Lineshape analysis of coherent multidimensional optical spectroscopy using incoherent light
- Department of Chemistry, Concordia College, Moorhead, Minnesota 56562 (United States)
Coherent two-dimensional electronic spectroscopy using incoherent (noisy) light, I{sup (4)} 2D ES, holds intriguing challenges and opportunities. One challenge is to determine how I{sup (4)} 2D ES compares to femtosecond 2D ES. Here, we merge the sophisticated energy-gap Hamiltonian formalism that is often used to model femtosecond 2D ES with the factorized time-correlation formalism that is needed to describe I{sup (4)} 2D ES. The analysis reveals that in certain cases the energy-gap Hamiltonian is insufficient to model the spectroscopic technique correctly. The results using a modified energy-gap Hamiltonian show that I{sup (4)} 2D ES can reveal detailed lineshape information, but, contrary to prior reports, does not reveal dynamics during the waiting time.
- OSTI ID:
- 22415896
- Journal Information:
- Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 142; ISSN JCPSA6; ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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