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Vibrational dephasing in molecular mixed crystals: A picosecond time domain CARS study of pentacene in naphthalene and benzoic acid

Duppen, Koos and Weitekamp, D. P. and Wiersma, Douwe A. (1983) Vibrational dephasing in molecular mixed crystals: A picosecond time domain CARS study of pentacene in naphthalene and benzoic acid. Journal of Chemical Physics, 79 (12). pp. 5835-5844. ISSN 0021-9606. http://resolver.caltech.edu/CaltechAUTHORS:DUPjcp83

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Abstract

Multiresonant time-domain coherent anti-Stokes Raman scattering (CARS) experiments have been employed in a study of the decay of vibrational coherences of pentacene doped into naphthalene and benzoic acid. In all cases, the CARS decay is found to be exponential, which indicates that the electronic and vibronic inhomogeneities in this system are strongly correlated. The temperature dependence of vibrational dephasing shows no effect of coupling to the lowest-frequency librational mode of pentacene that is known to dominate electronic dephasing. This surprising result can be understood on basis of a dephasing model where rapid coherence exchange exists between a cold vibrational transition and a corresponding near-resonant librationally hot one. For the 767 cm^−1 vibrational transition, oscillations of the CARS signal as a function of delay are shown to arise from interference at the detector with a nearby naphthalene host signal. An inconsistency with a previously reported spontaneous Raman study is resolved by showing that the signal observed there is actually site-selected fluorescence.


Item Type:Article
Additional Information:Copyright © 1983 American Institute of Physics. Received 1 June 1983; accepted 31 August 1983. The investigations were supported by the Netherlands Foundation for Chemical Research (S.O.N.) with financial aid from the Netherlands Organization for the Advancement of Pure Research (Z.W.O.).
Subject Keywords:MOLECULAR CRYSTALS, NAPHTHALENE, BENZOIC ACID, RAMAN SPECTROSCOPY, VIBRATIONAL STATES, DOPED MATERIALS
Record Number:CaltechAUTHORS:DUPjcp83
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:DUPjcp83
Alternative URL:http://dx.doi.org/10.1063/1.445753
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:10866
Collection:CaltechAUTHORS
Deposited By: Archive Administrator
Deposited On:14 Jun 2008
Last Modified:26 Dec 2012 10:05

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