Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH3CH2NH3)4Pb3Br10–xClx

Mao, Lingling; Wu, Yilei; Stoumpos, Constantinos C.; Traore, Boubacar; Katan, Claudine; Even, Jacky; Wasielewski, Michael R.; Kanatzidis, Mercouri G.

doi:10.1021/jacs.7b06143

Title: Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH₃CH₂NH₃)₄Pb₃Br_10–xCl_x

Journal Article · Wed Jul 26 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b06143· OSTI ID:1599737

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Northwestern Univ., Evanston, IL (United States)
Université de Rennes (France)
Fonctions Optiques pour les Technologies de l’Information (FOTON), INSA de Rennes (France)

Two-dimensional (2D) hybrid halide perovskites come as a family (B)₂(A)_n-1Pb_nX_3n+1 (B and A= cations; X= halide). These perovskites are promising semiconductors for solar cells and optoelectronic applications. Among the fascinating properties of these materials is white-light emission, which has been mostly observed in single-layered 2D lead bromide or chloride systems (n = 1), where the broad emission comes from the transient photoexcited states generated by self-trapped excitons (STEs) from structural distortion. In this paper, we report a multilayered 2D perovskite (n = 3) exhibiting a tunable white-light emission. Ethylammonium (EA⁺) can stabilize the 2D perovskite structure in EA₄Pb₃Br_10–xCl_x (x = 0, 2, 4, 6, 8, 9.5, and 10) with EA⁺ being both the A and B cations in this system. Because of the larger size of EA, these materials show a high distortion level in their inorganic structures, with EA₄Pb₃Cl₁₀ having a much larger distortion than that of EA₄Pb₃Br₁₀, which results in broadband white-light emission of EA₄Pb₃Cl₁₀ in contrast to narrow blue emission of EA₄Pb₃Br₁₀. The average lifetime of the series decreases gradually from the Cl end to the Br end, indicating that the larger distortion also prolongs the lifetime (more STE states). The band gap of EA₄Pb₃Br_10–xCl_x ranges from 3.45 eV (x = 10) to 2.75 eV (x = 0), following Vegard’s law. First-principles density functional theory calculations (DFT) show that both EA₄Pb₃Cl₁₀ and EA₄Pb₃Br₁₀ are direct band gap semiconductors. Finally, the color rendering index (CRI) of the series improves from 66 (EA₄Pb₃Cl₁₀) to 83 (EA₄Pb₃Br_0.5Cl_9.5), displaying high tunability and versatility of the title compounds.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012541; AC02-06CH11357

OSTI ID:: 1599737

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 34; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 278 works

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Recent Advances toward High-Efficiency Halide Perovskite Light-Emitting Diodes: Review and Perspective Van Le, Quyet; Jang, Ho Won; Kim, Soo Young Small Methods, Vol. 2, Issue 10 https://doi.org/10.1002/smtd.201700419	journal	July 2018
Tracking the dimensional conversion process of semiconducting lead bromide perovskites by mass spectroscopy, powder X-ray diffraction, microcalorimetry and crystallography Hu, Yue-Qiao; Hui, Hong-Yan; Wen, Hong-Qiang Dalton Transactions, Vol. 48, Issue 34 https://doi.org/10.1039/c9dt02068c	journal	January 2019
Solution Route to Single-Crystalline Ethylammonium Lead Halide Microstructures Ma, Dewei; Dai, Ning; Lan, Yuguo ChemistrySelect, Vol. 4, Issue 7 https://doi.org/10.1002/slct.201804046	journal	February 2019
Negative Thermal Quenching of Efficient White‐Light Emission in a 1D Ladder‐Like Organic/Inorganic Hybrid Material Barkaoui, Hamdi; Abid, Haitham; Zelewski, Szymon Advanced Optical Materials, Vol. 7, Issue 20 https://doi.org/10.1002/adom.201900763	journal	July 2019
Single‐Component White‐Light Emission in 2D Hybrid Perovskites with Hybridized Halogen Atoms Zhou, Guojun; Li, Mingze; Zhao, Jing Advanced Optical Materials, Vol. 7, Issue 24 https://doi.org/10.1002/adom.201901335	journal	September 2019
Two low-dimensional metal halides: ionothermal synthesis, photoluminescence, and nonlinear optical properties Deng, Yuandan; Dong, Xuehua; Yang, Meng Dalton Transactions, Vol. 48, Issue 47 https://doi.org/10.1039/c9dt04102h	journal	January 2019
Pressure‐Induced Emission (PIE) and Phase Transition of a Two‐dimensional Halide Double Perovskite (BA) ₄ AgBiBr ₈ (BA=CH ₃ (CH ₂ ) ₃ NH ₃ ⁺ ) Fang, Yuanyuan; Zhang, Long; Wu, Lianwei Angewandte Chemie International Edition, Vol. 58, Issue 43 https://doi.org/10.1002/anie.201906311	journal	October 2019
Syntheses of two-dimensional propylammonium lead halide perovskite microstructures by a solution route Ma, Dewei; Xu, Zhousu; Wang, Fangjie CrystEngComm, Vol. 21, Issue 9 https://doi.org/10.1039/c8ce02005a	journal	January 2019
Recent Progress in Metal Halide Perovskite Micro‐ and Nanolasers Wei, Qi; Li, Xiaojun; Liang, Chao Advanced Optical Materials, Vol. 7, Issue 17 https://doi.org/10.1002/adom.201900080	journal	April 2019
Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides Benin, Bogdan M.; Dirin, Dmitry N.; Morad, Viktoriia Angewandte Chemie, Vol. 130, Issue 35 https://doi.org/10.1002/ange.201806452	journal	July 2018
Self‐Trapped Exciton to Dopant Energy Transfer in Rare Earth Doped Lead‐Free Double Perovskite Li, Shunran; Hu, Qingsong; Luo, Jiajun Advanced Optical Materials, Vol. 7, Issue 23 https://doi.org/10.1002/adom.201901098	journal	September 2019
A 3D Haloplumbate Framework Constructed From Unprecedented Lindqvist-like Highly Coordinated [Pb ₆ Br ₂₅ ] ¹³⁻ Nanoclusters with Temperature-Dependent Emission Li, Xinxiong; Do, T. Thu Ha; Granados del Águila, A. Chemistry - An Asian Journal, Vol. 13, Issue 21 https://doi.org/10.1002/asia.201801292	journal	October 2018
Structural and thermodynamic limits of layer thickness in 2D halide perovskites Soe, Chan Myae Myae; Nagabhushana, G. P.; Shivaramaiah, Radha Proceedings of the National Academy of Sciences, Vol. 116, Issue 1 https://doi.org/10.1073/pnas.1811006115	journal	December 2018
Perovskite-Based Nanocrystals: Synthesis and Applications beyond Solar Cells Wang, Ning; Liu, Wenbo; Zhang, Qichun Small Methods, Vol. 2, Issue 6 https://doi.org/10.1002/smtd.201700380	journal	April 2018
Highly efficient white-light emission in a polar two-dimensional hybrid perovskite Wang, Sasa; Yao, Yunpeng; Kong, Jintao Chemical Communications, Vol. 54, Issue 32 https://doi.org/10.1039/c8cc01663a	journal	January 2018
Unraveling the mechanochemical synthesis and luminescence in MnII-based two-dimensional hybrid perovskite (C4H9NH3)2PbCl4 Zhou, Guojun; Guo, Shaoqiang; Zhao, Jing Science China Materials, Vol. 62, Issue 7 https://doi.org/10.1007/s40843-018-9404-4	journal	March 2019
A 3D Iodoplumbate Semiconducting Open Framework with Visible‐light‐induced Photocatalytic Performance Ge, Bang‐Di; Wei, Qi; Sun, Ai‐Huan Chemistry – An Asian Journal, Vol. 14, Issue 12 https://doi.org/10.1002/asia.201900392	journal	May 2019
Melting temperature suppression of layered hybrid lead halide perovskites via organic ammonium cation branching Li, Tianyang; Dunlap-Shohl, Wiley A.; Reinheimer, Eric W. Chemical Science, Vol. 10, Issue 4 https://doi.org/10.1039/c8sc03863e	journal	January 2019
White light emission in low-dimensional perovskites Cortecchia, Daniele; Yin, Jun; Petrozza, Annamaria Journal of Materials Chemistry C, Vol. 7, Issue 17 https://doi.org/10.1039/c9tc01036j	journal	January 2019
Merits and Challenges of Ruddlesden-Popper Soft Halide Perovskites in Electro-Optics and Optoelectronics Chen, Zhizhong; Guo, Yuwei; Wertz, Esther Advanced Materials, Vol. 31, Issue 1 https://doi.org/10.1002/adma.201803514	journal	October 2018
Molecular engineering of organic–inorganic hybrid perovskites quantum wells Gao, Yao; Shi, Enzheng; Deng, Shibin Nature Chemistry, Vol. 11, Issue 12 https://doi.org/10.1038/s41557-019-0354-2	journal	November 2019
Organic intercalation engineering of quasi-2D Dion–Jacobson α-CsPbI ₃ perovskites Fang, Zhi; Shang, Minghui; Zheng, Yapeng Materials Horizons, Vol. 7, Issue 4 https://doi.org/10.1039/c9mh01788g	journal	January 2020
Organic cation directed one-dimensional cuprous halide compounds: syntheses, crystal structures and photoluminescence properties Yue, Cheng-Yang; Lin, Na; Gao, Lu Dalton Transactions, Vol. 48, Issue 27 https://doi.org/10.1039/c9dt01460h	journal	January 2019
Realization of “warm” white light via halide substitution in polar two-dimensional hybrid perovskites (2meptH ₂ )PbCl _x Br _4−x Wang, Sasa; Yao, Yunpeng; Wu, Zhenyue Journal of Materials Chemistry C, Vol. 6, Issue 45 https://doi.org/10.1039/c8tc03167c	journal	January 2018
Fluorination of Organic Spacer Impacts on the Structural and Optical Response of 2D Perovskites García-Benito, Inés; Quarti, Claudio; Queloz, Valentin I. E. Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00946	journal	January 2020
Broadband white light emission from one-dimensional zigzag edge-sharing perovskite Jung, Mi-Hee New Journal of Chemistry, Vol. 44, Issue 1 https://doi.org/10.1039/c9nj04758a	journal	January 2020
Intrinsic Self‐Trapped Emission in 0D Lead‐Free (C ₄ H ₁₄ N ₂ ) ₂ In ₂ Br ₁₀ Single Crystal Zhou, Lei; Liao, Jin‐Feng; Huang, Zeng‐Guang Angewandte Chemie, Vol. 131, Issue 43 https://doi.org/10.1002/ange.201907503	journal	September 2019
Dual phosphorescence from the organic and inorganic moieties of 1D hybrid perovskites of the Pb _n′ Br _4n′+2 series ( n ′ = 2, 3, 4, 5) Ben Haj Salah, Maroua; Mercier, Nicolas; Allain, Magali Journal of Materials Chemistry C, Vol. 7, Issue 15 https://doi.org/10.1039/c9tc00340a	journal	January 2019
Surface Termination, Morphology, and Bright Photoluminescence of Cesium Lead Halide Perovskite Nanocrystals ten Brinck, Stephanie; Infante, Ivan ACS Energy Letters, Vol. 1, Issue 6 https://doi.org/10.1021/acsenergylett.6b00595	journal	November 2016
Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides Benin, Bogdan M.; Dirin, Dmitry N.; Morad, Viktoriia Angewandte Chemie International Edition, Vol. 57, Issue 35 https://doi.org/10.1002/anie.201806452	journal	July 2018

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Title: Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH₃CH₂NH₃)₄Pb₃Br_10–xCl_x