Sharon Hammes-Schiffer
About
Biography
Sharon Hammes-Schiffer received her B.A. from Princeton University and her Ph.D. from Stanford University, followed by two years at AT&T Bell Labs. She was the Clare Boothe Luce Assistant Professor at the University of Notre Dame from 1995-2000 and spent the next twelve years at The Pennsylvania State University as the Eberly Professor of Biotechnology. She became the Swanlund Professor of Chemistry at the University of Illinois Urbana-Champaign in 2012 and the Kirkwood Professor of Chemistry at Yale University in 2018. Her research centers on the investigation of charge transfer reactions, dynamics, and quantum mechanical effects in chemical, biological, and interfacial processes. Her work encompasses the development of analytical theories and computational methods, as well as applications to a wide range of experimentally relevant systems. She is a Fellow of the APS, ACS, AAAS, and Biophysical Society. She is a member of the American Academy of Arts and Sciences, National Academy of Sciences, and International Academy of Quantum Molecular Science. She is the Editor-in-Chief of Chemical Reviews and on the Board of Reviewing Editors for Science.
Education & Training
- Postdoctoral Research Scientist
- AT&T Bell Laboratories (1995)
- PhD
- Stanford University, Chemistry (1993)
- BA
- Princeton University, Chemistry (1988)
Research
Overview
Research in the Hammes-Schiffer group centers on the development and application of theoretical and computational methods for describing chemical reactions in condensed phases and at interfaces. Our overall objective is to elucidate the fundamental physical principles underlying charge transfer reactions, dynamics, and quantum mechanical effects in chemical, biological, and interfacial processes. Our research encompasses the development of analytical theories and computational methods, as well as applications to a wide range of experimentally relevant systems. The group is divided into three general areas: proton-coupled electron transfer reactions, enzymatic processes, and non-Born-Oppenheimer electronic structure methods.
Proton-coupled electron transfer (PCET) reactions play a critical role in a wide range of chemical and biological processes. We have developed a general theory for PCET, which allows the calculation of rate constants and deuterium kinetic isotope effects, and have applied this theory to experimentally studied reactions in solution, proteins, and electrochemistry. We have also developed methodology to simulate the nonadiabatic ultrafast dynamics of photoinduced PCET reactions. Applications of these theories have assisted in the interpretation of experimental data and provided experimentally testable predictions. Our calculations have also guided the design of molecular electrocatalysts and photocatalysts for energy conversion devices such as solar cells. Current applications within the group center on PCET in photoreduced metal-oxide nanocrystals, artificial photosynthetic systems, electrode/solution interfaces, and photoreceptor proteins.
Our studies of enzymatic processes have focused on the catalytic roles of protein motion, hydrogen bonding, hydrogen tunneling, electrostatics, conformational sampling, and metal ions. To study these properties, we have developed hybrid quantum/classical molecular dynamics approaches, as well as methods for calculating the vibrational shifts of nitrile probes in enzyme active sites. Current applications within the group include DNA polymerases, ribozymes, and various metalloenzymes.
Our group has also developed the nuclear-electronic orbital (NEO) method for incorporating nuclear quantum effects and non-Born-Oppenheimer effects into electronic structure calculations. In the NEO approach, specified nuclei are treated quantum mechanically on the same level as the electrons using molecular orbital techniques. Our current focus is on the development of multicomponent density functional theory (NEO-DFT), which treats both electrons and specified protons quantum mechanically with a proper description of electron-electron and electron-proton correlation effects. This method includes proton delocalization and zero point energy directly into geometry optimizations, reaction paths, and dynamics and avoids the Born-Oppenheimer separation between electrons and protons in a computationally practical manner. An analogous time-dependent DFT approach, NEO-TDDFT, enables the calculation of excited electron-proton vibronic states.