Simulations of nonradiative processes in semiconductor nanocrystals
arXiv:2204.06551 · doi:10.1063/5.0095897
Abstract
The description of carrier dynamics in spatially confined semiconductor nanocrystals (NCs), which have enhanced electron-hole and exciton-phonon interactions, is a great challenge for modern computational science. These NCs typically contain thousands of atoms and tens of thousands of valence electrons with a discrete spectrum at low excitation energies, similar to atoms and molecules, that converges to the continuum bulk limit at higher energies. Computational methods developed for molecules are limited to very small nanoclusters, and methods for bulk systems with periodic boundary conditions are not suitable due to the lack of translational symmetry in NCs. This perspective focuses on our recent efforts in developing a unified atomistic model based on the semiempirical pseudopotential approach, which is parametrized by first-principles calculations and validated against experimental measurements, to describe two of the main nonradiative relaxation processes of quantum confined excitons: exciton cooling and Auger recombination. We focus on the description of both electron-hole and exciton-phonon interactions in our approach and discuss the role of size, shape, and interfacing on the electronic properties and dynamics for II-VI and III-V semiconductor NCs.
References in corpus (6)
- Coherent Single Photon Emission from Colloidal Lead Halide Perovskite Quantum Dots
- Excitons in core-only, core-shell and core-crown CdSe nanoplatelets: interplay between in-plane electron-hole correlation, spatial and dielectric confinement
- Perspective on Coupled Colloidal Quantum Dot Molecules
- Origins of singlet fission in solid pentacene from an ab initio Green's-function approach
- Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals
- Room temperature single-photon superfluorescence from a single epitaxial cuboid nano-heterostructure