Purcell-Enhanced Spontaneous Emission of Molecular Vibrations

Author
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\&nbsp;T<sub>2,vib</sub>, based on the coupling-induced population decay with\&nbsp;T<sub>κ</sub>≃550 fs\&nbsp;and an associated Purcell factor of\&nbsp;\&gt;10<sup>6</sup>. 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.
Year of Publication
2019
Journal
Physical Review Letters
Volume
123
Date Published
2019-10
ISSN Number
0031-9007
URL
https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.123.153001
DOI
10.1103/PhysRevLett.123.153001
JILA PI
Associated Institutes
Journal Article