Abstract

Perovskite nanocrystals (NCs) have strong nonlinear optical responses with a number of potential applications, ranging from upconverted blue-lasing to the tagging of specific cellular components in multicolor fluorescence microscopy. Here, we determine the one-photon linear absorption cross section of two kinds of blue-emitting perovskite NCs, i.e., CsPbCl3 and CsPb(Cl0.53Br0.47)3, by utilizing femtosecond transient absorption spectroscopy. The wavelength-dependent nonlinear refraction and two-photon absorption have been measured at wavelengths from 620 to 720 nm by performing Z-scan measurements. The nonlinear optical responses of CsPb(Cl0.53Br0.47)3 are much more pronounced than those of CsPbCl3 due to the larger structural destabilization of the former.

© 2018 Chinese Laser Press

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2018 (1)

W. Hu, M. Xie, H. Zhao, Y. Tang, S. Yao, T. He, C. Ye, Q. Wang, X. Lu, W. Huang, and Q. Fan, “Nitric oxide activatable photosensitizer accompanying extremely elevated two-photon absorption for efficient fluorescence imaging and photodynamic therapy,” Chem. Sci. 9, 999–1005 (2018).
[Crossref]

2017 (9)

W. Hu, T. He, R. Jiang, J. Yin, L. Li, X. Lu, H. Zhao, L. Zhang, L. Huang, H. Sun, W. Huang, and Q. Fan, “Inner salt-shaped small molecular photosensitizer with extremely enhanced two-photon absorption for mitochondrial-targeted photodynamic therapy,” Chem. Commun. 53, 1680–1683 (2017).
[Crossref]

T. He, J. Li, C. Ren, S. Xiao, Y. Li, R. Chen, and X. Lin, “Strong two-photon absorption of Mn-doped CsPbCl3 perovskite nanocrystals,” Appl. Phys. Lett. 111, 211105 (2017).
[Crossref]

X. Wang, H. Zhou, S. Yuan, W. Zheng, Y. Jiang, X. Zhuang, H. Liu, Q. Zhang, X. Zhu, X. Wang, and A. Pan, “Cesium lead halide perovskite triangular nanorods as high-gain medium and effective cavities for multiphoton-pumped lasing,” Nano Res. 10, 3385–3395 (2017).
[Crossref]

W. Chen, S. Bhaumik, S. A. Veldhuis, G. Xing, Q. Xu, M. Gratzel, S. Mhaisalkar, N. Mathews, and T. C. Sum, “Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals,” Nat. Commun. 8, 15198 (2017).
[Crossref]

M. C. Brennan, J. Zinna, and M. Kuno, “Existence of a size-dependent Stokes shift in CsPbBr3 perovskite nanocrystals,” ACS Energy Lett. 2, 1487–1488 (2017).
[Crossref]

J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
[Crossref]

J. Butkus, P. Vashishtha, K. Chen, J. K. Gallaher, S. K. K. Prasad, D. Z. Metin, G. Laufersky, N. Gaston, J. E. Halpert, and J. M. Hodgkiss, “The evolution of quantum confinement in CsPbBr3 perovskite nanocrystals,” Chem. Mater. 29, 3644–3652 (2017).
[Crossref]

S. Liu, G. Chen, Y. Huang, S. Lin, Y. Zhang, M. He, W. Xiang, and X. Liang, “Tunable fluorescence and optical nonlinearities of all inorganic colloidal cesium lead halide perovskite nanocrystals,” J. Alloys Compd. 724, 889–896 (2017).
[Crossref]

J. Li, H. Dong, B. Xu, S. Zhang, Z. Cai, J. Wang, and L. Zhang, “CsPbBr3 perovskite quantum dots: saturable absorption properties and passively Q-switched visible lasers,” Photon. Res. 5, 457–460 (2017).
[Crossref]

2016 (10)

W.-G. Lu, C. Chen, D. Han, L. Yao, J. Han, H. Zhong, and Y. Wang, “Nonlinear optical properties of colloidal CH3NH3PbBr3 and CsPbBr3 quantum dots: a comparison study using Z-scan technique,” Adv. Opt. Mater. 4, 1732–1737 (2016).
[Crossref]

B. Zhao, X. Jia, J. Liu, X. Ma, H. Zhang, X. Wang, and T. Wang, “Synthesis and characterization of novel 1,4-bis(carbazolyl)benzene derivatives with blue-violet two-photon-excited fluorescence,” Ind. Eng. Chem. Res. 55, 1801–1807 (2016).
[Crossref]

R. Zhang, J. Fan, X. Zhang, H. Yu, H. Zhang, Y. Mai, T. Xu, J. Wang, and H. J. Snaith, “Nonlinear optical response of organic-inorganic halide perovskites,” ACS Photon. 3, 371–377 (2016).
[Crossref]

T. He, S. Yao, J. Zhang, Y. Li, X. Li, J. Hu, R. Chen, and X. Lin, “Strong multiphoton absorption properties of one styrylpyridinium salt in a highly polar solvent,” Opt. Express 24, 11091–11102 (2016).
[Crossref]

K. Wei, Z. Xu, R. Chen, X. Zheng, X. Cheng, and T. Jiang, “Temperature-dependent excitonic photoluminescence excited by two-photon absorption in perovskite CsPbBr3 quantum dots,” Opt. Lett. 41, 3821–3824 (2016).
[Crossref]

S. Lu, Y. Ge, Z. Sun, Z. Huang, R. Cao, C. Zhao, S. Wen, D. J. Li, and H. Zhang, “Ultrafast nonlinear absorption and nonlinear refraction in few-layer oxidized black phosphorus,” Photon. Res. 4, 286–292 (2016).
[Crossref]

N. S. Makarov, S. Guo, O. Isaienko, W. Liu, I. Robel, and V. I. Klimov, “Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots,” Nano Lett. 16, 2349–2362 (2016).
[Crossref]

Y. Xu, Q. Chen, C. Zhang, R. Wang, H. Wu, X. Zhang, G. Xing, W. W. Yu, X. Wang, Y. Zhang, and M. Xiao, “Two-photon-pumped perovskite semiconductor nanocrystal lasers,” J. Am. Chem. Soc. 138, 3761–3768 (2016).
[Crossref]

T. He, Y. Gao, S. Sreejith, X. Tian, L. Liu, Y. Wang, H. Joshi, S. Z. F. Phua, S. Yao, X. Lin, Y. Zhao, A. C. Grimsdale, and H. Sun, “Biocompatible two-photon absorbing dipyridyldiketopyrrolopyrroles for metal-ion-mediated self-assembly modulation and fluorescence imaging,” Adv. Opt. Mater. 4, 746–755 (2016).
[Crossref]

Y. Wang, X. Li, X. Zhao, L. Xiao, H. Zeng, and H. Sun, “Nonlinear absorption and low-threshold multiphoton pumped stimulated emission from all-inorganic perovskite nanocrystals,” Nano Lett. 16, 448–453 (2016).
[Crossref]

2015 (5)

T. He, W. Hu, H. Shi, Q. Pan, and X. Lin, “Strong nonlinear optical phosphorescence from water-soluble polymer dots: towards the application of two-photon bioimaging,” Dyes Pigm. 123, 218–221 (2015).
[Crossref]

A. K. Mandal, S. Sreejith, T. He, S. K. Maji, X. Wang, S. L. Ong, J. Joseph, H. Sun, and Y. Zhao, “Three-photon-excited luminescence from unsymmetrical cyanostilbene aggregates: morphology tuning and targeted bioimaging,” ACS Nano 9, 4796–4805 (2015).
[Crossref]

L. Protesescu, S. Yakunin, M. I. Bodnarchuk, F. Krieg, R. Caputo, C. H. Hendon, R. X. Yang, A. Walsh, and M. V. Kovalenko, “Nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut,” Nano Lett. 15, 3692–3696 (2015).
[Crossref]

J. Song, J. Li, X. Li, L. Xu, Y. Dong, and H. Zeng, “Quantum dot light-emitting diodes based on inorganic perovskite cesium lead halides (CsPbX3),” Adv. Mater. 27, 7162–7167 (2015).
[Crossref]

B. Guzelturk, A. L. Kanibolotsky, C. Orofino-Pena, N. Laurand, M. D. Dawson, P. J. Skabara, and H. V. Demir, “Ultralow-threshold up-converted lasing in oligofluorenes with tailored strong nonlinear absorption,” J. Mater. Chem. C 3, 12018–12025 (2015).
[Crossref]

2014 (3)

C. Wehrenfennig, M. Liu, H. J. Snaith, M. B. Johnston, and L. M. Herz, “Homogeneous emission line broadening in the organo lead halide perovskite CH3NH3PbI3-xClx,” J. Phys. Chem. Lett. 5, 1300–1306 (2014).
[Crossref]

M. Zhang, H. Yu, M. Lyu, Q. Wang, J. Yun, and L. Wang, “Composition-dependent photoluminescence intensity and prolonged recombination lifetime of perovskite CH3NH3PbBr3-xClx films,” Chem. Commun. 50, 11727–11730 (2014).
[Crossref]

Y. Wang, V. D. Ta, Y. Gao, T. C. He, R. Chen, E. Mutlugun, H. V. Demir, and H. D. Sun, “Stimulated emission and lasing from CdSe/CdS/ZnS core-multi-shell quantum dots by simultaneous three-photon absorption,” Adv. Mater. 26, 2954–2961 (2014).
[Crossref]

2012 (2)

T. He, P. C. Too, R. Chen, S. Chiba, and H. Sun, “Concise synthesis and two-photon-excited deep-blue emission of 1,8-diazapyrenes,” Chem. Asian J. 7, 2090–2095 (2012).
[Crossref]

H. Fan, L. Guo, K. Li, M. Wong, and K. W. Cheah, “Exceptionally strong multiphoton-excited blue photoluminescence and lasing from ladder-type oligo(p-phenylene)s,” J. Am. Chem. Soc. 134, 7297–7300 (2012).
[Crossref]

2011 (1)

G. S. He, J. Zhu, A. Baev, M. Samoć, D. L. Frattarelli, N. Watanabe, A. Facchetti, H. Ågren, T. J. Marks, and P. N. Prasad, “Twisted π-system chromophores for all-optical switching,” J. Am. Chem. Soc. 133, 6675–6680 (2011).
[Crossref]

2009 (1)

P. L. Wu, X. Feng, H. L. Tam, M. S. Wong, and K. W. Cheah, “Efficient three-photon excited deep blue photoluminescence and lasing of diphenylamino and 1,2,4-triazole endcapped oligofluorenes,” J. Am. Chem. Soc. 131, 886–887 (2009).
[Crossref]

2008 (2)

A. D. Lad, P. P. Kiran, D. More, G. R. Kumar, and S. Mahamuni, “Two-photon absorption in ZnSe and ZnSe/ZnS core/shell quantum structures,” Appl. Phys. Lett. 92, 043126 (2008).
[Crossref]

G. S. He, L. S. Tan, Q. Zheng, and P. N. Prasad, “Multiphoton absorbing materials: molecular designs, characterizations, and applications,” Chem. Rev. 108, 1245–1330 (2008).
[Crossref]

2004 (1)

V. V. Nikesh, A. Dharmadhikari, H. Ono, S. Nozaki, G. R. Kumar, and S. Mahamuni, “Optical nonlinearity of monodispersed, capped ZnS quantum particles,” Appl. Phys. Lett. 84, 4602–4604 (2004).
[Crossref]

1998 (1)

M. Albota, D. Beljonne, J. Brédas, J. E. Ehrlich, J. Fu, A. A. Heikal, S. E. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Röckel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1656 (1998).
[Crossref]

1995 (1)

1993 (1)

G. I. Stegeman, “Material figures of merit and implications to all-optical waveguide switching,” Proc. SPIE 1852, 75–89 (1993).
[Crossref]

1990 (1)

M. Sheik-Bahae, A. A. Said, T.-H. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive measurement of optical nonlinearities using a single beam,” IEEE J. Quantum Electron. 26, 760–769 (1990).
[Crossref]

Ågren, H.

G. S. He, J. Zhu, A. Baev, M. Samoć, D. L. Frattarelli, N. Watanabe, A. Facchetti, H. Ågren, T. J. Marks, and P. N. Prasad, “Twisted π-system chromophores for all-optical switching,” J. Am. Chem. Soc. 133, 6675–6680 (2011).
[Crossref]

Albota, M.

M. Albota, D. Beljonne, J. Brédas, J. E. Ehrlich, J. Fu, A. A. Heikal, S. E. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Röckel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1656 (1998).
[Crossref]

Al-Marri, M. J.

J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
[Crossref]

Baev, A.

G. S. He, J. Zhu, A. Baev, M. Samoć, D. L. Frattarelli, N. Watanabe, A. Facchetti, H. Ågren, T. J. Marks, and P. N. Prasad, “Twisted π-system chromophores for all-optical switching,” J. Am. Chem. Soc. 133, 6675–6680 (2011).
[Crossref]

Beljonne, D.

M. Albota, D. Beljonne, J. Brédas, J. E. Ehrlich, J. Fu, A. A. Heikal, S. E. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Röckel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1656 (1998).
[Crossref]

Bhatt, J. C.

Bhaumik, S.

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Y. Wang, V. D. Ta, Y. Gao, T. C. He, R. Chen, E. Mutlugun, H. V. Demir, and H. D. Sun, “Stimulated emission and lasing from CdSe/CdS/ZnS core-multi-shell quantum dots by simultaneous three-photon absorption,” Adv. Mater. 26, 2954–2961 (2014).
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C. Wehrenfennig, M. Liu, H. J. Snaith, M. B. Johnston, and L. M. Herz, “Homogeneous emission line broadening in the organo lead halide perovskite CH3NH3PbI3-xClx,” J. Phys. Chem. Lett. 5, 1300–1306 (2014).
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A. D. Lad, P. P. Kiran, D. More, G. R. Kumar, and S. Mahamuni, “Two-photon absorption in ZnSe and ZnSe/ZnS core/shell quantum structures,” Appl. Phys. Lett. 92, 043126 (2008).
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N. S. Makarov, S. Guo, O. Isaienko, W. Liu, I. Robel, and V. I. Klimov, “Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots,” Nano Lett. 16, 2349–2362 (2016).
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M. Albota, D. Beljonne, J. Brédas, J. E. Ehrlich, J. Fu, A. A. Heikal, S. E. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Röckel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1656 (1998).
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L. Protesescu, S. Yakunin, M. I. Bodnarchuk, F. Krieg, R. Caputo, C. H. Hendon, R. X. Yang, A. Walsh, and M. V. Kovalenko, “Nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut,” Nano Lett. 15, 3692–3696 (2015).
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A. D. Lad, P. P. Kiran, D. More, G. R. Kumar, and S. Mahamuni, “Two-photon absorption in ZnSe and ZnSe/ZnS core/shell quantum structures,” Appl. Phys. Lett. 92, 043126 (2008).
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Li, J.

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T. He, S. Yao, J. Zhang, Y. Li, X. Li, J. Hu, R. Chen, and X. Lin, “Strong multiphoton absorption properties of one styrylpyridinium salt in a highly polar solvent,” Opt. Express 24, 11091–11102 (2016).
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T. He, J. Li, C. Ren, S. Xiao, Y. Li, R. Chen, and X. Lin, “Strong two-photon absorption of Mn-doped CsPbCl3 perovskite nanocrystals,” Appl. Phys. Lett. 111, 211105 (2017).
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T. He, S. Yao, J. Zhang, Y. Li, X. Li, J. Hu, R. Chen, and X. Lin, “Strong multiphoton absorption properties of one styrylpyridinium salt in a highly polar solvent,” Opt. Express 24, 11091–11102 (2016).
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S. Liu, G. Chen, Y. Huang, S. Lin, Y. Zhang, M. He, W. Xiang, and X. Liang, “Tunable fluorescence and optical nonlinearities of all inorganic colloidal cesium lead halide perovskite nanocrystals,” J. Alloys Compd. 724, 889–896 (2017).
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S. Liu, G. Chen, Y. Huang, S. Lin, Y. Zhang, M. He, W. Xiang, and X. Liang, “Tunable fluorescence and optical nonlinearities of all inorganic colloidal cesium lead halide perovskite nanocrystals,” J. Alloys Compd. 724, 889–896 (2017).
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T. He, J. Li, C. Ren, S. Xiao, Y. Li, R. Chen, and X. Lin, “Strong two-photon absorption of Mn-doped CsPbCl3 perovskite nanocrystals,” Appl. Phys. Lett. 111, 211105 (2017).
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T. He, S. Yao, J. Zhang, Y. Li, X. Li, J. Hu, R. Chen, and X. Lin, “Strong multiphoton absorption properties of one styrylpyridinium salt in a highly polar solvent,” Opt. Express 24, 11091–11102 (2016).
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J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
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N. S. Makarov, S. Guo, O. Isaienko, W. Liu, I. Robel, and V. I. Klimov, “Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots,” Nano Lett. 16, 2349–2362 (2016).
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W. Hu, M. Xie, H. Zhao, Y. Tang, S. Yao, T. He, C. Ye, Q. Wang, X. Lu, W. Huang, and Q. Fan, “Nitric oxide activatable photosensitizer accompanying extremely elevated two-photon absorption for efficient fluorescence imaging and photodynamic therapy,” Chem. Sci. 9, 999–1005 (2018).
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A. D. Lad, P. P. Kiran, D. More, G. R. Kumar, and S. Mahamuni, “Two-photon absorption in ZnSe and ZnSe/ZnS core/shell quantum structures,” Appl. Phys. Lett. 92, 043126 (2008).
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N. S. Makarov, S. Guo, O. Isaienko, W. Liu, I. Robel, and V. I. Klimov, “Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots,” Nano Lett. 16, 2349–2362 (2016).
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A. K. Mandal, S. Sreejith, T. He, S. K. Maji, X. Wang, S. L. Ong, J. Joseph, H. Sun, and Y. Zhao, “Three-photon-excited luminescence from unsymmetrical cyanostilbene aggregates: morphology tuning and targeted bioimaging,” ACS Nano 9, 4796–4805 (2015).
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M. Albota, D. Beljonne, J. Brédas, J. E. Ehrlich, J. Fu, A. A. Heikal, S. E. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Röckel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1656 (1998).
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G. S. He, J. Zhu, A. Baev, M. Samoć, D. L. Frattarelli, N. Watanabe, A. Facchetti, H. Ågren, T. J. Marks, and P. N. Prasad, “Twisted π-system chromophores for all-optical switching,” J. Am. Chem. Soc. 133, 6675–6680 (2011).
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J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
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J. Butkus, P. Vashishtha, K. Chen, J. K. Gallaher, S. K. K. Prasad, D. Z. Metin, G. Laufersky, N. Gaston, J. E. Halpert, and J. M. Hodgkiss, “The evolution of quantum confinement in CsPbBr3 perovskite nanocrystals,” Chem. Mater. 29, 3644–3652 (2017).
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W. Chen, S. Bhaumik, S. A. Veldhuis, G. Xing, Q. Xu, M. Gratzel, S. Mhaisalkar, N. Mathews, and T. C. Sum, “Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals,” Nat. Commun. 8, 15198 (2017).
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A. D. Lad, P. P. Kiran, D. More, G. R. Kumar, and S. Mahamuni, “Two-photon absorption in ZnSe and ZnSe/ZnS core/shell quantum structures,” Appl. Phys. Lett. 92, 043126 (2008).
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V. V. Nikesh, A. Dharmadhikari, H. Ono, S. Nozaki, G. R. Kumar, and S. Mahamuni, “Optical nonlinearity of monodispersed, capped ZnS quantum particles,” Appl. Phys. Lett. 84, 4602–4604 (2004).
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J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
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A. K. Mandal, S. Sreejith, T. He, S. K. Maji, X. Wang, S. L. Ong, J. Joseph, H. Sun, and Y. Zhao, “Three-photon-excited luminescence from unsymmetrical cyanostilbene aggregates: morphology tuning and targeted bioimaging,” ACS Nano 9, 4796–4805 (2015).
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B. Guzelturk, A. L. Kanibolotsky, C. Orofino-Pena, N. Laurand, M. D. Dawson, P. J. Skabara, and H. V. Demir, “Ultralow-threshold up-converted lasing in oligofluorenes with tailored strong nonlinear absorption,” J. Mater. Chem. C 3, 12018–12025 (2015).
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X. Wang, H. Zhou, S. Yuan, W. Zheng, Y. Jiang, X. Zhuang, H. Liu, Q. Zhang, X. Zhu, X. Wang, and A. Pan, “Cesium lead halide perovskite triangular nanorods as high-gain medium and effective cavities for multiphoton-pumped lasing,” Nano Res. 10, 3385–3395 (2017).
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Pan, Q.

T. He, W. Hu, H. Shi, Q. Pan, and X. Lin, “Strong nonlinear optical phosphorescence from water-soluble polymer dots: towards the application of two-photon bioimaging,” Dyes Pigm. 123, 218–221 (2015).
[Crossref]

Perry, J. W.

M. Albota, D. Beljonne, J. Brédas, J. E. Ehrlich, J. Fu, A. A. Heikal, S. E. Hess, T. Kogej, M. D. Levin, S. R. Marder, D. McCord-Maughon, J. W. Perry, H. Röckel, M. Rumi, G. Subramaniam, W. W. Webb, X.-L. Wu, and C. Xu, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1656 (1998).
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T. He, Y. Gao, S. Sreejith, X. Tian, L. Liu, Y. Wang, H. Joshi, S. Z. F. Phua, S. Yao, X. Lin, Y. Zhao, A. C. Grimsdale, and H. Sun, “Biocompatible two-photon absorbing dipyridyldiketopyrrolopyrroles for metal-ion-mediated self-assembly modulation and fluorescence imaging,” Adv. Opt. Mater. 4, 746–755 (2016).
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G. S. He, J. Zhu, A. Baev, M. Samoć, D. L. Frattarelli, N. Watanabe, A. Facchetti, H. Ågren, T. J. Marks, and P. N. Prasad, “Twisted π-system chromophores for all-optical switching,” J. Am. Chem. Soc. 133, 6675–6680 (2011).
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L. Protesescu, S. Yakunin, M. I. Bodnarchuk, F. Krieg, R. Caputo, C. H. Hendon, R. X. Yang, A. Walsh, and M. V. Kovalenko, “Nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I): novel optoelectronic materials showing bright emission with wide color gamut,” Nano Lett. 15, 3692–3696 (2015).
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J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
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Reinhardt, B. A.

Ren, C.

T. He, J. Li, C. Ren, S. Xiao, Y. Li, R. Chen, and X. Lin, “Strong two-photon absorption of Mn-doped CsPbCl3 perovskite nanocrystals,” Appl. Phys. Lett. 111, 211105 (2017).
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Robel, I.

N. S. Makarov, S. Guo, O. Isaienko, W. Liu, I. Robel, and V. I. Klimov, “Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots,” Nano Lett. 16, 2349–2362 (2016).
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M. Zhang, H. Yu, M. Lyu, Q. Wang, J. Yun, and L. Wang, “Composition-dependent photoluminescence intensity and prolonged recombination lifetime of perovskite CH3NH3PbBr3-xClx films,” Chem. Commun. 50, 11727–11730 (2014).
[Crossref]

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Y. Wang, X. Li, X. Zhao, L. Xiao, H. Zeng, and H. Sun, “Nonlinear absorption and low-threshold multiphoton pumped stimulated emission from all-inorganic perovskite nanocrystals,” Nano Lett. 16, 448–453 (2016).
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Y. Xu, Q. Chen, C. Zhang, R. Wang, H. Wu, X. Zhang, G. Xing, W. W. Yu, X. Wang, Y. Zhang, and M. Xiao, “Two-photon-pumped perovskite semiconductor nanocrystal lasers,” J. Am. Chem. Soc. 138, 3761–3768 (2016).
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S. Liu, G. Chen, Y. Huang, S. Lin, Y. Zhang, M. He, W. Xiang, and X. Liang, “Tunable fluorescence and optical nonlinearities of all inorganic colloidal cesium lead halide perovskite nanocrystals,” J. Alloys Compd. 724, 889–896 (2017).
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J. Chen, K. Žídek, P. Chábera, D. Liu, P. Cheng, L. Nuuttila, M. J. Al-Marri, H. Lehtivuori, M. E. Messing, K. Han, K. Zheng, and T. Pullerits, “Size- and wavelength-dependent two-photon absorption cross-section of CsPbBr3 perovskite quantum dots,” J. Phys. Chem. Lett. 8, 2316–2321 (2017).
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Figures (6)

Fig. 1.
Fig. 1. (a) Normalized linear absorption and fluorescence spectra for the perovskite NCs. The insets are the emission images of the NCs in solution: 1 for CsPbCl3 NCs and 2 for CsPb(Cl0.53Br0.47)3 NCs. TEM images of (b) CsPbCl3 NCs and (c) CsPb(Cl0.53Br0.47)3 NCs. The insets are high-resolution TEM images of the NCs. (d) Fluorescence decay kinetics of the perovskite NCs under excitation at 365 nm.
Fig. 2.
Fig. 2. TA kinetics (a) for CsPbCl3 NCs probed at 398 nm and (c) for CsPb(Cl0.53Br0.47)3 NCs probed at 432 nm. Initially, the presence of biexcitons and even higher order multi-excitons causes a fast decay (Auger process). At time 1  ns, the signals decay exponentially, which corresponds to a single-exciton signal. GSB signal amplitude at a time delay of 1 ns as a function of excitation intensity for (b) CsPbCl3 NCs and (d) CsPb(Cl0.53Br0.47)3 NCs.
Fig. 3.
Fig. 3. Measured fluorescence intensity as a function of the input laser intensity at 650 nm. The insets are the two-photon excited emission imaging of the NC solution and the best-fitting straight lines on logarithmic scales: 1 for CsPbCl3 NCs and 2 for CsPb(Cl0.53Br0.47)3 NCs. The concentration of CsPb(Cl0.53Br0.47)3 NCs solution is 1×106  M, while the concentration of CsPbCl3 NCs solution is 2.57×106  M.
Fig. 4.
Fig. 4. (a) Divided Z-scan results of the OA signal for NCs at a wavelength of 650 nm. The solid lines are the fittings to the data using the Z-scan theory. (b) TPA spectra of NCs between 620 and 720 nm. The concentration of both CsPbCl3 and CsPb(Cl0.53Br0.47)3 NCs was 5.95×106  M.
Fig. 5.
Fig. 5. (a) Divided Z-scan results of the CA signal by the OA signal at a wavelength of 650 nm. The solid lines are the fittings to the data using the Z-scan theory. (b) Wavelength-dependent intrinsic nonlinear refractive index of CsPb(Cl0.53Br0.47)3 NCs. The concentration of both CsPbCl3 and CsPb(Cl0.53Br0.47)3 NCs was 5.95×106  M.
Fig. 6.
Fig. 6. Wavelength-dependent figure of merit (T) of CsPb(Cl0.53Br0.47)3 NCs.

Tables (1)

Tables Icon

Table 1. Calculated NLO Parameters of the CsPbCl3 and CsPb(Cl0.53Br0.47)3 NCs and Other Materials Reported Elsewhere

Equations (2)

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A(I/I0)=Amax[1e(I/I0)·σ·I0],
n2(solution)=gn2(intrinsic)+(1g)n2(hexane),