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  • Quantum Interference in the fluorescence of a molecular system

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    Author(s)
    Wang, J
    Wiseman, HM
    Ficek, Z
    Griffith University Author(s)
    Wiseman, Howard M.
    Year published
    2000
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    Abstract
    It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. 77, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifest in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory that explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state ...
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    It has been observed experimentally [H.R. Xia, C.Y. Ye, and S.Y. Zhu, Phys. Rev. Lett. 77, 1032 (1996)] that quantum interference between two molecular transitions can lead to a suppression or enhancement of spontaneous emission. This is manifest in the fluorescent intensity as a function of the detuning of the driving field from the two-photon resonance condition. Here we present a theory that explains the observed variation of the number of peaks with the mutual polarization of the molecular transition dipole moments. Using master equation techniques we calculate analytically as well as numerically the steady-state fluorescence, and find that the number of peaks depends on the excitation process. If the molecule is driven to the upper levels by a two-photon process, the fluorescent intensity consists of two peaks regardless of the mutual polarization of the transition dipole moments. If the excitation process is composed of both a two-step, one-photon process and a one-step, two-photon process, then there are two peaks on transitions with parallel dipole moments and three peaks on transitions with antiparallel dipole moments. This latter case is in excellent agreement with the experiment.
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    Journal Title
    Physical Review A: Atomic, Molecular and Optical Physics
    Volume
    62
    Issue
    1
    Publisher URI
    https://journals.aps.org/pra/issues/62/1
    DOI
    https://doi.org/10.1103/PhysRevA.62.013818
    Copyright Statement
    © 2000 American Physical Society. This is the author-manuscript version of this paper. Reproduced in accordance with the copyright policy of the publisher. Please refer to the journal's website for access to the definitive, published version.
    Subject
    Mathematical sciences
    Physical sciences
    Chemical sciences
    History, heritage and archaeology
    Publication URI
    http://hdl.handle.net/10072/3121
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    • Journal articles

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