Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
In the past decades, single quantum emitters have enabled a wide range of applications from nanoscopic probes to deterministic on demand single photon sources for quantum cryptography. Metal-halide perovskite nanocrystals have gained attraction due to their facile solution processability, and have recently proven very successfully for high-efficiency photovoltaics and bright light sources. Ultrahigh photoluminescence quantum yields of up to 90% were observed for fully inorganic cesium lead halide (CsPbX3, where X=Cl/Br) perovskite nanocrystals. However, it has not yet been possible to harness their exceptional photophysical properties for quantum light sources and the knowledge of their optical properties remains insufficient. Here we show that single colloidal cesium lead halide nanocrystals exhibit stable, narrowband emission with suppressed blinking and small spectral diffusion at low temperatures. The absence of Auger recombination without any shell passivation and even in the multi-exciton regime has been explained considering the relative large QD diameter (9 nm compared to the 5-7 nm Bohr radius) and the peculiar role played by defects in perovskite materials. Non-classical single-photon emission is indisputably confirmed by photon anti-bunching with energy-dependent radiative decay times on the order of 150-250 ps for CsPb(Br/Cl)3 nanocrystals, representing a significant enhancement of the recombination rate compared to other quantum emitters. Our results provide insight into the complex nature of the emission process via high-resolution and polarization-resolved spectroscopy, revealing the exciton fine structure splitting and the charged exciton emission. Due to the size- and compositional tunability combined with high oscillator strength, high quantum yield, cesium lead halide perovskite nanocrystals serve perfectly as quantum light sources. Moreover, their general versatile processibility allows integration into optical microcavities and offering a clear pathway for electrical control.
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