, the spatial separation between electrons and holes slows down their radiative recombination. With increasing excitation intensity, Auger recombination quickly becomes the dominate recombination channel, and it produces carrier ejection from the quantum well. Here, we show that in Si/SiGe three-dimensional nanostructures, this efficient process facilitates the formation of an electron-hole plasma (EHP) and/or electron-hole droplets (EHDs) in thin Si barriers separating SiGe clusters. In contrast to conventional, strongly tem…
Ion beams are used routinely for processing of semiconductors, particularly sputtering, ion implantation and direct-write fabrication of nanostructures. However, the utility of ion beam techniques is limited by crystal damage and surface roughening. Damage can be reduced or eliminated by performing irradiation at elevated temperatures. However, at these conditions, surface roughening is highly problematic due to thermal mobility of adatoms and surface vacancies. Here we solve this problem using hydrogen gas, which we use to stabilize surface mass flow and suppress roughening during ion bombard…
