Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 153, Issue 9, Pages -Publisher
AIP Publishing
DOI: 10.1063/5.0021033
Keywords
-
Funding
- DOE Photonics at Thermodynamic Limits Energy Frontier Research Center [DE-SC0019140]
- Deutsche Forschungsgemeinschaft (DFG Forschungsstipendium) [FL997/1-1]
Ask authors/readers for more resources
Advances in nanophotonics, quantum optics, and low-dimensional materials have enabled precise control of light-matter interactions down to the nanoscale. Combining concepts from each of these fields, there is now an opportunity to create and manipulate photonic matter via strong coupling of molecules to the electromagnetic field. Toward this goal, here we demonstrate a first principles framework to calculate polaritonic excited-state potential-energy surfaces, transition dipole moments, and transition densities for strongly coupled light-matter systems. In particular, we demonstrate the applicability of our methodology by calculating the polaritonic excited-state manifold of a formaldehyde molecule strongly coupled to an optical cavity. This proof-of-concept calculation shows how strong coupling can be exploited to alter photochemical reaction pathways by influencing avoided crossings with tuning of the cavity frequency and coupling strength. Therefore, by introducing an ab initio method to calculate excited-state potential-energy surfaces, our work opens a new avenue for the field of polaritonic chemistry.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available