Advanced quantum and semiclassical methods for simulating photoinduced molecular dynamics and spectroscopy

Abstract

Molecular-level understanding of photoinduced processes is critically important for breakthroughs in transformative technologies utilizing light, ranging from photomedicine to photoresponsive materials. Theory and simulation play a crucial role in this task. Despite great advances in hardware and computational methods, the theoretical description of photoinduced phenomena in the presence of complex environments and external photoexcitation conditions still poses formidable challenges for theoreticians and there are numerous formal and computational difficulties that must be overcome. The development of predictive, accurate, and at the same time, computationally efficient theoretical approaches to describe complex problems in photochemistry and photophysics is an active field of research in contemporary theoretical and computational chemistry. In this advanced review, we discuss modern computational advances and novel approaches that have been recently developed in excited-electronic structure methods, and multiscale modeling, with a special emphasis on coupled electron-nuclear dynamics and spectroscopy, from fully quantum to semi-classical methodologies—including dissipative effects, the explicit light field interaction, femtosecond time-resolved spectroscopy, and software infrastructure. This article is categorized under: Software > Quantum Chemistry Electronic Structure Theory > Combined QM/MM Methods Theoretical and Physical Chemistry > Spectroscopy Software > Molecular Modeling.