@article{11978,
author = {Bernd Metzger and Eric Muller and Jun Nishida and Benjamin Pollard and Mario Hentschel and Markus Raschke},
title = {Purcell-Enhanced Spontaneous Emission of Molecular Vibrations},
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\ Tκ≃550 fs\ 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.},
year = {2019},
journal = {Physical Review Letters},
volume = {123},
pages = {153001},
month = {2019-10},
issn = {0031-9007},
url = {https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.123.153001},
doi = {10.1103/PhysRevLett.123.153001},
}