We have implemented and studied the continuous-configuration time-dependent self-consistent field scheme, a variation of the multiconfiguration time-dependent Hartree method, which aims to get around the latter's exponential scaling problem, especially with regard to system-bath dynamics. We present applications to quantum dissipative dynamics and an analysis of the computational effort. Namely, propagation times within this scheme scale linearly with the number of bath modes.
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http://dx.doi.org/10.1063/1.3351903 | DOI Listing |
Membranes (Basel)
February 2021
Institut Européen des Membranes, UMR 5635, CNRS, ENSCM, University of Montpellier, 34095 Montpellier, France .
As world demand for clean water increases, reverse osmosis (RO) desalination has emerged as an attractive solution. Continuous RO is the most used desalination technology today. However, a new generation of configurations, working in unsteady-state feed concentration and pressure, have gained more attention recently, including the batch RO process.
View Article and Find Full Text PDFJ Chem Phys
March 2011
Technische Universität München, Theoretische Chemie, Lichtenbergstr. 4, 85747 Garching, Germany.
In this paper, we present benchmark results for dissipative dynamics of a harmonic oscillator coupled to an anharmonic bath of Morse oscillators. The microscopic Hamiltonian has been chosen so that the anharmonicity can be adjusted as a free parameter, and its effect can be isolated. This leads to a temperature dependent spectral density of the bath, which is studied for ohmic and lorentzian cases.
View Article and Find Full Text PDFJ Chem Phys
January 2011
Department of Theoretical Chemistry, Technische Universität München, Lichtenbergstraße 4, 85747 Garching, Germany.
Typical (sub)system-bath quantum dynamical problems are often investigated by means of (approximate) reduced equations of motion. Wavepacket approaches to the dynamics of the whole system have gained momentum in recent years and there is hope that properly designed approximations to the wavefunction will allow one to correctly describe the subsystem evolution. The continuous-configuration time-dependent self-consistent field (CC-TDSCF) and local coherent-state approximation (LCSA) methods, for instance, use a simple Hartree product of bath single-particle-functions for each discrete variable representation (DVR) state introduced in the Hilbert space of the subsystem.
View Article and Find Full Text PDFJ Chem Phys
March 2010
Department of Theoretical Chemistry, Technische Universität Munchen, Lichtenbergstrasse 4, 85747 Garching, Germany.
We have implemented and studied the continuous-configuration time-dependent self-consistent field scheme, a variation of the multiconfiguration time-dependent Hartree method, which aims to get around the latter's exponential scaling problem, especially with regard to system-bath dynamics. We present applications to quantum dissipative dynamics and an analysis of the computational effort. Namely, propagation times within this scheme scale linearly with the number of bath modes.
View Article and Find Full Text PDFJ Phys Chem A
April 2006
Department of Computational Science, National University of Singapore, Kent Ridge, Singapore 119260.
The continuous configuration time-dependent self-consistent field (CC-TDSCF) method is employed to calculate the flux-flux autocorrelation functions for the H + CH4 reaction on the potential energy surface recently developed by Manthe and co-workers. We include up to 10 out of the total 12 degrees of freedom in our calculations, only with the doubly degenerate bending modes involving the motion of the hydrogens in nonreacting CH3 group excluded. Comparison of flux-flux autocorrelation functions obtained by using the exact dynamics method and the CC-TDSCF method shows that the CC-TDSCF method is capable of producing very accurate results.
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