(274a) Real Time Electron Dynamics of Chemical and Material Systems

Light-harvesting systems and electronic materials continue to garner significant attention due to their importance in energy conversion and modern technological advances. However, several challenges exist in improving their performance: these multifunctional electronic systems are complex, coupled, many-body systems with structural and electronic interactions with their surrounding environments. To address these issues, we have developed several computational approaches based on real-time, time-dependent density functional theory (RT-TDDFT) to directly predict and probe these complex material systems. Our approach significantly differs from conventional DFT methods in that we can directly calculate real-time dynamical effects in the presence of strong interactions with the surrounding environment. Furthermore, recent RT-TDDFT developments in my group allow us to calculate the electronic and structural properties of large systems (~10,000 atoms), whereas conventional DFT approaches are typically limited to only hundreds of atoms. Using these RT-TDDFT capabilities (in conjunction with custom computational hardware developed in my group), I will highlight our recent work on representative light-harvesting systems and complex materials. By treating these large systems at a quantum-mechanical level of detail, we show that the energy-transfer dynamics in these materials are surprisingly rich and complex. Most importantly, these time-resolved studies provide a new approach to probe real-time energy-transfer mechanisms to understand and tailor these complex systems for realistic engineering applications.