Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 130, Issue 18, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3120771
Keywords
biexcitons; infrared spectra; Liouville equation; molecular orientation; phonon-exciton interactions; water
Funding
- NIGMS NIH HHS [R01 GM059230, GM59230] Funding Source: Medline
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0745892] Funding Source: National Science Foundation
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The two-dimensional vibrational response of the disordered strongly fluctuating OH exciton band in liquid water is investigated using a new simulation protocol. The direct nonlinear exciton propagation generalizes the nonlinear exciton equations to include nonadiabatic time dependent Hamiltonian and transition dipole fluctuations. The excitonic picture is retained and the large cancellation between Liouville pathways is built-in from the outset. The sensitivity of the photon echo and double-quantum-coherence techniques to frequency fluctuations, molecular reorientation, intermolecular coupling, and the two-exciton coherence is investigated. The photon echo is particularly sensitive to the frequency fluctuations and molecular reorientation, whereas the double-quantum coherence provides a unique probe for intermolecular couplings and two-exciton coherence.
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