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Practical applications of laboratory chemical reactions require affordable, stable and non-toxic components, and metal oxides provide one such platform. Indeed, SiO2 is just sand, Fe2O3 is rust, and TiO2 is a common component of paints, enamels, sunscreens, toothpastes and food. To be used in chemistry, metal oxides are typically modified further by doping, molecular adsorption, nanoscale formulations, sensitization with atomic catalysts, etc. Focusing on solar energy applications, we studied a variety of photochemical processes that occur on metal oxide surfaces.
Invented in 1988, the dye-sensitized TiO2 solar cell, known as the Gratzel cell, is an affordable type of solar cell with relatively high efficiency. Motivated by the need to study quantum dynamics of charges in these systems, we developed novel computational tools and studied various chromophore/TiO2 interfaces.
A. V. Akimov, A. J. Neukirch, O. V. Prezhdo “Theoretical insights into photoinduced charge transfer and catalysis at metal oxide surfaces”, Chem. Rev., 113, 4496 (2013)
W. R. Duncan, O. V. Prezhdo, “Theoretical studies of photoinduced electron transfer in dye-sensitized TiO2”, Ann. Rev. Phys. Chem., 58, 143 (2007)
W. Stier and O. V. Prezhdo, “Non-adiabatic molecular dynamics simulation of light-induced electron transfer from an anchored molecular electron donor to a semiconductor acceptor”, J. Phys. Chem. B, 106 8047 (2002).
Metal oxides are used commonly a photocatalysts. However, the mechanisms of how they operate are often unclear, since relevant molecular states can be populated only transiently, because molecular orbitals reside inside metal oxide conduction or valence bands. The photochemical reactions of interest are complicated by other phenomena, such as polaron formation, proton transfer, and presence of co-catalysts. Our time-domain atomistic quantum dynamics simulations establish the reaction mechanisms, and detail the complex interplay among different processes.
C. Cheng, Y. H. Zhu, W. F. Fang, R. Long, O. V. Prezhdo, “Co Adsorbate Promotes Polaron Photoactivity on the Reduced Rutile TiO2(110) Surface”, JACS Au, 2, 234-245 (2022).
C. Cheng, O. V. Prezhdo, R. Long, W. H. Fang, “Photolysis versus Photothermolysis of N2O on a Semiconductor Surface Revealed by Nonadiabatic Molecular Dynamics”, J. Am. Chem. Soc., 145, 476-486 (2022).
W. B. Chu, S. J. Tan, Q. J. Zheng, W. Fang, Y. X. Feng, O. V. Prezhdo, B. Wang, X. Z. Li, J. Zhao, “Ultrafast Charge Transfer Coupled to Quantum Proton Motion at Molecule/Metal Oxide Interface”, Sci. Adv., 8, eabo2675 (2022).
C. Cheng, W. H. Fang, R. Long, O. V. Prezhdo, “Water Splitting with a Single-Atom Cu/TiO2 Photocatalyst: Atomistic Origin of High Efficiency and Proposed Enhancement by Spin Selection”, JACS Au, 1, 550-559 (2021).
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