Multiply Resonant Coherent Multidimensional Spectroscopy: Implications for Materials Science

Abstract

Coherent multidimensional spectroscopy (CMDS) has greatly expanded the capabilities of molecular spectroscopy, and it promises to be equally important for materials chemistry. CMDS includes both time domain and multiply resonant frequency domain approaches. Although time domain CMDS has dominated applications, new work shows that multiply resonant CMDS has attractive features for fully coherent spectroscopy of the quantum states that are important for materials spectroscopy. Rather than resolving the temporal oscillations of each coherence, multiply resonant CMDS is an older method that measures the resonance enhancements for different excitation frequencies. It does not require the long-term phase coherence that restricts the coherent pathways and quantum states accessible by time domain methods. This Perspective reviews the multiply resonant CMDS vibrational methods and shows how they can be adapted to the diverse electronic and vibrational states of materials chemistry.