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Nonadiabatic Dynamics of Photoinduced Proton-Coupled Electron Transfer Processes

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Technical Report,01 Sep 2014,31 Mar 2018

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University of Illinois Champaign Urbana United States

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The design of efficient and economical devices for the conversion of solar energy to chemical fuel and electrical power is important for national security and therefore is critical to the mission of the Air Force. Photoinduced proton-coupled electron transfer PCET is essential for a wide range of energy conversion processes in chemical and biological systems. Understanding the underlying principles of photoinduced PCET at a level that allows tuning and control of the ultrafast dynamics is crucial for designing renewable and sustainable energy sources, such as artificial photosynthesis devices and photoelectrochemical cells. Theoretical methodology for simulating the nonadiabatic dynamics of photoinduced PCET reactions in solution has been developed. The electronic potential energy surfaces are generated on-the-fly with a hybrid quantum mechanicalmolecular mechanical approach that describes the solute with a multiconfigurational method in a bath of explicit solvent molecules. The transferring hydrogen nucleus is represented as a quantum mechanical wavefunction calculated with grid-based methods, and surface hopping trajectories are propagated onthe adiabatic electron-proton vibronic surfaces. This approach was applied to an experimentally studied phenol-amine complex in 1,2-dichloroethane.

Subject Categories:

  • Non-electrical Energy Conversion
  • Astrophysics

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