In the framework of four-band envelope-function formalism, developed earlier for spherical semiconductor nanocrystals, we study the electronic structure and optical properties of quantum-confined lead-salt (PbSe and PbS) nanowires (NWs) with a strong coupling between the conduction and the valence bands. We derive spatial quantization equations, and calculate numerically energy levels of spatially quantized states of a transverse electron motion in the plane perpendicular to the NW axis, and electronic subbands developed due to a free longitudinal motion along the NW axis. Using explicit expressions for eigenfunctions of the electronic states, we also derive analytical expressions for matrix elements of optical transitions and study selection rules for interband absorption.
Next we study a two-particle problem with a conventional long-range Coulomb interaction and an interparticle coupling via medium polarization. The obtained results show that due to a large magnitude of the high-frequency dielectric permittivity of PbSe material, and hence, a high dielectric NW/vacuum contrast, the effective coupling via medium polarization significantly exceeds the effective direct Coulomb coupling at all interparticle separations along the NW axis. Furthermore, the strong coupling via medium polarization results in a bound state of the longitudinal motion of the lowest-energy electron-hole pair (a longitudinal exciton), while fast transverse motions of charge carriers remain independent of each other.
Auger recombination (AR) of the ground biexciton state in quantum-confined lead salt nanowires (NWs) with a strong coupling between the conduction and the valence bands is shown to be strongly suppressed, and only excited biexciton states contribute to Auger decay. The AR rate is predicted to be greatly reduced when temperature or the NW radius are decreased, and the effect is explained by decrease in both the population of excited biexciton states and overlap of phonon-broadened single- and biexciton states. Suppression of AR of multiexciton states exhibiting strong radiative decay makes obvi…
Electron spin relaxation in nanowire-based quantum dots induced by confined phonons is investigated theoretically. Due to the one-dimensional nature of the confined phonons, the van Hove singularities of the confined phonons and the zero of the form factor of the electron-phonon coupling can lead to unique features of the spin relaxation rate. Extremely strong spin relaxation can be obtained at the van Hove singularity. Meanwhile the spin relaxation rate can also be greatly suppressed at the zero of the form factor. This unique feature indicates the flexibility of nanowire-based quantum dots i…
Moire based strain analysis in wurtzite GaAs -- rock-salt (Pb,Sn)Te core-shell nanowires grown by molecular beam epitaxy
Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Faculty of Physics, University of Warsaw（华沙大学物理学院）；Ensemble3 Centre of Excellence（Ensemble3卓越中心）；International Research Center MagTop, Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所国际研究中心MagTop）
The singlet-triplet relaxation in nanowire-based quantum dots induced by confined phonons is investigated theoretically. Due to the quasi-one-dimensional nature of the confined phonons, the singlet-triplet relaxation rates exhibit multi-peaks as function of magnetic field and the relaxation rate between the singlet and the spin up triplet state is found to be enhanced at the vicinity of the singlet-triplet anti-crossing. We compare the effect of the deformation-potential coupling and the piezoelectric coupling and find that the deformation-potential coupling dominates the relaxation rates in m…
We analyze the emission of single GaN nanowires with (In,Ga)N insertions using both micro-photoluminescence and cathodoluminescence spectroscopy. The emission spectra are dominated by a green luminescence band that is strongly blueshifted with increasing excitation density. In conjunction with finite-element simulations of the structure to obtain the piezoelectric polarization, these results demonstrate that our (In,Ga)N/GaN nanowire heterostructures are subject to the quantum-confined Stark effect. Additional sharp peaks in the spectra, which do not shift with excitation density, are attribut…
Confining two dimensional Dirac fermions on the surface of topological insulators has remained an outstanding conceptual challenge. Here we show that Dirac fermion confinement is achievable in topological crystalline insulators (TCI), which host multiple surface Dirac cones depending on the surface termination and the symmetries it preserves. This confinement is most dramatically reflected in the flux dependence of these Dirac states in the nanowire geometry, where different facets connect to form a closed surface. Using SnTe as a case study, we show how wires with all four facets of the <100>…
We investigate theoretically the electron spin relaxation in single-electron nanowire-based semiconductor double quantum dots induced by confined phonons and find that the electron spin relaxation rate can be efficiently manipulated by external electric fields in such system. An anti-crossing, due to the coaction of the electric field, the magnetic field and the spin-orbit coupling, exists between the lowest two excited states. Both energies and spins of the electron states can be efficiently tuned by the electric field around the anti-crossing point. Multiple sharp peaks exist in the electric…
Confined optical phonons are discussed for a semiconductor nanowire of the Ge (Si)prototype on the basis of a theory developed some years ago. In the present work this theory is adapted to a non polar material and generalized to the case when the phonon dispersion law involves both linear and quadratic terms in the wave vector. The treatment is considered along the lines of a continuous medium model and leads to a system of coupled differential equations describing oscillations of mixed nature. The nanowire is modelled in the form of an infinite circular cylinder and the solutions of the funda…
We report on electrostatic screening of polarization-induced internal electric fields in AlN/GaN nanowire heterostructures with Germanium-doped GaN nanodiscs embedded between AlN barriers. The incorporation of Germanium at concentrations above $10^{20}\,\text{cm}^{-3}$ shifts the photoluminescence emission energy of GaN nanodiscs to higher energies accompanied by a decrease of the photoluminescence decay time. At the same time, the thickness-dependent shift in emission energy is significantly reduced. In spite of the high donor concentration a degradation of the photoluminescence properties is…
We have performed first-principles calculations to study the lattice vibrational modes and their Raman activities in silicon nanowires (SiNWs). Two types of characteristic vibrational modes are examined: high-frequency optical modes and low-frequency confined modes. Their frequencies have opposite size dependence with a red shift for the optical modes and a blue shift for the confined modes as the diameter of SiNWs decreases. In addition, our calculations show that these vibrational modes can be detected by Raman scattering measurements, providing an efficient way to estimate the size of SiNWs…
Several of the key issues of planar (Al,Ga)N-based deep-ultraviolet light emitting diodes could potentially be overcome by utilizing nanowire heterostructures, exhibiting high structural perfection and improved light extraction. Here, we study the spontaneous emission of GaN/(Al,Ga)N nanowire ensembles grown on Si(111) by plasma-assisted molecular beam epitaxy. The nanowires contain single GaN quantum disks embedded in long (Al,Ga)N nanowire segments essential for efficient light extraction. These quantum disks are found to exhibit intense emission at unexpectedly high energies, namely, signif…
An optical characterization tool of Raman spectroscopy with extremely weak scattering cross section tool is not popular to analyze scattered signal from a single nanostructure in the sub-diffraction regime. In this regard, plasmonic assisted characterization tools are only relevant in spectroscopic studies of nanoscale object in the sub-diffraction limit. We have reported polarized resonance Raman spectroscopic (RRS) studies with strong electron-phonon coupling to understand the crystalline orientation of a single AlGaN nanowire of diameter about 100 nm. AlGaN nanowire is grown by chemical vap…
Nearly 30% increase of the ferromagnetic phase transition temperature has been achieved in strained MnAs nanocrystals embedded in a wurtzite GaAs matrix. Wurtzite GaAs exerts tensile stress on hexagonal MnAs nanocrystals, preventing a hexagonal to orthorhombic structural phase transition, which in the bulk MnAs is combined with the magnetic one. This effect results in a remarkable shift of the magneto-structural phase transition temperature from 313 K in the bulk MnAs to above 400 K in the tensely strained MnAs nanocrystals. This finding is corroborated by the state of the art transmission ele…
Wireless technology relies on the conversion of alternating electromagnetic fields to direct currents, a process known as rectification. While rectifiers are normally based on semiconductor diodes, quantum mechanical non-reciprocal transport effects that enable highly controllable rectification have recently been discovered. One such effect is magnetochiral anisotropy (MCA), where the resistance of a material or a device depends on both the direction of current flow and an applied magnetic field. However, the size of rectification possible due to MCA is usually extremely small, because MCA rel…
The radial confining potential in a semiconductor nanowire plays a key role in determining its quantum transport properties. Previous reports have shown that an axial magnetic field induces flux-periodic conductance oscillations when the electronic states are confined to a shell. This effect is due to the coupling of orbital angular momentum to the magnetic flux. Here, we perform calculations of the energy level structure, and consequently the conductance, for more general cases ranging from a flat potential to strong surface band bending. The transverse states are not confined to a shell, but…
We report on a detailed study of the intensity dependent optical properties of individual GaN/AlN Quantum Disks (QDisks) embedded into GaN nanowires (NW). The structural and optical properties of the QDisks were probed by high spatial resolution cathodoluminescence (CL) in a scanning transmission electron microscope (STEM). By exciting the QDisks with a nanometric electron beam at currents spanning over 3 orders of magnitude, strong non-linearities (energy shifts) in the light emission are observed. In particular, we find that the amount of energy shift depends on the emission rate and on the …
The experimental assessment of the strength ($α_R$) of the Rashba spin-orbit coupling is rather indirect and involves the measurement of the spin relaxation length from magnetotransport, together with a model of weak antilocalization. The analysis of the spin relaxation length in nanowires, however, clouds the experimental assessment of the $α_R$ and leads to the prevailing belief that it can be tuned freely with electric field--a central tenant of spintronics. Here, we report direct theory of $α_R$ leading to atomistic calculations of the spin band structure of InAs nanowires upon application…
We performed an {\it ab initio} investigation on the properties of rutile tin oxide (SnO$_{x}$) nanowires. We computed the wire properties determining the equilibrium geometries, binding energies and electronic band structures for several wire dimensions and surface facet configurations. The results allowed to establish scaling laws for the structural properties, in terms of the nanowire perimeters. The results also showed that the surface states control most of the electronic properties of the nanowires. Oxygen incorporation in the nanowire surfaces passivated the surface-related electronic s…
Achieving significant doping in GaAs/AlAs core/shell nanowires (NWs) is of considerable technological importance but remains a challenge due to the amphoteric behavior of the dopant atoms. Here we show that placing a narrow GaAs quantum well in the AlAs shell effectively getters residual carbon acceptors leading to an \emph{unintentional} p-type doping. Magneto-optical studies of such a GaAs/AlAs core multi-shell NW reveal quantum confined emission. Theoretical calculations of NW electronic structure confirm quantum confinement of carriers at the core/shell interface due to the presence of ion…
Light emitting diodes (LEDs) were fabricated using ensembles of free-standing (In,Ga)N/GaN nanowires (NWs) grown on Si substrates in the self-induced growth mode by molecular beam epitaxy. Electron beam induced current analysis, cathodoluminescence as well as biased $μ$-photoluminescence spectroscopy, transmission electron microscopy, and electrical measurements indicate that the electroluminescence of such LEDs is governed by the differences in the individual current densities of the single-NW LEDs operated in parallel, i.e. by the inhomogeneity of the current path in the ensemble LED. In add…
Electronic properties of graphene quantum dots (GQDs) constitute a subject of intense scientific interest. Being smaller than 20 nm, GQDs contain confined excitons in all dimensions simultaneously. GQDs feature a non-zero band gap and luminesce on excitation. Tuning their electronic structure is an attractive goal with a technological promise. In this work, we apply density functional theory to study an effect of neutral ionic clusters adsorbed on GQD surface. We conclude that both HOMO and LUMO of GQD are very sensitive to the presence of ions and to their distance from the GQD surface. Howev…
We report the detection of quantum confinement in single InAs-InP core-shell nanowires. The wires having an InAs core with ~25 nm diameter are characterized by emission spectra in which two peaks are identified under high excitation intensity conditions. The peaks are caused by emission from the ground and excited quantized levels, due to the quantum confinement in the plane perpendicular to the nanowire axis. We have identified in the emission spectra different energy contributions related to the wurtzite structure of the wires, the strain between the wurtzite core and shell, and the confinem…
Semiconductor nanowires have opened new research avenues in quantum transport owing to their confined geometry and electrostatic tunability. They have offered an exceptional testbed for superconductivity, leading to the realization of hybrid systems combining the macroscopic quantum properties of superconductors with the possibility to control charges down to a single electron. These advances brought semiconductor nanowires to the forefront of efforts to realize topological superconductivity and Majorana modes. A prime challenge to benefit from the topological properties of Majoranas is to red…
Reduced dimensionality leads to emergent phenomena in quantum materials and there is a need for accelerated materials discovery of nanoscale quantum materials in reduced dimensions. Thermomechanical nanomolding is a rapid synthesis method that produces high quality single-crystalline quantum nanowires with controlled dimensions over wafer-scale sizes. Herein, we apply nanomolding to fabricate nanowires from bulk feedstock of MoP, a triple-point topological metal with extremely high conductivity that is promising for low-resistance interconnects. Surprisingly, we obtained single-crystalline Mo$…
In the experimental electroluminescence (EL) spectra of light-emitting diodes (LEDs) based on N-polar (In,Ga)N/GaN nanowires (NWs), we observed a double peak structure. The relative intensity of the two peaks evolves in a peculiar way with injected current. Spatially and spectrally resolved EL maps confirmed the presence of two main transitions in the spectra, and suggested that they are emitted by the majority of single nano-LEDs. In order to elucidate the physical origin of this effect, we performed theoretical calculations of the strain, electric field, and charge density distributions both…
The non-trivial topology of the three-dimensional (3D) topological insulator (TI) dictates the appearance of gapless Dirac surface states. Intriguingly, when a 3D TI is made into a nanowire, a gap opens at the Dirac point due to the quantum confinement, leading to a peculiar Dirac sub-band structure. This gap is useful for, e.g., future Majorana qubits based on TIs. Furthermore, these Dirac sub-bands can be manipulated by a magnetic flux and are an ideal platform for generating stable Majorana zero modes (MZMs), which play a key role in topological quantum computing. However, direct evidence f…
We report the spectral imaging in the UV to visible range with nanometer scale resolution of closely packed GaN/AlN quantum disks in individual nanowires using an improved custom-made cathodoluminescence system. We demonstrate the possibility to measure full spectral features of individual quantum emitters as small as 1 nm and separated from each other by only a few nanometers and the ability to correlate their optical properties to their size, measured with atomic resolution. The direct correlation between the quantum disk size and emission wavelength provides evidence of the quantum confined…
Intersubband optoelectronic devices rely on transitions between quantum-confined electron levels in semiconductor heterostructures, which enables infrared (IR) photodetection in the 1-30 $μ$m wavelength window with picosecond response times. Incorporating nanowires as active media could enable an independent control over the electrical cross-section of the device and the optical absorption cross-section. Furthermore, the three-dimensional carrier confinement in nanowire heterostructures opens new possibilities to tune the carrier relaxation time. However, the generation of structural defects a…
Till now the nanoscale focussing and imaging in the sub-diffraction limit is achieved mainly with the help of plasmonic field enhancement assisted with noble metal nanoparticles. Using far field imaging technique, we have recorded polarized spectroscopic photoluminescence (PL) imaging of a single AlGaN nanowire (NW) of diameter ~ 100 nm using confinement of polarized light. The nanowires on the substrate have a nematic ordering. It is found that the PL from a single NW is influenced by the proximity to other NWs with the PL intensity scaling as 1/(lxd), where l and d are the NW length and the …
Monolithic axial InGaAs quantum dot emitters in GaAs-based nanowires via Sb-mediated facet engineering
Walter Schottky Institute, TUM School of Natural Sciences, Technical University of Munich（慕尼黑工业大学沃尔特·施科特基研究所自然科学学院）；Institute for Physics and Astronomy, Technical University Berlin（柏林工业大学物理与天文学研究所）；Department of Chemistry, Ludwig-Maximilians-University of Munich（慕尼黑大学化学系）；Walter Schottky Institute, TUM School of Computation, Information and Technology, Technical University of Munich（慕尼黑工业大学沃尔特·施科特基研究所计算、信息与技术学院）；Department of Physics, University of California, Berkeley（加州大学伯克利分校物理系）
CdS nanotubes with wall thickness comparable to excitonic diameter of the bulk material are synthesized by a chemical route. A change in experimental conditions result in formation of nanowires, and well-separated nanoparticles. The diameter and wall thickness of nanotubes measured to be 14.4 $\pm$ 6.1 and 4.7 $\pm$ 2.2 nm, respectively. A large number of CdS nanocrystallites having wurzite structure constitute these nanotubes. These nanotubes show high energy shifting of optical absorption and photoluminescence peak positions, compared to its bulk value, due to quantum confinement effect. It …
Emissive perovskite quantum wires in robust nanocontainers
Institute for Solid State Physics and Optics, HUN-REN Wigner Research Centre for Physics（固态物理与光学研究所，匈牙利研究网络温格物理学研究中心）；Institute for Technical Physics and Materials Science, HUN-REN Centre for Energy Research（技术物理与材料科学研究所，匈牙利研究网络能源研究中心）
X-ray diffraction experiments were performed on MnO confined in mesoporous silica SBA-15 and MCM-41 matrices with different channel diameters. The measured patterns were analyzed by profile analysis and compared to numerical simulations of the diffraction from confined nanoparticles. From the lineshape and the specific shift of the diffraction reflections it was shown that the embedded objects form ribbon-like structures in the SBA-15 matrices with channels diameters of 47-87 Å, and nanowire-like structures in the MCM-41 matrices with channels diameters of 24-35 Å. In the latter case the confi…
The virtual (i.e., fundamental many body quantum theory-based, computational) synthesis method is used to establish electronic templates of about 30 non-stoichiometric nanosystems composed of nickel and oxygen atoms and ranging from about 6 Å to 6 nm in linear dimensions. Flexible and stretchable Ni-O bond in such structures accommodates various ratios of Ni to O atoms, and both antiferromagnetic and ferromagnetic spin alignments. Depending on synthesis conditions, smaller Ni-O quantum dots (QDs) composed of up to 14 atoms or so may have both types of spin alignments, while quantum-confined, q…
Surface confined dehalogenation reactions are versatile bottom-up approaches for the synthesis of carbon-based nanostructures with predefined chemical properties. However, for devices generally requiring low conductivity substrates, potential applications are so far severely hampered by the necessity of a metallic surface to catalyze the reactions. In this work we report the synthesis of ordered arrays of poly(p-phenylene) chains on the surface of semiconducting TiO2(110) via a dehalogenative homocoupling of 4,4"-dibromoterphenyl precursors. The supramolecular phase is clearly distinguished fr…
