Cavity-induced modifications of molecular structure in the strong-coupling regime
Entidad
UAM. Departamento de Física Teórica de la Materia CondensadaEditor
American Physical SocietyFecha de edición
2015-11-09Cita
10.1103/PhysRevX.5.041022
Physical Review X 5.4 (2015): 041022
ISSN
2160-3308 (online)DOI
10.1103/PhysRevX.5.041022Financiado por
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-RProyecto
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/FP7/290981Versión del editor
http://dx.doi.org/10.1103/PhysRevX.5.041022Materias
Chemical physics; Plasmonics; Quantum physics; FísicaDerechos
© 2015 American Physical SocietyResumen
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
Lista de ficheros
Google Scholar:Galego, Javier
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Feist, Johannes
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García Vidal, Fco. José
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