Quantitative understanding and modeling of exciton and charge transfer/transport dynamics in complex and confined molecular environments such as interfaces and disordered molecular wires is crucial for the development and refinement of novel solar light harvesting, energy storage, and quantum sensing devices.  However, despite recent advances in theories and computational methods, a satisfactory and integrative theoretical approach that offers unambiguous interpretation of various spectroscopic and imaging data on exciton and charge transfer/transport dynamics in a consistent manner while also based on well-established molecular level models is difficult to find.  This is because of the confluence of intrinsic quantum nature of excitons and charge carriers and their interactions with environments that have the following three notable features: (i) Energetics that tend to be sensitive to minute molecular level details; (ii) Dynamics and fluctuations spanning a broad range of time and length scales; (iii) Lack of symmetries that disallows reduction of actual dimensionality of calculation and simulation.  The present talk highlights some of our on-going development of theoretical and computational suitable for addressing these issues, which include kinetic Monte Carlo simulations with general quantum rate kernels, new versions of polaron transformed quantum master equation approaches that allow broader class of exciton and charge transport dynamics, and new theories for modeling time resolved spectroscopic and imaging data.  The possibility of integration of these approaches in a consistent manner based on model Hamiltonian and its impact are illustrated by both simple model systems and actual molecular aggregates.

Integrative and coarse-grained quantum simulation approaches for exciton and charge transport dynamics in complex and confined molecular environments

ACS Spring 2022

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