Semiclassical methods face numerical challenges as the dimensionality of the system increases. In the general context of the theory of differential equations, this is known as the curse of dimensionality. In the present manuscript, we apply the recently-introduced multi-coherent states semiclassical initial value representation (MC-SC-IVR) approach to extend the applicability of first-principles semiclassical calculations. The proposed strategy involves the use of non-local coherent states with the goal of increasing accuracy in the Fourier transforms, and on the other hand, allows for the selection of peaks of different frequencies. The ability to filter desired peaks is important for analyzing the power spectra of complex systems. The MC-SC-IVR approach allows us to solve a 19-dimensional test system and to resolve on-the-fly the power spectra of the formaldehyde molecule with very few classical trajectories.

Fighting the curse of dimensionality in first-principles semiclassical calculations : Non-local reference states for large number of dimensions / M. Ceotto, G.F. Tantardini, A. Aspuru-Guzik. - In: THE JOURNAL OF CHEMICAL PHYSICS. - ISSN 0021-9606. - 135:21(2011 Dec 06).

Fighting the curse of dimensionality in first-principles semiclassical calculations : Non-local reference states for large number of dimensions

M. Ceotto;G.F. Tantardini;
2011-12-06

Abstract

Semiclassical methods face numerical challenges as the dimensionality of the system increases. In the general context of the theory of differential equations, this is known as the curse of dimensionality. In the present manuscript, we apply the recently-introduced multi-coherent states semiclassical initial value representation (MC-SC-IVR) approach to extend the applicability of first-principles semiclassical calculations. The proposed strategy involves the use of non-local coherent states with the goal of increasing accuracy in the Fourier transforms, and on the other hand, allows for the selection of peaks of different frequencies. The ability to filter desired peaks is important for analyzing the power spectra of complex systems. The MC-SC-IVR approach allows us to solve a 19-dimensional test system and to resolve on-the-fly the power spectra of the formaldehyde molecule with very few classical trajectories.
semiclassical; spectrum; formaldehyde; molecular dynamics; coherent states; initial value representation; multiple coherent states
Settore CHIM/02 - Chimica Fisica
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2434/165697
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