Relevance of Rabi splitting effect for tunable enhancement of Raman scattering in self-assembled silver - Fullerene nanocomposite films

0558933 - ÚJF 2023 RIV GB eng J - Journal Article
Lavrentiev, Vasyl - Pokorný, Jan - Chvostová, Dagmar - Klementová, Mariana - Lavrentieva, Inna - Vacík, Jiří - Dejneka, Alexandr
Relevance of Rabi splitting effect for tunable enhancement of Raman scattering in self-assembled silver - Fullerene nanocomposite films.
Carbon. Roč. 196, AUG (2022), s. 988-1000. ISSN 0008-6223. E-ISSN 1873-3891
R&D Projects: GA MŠMT(CZ) EF16_019/0000760; GA ČR GA22-17346S
Research Infrastructure: CANAM II - 90056; CzechNanoLab - 90110
Institutional support: RVO:68378271 ; RVO:61389005
Keywords : Fullerene molecules * silver nanoparticles * Self-assembly * Raman scattering enhancement * Plasmonic interactions
OECD category: Coating and films; Condensed matter physics (including formerly solid state physics, supercond.) (FZU-D)
Impact factor: 10.9, year: 2022
Method of publishing: Limited access
https://doi.org/10.1016/j.carbon.2022.06.002

We report on detection of plasmon-enhanced Raman scattering (PERS) in self-assembled AgxC60 nanocomposite films and on evolution of this effect with increase of the Ag concentration, x, in the interval of 2 < x < 25. Optical absorption spectra show that origin of the PERS effect is closely related with dipolar plasmonic mode generated by uniform 3D-ensemble of Ag nanoparticles, which arise in the C-60-based matrix during the film deposition. Careful analysis of the absorption spectra designates features of strong coupling between dipolar plasmon mode and the C-60 low-energy exciton suggesting energy exchange between the arisen high- and low-energy polaritonic states. Evaluation of dispersion spectra of the polaritons revealed anti-crossing effect as a sign of the strong plasmon-exciton coupling with Rabi splitting energy of about 300 meV. In frames of the recently-reported quantum-electrodynamics model, the detected PERS effect was ascribed to abundant population of the low- energy polaritonic states caused by asymmetric transitions between the low- and high-energy polaritons. The obtained PERS-spectra display sensitivity of the C-60 vibrational modes to the x-driven plasmonic field strength, which demonstrates some reduction at higher x due to charge transfer through C-60 molecular junctions. The evident tunability of PERS suggests an emerging potential of the self-assembled AgxC60 films for their application in molecular electronics and molecular photochemistry.
Permanent Link: https://hdl.handle.net/11104/0332420