We employ a simple multiconfiguration time-dependent Hartree (MCTDH) ansatz tailored to an effective-mode transformation of environmental variables that brings the bath into a linear chain form. In this form, important (primary) degrees of freedom can be easily identified and treated at a high correlation level, whereas secondary modes are left uncorrelated. The resulting approach scales linearly with the bath dimensions and allows us to easily access recurrence times much longer than usually possible, at a very small computational cost. Test calculations for model atom–surface problems show that the system dynamics is correctly reproduced in the relevant time window, and quantitative agreement is attained for energy relaxation and sticking, particularly in non-Markovian environments. These results pave the way for tackling realistic system-bath quantum dynamical problems on the picosecond scale.

Compact MCTDH Wave Functions for High-Dimensional System-Bath Quantum Dynamics / M. Bonfanti, G.F. Tantardini, K.H. Hughes, R. Martinazzo, I. Burghardt. - In: JOURNAL OF PHYSICAL CHEMISTRY. A, MOLECULES, SPECTROSCOPY, KINETICS, ENVIRONMENT, & GENERAL THEORY. - ISSN 1089-5639. - 116:46(2012 Nov 22), pp. 11406-11413.

Compact MCTDH Wave Functions for High-Dimensional System-Bath Quantum Dynamics

M. Bonfanti;G.F. Tantardini;R. Martinazzo;
2012-11-22

Abstract

We employ a simple multiconfiguration time-dependent Hartree (MCTDH) ansatz tailored to an effective-mode transformation of environmental variables that brings the bath into a linear chain form. In this form, important (primary) degrees of freedom can be easily identified and treated at a high correlation level, whereas secondary modes are left uncorrelated. The resulting approach scales linearly with the bath dimensions and allows us to easily access recurrence times much longer than usually possible, at a very small computational cost. Test calculations for model atom–surface problems show that the system dynamics is correctly reproduced in the relevant time window, and quantitative agreement is attained for energy relaxation and sticking, particularly in non-Markovian environments. These results pave the way for tackling realistic system-bath quantum dynamical problems on the picosecond scale.
TIME-DEPENDENT HARTREE ; REACTION CROSS-SECTIONS ; GAUSSIAN WAVEPACKETS ; MOLECULAR-DYNAMICS ; PACKET PROPAGATION ; PHOTODISSOCIATION ; SCATTERING ; SIMULATIONS ; ALGORITHM ; SURFACE
Settore CHIM/02 - Chimica Fisica
JOURNAL OF PHYSICAL CHEMISTRY. A, MOLECULES, SPECTROSCOPY, KINETICS, ENVIRONMENT, & GENERAL THEORY
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2434/210532
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