Quantum Monte Carlo simulations of Energy Materials

Can Ataca,Department of Physics

Rational design of new materials that are optimized to take maximum advantage of charge storage in both transition metals and oxygen requires deep theoretical understanding and predictive computation of the bonding characteristics, structural stability and redox reaction energies in materials exhibiting such phenomena. Unfortunately, currently there are no fully first-principles methods that can reliably describe charge transfer in d-orbitals. We propose to develop high-accuracy first principles computational methods required to make progress on the understanding and design of future materials with increased energy density due to reversible activity of oxygen coupled to transition metals. Specifically, we will apply quantum Monte Carlo (QMC) methods to understand how bonding occurs in Li-rich layered oxide materials, and to accurately predict operating voltages and energies of the d-states of transition-metal atoms without any empirical parameters. The QMC results will serve as a critical benchmark for calibrating DFT-based methods for the accurate materials design of such systems.