Purcell-Enhanced Spontaneous Emission of Molecular Vibrations
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\ T<sub>2,vib</sub>, based on the coupling-induced population decay with\ T<sub>κ</sub>≃550 fs\ and an associated Purcell factor of\ \>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||
Physical Review Letters