Practical witness for electronic coherences
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Published version
Author(s)
Johnson, AS
Yuen-Zhou, J
Aspuru-Guzik, A
Krich, JJ
Type
Journal Article
Abstract
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently, it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond exclusively to electronic coherences, and thus such experiments can be used to form a test for electronic vs. vibrational oscillations in such systems. Here, we demonstrate a method for practically implementing such a test, whereby pump-probe signals are taken at several different pulse durations and used to extrapolate to the ultrashort-pulse limit. We present analytic and numerical results determining requirements for pulse durations and the optimal choice of pulse central frequency, which can be determined from an absorptionspectrum. Our results suggest that for numerous systems, the required experiment could be implemented by many ultrafast spectroscopy laboratories using pulses of tens of femtoseconds in duration. Such experiments could resolve the standing debate over the nature of coherences in photosynthetic complexes.
Date Issued
2014-12-29
Date Acceptance
2014-12-01
Citation
Journal of Chemical Physics, 2014, 141 (24)
ISSN
1089-7690
Publisher
AIP Publishing
Journal / Book Title
Journal of Chemical Physics
Volume
141
Issue
24
Copyright Statement
© 2014 AIP Publishing LLC. This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. The version of record is available at http://dx.doi.org/10.1063/1.4903982.
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
LIGHT-HARVESTING COMPLEXES
EXCITED-STATE ABSORPTION
ENERGY-TRANSFER
2-DIMENSIONAL SPECTROSCOPY
PHOTOSYNTHETIC COMPLEXES
PROCESS TOMOGRAPHY
QUANTUM COHERENCE
2D SPECTRA
TEMPERATURE
SYSTEMS
Computer Simulation
Dimerization
Electromagnetic Phenomena
Models, Chemical
Spectrum Analysis
Vibration
Chemical Physics
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Publication Status
Published
Article Number
244109