Giant suppression of Auger electron cooling in charged nanocrystals

This letter presents a detailed study of the electron relaxation lifetimes from the excited p-like state into the ground s-like state via Auger cooling in positively and negatively charged CdSe nanocrystals, where the dependence of Auger cooling rates on size, temperature and carrier-carrier interaction effects is investigated. A nearly two-orders-of-magnitude reduction of Auger rates is found in small nanocrystals populated by two electrons and one hole at room temperature. This effect increases with decreasing temperature leading to a total lifetime increase of up to 4 orders of magnitude for T ∼ 10 K. Such a giant suppression of Auger cooling rates appears to be a general property of semiconductor nanocrystals. A similar reduction of Auger rates at room T is found in negatively charged PbSe nanocrystals as well

Approximate methods for the solution of quantum wires and dots : Connection rules between pyramidal, cuboidal, and cubic dots

Energy eigenvalues of the electronic ground state are calculated for rectangular and triangular GaAs/Ga(0.6)Al(0.4)As quantum wires as well as for cuboidal and pyramidal quantum dots of the same material. The wire (dot) geometries are approximated by a superposition of perpendicular independent finite one-dimensional potential wells. A perturbation is added to the system to improve the approximation. Excellent agreement with more complex treatments is obtained. The method is applied to investigate the ground state energy dependence on volume and aspect ratio for finite barrier cubic, cuboidal, and pyramidal quantum dots. It is shown that the energy eigenvalues of cubes are equal to those of cuboids of the same volume and aspect ratio similar to one. In addition, a relationship has been found between the volumes of pyramidal quantum dots (often the result of self-assembling in strain layered epitaxy) and cuboidal dots with the same ground state energy and aspect ratios close to one. © 1999 American Institute of Physics

Breaking of Larmor's theorem in quantum Hall states with spin-orbit coupling

We investigate the effect of spin-orbit (SO) interaction on the long-wavelength collective spin excitation in a two-dimensional electron gas in the fractional quantum Hall regime. The many-body correction to the single-particle electron spin resonance (ESR) energy is found to be nonzero, providing theoretical evidence of a breaking of Larmor's theorem. Such breaking is due to the loss of spin-rotational invariance introduced by the SO-induced structural inversion asymmetry in the system. This effect, whose magnitude is a significant percentage of the single-particle ESR, exhibits remarkable features in a wide range of experimentally relevant parameters and is found to be nearly material independent

Excited-state relaxation in PbSe quantum dots

In solids the phonon-assisted, nonradiative decay from high-energy electronic excited states to low-energy electronic excited states is picosecond fast. It was hoped that electron and hole relaxation could be slowed down in quantum dots, due to the unavailability of phonons energy matched to the large energy-level spacings (“phonon-bottleneck”). However, excited-state relaxation was observed to be rather fast (1 ps) in InP, CdSe, and ZnO dots, and explained by an efficient Auger mechanism, whereby the excess energy of electrons is nonradiatively transferred to holes, which can then rapidly decay by phonon emission, by virtue of the densely spaced valence-band levels. The recent emergence of PbSe as a novel quantum-dot material has rekindled the hope for a slow down of excited-state relaxation because hole relaxation was deemed to be ineffective on account of the widely spaced hole levels. The assumption of sparse hole energy levels in PbSe was based on an effective-mass argument based on the light effective mass of the hole. Surprisingly, fast intraband relaxation times of 1–7 ps were observed in PbSe quantum dots and have been considered contradictory with the Auger cooling mechanism because of the assumed sparsity of the hole energy levels. Our pseudopotential calculations, however, do not support the scenario of sparse hole levels in PbSe: Because of the existence of three valence-band maxima in the bulk PbSe band structure, hole energy levels are densely spaced, in contradiction with simple effective-mass models. The remaining question is whether the Auger decay channel is sufficiently fast to account for the fast intraband relaxation. Using the atomistic pseudopotential wave functions of Pb2046Se2117 and Pb260Se249 quantum dots, we explicitly calculated the electron-hole Coulomb integrals and the PS electron Auger relaxation rate. We find that the Auger mechanism can explain the experimentally observed PS intraband decay time scale without the need to invoke any exotic relaxation mechanisms

Quantum box energies as a route to the ground state levels of self-assembled InAs pyramidal dots

A theoretical investigation of the ground state electronic structure of InAs/GaAs quantum confined structures is presented. Energy levels of cuboids and pyramidal shaped dots are calculated using a single-band, constant-confining-potential model that in former applications has proved to reproduce well both the predictions of very sophisticated treatments and several features of many experimental photoluminescence spectra. A connection rule between their ground state energies is found which allows the calculation of the energy levels of pyramidal dots using those of cuboids of suitably chosen dimensions, whose solution requires considerably less computational effort. The purpose of this work is to provide experimentalists with a versatile and simple method to analyze their spectra. As an example, this rule is then applied to successfully reproduce the position of the ground state transition peaks of some experimental photoluminescence spectra of self-assembled pyramidal dots. Furthermore the rule is used to predict the dimensions of a pyramidal dot, starting from the knowledge of the ground state transition energy and an estimate for the aspect ratio Q. © 2000 American Institute of Physics

Atomic Effective Pseudopotentials for Semiconductors

We derive an analytic connection between the screened self-consistent effective potential from density functional theory (DFT) and atomic effective pseudopotentials (AEPs). The motivation to derive AEPs is to address structures with thousands to hundred thousand atoms, as given in most nanostructures. The use of AEPs allows to bypass a self-consistent procedure and to address eigenstates around a certain region of the spectrum (e.g., around the band gap). The bulk AEP construction requires two simple DFT calculations of slightly deformed elongated cells. The ensuing AEPs are given on a fine reciprocal space grid, including the small reciprocal vector components, are free of parameters, and involve no fitting procedure. We further show how to connect the AEPs of different bulk materials, which is necessary to obtain accurate band offsets. We derive a total of 20 AEPs for III-V, II-VI and group IV semiconductors and demonstrate their accuracy and transferability by comparison to DFT calculations of strained bulk structures, quantum wells with varying thickness, and semiconductor alloys.Comment: 10 pages, 5 figures, submitted to PR

Theoretical Characterization of GaSb Colloidal Quantum Dots and Their Application to Photocatalytic CO₂ Reduction with Water

With a large exciton Bohr radius and a high hole mobility in the bulk, GaSb is an important semiconductor material for technological applications. Here, we present a theoretical investigation into the evolution of some of its most fundamental characteristics at the nanoscale. GaSb emerges as a widely tunable, potentially disruptive new colloidal material with huge potential for application in a wide range of fields