Recent progress in computational exploration and design of functional materials

Abstract

In this review, we summarize our work for the computational study and design of functional materials. Emphasis is laid on computational spectroscopy in the condensed phase as well as exploration of solar light-driven water splitting. In particular, dynamic ab initio methods have been in the focus of recent developments. This has enabled computationally efficient access to spectroscopic signatures, local properties, and innovative analysis of complex systems. Examples involve periodic subsystem density functional theory and density functional perturbation theory as well as (vibrational) spectroscopy such as Raman (optical activity) spectroscopy or sum frequency generation for in-depth study of interfaces. In addition, sophisticated approaches for exploration of water splitting processes are outlined, especially for water oxidation as one of the limiting factors for efficient water splitting devices. In-depth study of water oxidation mechanisms and related reaction networks in combination with (dynamic) consideration of environmental effects has allowed unprecedented new insight and discovery of essential factors influencing water oxidation behaviour, thus paving the way for novel design approaches for more efficient catalysts.