Quantum-classical path integral simulation of electronic transitions

Nancy Makri, University of Illinois at Urbana-Champaign

Usage Details

The quantum-classical path integral (QCPI) methodology provides a powerful computational tool for simulating the time evolution of condensed phase processes characterized by a few coupled electronic states whose quantum dynamical effects must be treated with high accuracy, while the time evolution of the nuclei can be captured via classical trajectories. The QCPI formulation is free of approximations besides the classical trajectory description of the nuclei, thus able to capture the delicate 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, and recent advances continue to increase the efficiency of the algorithm. We seek a new general allocation in order to apply the QCPI methodology to more challenging reactive processes in solution, to augment the code with the inclusion of zero-point energy of important nuclear degrees of freedom, and to investigate the dynamics of nitrogen vacancy defects in diamond lattices.