Nonequilibrium steady-state picture of incoherent light-induced excitation harvesting
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F20%3A10422757" target="_blank" >RIV/00216208:11320/20:10422757 - isvavai.cz</a>
Result on the web
<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=-s-E86K..M" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=-s-E86K..M</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1063/5.0029918" target="_blank" >10.1063/5.0029918</a>
Alternative languages
Result language
angličtina
Original language name
Nonequilibrium steady-state picture of incoherent light-induced excitation harvesting
Original language description
We formulate a comprehensive theoretical description of excitation harvesting in molecular aggregates photoexcited by weak incoherent radiation. An efficient numerical scheme that respects the continuity equation for excitation fluxes is developed to compute the nonequilibrium steady state (NESS) arising from the interplay between excitation generation, excitation relaxation, dephasing, trapping at the load, and recombination. The NESS is most conveniently described in the so-called preferred basis in which the steady-state excitonic density matrix is diagonal. The NESS properties are examined by relating the preferred-basis description to the descriptions in the site or excitonic bases. Focusing on a model photosynthetic dimer, we find that the NESS in the limit of long trapping time is quite similar to the excited-state equilibrium in which the stationary coherences originate from the excitation-environment entanglement. For shorter trapping times, we demonstrate how the properties of the NESS can be extracted from the time-dependent description of an incoherently driven but unloaded dimer. This relation between stationary and time-dependent pictures is valid, provided that the trapping time is longer than the decay time of dynamic coherences accessible in femtosecond spectroscopy experiments.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)
Result continuities
Project
<a href="/en/project/GA18-18022S" target="_blank" >GA18-18022S: Graphene-based Biomimetic Light-Harvesting Systems</a><br>
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)
Others
Publication year
2020
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
Journal of Chemical Physics
ISSN
0021-9606
e-ISSN
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Volume of the periodical
153
Issue of the periodical within the volume
24
Country of publishing house
US - UNITED STATES
Number of pages
17
Pages from-to
244110
UT code for WoS article
000603068300010
EID of the result in the Scopus database
2-s2.0-85099188554