Quantum Interference in the fluorescence of a molecular system

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Title Quantum Interference in the fluorescence of a molecular system
Author Wang, Jin.; Wiseman, Howard Mark; Ficek, Z.
Journal Name Physical Review A: Atomic, Molecular and Optical Physics
Year Published 2000
Place of publication USA
Publisher American Physical Society
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 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.
Peer Reviewed Yes
Published Yes
Publisher URI http://prola.aps.org/browse/PRA
Alternative URI http://dx.doi.org/10.1103/PhysRevA.62.013818
Copyright Statement Copyright 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.
Volume 62
Issue Number 1
Page from 013818.1
Page to 013818.10
ISSN 1050-2947
Date Accessioned 2001-01-01
Language en_AU
Research Centre Centre for Quantum Dynamics
Faculty Faculty of Science
Subject PRE2009-Science & Technology
URI http://hdl.handle.net/10072/3121
Publication Type Article in Scholarly Refereed Journal
Publication Type Code c1

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