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.

References in corpus (10)

• Relativistic separable dual-space Gaussian Pseudopotentials from H to Rn
• Fast and Accurate Modeling of Molecular Atomization Energies with Machine Learning
• The virtual crystal approximation revisited: Application to dielectric and piezoelectric properties of perovskites
• Machine Learning Energies of 2 M Elpasolite (ABC${}_2$D${}_6$) Crystals
• Unfolding the band structure of disordered solids: from bound states to high-mobility Kane fermions
• Inverse Quantum Chemistry: Concepts and Strategies for Rational Compound Design
• Accurate Ab-initio Predictions of III-V Direct-Indirect Band Gap Crossovers
• Fast and accurate predictions of covalent bonds in chemical space
• Low-Energy Polymeric Phases of Alanates
• Exploring water adsorption on isoelectronically doped graphene using alchemical derivatives

Cited by in corpus (10)

• Operators in Machine Learning: Response Properties in Chemical Space
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• Modeling the Ga/As binary system across temperaturesand compositions from first principles
• Effects of perturbation order and basis set on alchemical predictions
• Alchemical geometry relaxation
• Evolutionary Monte Carlo of QM properties in chemical space: Electrolyte design
• Extending the definition of atomic basis sets to atoms with fractional nuclear charge
• Alchemical perturbation density functional theory (APDFT)
• Antisymmetry rules of response properties in certain chemical spaces