Single-molecule mid-IR detection through vibrationally-assisted luminescence

Abstract Room temperature detection of molecular vibrations in the mid-infrared (MIR, λ=3-30µm) has numerous applications including real-time gas sensing, chemical reactivity, medical imaging, astronomical surveys, and quantum communication [1,2]. However, MIR detection is severely hindered by thermal noise, hence current technologies rely on energy-intensive cooled semiconductor detectors (mercury cadmium telluride, MCT) [3–5]. One way to overcome this challenge is to upconvert the low-energy MIR light into high-energy visible wavelengths (λ=500-800nm) where detection of single photons is easily achieved using silicon technologies [6,7]. This process suffers from weak cross sections and the mismatch between MIR and visible wavelengths, limiting its efficiency. Here, we exploit molecular emitters possessing both MIR and visible transitions from molecular vibrations and electronic states, coupled through Frank–Condon factors. By assembling molecules into a nanoscale cavity and continuously optically pumping them below the electronic absorption band, we show the transduction of MIR light absorbed by the molecular vibrations. The upconverted signal is observed as enhanced high-energy luminescence. Combining Purcell-enhanced visible luminescence with enhanced rates of vibrational pumping gives transduction efficiencies exceeding 10%. By down-scaling the cavity volume below 1nm^3, we show MIR detection of single-molecular bonds, inaccessible to any previous detector.