Reference : Nonequilibrium thermodynamics of light-induced reactions
Scientific journals : Article
Physical, chemical, mathematical & earth Sciences : Physics
Physics and Materials Science
http://hdl.handle.net/10993/48119
Nonequilibrium thermodynamics of light-induced reactions
English
Penocchio, Emanuele mailto [University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS) >]
Rao, Riccardo mailto [Institute for Advanced Study, Princeton > Simons Center for Systems Biology]
Esposito, Massimiliano mailto [University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS) >]
15-Sep-2021
Journal of Chemical Physics
American Institute of Physics
155
114101
Yes (verified by ORBilu)
International
0021-9606
1089-7690
New York
NY
[en] nonequilibrium thermodynamics ; photochemistry ; chemical reaction network
[en] Current formulations of nonequilibrium thermodynamics of open chemical reaction networks only consider chemostats as free-energy sources sustaining nonequilibrium behaviors. Here, we extend the theory to include incoherent light as a source of free energy. We do so by relying on a local equilibrium assumption to derive the chemical potential of photons relative to the system they interact with. This allows us to identify the thermodynamic potential and the thermodynamic forces driving light-reacting chemical systems out-of-equilibrium. We use this framework to treat two paradigmatic photochemical mechanisms describing light-induced unimolecular reactions—namely, the adiabatic and diabatic mechanisms—and highlight the different thermodynamics they lead to. Furthermore, using a thermodynamic coarse-graining procedure, we express our findings in terms of commonly measured experimental quantities, such as quantum yields.
http://hdl.handle.net/10993/48119

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