Abstract

The hybrid organic-inorganic perovskites (HOIPs) have attracted much attention recently due to their preeminent efficiency in solar cells. According to the difference on the crystalline structure, the HOIPs could be classified into layered and non-layered perovskites. Very recently, it has been realized that the non-layered HOIPs with common-vertex structure possess even better opto-electrical performance. Yet the carrier recombination mechanism in perovskite remains not very clear, and a clear understanding of this mechanism is essential to pinpoint the working mechanism of photovoltaic and electroluminescent materials. Here we report the optical studies on the hybrid perovskite crystalline nano-sheet of CH3NH3PbBr3 with common-vertex structure. It is shown that the non-layered perovskite crystalline nanosheets possess the exciton binding energy about two orders of magnitude smaller than that of the layered perovskite and the colloidal nanoplates, which is beneficial for the designing of the high-efficiency photovoltaic devices. By measuring the temperature-dependent photoluminescence (PL) spectra, the excitation-power-variant PL spectra, and the time-resolved PL spectra, we identify that both the free-carrier and the localized exciton recombination channels may coexist in the crystallites. Further, for the thin crystallite (∼60 nm), the free-carrier recombination channel dominates; whereas when the thickness increases beyond 200 nm, the localized exciton recombination channel plays the major role. We suggest these results are helpful to improve further the photovoltaic and electroluminescent performances of perovskite devices.

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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2018 (6)

B. Du, W. Yang, Q. Jiang, H. Shan, D. Luo, B. Li, W. Tang, F. Lin, B. Shen, Q. Gong, X. Zhu, R. Zhu, and Z. Fang, “Plasmonic-Functionalized Broadband Perovskite Photodetector,” Adv. Opt. Mater. 6(8), 1701271 (2018).
[Crossref]

Z. Yang, Y. Deng, X. Zhang, S. Wang, H. Chen, S. Yang, J. Khurgin, N. X. Fang, X. Zhang, and R. Ma, “High-Performance Single-Crystalline Perovskite Thin-Film Photodetector,” Adv. Mater. 30(8), 1704333 (2018).
[Crossref] [PubMed]

J. Xing, Y. Zhao, M. Askerka, L. N. Quan, X. Gong, W. Zhao, J. Zhao, H. Tan, G. Long, L. Gao, Z. Yang, O. Voznyy, J. Tang, Z. H. Lu, Q. Xiong, and E. H. Sargent, “Color-stable highly luminescent sky-blue perovskite light-emitting diodes,” Nat. Commun. 9(1), 3541 (2018).
[Crossref] [PubMed]

F. Sahli, J. Werner, B. A. Kamino, M. Bräuninger, R. Monnard, B. Paviet-Salomon, L. Barraud, L. Ding, J. J. Diaz Leon, D. Sacchetto, G. Cattaneo, M. Despeisse, M. Boccard, S. Nicolay, Q. Jeangros, B. Niesen, and C. Ballif, “Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency,” Nat. Mater. 17(9), 820–826 (2018).
[Crossref]

G. Jia, Z. J. Shi, Y. D. Xia, Q. Wei, Y. H. Chen, G. C. Xing, and W. Huang, “Super air stable quasi-2D organic-inorganic hybrid perovskites for visible light-emitting diodes,” Opt. Express 26(2), A66–A74 (2018).
[Crossref] [PubMed]

Y. Song, C. Zhang, W. Liu, X. Li, H. Long, K. Wang, B. Wang, and P. Lu, “High-efficiency energy transfer in perovskite heterostructures,” Opt. Express 26(14), 18448–18456 (2018).
[Crossref] [PubMed]

2017 (5)

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, 14417 (2017).
[Crossref] [PubMed]

D. Niesner, O. Schuster, M. Wilhelm, I. Levchuk, A. Osvet, S. Shrestha, M. Batentschuk, C. Brabec, and T. Fauster, “Temperature-dependent optical spectra of single-crystal (CH3NH3)PbBr3 cleaved in ultrahigh vacuum,” Phys. Rev. B 95(7), 075207 (2017).
[Crossref]

T. T. H. Do, A. G. Aguila, C. Cui, J. Xing, Z. Ning, and Q. Xiong, “Optical study on intrinsic exciton states in high-quality CH3NH3PbBr3 single crystals,” Phys. Rev. B 96(7), 075308 (2017).
[Crossref]

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
[Crossref] [PubMed]

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
[Crossref] [PubMed]

2016 (15)

J. M. Richter, M. Abdi-Jalebi, A. Sadhanala, M. Tabachnyk, J. P. H. Rivett, L. M. Pazos-Outón, K. C. Gödel, M. Price, F. Deschler, and R. H. Friend, “Enhancing photoluminescence yields in lead halide perovskites by photon recycling and light out-coupling,” Nat. Commun. 7, 13941 (2016).
[Crossref] [PubMed]

X. Wen, Y. Feng, S. Huang, F. Huang, Y. B. Cheng, M. Green, and A. H. Baillie, “Defect trapping states and charge carrier recombination in organic–inorganic halide perovskites,” J. Mater. Chem. C Mater. Opt. Electron. Devices 4(4), 793–800 (2016).
[Crossref]

T. Ye, X. Jiang, D. Wan, X. Wang, J. Xing, T. Venkatesan, Q. Xiong, and S. Ramakrishna, “Ultrafast Photogenerated Hole Extraction/Transport Behavior in a CH3 NH3 PbI3 /Carbon Nanocomposite and Its Application in a Metal-Electrode-Free Solar Cell,” ChemPhysChem 17(24), 4102–4109 (2016).
[Crossref] [PubMed]

S. Ke, C. Chen, N. Fu, H. Zhou, M. Ye, P. Lin, W. Yuan, X. Zeng, L. Chen, and H. Huang, “Transparent Indium Tin Oxide Electrodes on Muscovite Mica for High-Temperature-Processed Flexible Optoelectronic Devices,” ACS Appl. Mater. Interfaces 8(42), 28406–28411 (2016).
[Crossref] [PubMed]

M. Saba, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

H. He, Q. Yu, H. Li, J. Li, J. Si, Y. Jin, N. Wang, J. Wang, J. He, X. Wang, Y. Zhang, and Z. Ye, “Exciton localization in solution-processed organolead trihalide perovskites,” Nat. Commun. 7, 10896 (2016).
[Crossref] [PubMed]

S. Colella, M. Mazzeo, A. Rizzo, G. Gigli, and A. Listorti, “The Bright Side of Perovskites,” J. Phys. Chem. Lett. 7(21), 4322–4334 (2016).
[Crossref] [PubMed]

S. A. Veldhuis, P. P. Boix, N. Yantara, M. Li, T. C. Sum, N. Mathews, and S. G. Mhaisalkar, “Perovskite Materials for Light-Emitting Diodes and Lasers,” Adv. Mater. 28(32), 6804–6834 (2016).
[Crossref] [PubMed]

A. R. Srimath Kandada and A. Petrozza, “Photophysics of Hybrid Lead Halide Perovskites: The Role of Microstructure,” Acc. Chem. Res. 49(3), 536–544 (2016).
[Crossref] [PubMed]

M. Saba, F. Quochi, A. Mura, G. Bongiovanni, V. Sarritzu, N. Sestu, C. Figus, M. Aresti, R. Piras, A. Geddo Lehmann, C. Cannas, A. Musinu, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

W. Zhang, G. E. Eperon, and H. J. Snaith, “Metal halide perovskites for energy applications,” Nat. Energy 1(6), 16048 (2016).
[Crossref]

A. Polman, M. Knight, E. C. Garnett, B. Ehrler, and W. C. Sinke, “Photovoltaic materials: Present efficiencies and future challenges,” Science 352(6283), aad4424 (2016).
[Crossref] [PubMed]

Z. Guo, X. Wu, T. Zhu, X. Zhu, L. Huang, Z. Guo, X. Wu, T. Zhu, X. Zhu, and L. Huang, “Electron-Phonon Scattering in Atomically Thin 2D Perovskites,” ACS Nano 10(11), 9992–9998 (2016).
[Crossref] [PubMed]

S. Kumar, J. Jagielski, S. Yakunin, P. Rice, Y. C. Chiu, M. Wang, G. Nedelcu, Y. Kim, S. Lin, E. J. Santos, M. V. Kovalenko, and C. J. Shih, “Efficient Blue Electroluminescence Using Quantum-Confined Two-Dimensional Perovskites,” ACS Nano 10(10), 9720–9729 (2016).
[Crossref] [PubMed]

M. S. Alias, I. Dursun, M. I. Saidaminov, E. M. Diallo, P. Mishra, T. K. Ng, O. M. Bakr, and B. S. Ooi, “Optical constants ofCH3NH3PbBr3 perovskite thin films measured by spectroscopic ellipsometry,” Opt. Express 24(15), 16586–16594 (2016).
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2015 (6)

O. Yaffe, A. Chernikov, Z. M. Norman, Y. Zhong, A. Velauthapillai, A. van der Zande, J. S. Owen, and T. F. Heinz, “Excitons in ultrathin organic-inorganic perovskite crystals,” Phys. Rev. B Condens. Matter Mater. Phys. 92(4), 045414 (2015).
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H. S. Duan, H. Zhou, Q. Chen, P. Sun, S. Luo, T.-B. Song, B. Bob, and Y. Yang, “The identification and characterization of defect states in hybrid organic-inorganic perovskite photovoltaics,” Phys. Chem. Chem. Phys. 17(1), 112–116 (2015).
[Crossref] [PubMed]

D. Shi, V. Adinolfi, R. Comin, M. Yuan, E. Alarousu, A. Buin, Y. Chen, S. Hoogland, A. Rothenberger, K. Katsiev, Y. Losovyj, X. Zhang, P. A. Dowben, O. F. Mohammed, E. H. Sargent, and O. M. Bakr, “Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
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D. W. deQuilettes, S. M. Vorpahl, S. D. Stranks, H. Nagaoka, G. E. Eperon, M. E. Ziffer, H. J. Snaith, and D. S. Ginger, “Impact of microstructure on local carrier lifetime in perovskite solar cells,” Science 348(6235), 683–686 (2015).
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M. I. Saidaminov, A. L. Abdelhady, B. Murali, E. Alarousu, V. M. Burlakov, W. Peng, I. Dursun, L. Wang, Y. He, G. Maculan, A. Goriely, T. Wu, O. F. Mohammed, and O. M. Bakr, “High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization,” Nat. Commun. 6(1), 7586 (2015).
[Crossref] [PubMed]

L. Dou, A. B. Wong, Y. Yu, M. Lai, N. Kornienko, S. W. Eaton, A. Fu, C. G. Bischak, J. Ma, T. Ding, N. S. Ginsberg, L. W. Wang, A. P. Alivisatos, and P. Yang, “Atomically thin two-dimensional organic-inorganic hybrid perovskites,” Science 349(6255), 1518–1521 (2015).
[Crossref] [PubMed]

2014 (4)

T. J. Savenije, C. S. Ponseca, L. Kunneman, M. Abdellah, K. Zheng, Y. Tian, Q. Zhu, S. E. Canton, I. G. Scheblykin, T. Pullerits, A. Yartsev, and V. Sundström, “Thermally activated exciton dissociation and recombination control the carrier dynamics in organometal halide perovskite,” J. Phys. Chem. Lett. 5(13), 2189–2194 (2014).
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G. Xing, N. Mathews, S. S. Lim, N. Yantara, X. Liu, D. Sabba, M. Grätzel, S. Mhaisalkar, and T. C. Sum, “Low-temperature solution-processed wavelength-tunable perovskites for lasing,” Nat. Mater. 13(5), 476–480 (2014).
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W. J. Yin, T. Shi, and Y. Yan, “Unusual defect physics in CH3NH3PbI3 perovskite solar cell absorber,” Appl. Phys. Lett. 104(6), 063903 (2014).
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V. D’Innocenzo, G. Grancini, M. J. P. Alcocer, A. R. S. Kandada, S. D. Stranks, M. M. Lee, G. Lanzani, H. J. Snaith, and A. Petrozza, “Excitons versus free charges in organo-lead tri-halide perovskites,” Nat. Commun. 5(1), 3586 (2014).
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2013 (1)

S. Tongay, J. Suh, C. Ataca, W. Fan, A. Luce, J. S. Kang, J. Liu, C. Ko, R. Raghunathanan, J. Zhou, F. Ogletree, J. Li, J. C. Grossman, and J. Wu, “Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons,” Sci. Rep. 3(1), 2657 (2013).
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2012 (1)

F. Luckert, M. V. Yakushev, C. Faugeras, A. V. Karotki, A. V. Mudryi, and R. W. Martin, “Excitation power and temperature dependence of excitons in CuInSe2,” J. Appl. Phys. 111(9), 093507 (2012).
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2009 (1)

A. Kojima, K. Teshima, Y. Shirai, and T. Miyasaka, “Organometal halide perovskites as visible-light sensitizers for photovoltaic cells,” J. Am. Chem. Soc. 131(17), 6050–6051 (2009).
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2005 (1)

T. Onuma, A. Chakraborty, B. A. Haskell, S. Keller, S. P. DenBaars, J. S. Speck, S. Nakamura, U. K. Mishra, T. Sota, and S. F. Chichibu, “Localized exciton dynamics in nonpolar (11-20) InxGa1-xN multiple quantum wells grown on GaN templates prepared by lateral epitaxial overgrowth,” Appl. Phys. Lett. 86(15), 151918 (2005).
[Crossref]

2003 (1)

Y. Sun, O. Brandt, S. Cronenberg, S. Dhar, H. T. Grahn, K. H. Ploog, P. Waltereit, and J. S. Speck, “Nonpolar InxGa1-xN/GaN (1-100) multiple quantum wells grown on γ-LiAlO2 (100) by plasma-assisted molecular-beam epitaxy,” Phys. Rev. B Condens. Matter Mater. Phys. 67(4), 041306 (2003).
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1999 (1)

M. Leroux, N. Grandjean, B. Beaumont, G. Nataf, F. Semond, J. Massies, and P. Gibart, “Temperature quenching of photoluminescence intensities in undoped and doped GaN,” J. Appl. Phys. 86(7), 3721–3728 (1999).
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1997 (1)

J. Enderlein and R. Erdmann, “Fast fitting of multi-exponential decay curves,” Opt. Commun. 134(1-6), 371–378 (1997).
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1996 (1)

H. W. Yoon, D. R. Wake, and J. P. Wolfe, “Effect of exciton-carrier thermodynamics on the GaAs quantum well photoluminescence,” Phys. Rev. B Condens. Matter 54(4), 2763–2774 (1996).
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1992 (1)

T. Schmidt, K. Lischka, and W. Zulehner, “Excitation-power dependence of the near-band-edge photoluminescence of semiconductors,” Phys. Rev. B Condens. Matter 45(16), 8989–8994 (1992).
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1987 (2)

F. A. Majumder, S. Shevel, V. G. Lyssenko, H. E. Swoboda, and C. Klingshirn, “Luminescence and gain spectroscopy of disordered CdS1−xSe x under high excitation,” Z. Phys. B Con. Mat. 66, 409–418 (1987).

A. Poglitsch and D. Weber, “Dynamic disorder in methylammoniumtrihalogenoplumbates (II) observed by millimeter‐wave spectroscopy,” J. Chem. Phys. 87(11), 6373–6378 (1987).
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Abdelhady, A. L.

M. I. Saidaminov, A. L. Abdelhady, B. Murali, E. Alarousu, V. M. Burlakov, W. Peng, I. Dursun, L. Wang, Y. He, G. Maculan, A. Goriely, T. Wu, O. F. Mohammed, and O. M. Bakr, “High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization,” Nat. Commun. 6(1), 7586 (2015).
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Abdellah, M.

T. J. Savenije, C. S. Ponseca, L. Kunneman, M. Abdellah, K. Zheng, Y. Tian, Q. Zhu, S. E. Canton, I. G. Scheblykin, T. Pullerits, A. Yartsev, and V. Sundström, “Thermally activated exciton dissociation and recombination control the carrier dynamics in organometal halide perovskite,” J. Phys. Chem. Lett. 5(13), 2189–2194 (2014).
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Abdi-Jalebi, M.

J. M. Richter, M. Abdi-Jalebi, A. Sadhanala, M. Tabachnyk, J. P. H. Rivett, L. M. Pazos-Outón, K. C. Gödel, M. Price, F. Deschler, and R. H. Friend, “Enhancing photoluminescence yields in lead halide perovskites by photon recycling and light out-coupling,” Nat. Commun. 7, 13941 (2016).
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Adinolfi, V.

D. Shi, V. Adinolfi, R. Comin, M. Yuan, E. Alarousu, A. Buin, Y. Chen, S. Hoogland, A. Rothenberger, K. Katsiev, Y. Losovyj, X. Zhang, P. A. Dowben, O. F. Mohammed, E. H. Sargent, and O. M. Bakr, “Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
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Aguila, A. G.

T. T. H. Do, A. G. Aguila, C. Cui, J. Xing, Z. Ning, and Q. Xiong, “Optical study on intrinsic exciton states in high-quality CH3NH3PbBr3 single crystals,” Phys. Rev. B 96(7), 075308 (2017).
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Ajayan, P. M.

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
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J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
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Alarousu, E.

M. I. Saidaminov, A. L. Abdelhady, B. Murali, E. Alarousu, V. M. Burlakov, W. Peng, I. Dursun, L. Wang, Y. He, G. Maculan, A. Goriely, T. Wu, O. F. Mohammed, and O. M. Bakr, “High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization,” Nat. Commun. 6(1), 7586 (2015).
[Crossref] [PubMed]

D. Shi, V. Adinolfi, R. Comin, M. Yuan, E. Alarousu, A. Buin, Y. Chen, S. Hoogland, A. Rothenberger, K. Katsiev, Y. Losovyj, X. Zhang, P. A. Dowben, O. F. Mohammed, E. H. Sargent, and O. M. Bakr, “Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
[Crossref] [PubMed]

Alcocer, M. J. P.

V. D’Innocenzo, G. Grancini, M. J. P. Alcocer, A. R. S. Kandada, S. D. Stranks, M. M. Lee, G. Lanzani, H. J. Snaith, and A. Petrozza, “Excitons versus free charges in organo-lead tri-halide perovskites,” Nat. Commun. 5(1), 3586 (2014).
[Crossref] [PubMed]

Alias, M. S.

Alivisatos, A. P.

L. Dou, A. B. Wong, Y. Yu, M. Lai, N. Kornienko, S. W. Eaton, A. Fu, C. G. Bischak, J. Ma, T. Ding, N. S. Ginsberg, L. W. Wang, A. P. Alivisatos, and P. Yang, “Atomically thin two-dimensional organic-inorganic hybrid perovskites,” Science 349(6255), 1518–1521 (2015).
[Crossref] [PubMed]

Appavoo, K.

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
[Crossref] [PubMed]

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
[Crossref] [PubMed]

Aresti, M.

M. Saba, F. Quochi, A. Mura, G. Bongiovanni, V. Sarritzu, N. Sestu, C. Figus, M. Aresti, R. Piras, A. Geddo Lehmann, C. Cannas, A. Musinu, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

Askerka, M.

J. Xing, Y. Zhao, M. Askerka, L. N. Quan, X. Gong, W. Zhao, J. Zhao, H. Tan, G. Long, L. Gao, Z. Yang, O. Voznyy, J. Tang, Z. H. Lu, Q. Xiong, and E. H. Sargent, “Color-stable highly luminescent sky-blue perovskite light-emitting diodes,” Nat. Commun. 9(1), 3541 (2018).
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Ataca, C.

S. Tongay, J. Suh, C. Ataca, W. Fan, A. Luce, J. S. Kang, J. Liu, C. Ko, R. Raghunathanan, J. Zhou, F. Ogletree, J. Li, J. C. Grossman, and J. Wu, “Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons,” Sci. Rep. 3(1), 2657 (2013).
[Crossref] [PubMed]

Baillie, A. H.

X. Wen, Y. Feng, S. Huang, F. Huang, Y. B. Cheng, M. Green, and A. H. Baillie, “Defect trapping states and charge carrier recombination in organic–inorganic halide perovskites,” J. Mater. Chem. C Mater. Opt. Electron. Devices 4(4), 793–800 (2016).
[Crossref]

Bakr, O. M.

M. S. Alias, I. Dursun, M. I. Saidaminov, E. M. Diallo, P. Mishra, T. K. Ng, O. M. Bakr, and B. S. Ooi, “Optical constants ofCH3NH3PbBr3 perovskite thin films measured by spectroscopic ellipsometry,” Opt. Express 24(15), 16586–16594 (2016).
[Crossref] [PubMed]

M. I. Saidaminov, A. L. Abdelhady, B. Murali, E. Alarousu, V. M. Burlakov, W. Peng, I. Dursun, L. Wang, Y. He, G. Maculan, A. Goriely, T. Wu, O. F. Mohammed, and O. M. Bakr, “High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization,” Nat. Commun. 6(1), 7586 (2015).
[Crossref] [PubMed]

D. Shi, V. Adinolfi, R. Comin, M. Yuan, E. Alarousu, A. Buin, Y. Chen, S. Hoogland, A. Rothenberger, K. Katsiev, Y. Losovyj, X. Zhang, P. A. Dowben, O. F. Mohammed, E. H. Sargent, and O. M. Bakr, “Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
[Crossref] [PubMed]

Ballif, C.

F. Sahli, J. Werner, B. A. Kamino, M. Bräuninger, R. Monnard, B. Paviet-Salomon, L. Barraud, L. Ding, J. J. Diaz Leon, D. Sacchetto, G. Cattaneo, M. Despeisse, M. Boccard, S. Nicolay, Q. Jeangros, B. Niesen, and C. Ballif, “Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency,” Nat. Mater. 17(9), 820–826 (2018).
[Crossref]

Barraud, L.

F. Sahli, J. Werner, B. A. Kamino, M. Bräuninger, R. Monnard, B. Paviet-Salomon, L. Barraud, L. Ding, J. J. Diaz Leon, D. Sacchetto, G. Cattaneo, M. Despeisse, M. Boccard, S. Nicolay, Q. Jeangros, B. Niesen, and C. Ballif, “Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency,” Nat. Mater. 17(9), 820–826 (2018).
[Crossref]

Batentschuk, M.

D. Niesner, O. Schuster, M. Wilhelm, I. Levchuk, A. Osvet, S. Shrestha, M. Batentschuk, C. Brabec, and T. Fauster, “Temperature-dependent optical spectra of single-crystal (CH3NH3)PbBr3 cleaved in ultrahigh vacuum,” Phys. Rev. B 95(7), 075207 (2017).
[Crossref]

Beaumont, B.

M. Leroux, N. Grandjean, B. Beaumont, G. Nataf, F. Semond, J. Massies, and P. Gibart, “Temperature quenching of photoluminescence intensities in undoped and doped GaN,” J. Appl. Phys. 86(7), 3721–3728 (1999).
[Crossref]

Bischak, C. G.

L. Dou, A. B. Wong, Y. Yu, M. Lai, N. Kornienko, S. W. Eaton, A. Fu, C. G. Bischak, J. Ma, T. Ding, N. S. Ginsberg, L. W. Wang, A. P. Alivisatos, and P. Yang, “Atomically thin two-dimensional organic-inorganic hybrid perovskites,” Science 349(6255), 1518–1521 (2015).
[Crossref] [PubMed]

Blancon, J. C.

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
[Crossref] [PubMed]

J. C. Blancon, H. Tsai, W. Nie, C. C. Stoumpos, L. Pedesseau, C. Katan, M. Kepenekian, C. M. M. Soe, K. Appavoo, M. Y. Sfeir, S. Tretiak, P. M. Ajayan, M. G. Kanatzidis, J. Even, J. J. Crochet, and A. D. Mohite, “Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites,” Science 355(6331), 1288–1292 (2017).
[Crossref] [PubMed]

Bob, B.

H. S. Duan, H. Zhou, Q. Chen, P. Sun, S. Luo, T.-B. Song, B. Bob, and Y. Yang, “The identification and characterization of defect states in hybrid organic-inorganic perovskite photovoltaics,” Phys. Chem. Chem. Phys. 17(1), 112–116 (2015).
[Crossref] [PubMed]

Boccard, M.

F. Sahli, J. Werner, B. A. Kamino, M. Bräuninger, R. Monnard, B. Paviet-Salomon, L. Barraud, L. Ding, J. J. Diaz Leon, D. Sacchetto, G. Cattaneo, M. Despeisse, M. Boccard, S. Nicolay, Q. Jeangros, B. Niesen, and C. Ballif, “Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency,” Nat. Mater. 17(9), 820–826 (2018).
[Crossref]

Boix, P. P.

S. A. Veldhuis, P. P. Boix, N. Yantara, M. Li, T. C. Sum, N. Mathews, and S. G. Mhaisalkar, “Perovskite Materials for Light-Emitting Diodes and Lasers,” Adv. Mater. 28(32), 6804–6834 (2016).
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Bongiovanni, G.

M. Saba, F. Quochi, A. Mura, G. Bongiovanni, V. Sarritzu, N. Sestu, C. Figus, M. Aresti, R. Piras, A. Geddo Lehmann, C. Cannas, A. Musinu, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

M. Saba, F. Quochi, A. Mura, G. Bongiovanni, V. Sarritzu, N. Sestu, C. Figus, M. Aresti, R. Piras, A. Geddo Lehmann, C. Cannas, A. Musinu, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

M. Saba, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

Brabec, C.

D. Niesner, O. Schuster, M. Wilhelm, I. Levchuk, A. Osvet, S. Shrestha, M. Batentschuk, C. Brabec, and T. Fauster, “Temperature-dependent optical spectra of single-crystal (CH3NH3)PbBr3 cleaved in ultrahigh vacuum,” Phys. Rev. B 95(7), 075207 (2017).
[Crossref]

Brandt, O.

Y. Sun, O. Brandt, S. Cronenberg, S. Dhar, H. T. Grahn, K. H. Ploog, P. Waltereit, and J. S. Speck, “Nonpolar InxGa1-xN/GaN (1-100) multiple quantum wells grown on γ-LiAlO2 (100) by plasma-assisted molecular-beam epitaxy,” Phys. Rev. B Condens. Matter Mater. Phys. 67(4), 041306 (2003).
[Crossref]

Bräuninger, M.

F. Sahli, J. Werner, B. A. Kamino, M. Bräuninger, R. Monnard, B. Paviet-Salomon, L. Barraud, L. Ding, J. J. Diaz Leon, D. Sacchetto, G. Cattaneo, M. Despeisse, M. Boccard, S. Nicolay, Q. Jeangros, B. Niesen, and C. Ballif, “Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency,” Nat. Mater. 17(9), 820–826 (2018).
[Crossref]

Buin, A.

D. Shi, V. Adinolfi, R. Comin, M. Yuan, E. Alarousu, A. Buin, Y. Chen, S. Hoogland, A. Rothenberger, K. Katsiev, Y. Losovyj, X. Zhang, P. A. Dowben, O. F. Mohammed, E. H. Sargent, and O. M. Bakr, “Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
[Crossref] [PubMed]

Burlakov, V. M.

M. I. Saidaminov, A. L. Abdelhady, B. Murali, E. Alarousu, V. M. Burlakov, W. Peng, I. Dursun, L. Wang, Y. He, G. Maculan, A. Goriely, T. Wu, O. F. Mohammed, and O. M. Bakr, “High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization,” Nat. Commun. 6(1), 7586 (2015).
[Crossref] [PubMed]

Cannas, C.

M. Saba, F. Quochi, A. Mura, G. Bongiovanni, V. Sarritzu, N. Sestu, C. Figus, M. Aresti, R. Piras, A. Geddo Lehmann, C. Cannas, A. Musinu, F. Quochi, A. Mura, and G. Bongiovanni, “Excited State Properties of Hybrid Perovskites,” Acc. Chem. Res. 49(1), 166–173 (2016).
[Crossref] [PubMed]

Canton, S. E.

T. J. Savenije, C. S. Ponseca, L. Kunneman, M. Abdellah, K. Zheng, Y. Tian, Q. Zhu, S. E. Canton, I. G. Scheblykin, T. Pullerits, A. Yartsev, and V. Sundström, “Thermally activated exciton dissociation and recombination control the carrier dynamics in organometal halide perovskite,” J. Phys. Chem. Lett. 5(13), 2189–2194 (2014).
[Crossref] [PubMed]

Cattaneo, G.

F. Sahli, J. Werner, B. A. Kamino, M. Bräuninger, R. Monnard, B. Paviet-Salomon, L. Barraud, L. Ding, J. J. Diaz Leon, D. Sacchetto, G. Cattaneo, M. Despeisse, M. Boccard, S. Nicolay, Q. Jeangros, B. Niesen, and C. Ballif, “Fully textured monolithic perovskite/silicon tandem solar cells with 25.2% power conversion efficiency,” Nat. Mater. 17(9), 820–826 (2018).
[Crossref]

Chakraborty, A.

T. Onuma, A. Chakraborty, B. A. Haskell, S. Keller, S. P. DenBaars, J. S. Speck, S. Nakamura, U. K. Mishra, T. Sota, and S. F. Chichibu, “Localized exciton dynamics in nonpolar (11-20) InxGa1-xN multiple quantum wells grown on GaN templates prepared by lateral epitaxial overgrowth,” Appl. Phys. Lett. 86(15), 151918 (2005).
[Crossref]

Chen, C.

S. Ke, C. Chen, N. Fu, H. Zhou, M. Ye, P. Lin, W. Yuan, X. Zeng, L. Chen, and H. Huang, “Transparent Indium Tin Oxide Electrodes on Muscovite Mica for High-Temperature-Processed Flexible Optoelectronic Devices,” ACS Appl. Mater. Interfaces 8(42), 28406–28411 (2016).
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Chen, H.

Z. Yang, Y. Deng, X. Zhang, S. Wang, H. Chen, S. Yang, J. Khurgin, N. X. Fang, X. Zhang, and R. Ma, “High-Performance Single-Crystalline Perovskite Thin-Film Photodetector,” Adv. Mater. 30(8), 1704333 (2018).
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Figures (5)

Fig. 1
Fig. 1 (a) The optical micrograph of the as-grown MAPbBr3 sheets on a mica substrate. (b) Green luminescence of the as-grown MAPbBr3 sheets observed in fluorescence microscopy. (c) Structure of a single cell MAPbBr3 crystal (the gray octahedra stand for [PbBr6]-; the dark red balls stand for [CH3NH3]+ ions). (d) The XRD spectrum of the as-grown 2D MAPbBr3 sheet. (e) The electron diffraction pattern and TEM micrograph of the MAPbBr3 sheet. (f) SEM micrograph of an ultrathin MAPbBr3 and EDS mapping of element distributions for lead and bromine, respectively.
Fig. 2
Fig. 2 (a) Steady-state absorption (blue line) and photoluminescence (red line) spectra of an 2D MAPbBr3 sheet (thickness 65.4 nm) at room temperature. The PL spectrum is excited by a continuous wave laser (450 nm). (b) The PL spectrum can be de-convoluted into two-Gaussian profile functions, the free-carrier recombination peak (green solid line) and exciton recombination peak (blue solid line). (c) The theoretical absorption coefficient (black solid line) is calculated based on Elliott’s formula, which includes the excitonic (green solid line) and free-carrier continuum (red solid line) components. In both b and c, the experimental data (open circles) and the calculated ones (solid lines) are in good agreement.
Fig. 3
Fig. 3 (a) The temperature-dependent PL spectra of MAPbBr3 sheets. By decreasing temperature, the 545 nm peak (Peak2) enhances gradually and red-shift; in contrast, the 532 nm peak (Peak1) decays. (b) The temperature-dependent PL mapping of the 2D MAPbBr3 sheet. (c) Temperature dependence of the intensities of Peak2. By fitting the experiment data, we estimate EB as 14 meV.
Fig. 4
Fig. 4 (a)Power-dependent PL spectra at room temperature for a crystallite 65.4 nm in thickness. (b) The logarithm plot of the integrated intensity of the photoluminescence peaks at 532 and 545 nm, respectively, as a function of the excitation power. (c) Power-dependent PL spectra at 100K for a crystallite 60.7 nm in thickness. (d) The logarithm plot of the integrated PL intensity for (c). (e) The decay-time spectra of 532 nm (Peak1) and 545 nm (Peak2) at room temperature, respectively.
Fig. 5
Fig. 5 (a) Steady-state PL spectra of ultrathin MAPbBr3 sheets with different thickness. (b) Schematics to show different carrier recombination channels in aMAPbBr3 sheet based on PL studies. The yellow dots in the conduction band and the whitedots in the valence band respectively represent electrons and holes created by the absorption ofexcitation light. The excited electrons rapidly release to the bottom of conduction band and return to the ground state via two radiative recombination channels: the free-carrier channel (λ1), and the exciton channel (λ2).

Equations (3)

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α(ω) μ CV 2 ω E B [ n 4π E B n 3 δ(ω E n B )+ 2π E B θ(ω E g ) 1 e 2π E B /(ω E g ) ]
I e (T)= I 0 1+A e E B / k B T ,
I(t)= i=1 M A i exp(t/ τ i ) ,

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