Detecting mid-infrared light by molecular frequency upconversion with dual-wavelength hybrid nanoantennas

Abstract: Coherent interconversion of signals between optical and mechanical domains is enabled by optomechanical interactions. Extreme light-matter coupling produced by confining light to nanoscale mode volumes can then access single mid-infrared (MIR) photon sensitivity. Here we utilise the infrared absorption and Raman activity of molecular vibrations in plasmonic nanocavities to demonstrate frequency upconversion. We convert {\lambda}~10 {\mu}m incoming light to visible via surface-enhanced Raman scattering (SERS) in doubly-resonant antennas that enhance upconversion by >10^10. We show >200% amplification of the SERS antiStokes emission when a MIR pump is tuned to a molecular vibrational frequency, obtaining lowest detectable powers ~1 {\mu}W/{\mu}m^2 at room temperature. These results have potential for low-cost and large-scale infrared detectors and spectroscopic techniques, and bring single-molecule sensing into the infrared