Coulomb matrix elements for the impact ionization process in nanocrystals: the envelope function approach

TL;DR

This paper introduces a method to calculate Coulomb matrix elements in semiconductor nanocrystals using the envelope function approach, revealing size-dependent scaling and state mixing effects relevant for impact ionization.

Contribution

It provides a novel calculation framework for Coulomb interactions in nanocrystals that accounts for Bloch functions and size scaling, improving understanding of exciton-biexciton coupling.

Findings

Coulomb matrix elements scale as 1/R^2 with nanocrystal radius.

Biexciton states show power-law scaling with coupling strength.

Biexciton admixture to exciton states can reach 80% at high energies.

Abstract

We propose a method for calculating Coulomb matrix elements between exciton and biexciton states in semiconductor nanocrystals based on the envelope function formalism. We show that such a calculation requires proper treatment of the Bloch parts of the carrier wave functions which, in the leading order, leads to spin selection rules identical to those holding for optical interband transitions. Compared to the usual (intraband) Coulomb couplings, the resulting matrix elements are additionally scaled by the ratio of the lattice constant to the nanocrystal radius. As a result, the Coulomb coupling between exciton and biexciton states scale as 1/R^2. We present also some statistical estimates of the distribution of the coupling magnitudes and energies of the coupled states The number of biexciton states coupled to exciton states form a certain energy range shows a power-law scaling with the ratio of the coupling magnitude to the energy separation. We estimate also the degree of mixing between exciton and biexciton states. The amount of biexciton admixture to exciton states at least 1 eV above the multiple exciton generation threshold can reach 80% but varies strongly with the nanocrystal size.