Pengfei Huo of the University of Rochester is supported by a CAREER award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry for theoretical research relevant to solar energy conversion. Huo and coworkers develop new quantum dynamics approaches for investigating photochemical reaction. These reactions are crucial for solar fuel production. In solar-to-fuel reactions, a molecule is excited by absorption of light, and this process allows the molecule to transfer of both electrons and protons to another molecule. A quantitative and predictive understanding of these reactions is hampered by the lack of efficient and accurate theoretical approaches. The Huo group develops new quantum dynamics methods that aim to address these theoretical challenges. They use computational tools to simulate coupled electron and proton transfer reactions in photocatalytic conversions. Such insights inspire new design principles and paradigms for next-generation photocatalytic energy production. Dr. Huo's research program is integrated with an educational component centered on theoretical chemistry, including the 'Journey to the Molecular World' summer school for high school students in the Rochester City School District. This project aims to inspires student curiosity and enthusiasm about molecular science and encourage high school students to pursue higher education in Science, Technology, Engineering, and Mathematics.
On-the-fly quantum dynamics simulation is one of the most desirable approaches to investigate non-equilibrium photochemical reactions. Accurately performing such simulations remains a significant challenge in theoretical chemistry, due to a lack of efficient quantum dynamics methods as well as the discrepancy between diabatic dynamics methods and adiabatic electronic structure calculations. To address these long-standing challenges, Dr. Huo and his team are developing new path-integral quantum dynamics approaches that can accurately simulate non-adiabatic electronic transitions and explicitly incorporate nuclear quantum effects through a classical-like description for all degrees of freedom. They are also developing new propagation schemes that enable a seamless interface between diabatic dynamics methods and adiabatic electronic structure calculations, explicitly avoiding additional efforts to reformulate diabatic dynamics methods to the adiabatic representations. Combining the above two types of techniques, the Huo group is performing on-the-fly simulations to investigate the fundamental mechanisms of photoinduced proton-coupled electron transfer (PI-PCET) reactions which are at the center of many solar energy conversion processes. His team is exploring experimentally-testable mechanistic hypotheses that take advantage of the non-equilibrium and quantum mechanical nature of PI-PCET to achieve new chemical reactivities. These investigations may yield a set of general and widely applicable theoretical tools that can significantly expand the scope of quantum dynamics simulations, as well as provide fundamental knowledge and new design principles to predict and control the reactivities of next-generation photocatalysts.
This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.
