Multiple coherent states for first-principles semiclassical initial value representation molecular dynamics.
A multiple coherent states implementation of the semiclassical approximation is introduced and employed to obtain the power spectra with a few classical trajectories. The method is integrated with the time-averaging semiclassical initial value representation to successfully reproduce anharmonicity and Fermi resonance splittings at a level of accuracy comparable to semiclassical simulations of thousands of trajectories. The method is tested on two different model systems with analytical potentials and implemented in conjunction with the first-principles molecular dynamics scheme to obtain the power spectrum for the carbon dioxide molecule.
Ceotto
Michele
M
Dipartimento di Chimica Fisica ed Elettrochimica, Università degli Studi di Milano, via Golgi 19, 20133 Milano, Italy. michele.ceotto@unimi.it
Atahan
Sule
S
Tantardini
Gian Franco
GF
Aspuru-Guzik
Alán
A