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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 plasmonsemiconductor 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 twodimensional (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. P colloidal semiconductor nanocrystals (NCs)/ nanoplates (NPs) are an emerging class of nonlinear optical (NLO)/photonic materials because of their remarkable optoelectronic properties and promising applications in the field of light-emitting diodes (LEDs). The evolution of the organic−inorganic lead halide perovskites (OIHPs) has sparked research interest in both academia and industry because of OIHPs’ intriguing properties. Halide perovskites possess galvanizing properties such as high carrier mobility and tunable photoluminescence (PL) and have been widely investigated in the field of photovoltaics, light-emitting diodes, and lasing applications. To date, most of the research has been devoted to enhancing the efficient phononassisted photoluminescence (PL) up conversion and near-unity external quantum efficiencies (EQEs) of the all-inorganic perovskite quantum dots (QDs). However, the profound understanding of the photophysical properties of all-inorganic lead halide perovskites (IHPs) has not been fully explored. Among the all IHP NCs, CsPbX3 (X = Cl, Br, I) based NCs are alluring candidates for promising light emitters, by virtue of their tunable (sizeand composition-dependent) band gap from the violet to the near-infrared region, and also possess extremely narrow full width at half-maximum (fwhm). The added advantage is the facile tunability of their absorption edges and emission colors via anion and or cation exchange reactions. The IHP two-dimensional (2D) colloidal NCs have been demonstrated to exhibit strong multiphoton absorption (MPA). The semiconductor NC geometries are known to induce a promising effect on the NLO properties. Semiconductor 2D NPs possess striking optical properties, such as narrow PL emission at room temperature together with their substantial oscillator strength, which can be altered by their vertical thickness. It is anticipated that the strong confinement in the vertical direction for perovskite 2D NCs can improve their linear optical as well as the NLO properties. These properties are the prerequisites for high performance in NLO and photonic applications. Additionally, CsPbX3 NCs possess high photoluminescence quantum yields (PLQY), in some cases as high as up to 90%; narrow emission bandwidth; tunable PL emission spectra; and higher stability compared with CH3NH3PbX3, making them alluring semiconductors for next-generation optoelectronic applications. Received: August 1, 2019 Accepted: August 30, 2019 Published: August 30, 2019 Letter pubs.acs.org/JPCL Cite This: J. Phys. Chem. Lett. 2019, 10, 5577−5584 © XXXX American Chemical Society 5577 DOI: 10.1021/acs.jpclett.9b02244 J. Phys. Chem. Lett. 2019, 10, 5577−5584 D ow nl oa de d vi a U N IV O F H Y D E R A B A D o n Se pt em be r 13 , 2 01 9 at 0 7: 38 :5 6 (U T C ). Se e ht tp s: //p ub s. ac s. or g/ sh ar in gg ui de lin es f or o pt io ns o n ho w to le gi tim at el y sh ar e pu bl is he d ar tic le s.

Deciphering the Ultrafast Nonlinear Optical Properties and Dynamics of Pristine and Ni-Doped CsPbBr 3 Colloidal Two-Dimensional Nanocrystals