Abstract

Optical performance of the lead halide perovskites with zero-dimension (0D) structure has been in a hot debate for optoelectronic applications. Here, Cs4PbBr6 hexagonal micro-particles with a remarkable green emission are first fabricated via a low-temperature solution-process employed ethanol as solvent. Our results underline that the existence of bromine vacancies and the introduction of hydroxyl induce a narrowed band gap with the formation of a defect level, which contributes to the extrinsic photoluminescence (PL) properties synergistically. Thanks to the high exciton binding energy and the unique morphology with a regular geometric structure of the as-obtained micro-particles, two-photon pumped amplified spontaneous emission (ASE) and single mode lasing from an individual Cs4PbBr6 particle are realized. Our results not only provide an insight into the origin of optical emission from Cs4PbBr6, but also demonstrate that the versatile Cs4PbBr6 offers a new opportunity for novel nonlinear photonics applications as an up-conversion laser.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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    [Crossref]
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    [Crossref]
  4. M. Wei, F. P. G. de Arquer, G. Walters, Z. Yang, L. N. Quan, Y. Kim, R. Sabatini, R. Quintero-Bermudez, L. Gao, J. Z. Fan, F. Fan, A. Gold-Parker, M. F. Toney, and E. H. Sargent, “Ultrafast narrowband exciton routing within layered perovskite nanoplatelets enables low-loss luminescent solar concentrators,” Nat. Energy 4(3), 197–205 (2019).
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    [Crossref]
  6. J. Yin, Y. Zhang, A. Bruno, C. Soci, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Intrinsic Lead Ion Emissions in Zero-Dimensional Cs4PbBr6 Nanocrystals,” ACS Energy Lett. 2(12), 2805–2811 (2017).
    [Crossref]
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    [Crossref]
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    [Crossref]
  13. Z. Zhang, Y. Zhu, W. Wang, W. Zheng, R. Lin, X. Li, H. Zhang, D. Zhong, and F. Huang, “Aqueous Solution Growth of Millimeter-Sized Nongreen-Luminescent Wide Bandgap Cs4PbBr6 Bulk Crystal,” Cryst. Growth Des. 18(11), 6393–6398 (2018).
    [Crossref]
  14. Q. A. Akkerman, S. Park, E. Radicchi, F. Nunzi, E. Mosconi, F. De Angelis, R. Brescia, P. Rastogi, M. Prato, and L. Manna, “Nearly Monodisperse Insulator Cs4PbX6 (X = Cl, Br, I) Nanocrystals, Their Mixed Halide Compositions, and Their Transformation into CsPbX3 Nanocrystals,” Nano Lett. 17(3), 1924–1930 (2017).
    [Crossref]
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    [Crossref]
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    [Crossref]
  17. Y. Wang, D. Yu, Z. Wang, X. Li, X. Chen, V. Nalla, H. Zeng, and H. Sun, “Solution-Grown CsPbBr3/Cs4PbBr6 Perovskite Nanocomposites: Toward Temperature-Insensitive Optical Gain,” Small 13(34), 1701587 (2017).
    [Crossref]
  18. J. Yin, H. Yang, K. Song, A. M. El-Zohry, Y. Han, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Point Defects and Green Emission in Zero-Dimensional Perovskites,” J. Phys. Chem. Lett. 9(18), 5490–5495 (2018).
    [Crossref]
  19. S. Seth, N. Mondal, S. Patra, and A. Samanta, “Fluorescence Blinking and Photoactivation of All-Inorganic Perovskite Nanocrystals CsPbBr3 and CsPbBr2I,” J. Phys. Chem. Lett. 7(2), 266–271 (2016).
    [Crossref]
  20. J. M. Ball and A. Petrozza, “Defects in perovskite-halides and their effects in solar cells,” Nat. Energy 1(11), 16149 (2016).
    [Crossref]
  21. J. Kang and L.-W. Wang, “High Defect Tolerance in Lead Halide Perovskite CsPbBr3,” J. Phys. Chem. Lett. 8(2), 489–493 (2017).
    [Crossref]
  22. S. Seth and A. Samanta, “Fluorescent Phase-Pure Zero-Dimensional Perovskite-Related Cs4PbBr6 Microdisks: Synthesis and Single-Particle Imaging Study,” J. Phys. Chem. Lett. 8(18), 4461–4467 (2017).
    [Crossref]
  23. L. N. Quan, M. Yuan, R. Comin, O. Voznyy, E. M. Beauregard, S. Hoogland, A. Buin, A. R. Kirmani, K. Zhao, A. Amassian, D. H. Kim, and E. H. Sargent, “Ligand-Stabilized Reduced-Dimensionality Perovskites,” J. Am. Chem. Soc. 138(8), 2649–2655 (2016).
    [Crossref]
  24. Y. Fang, H. Wei, Q. Dong, and J. Huang, “Quantification of re-absorption and re-emission processes to determine photon recycling efficiency in perovskite single crystals,” Nat. Commun. 8(1), 14417 (2017).
    [Crossref]
  25. B. Turedi, K. J. Lee, I. Dursun, B. Alamer, Z. Wu, E. Alarousu, O. F. Mohammed, N. Cho, and O. M. Bakr, “Water-induced dimensionality reduction in metal-halide perovskites,” J. Phys. Chem. C 122(25), 14128–14134 (2018).
    [Crossref]
  26. X. Gong, M. Li, X.-B. Shi, H. Ma, Z.-K. Wang, and L.-S. Liao, “Controllable Perovskite Crystallization by Water Additive for High-Performance Solar Cells,” Adv. Funct. Mater. 25(42), 6671–6678 (2015).
    [Crossref]
  27. W. Zhou, Y. Zhao, C. Shi, H. Huang, J. Wei, R. Fu, K. Liu, D. Yu, and Q. Zhao, “Reversible Healing Effect of Water Molecules on Fully Crystallized Metal–Halide Perovskite Film,” J. Mater. Chem. C 120(9), 4759–4765 (2016).
    [Crossref]
  28. S. J. Clark, M. D. Segall, C. J. Pickard, P. J. Hasnip, M. I. Probert, K. Refson, and M. C. Payne, “First principles methods using CASTEP,” Z. Kristallogr. - Cryst. Mater. 220(5/6), 567–570 (2005).
    [Crossref]
  29. D. Vanderbilt, “Soft self-consistent pseudopotentials in a generalized eigenvalue formalism,” Phys. Rev. B 41(11), 7892–7895 (1990).
    [Crossref]
  30. J. P. Perdew, K. Burke, and K. M. Ernzerhof, “Generalized Gradient Approximation Made Simple,” Phys. Rev. Lett. 77(18), 3865–3868 (1996).
    [Crossref]
  31. H. J. Monkhorst and J. D. Pack, “Special points for Brillouin-zone integrations,” Phys. Rev. B 13(12), 5188–5192 (1976).
    [Crossref]
  32. L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
    [Crossref]
  33. B. Kang and K. Biswas, “Exploring Polaronic, Excitonic Structures and Luminescence in Cs4PbBr6/CsPbBr3,” J. Phys. Chem. Lett. 9(4), 830–836 (2018).
    [Crossref]
  34. N. Riesen, M. Lockrey, K. Badek, and H. Riesen, “On the origins of the green luminescence in the “zero-dimensional perovskite” Cs4PbBr6: conclusive results from cathodoluminescence imaging,” Nanoscale 11(9), 3925–3932 (2019).
    [Crossref]
  35. Q. A. Akkerman, A. L. Abdelhady, and L. Manna, “Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges,” J. Phys. Chem. Lett. 9(9), 2326–2337 (2018).
    [Crossref]
  36. S. Chen, X. Wen, S. Huang, F. Huang, Y.-B. Cheng, M. Green, and A. Ho-Baillie, “Light Illumination Induced Photoluminescence Enhancement and Quenching in Lead Halide Perovskite,” Sol. RRL 1(1), 1600001 (2017).
    [Crossref]
  37. B. Zhou, M. Jiang, H. Dong, W. Zheng, Y. Huang, J. Han, A. Pan, and L. Zhang, “High-Temperature Upconverted Single-Mode Lasing in 3D Fully Inorganic Perovskite Microcubic Cavity,” ACS Photonics 6(3), 793–801 (2019).
    [Crossref]

2019 (7)

M. Abdi-Jalebi, M. Ibrahim Dar, S. P. Senanayak, A. Sadhanala, Z. Andaji-Garmaroudi, L. M. Pazos-Outón, J. M. Richter, A. J. Pearson, H. Sirringhaus, M. Grätzel, and R. H. Friend, “Charge extraction via graded doping of hole transport layers gives highly luminescent and stable metal halide perovskite devices,” Sci. Adv. 5(2), eaav2012 (2019).
[Crossref]

M. Wei, F. P. G. de Arquer, G. Walters, Z. Yang, L. N. Quan, Y. Kim, R. Sabatini, R. Quintero-Bermudez, L. Gao, J. Z. Fan, F. Fan, A. Gold-Parker, M. F. Toney, and E. H. Sargent, “Ultrafast narrowband exciton routing within layered perovskite nanoplatelets enables low-loss luminescent solar concentrators,” Nat. Energy 4(3), 197–205 (2019).
[Crossref]

J. W. Choi, N. Cho, H. C. Woo, B. M. Oh, J. Almutlaq, O. M. Bakr, S.-H. Kim, C.-L. Lee, and J. H. Kim, “Investigation of high contrast and reversible luminescence thermochromism of the quantum confined Cs4PbBr6 perovskite solid,” Nanoscale 11(12), 5754–5759 (2019).
[Crossref]

Q. Luo, H. Wang, X. Yin, and L. Wang, “Hydrophilic perovskite microdisks with excellent stability and strong fluorescence for recyclable temperature sensing,” Sci. China Mater. 62(7), 1065–1070 (2019).
[Crossref]

L. Rao, X. Ding, X. Du, G. Liang, Y. Tang, K. Tang, and J. Z. Zhang, “Ultrasonication-assisted synthesis of CsPbBr3 and Cs4PbBr6 perovskite nanocrystals and their reversible transformation,” Beilstein J. Nanotechnol. 10(1), 666–676 (2019).
[Crossref]

N. Riesen, M. Lockrey, K. Badek, and H. Riesen, “On the origins of the green luminescence in the “zero-dimensional perovskite” Cs4PbBr6: conclusive results from cathodoluminescence imaging,” Nanoscale 11(9), 3925–3932 (2019).
[Crossref]

B. Zhou, M. Jiang, H. Dong, W. Zheng, Y. Huang, J. Han, A. Pan, and L. Zhang, “High-Temperature Upconverted Single-Mode Lasing in 3D Fully Inorganic Perovskite Microcubic Cavity,” ACS Photonics 6(3), 793–801 (2019).
[Crossref]

2018 (7)

B. Kang and K. Biswas, “Exploring Polaronic, Excitonic Structures and Luminescence in Cs4PbBr6/CsPbBr3,” J. Phys. Chem. Lett. 9(4), 830–836 (2018).
[Crossref]

Q. A. Akkerman, A. L. Abdelhady, and L. Manna, “Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges,” J. Phys. Chem. Lett. 9(9), 2326–2337 (2018).
[Crossref]

B. Turedi, K. J. Lee, I. Dursun, B. Alamer, Z. Wu, E. Alarousu, O. F. Mohammed, N. Cho, and O. M. Bakr, “Water-induced dimensionality reduction in metal-halide perovskites,” J. Phys. Chem. C 122(25), 14128–14134 (2018).
[Crossref]

Y. Li, H. Huang, Y. Xiong, S. V. Kershaw, and A. L. Rogach, “Reversible transformation between CsPbBr3 and Cs4PbBr6 nanocrystals,” CrystEngComm 20(34), 4900–4904 (2018).
[Crossref]

Z. Zhang, Y. Zhu, W. Wang, W. Zheng, R. Lin, X. Li, H. Zhang, D. Zhong, and F. Huang, “Aqueous Solution Growth of Millimeter-Sized Nongreen-Luminescent Wide Bandgap Cs4PbBr6 Bulk Crystal,” Cryst. Growth Des. 18(11), 6393–6398 (2018).
[Crossref]

D. Wang, W.-B. Shi, H. Jing, C. Yin, Y. Zhu, J. Su, G.-B. Ma, R. Peng, X. Wang, and M. Wang, “Photon-induced carrier recombination in the nonlayered-structured hybrid organicinorganic perovskite nano-sheets,” Opt. Express 26(21), 27504–27514 (2018).
[Crossref]

J. Yin, H. Yang, K. Song, A. M. El-Zohry, Y. Han, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Point Defects and Green Emission in Zero-Dimensional Perovskites,” J. Phys. Chem. Lett. 9(18), 5490–5495 (2018).
[Crossref]

2017 (13)

Y. Wang, D. Yu, Z. Wang, X. Li, X. Chen, V. Nalla, H. Zeng, and H. Sun, “Solution-Grown CsPbBr3/Cs4PbBr6 Perovskite Nanocomposites: Toward Temperature-Insensitive Optical Gain,” Small 13(34), 1701587 (2017).
[Crossref]

Q. A. Akkerman, S. Park, E. Radicchi, F. Nunzi, E. Mosconi, F. De Angelis, R. Brescia, P. Rastogi, M. Prato, and L. Manna, “Nearly Monodisperse Insulator Cs4PbX6 (X = Cl, Br, I) Nanocrystals, Their Mixed Halide Compositions, and Their Transformation into CsPbX3 Nanocrystals,” Nano Lett. 17(3), 1924–1930 (2017).
[Crossref]

M. De Bastiani, I. Dursun, Y. Zhang, B. A. Alshankiti, X.-H. Miao, J. Yin, E. Yengel, E. Alarousu, B. Turedi, J. M. Almutlaq, M. I. Saidaminov, S. Mitra, I. Gereige, A. AlSaggaf, Y. Zhu, Y. Han, I. S. Roqan, J.-L. Bredas, O. F. Mohammed, and O. M. Bakr, “Inside Perovskites: Quantum Luminescence from Bulk Cs4PbBr6 Single Crystals,” Chem. Mater. 29(17), 7108–7113 (2017).
[Crossref]

J. H. Cha, J. H. Han, W. Yin, C. Park, Y. Park, T. K. Ahn, J. H. Cho, and D. Y. Jung, “Photoresponse of CsPbBr3 and Cs4PbBr6 Perovskite Single Crystals,” J. Phys. Chem. Lett. 8(3), 565–570 (2017).
[Crossref]

X. Du, G. Wu, J. Cheng, H. Dang, K. Ma, Y. W. Zhang, P. F. Tan, and S. Chen, “High-quality CsPbBr3 perovskite nanocrystals for quantum dot light-emitting diodes,” RSC Adv. 7(17), 10391–10396 (2017).
[Crossref]

E. L. Unger, L. Kegelmann, K. Suchan, D. Sörell, L. Korte, and S. Albrecht, “Roadmap and roadblocks for the band gap tunability of metal halide perovskites,” J. Mater. Chem. A 5(23), 11401–11409 (2017).
[Crossref]

J. Yin, Y. Zhang, A. Bruno, C. Soci, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Intrinsic Lead Ion Emissions in Zero-Dimensional Cs4PbBr6 Nanocrystals,” ACS Energy Lett. 2(12), 2805–2811 (2017).
[Crossref]

Y. Zhang, M. I. Saidaminov, I. Dursun, H. Yang, B. Murali, E. Alarousu, E. Yengel, B. A. Alshankiti, O. M. Bakr, and O. F. Mohammed, “Zero-Dimensional Cs4PbBr6 Perovskite Nanocrystals,” J. Phys. Chem. Lett. 8(5), 961–965 (2017).
[Crossref]

J. Kang and L.-W. Wang, “High Defect Tolerance in Lead Halide Perovskite CsPbBr3,” J. Phys. Chem. Lett. 8(2), 489–493 (2017).
[Crossref]

S. Seth and A. Samanta, “Fluorescent Phase-Pure Zero-Dimensional Perovskite-Related Cs4PbBr6 Microdisks: Synthesis and Single-Particle Imaging Study,” J. Phys. Chem. Lett. 8(18), 4461–4467 (2017).
[Crossref]

S. Chen, X. Wen, S. Huang, F. Huang, Y.-B. Cheng, M. Green, and A. Ho-Baillie, “Light Illumination Induced Photoluminescence Enhancement and Quenching in Lead Halide Perovskite,” Sol. RRL 1(1), 1600001 (2017).
[Crossref]

Y. Fang, H. Wei, Q. Dong, and J. Huang, “Quantification of re-absorption and re-emission processes to determine photon recycling efficiency in perovskite single crystals,” Nat. Commun. 8(1), 14417 (2017).
[Crossref]

L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
[Crossref]

2016 (5)

L. N. Quan, M. Yuan, R. Comin, O. Voznyy, E. M. Beauregard, S. Hoogland, A. Buin, A. R. Kirmani, K. Zhao, A. Amassian, D. H. Kim, and E. H. Sargent, “Ligand-Stabilized Reduced-Dimensionality Perovskites,” J. Am. Chem. Soc. 138(8), 2649–2655 (2016).
[Crossref]

W. Zhou, Y. Zhao, C. Shi, H. Huang, J. Wei, R. Fu, K. Liu, D. Yu, and Q. Zhao, “Reversible Healing Effect of Water Molecules on Fully Crystallized Metal–Halide Perovskite Film,” J. Mater. Chem. C 120(9), 4759–4765 (2016).
[Crossref]

D. Chen, Z. Wan, X. Chen, Y. Yuan, and J. Zhong, “Large-scale room-temperature synthesis and optical properties of perovskite-related Cs4PbBr6 fluorophores,” J. Mater. Chem. C 4(45), 10646–10653 (2016).
[Crossref]

S. Seth, N. Mondal, S. Patra, and A. Samanta, “Fluorescence Blinking and Photoactivation of All-Inorganic Perovskite Nanocrystals CsPbBr3 and CsPbBr2I,” J. Phys. Chem. Lett. 7(2), 266–271 (2016).
[Crossref]

J. M. Ball and A. Petrozza, “Defects in perovskite-halides and their effects in solar cells,” Nat. Energy 1(11), 16149 (2016).
[Crossref]

2015 (1)

X. Gong, M. Li, X.-B. Shi, H. Ma, Z.-K. Wang, and L.-S. Liao, “Controllable Perovskite Crystallization by Water Additive for High-Performance Solar Cells,” Adv. Funct. Mater. 25(42), 6671–6678 (2015).
[Crossref]

2005 (1)

S. J. Clark, M. D. Segall, C. J. Pickard, P. J. Hasnip, M. I. Probert, K. Refson, and M. C. Payne, “First principles methods using CASTEP,” Z. Kristallogr. - Cryst. Mater. 220(5/6), 567–570 (2005).
[Crossref]

1996 (1)

J. P. Perdew, K. Burke, and K. M. Ernzerhof, “Generalized Gradient Approximation Made Simple,” Phys. Rev. Lett. 77(18), 3865–3868 (1996).
[Crossref]

1990 (1)

D. Vanderbilt, “Soft self-consistent pseudopotentials in a generalized eigenvalue formalism,” Phys. Rev. B 41(11), 7892–7895 (1990).
[Crossref]

1976 (1)

H. J. Monkhorst and J. D. Pack, “Special points for Brillouin-zone integrations,” Phys. Rev. B 13(12), 5188–5192 (1976).
[Crossref]

Abdelhady, A. L.

Q. A. Akkerman, A. L. Abdelhady, and L. Manna, “Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges,” J. Phys. Chem. Lett. 9(9), 2326–2337 (2018).
[Crossref]

Abdi-Jalebi, M.

M. Abdi-Jalebi, M. Ibrahim Dar, S. P. Senanayak, A. Sadhanala, Z. Andaji-Garmaroudi, L. M. Pazos-Outón, J. M. Richter, A. J. Pearson, H. Sirringhaus, M. Grätzel, and R. H. Friend, “Charge extraction via graded doping of hole transport layers gives highly luminescent and stable metal halide perovskite devices,” Sci. Adv. 5(2), eaav2012 (2019).
[Crossref]

Ahn, T. K.

J. H. Cha, J. H. Han, W. Yin, C. Park, Y. Park, T. K. Ahn, J. H. Cho, and D. Y. Jung, “Photoresponse of CsPbBr3 and Cs4PbBr6 Perovskite Single Crystals,” J. Phys. Chem. Lett. 8(3), 565–570 (2017).
[Crossref]

Akkerman, Q. A.

Q. A. Akkerman, A. L. Abdelhady, and L. Manna, “Zero-Dimensional Cesium Lead Halides: History, Properties, and Challenges,” J. Phys. Chem. Lett. 9(9), 2326–2337 (2018).
[Crossref]

Q. A. Akkerman, S. Park, E. Radicchi, F. Nunzi, E. Mosconi, F. De Angelis, R. Brescia, P. Rastogi, M. Prato, and L. Manna, “Nearly Monodisperse Insulator Cs4PbX6 (X = Cl, Br, I) Nanocrystals, Their Mixed Halide Compositions, and Their Transformation into CsPbX3 Nanocrystals,” Nano Lett. 17(3), 1924–1930 (2017).
[Crossref]

Alamer, B.

B. Turedi, K. J. Lee, I. Dursun, B. Alamer, Z. Wu, E. Alarousu, O. F. Mohammed, N. Cho, and O. M. Bakr, “Water-induced dimensionality reduction in metal-halide perovskites,” J. Phys. Chem. C 122(25), 14128–14134 (2018).
[Crossref]

Alarousu, E.

B. Turedi, K. J. Lee, I. Dursun, B. Alamer, Z. Wu, E. Alarousu, O. F. Mohammed, N. Cho, and O. M. Bakr, “Water-induced dimensionality reduction in metal-halide perovskites,” J. Phys. Chem. C 122(25), 14128–14134 (2018).
[Crossref]

M. De Bastiani, I. Dursun, Y. Zhang, B. A. Alshankiti, X.-H. Miao, J. Yin, E. Yengel, E. Alarousu, B. Turedi, J. M. Almutlaq, M. I. Saidaminov, S. Mitra, I. Gereige, A. AlSaggaf, Y. Zhu, Y. Han, I. S. Roqan, J.-L. Bredas, O. F. Mohammed, and O. M. Bakr, “Inside Perovskites: Quantum Luminescence from Bulk Cs4PbBr6 Single Crystals,” Chem. Mater. 29(17), 7108–7113 (2017).
[Crossref]

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L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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B. Turedi, K. J. Lee, I. Dursun, B. Alamer, Z. Wu, E. Alarousu, O. F. Mohammed, N. Cho, and O. M. Bakr, “Water-induced dimensionality reduction in metal-halide perovskites,” J. Phys. Chem. C 122(25), 14128–14134 (2018).
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L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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J. Yin, H. Yang, K. Song, A. M. El-Zohry, Y. Han, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Point Defects and Green Emission in Zero-Dimensional Perovskites,” J. Phys. Chem. Lett. 9(18), 5490–5495 (2018).
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M. Wei, F. P. G. de Arquer, G. Walters, Z. Yang, L. N. Quan, Y. Kim, R. Sabatini, R. Quintero-Bermudez, L. Gao, J. Z. Fan, F. Fan, A. Gold-Parker, M. F. Toney, and E. H. Sargent, “Ultrafast narrowband exciton routing within layered perovskite nanoplatelets enables low-loss luminescent solar concentrators,” Nat. Energy 4(3), 197–205 (2019).
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Y. Zhang, M. I. Saidaminov, I. Dursun, H. Yang, B. Murali, E. Alarousu, E. Yengel, B. A. Alshankiti, O. M. Bakr, and O. F. Mohammed, “Zero-Dimensional Cs4PbBr6 Perovskite Nanocrystals,” J. Phys. Chem. Lett. 8(5), 961–965 (2017).
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Yin, J.

J. Yin, H. Yang, K. Song, A. M. El-Zohry, Y. Han, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Point Defects and Green Emission in Zero-Dimensional Perovskites,” J. Phys. Chem. Lett. 9(18), 5490–5495 (2018).
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Q. Luo, H. Wang, X. Yin, and L. Wang, “Hydrophilic perovskite microdisks with excellent stability and strong fluorescence for recyclable temperature sensing,” Sci. China Mater. 62(7), 1065–1070 (2019).
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Yin, Y.

L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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Y. Wang, D. Yu, Z. Wang, X. Li, X. Chen, V. Nalla, H. Zeng, and H. Sun, “Solution-Grown CsPbBr3/Cs4PbBr6 Perovskite Nanocomposites: Toward Temperature-Insensitive Optical Gain,” Small 13(34), 1701587 (2017).
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W. Zhou, Y. Zhao, C. Shi, H. Huang, J. Wei, R. Fu, K. Liu, D. Yu, and Q. Zhao, “Reversible Healing Effect of Water Molecules on Fully Crystallized Metal–Halide Perovskite Film,” J. Mater. Chem. C 120(9), 4759–4765 (2016).
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L. N. Quan, M. Yuan, R. Comin, O. Voznyy, E. M. Beauregard, S. Hoogland, A. Buin, A. R. Kirmani, K. Zhao, A. Amassian, D. H. Kim, and E. H. Sargent, “Ligand-Stabilized Reduced-Dimensionality Perovskites,” J. Am. Chem. Soc. 138(8), 2649–2655 (2016).
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D. Chen, Z. Wan, X. Chen, Y. Yuan, and J. Zhong, “Large-scale room-temperature synthesis and optical properties of perovskite-related Cs4PbBr6 fluorophores,” J. Mater. Chem. C 4(45), 10646–10653 (2016).
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Y. Wang, D. Yu, Z. Wang, X. Li, X. Chen, V. Nalla, H. Zeng, and H. Sun, “Solution-Grown CsPbBr3/Cs4PbBr6 Perovskite Nanocomposites: Toward Temperature-Insensitive Optical Gain,” Small 13(34), 1701587 (2017).
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Z. Zhang, Y. Zhu, W. Wang, W. Zheng, R. Lin, X. Li, H. Zhang, D. Zhong, and F. Huang, “Aqueous Solution Growth of Millimeter-Sized Nongreen-Luminescent Wide Bandgap Cs4PbBr6 Bulk Crystal,” Cryst. Growth Des. 18(11), 6393–6398 (2018).
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Zhang, J. Z.

L. Rao, X. Ding, X. Du, G. Liang, Y. Tang, K. Tang, and J. Z. Zhang, “Ultrasonication-assisted synthesis of CsPbBr3 and Cs4PbBr6 perovskite nanocrystals and their reversible transformation,” Beilstein J. Nanotechnol. 10(1), 666–676 (2019).
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L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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Zhang, Y.

M. De Bastiani, I. Dursun, Y. Zhang, B. A. Alshankiti, X.-H. Miao, J. Yin, E. Yengel, E. Alarousu, B. Turedi, J. M. Almutlaq, M. I. Saidaminov, S. Mitra, I. Gereige, A. AlSaggaf, Y. Zhu, Y. Han, I. S. Roqan, J.-L. Bredas, O. F. Mohammed, and O. M. Bakr, “Inside Perovskites: Quantum Luminescence from Bulk Cs4PbBr6 Single Crystals,” Chem. Mater. 29(17), 7108–7113 (2017).
[Crossref]

J. Yin, Y. Zhang, A. Bruno, C. Soci, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Intrinsic Lead Ion Emissions in Zero-Dimensional Cs4PbBr6 Nanocrystals,” ACS Energy Lett. 2(12), 2805–2811 (2017).
[Crossref]

Y. Zhang, M. I. Saidaminov, I. Dursun, H. Yang, B. Murali, E. Alarousu, E. Yengel, B. A. Alshankiti, O. M. Bakr, and O. F. Mohammed, “Zero-Dimensional Cs4PbBr6 Perovskite Nanocrystals,” J. Phys. Chem. Lett. 8(5), 961–965 (2017).
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Zhang, Y. W.

X. Du, G. Wu, J. Cheng, H. Dang, K. Ma, Y. W. Zhang, P. F. Tan, and S. Chen, “High-quality CsPbBr3 perovskite nanocrystals for quantum dot light-emitting diodes,” RSC Adv. 7(17), 10391–10396 (2017).
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Z. Zhang, Y. Zhu, W. Wang, W. Zheng, R. Lin, X. Li, H. Zhang, D. Zhong, and F. Huang, “Aqueous Solution Growth of Millimeter-Sized Nongreen-Luminescent Wide Bandgap Cs4PbBr6 Bulk Crystal,” Cryst. Growth Des. 18(11), 6393–6398 (2018).
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L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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D. Chen, Z. Wan, X. Chen, Y. Yuan, and J. Zhong, “Large-scale room-temperature synthesis and optical properties of perovskite-related Cs4PbBr6 fluorophores,” J. Mater. Chem. C 4(45), 10646–10653 (2016).
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L. Wu, H. Hu, Y. Xu, S. Jiang, M. Chen, Q. Zhong, D. Yang, Q. Liu, Y. Zhao, B. Sun, Q. Zhang, and Y. Yin, “From Nonluminescent Cs4PbX6 (X = Cl, Br, I) Nanocrystals to Highly Luminescent CsPbX3 Nanocrystals: Water-Triggered Transformation through a CsX-Stripping Mechanism,” Nano Lett. 17(9), 5799–5804 (2017).
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J. Yin, Y. Zhang, A. Bruno, C. Soci, O. M. Bakr, J.-L. Brédas, and O. F. Mohammed, “Intrinsic Lead Ion Emissions in Zero-Dimensional Cs4PbBr6 Nanocrystals,” ACS Energy Lett. 2(12), 2805–2811 (2017).
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Z. Zhang, Y. Zhu, W. Wang, W. Zheng, R. Lin, X. Li, H. Zhang, D. Zhong, and F. Huang, “Aqueous Solution Growth of Millimeter-Sized Nongreen-Luminescent Wide Bandgap Cs4PbBr6 Bulk Crystal,” Cryst. Growth Des. 18(11), 6393–6398 (2018).
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D. Chen, Z. Wan, X. Chen, Y. Yuan, and J. Zhong, “Large-scale room-temperature synthesis and optical properties of perovskite-related Cs4PbBr6 fluorophores,” J. Mater. Chem. C 4(45), 10646–10653 (2016).
[Crossref]

W. Zhou, Y. Zhao, C. Shi, H. Huang, J. Wei, R. Fu, K. Liu, D. Yu, and Q. Zhao, “Reversible Healing Effect of Water Molecules on Fully Crystallized Metal–Halide Perovskite Film,” J. Mater. Chem. C 120(9), 4759–4765 (2016).
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Figures (5)

Fig. 1.
Fig. 1. Scheme Illustration of the preparation process.
Fig. 2.
Fig. 2. (a) The calculated XRD patterns of Cs4PbBr6 and the experimental XRD patterns. (b) SEM and (c) element mapping images of the as-obtained Cs4PbBr6 with a mean size of 30 µm and a thickness less than 3.4 µm, (the inset in the upper right corner of Fig. 1(b) exhibits the morphology of a single particle and the histogram of the inset describes the size and thickness distribution of the as-obtained Cs4PbBr6 particles). (d) PL and absorption spectra of Cs4PbBr6 particles (the inset of Fig. 2(d) shows the bright green emission from a single particle).
Fig. 3.
Fig. 3. (a) FT-IR spectra of the Cs4PbBr6 micro-particles obtained via the hot-injection and the polar solution-based synthesis method, respectively. (b) XPS spectrum of Pb 4f in Cs4PbBr6 micro-particles synthesized via the polar solution-based synthesis method, and the XPS spectrum were calibrated using C1s peak at 284.8 eV. Band structure and density of state of (c) Cs4PbBr6; (d) Cs4PbBr6+VBr; (e) Cs4PbBr6+OH; and (f) Cs4PbBr6+VBr +OH, respectively.
Fig. 4.
Fig. 4. (a) PL spectra and (b) the corresponding PL mapping versus pumping density at room temperature under 800 nm laser, and the inset in Fig. 4(a) is the photograph of an individual hexagonal particle under 800 nm femtosecond laser pumping from the edge of the particle. (c) Schematic description of the Cs4PbBr6 micro-particle under 800 nm femtosecond laser excitation. (d) The dependence of the PL intensity and FWHM as a function of pumping density under 800 nm femtosecond laser excitation.
Fig. 5.
Fig. 5. (a) Lasing spectra and (b) the corresponding lasing spectra mapping from a single Cs4PbBr6 micro-particle around the lasing threshold, and the inset in Fig. 5(a) is the photograph of an individual hexagonal particle under 800 nm femtosecond laser pumping focused on the center region of the particle. (c) Schematic description of the Cs4PbBr6 micro-particle under 800 nm femtosecond laser excitation focused on the center region of the particle. (d) The dependence of the output intensity and linewidth as a function of pumping density under 800 nm femtosecond laser excitation, showing the threshold of around 153 µJ cm−2.

Equations (1)

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Δ λ = λ 2 / ( 2 n g L )

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