Continuous-wave frequency upconversion with a molecular optomechanical nanocavity

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Reference W. Chen, P. Roelli, H. Hu, S. Verlekar, S.P. Amirtharaj, A.I. Barreda, T.J. Kippenberg, M. Kovylina, E. Verhagen, A. Martínez and C. Galland, Continuous-wave frequency upconversion with a molecular optomechanical nanocavity, Science 374, 6572: 1264-1267 (2021)
Group Photonic Forces

Coherent upconversion of terahertz and mid-infrared signals into visible light opens new horizons for spectroscopy, imaging, and sensing but represents a challenge for conventional nonlinear optics. Here, we used a plasmonic nanocavity hosting a few hundred molecules to demonstrate optomechanical transduction of submicrowatt continuous-wave signals from the mid-infrared (32 terahertz) onto the visible domain at ambient conditions. The incoming field resonantly drives a collective molecular vibration, which imprints a coherent modulation on a visible pump laser and results in upconverted Raman sidebands with subnatural linewidth. Our dual-band nanocavity offers an estimated 13 orders of magnitude enhancement in upconversion efficiency per molecule. Our results demonstrate that molecular cavity optomechanics is a flexible paradigm for frequency conversion leveraging tailorable molecular and plasmonic properties.