Harnessing Non-Boltzmann Steady States in Lanthanide Nanocrystals for Mid-Infrared Optoelectronics

Abstract

Converting mid-infrared (MIR) radiation to visible or near-infrared wavelengths is essential for imaging and sensing, yet achieving sensitive, low-power, and scalable detection remains challenging. Lanthanide nanocrystals provide an alternative through ratiometric luminescence but are typically constrained by Boltzmann statistics, which tie population distributions to lattice temperature and limit signal contrast. Here we show that MIR irradiation rebalances dissipative relaxation pathways, driving lanthanide emitters into a non-Boltzmann steady state that enables non-thermal control of population distributions. This allows emission behaviors inaccessible under thermal equilibrium. We exploit this regime to achieve linear MIR detection with respect to MIR power across 6.8 to 8.6 micrometers. The ratiometric response is intrinsically independent of the pump power, enabling operation at an ultralow excitation power of 10 uW, several orders of magnitude lower than conventional approaches. Using standard silicon photodetectors, we then demonstrate room-temperature MIR imaging with detection limits approaching 4 nW um-2. Our results establish lanthanide nanoparticles as an efficient platform for MIR conversion and sensing in nanophotonic systems.