Detecting Mid-infrared Light by Molecular Frequency Upconversion in Dual-wavelength Nanoantennas

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 used the infrared absorption and Raman activity of molecular vibrations in plasmonic nanocavities to demonstrate frequency upconversion. We converted approximately 10-micrometer-wavelength incoming light to visible light by surface-enhanced Raman scattering (SERS) in doubly resonant antennas that enhanced upconversion by more than 10. We showed 140% amplification of the SERS anti-Stokes emission when an MIR pump was tuned to a molecular vibrational frequency, obtaining lowest detectable powers of 1 to 10 microwatts per square micrometer at room temperature. These results have potential for low-cost and large-scale infrared detectors and spectroscopic techniques.