Real-space observation of vibrational strong coupling between propagating phonon polaritons and organic molecules

Phonon polaritons in van der Waals materials can strongly enhance light–matter interactions at mid-infrared frequencies, owing to their extreme field confinement and long lifetimes1–7. Phonon polaritons thus bear potential for vibrational strong coupling with molecules. Although the onset of vibrati...

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Bibliographic Details
Published in:Nature photonics 2021-03, Vol.15 (3), p.197-202
Main Authors: Bylinkin, Andrei, Schnell, Martin, Autore, Marta, Calavalle, Francesco, Li, Peining, Taboada-Gutièrrez, Javier, Liu, Song, Edgar, James H., Casanova, Fèlix, Hueso, Luis E., Alonso-Gonzalez, Pablo, Nikitin, Alexey Y., Hillenbrand, Rainer
Format: Article
Language:English
Subjects:
Boron
Boron nitride
Chemical properties
Coupling (molecular)
Crystals
Electric fields
Experiments
Group velocity
Hybrid modes
Interferometry
Numerical prediction
Organic chemistry
Phonons
Photonics
Polaritons
Propagation
Propagation modes
Propagation velocity
Spectroscopy
Spectrum analysis
Thin films
Vibrations
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Summary:Phonon polaritons in van der Waals materials can strongly enhance light–matter interactions at mid-infrared frequencies, owing to their extreme field confinement and long lifetimes1–7. Phonon polaritons thus bear potential for vibrational strong coupling with molecules. Although the onset of vibrational strong coupling was observed spectroscopically with phonon-polariton nanoresonators8, no experiments have resolved vibrational strong coupling in real space and with propagating modes. Here we demonstrate by nanoimaging that vibrational strong coupling can be achieved between propagating phonon polaritons in thin van der Waals crystals (hexagonal boron nitride) and molecular vibrations in adjacent thin molecular layers. We performed near-field polariton interferometry, showing that vibrational strong coupling leads to the formation of a propagating hybrid mode with a pronounced anti-crossing region in its dispersion, in which propagation with negative group velocity is found. Numerical calculations predict vibrational strong coupling for nanometre-thin molecular layers and phonon polaritons in few-layer van der Waals materials, which could make propagating phonon polaritons a promising platform for ultrasensitive on-chip spectroscopy and strong-coupling experiments.Real-space mid-infrared nanoimaging reveals vibrational strong coupling between molecules and propagating phonon polaritons in unstructured, thin hexagonal boron nitride layers, which could provide a platform for testing strong coupling and local control of chemical properties.
ISSN:1749-4885
1749-4893
DOI:10.1038/s41566-020-00725-3