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Nanoimaging and Control of Molecular Vibrations through Electromagnetically Induced Scattering Reaching the Strong Coupling Regime
journal contribution
posted on 2018-08-06, 00:00 authored by Eric A. Muller, Benjamin Pollard, Hans A. Bechtel, Ronen Adato, Dordaneh Etezadi, Hatice Altug, Markus B. RaschkeOptical
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.
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quantum statesvibrational coherencenanotip-induced quantum interferencetransition dipolesvibrational excitation pathwaysphase-controlled extensionchemical reactionsdephasing timesplasmonic electromagnetically2 ordersinteractionRegime Optical resonatorsIR spectroscopyElectromagnetically Induced Scatteringmode splittingspectroscopic nanoimagingdephasing rateMolecular Vibrationsradiative emission rates
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