Time domain CMDS is constrained by the narrow range of wavelengths created by an ultrafast pulse but frequency domain CMDS is not. 2D-IR is constrained to strong modes by its short pulse width. There is not enough time to build up a coherence amplitude. This presentation first determines coherence amplitudes for different excitation pulse widths and representative C=O and fingerprint vibrational modes. Then it compares the output coherence amplitudes and output electric field amplitudes for different CMDS methods including fully coherent 2D-IR, stimulated photon echo (SPE), stimulated Raman spectroscopy (SRS and FSRS), Triply Vibrationally Enhanced (TRIVE) spectroscopy, Doubly Vibrationally Enhanced (DOVE) spectroscopy, Coherent Anti-Stokes Raman Spectroscopy (CARS) and partially coherent 2D-IR, pump-probe, and photon echo using typical experimental and molecular parameter values. It also compares homodyne and heterodyne detection.

Schrodinger cat state spectroscopy and the expansion of coherent multidimensional spectroscopy (CMDS) beyond physical chemistry

ACS Spring Meeting 2021

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