Basis set truncation further clarifies vibrational coherence spectra*

Coherent vibrational oscillations in femtosecond transient-absorption spectra have been interpreted since the 1990s using a model based on Gaussian wavepacket dynamics. The oscillations are often studied using probe-wavelength dependent plots of the oscillation amplitude and phase that are known as vibrational coherence spectra. Here we show that restricting the basis of the wavepacket to a small number of eigenstates clarifies several features in vibrational coherence spectra. Improving the understanding of vibrational coherence signatures will help distinguish them from signatures of electronic coherence that arise from measurements of strongly coupled excitonic states in molecular aggregates and light-harvesting proteins.