Abstract

Inorganic solution processed CsPbBr3 perovskite thin films are highly promising optoelectronic materials and have been applied in solar cells, light emitting diodes, and photodetectors. They show good electroluminescence properties combined with high thermal stability. In this work, CsPbBr3 perovskite thin films doped with a series of organic cations of various chain lengths, namely, methylammonium (MA), ethylammonium (EA), butylammonium (BA) and octylammonium (OA) at optimized molar ratios of (organic cations: Cs+), were fabricated with a two-step solution process. The crystalline structure, surface morphology and photophysical properties of the films were characterized in detail. The surface morphology of the films was improved with reduced surface roughness, accompanying by doping with the organic cations. The amplified spontaneous emissions (ASE) were observed from all of the different CsPbBr3 films at room temperature. The gain coefficients for the doped CsPbBr3 films were higher than the pristine films, due to much reduced bulk defects, reduced non-radiative recombination in the films, as well as improved surface quality of the films. This work provides a simple method of preparing organic cations modified CsPbBr3 laser gain media of high performance.

© 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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2019 (2)

H. Kim, A. Hagfeldt, and N. Park, “Morphological and compositional progress in halide perovskite solar cells,” Chem. Commun. 55(9), 1192–1200 (2019).
[Crossref]

Y. Liu, Z. Gao, W. Zhang, X. Sun, Z. Wang, X. Wang, B. Xu, and X. Meng, “Stimulated emission from CsPbBr3 quantum dot nanoglass,” Opt. Mater. Express 9(8), 3390 (2019).
[Crossref]

2018 (3)

Y. Cao, N. Wang, H. Tian, J. Guo, Y. Wei, H. Chen, Y. Miao, W. Zou, K. Pan, Y. He, H. Cao, Y. Ke, M. Xu, Y. Wang, M. Yang, K. Du, Z. Fu, D. Kong, D. Dai, Y. Jin, G. Li, H. Li, Q. Peng, J. Wang, and W. Huang, “Perovskite light-emitting diodes based on spontaneously formed submicrometre-scale structures,” Nature 562(7726), 249–253 (2018).
[Crossref]

B. Salhi, Y. S. Wudil, M. K. Hossain, A. Al-Ahmed, and F. A. Al-Sulaiman, “Review of recent developments and persistent challenges in stability of perovskite solar cells,” Renewable Sustainable Energy Rev. 90, 210–222 (2018).
[Crossref]

Y. Wang, L. Yang, H. Chen, C. Liu, W. Liu, H. Xu, C. Zhang, Z. Wang, and Y. Liu, “White LED based on CsPbBr3 nanocrystal phosphors via a facile two-step solution synthesis route,” Mater. Res. Bull. 104, 48–52 (2018).
[Crossref]

2017 (6)

D. Liu, Z. Hu, W. Hu, P. Wangyang, K. Yu, M. Wen, Z. Zu, J. Liu, M. Wang, W. Chen, M. Zhou, X. Tang, and Z. Zang, “Two-step method for preparing all-inorganic CsPbBr3 perovskite film and its photoelectric detection application,” Mater. Lett. 186, 243–246 (2017).
[Crossref]

L. Zhang, X. Yang, Q. Jiang, P. Wang, Z. Yin, X. Zhang, H. Tan, Y. M. Yang, M. Wei, B. R. Sutherland, E. H. Sargent, and J. You, “Ultra-bright and highly efficient inorganic based perovskite light-emitting diodes,” Nat. Commun. 8(1), 15640 (2017).
[Crossref]

B. Tang, H. Dong, L. Sun, W. Zheng, Q. Wang, F. Sun, X. Jiang, A. Pan, and L. Zhang, “Single-Mode Lasers Based on Cesium Lead Halide Perovskite Submicron Spheres,” ACS Nano 11(11), 10681–10688 (2017).
[Crossref]

C. Li, Z. Zang, C. Han, Z. Hu, X. Tang, J. Du, Y. Leng, and K. Sun, “Highly compact CsPbBr3 perovskite thin films decorated by ZnO nanoparticles for enhanced random lasing,” Nano Energy 40, 195–202 (2017).
[Crossref]

M. L. De Giorgi, A. Perulli, N. Yantara, P. P. Boix, and M. Anni, “Amplified Spontaneous Emission Properties of Solution Processed CsPbBr3 Perovskite Thin Films,” J. Phys. Chem. C 121(27), 14772–14778 (2017).
[Crossref]

H. Zhou, S. Yuan, X. Wang, T. Xu, X. Wang, H. Li, W. Zheng, P. Fan, Y. Li, and L. Sun, “Vapor Growth and Tunable Lasing of Band Gap Engineered Cesium Lead Halide Perovskite Micro/Nanorods with Triangular Cross Section,” ACS Nano 11(2), 1189–1195 (2017).
[Crossref]

2016 (13)

F. Sasaki, H. Mochizuki, Y. Zhou, Y. Sonoda, and R. Azumi, “Optical pumped lasing in solution processed perovskite semiconducting materials: Self-assembled microdisk lasing,” Jpn. J. Appl. Phys. 55(4S), 04ES02 (2016).
[Crossref]

K. Wang, W. Sun, J. Li, Z. Gu, S. Xiao, and Q. Song, “Unidirectional Lasing Emissions from CH3NH3PbBr3 Perovskite Microdisks,” ACS Photonics 3(6), 1125–1130 (2016).
[Crossref]

S. Liu, W. Sun, Z. Gu, K. Wang, N. Zhang, S. Xiao, and Q. Song, “Tailoring the lasing modes in CH3NH3PbBr3 perovskite microplates via micro-manipulation,” RSC Adv. 6(56), 50553–50558 (2016).
[Crossref]

Z. Gu, K. Wang, W. Sun, J. Li, S. Liu, Q. Song, and S. Xiao, “Two-Photon Pumped CH3NH3PbBr3 Perovskite Microwire Lasers,” Adv. Opt. Mater. 4(3), 472–479 (2016).
[Crossref]

B. R. Sutherland and E. H. Sargent, “Perovskite photonic sources,” Nat. Photonics 10(5), 295–302 (2016).
[Crossref]

Y. Ling, Y. Tian, X. Wang, J. C. Wang, J. M. Knox, F. Perez-Orive, Y. Du, L. Tan, K. Hanson, B. Ma, and H. Gao, “Enhanced Optical and Electrical Properties of Polymer-Assisted All-Inorganic Perovskites for Light-Emitting Diodes,” Adv. Mater. 28(40), 8983–8989 (2016).
[Crossref]

S. W. Eaton, M. Lai, N. A. Gibson, A. B. Wong, L. Dou, J. Ma, L. Wang, S. R. Leone, and P. Yang, “Lasing in robust cesium lead halide perovskite nanowires,” Proc. Natl. Acad. Sci. U. S. A. 113(8), 1993–1998 (2016).
[Crossref]

X. Tang, Z. Hu, W. Chen, X. Xing, W. Hu, J. Qiu, Z. Zang, J. Du, Y. Leng, X. Jiang, and L. Mai, “Room temperature single-photon emission and lasing for all-inorganic colloidal perovskite quantum dots,” Nano Energy 28, 462–468 (2016).
[Crossref]

S. Chen, K. Roh, J. Lee, W. K. Chong, Y. Lu, N. Mathews, T. C. Sum, and A. Nurmikko, “A Photonic Crystal Laser from Solution Based Organo-Lead Iodide Perovskite Thin Films,” ACS Nano 10(4), 3959–3967 (2016).
[Crossref]

Y. Zhao and K. Zhu, “Organic-inorganic hybrid lead halide perovskites for optoelectronic and electronic applications,” Chem. Soc. Rev. 45(3), 655–689 (2016).
[Crossref]

X. Zhang, B. Xu, J. Zhang, Y. Gao, Y. Zheng, K. Wang, and X. W. Sun, “All-Inorganic Perovskite Nanocrystals for High-Efficiency Light Emitting Diodes: Dual-Phase CsPbBr3-CsPb2Br5 Composites,” Adv. Funct. Mater. 26(25), 4595–4600 (2016).
[Crossref]

L. Meng, J. You, T. Guo, and Y. Yang, “Recent Advances in the Inverted Planar Structure of Perovskite Solar Cells,” Acc. Chem. Res. 49(1), 155–165 (2016).
[Crossref]

X. Zhang, X. Bing, J. Zhang, G. Yuan, and W. S. Xiao, “All-Inorganic Perovskite Nanocrystals for High-Efficiency Light Emitting Diodes: Dual-Phase CsPbBr3 -CsPb2Br5 Composites,” Adv. Funct. Mater. 26(25), 4595–4600 (2016).
[Crossref]

2015 (11)

Z. Yuan, Y. Shu, Y. Tian, Y. Xin, and B. Ma, “A facile one-pot synthesis of deep blue luminescent lead bromide perovskite microdisks,” Chem. Commun. 51(91), 16385–16388 (2015).
[Crossref]

H. Cho, S. Jeong, M. Park, Y. Kim, C. Wolf, C. Lee, J. H. Heo, A. Sadhanala, N. Myoung, S. Yoo, S. H. Im, R. H. Friend, and T. Lee, “Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes,” Science 350(6265), 1222–1225 (2015).
[Crossref]

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, “Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
[Crossref]

N. J. Jeon, J. H. Noh, W. S. Yang, Y. C. Kim, S. Ryu, J. Seo, and S. I. Seok, “Compositional engineering of perovskite materials for high-performance solar cells,” Nature 517(7535), 476–480 (2015).
[Crossref]

N. Yantara, S. Bhaumik, F. Yan, D. Sabba, H. A. Dewi, N. Mathews, P. P. Boix, H. V. Demir, and S. Mhaisalkar, “Inorganic Halide Perovskites for Efficient Light-Emitting Diodes,” J. Phys. Chem. Lett. 6(21), 4360–4364 (2015).
[Crossref]

D. Priante, I. Dursun, M. S. Alias, D. Shi, V. A. Melnikov, T. K. Ng, O. F. Mohammed, O. M. Bakr, and B. S. Ooi, “The recombination mechanisms leading to amplified spontaneous emission at the true-green wavelength in CH3NH3PbBr3 perovskites,” Appl. Phys. Lett. 106(8), 081902 (2015).
[Crossref]

S. Yakunin, L. Protesescu, F. Krieg, M. I. Bodnarchuk, G. Nedelcu, M. Humer, G. D. Luca, M. Fiebig, W. Heiss, and M. V. Kovalenko, “Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites,” Nat. Commun. 6(1), 8056 (2015).
[Crossref]

H. Zhu, Y. Fu, F. Meng, X. Wu, Z. Gong, Q. Ding, M. V. Gustafsson, M. T. Trinh, S. Jin, and X. Zhu, “Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors,” Nat. Mater. 14(6), 636–642 (2015).
[Crossref]

Y. Wang, X. Li, J. Song, L. Xiao, H. Zeng, and H. Sun, “All-Inorganic Colloidal Perovskite Quantum Dots: A New Class of Lasing Materials with Favorable Characteristics,” Adv. Mater. 27(44), 7101–7108 (2015).
[Crossref]

D. Zhang, S. W. Eaton, Y. Yu, L. Dou, and P. Yang, “Solution-Phase Synthesis of Cesium Lead Halide Perovskite Nanowires,” J. Am. Chem. Soc. 137(29), 9230–9233 (2015).
[Crossref]

Q. Liao, K. Hu, H. Zhang, X. Wang, J. Yao, and H. Fu, “Perovskite Microdisk Microlasers Self-Assembled from Solution,” Adv. Mater. 27(22), 3405–3410 (2015).
[Crossref]

2014 (3)

B. R. Sutherland, S. Hoogland, M. M. Adachi, C. T. O. Wong, and E. H. Sargent, “Conformal Organohalide Perovskites Enable Lasing on Spherical Resonators,” ACS Nano 8(10), 10947–10952 (2014).
[Crossref]

T. S. Kao, Y. Chou, C. Chou, F. Chen, and T. Lu, “Lasing behaviors upon phase transition in solution-processed perovskite thin films,” Appl. Phys. Lett. 105(23), 231108 (2014).
[Crossref]

G. Xing, N. Mathews, S. S. Lim, N. Yantara, X. Liu, D. Sabba, M. Gratzel, S. Mhaisalkar, and T. C. Sum, “Low-temperature solution-processed wavelength-tunable perovskites for lasing,” Nat. Mater. 13(5), 476–480 (2014).
[Crossref]

2013 (2)

G. Xing, N. Mathews, S. Sun, S. S. Lim, Y. M. Lam, M. Graetzel, S. Mhaisalkar, and T. C. Sum, “Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3,” Science 342(6156), 344–347 (2013).
[Crossref]

C. C. Stoumpos, C. D. Malliakas, and M. G. Kanatzidis, “Semiconducting tin and lead iodide perovskites with organic cations: phase transitions, high mobilities, and near-infrared photoluminescent properties,” Inorg. Chem. 52(15), 9019–9038 (2013).
[Crossref]

2008 (1)

D. M. Trots and S. V. Myagkota, “High-temperature structural evolution of caesium and rubidium triiodoplumbates,” J. Phys. Chem. Solids 69(10), 2520–2526 (2008).
[Crossref]

2002 (1)

J. Valenta, I. Pelant, and J. Linnros, “Waveguiding effects in the measurement of optical gain in a layer of Si nanocrystals,” Appl. Phys. Lett. 81(8), 1396–1398 (2002).
[Crossref]

Adachi, M. M.

B. R. Sutherland, S. Hoogland, M. M. Adachi, C. T. O. Wong, and E. H. Sargent, “Conformal Organohalide Perovskites Enable Lasing on Spherical Resonators,” ACS Nano 8(10), 10947–10952 (2014).
[Crossref]

Adinolfi, V.

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N. Yantara, S. Bhaumik, F. Yan, D. Sabba, H. A. Dewi, N. Mathews, P. P. Boix, H. V. Demir, and S. Mhaisalkar, “Inorganic Halide Perovskites for Efficient Light-Emitting Diodes,” J. Phys. Chem. Lett. 6(21), 4360–4364 (2015).
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N. Yantara, S. Bhaumik, F. Yan, D. Sabba, H. A. Dewi, N. Mathews, P. P. Boix, H. V. Demir, and S. Mhaisalkar, “Inorganic Halide Perovskites for Efficient Light-Emitting Diodes,” J. Phys. Chem. Lett. 6(21), 4360–4364 (2015).
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S. Yakunin, L. Protesescu, F. Krieg, M. I. Bodnarchuk, G. Nedelcu, M. Humer, G. D. Luca, M. Fiebig, W. Heiss, and M. V. Kovalenko, “Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites,” Nat. Commun. 6(1), 8056 (2015).
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H. Cho, S. Jeong, M. Park, Y. Kim, C. Wolf, C. Lee, J. H. Heo, A. Sadhanala, N. Myoung, S. Yoo, S. H. Im, R. H. Friend, and T. Lee, “Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes,” Science 350(6265), 1222–1225 (2015).
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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, “Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals,” Science 347(6221), 519–522 (2015).
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Q. Liao, K. Hu, H. Zhang, X. Wang, J. Yao, and H. Fu, “Perovskite Microdisk Microlasers Self-Assembled from Solution,” Adv. Mater. 27(22), 3405–3410 (2015).
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Acc. Chem. Res. (1)

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ACS Nano (4)

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Figures (13)

Fig. 1.
Fig. 1. Schematic diagram of the fabrication process of inorganic perovskite films.
Fig. 2.
Fig. 2. SEM images of different organic cations doped perovskite films ((a). CsPbBr3, (b). CsPbBr3:MA, (c). CsPbBr3:EA, (d). CsPbBr3:BA, (e). CsPbBr3:OA).
Fig. 3.
Fig. 3. XRD patterns of the additives doped perovskite films.
Fig. 4.
Fig. 4. Absorption spectra (a) and normalized PL spectra (b) of the perovskite films doped with different organic cations (Excitation wavelength: 400 nm).
Fig. 5.
Fig. 5. Time-resolved fluorescence spectra of the perovskite films with organic cations.
Fig. 6.
Fig. 6. ASE spectra of the CsPbBr3 films pumped by a 400 nm lasing output with a 5 ns pulse width at a repetition rate of 10 Hz. The top shows the fluorescence spectra at different pump energies and the down shows the fluorescence intensity variation as the pump energy increased. (CsPbBr3 films (a)&(f), CsPbBr3:MA films (b)&(g), CsPbBr3:EA films (c)&(h), CsPbBr3:BA films (d)&(i), CsPbBr3:OA films (e) &(j)).
Fig. 7.
Fig. 7. Stability of different organic cations doped perovskite films (Pump energy: 1127 µJ/cm2 above threshold).
Fig. 8.
Fig. 8. Images of the CsPbBr3 films prepared at different soaking time.
Fig. 9.
Fig. 9. XRD patterns of CsPbBr3 films prepared at different soaking time.
Fig. 10.
Fig. 10. AFM images of different organic cations doped perovskite films.
Fig. 11.
Fig. 11. Absorption spectra ((a). CsPbBr3, (c). CsPbBr3:MA, (e). CsPbBr3:EA, (g). CsPbBr3:BA, (i). CsPbBr3:OA) and PL spectra ((b). CsPbBr3, (d). CsPbBr3:MA, (f). CsPbBr3:EA, (h). CsPbBr3:BA, (j). CsPbBr3:OA) of different organic cations doped perovskite films (excitation wavelength: 400 nm).
Fig. 12.
Fig. 12. Gain and loss of the CsPbBr3 films (CsPbBr3 films (a)&(b), CsPbBr3:MA films (c)&(d), CsPbBr3:EA films (e)&(f), CsPbBr3:BA films (g)&(h), CsPbBr3:OA films (i) &(j)).
Fig. 13.
Fig. 13. Stability study of perovskite films at room temperature in air (The left column shows the initial ASE thresholds; the right column shows the ASE thresholds after 5 days) ((a),(b) CsPbBr3 film, (c),(d) CsPbBr3:MA film, (e),(f) CsPbBr3:EA film, (g),(h) CsPbBr3:BA film, i,j CsPbBr3:OA film).

Tables (3)

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Table 1. Absorption spectra and fluorescence spectra of the CsPbBr3 films doped with organic cations

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Table 2. Gain and loss coefficients of the CsPbBr3 films with different organic cations

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Table 3. Photostability of perovskite films at room temperature in air

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