A novel quantum methods to deal with typical system-bath dynamical problems is introduced. Subsystem discrete variable representation and bath coherent-state sets are used to write down a multiconfigurational expansion of the wave function of the whole system. With the help of the Dirac-Frenkel varational principle, simple equations of motion-a kind of Schrodinger-Langevin equation for the subsystem coupled to (pseudo) classical equations for the bath-are derived. True dissipative dynamics at all times is obtained by coupling the bath to a secondary, classical Ohmic bath, which is modeled by adding a friction coefficient in the derived pseudoclassical bath equations. the resulting equations are then solved for a number of model problems, ranging from tunneling to vibrational relaxation dynamics. Comparison of the result with those of exact, multiconfiguration time-dependent Hartree calculations in systems with up to 80 bath oscillators shows that the proposed methods can be very accurate and might be of help in studying realistic problems with very large baths. To this ens, its linear scaling behavior with respect to the number of bath degrees of freedom is shown in practice with model calculations using tens of thousands of bath oscillators.

A local coherent-state approxiamtion to system-bath quantum dynamics / R. Martinazzo, M. Nest, P. Saalfrank, G. F. Tantardini. - In: THE JOURNAL OF CHEMICAL PHYSICS. - ISSN 0021-9606. - 125:19(2006 Nov 21), pp. 194102.194102-194102.194102-16.

A local coherent-state approxiamtion to system-bath quantum dynamics

R. Martinazzo
Primo
;
G. F. Tantardini
Ultimo
2006-11-21

Abstract

A novel quantum methods to deal with typical system-bath dynamical problems is introduced. Subsystem discrete variable representation and bath coherent-state sets are used to write down a multiconfigurational expansion of the wave function of the whole system. With the help of the Dirac-Frenkel varational principle, simple equations of motion-a kind of Schrodinger-Langevin equation for the subsystem coupled to (pseudo) classical equations for the bath-are derived. True dissipative dynamics at all times is obtained by coupling the bath to a secondary, classical Ohmic bath, which is modeled by adding a friction coefficient in the derived pseudoclassical bath equations. the resulting equations are then solved for a number of model problems, ranging from tunneling to vibrational relaxation dynamics. Comparison of the result with those of exact, multiconfiguration time-dependent Hartree calculations in systems with up to 80 bath oscillators shows that the proposed methods can be very accurate and might be of help in studying realistic problems with very large baths. To this ens, its linear scaling behavior with respect to the number of bath degrees of freedom is shown in practice with model calculations using tens of thousands of bath oscillators.
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/2434/28861
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