Modular Path Integral Methodology for Exciton-Vibration Dynamics of Extended Systems
Abstract
To address the computational challenges associated with solving the quantum mechanical equations, this work proposes to devise a decomposition of the path integral, which will enable accurate simulation of coupled exciton-vibration dynamics in large molecular aggregates. This decomposition leads to a modular algorithm, which is applicable to large molecular units with anharmonic intramolecular potentials and leads to linear scaling with system size. The modular path integral methodology will help elucidate the intriguing effects arising from the interplay of anharmonicity, quantum interference and electronic coupling on the vibrational and exciton dynamics of large organic molecules and molecular aggregates. These effects play a prominent role in conductance along molecular wires, energy funneling in light harvesting complexes, and solar energy harvest. Simulations of molecular heat transport along hydrocarbon chains and of singlet fission in pentacene dimers will clarify important mechanistic aspects of these processes.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Jul 11, 2018
- Source ID
- FA95501810291
Entities
People
- Nancy Makri
Organizations
- Air Force Office of Scientific Research
- United States Air Force
- University of Illinois Urbana–Champaign