Role of Symmetry Breaking in Observing Strong Molecule-Cavity Coupling Using Dielectric Microspheres

Overview

Journal Nano Lett

Publisher American Chemical Society

Specialty Biotechnology

Date 2022 Aug 3

PMID 35920815

Authors

Adarsh B Vasista

Eduardo J C Dias

F Javier Garcia de Abajo

William L Barnes

Affiliations

Soon will be listed here.

Abstract

The emergence of dielectric open optical cavities has opened a new research avenue in nanophotonics. In particular, dielectric microspheres support a rich set of cavity modes with varying spectral characteristics, making them an ideal platform to study molecule-cavity interactions. The symmetry of the structure plays a critical role in the outcoupling of these modes and, hence, the perceived molecule-cavity coupling strength. Here, we experimentally and theoretically study molecule-cavity coupling mediated by the Mie scattering modes of a dielectric microsphere placed on a glass substrate and excited with far-field illumination, from which we collect scattering signatures both in the air and glass sides. Glass-side collection reveals clear signatures of strong molecule-cavity coupling (coupling strength 2 = 74 meV), in contrast to the air-side scattering signal. Rigorous electromagnetic modeling allows us to understand molecule-cavity coupling and unravel the role played by the spatial mode profile in the observed coupling strength.

Citing Articles

Recent advances in quantum nanophotonics: plexcitonic and vibro-polaritonic strong coupling and its biomedical and chemical applications.

Kim Y, Barulin A, Kim S, Lee L, Kim I Nanophotonics. 2024; 12(3):413-439.

PMID: 39635391 PMC: 11501129. DOI: 10.1515/nanoph-2022-0542.

References

Liu M, Powell D, Shadrivov I, Lapine M, Kivshar Y . Spontaneous chiral symmetry breaking in metamaterials. Nat Commun. 2014; 5:4441. DOI: 10.1038/ncomms5441. View

Song M, Dellinger J, Demichel O, Buret M, Colas des Francs G, Zhang D . Selective excitation of surface plasmon modes propagating in Ag nanowires. Opt Express. 2017; 25(8):9138-9149. DOI: 10.1364/OE.25.009138. View

Dietrich C, Steude A, Tropf L, Schubert M, Kronenberg N, Ostermann K . An exciton-polariton laser based on biologically produced fluorescent protein. Sci Adv. 2016; 2(8):e1600666. PMC: 4991930. DOI: 10.1126/sciadv.1600666. View

Vasista A, Barnes W . Molecular Monolayer Strong Coupling in Dielectric Soft Microcavities. Nano Lett. 2020; 20(3):1766-1773. PMC: 7581308. DOI: 10.1021/acs.nanolett.9b04996. View

Zengin G, Wersall M, Nilsson S, Antosiewicz T, Kall M, Shegai T . Realizing Strong Light-Matter Interactions between Single-Nanoparticle Plasmons and Molecular Excitons at Ambient Conditions. Phys Rev Lett. 2015; 114(15):157401. DOI: 10.1103/PhysRevLett.114.157401. View

Anderson P . More is different. Science. 1972; 177(4047):393-6. DOI: 10.1126/science.177.4047.393. View

Coles D, Somaschi N, Michetti P, Clark C, Lagoudakis P, Savvidis P . Polariton-mediated energy transfer between organic dyes in a strongly coupled optical microcavity. Nat Mater. 2014; 13(7):712-9. DOI: 10.1038/nmat3950. View

Das A, Heo J, Jankowski M, Guo W, Zhang L, Deng H . Room temperature ultralow threshold GaN nanowire polariton laser. Phys Rev Lett. 2011; 107(6):066405. DOI: 10.1103/PhysRevLett.107.066405. View

Vollmer F, Arnold S . Whispering-gallery-mode biosensing: label-free detection down to single molecules. Nat Methods. 2008; 5(7):591-6. DOI: 10.1038/nmeth.1221. View

10.

Song M, Bouhelier A, Bramant P, Sharma J, Dujardin E, Zhang D . Imaging symmetry-selected corner plasmon modes in penta-twinned crystalline Ag nanowires. ACS Nano. 2011; 5(7):5874-80. DOI: 10.1021/nn201648d. View

11.

Garcia de Abajo F, Gomez-Santos G, Blanco L, Borisov A, Shabanov S . Tunneling mechanism of light transmission through metallic films. Phys Rev Lett. 2005; 95(6):067403. DOI: 10.1103/PhysRevLett.95.067403. View

12.

Weitz R, Allen M, Feldman B, Martin J, Yacoby A . Broken-symmetry states in doubly gated suspended bilayer graphene. Science. 2010; 330(6005):812-6. DOI: 10.1126/science.1194988. View

13.

Greybush N, Pacheco-Pena V, Engheta N, Murray C, Kagan C . Plasmonic Optical and Chiroptical Response of Self-Assembled Au Nanorod Equilateral Trimers. ACS Nano. 2019; 13(2):1617-1624. DOI: 10.1021/acsnano.8b07619. View

14.

Thomas A, Lethuillier-Karl L, Nagarajan K, Vergauwe R, George J, Chervy T . Tilting a ground-state reactivity landscape by vibrational strong coupling. Science. 2019; 363(6427):615-619. DOI: 10.1126/science.aau7742. View

15.

Vasista A, Barnes W . Strong Coupling of Multimolecular Species to Soft Microcavities. J Phys Chem Lett. 2022; 13(4):1019-1024. PMC: 8819692. DOI: 10.1021/acs.jpclett.1c03678. View

16.

Pang Y, Thomas A, Nagarajan K, Vergauwe R, Joseph K, Patrahau B . On the Role of Symmetry in Vibrational Strong Coupling: The Case of Charge-Transfer Complexation. Angew Chem Int Ed Engl. 2020; 59(26):10436-10440. PMC: 7318350. DOI: 10.1002/anie.202002527. View

17.

Inaki M, Liu J, Matsuno K . Cell chirality: its origin and roles in left-right asymmetric development. Philos Trans R Soc Lond B Biol Sci. 2016; 371(1710). PMC: 5104503. DOI: 10.1098/rstb.2015.0403. View

18.

High A, Devlin R, Dibos A, Polking M, Wild D, Perczel J . Visible-frequency hyperbolic metasurface. Nature. 2015; 522(7555):192-6. DOI: 10.1038/nature14477. View

19.

Kuhler P, Garcia de Abajo F, Solis J, Mosbacher M, Leiderer P, Afonso C . Imprinting the optical near field of microstructures with nanometer resolution. Small. 2009; 5(16):1825-9. DOI: 10.1002/smll.200900393. View

20.

Aoki T, Dayan B, Wilcut E, Bowen W, Parkins A, Kippenberg T . Observation of strong coupling between one atom and a monolithic microresonator. Nature. 2006; 443(7112):671-4. DOI: 10.1038/nature05147. View