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Bulletin of the American Physical Society

Room temperature superfluorescence from a single nanocuboid

John P. Philbin, Joseph Kelly, Lintao Peng, Igor Coropceanu, Dmitri V. Talapin, Eran Rabani, Xuedan Ma, Prineha Narang

Published Mar 16, 2021• 0 citations
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Superfluorescence (SF) is a unique quantum mechanical behavior arising from the self-organization between emitters, thus forming a cooperatively coupled assembly. In contrast to isotropic spontaneous emission or normal fluorescence, SF produces a short but intense burst of light, which makes it ideal for a wide variety of applications in photonics, electronics, and optical computing. Due to the prerequisite of cooperative emitter coupling, SF has been conventionally observed under cryogenic conditions in limited systems, such as atomic gases, and a few bulk material systems. Here we show lanthanide-doped upconversion nanoparticles (UCNPs) as a medium to achieve antiStokes shift SF at room temperature. We observe such room temperature upconverted SF in a few nanoparticles assembly, and in a single nanoparticle, the latter of which is the smallest-ever SF media. In particular, we found that under near-infrared light (800 nm) excitation, each lanthanide ion in a single UCNP nanocrystal can be considered as an individual emitter that interact with each other to establish coherence and to enable anti-Stokes shift SF emission. More importantly, when compared to the microsecond scale slow lifetime of typical upconversion luminescence, the upconverted SF has a 10,000-fold accelerated lifetime (τ = 46 ns of SF v.s. τ = 455.8 μs of normal upconversion luminescence). When taken together, the observed ultrafast upconverted SF in both UCNP assembly and single nanocrystals under NIR light excitations, is uniquely well-positioned for applications in on-chip optical computing, and biophotonics, especially in deep tissue ultra-fast dynamic sensing.
Superfluorescence is a quantum optical phenomenon in which an initially excited ensemble of incoherent dipoles first acquire macroscopic coherence and then collectively recombine and radiate a burst of photons. This process is a symmetry breaking macroscopic quantum phase transition similar to superconductivity and Bose-Einstein condensation. Since quantum coherence is extremely fragile at high temperatures, similar to other macroscopic quantum phase transitions, superfluorescence has been almost always observed at cryogenic temperatures. In this presentation I will first present our results on room temperature superfluorescence in lead-halide perovskites and then present the mechanism that enables this exotic quantum phase transition at room temperature.
Superfluorescence is a collective emission from several quantum emitters that initially have random phases and are then synchronized through vacuum field interactions. Despite its fascinating prospects in quantum information processing, optical computing and advanced photonic devices, a key challenge in harnessing superfluorescence is alleviating its reliance on cryogenic conditions. Recently, room-temperature superfluorescence has been successfully achieved using upconverted nanoparticles and quasi two-dimensional lead halide perovskites. These approaches, however, are restricted to a few specific material designs and unsuitable for wide promotion. Here, we report a universal strategy to elevate the operating temperature of superfluorescence. We reveal that the symmetry-protected optical bound state in the continuum (BIC) can break the size limitation of superfluorescence (λ^3) and correlate distant but similar emitters without violating the selection rules, significantly accelerating synchronization process and promoting the possibility of room-temperature superfluorescence. This effect has been experimentally verified using a series of BIC metasurfaces made of different lead halide perovskites. Key features such as the quadratic increase in transient peak intensity and the reduction in pulse width and build-up time at the BIC wavelength confirm the realization of room-temperature superfluorescence that is absent in the pristine material. A theoretical model is also built to explain the experimental observations. This research demonstrates that the operating temperatures of coherent macroscopic states can be effectively improved by artificial field, paving a critical step towards constructing building blocks for optical and quantum applications.