A comparative study of ab initio nonradiative recombination rate calculations under different formalisms

TL;DR

This study compares five ab initio formalisms for calculating nonradiative recombination rates in semiconductors, finding that static coupling theory aligns best with experimental data and providing insights into the most appropriate computational approach.

Contribution

The paper systematically evaluates different ab initio formalisms for nonradiative recombination, highlighting the effectiveness of static coupling theory in matching experimental results.

Findings

Static coupling theory yields capture coefficients close to experimental values.

Calculated electron-phonon coupling constants support the use of static coupling.

Arguments are provided for preferring static coupling in semiconductor recombination calculations.

Abstract

Nonradiative carrier recombination is of both great applied and fundamental importance.But the correct ab initio approaches to calculate it remains to be inconclusive. Here we used 5 different formalisms to calculate the nonradiative carrier recombinations of two complex defect structures GaP:Zn_Ga-O_P and GaN:Zn_Ga-V_N, and compared the results with experiments.In order to apply different multiphonon assisted electron transition formalisms, we have calculated the electron-phonon coupling constants by ab initio density functional theory for all phonon modes. Compared with different methods, the capture coefficients calculated by the static coupling theory are 4.30*10^-8 and 1.46*10^-7 cm^3/s for GaP:Zn_Ga-O_P and GaN:Zn_Ga-V_N, which are in good agreement with the experiment results, 4*10^-8 and 3.0*10^-7 cm^3/s respectively. We also provided arguments for why the static coupling theory should be used to calculate the nonradiative decays of semiconductors.