In situ morphological investigation of the {105} faceted Ge islands on the Si(001) surface (hut clusters) have been carried out using an ultra high vacuum instrument integrating a high resolution scanning tunnelling microscope and a molecular beam epitaxy vessel. Both species of hut clusters--pyramids and wedges--were found to have the same structure of the {105} facets which was visualized. Structures of vertexes of the pyramidal clusters and ridges of the wedge-shaped clusters were revealed as well and found to be different. This allowed us to propose a crystallographic model of the {105} facets as well as models of the atomic structure of both species of the hut clusters. An inference is made that transitions between the cluster shapes are impossible.
In monolayers of transition metal dichalcogenides the nonlocal nature of the effective dielectric screening leads to large binding energies of excitons. Additional lateral confinement gives rise to exciton localization in quantum dots. By assuming parabolic confinement for both the electron and the hole, we derive model wave functions for the relative and the center-of-mass motions of electron-hole pairs, and investigate theoretically resonant energy transfer among excitons localized in two neighboring quantum dots. We quantify the probability of energy transfer for a direct-gap transition by …
Strong confinement of charges in few electron systems such as in atoms, molecules and quantum dots leads to a spectrum of discrete energy levels that are often shared by several degenerate quantum states. Since the electronic structure is key to understanding their chemical properties, methods that probe these energy levels in situ are important. We show how electrostatic force detection using atomic force microscopy reveals the electronic structure of individual and coupled self-assembled quantum dots. An electron addition spectrum in the Coulomb blockade regime, resulting from a change in ca…
We report on a combined photoluminescence imaging and atomic force microscopy study of single, isolated self-assembled InAs quantum dots (density <0.01 um^(-2) capped by a 95 nm GaAs layer, and emitting around 950 nm. By combining optical and scanning probe characterization techniques, we determine the position of single quantum dots with respect to comparatively large (100 nm to 1000 nm in-plane dimension) topographic features. We find that quantum dots often appear (>25% of the time) in the vicinity of these features, but generally do not exhibit significant differences in their non-resonant…
We present here a theory and a computational tool, Silicon-{\sc Qnano}, to describe atomic scale quantum dots in Silicon. The methodology is applied to model dangling bond quantum dots (DBQDs) created on a passivated H:Si-(100)-(2$\times$1) surface by removal of a Hydrogen atom. The electronic properties of DBQD are computed by embedding it in a computational box of Silicon atoms. The surfaces of the computational box were constructed by using DFT as implemented in {\sc Abinit} program. The top layer was reconstructed by the formation of Si dimers passivated with H atoms while the bottom layer…
Electron spins in Si/SiGe quantum wells suffer from nearly degenerate conduction band valleys, which compete with the spin degree of freedom in the formation of qubits. Despite attempts to enhance the valley energy splitting deterministically, by engineering a sharp interface, valley splitting fluctuations remain a serious problem for qubit uniformity, needed to scale up to large quantum processors. Here, we elucidate and statistically predict the valley splitting by the holistic integration of 3D atomic-level properties, theory and transport. We find that the concentration fluctuations of Si …
Material properties depend sensitively on the atomic arrangements and atomic bonding, but these are notoriously difficult to measure in nanosized atomic clusters due to the small size of the objects and the challenge of obtaining bulk samples of identical clusters. Here we have combined the recent ability to make gram quantities of identical semiconductor quantum-dot nanoparticles with the ability to measure lattice dynamics on small sample quantities of hydrogenated materials using high energy resolution inelastic x-ray scattering (HERIX), to measure the size-dependence of the phonon density …
We report influence of encapsulated C60 molecules on electron transport in carbon-nanotube peapod quantum dots. We find atomic-like behaviors with doubly degenerate electronic levels, which exist only around ground states, by single electron spectroscopy measured at low back-gate voltages (Vbg). Correlation with presence of nearly free electrons (NFEs) unique to the peapods is discussed. Moreover, we find anomalously high values of power a observed in power laws in conductance versus energy relationships, which are strongly associated with the doubly degenerate levels. It is revealed that the …
We have demonstrated surface-plasmon induced change in spontaneous emission rate in the ultraviolet regime at ~ 375-380 nm, using AlN/GaN quantum dots (QD). Using time-resolved and continuous-wave photoluminescence measurements, the recombination rate in AlN/GaN QD is shown to be enhanced when spontaneous emission is resonantly coupled to a metal-surface plasmon mode. The exciton recombination process via Ag-surface plasmon modes is observed to be as much as 3-7 times faster than in normal QD spontaneous emission and depends strongly on the emission wavelength and silver thickness.
We report a direct observation of Ge hut nucleation on Si(001) during UHV MBE. The study was carried out using a UHV instrument coupling MBE chamber and STM which enables the sample study on atomic level at any stage of treatment. Si wafers were deoxidized by annealing at 925C. Ge was deposited by electron beam evaporation; the coverage was varied from 3 to 14 Å; the wafer temperature was 360C. The nuclei of pyramids and wedges were observed on the (MxN) wetting layer (WL) patches and found to have different structures. The atomic models of nuclei of both hut species have been built as well as…
Surface plasmon-polaritons in a multilayer structure consisting of a metallic film and one or more layers of nanocrystal (NC) quantum dots (QDs) are studied. It is shown that there is resonance coupling between the plasmon-polaritons propagating along the metal/NC-layer interface and excitons confined in the dots, which makes a considerable effect on the optical properties of the structure unless the dispersion of the QD size is too large. This coupling can be explored in order to selectively excite QDs of different size by using an attenuated total reflection (ATR) structure. It opens the pos…
We develop a quantum theory of the nonlinear interaction between intense surface acoustic waves and electrons of a quantum well in the regime of moving quantum wires and dots. The quantum nonlinear interaction qualitatively differs from the classical one. In a system of electron wires driven by an acoustic wave the sound attenuation strongly decreases with increasing the sound intensity. However, even in the quantum limit the sound attenuation in the electron system remains nonzero due to residual scattering by impurities in the lowest subband. In the case of electron dots formed by two waves …
We calculate the acoustic phonon-assisted exciton spin relaxation in single self-assembled In$_{1-x}$Ga$_x$As/GaAs quantum dots using an atomic empirical pseudopotential method. We show that the transition from bright to dark exciton states is induced by Coulomb correlation effects. The exciton spin relaxation time obtained from sophisticated configuration interaction calculations is approximately 15--55 $μ$s in pure InAs/GaAs QDs and even longer in alloy dots. These results contradict previous theoretical and experimental results, which suggest very short exciton spin times (a few ns), but ag…
The tip artifact in atomic force microscopy (AFM) observations of InAs islands was evaluated quantitatively. The islands were grown in the Stranski-Krastanow mode of molecular beam epitaxy. The width and height of the islands were determined using transmission electron microscopy (TEM) and AFM. The average $[\bar{1}10]$ in-plane width and height determined using TEM excluding native oxide were 22 and 7 nm, respectively; those determined using AFM including the oxide were 35 and 8 nm, respectively. The difference in width was due to the oxide and the tip artifact. The sizes including the oxide …
By means of a microscopic valence force field model, a series of novel microscopic interface phonon modes are identified in shell quantum dots(SQDs) composed of a GaAs quantum dot of nanoscale embedded in an AlAs shell of a few atomic layers in thickness. In SQDs with such thin shells, the basic principle of the continuum dielectric model and the macroscopic dielectric function are not valid any more. The frequencies of these microscopic interface modes lie inside the gap between the bulk GaAs band and the bulk AlAs band, contrary to the macroscopic interface phonon modes. The average vibratio…
Previous studies have shown that positron-annihilation spectroscopy is a highly sensitive probe of the electronic structure and surface composition of ligand-capped semiconductor Quantum Dots (QDs) embedded in thin films. Nature of the associated positron state, however, whether the positron is confined inside the QDs or localized at their surfaces, has so far remained unresolved. Our positron-annihilation lifetime spectroscopy (PALS) studies of CdSe QDs reveal the presence of a strong lifetime component in the narrow range of 358-371 ps, indicating abundant trapping and annihilation of positr…
It is discovered that the zero-dimensional character of the silicon atom dangling bond (DB) state allows controlled formation and occupation of a new form of quantum dot assemblies. Whereas on highly doped n-type substrates isolated DBs are negatively charged, it is found that Coulomb repulsion causes DBs separated by less than ~2 nm to experience reduced localized charge. The unoccupied states so created allow a previously unobserved electron tunnel-coupling of DBs, evidenced by a pronounced change in the time-averaged view recorded by scanning tunneling microscopy. Direct control over net el…
The influences of Si sheet doping levels on the properties of InAs/GaAs quantum dots (QDs) are investigated by atomic force microscopy (AFM) and photoluminescence (PL). AFM measurements reveal that Si sheet doping doesn't change the morphology of InAs QDs. Conductive AFM exhibits a quick current decrease when the Si doping density reaches 5\times1011cm-2. PL measurements show that the Si doping can significantly enhance the PL intensity. The PL peak intensity of InAs QDs doped to 5\times1011cm-2 is increased about thirty-five times from that of the undoped ones at 300K. The results observed he…
We report formation of self organized InP nano dots using 3 keV Ar+ ion sputtering, at $15^\circ$ incidence from surface normal, on InP(111) surface. Morphology and optical properties of the sputtered surface, as a function of sputtering time, have been investigated by Scanning Probe Microscopy and Raman Scattering techniques. Uniform patterns of nano dots are observed for different durations of sputtering. The sizes and the heights of these nano dots vary between 10 to 100 nm and 20 to 40 nm, respectively. With increasing of sputtering time, t, the size and height of these nano dots increases…
First-order perturbation theory and many-body Green function analysis are used to quantify the influence of size, surface reconstruction and surface treatment on exciton transport between small silicon quantum dots. Competing radiative processes are also considered in order to determine how exciton transport efficiency is influenced. The analysis shows that quantum confinement causes small (~1 nm) Si quantum dots to exhibit exciton transport efficiencies far exceeding that of their larger counterparts. We also find that surface reconstruction significantly influences the absorption cross secti…
The optical emission of InGaN quantum dots embedded in GaN nanowires is dynamically controlled by a surface acoustic wave (SAW). The emission energy of both the exciton and biexciton lines is modulated over a 1.5 meV range at ~330 MHz. A small but systematic difference in the exciton and biexciton spectral modulation reveals a linear change of the biexciton binding energy with the SAW amplitude. The present results are relevant for the dynamic control of individual single photon emitters based on nitride semiconductors.
The equilibrium shapes of InAs quantum dots (i.e., dislocation-free, strained islands with sizes >= 10,000 atoms) grown on a GaAs (001) substrate are studied using a hybrid approach which combines density functional theory (DFT) calculations of microscopic parameters, surface energies, and surface stresses with elasticity theory for the long-range strain fields and strain relaxations. In particular we report DFT calculations of the surface stresses and analyze the influence of the strain on the surface energies of the various facets of the quantum dot. The surface stresses have been neglected …
Low temperature epitaxial breakdown of inhomogeneously strained Si capping layers is investigated. By growing Si films on coherently strained GeSi quantum dot surfaces, we differentiate effects of surface roughness, strain, and growth orientation on the mechanism of epitaxial breakdown. Using atomic force microscopy and high resolution cross-sectional transmission electron microscopy we find that while local lattice strain up to 2% has a negligible effect, growth on higher-index facets such as {113} significantly reduces the local breakdown thickness. Nanoscale growth mound formation is observ…
A model for realistic InAs quantum dot composition profile is proposed and analyzed, consisting of a double region scheme with an In-rich internal core and an In-poor external shell, in order to mimic the atomic scale phenomena such as In-Ga intermixing and In segregation during the growth and overgrowth with GaAs. The parameters of the proposed model are derived by reproducing the experimentally measured polarization data. Further understanding is developed by analyzing the strain fields which suggests that the two-composition model indeed results in lower strain energies than the commonly ap…
Ultra-Confinement of Polaritons in Single Atomic Layer Ag Photonic Quantum Dots
The Pennsylvania State University（宾夕法尼亚州立大学）；Joint School of Nanoscience and Nanoengineering, the University of North Carolina at Greensboro（北卡罗来纳大学格林斯伯勒分校纳米科学与工程联合学院）
Positron Two Dimensional Angular Correlation of Annihilation Radiation (2D-ACAR) measurements reveal modifications of the electronic structure and composition at the surfaces of PbSe quantum dots (QDs), deposited as thin films, produced by various ligands containing either oxygen or nitrogen atoms. In particular, the 2D-ACAR measurements on thin films of colloidal PbSe QDs capped with oleic acid ligands yield an increased intensity in the electron momentum density (EMD) at high momenta compared to PbSe quantum dots capped with oleylamine. Moreover, the EMD of PbSe QDs is strongly affected by t…
A direct observation of nucleation of Ge hut clusters formed by ultrahigh vacuum molecular beam epitaxy is reported for the first time. The nuclei of the pyramidal and wedge-like clusters have been observed on the wetting layer blocks and found to have different structures. The growth of the clusters of both species goes on following different scenarios: Formation of the second atomic layer of the wedge-like cluster results in rearrangement of its first layer. Its ridge structure does not replicate the structure of the nucleus. The pyramidal cluster grows without phase transitions. The structu…
We implement substrate rotation in a 2+1 dimensional solid-on-solid model of ion beam sputtering of solid surfaces. With this extension of the model, we study the effect of concurrent rotation, as the surface is sputtered, on possible topographic regions of surface patterns. In particular we perform a detailed numerical analysis of the time evolution of dots obtained from our Monte Carlo simulations at off-normal-incidence sputter erosion. We found the same power-law scaling exponents of the dot characteristics for two different sets of ion-material combinations, without and with substrate rot…
We present an atomistic study of the strain field, the one-particle electronic spectrum and the oscillator strength of the fundamental optical transition in chemically disordered In$_{x}$Ga$_{1-x}$As pyramidal quantum dots (QDs). Interdiffusion across the interfaces of an originally ``pure'' InAs dot buried in a GaAs matrix is simulated through a simple model, leading to atomic configurations where the abrupt hetero-interfaces are replaced by a spatially inhomogeneous composition profile $x$. Structural relaxation and the strain field calculations are performed through the Keating valence forc…
Black phosphorus (BP) nanostructures enable a new strategy to tune the electronic and optical properties of this atomically thin material. In this paper we show, via density functional theory calculations, the possibility to modify the optical properties of BP quantum dots via covalent functionalization. The quantum dot selected in this study has chemical formula P24H12 and has been covalent functionalized with one or more benzene rings or anthracene. The effect of functionalization is highlighted in the absorption spectra, where a red shift of the absorption is noticeable. The shift can be as…
Thin layers of GaMnAs ferromagnetic semiconductor grown by molecular beam epitaxy on GaAs(001) substrates were studied. To improve their magnetic properties the post-growth annealing procedures were applied, using the surface passivation layers of amorphous arsenic. This post growth treatment effectively increases the ferromagnetic-to-paramagnetic phase transition temperature in GaMnAs, and provides surface-rich MnAs layer which can be used for formation of low dimensional structures such as superlattices. If the surface rich MnAs layer consists of MnAs dots, then it is possible to grow Mn-dop…
Formation of MnAs quantum dots in a regular ring-like distribution has been found on MBE-grown (GaMn)As surfaces after low-temperature annealing under As capping. The Mn was supplied by out-diffusing Mn interstitials from (GaMn)As. With 5 at% substitutional Mn the quantum dots appeared for (GaMn)As layers thicker than 500 A. For thinner layers the Mn-rich surfaces, presumably monolayer thick MnAs, are smooth and well-ordered (1x2), and are well suited for continued epitaxial growth.
Polarization effects are included exactly in a model for a quantum dot in close proximity to a planar interface. Efficient incorporation of this potential into the Schrödinger equation is utilized to map out the influence of the image potential effects on carrier tunneling in such heterostructures. In particular, the interplay between carrier mass and the dielectric constants of a quantum dot, its surrounding matrix, and the electrode is studied. We find that the polarizability of the planar electrode structure can significantly increase the tunneling rates for heavier carriers, potentially re…
We use atomistic tight-binding theory with a configuration interaction description of Coulomb and exchange effects to describe excitons in symmetric quantum dots in a vertical electric field. We show that field-induced manipulation of exciton orientation and phase produces a drastic reduction of fine structure splitting, an anticrossing, and a 90 degree rotation of polarization, similar to experiment. An atomistic analysis is needed to explain how exciton reorientation modifies anisotropic exchange and fine structure splitting without significantly altering other splittings.
We report the growth of self-assembled Bi2Se3 quantum dots (QDs) by molecular beam epitaxy on GaAs substrates using the droplet epitaxy technique. The QD formation occurs after anneal of Bismuth droplets under Selenium flux. Characterization by atomic force microscopy, scanning electron microscopy, X-ray diffraction, high-resolution transmission electron microscopy and X-ray reflectance spectroscopy is presented. The quantum dots are crystalline, with hexagonal shape, and have average dimensions of 12 nm height (12 quintuple layers) and 46 nm width, and a density of $8.5 \cdot 10^9 cm^{-2}$. T…
Long range dipole-dipole correlation in a ferromagnetic sample can be treated in terms of collective excitations of the system as a whole. Ferrite samples with linear dimensions smaller than the dephasing length, but still much larger than the exchange-interaction scales are mesoscopic structures. Recently, it was shown that mesoscopic quasi-2D ferrite disks, distinguishing by multiresonance magneto-dipolar-mode (MDM) spectra, demonstrate unique properties of artificial atomic structures: energy eigenstates, eigen power-flow vortices and eigen helicity parameters. Because of these properties, …
MnAs has been grown by means of MBE on the GaN(0001)-(1x1) surface. Two options of initiating the crystal growth were applied: (a) a regular MBE procedure (manganese and arsenic were delivered simultaneously) and (b) subsequent deposition of manganese and arsenic layers. It was shown that spontaneous formation of MnAs dots with the surface density of 1$\cdot 10^{11}$ cm$^{-2}$ and $2.5\cdot 10^{11}$ cm$^{-2}$, respectively (as observed by AFM), occurred for the layer thickness higher than 5 ML. Electronic structure of the MnAs/GaN systems was studied by resonant photoemission spectroscopy. Tha…
Eliminating the fine structure splitting (FSS) of excitons in self-assembled quantum dots (QDs) is essential to the generation of high quality entangled photon pairs. It has been shown that the FSS has a lower bound under uniaxial stress. In this letter, we show that the FSS of excitons in a general self-assembled InGaAs/GaAs QD can be fully suppressed via combined stresses along the [110] and [010] directions. The result is confirmed by atomic empirical pseudopotential calculations. For all the QDs we studied, the FSS can be tuned to be vanishingly small ($<$ 0.1 $μ$eV), which is sufficient s…
Heteroepitaxial self-assembled quantum dots (SAQDs) will allow breakthroughs in electronics and optoelectronics. SAQDs are a result of Stranski-Krastanow growth whereby a growing planar film becomes unstable after an initial wetting layer is formed. Common systems are Ge$_{x}$Si$_{1-x}$/Si and In$_{x}$Ga$_{1-x}$As/GaAs. For applications, SAQD arrays need to be ordered. The role of crystal anisotropy, random initial conditions and thermal fluctuations in influencing SAQD order during early stages of SAQD formation is studied through a simple stochastic model of surface diffusion. Surface diffus…
Classical contact lithography involves patterning of surfaces by embossing or by transfer of ink. We report direct lithographic transfer of parts of sacrificial stamps onto counterpart surfaces. Using sacrificial stamps consisting of the block copolymer polystyrene-block-poly(2-pyridine) (PS-b-P2VP), we deposited arrays of nanostructured submicron PS-b-P2VP dots with heights of about 100 nm onto silicon wafers and glass slides. The sacrificial PS-b-P2VP stamps were topographically patterned with truncated-pyramidal contact elements and penetrated by spongy-continuous nanopore systems. The spon…
The evolution of InAs quantum dots grown on InP substrates by metal-organic vapour phase epitaxy is studied as a function of InAs coverage. Under specific growth conditions, the onset of the two- to three-dimensional transition is seen to proceed via two distinct pathways: through (i) an abrupt appearance of quantum dots as expected in the usual Stranski-Krastanov growth picture and (ii) a continuous evolution of small surface features into well developed quantum dots. The average size of the features in both these families increases with coverage, leading to a bimodal distribution in dot size…
The formation of dislocation-free three-dimensional islands during the heteroepitaxial growth of lattice-mismatched materials has been observed experimentally for several material systems. The equilibrium shape of the islands is governed by the competition between the surface energy and the elastic relaxation energy of the islands as compared to the uniform strained film. As an exemplification we consider the experimentally intensively investigated growth of InAs quantum dots on a GaAs(001) substrate, deriving the equilibrium shape as a function of island volume. For this purpose InAs surface …
We report on the growth and optical characterisation of droplet GaAs quantum dots with extremely-thin (11 nm) capping layers. To achieve such result, an internal thermal heating step is introduced during the growth and its role in the morphological properties of the quantum dots obtained is investigated via scanning electron and atomic force microscopy. Photoluminescence measurements at cryogenic temperatures show optically stable, sharp and bright emission from single quantum dots, at near-infrared wavelengths. Given the quality of their optical properties and the proximity to the surface, su…
Self-assembled InAs quantum dots (QDs) grown on GaAs(001) surface by molecular beam epitaxy under continuous and growth-interruption modes exhibit two families of QDs, quasi-3D (Q3D) and 3D QDs, whose volume density evolution is quantitatively described by a rate-equation kinetic model. The volume density of small Q3D QDs decreases exponentially with time during the interruption, while the single-dot mean volume of the large QDs increases by Ostwald ripening. The kinetics of growth involves conversion of quasi-3D to 3D QDs at a rate determined by superstress and participation of the wetting la…
In this work, we have investigated the optical properties of two samples of CdSe quantum dots by using submicro-photoluminescence spectroscopy. The effect of vicinal-surface GaAs substrates on their properties has been also assessed. The thinner sample, grown on a substrate with vicinal surface, includes only dots with a diameter of less than 10 nm (type A islands). Islands of an average diameter of about 16 nm (type B islands) that are related to a phase transition via a Stranski-Krastanow growth process are also distributed in the thicker sample grown on an oriented substrate. We have studie…
The screening of point charges in hydrogenated Si quantum dots ranging in diameter from 10 A to 26 A has been studied using first-principles density-functional methods. We find that the main contribution to the screening function originates from the electrostatic field set up by the polarization charges at the surface of the nanocrystals. This contribution is well described by a classical electrostatics model of dielectric screening.
The interaction of Mn with Ge quantum dots (QD), which are bounded by {105} facets, and the strained Ge wetting layer (WL), terminated by a (001) surface, is investigated with scanning tunneling microscopy (STM). Mn is deposited on the Ge QD and WL surface in sub-monolayer concentrations, and subsequently annealed up to temperature of 400 C. Bonding and surface topography were measured with STM during the annealing process. Mn forms flat islands on the Ge {105} facet, whose shape and position is guided by the rebonded step reconstruction. The images show a hybridization of Mn-d band and empty …
Epitaxial self-assembled quantum dots (SAQDs) represent an important step in the advancement of semiconductor fabrication at the nanoscale that will allow breakthroughs in electronics and optoelectronics. In these applications, order is a key factor. Here, the role of crystal anisotropy in promoting order during early stages of SAQD formation is studied through a linear analysis of a commonly used surface evolution model. Elastic anisotropy is used a specific example. It is found that there are two relevant and predictable correlation lengths. One of them is related to crystal anisotropy and i…
The equilibrium shape of strained InAs quantum dots grown epitaxially on a GaAs(001) substrate is derived as a function of volume. InAs surface energies are calculated within density-functional theory, and a continuum approach is applied for the elastic relaxation energies.
We show that the emergence of different surface patterns (ripples, dots) can be well understood by a suitable mapping onto the simplest nonequilibrium lattice gases and cellular automata.Using this efficient approach difficult, unanswered questions of surface growth and its scaling can be studied. The mapping onto binary variables facilitates effective simulations and enables one to consider very large system sizes.We have confirmed that the fundamental Kardar-Parisi-Zhang (KPZ) universality class is stable against a competing roughening diffusion,while a strong smoothing diffusion leads to lo…
