Single nanocrystal anti-stokes shifted superfluorescence

Superfluorescence (SF) is a unique optical phenomenon that consists of an ensemble of emitters coupling collectively to produce a short but extremely intense burst of light. SF has also only been realized in extreme conditions (at low temperatures of around 6 K). Moreover, no anti-Stokes shift SF has been discovered in either an ensemble of nanoparticles or at bulky crystal levels. We report on a new lanthanidedoped upconversion nanoparticles (UCNPs) as a medium to achieve cavity free anti-Stokes shifted SF at room temperature, culminating in rapid, intense, and narrow spectral peaks of upconverted SF. This is the first time that SF has been discovered in a single nanocrystal regime and is the smallest-ever SF media. We observed the resultant UCNP SF with an extremely narrow spectral width at single nanocrystal-level (full-width at half-maximum, FWHM = 2 nm), and to have a significantly shortened lifetime (τ = 46 ns, 10,000-fold accelerated radiative decay, when compared to the lifetime of τ = 455.8 μs of normal upconversion luminescence (UCL). The significantly upspeeded upconverted SF lifetimes at tens of nanoseconds scale should break through the key limitation in normal UCL. This will open up the opportunity to carry out high speed bioimaging using upconversion nanoparticles without compromising the imaging quality. In addition, our ultrafast upconverted SF will achieve fine temporal resolution control of highly dynamic physiological processes that have been constrained by normal UCL.