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Multiply Resonant Coherent Multidimensional Spectroscopy

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Abstract

Coherent Multidimensional Spectroscopy (CMDS) is a new field that includes both time domain and multiply-resonant frequency domain approaches. Multiply-resonant CMDS has attractive features for fully coherent spectroscopy of the quantum states because it 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 paper shows how multiply-resonant CMDS methods use multiple quantum coherences containing a diverse mixture of electronic and vibrational states to measure quantum state resolved intra-state couplings and their coherent and incoherent dynamics.

© 2010 Optical Society of America

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