Pengfei Huo of the University of Rochester is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to theoretically investigate new types of reactions caused by interactions between molecules and light. Discovering new types of reactions is a central goal of Chemistry. When molecules and light are introduced into small, confined spaces new possibilities arise for how they interact. One possible outcome is the generation of "entangled" molecule-photon states, which is a feature that arises due to the quantum mechanical nature of light and matter. Understanding how these systems change over time will uncover design principles that should lead to new, unexpected chemical transformations. However, simulating these systems accurately is one of the most challenging tasks in modern theoretical chemistry. To address this challenge, the PI and his group develop and apply new approaches to investigate this cavity-induced entangled photochemistry. These investigations provide fundamental knowledge about quantum light-matter-interaction-induced chemistry. Dr. Huo is organizing international conferences that focus on this emerging field to facilitate advances that could lead to new technologies and applications using systems of this type.
Coupling molecules to a quantized radiation field in an optical cavity has shown great promise to enable new paradigms for chemical reactivities and transformations. The resulting new photon-matter entangled states, so-called polaritons, have new conical intersections or avoid crossings which significantly influence the photochemistry of molecules, and thus, open up new possibilities to tune and control chemical reactivities. The non-adiabatic dynamics of such hybrid matter-field systems remains unclear and beyond the usual paradigm of photochemistry which does not include quantum photons, or quantum optics which has not focused on molecules. Theoretical investigations play a vital role in understanding the fundamental limits and new principles in this emerging field. However, existing approaches and models that are commonly used in quantum optics are significantly limited by their scope and applicability for describing photochemistry. To provide fundamental knowledge in this emerging field, located between photochemistry and quantum optics, the PI and his research group are (1) investigating the fundamental limit, the basic mechanisms, and new principles in cavity quantum electrodynamics (QED) induced photochemistry, and (2) developing accurate and efficient path-integral based approaches to simulate quantum transitions among polariton states induced by cavity QED. The results of these investigations provide the fundamental understanding of quantum light-matter induced chemistry and new theoretical approaches that facilitate the merger of quantum optics and photochemistry. The conferences organized by the PI will stimulate new approaches in the field that can expand its potential impact.
This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.
