Giant Third-Order Nonlinear Response of Mixed Perovskite Nanocrystals |
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Authors: | Aya M Abu Baker Ganjaboy S Boltaev Mazhar Iqbal Mikhail Pylnev Nasser M Hamdan Ali S Alnaser |
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Institution: | 1.Department of Physics, American University of Sharjah, Sharjah 26666, United Arab Emirates; (A.M.A.B.); (M.I.); (N.M.H.);2.Institute of Ion Plasma and Laser Technologies, Uzbek Academy of Sciences, Tashkent 100125, Uzbekistan;3.Centre for Advanced Materials Research, University of Sharjah, Sharjah 27272, United Arab Emirates; |
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Abstract: | Mixed (FAPbI3)0.92(MAPbBr3)0.08 perovskite thin films exhibit strong nonlinear optical responses, rendering them promising candidates for applications in photonics and optical communications. In this work, we present a systematic study on the ultrafast third-order nonlinear optical processes in mixed perovskite nanocrystals (NCs) by exploring the generation of third harmonic radiation and giant two-photon absorption-based photoluminescence (PL) when excited by femtosecond laser pulses of a 1030 nm central wavelength. A comparative analysis of the coherent third harmonic generation in the thin-film-containing perovskite nanocrystals has shown a 40× enhancement of the third harmonic signal compared to the signal generated in the pure quartz substrate. The cubic dependence of the third-nonlinear optical response of the (FAPbI3)0.92(MAPbBr3)0.08 perovskites on the intensity of the driving radiation was identified using broadband 38 femtosecond driving pulses. The positive nonlinear refractive index (γ = +1.4 × 10−12 cm2·W−1) is found to play an important role in improving the phase-matching conditions of the interacting pulses by generating a strong third order harmonic. The giant two-photon absorption (TPA)-assisted PL peak was monitored and a blue shift of the PL was obtained in the higher intensity range of the laser pulses, with the absorption coefficient β estimated to be~+7.0 cm·MW−1 at a 1030 nm laser wavelength. |
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Keywords: | ultrashort pulses mixed perovskite third harmonic generation two-photon absorption laser– matter interactions |
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