Real-Time Electron-Nuclear Dynamics of Large Material Systems with Density Functional Tight Binding Approaches

In this talk, I will present two applications from our recently developed real-time time-dependent density functional tight-binding (RT-TDDFTB) approach for simulating excited-state electron–nuclear dynamics in large, complex, periodic condensed matter systems. These simulations go beyond the capabilities and scope of traditional adiabatic Born–Oppenheimer molecular dynamics (BOMD) simulations or conventional time-dependent density functional theory (TDDFT), especially for large periodic nanoscale systems and long picosecond time scales. The first application of our RT-TDDFTB approach focuses solvent-mediated electron–nuclear dynamics to give a wholistic approach for exploring excited-state processes, such as hot carrier transport in nanomaterials in solvated environments. The second topic will highlight photoinduced degradation of chemical systems on a plasmonic Au(111) surface with visible light. Collectively, these examples highlight the capability of RT-TDDFTB to enable mechanistic insight into electron–nuclear dynamics in condensed-phase systems and provide a comprehensive paradigm for exploring time-resolved excited-state dynamics of large chemical/material systems in realistic environments.