Cavity-induced modifications of molecular structure in the strong-coupling regime
Entity
UAM. Departamento de Física Teórica de la Materia CondensadaPublisher
American Physical SocietyDate
2015-11-09Citation
10.1103/PhysRevX.5.041022
Physical Review X 5.4 (2015): 041022
ISSN
2160-3308 (online)DOI
10.1103/PhysRevX.5.041022Funded by
This work has been funded by the European Research Council (ERC-2011-AdG Proposal No. 290981), by the European Union Seventh Framework Programme under Grant Agreement FP7-PEOPLE-2013-CIG-618229, and the Spanish MINECO under Contracts No. MAT2011-28581-C02-01 and No. MAT2014-53432-C5-5-RProject
Gobierno de España. MAT2011-28581-C02-01; Gobierno de España. MAT2014-53432-C5-5-R; info:eu-repo/grantAgreement/EC/FP7/618229; info:eu-repo/grantAgreement/EC/FP7/290981Editor's Version
http://dx.doi.org/10.1103/PhysRevX.5.041022Subjects
Chemical physics; Plasmonics; Quantum physics; FísicaRights
© 2015 American Physical SocietyAbstract
In most theoretical descriptions of collective strong coupling of organic molecules to a cavity mode, the molecules are modeled as simple two-level systems. This picture fails to describe the rich structure provided by their internal rovibrational (nuclear) degrees of freedom. We investigate a first-principles model that fully takes into account both electronic and nuclear degrees of freedom, allowing an exploration of the phenomenon of strong coupling from an entirely new perspective. First, we demonstrate the limitations of applicability of the Born-Oppenheimer approximation in strongly coupled molecule-cavity structures. For the case of two molecules, we also show how dark states, which within the two-level picture are effectively decoupled from the cavity, are indeed affected by the formation of collective strong coupling. Finally, we discuss ground-state modifications in the ultrastrong-coupling regime and show that some molecular observables are affected by the collective coupling strength, while others depend only on the single-molecule coupling constant
Files in this item
Google Scholar:Galego, Javier
-
Feist, Johannes
-
García Vidal, Fco. José
This item appears in the following Collection(s)
Related items
Showing items related by title, author, creator and subject.