Discretized hierarchical equations of motion in mixed Liouville--Wigner space for two-dimensional vibrational spectroscopies of liquid water
arXiv:2302.09799 · doi:10.1063/5.0135725
Abstract
A model of a bulk water system describing the vibrational motion of intramolecular and intermolecular modes is constructed, enabling analysis of its linear and nonlinear vibrational spectra, as well as the energy transfer processes between the vibrational modes. The model is described as a system of four interacting anharmonic oscillators nonlinearly coupled to their respective heat baths. To perform a rigorous numerical investigation of the non-Markovian and nonperturbative quantum dissipative dynamics of the model, we derive discretized hierarchical equations of motion in mixed Liouville-Wigner space (DHEOM-MLWS), with Lagrange-Hermite mesh discretization being employed in the Liouville space of the intramolecular modes and Lagrange-Hermite mesh discretization and Hermite discretization in the Wigner space of the intermolecular modes. One-dimensional infrared and Raman spectra and two-dimensional terahertz-infrared-visible and infrared-infrared-Raman spectra are computed as demonstrations of the quantum dissipative description provided by our model.
14 pages 6 figures
References in corpus (10)
- Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
- Reduced hierarchical equations of motion in real and imaginary time: Correlated initial states and thermodynamic quantities
- Real-Time and Imaginary-Time Quantum Hierarchal Fokker-Planck Equations
- On the Consistency of Approximate Quantum Dynamics Simulation Methods for Vibrational Spectra in the Condensed Phase
- Removing instabilities in the hierarchical equations of motion: exact and approximate projection approaches
- Analysis of 2D THz-Raman spectroscopy using a non-Markovian Brownian oscillator model with nonlinear system-bath interactions
- On the Applicability of the Caldeira-Leggett Model to Condensed Phase Vibrational Spectroscopy
- Low-Temperature Quantum Fokker-Planck and Smoluchowski Equations and Their Extension to Multistate Systems
- Parametrizing linear generalized Langevin dynamics from explicit molecular dynamics simulations
- A simple improved low temperature correction for the hierarchical equations of motion