Fundamental understanding of visible light-activated excited state chemistry is of great importance in elucidating the mechanisms, structures, and design features for catalysis, energy, and biomedicine. Important chemical reactions such as CO2 reduction, water-splitting, and electron transfer in novel inorganic materials are revealed by spectroscopic probes of excited-state manifolds and charge transfer pathways leading to observable reaction intermediates or products. The light-harvesting properties of these soft nanomaterials can be tuned through core-molecule-shell fabrication schemes that will alter the size, shape, and material composition to include both traditional plasmonic metals to earth abundant metal composites exhibiting novel plasmonic surface effects in the near ultraviolet to visible regime. Modern optical spectroscopy techniques are then utilized to map out these dynamics across multiple timescales—from the seconds timescale of oxygen-evolving reactions to the ultrafast timescales of nuclear and vibrational motion with microscopic detail. The Klein group aims to deepen our understanding and expand the scope of nanoscale photocatalysis by mapping dynamics in extreme interaction regimes for enhanced localized control over plasmon-driven chemistry. More generally, we seek to address the challenges the world faces in renewable energy, photovoltaics, and nanomedicine by elucidating the fundamental photophysical and photochemical processes that underlie important light-driven chemical reactions in soft nanomaterials.
Areas of Interest
- Photo-electrochemistry & Catalysis
- Single Nanoparticle Optical Spectroscopy
- Vibrational Spectroscopy
- Optical/X-ray Transient Absorption Spectroscopy
- Surface Science and Soft Nanomaterials
- 2018 – Ph.D.: Northwestern University
- 2012 – B.S.: University of Illinois at Urbana-Champaign
E. A. Sprague-Klein, M. O. McAnally, D. V. Zhdanov, A. B. Zrimsek, V. A. Apkarian, T. Seideman, G. C. Schatz, and R. P. Van Duyne, “Observation of Single Molecule Plasmon-Driven Electron Transfer in Isotopically Edited 4,4’-Bipyridine Gold Nanosphere Oligomers.” Journal of the American Chemical Society, 2017, 139, 15212-15221.
B. Negru, M. O. McAnally, H. E. Mayhew, T. W. Ueltschi, L. Peng, E. A. Sprague-Klein, G. C. Schatz, and R. P. Van Duyne, “Fabrication of Gold Nanosphere Oligomers for Surface-Enhanced Femtosecond Stimulated Raman Spectroscopy.” Journal of Physical Chemistry C, 2017, 121, 27004-27008.
E. A. Sprague-Klein, B. Negru, L. R. Madison, S. C. Coste, B. K. Rugg, A. M. Felts, M. O. McAnally, M. Banik, V. A. Apkarian, M. R. Wasielewski, M. A. Ratner, T. Seideman, G. C. Schatz, R. P. Van Duyne, “Photoinduced Plasmon-Driven Chemistry in trans-1,2-Bis(4-pyridyl)ethylene Gold Nanosphere Oligomers.” Journal of the American Chemical Society, 2018, 140, 10583-10592.
B. V. Kramer, B. T. Phelan, E. A. Sprague-Klein, B. T. Diroll, S. Lee, K. Otake, R. Palmer, M. W. Mara, O. K. Farha, J. T. Hupp, L. X. Chen, “Single-Atom Metal Oxide Sites as Traps for Charge Separation in nano Zr-MOF NDC-NU-1000.” ACS Energy & Fuels, 2021, 35, 23, 19081–19095.
E. A. Sprague-Klein, R. Ho-Wu, D. Nguyen, S. C. Coste, Y. Wu, T. Seideman, G. C. Schatz, R. P. Van Duyne, “Modulating the Electron Affinity of Polypyridine Molecules on Single Gold Nanoparticles for Plasmon-Driven Electron Transfer.” Journal of Physical Chemistry C, 2021, 125, 40, 22142-22153.
L. Gimeno, B. Phelan, E.A. Sprague-Klein, T. Roisnel, E. Blart, C. Gourlaouen, L.X. Chen, Y. Pellegrin. A very bulky and stable copper(I)-phenanthroline complex: impact of steric strain and symmetry on the excited state properties. Inorganic Chemistry, 2022, 61, 19, 7296–7307.
E. A. Sprague-Klein, X. He, M. W. Mara, B. J. Reinhart, S. Lee, L. M. Utschig, K. L. Mulfort, L. X. Chen, D. M. Tiede. “Photo-Electrochemical Effect in the Water Oxidation Catalyst Cobalt-Phosphate (CoPi).” ACS Energy Letters, 2022 (Under Review).