Simulating two-dimensional correlation spectroscopies with third-order infrared and fifth-order infrared--Raman processes of liquid water

Abstract

To investigate the possibility of measuring the intermolecular and intramolecular anharmonic coupling of balk water, we calculate third-order two-dimensional (2D) infrared (IR) spectra and fifth-order 2D IR-IR-Raman-Raman spectra expressed in terms of four-body correlation functions of optical observables. For this purpose, a multimode Brownian oscillator model of four interacting anharmonic oscillators strongly coupled to their respective heat baths is employed. The nonlinearity of the system-bath interactions is considered to describe thermal relaxation and vibrational dephasing. The linear and nonlinear spectra are then computed in a non-Markovian and nonperturbative regime in a rigorous manner using the discretized hierarchical equations of motion in mixed Liouville-Wigner space (DHEOM-MLWS). The calculated 2D spectra for stretching-bending, bending-librational, stretching-librational, and stretching-translational modes consist of various positive and negative peaks exhibiting essential details of the intermolecular and intramolecular mode-mode interactions under thermal relaxation and dephasing at finite temperature.

arXiv comment12 pages, 7 figures

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Cited by in corpus (7)

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• A Multimode Classical Hierarchical Fokker-Planck Equations Approach to Molecular Vibrations: Simulating Two-Dimensional Spectra
• Twin-Space Representation of Classical Mapping Model in the Constraint Phase Space Representation: Numerically Exact Approach to Open Quantum Systems
• System-Bath Modeling in Vibrational Spectroscopy via Molecular Dynamics: A Machine Learning Framework for Hierarchical Equations of Motion (HEOM)
• sbml4md: A computational platform for System-Bath Modeling via Molecular Dynamics powered by Machine Learning