Quantum dynamics of a driven two-level molecule with variable dephasing
File(s)
Published version
Author(s)
Type
Journal Article
Abstract
The longitudinal (1) and transverse (2) decay rates of a two-level quantum system have a profound influence
on its evolution. Atomic systems with 2 = 1
21 have been studied extensively, but with the rise of solid-state
quantum devices it is also important to consider the effect of stronger transverse relaxation due to interactions
with the solid environment. Here we study the quantum dynamics of a single organic dye molecule driven by a
laser. We measure the variation of 2 with temperature and determine the activation energy for thermal dephasing
of the optical dipole. Then we measure the second-order correlation function g(2)(τ ) of the light emitted by the
molecule for various ratios 2/1 and saturation parameters S. We show that the general solution to the optical
Bloch equations accurately describes the observed quantum dynamics over a wide range of these parameters,
and we discuss the limitations of the various approximate expressions for g(2)(τ ) that appear in the literature.
DOI:
on its evolution. Atomic systems with 2 = 1
21 have been studied extensively, but with the rise of solid-state
quantum devices it is also important to consider the effect of stronger transverse relaxation due to interactions
with the solid environment. Here we study the quantum dynamics of a single organic dye molecule driven by a
laser. We measure the variation of 2 with temperature and determine the activation energy for thermal dephasing
of the optical dipole. Then we measure the second-order correlation function g(2)(τ ) of the light emitted by the
molecule for various ratios 2/1 and saturation parameters S. We show that the general solution to the optical
Bloch equations accurately describes the observed quantum dynamics over a wide range of these parameters,
and we discuss the limitations of the various approximate expressions for g(2)(τ ) that appear in the literature.
DOI:
Date Issued
2016-12-19
Date Acceptance
2016-12-01
Citation
Physical Review A, 2016, 94 (6)
ISSN
1094-1622
Publisher
American Physical Society
Journal / Book Title
Physical Review A
Volume
94
Issue
6
Copyright Statement
© 2016 The Authors.Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license (https://creativecommons.org/licenses/by/4.0/). Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.
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Subjects
General Physics
02 Physical Sciences
01 Mathematical Sciences
03 Chemical Sciences
Publication Status
Published
Article Number
ARTN 063839