Journal
SCIENCE
Volume 374, Issue 6572, Pages 1264-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abk3106
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Funding
- European Union [829067, 820196, 732894]
- Swiss National Science Foundation [170684, 198898]
- Alexander von Humboldt Foundation
- European Research Council (ERC) [820196] Funding Source: European Research Council (ERC)
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Coherent upconversion of terahertz and mid-infrared signals into visible light was achieved using a plasmonic nanocavity hosting a few hundred molecules, demonstrating significant enhancement in upconversion efficiency per molecule. The results showcase that molecular cavity optomechanics is a flexible paradigm for frequency conversion leveraging tailorable molecular and plasmonic properties.
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.
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