Enhanced Higher Harmonic Generation in Modified MAPbBr3-xClx Single Crystal by Additive Engineering.

Mixed-halide perovskite materials (MHSCs) hold significant interest in photonics applications owing to their inherent advantages, including tunable bandgap properties, remarkable defect tolerance characteristics, and facile processability. These attributes position MHSCs as up-and-coming materials for various applications. However, the commercialization of these materials is severely affected by external factors, such as humidity and oxygen. The current work studies change in higher harmonics generation (HHG) in MAPbBr3-xClx single crystals (MHSC) with changing nitrogen-based additives. These additives act as a passivating layer and improve the nanolevel crystallinity. The additive engineering strategy impacts morphological and optical properties, depending on the additive's interaction.

High-order harmonics generation in nanosecond-pulses-induced plasma containing Ni-doped CsPbBr3perovskite nanocrystals using chirp-free and chirped femtosecond pulses.

We demonstrate high-order harmonic generation in Ni-doped CsPbBr3perovskite nanocrystals ablated by nanosecond pulses using chirp-free 35 fs, and chirped 135 fs pulses in the case of single-color pump (800 nm) and a two-color pump (800 and 400 nm). We analyzed the spectral shift, cut-off, and intensity distribution of harmonics in the case of chirped drving pulses compared to chirp-free pulses. It is shown that the presence of Ni dopants and CsPbBr3plasma components improves the harmonics emission. Also, we measured the third-order nonlinear optical (NLO) properties of these nanocrystals using 800 nm, 60 fs, 1 kHz pulses. The variations of measured NLO parameters of CsPbBr3perovskite nanocrystals containing different concentrations of nickel correlate with variations of generated high-order harmonics from laser induced plasmas of studied nanocrystals in terms of harmonics intensity, cut-off, and spectral shift (in case of chirped driving pulses). The spectral shift of the harmonics generated from the Ni-doped CsPbBr3perovskite nanocrystals can be used to form tunable extreme ultraviolet sources.

Deciphering the Ultrafast Nonlinear Optical Properties and Dynamics of Pristine and Ni-Doped CsPbBr3 Colloidal Two-Dimensional Nanocrystals.

While the unabated race persists in achieving record efficiencies in solar cells and other photonic/optoelectronic devices using lead halide perovskite absorbers, a comprehensive picture of the correlated third-order nonlinear optical (NLO) properties is yet to be established. The present study is aimed at deciphering the role of dopants in multiphoton absorption properties of intentionally engineered CsPbBr3 colloidal nanocrystals (NCs). The charge separation of the plasmon-semiconductor conduction band owing to the hot electron transfer at the interface was demystified using the dynamics of the bleached spectral data from femtosecond (fs) transient absorption spectroscopy with broadband capabilities. The NLO properties studied through the fs Z-scan technique revealed that Ni-doped CsPbBr3 NCs exhibited strong third-order NLO susceptibility of ∼10-10 esu. The exotic photophysical phenomena in these pristine and Ni-doped CsPbBr3 colloidal two-dimensional (2D) NCs reported herein are believed to provide the avenues to address the critical variables involved in the structural differences and their correlated optoelectronic properties.