Abstract
Nonlinear optical responses such as two-photon absorption and photoluminescence with halide perovskites are promising for the implications of fluorescence microscopy, high-density data storage, and microfabrication. Since a high degree of structural coherence can help improve the nonlinear optical responses, this study experimentally demonstrates that for individual CsPbBr3 nanocrystal superlattices, the two-photon luminescence is enhanced by about 16 times compared with that of randomly oriented nanocrystal films, and the polarization-dependent luminescence spectra reveal that the nanocrystal superlattices possess a 4-fold symmetry, which is similar to the single-crystal film structures. Due to their broad nonlinear absorption responses, wide-range interband photoluminescence is observed below the band gap. Furthermore, the intensity-dependent absorption results demonstrate that the two-photon absorption coefficient can be as large as 0.644 cm/MW, which is comparable with that of the semiconductor materials such as WS2 and ZnO. These superior performances make the CsPbBr3 nanocrystal superlattices promising for the implications of nonlinear devices such as optical power limiting and optical switches.
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