McCusker, James - Michigan State University

个人简介

Education B.S. cum laude, 1987, Bucknell University (Major: Chemistry; Minors: Physics, Music) M.S., 1987, Bucknell University (Chemistry, with Charles A. Root) Ph.D., 1992, University of Illinois at Urbana-Champaign (Chemistry, with David N. Hendrickson) Postdoctoral Fellow, 1992-1994, University of North Carolina at Chapel Hill (with Thomas J.Meyer) Academic Appointments Assistant Professor of Chemistry, 1994 – 2001, University of California at Berkeley Associate Professor of Chemistry, 2001 – 2008, Michigan State University Professor of Chemistry, 2008 – 2017, Michigan State University Associate Chair for Research, 2011 – 2013, Department of Chemistry, Michigan State University Director, Center of Research Excellence in Complex Materials (CORE-CM), 2013 – 2017, Michigan State University Michigan State University Foundation Professor in Chemistry, 2017 – present

研究领域

Ultrafast Spectroscopy of Transition Metal Complexes Research efforts in this area are concerned with the short timescale photo-induced dynamics of transition metal complexes. By “short timescale”, we refer to processes occurring between the time a photon is absorbed by a molecule and the point at which that molecule is fully relaxed in its lowest-lying excited state. Some of the questions we are addressing with this research include the following: 1) what is the general timescale for excited-state evolution in transition metal complexes? 2) what is the mechanism of this process? 3) how do the geometric and electronic structures of the compounds, the surrounding medium, and other factors couple to and/or influence this process? and 4) to what extent can we use this information to control excited-state dynamics? Some of these questions are very fundamental in nature, whereas others are geared toward applications involving solar energy conversion or catalysis. What distinguishes this group, we believe, is our ability to carry out both the synthesis and spectroscopic characterization of a wide range of inorganic molecules. This enables us to systematically examine chemical perturbations to excited-state electronic and geometric structure, and as a result, develop a comprehensive picture of how transition metal chromophores absorb and dissipate energy. Electron Exchange and Chemical Dynamics Electron exchange is a term which describes the electrostatic interactions that can exist among unpaired electrons in molecules. Our group is interested in understanding the influence electron exchange has on the chemistry of inorganic compounds. Metal-quinone complexes provide the framework for studying the photophysics of exchange-coupled molecules. The redox activity of the quinone ligand provides a facile mechanism for turning “on” or “off” electron exchange, allowing us to probe the effects of spin coupling on excited-state dynamics in closely related sets of chemical systems. A second area concerns reaction dynamics, where the emphasis is on electron and energy transfer processes in polynuclear metal clusters. Through detailed studies of synthetically tailored molecules, we are examining whether or not the electron exchange interactions present in such clusters plays a functional role in their reactivity.

近期论文

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"Observation of parallel intersystem crossing and charge transfer-state dynamics in [Fe(bpy)3]2+ from ultrafast 2D electronic spectroscopy" Lee, A.; Son, M.; Deegbey, M.; Woodhouse, M. D.; Hart, S. M.; Beissel, H. F.; Cesana, P. T.; Jakubikova, E.; McCusker, J. K.; Schlau-Cohen, G. S. Chem. Sci. 2023, Advance Article. "Exploiting the Marcus inverted region for first-row transition metal-based photoredox catalysis" Chan, A. Y.; Ghosh, A.; Yarranton, J. T.; Twilton, J.; Jin, J.; Arias-Rotondo, D. M.; Sakai, H. A.; McCusker, J. K.; MacMillan, D. W. C. Science 2023, 384, 191-197. "Direct Evidence for Excited Ligand Field State-based Oxidative Photoredox Chemistry of Cobalt(III) Polypyridyl Photosensitizer" Alowakennu, M. M.; Ghosh, A.; McCusker, J. K. J. Am. Chem. Soc. 2023, 145, 20786-20791. "Ligand-Field Spectroscopy of Co(III) Complexes and the Development of a Spectrochemical Series for Low-Spin d6 Charge-Transfer Chromophores" Yarranton, J. T.; McCusker, J. K. J. Am. Chem. Soc. 2022, 144, 12488-12500. "On the use of vibronic coherence to identify reaction coordinates for ultrafast excited-state dyanmics of transition metal-based chromophores" Paulus, B. C.; McCusker, J. K. Faraday Discuss. 2022, 237, 274-299. "Ion-Pair Reorganization Regulates Reactivity in Photoredox Catalysts" Earley, J. D.; Zieleniewska, A.; Ripberger, H. H.; Shin, N. Y.; Lazorski, M. S.; Mast, Z. J.; Sayre, H. J.; McCusker, J. K.; Scholes, G. D.; Knowles, R. R.; Reid, O. G.; Rumbles, G. Nat. Chem. 2022, 14, 746-753. "A Modular Approach to Light Capture and Synthetic Tuning of the Excited-State Properties of Fe(II)-Based Chromophores" Paulus, B. C.; Nielsen, K. C.; Tichnell, C. R.; Carey, M. C.; McCusker, J, K. J. Am. Chem. Soc. 2021, 143, 8086-8098. "Optical and Infrared Spectroelectrochemical Studies of CN-Substituted Bipyridyl Complexes of Ruthenium(II)" Taylor, J. O.; Pižl, M.; Kloz, M.; Rebarz, M.; McCusker, C. E.; McCusker, J. K. Záliš, S.; Hartl, F.; Vlček, A. Inorg. Chem. 2021, 60, 3514-3523. "Mechanistic Origin of Photoredox Catalysis Involving Iron(II) Polypyridyl Chromophores" Woodhouse, M. D.; McCusker, J. K. J. Am. Chem. Soc. 2020, 142, 16229-16233. "Exploiting Chemistry and Molecular Systems for Quantum Information Science" Wasielewski, M. R.; Forbes, M. D. E.; Frank, N. L.; Kowalski, K.; Scholes, G. D.; Yuen-Zhou, J.; Baldo, M. A.; Freedman, D. E. Goldsmith, R. H.; Goodson III, T.; Kirk, M. L.; McCusker, J. K.; Ogilvie, J. P.; Shultz, D. A.; Stoll, S.; Whaley, B. Nat. Rev. Chem. 2020, https://doi.org/10.1038/s41570-020-0200-5. "Leveraging Excited-State Coherence for Synthetic Control of Ultrafast Dynamics" Paulus, B. C.; Adelman, S. L; Jamula, L. L.; McCusker, J. K. Nature 2020, 582, 214-219. "Outer-Sphere Effects on Ligand-Field Excited-State Dynamics: Solvent Dependence of High-Spin to Low-Spin Conversion in [Fe(bpy)3]2+" Miller, J. N.; McCusker, J. K. Chem. Sci. 2020, 11, 5191-5204. "Influence of Electrolyte Composition on Ultrafast Interfacial Electron Transfer in Fe-Sensitized TiO2-Based Solar Cells" Tichnell, C. R.; Miller, J. N.; Liu, C.; Mukherjee, S.; Jakubikova, E.; McCusker, J. K. J. Phys. Chem. C 2020, 124, 1794-1811. "Using Ultrafast X-ray Spectroscopy To Address Questions in Ligand-Field Theory: The Excited State Spin and Structure of [Fe(dcpp)2]2+" Britz, A.; Gawelda, W.; Assefa, T. A.; Jamula, L. L.; Yarranton, J. T.; Galler, A.; Khakhulin, D.; Diez, M.; Harder, M.; Doumy, G.; March, A. M.; Bajnóczi, E.; Németh, Z.; Pápai, M.; Rozsályi, E.; Szemes, D. S.; Cho, H.; Mukherjee, S.; Liu, C.; Kim, T. K.; Schoenlein, R. W.; Southworth, S. H.; Young, L.; Jakubikova, E.; Huse, N.; Vankó, G.; Bressler, C.; McCusker, J. K. Inorg. Chem. 2019, 58, 9341-9350. "Electronic structure in the transition metal block and its implications for light harvesting" McCusker, J. K. Science 2019, 363, 484-488. "Insights into the excited state dynamics of Fe(II) polypyridyl complexes from variable-temperature ultrafast spectroscopy" Carey, M. C.; Adelman, S. L.; McCusker, J. K. Chem. Sci. 2019, 10, 134. "Vibrational Relaxation and Redistribution Dynamics in Ruthenium(II) Polypyridyl-Based Charge-Transfer Excited States: A Combined Electronic and Infrared Absorption Study" Brown, A. M.; McCusker, C. E.; Carey, M. C.; Blanco-Rodríguez, A. M.; Towrie, M.; Clark, I. P.; Vlček, A.; McCusker, J. K. J. Phys. Chem. A 2018, 122, 7941-7953.