Non-Markovian dephasing of molecules in solution measured with three-pulse femtosecond photon echoes

The electronic dephasing of large molecules in solution is investigated with three-pulse photon echoes generated by 6-fs optical pulses. The observed dephasing behavior, which is analyzed with a model based on a stochastic coupling of the molecules with their heat bath, is clearly shown to be non-Ma...

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Bibliographic Details
Published in:Physical review letters 1991-03, Vol.66 (9), p.1138-1141
Main Authors: BIGOT, J.-Y, PORTELLA, M. T, SCHOENLEIN, R. W, BARDEEN, C. J, MIGUS, A, SHANK, C. V
Format: Article
Language:English
Subjects:
640302 - Atomic, Molecular & Chemical Physics- Atomic & Molecular Properties & Theory
ATOMIC AND MOLECULAR PHYSICS
CORRELATION FUNCTIONS
COUPLING
DATA
DISPERSIONS
Exact sciences and technology
EXPERIMENTAL DATA
FLUCTUATIONS
FUNCTIONS
Fundamental areas of phenomenology (including applications)
HEAT SINKS
INFORMATION
MIXTURES
MOLECULES
NUMERICAL DATA
Optics
Physics
PULSES
QUANTUM ELECTRONICS
Quantum optics
SINKS
SOLUTIONS
SOLVENTS
STOCHASTIC PROCESSES
THEORETICAL DATA
TIME DEPENDENCE
VARIATIONS
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Summary:The electronic dephasing of large molecules in solution is investigated with three-pulse photon echoes generated by 6-fs optical pulses. The observed dephasing behavior, which is analyzed with a model based on a stochastic coupling of the molecules with their heat bath, is clearly shown to be non-Markovian. Moreover, the correlation function of the fluctuations asymptotically approaches an exponential with characteristic times varying from 20 to 80 fs, depending on the solvent environment.
ISSN:0031-9007
1079-7114
DOI:10.1103/PhysRevLett.66.1138