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Nanoscale momentum-resolved vibrational spectroscopy.

ABSTRACT: Vibrational modes affect fundamental physical properties such as the conduction of sound and heat and can be sensitive to nano- and atomic-scale structure. Probing the momentum transfer dependence of vibrational modes provides a wealth of information about a materials system; however, experimental work has been limited to essentially bulk and averaged surface approaches or to small wave vectors. We demonstrate a combined experimental and theoretical methodology for nanoscale mapping of optical and acoustic phonons across the first Brillouin zone, in the electron microscope, probing a volume ~10¹⁰ to 10²⁰ times smaller than that of comparable bulk and surface techniques. In combination with more conventional electron microscopy techniques, the presented methodology should allow for direct correlation of nanoscale vibrational mode dispersions with atomic-scale structure and chemistry.

SUBMITTER: Hage FS

PROVIDER: S-EPMC6018998 | biostudies-literature | 2018 Jun

REPOSITORIES: biostudies-literature

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Nanoscale momentum-resolved vibrational spectroscopy.

Hage Fredrik S FS Nicholls Rebecca J RJ Yates Jonathan R JR McCulloch Dougal G DG Lovejoy Tracy C TC Dellby Niklas N Krivanek Ondrej L OL Refson Keith K Ramasse Quentin M QM

Science advances 20180615 6

Vibrational modes affect fundamental physical properties such as the conduction of sound and heat and can be sensitive to nano- and atomic-scale structure. Probing the momentum transfer dependence of vibrational modes provides a wealth of information about a materials system; however, experimental work has been limited to essentially bulk and averaged surface approaches or to small wave vectors. We demonstrate a combined experimental and theoretical methodology for nanoscale mapping of optical a ...[more]

PMID: 29951584

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Project description:Vibrational polaritons, which have been primarily studied in Fabry-Pérot cavities with a large number of molecules (N ∼ 106-1010) coupled to the resonator mode, exhibit various experimentally observed effects on chemical reactions. However, the exact mechanism is elusively understood from the theoretical side, as the large number of molecules involved in an experimental strong coupling condition cannot be represented completely in simulations. This discrepancy between theory and experiment arises from computational descriptions of polariton systems typically being limited to only a few molecules, thus failing to represent the experimental conditions adequately. To address this mismatch, we used surface phonon polariton (SPhP) resonators as an alternative platform for vibrational strong coupling. SPhPs exhibit strong electromagnetic confinement on the surface and thus allow for coupling to a small number of molecules. As a result, this platform can enhance nonlinearity and slow down relaxation to the dark modes. In this study, we fabricated a pillar-shaped quartz resonator and then coated it with a thin layer of cobalt phthalocyanine (CoPc). By employing scattering-type scanning near-field optical microscopy (s-SNOM), we spatially investigated the dependency of vibrational strong coupling on the spatially varying electromagnetic field strength and demonstrated strong coupling with 38,000 molecules only-reaching to the small N limit. Through s-SNOM analysis, we found that strong coupling was observed primarily on the edge of the quartz pillar and the apex of the s-SNOM tip, where the maximum field enhancement occurs. In contrast, a weak resonance signal and lack of coupling were observed closer to the center of the pillar. This work demonstrates the importance of spatially resolved polariton systems in nanophotonic platforms and lays a foundation to explore polariton chemistry and chemical dynamics at the small N limit-one step closer to reconcile with high-level quantum calculations.

Dataset Information

Nanoscale momentum-resolved vibrational spectroscopy.

Publications

Nanoscale momentum-resolved vibrational spectroscopy.

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