Inhomogeneous dephasing masks coherence lifetimes in ensemble measurements

The Journal of Chemical Physics
Kenley M PelzerGregory S Engel

Abstract

An open question at the forefront of modern physical sciences is what role, if any, quantum effects may play in biological sensing and energy transport mechanisms. One area of such research concerns the possibility of coherent energy transport in photosynthetic systems. Spectroscopic evidence of long-lived quantum coherence in photosynthetic light-harvesting pigment protein complexes (PPCs), along with theoretical modeling of PPCs, has indicated that coherent energy transport might boost efficiency of energy transport in photosynthesis. Accurate assessment of coherence lifetimes is crucial for modeling the extent to which quantum effects participate in this energy transfer, because such quantum effects can only contribute to mechanisms proceeding on timescales over which the coherences persist. While spectroscopy is a useful way to measure coherence lifetimes, inhomogeneity in the transition energies across the measured ensemble may lead to underestimation of coherence lifetimes from spectroscopic experiments. Theoretical models of antenna complexes generally model a single system, and direct comparison of single system models to ensemble averaged experimental data may lead to systematic underestimation of coherence lifetimes, ...Continue Reading

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Citations

Jun 20, 2012·Journal of the American Chemical Society·Hyun Woo KimYoung Min Rhee
Jan 2, 2013·The Journal of Physical Chemistry. B·Daryl B WongMichael D Fayer
Apr 11, 2014·The Journal of Physical Chemistry Letters·Justin R CaramGregory S Engel
Apr 5, 2014·The Journal of Chemical Physics·Katherine A Kitney-HayesDavid M Jonas
Sep 12, 2015·Nano Letters·Shuo DongZhi-Heng Loh
Sep 17, 2015·The Journal of Chemical Physics·Peter D DahlbergGregory S Engel
Apr 24, 2015·The Journal of Chemical Physics·Patrick S WalshTimothy S Zwier
Jan 20, 2015·Nature Communications·Elsa CassetteGregory D Scholes
Sep 1, 2019·The Journal of Chemical Physics·Nathanael M KidwellTimothy S Zwier
Apr 15, 2016·Physical Review. E·Giulio G GiusteriFausto Borgonovi
Jul 20, 2021·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·Elisabetta Collini
Jul 24, 2013·The Journal of Physical Chemistry Letters·Andrew F FidlerGregory S Engel
Sep 11, 2021·Annals of Surgical Oncology·Yara W KassamaniAlphonse G Taghian

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