TY - JOUR
AU - Bernd Metzger
AU - Eric Muller
AU - Jun Nishida
AU - Benjamin Pollard
AU - Mario Hentschel
AU - Markus Raschke
AB - 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.
BT - Physical Review Letters
DA - 2019-10
DO - 10.1103/PhysRevLett.123.153001
N2 - 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.
PY - 2019
EP - 153001
T2 - Physical Review Letters
TI - Purcell-Enhanced Spontaneous Emission of Molecular Vibrations
UR - https://journals.aps.org/prl/abstract/10.1103/PhysRevLett.123.153001
VL - 123
SN - 0031-9007
ER -