Quantum-Classical Path Integral Simulation of Charge Transfer Reactions

Nancy Makri, University of Illinois at Urbana-Champaign

Usage Details

This allocation will allow continuation of our work, which uses the quantum-classical path integral (QCPI) methodology to simulate the time evolution of a small quantum subsystem in an environment (solvent or biological molecule) that is treated via classical molecular dynamics, and its extension to cases where the phase space density of the environment must be quantized. The QCPI methodology is free of approximations besides the classical trajectory description of the solvent, thus able to capture the delicate dynamical interaction of the quantum system with its environment correctly and at full atomistic complexity. It has already been used on Blue Waters with excellent, practically linear scaling, and has been applied to simulate a charge transfer reaction in solution with unprecedented accuracy. In addition, a recent algorithmic advance has led to a dramatic acceleration of the code which will enable simulations in more demanding cases. We seek a new general allocation in order to apply the QCPI methodology to challenging reactive processes in solution, biomolecules, and materials of importance to photovoltaics.