QEDControl · Development of Coupled Cluster Theory in Optical Cavities for Molecular Polaritonic Response Functions

Introducing molecules into quantum cavities to enhance selected physical properties or to control chemical processes is a highly active domain of research. The coupled system of molecules and the resonant electromagnetic field, called a molecular polariton, have properties very different from those of free molecules, providing a possibility of non-invasively influencing molecular systems on a quantum level. Developments in experimental techniques and electronic structure methods continuously open up new possibilities of tuning polaritons for specific applications. The description of molecules in quantum cavities requires models deeply rooted in quantum electrodynamics and necessitates novel perspectives in wavefunction-based methods. Although it is now possible to calculate the potential energy surfaces of polaritons, the description of other properties, especially response functions, is an open challenge.In this project, we aim to develop theories and methods for the calculation of polaritonic response properties in quantum cavities, with the goal to understand the possibilities of quantum control of intra- and intermolecular processes. Our developments are expected to provide experimental and fundamental research with a theoretical framework and software implementations for the future design of chemical processes in quantum cavities. Achieving this result will rely on an interdisciplinary work between theoretical molecular physics, high-performance software development, as well as applied computational chemistry methods. This synergy between electronic structure theory expertise of the Host with the background in response function theory of the Applicant will also be supported by a larger effort at the Saarland University to utilize quantum cavities in molecular science. Overall, the successful project will give a theoretical background for planning polaritonic devices for tailored applications by a non-invasive altering physical and chemical properties.