Remote near-field spectroscopy of vibrational strong coupling between organic molecules and phononic nanoresonators

Irene Dolado, Carlos Maciel-Escudero, Elizaveta Nikulina, Evgenii Modin, Francesco Calavalle, Shu Chen, Andrei Bylinkin, Francisco Javier Alfaro-Mozaz, Jiahan Li, James H. Edgar, Fèlix Casanova, Saül Vélez, Luis E. Hueso, Ruben Esteban, Javier Aizpurua and Rainer Hillenbrand ()
Additional contact information
Irene Dolado: CIC nanoGUNE BRTA
Carlos Maciel-Escudero: CIC nanoGUNE BRTA
Elizaveta Nikulina: CIC nanoGUNE BRTA
Evgenii Modin: CIC nanoGUNE BRTA
Francesco Calavalle: CIC nanoGUNE BRTA
Shu Chen: CIC nanoGUNE BRTA
Andrei Bylinkin: CIC nanoGUNE BRTA
Francisco Javier Alfaro-Mozaz: Donostia International Physics Center (DIPC)
Jiahan Li: Kansas State University
James H. Edgar: Kansas State University
Fèlix Casanova: CIC nanoGUNE BRTA
Saül Vélez: Universidad Autónoma de Madrid
Luis E. Hueso: CIC nanoGUNE BRTA
Ruben Esteban: Materials Physics Center, CSIC-UPV/EHU
Javier Aizpurua: Materials Physics Center, CSIC-UPV/EHU
Rainer Hillenbrand: IKERBASQUE, Basque Foundation for Science

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Phonon polariton (PhP) nanoresonators can dramatically enhance the coupling of molecular vibrations and infrared light, enabling ultrasensitive spectroscopies and strong coupling with minute amounts of matter. So far, this coupling and the resulting localized hybrid polariton modes have been studied only by far-field spectroscopy, preventing access to modal near-field patterns and dark modes, which could further our fundamental understanding of nanoscale vibrational strong coupling (VSC). Here we use infrared near-field spectroscopy to study the coupling between the localized modes of PhP nanoresonators made of h-BN and molecular vibrations. For a most direct probing of the resonator-molecule coupling, we avoid the direct near-field interaction between tip and molecules by probing the molecule-free part of partially molecule-covered nanoresonators, which we refer to as remote near-field probing. We obtain spatially and spectrally resolved maps of the hybrid polariton modes, as well as the corresponding coupling strengths, demonstrating VSC on a single PhP nanoresonator level. Our work paves the way for near-field spectroscopy of VSC phenomena not accessible by conventional techniques.

Date: 2022
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DOI: 10.1038/s41467-022-34393-4

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