Building and testing semiclassical models for molecular plasmonics

Molecular plasmonics has been a hot topic for the past several years. At the heart of the primary interest in plasmonics is the strong electromagnetic field localization at resonant frequencies corresponding to surface plasmon-polariton modes. Thanks to riveting advancements in nanofabrication technologies, we have achieved nearly 1 nm spatial resolution (and in some cases even below that!) and are able to fabricate a wide variety of nanosystems ranging from
nanoparticles of various shapes to metasurfaces comprised of periodic arrays of nanoparticles and/or nanoholes of any imaginable geometry. Such systems have recently emerged as new platforms for strong light-matter interactions. Combined with molecular ensembles, these constructs exhibit a remarkable set of optical phenomena ranging from the exciton-plasmon strong coupling to the second harmonic generation altered by molecular resonances. In this talk I will discuss both linear and nonlinear optical properties of plasmonic materials coupled to quantum emitters of various complexity. I will also introduce a newly developed computational approach that can be used to efficiently simulate a large number of complex molecules driven by electromagnetic radiation crafted at plasmonic interfaces.

Representative publications:
1. “Efficient parallel strategy for molecular plasmonics – a new numerical tool for Maxwell-Schrödinger equations in three dimensions”, M. Sukharev, Journal of Computational Physics 477, 111920 (2023).
2. “Dissociation slowdown by collective optical response under strong coupling conditions”, M. Sukharev, J. Subotnik, A. Nitzan, (Editor’s Choice) Journal of Chemical Physics 158, 084104 (2023).
3. “Fano plasmonics goes nonlinear”, M. Sukharev, E. Drobnyh, R. Pachter, Journal of Chemical Physics 157, 134105 (2022).
4. “Second harmonic generation by strongly coupled exciton-plasmons: the role of polaritonic states in nonlinear dynamics”, M. Sukharev, A. Salomon, J. Zyss, Journal of Chemical Physics 154, 244701 (2021).
5. “Second harmonic generation from a single plasmonic nanorod strongly coupled to a WSe2 monolayer”, C. Li, X. Lu, A. Srivastava, S. D. Storm, R. Gelfand, M. Pelton, M. Sukharev, H. Harutyunyan, Nano Letters 21, 1599 (2020).
6. “Plasmon enhanced second harmonic generation by periodic arrays of triangular nanoholes coupled to molecular emitters”, E. Drobnyh and M. Sukharev, Journal of Chemical Physics 152, 094706 (2020).
7. “Energy transfer and interference by collective electromagnetic coupling”, M. Gómez-Castaño, A. R. Cubero, L. Buisson, J. L. Pau, A. Mihi, S. Ravaine, R. A. L. Vallée, A. Nitzan, M. Sukharev, Nano Letters 19, 5790 (2019).