6533b857fe1ef96bd12b461c
RESEARCH PRODUCT
Dipolar coupling of nanoparticle-molecule assemblies: An efficient approach for studying strong coupling
Tomasz J. AntosiewiczJakub FojtPaul ErhartMikael KuismaTuomas P. Rossisubject
Degrees of freedom (statistics)General Physics and AstronomyNanoparticleFOS: Physical sciences010402 general chemistryoptiset ominaisuudet01 natural scienceslinear combination of atomic orbitalstime dependent density functional theorynanorakenteet0103 physical sciencesMesoscale and Nanoscale Physics (cond-mat.mes-hall)MoleculePhysical and Theoretical Chemistryoptical spectroscopyQuantumPhysicssurface optics010304 chemical physicsCondensed Matter - Mesoscale and Nanoscale Physicstiheysfunktionaaliteoriapolarizability0104 chemical sciencesplasmonitRange (mathematics)DipoleChemical physicsDensity functional theorynanoparticlesnanohiukkasetplasmonsMagnetic dipole–dipole interactiondescription
Strong light-matter interactions facilitate not only emerging applications in quantum and non-linear optics but also modifications of materials properties. In particular the latter possibility has spurred the development of advanced theoretical techniques that can accurately capture both quantum optical and quantum chemical degrees of freedom. These methods are, however, computationally very demanding, which limits their application range. Here, we demonstrate that the optical spectra of nanoparticle-molecule assemblies, including strong coupling effects, can be predicted with good accuracy using a subsystem approach, in which the response functions of the different units are coupled only at the dipolar level. We demonstrate this approach by comparison with previous time-dependent density functional theory calculations for fully coupled systems of Al nanoparticles and benzene molecules. While the present study only considers few-particle systems, the approach can be readily extended to much larger systems and to include explicit optical-cavity modes.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2021-01-13 |