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Accurate description of finite-temperature vibrational dynamics isindispensable in the computation of two-dimensional electronic spectra. Suchsimulations are often based on the density matrix evolution, statisticalaveraging of initial vibrational states, or approximate classical orsemiclassical limits. While many practical approaches exist, they are often oflimited accuracy and difficult to interpret. Here, we use the concept ofthermo-field dynamics to derive an exact finite-temperature expression thatlends itself to an intuitive wavepacket-based interpretation. Furthermore, anefficient method for computing finite-temperature two-dimensional spectra isobtained by combining the exact thermo-field dynamics approach with the thawedGaussian approximation for the wavepacket dynamics, which is exact for anydisplaced, distorted, and Duschinsky-rotated harmonic potential but alsoaccounts partially for anharmonicity effects in general potentials. Using thisnew method, we directly relate a symmetry breaking of the two-dimensionalsignal to the deviation from the conventional Brownian oscillator picture.

the journal of physical chemistry letters

Finite-temperature, anharmonicity, and Duschinsky effects on the  two-dimensional electronic spectra from ab initio thermo-field Gaussian  wavepacket dynamics