Semiclassical "Divide-and-Conquer" Method for Spectroscopic Calculations of High Dimensional Molecular Systems

Abstract

A new semiclassical "divide-and-conquer" method is presented with the aim of demonstrating that quantum dynamics simulations of high dimensional molecular systems are doable. The method is first tested by calculating the quantum vibrational power spectra of water, methane, and benzene - three molecules of increasing dimensionality for which benchmark quantum results are available - and then applied to C60, a system characterized by 174 vibrational degrees of freedom. Results show that the approach can accurately account for quantum anharmonicities, purely quantum features like overtones, and the removal of degeneracy when the molecular symmetry is broken.

References in corpus (11)

• Diamondoid Molecules
• Semiclassical Approximations in Phase Space with Coherent States
• First-Principles Semiclassical Initial Value Representation Molecular Dynamics
• On-the-fly ab initio semiclassical dynamics: Identifying degrees of freedom essential for emission spectra of oligothiophenes
• Introduction to Quantum Mechanics
• The Importance of the Pre-exponential Factor in Semiclassical Molecular Dynamics
• Mixed Semiclassical Initial Value Representation Time-Averaging Propagator for Spectroscopic Calculations
• Long-time and unitary properties of semiclassical initial value representations
• Graphics processing units accelerated semiclassical initial value representation molecular dynamics
• Generalized Gaussian wave packet dynamics: Integrable and Chaotic Systems
• Improving the accuracy and efficiency of time-resolved electronic spectra calculations: Cellular dephasing representation with a prefactor

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