Lecture
Van Marum Colloquium/RISE Lecture: Quantum-Derived Kinetics of Photo/electrocatalysis on Metals
- Date
- Tuesday 27 May 2025
- Time
- Location
-
Lecture Hall
Einsteinweg 57
2333 CC Leiden - Room
- C1
RISE is pleased to support the visiting lecture by Prof. Dr. Emily A. Carter as part of the Lorentz workshop, Predicting Barriers for Reactions on Metals, taking place at the Lorentz Center of Leiden University from May 26 to May 28, 2025. Prof. Carter holds the Gerhard R. Andlinger Professorship in Energy and the Environment and serves as a Professor of Mechanical and Aerospace Engineering, the Andlinger Center for Energy and the Environment, and Applied and Computational Mathematics at Princeton University. A passionate advocate for socioeconomic equality and gender equity in science, she prioritized the creation of an associate dean for diversity and inclusion during her tenure as dean of Princeton University to address inequities in STEM. With her distinguished career in both research and science administration, Prof. Carter stands out as an inspiring role model for women pursuing academic and leadership roles in science.
Abstract
I will discuss my group’s multi-level, quantum-mechanics-based simulation methods and their application to assessing reaction mechanisms and energetics of photo/electrocatalysis. While, like most researchers studying chemical reactions at surfaces, we begin our assessments with periodic density functional theory (DFT) - e.g., for structural optimization or molecular dynamics - we frequently do not end there. Pure DFT exchange-correlation (XC) functionals manifest significant errors in predictions of excitation energies relevant for photocatalysis and in predicted ground-state free energetics relevant for electrocatalysis. The physical origin of these errors is well-known: spurious electron self-interaction producing too-easy electron delocalization and the lack of an XC derivative discontinuity yielding too-small excitation (or quasiparticle) energies. These errors are most prominent when studying, e.g., charge transfer or ions in solution, both of which appear in electrocatalysis, or excited-state catalysis as happens in, e.g., plasmonic photocatalysis. In these cases, and others where DFT approximations fail (e.g., CO adsorption on metals), we need to refine the solution further. We do so by identifying a region of the periodic cell that encompasses active sites, solvation shells, etc., and then divide the system into a region to be refined beyond DFT and the remainder of the periodic cell to be described still by DFT. Then our density functional embedding theory is used to derive an exact (within a given XC approximation) interaction potential between the embedded region and its surroundings. That “embedding potential” is then used with higher-level quantum mechanics methods (e.g., multireference perturbation theory and more recently, the random phase approximation) to obtain more accurate energetics for the atoms in the embedded region, an embedded correlated wavefunction theory. I will present selected examples related to electrocatalytic carbon dioxide conversion and photocatalytic ammonia decomposition, where this multi-level theory is necessary to obtain reliable predictions of reaction mechanisms, to thoroughly explain experimental data.
Biography
Emily A. Carter is a renowned scholar and educator (Princeton University’s Inaugural Andlinger Professor in Energy and the Environment) and visionary administrative leader (Princeton’s Andlinger Center for Energy and Environment Founding Director, Princeton’s Dean of Engineering and Applied Science, UCLA’s Executive Vice Chancellor and Provost, now Princeton Plasma Physics Laboratory’s Senior Strategic Advisor and Associate Laboratory Director for Applied Materials and Sustainability Sciences) with a research career spanning chemistry, materials science, mechanical and aerospace engineering, and applied/computational mathematics/physics. She pioneered development and application of quantum simulation techniques enabling design of materials and processes for sustainable energy and carbon mitigation. She has co-authored over 475 publications, patents, and codes; mentored nearly 100 postdoctoral fellows and Ph.D. students; and delivered over 600 invited, keynote, and plenary lectures worldwide. Her many honors include election to the U.S. National Academy of Sciences, American Academy of Arts and Sciences, U.S. National Academy of Inventors, U.S. National Academy of Engineering, European Academy of Sciences, and as Foreign Member of Great Britain’s Royal Society. She strategically lends her expertise to various entities, from the U.S. National Academies (recently chairing a three-year Congressionally mandated study on carbon utilization) to private science foundations (launching an initiative for the Simons Foundation on solar radiation management science and serving on the Kavli Foundation’s board of directors) to the federal government (member of multiple national lab advisory and review boards) to advising companies (e.g., chairing a new scientific advisory board for a direct ocean capture company).
About RISE
RISE (Researchers In Science for Equality) is the network for female scientists of the Faculty of Science. RISE strives to create a community where female beta scientists can share their knowledge and experience with each other, but also to increase the diversity at the Faculty and improve the visibility of female top scientists.