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research article

High-order geometric integrators for the local cubic variational Gaussian wavepacket dynamics

Moghaddasi Fereidani, Roya  
•
Vanicek, Jiri J. L.  
January 28, 2024
Journal Of Chemical Physics

Gaussian wavepacket dynamics has proven to be a useful semiclassical approximation for quantum simulations of high-dimensional systems with low anharmonicity. Compared to Heller's original local harmonic method, the variational Gaussian wavepacket dynamics is more accurate, but much more difficult to apply in practice because it requires evaluating the expectation values of the potential energy, gradient, and Hessian. If the variational approach is applied to the local cubic approximation of the potential, these expectation values can be evaluated analytically, but they still require the costly third derivative of the potential. To reduce the cost of the resulting local cubic variational Gaussian wavepacket dynamics, we describe efficient high-order geometric integrators, which are symplectic, time-reversible, and norm-conserving. For small time steps, they also conserve the effective energy. We demonstrate the efficiency and geometric properties of these integrators numerically on a multidimensional, nonseparable coupled Morse potential.

  • Details
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Type
research article
DOI
10.1063/5.0180070
Web of Science ID

WOS:001153167200006

Author(s)
Moghaddasi Fereidani, Roya  
Vanicek, Jiri J. L.  

EPFL

Date Issued

2024-01-28

Publisher

Aip Publishing

Published in
Journal Of Chemical Physics
Volume

160

Issue

4

Article Number

044113

Subjects

Physical Sciences

•

Initial-Value Representation

•

Wave-Packet Dynamics

•

Molecular-Dynamics

•

Composition Constants

•

Quantum Dynamics

•

Photodissociation

•

Algorithm

•

Spectra

•

Propagation

•

Limit

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LCPT  
FunderGrant Number

Horizon 2020 Framework Programmehttps://doi.org/10.13039/100010661

683069-MOLEQULE

European Research Council (ERC) under the European Union

Available on Infoscience
February 23, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/205426
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