Abstract

Establishing the correct phase in multidimensional coherent spectroscopy (MDCS) experiments is critical because the interpretation of quantum pathways is based on the phase of their associated spectral features but is not trivial because the phase introduced by experimental conditions can contaminate the signal. Most phase-modulated MDCS (PM-MDCS) experiments study molecular systems for which the spectra can be phased to produce absorptive lineshapes, but this assumption of absorptive lineshapes can break down in more complicated systems. We present a robust technique for correcting the phase in PM-MDCS experiments and demonstrate accurate spectrum phasing for an anharmonic system.

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