QLC: EAGER: New Chemical Reactivity Enabled by Cavity Quantum Electrodynamics

罗彻斯特大学的霍鹏飞教授获得了化学系化学理论、模型和计算方法项目的奖项，从理论上研究由分子与光之间的相互作用引起的新型反应。发现新的反应类型是化学的中心目标。当分子和光被引入狭小的密闭空间时，它们如何相互作用就产生了新的可能性。一种可能的结果是产生“纠缠”的分子-光子状态，这是由于光和物质的量子力学性质而产生的特征。了解这些系统如何随着时间的推移而变化，将揭示设计原则，应该导致新的，意想不到的化学转化。然而，准确地模拟这些体系是现代理论化学中最具挑战性的任务之一。为了应对这一挑战，PI和他的团队开发并应用了新的方法来研究这种腔诱导的纠缠光化学。这些研究提供了量子光-物质相互作用诱导化学的基础知识。霍博士正在组织关注这一新兴领域的国际会议，以促进使用这类系统的新技术和应用的进步。耦合分子到光学腔中的量子化辐射场已经显示出巨大的希望，为化学反应和转化提供了新的范例。由此产生的新的光子-物质纠缠态，即所谓的极化，具有新的锥形交叉点或避免交叉点，这极大地影响了分子的光化学，从而开辟了调节和控制化学反应的新可能性。这种混合物质场系统的非绝热动力学仍然不清楚，超出了通常的光化学范式，不包括量子光子，或量子光学，不关注分子。理论研究在理解这一新兴领域的基本限制和新原理方面起着至关重要的作用。然而，量子光学中常用的现有方法和模型在描述光化学的范围和适用性方面受到很大限制。为了提供这个介于光化学和量子光学之间的新兴领域的基础知识，PI和他的研究小组正在(1)研究腔量子电动力学（QED）诱导光化学的基本极限，基本机制和新原理，以及(2)开发准确有效的基于路径积分的方法来模拟由腔量子电动力学诱导的极化态之间的量子跃迁。这些研究结果提供了对量子光物质诱导化学的基本认识，并为量子光学和光化学的融合提供了新的理论途径。PI组织的会议将在该领域激发可以扩大其潜在影响的新方法。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.