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A time–domain method for calculating two-dimensional infrared (2D-IR) spectra is developed and is applied to the case of the amide I band of liquid N,N-dimethylformamide. This method includes the effects of both the diagonal frequency modulations (of individual molecules in the system) and the off-diagonal (intermolecular) vibrational coupling. The effect of the off-diagonal vibrational coupling on...
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