Nanoimaging and Control of Molecular Vibrations through Electromagnetically Induced Scattering Reaching the Strong Coupling Regime.

Autor:	Muller EA; Department of Physics, Department of Chemistry, and JILA, University of Colorado, Boulder, Colorado 80309, United States., Pollard B; Department of Physics, Department of Chemistry, and JILA, University of Colorado, Boulder, Colorado 80309, United States., Bechtel HA; Advanced Light Source Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States., Adato R; Departments of Electrical and Computer Engineering and Photonics Center, Boston University, Boston, Massachusetts 02215, United States., Etezadi D; Institute of Bioengineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland., Altug H; Institute of Bioengineering, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland., Raschke MB; Department of Physics, Department of Chemistry, and JILA, University of Colorado, Boulder, Colorado 80309, United States.
Jazyk:	angličtina
Zdroj:	ACS photonics [ACS Photonics] 2018 Sep 19; Vol. 5 (9), pp. 3594-3600. Date of Electronic Publication: 2018 Aug 06.
DOI:	10.1021/acsphotonics.8b00425
Abstrakt:	Optical resonators can enhance light-matter interaction, modify intrinsic molecular properties such as radiative emission rates, and create new molecule-photon hybrid quantum states. To date, corresponding implementations are based on electronic transitions in the visible spectral region with large transition dipoles yet hampered by fast femtosecond electronic dephasing. In contrast, coupling molecular vibrations with their weaker dipoles to infrared optical resonators has been less explored, despite long-lived coherences with 2 orders of magnitude longer dephasing times. Here, we achieve excitation of molecular vibrations through configurable optical interactions of a nanotip with an infrared resonant nanowire that supports tunable bright and nonradiative dark modes. The resulting antenna-vibrational coupling up to 47 ± 5 cm -1 exceeds the intrinsic dephasing rate of the molecular vibration, leading to hybridization and mode splitting. We observe nanotip-induced quantum interference of vibrational excitation pathways in spectroscopic nanoimaging, which we model classically as plasmonic electromagnetically induced scattering as the phase-controlled extension of the classical analogue of electromagnetically induced transparency and absorption. Our results present a new regime of IR spectroscopy for applications of vibrational coherence from quantum computing to optical control of chemical reactions. Competing Interests: The authors declare no competing financial interest.
Databáze:	MEDLINE
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