TY - JOUR
T1 - Current theoretical challenges in proton-coupled electron transfer
T2 - Electron-proton nonadiabaticity, proton relays, and ultrafast dynamics
AU - Hammes-Schiffer, Sharon
N1 - Copyright:
Copyright 2011 Elsevier B.V., All rights reserved.
PY - 2011/6/16
Y1 - 2011/6/16
N2 - Proton-coupled electron transfer (PCET) reactions play an important role in a wide range of biological and chemical processes. The motions of the electrons, transferring protons, solute nuclei, and solvent nuclei occur on a wide range of time scales and are often strongly coupled. As a result, the theoretical description of these processes requires a combination of quantum and classical methods. This Perspective discusses three of the current theoretical challenges in the field of PCET. The first challenge is the calculation of electron-proton nonadiabatic effects, which are significant for these reactions because the hydrogen tunneling is often faster than the electronic transition. The second challenge is the modeling of electron transfer coupled to proton transport along hydrogen-bonded networks. The third challenge is the simulation of the ultrafast dynamics of nonequilibrium photoinduced PCET reactions in solution. Insights provided by theoretical studies may assist in the design of more effective catalysts for energy conversion processes.
AB - Proton-coupled electron transfer (PCET) reactions play an important role in a wide range of biological and chemical processes. The motions of the electrons, transferring protons, solute nuclei, and solvent nuclei occur on a wide range of time scales and are often strongly coupled. As a result, the theoretical description of these processes requires a combination of quantum and classical methods. This Perspective discusses three of the current theoretical challenges in the field of PCET. The first challenge is the calculation of electron-proton nonadiabatic effects, which are significant for these reactions because the hydrogen tunneling is often faster than the electronic transition. The second challenge is the modeling of electron transfer coupled to proton transport along hydrogen-bonded networks. The third challenge is the simulation of the ultrafast dynamics of nonequilibrium photoinduced PCET reactions in solution. Insights provided by theoretical studies may assist in the design of more effective catalysts for energy conversion processes.
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U2 - 10.1021/jz200277p
DO - 10.1021/jz200277p
M3 - Article
AN - SCOPUS:79959383570
SN - 1948-7185
VL - 2
SP - 1410
EP - 1416
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 12
ER -