Purcell-Enhanced Spontaneous Emission of Molecular Vibrations

Bernd Metzger, Eric Muller, Jun Nishida, Benjamin Pollard, Mario Hentschel, and Markus B. Raschke
Phys. Rev. Lett. 123, 153001 – Published 10 October 2019
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Abstract

Infrared (IR) spectroscopy of molecular vibrations provides insight into molecular structure, coupling, and dynamics. However, picosecond scale intermolecular and intramolecular many-body interactions, nonradiative relaxation, absorption, and thermalization typically dominate over IR spontaneous emission. We demonstrate how coupling to a resonant IR antenna can enhance spontaneous emission of molecular vibrations. Using time-domain nanoprobe spectroscopy we observe an up to 50% decrease in vibrational dephasing time T2,vib, based on the coupling-induced population decay with Tκ550fs and an associated Purcell factor of >106. This rate enhancement of the spontaneous emission of antenna-coupled molecular vibrations opens new avenues for IR coherent control, quantum information processing, and quantum chemistry.

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  • Received 25 February 2019
  • Revised 24 June 2019

DOI:https://doi.org/10.1103/PhysRevLett.123.153001

© 2019 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied PhysicsAtomic, Molecular & Optical

Authors & Affiliations

Bernd Metzger1, Eric Muller1, Jun Nishida1, Benjamin Pollard1, Mario Hentschel2, and Markus B. Raschke1,*

  • 1Department of Physics, Department of Chemistry, and JILA, University of Colorado at Boulder, Colorado 80309, USA
  • 24th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany

  • *markus.raschke@colorado.edu

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Issue

Vol. 123, Iss. 15 — 11 October 2019

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