Broadband femtosecond nonlinear optical properties of CsPbBr_3 perovskite nanocrystals

Katturi, Naga Krishnakanth; Seth, Sudipta; Samanta, Anunay; Soma, Venugopal Rao

doi:10.1364/ol.43.000603

Cited by 67 publications

(72 citation statements)

References 32 publications

(56 reference statements)

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“…The nonlinear absorption coefficient of the CsPbBr 3 film sample is obtained to be 19.4 ± 0.5 cm/GW by the fitting procedure . This value is far larger than the reported TPA coefficient of most CsPbBr 3 quantum dots and nanocrystals (below 1 cm/GW) . However, it is still reasonable compared with the ≈5.00 cm/GW of CsPbBr 3 bulk crystal, particularly considering the CsPbBr 3 nanosheets were proved to have a TPA coefficient (up to ≈10.94 cm/GW) inversely proportional with the thickness .…”

Section: Resultsmentioning

confidence: 71%

“…CsPbX 3 are not only efficient light‐harvesting materials, but also light‐emitting materials with extremely high fluorescence quantum yield, narrow emission bandwidth, low lasing threshold, and tunable bandgap, which make them strong contenders for high‐performance of light emitting diodes (LEDs), lasers, and photodetectors . CsPbX 3 are also proved to be excellent nonlinear optical absorbers with strong third order nonlinear susceptibility (≈10 −10 esu) and large two‐photon absorption (TPA) cross‐sections (≈10 5 GM), which are two orders of magnitude larger than those of traditional quantum dots . Meanwhile, these CsPbX 3 are also outstanding frequency up‐conversion emitters with low threshold of multiphoton pumped stimulated emission, large penetration depth, less damage threshold, and high spatial resolution, which make them significant in potential nonlinear optoelectronic applications such as two‐photon or multiphoton microscopy and spectroscopy .…”

Section: Introductionmentioning

confidence: 99%

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High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

Huang

et al. 2019

Adv Funct Materials

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High-order nonlinear optical phenomena are interesting from a fundamental point of view as they reveal intrinsic symmetries of the materials. Potentially they can also be used for practical optoelectronic applications. High-order shift current is one of these phenomena, and yet it has never been detected in experiments, primarily due to the difficulty in conventional contact detection. In this work, the shift current due to the two-photon absorption (TPA) from all-inorganic perovskite CsPbBr 3 is first observed by a contactless and nondestructive terahertz (THz) emission method. The results reveal that the THz emission is dominated by a high-order shift current (fourth-order nonlinear optical effect) with the below-bandgap photon energy of femtosecond laser excitation. The high-order shift current origins from the broken inversion symmetry induced by the dynamic stereochemical activity of the Pb 2+ lone pair. A microscopic TPA-assisted nonlinear optical model is presented to describe the photophysical process of the THz emission. The model matches well with the quadratic pump fluence and angular dependence of the THz emission. This work can not only open a new venue for the all-inorganic perovskite-based nonlinear optoelectronics and THz devices, but also afford a THz technology for the high-order nonlinear effect analysis.

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Section: Resultsmentioning

confidence: 71%

Section: Introductionmentioning

confidence: 99%

High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

Huang

et al. 2019

Adv Funct Materials

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“…The photoluminescence of MAPbBr 3 single crystal has also been observed in the green region (522–550 nm) with 1044 nm femtosecond laser excitation due to 2PA 26. Similar nonlinear optical properties were reported in inorganic perovskites, including CsPbI 3 and CsPbBr 3 22,27,28…”

Section: Introductionmentioning

confidence: 99%

Giant Nonlinear Optical Response in Triple Cation Halide Mixed Perovskite Films

Hamad

Kong

Venkatesh

et al. 2020

Advanced Optical Materials

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exceptional properties including high photostability, extremely long charge diffusion length, and thermal stability. The perovskites have become emerging high-performance materials for various optoelectronic applications such as solar cells, [1][2][3] light emitting diodes, [4,5] photodetectors, [6,7] and lasers. [8,9] The halide perovskites also exhibit strong nonlinear optical (NLO) responses, thus opening up possibilities for optoelectronic device applications. [10][11][12][13][14] For instance, organic-inorganic hybrid perovskites with large two-and three-photon absorption (2PA, 3PA) properties [14][15][16] can be utilized in applications such as bioimaging, [17,18] optical limiting, [19] optical sensor protection, [20] and optical data storage. [21] Nonlinear absorption properties of single crystal, nanocrystal, and filmed perovskites have been intensively studied. [10][11][12][13][14][15][16][22][23][24] Recently, lead halide perovskites such as MAPbI 3 (MA = CH 3 NH 3 ) and MAPbBr 3 have shown higher multiphoton absorption (MPA) probability as the excitation wavelength increases in the IR region. [10][11][12][13][14][22][23][24] Johnson et al. [25] reported that the observation of third-order nonlinearities and decay kinetics in MAPbBr 3 and MAPbBr 2 I with different halogen composition. They showed that the third-order nonlinearities of these materials are larger than those of conventional semiconductors. The photoluminescence of MAPbBr 3 single crystal has also been observed in the green region (522-550 nm) with 1044 nm femtosecond laser excitation due to 2PA. [26] Similar nonlinear optical properties were reported in inorganic perovskites, including CsPbI 3 and CsPbBr 3 . [22,27,28] Another type of perovskite, formamidinium lead iodide (FAPbI 3 ), has a low bandgap (1.47 eV) and greater photostability and thermal stability [29,30] than MAPbI 3 . However, FAPbI 3 has a weak structural stability due to humidity, which prevents it from real-life applications. [31] Recently, it has been demonstrated that the mixture of Cs and MAPbI 3 , CsMAPbI 3 , can lead to a stable solar cell with power conversion efficiency of ≈8%. [32] In addition, the mixture of Cs in FAPbI 3 , such as FA 0.9 Cs 0.1 PbI 3 , showed an improved thermal stability and results in high power conversion efficiency of ≈16.5%. [33] By using this material, Yi et al. have demonstrated power conversion efficiency up to 18% with a halide mixer I/Br. [34] The malleable association The versatility of perovskites through chemical composition modification is critical for enhancing performance of a range of potential applications such as light emitters and integrated photovoltaics. However, a systematic study on the nonlinear optical (NLO) responses of these perovskites is still lacking. Here, for the first time, the NLO properties of triple cation mixed halide perovskite (TCMHP) films, (Cs 0.06 FA 0.79 MA 0.15 )Pb (I 0.85 Br 0.15 ) 3 , using Z-scan and time-resolved spectroscopy, are investigated. It is found that TCMHP film shows strong saturable abs...

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“…On one hand, there have been many experimental reports [5][6][7][8][9][10][11][12][13][14][15] on the enhancement of MPA coefficients or cross-sections if one utilizes nanostructured perovskites, such as in 2D forms, or quantum dots (QDs). For example, the three-photon absorption (3PA) action cross sections have been reported as high as 10 −73 cm 6 s 2 photon −2 for perovskite QDs with diameters of 8-10 nm.…”

Section: Introductionmentioning

confidence: 99%

Layered Hybrid Perovskites for Highly Efficient Three‐Photon Absorbers: Theory and Experimental Observation

Zhou

Zhang

et al. 2018

Advanced Science

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Multiphoton absorption may find many technological applications, such as enhancing the conversion efficiency of solar cells by the utilization of sub‐band‐energy photons, below‐bandgap photodetection through the simultaneous absorption of several infrared photons for photocurrent generation, or light frequency upconversion for high‐resolution, 3D imaging. To enhance multiphoton absorption in semiconducting materials, one of the strategies is to explore low‐dimensional excitons. Here, a quantum perturbation theory on a giant enhancement in three‐photon absorption (3PA) arising from 2D excitons in multilayered crystals of organic–inorganic hybrid perovskites is presented. The maximal 3PA coefficient is predicted to be in the range of 2–7 cm 3 GW −2 at 1100 nm, the largest values reported so far for any 2D and bulk semiconductors at room temperature. Excellent agreement between theory and the experimental findings unambiguously demonstrates a pivotal role in the enhancement of 3PA played by 2D excitons. The theory predicts that the resonant 3PA coefficient should be enhanced further by at least two orders of magnitude with very low temperature. The findings are essential for understanding giant 3PA arising from 2D excitons in layered hybrid perovskites and may open new pathways for highly efficient conversion from infrared light energy to either electrical energy or higher‐frequency light emission/lasing.

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Broadband femtosecond nonlinear optical properties of CsPbBr_3 perovskite nanocrystals

Cited by 67 publications

References 32 publications

High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

Giant Nonlinear Optical Response in Triple Cation Halide Mixed Perovskite Films

Layered Hybrid Perovskites for Highly Efficient Three‐Photon Absorbers: Theory and Experimental Observation

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