Exploring water adsorption on isoelectronically doped graphene using alchemical derivatives

Abstract

The design and production of novel 2-dimensional materials has seen great progress in the last decade, prompting further exploration of the chemistry of such materials. Doping and hydrogenating graphene is an experimentally realised method of changing its surface chemistry, but there is still a great deal to be understood on how doping impacts on the adsorption of molecules. Developing this understanding is key to unlocking the potential applications of these materials. High throughput screening methods can provide particularly effective ways to explore vast chemical compositions of materials. Here, alchemical derivatives are used as a method to screen the dissociative adsorption energy of water molecules on various BN doped topologies of hydrogenated graphene. The predictions from alchemical derivatives are assessed by comparison to density functional theory. This screening method is found to predict dissociative adsorption energies that span a range of more than 2 eV, with a mean absolute error $<0.1$ eV. In addition, we show that the quality of such predictions can be readily assessed by examination of the Kohn-Sham highest occupied molecular orbital in the initial states. In this way, the root mean square error in the dissociative adsorption energies of water is reduced by almost an order of magnitude (down to $\sim 0.02$ eV) after filtering out poor predictions. The findings point the way towards a reliable use of first order alchemical derivatives for efficient screening procedures.

References in corpus (8)

• The electronic properties of graphene
• Control of graphene's properties by reversible hydrogenation
• Machine Learning Energies of 2 M Elpasolite (ABC${}_2$D${}_6$) Crystals
• Water on hexagonal boron nitride from diffusion Monte Carlo
• How strongly do hydrogen and water molecules stick to carbon nanomaterials?
• Fast and accurate predictions of covalent bonds in chemical space
• Water on BN doped benzene: A hard test for exchange-correlation functionals and the impact of exact exchange on weak binding
• Tuning dissociation using isoelectronically doped graphene and hexagonal boron nitride: water and other small molecules

Cited by in corpus (12)

• Atoms in molecules from alchemical perturbation density functional theory
• Rapid and accurate molecular deprotonation energies from quantum alchemy
• Al${}_x$Ga${}_{1-x}$As crystals with direct 2 eV band gaps from computational alchemy
• Effects of perturbation order and basis set on alchemical predictions
• Arbitrarily Precise Quantum Alchemy
• Alchemical geometry relaxation
• Ab initio machine learning in chemical compound space
• Alchemical perturbation density functional theory (APDFT)
• Extending the definition of atomic basis sets to atoms with fractional nuclear charge
• Antisymmetry rules of response properties in certain chemical spaces
• Simplifying inverse material design problems for fixed lattices with alchemical chirality
• Alchemical normal modes unify chemical space