Al$_x$Ga$_{1-x}$As crystals with direct 2 eV band gaps from computational alchemy

Abstract

We use alchemical first order derivatives for the rapid yet robust prediction of band structures. The power of the approach is demonstrated for the design challenge of finding Al$_x$Ga$_{1-x}$As semiconductor alloys with large direct band gap using computational alchemy within a genetic algorithm. Dozens of crystal polymorphs are identified for $x>\frac{2}{3}$ with direct band gaps larger than 2\:eV according to HSE approximated density functional theory. Based on a single generalized gradient approximated density functional theory band structure calculation of pure GaAs we observe convergence after visiting only $\sim$800 crystal candidates. The general applicability of alchemical gradients is demonstrated for band structure estimates in III-V and IV-IV crystals as well as for H$_2$ uptake in Sr and Ca-alanate crystals.