Enhancing cooperativity of molecular J-aggregates by resonantly coupled dielectric metasurfaces

Page view(s)
5
Checked on Dec 29, 2024
Enhancing cooperativity of molecular J-aggregates by resonantly coupled dielectric metasurfaces
Title:
Enhancing cooperativity of molecular J-aggregates by resonantly coupled dielectric metasurfaces
Journal Title:
Nanophotonics
Keywords:
Publication Date:
10 June 2024
Citation:
Marangi, M., Wang, Y., Wu, M., Tjiptoharsono, F., Kuznetsov, A. I., Adamo, G., & Soci, C. (2024). Enhancing cooperativity of molecular J-aggregates by resonantly coupled dielectric metasurfaces. Nanophotonics, 0(0). https://doi.org/10.1515/nanoph-2024-0117
Abstract:
J-aggregates are supramolecular assemblies of dyes exhibiting strong absorption and fluorescence with narrow linewidths, as well as large optical nonlinearities, induced by the formation of largely delocalized molecular excitons. The degree of cooperativity achievable in J-aggregates ensembles, however, is limited by local disorder and thermally induced decoherence effects. A way to overcome these limitations and increase molecular exciton delocalization and coherence is to couple the ensemble of highly ordered molecular dipoles to a common electromagnetic mode in an optical resonator. In this work, we use dielectric metasurfaces to alter the radiative properties of coupled J-aggregate films and demonstrate a 5-fold Purcell enhancement of the luminesce intensity and narrowing of the emission directivity down to ∼300 mrad around the normal. These results highlight the potential of designer dielectric metasurfaces to foster the emergence of cooperative phenomena in excitonic systems, including optical nonlinearities and superradiance.
License type:
Attribution 4.0 International (CC BY 4.0)
Funding Info:
This research / project is supported by the A*STAR AME - Nanoantenna Spatial Light Modulators for Next-Gen Display Technologies
Grant Reference no. : A18A7b0058

This research / project is supported by the National Research Foundation - Quantum Engineering Programme
Grant Reference no. : NRF2021- QEP2-01-P01

This research / project is supported by the Ministry of Education - NA
Grant Reference no. : MOE- T2EP50222-0015

This research / project is supported by the MTC - Nanoantenna Light-Emitting Devices
Grant Reference no. : M21J9b0085
Description:
ISSN:
2192-8606
2192-8614