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The Journal of Physical Chemistry A
Article . 2015 . Peer-reviewed
Data sources: Crossref
MPG.PuRe
Article . 2016
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Laser-Limited Signatures of Quantum Coherence

Authors: Tempelaar, R.; Halpin, A.; Johnson, P.; Cai, J.; Murphy, R.; Knoester, J.; Miller, R.; +1 Authors

Laser-Limited Signatures of Quantum Coherence

Abstract

Quantum coherence is proclaimed to promote efficient energy collection by light-harvesting complexes and prototype organic photovoltaics. However, supporting spectroscopic studies are hindered by the problem of distinguishing between the excited state and ground state origin of coherent spectral transients. Coherence amplitude maps, which systematically represent quantum beats observable in two-dimensional (2D) spectroscopy, are currently the prevalent tool for making this distinction. In this article, we present coherence amplitude maps of a molecular dimer, which have become significantly distorted as a result of the finite laser bandwidth used to record the 2D spectra. We argue that under standard spectroscopic conditions similar distortions are to be expected for compounds absorbing over a spectral range similar to, or exceeding, that of the dimer. These include virtually all photovoltaic polymers and certain photosynthetic complexes. With the distortion of coherence amplitude maps, alternative ways to identify quantum coherence are called for. Here, we use numerical simulations that reproduce the essential photophysics of the dimer to unambiguously determine the excited state origin of prominent quantum beats observed in the 2D spectral measurements. This approach is proposed as a dependable method for coherence identification.

Country
Netherlands
Keywords

Models, Molecular, LIGHT-HARVESTING COMPLEXES, PHOTOSYNTHESIS, Lasers, Molecular Conformation, 2-DIMENSIONAL ELECTRONIC SPECTROSCOPY, PROTEIN, POLYMER, Carbocyanines, VIBRATIONAL COHERENCES, EXCITON DYNAMICS, SPECTRA, Quantum Theory, ENERGY-TRANSFER, TEMPERATURE, Dimerization

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    21
    popularity
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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
21
Top 10%
Average
Top 10%
hybrid