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Avalanche phenomena leverage steeply nonlinear dynamics to generatedisproportionately high responses from small perturbations and are found in amultitude of events and materials, enabling technologies including opticalphase-conjugate imaging, infrared quantum counting, and efficient upconvertedlasing. However, the photon avalanching (PA) mechanism underlying these opticalinnovations has been observed only in bulk materials and aggregates, andtypically at cryogenic temperatures, limiting its utility and impact. Here, wereport the realization of PA at room temperature in singlenanostructures--small, Tm-doped upconverting nanocrystals--and demonstratetheir use in superresolution imaging at near-infrared (NIR) wavelengths withinspectral windows of maximal biological transparency. Avalanching nanoparticles(ANPs) can be pumped by continuous-wave or pulsed lasers and exhibit all of thedefining features of PA. These hallmarks include excitation power thresholds,long rise time at threshold, and a dominant excited-state absorption that is>13,000x larger than ground-state absorption. Beyond the avalanching threshold,ANP emission scales nonlinearly with the 26th power of pump intensity. Thisenables the realization of photon-avalanche single-beam superresolution imaging(PASSI), achieving sub-70 nm spatial resolution using only simple scanningconfocal microscopy and before any computational analysis. Pairing their steepnonlinearity with existing superresolution techniques and computationalmethods, ANPs allow for imaging with higher resolution and at ca. 100-foldlower excitation intensities than is possible with other probes. The low PAthreshold and exceptional photostability of ANPs also suggest their utility ina diverse array of applications including sub-wavelength bioimaging, IRdetection, temperature and pressure transduction, neuromorphic computing, andquantum optics.

Giant nonlinear optical responses from photon avalanching nanoparticles