Dynamical coupling of plasmons and molecular excitations by hybrid quantum/classical calculations: time-domain approach.
J Phys Condens Matter
; 26(31): 315013, 2014 Aug 06.
Article
em En
| MEDLINE
| ID: mdl-25028486
ABSTRACT
The presence of plasmonic material influences the optical properties of nearby molecules in untrivial ways due to the dynamical plasmon-molecule coupling. We combine quantum and classical calculation schemes to study this phenomenon in a hybrid system that consists of a Na(2) molecule located in the gap between two Au/Ag nanoparticles. The molecule is treated quantum-mechanically with time-dependent density-functional theory, and the nanoparticles with quasistatic classical electrodynamics. The nanoparticle dimer has a plasmon resonance in the visible part of the electromagnetic spectrum, and the Na(2) molecule has an electron-hole excitation in the same energy range. Due to the dynamical interaction of the two subsystems the plasmon and the molecular excitations couple, creating a hybridized molecular-plasmon excited state. This state has unique properties that yield e.g. enhanced photoabsorption compared to the freestanding Na(2) molecule. The computational approach used enables decoupling of the mutual plasmon-molecule interaction, and our analysis verifies that it is not legitimate to neglect the back coupling effect when describing the dynamical interaction between plasmonic material and nearby molecules. Time-resolved analysis shows nearly instantaneous formation of the coupled state, and provides an intuitive picture of the underlying physics.
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Bases de dados:
MEDLINE
Idioma:
En
Revista:
J Phys Condens Matter
Assunto da revista:
BIOFISICA
Ano de publicação:
2014
Tipo de documento:
Article