Polariton-Assisted InterMolecular Interactions

Description du projet

Un aperçu des réactions moléculaires avec les polaritons

La chimie polaritonique est un domaine émergent qui explore comment la lumière peut modifier le comportement chimique. Lorsque des molécules sont confinées à l’intérieur de cavités à l’échelle micrométrique, elles peuvent se coupler à la lumière pour former des polaritons. Les polaritons sont des états hybrides lumière-matière capables de modifier les structures moléculaires, les interactions et les voies de réaction. Les données expérimentales indiquent que les polaritons peuvent modifier la vitesse et l’efficacité des réactions chimiques, mais la théorie sous-jacente reste incomplète. Le projet PAIMI, financé par l’UE, développera des modèles avancés et des outils informatiques pour étudier comment la lumière infrarouge dans les cavités affecte les molécules et leurs interactions. La clarification de ces mécanismes ouvrira de nouvelles perspectives pour le contrôle des réactions chimiques par la lumière.

Objectif

Polaritonic chemistry is a new field of research bridging chemistry with quantum optics. It has been shown that confining molecules into microscale optical cavities can lead to the formation of polaritons, hybrid light-matter states offering a unique way to design and control chemical processes at the molecular level. The formation of polaritons can influence molecular structure, chemical reactivity and intermolecular interactions, and result in controlling chemical transformations, energy transfer, and internal motions of molecules. In the last five years it has been shown experimentally that polaritons in microfluidic infrared cavities can change the kinetics and thermodynamics of thermally activated chemical reactions. Despite much effort, theory is not yet able to provide a full understanding of these results. In addition to chemical reactions, the spectroscopy of molecular polaritons is also of high interest. The central questions we are looking to find answers to include a) How does the interaction with infrared cavity radiation manifest in the properties of rovibrational states of complex (multi)molecular systems? b) How does resonant light-matter interaction between the cavity modes and the molecules influence the interaction and coupling among the various degrees of freedom in weakly bound molecular complexes? c) What new phenomena can be learned from the collective polaritonic states simulated using realistic molecular models and/or large number of molecules? This project aims to extend the field of (ro)vibrational polaritonic chemistry by (a) delivering high-accuracy theoretical models and related computational tools capable of treating medium sized (floppy) molecular systems in an IR cavity, (b) revealing the characteristic phenomena which occur when weakly bound molecular complexes interact with IR cavity radiation, (c) extending simulations to the collective states of large number of molecules by exploiting massively parallel code implementation.