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

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

^[1]; ^[2]; ^[2]; Traore, Boubacar ^[3]; ^[3]; ^[4]; ^[2]; ^[2]

Northwestern Univ., Evanston, IL (United States); UC Santa Barbara
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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

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

OSTI ID:: 1599737

Alternate ID(s):: OSTI ID: 1395374

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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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
Edge stabilization in reduced-dimensional perovskites Na Quan, Li; Ma, Dongxin; Zhao, Yongbiao Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-019-13944-2	journal	January 2020
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
Two-dimensional halide perovskite nanomaterials and heterostructures Shi, Enzheng; Gao, Yao; Finkenauer, Blake P. Chemical Society Reviews, Vol. 47, Issue 16 https://doi.org/10.1039/c7cs00886d	journal	January 2018
Broadband white-light emission with a high color rendering index in a two-dimensional organic–inorganic hybrid perovskite Wu, Zhenyue; Ji, Chengmin; Sun, Zhihua Journal of Materials Chemistry C, Vol. 6, Issue 5 https://doi.org/10.1039/c7tc04868h	journal	January 2018
Extra thermo- and water-stable one-dimensional organic–inorganic hybrid perovskite [ N -methyldabconium]PbI ₃ showing switchable dielectric behaviour, conductivity and bright yellow-green emission Xue, Chen; Yao, Zhi-Yuan; Zhang, Jin Chemical Communications, Vol. 54, Issue 34 https://doi.org/10.1039/c8cc00786a	journal	January 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
White perovskite based lighting devices Bidikoudi, M.; Fresta, E.; Costa, R. D. Chemical Communications, Vol. 54, Issue 59 https://doi.org/10.1039/c8cc03166e	journal	January 2018
An ultrastable metal–organic material emits efficient and broadband bluish white-light emission for luminescent thermometers Yin, Jinlin; Zhang, Guiyang; Peng, Chengdong Chemical Communications, Vol. 55, Issue 12 https://doi.org/10.1039/c8cc08726a	journal	January 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
Rational chemical doping of metal halide perovskites Zhang, Xinyuan; Li, Lina; Sun, Zhihua Chemical Society Reviews, Vol. 48, Issue 2 https://doi.org/10.1039/c8cs00563j	journal	January 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
Efficient ambient-air-stable HTM-free carbon-based perovskite solar cells with hybrid 2D–3D lead halide photoabsorbers Zhou, Junshuai; Ye, Zhili; Hou, Jie Journal of Materials Chemistry A, Vol. 6, Issue 45 https://doi.org/10.1039/c8ta07836j	journal	January 2018
Molecular engineering of two-dimensional hybrid perovskites with broadband emission for white light-emitting diodes Hu, Hongwei; Morris, Samuel A.; Qiao, Xianfeng Journal of Materials Chemistry C, Vol. 6, Issue 38 https://doi.org/10.1039/c8tc03001d	journal	January 2018
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
(C ₃ H ₉ NI) ₄ AgBiI ₈ : a direct-bandgap layered double perovskite based on a short-chain spacer cation for light absorption Yao, Yunpeng; Kou, Bo; Peng, Yu Chemical Communications, Vol. 56, Issue 21 https://doi.org/10.1039/c9cc07796k	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
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
Broadband white-light emission from supramolecular piperazinium-based lead halide perovskites linked by hydrogen bonds Jung, Mi-Hee; Ko, Kyoung Chul; Lee, Woo Ram Dalton Transactions, Vol. 48, Issue 40 https://doi.org/10.1039/c9dt03469b	journal	January 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
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
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
Organic cation directed hybrid lead halides of zero-dimensional to two-dimensional structures with tunable photoluminescence properties Yue, Cheng-Yang; Sun, Hai-Xiao; Liu, Quan-Xiu Inorganic Chemistry Frontiers, Vol. 6, Issue 10 https://doi.org/10.1039/c9qi00684b	journal	January 2019
Luminescent perovskites: recent advances in theory and experiments Song, Zhen; Zhao, Jing; Liu, Quanlin Inorganic Chemistry Frontiers, Vol. 6, Issue 11 https://doi.org/10.1039/c9qi00777f	journal	January 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
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
Piperidine-induced Switching of the direct band gaps of Ag( i )/Bi( iii ) bimetallic iodide double perovskites Lassoued, Mohamed Saber; Bi, Le-Yu; Wu, Zhaoxin Journal of Materials Chemistry C https://doi.org/10.1039/d0tc01017k	journal	January 2020
Chirality control in white-light emitting 2D perovskites Trujillo-Hernández, Karla; Rodríguez-López, Germán; Espinosa-Roa, Arian Journal of Materials Chemistry C, Vol. 8, Issue 28 https://doi.org/10.1039/d0tc02118k	journal	January 2020
Structure-controlled optical thermoresponse in Ruddlesden-Popper layered perovskites Cortecchia, D.; Neutzner, S.; Yin, J. APL Materials, Vol. 6, Issue 11 https://doi.org/10.1063/1.5045782	journal	November 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
Microstructure and elastic constants of AlTiVMoNb refractory high-entropy alloy coating on Ti6Al4V by laser cladding Chen, Lin; Zhang, Xiaowei; Wang, Yueyi Materials Research Express, Vol. 6, Issue 11 https://doi.org/10.1088/2053-1591/ab49e7	journal	September 2019
Influence of π -conjugated cations and halogen substitution on the optoelectronic and excitonic properties of layered hybrid perovskites Leveillee, Joshua; Katan, Claudine; Zhou, Liujiang Physical Review Materials, Vol. 2, Issue 10 https://doi.org/10.1103/physrevmaterials.2.105406	journal	October 2018

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CCDC 1573846: Experimental Crystal Structure Determination Mao, Lingling; Wu, Yilei; Stoumpos, Constantinos C. https://doi.org/10.5517/ccdc.csd.cc1ptq7g The current record is supplemented by this dataset	dataset	January 2017
CCDC 1573847: Experimental Crystal Structure Determination Mao, Lingling; Wu, Yilei; Stoumpos, Constantinos C. https://doi.org/10.5517/ccdc.csd.cc1ptq8h The current record is supplemented by this dataset	dataset	January 2017