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Title: Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10–x Cl x

Abstract

Two-dimensional (2D) hybrid halide perovskites come as a family (B) 2(A) n-1PbnX 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. Here we report a multilayered 2D perovskite (n = 3) exhibiting a tunable white-light emission. Ethylammonium (EA+) can stabilize the 2D perovskite structure in EA 4Pb 3Br 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 EA 4Pb 3Br 10, which results in broadband white-light emission of EA 4Pb 3Cl 10 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 prolongsmore » the lifetime (more STE states). The band gap of EA 4Pb 3Br 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 EA 4Pb 3Cl 10 and EA 4Pb 3Br 10 are direct band gap semiconductors. The color rendering index (CRI) of the series improves from 66 (EA 4Pb 3Cl 10) to 83 (EA 4Pb 3Br 0.5Cl 9.5), displaying high tunability and versatility of the title compounds.« less

Authors:
ORCiD logo; ORCiD logo; ORCiD logo;  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo; ORCiD logo
  1. Institut des sciences chimiques de Rennes, CNRS, Université de Rennes 1, Ecole Nationale Supérieure de Chimie de Rennes, INSA de Rennes, 35042 Rennes, France
  2. Fonctions Optiques pour les Technologies de l’Information (FOTON), INSA de Rennes, UMR 6082, CNRS, 35708 Rennes, France
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1395374
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 34; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mao, Lingling, Wu, Yilei, Stoumpos, Constantinos C., Traore, Boubacar, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., and Kanatzidis, Mercouri G. Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10–x Cl x. United States: N. p., 2017. Web. doi:10.1021/jacs.7b06143.
Mao, Lingling, Wu, Yilei, Stoumpos, Constantinos C., Traore, Boubacar, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., & Kanatzidis, Mercouri G. Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10–x Cl x. United States. https://doi.org/10.1021/jacs.7b06143
Mao, Lingling, Wu, Yilei, Stoumpos, Constantinos C., Traore, Boubacar, Katan, Claudine, Even, Jacky, Wasielewski, Michael R., and Kanatzidis, Mercouri G. Wed . "Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10–x Cl x". United States. https://doi.org/10.1021/jacs.7b06143.
@article{osti_1395374,
title = {Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10–x Cl x},
author = {Mao, Lingling and Wu, Yilei and Stoumpos, Constantinos C. and Traore, Boubacar and Katan, Claudine and Even, Jacky and Wasielewski, Michael R. and Kanatzidis, Mercouri G.},
abstractNote = {Two-dimensional (2D) hybrid halide perovskites come as a family (B)2(A)n-1PbnX3n+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. Here we report a multilayered 2D perovskite (n = 3) exhibiting a tunable white-light emission. Ethylammonium (EA+) can stabilize the 2D perovskite structure in EA4Pb3Br10–xClx (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 EA4Pb3Br10–xClx 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. The color rendering index (CRI) of the series improves from 66 (EA4Pb3Cl10) to 83 (EA4Pb3Br0.5Cl9.5), displaying high tunability and versatility of the title compounds.},
doi = {10.1021/jacs.7b06143},
url = {https://www.osti.gov/biblio/1395374}, journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 34,
volume = 139,
place = {United States},
year = {2017},
month = {8}
}

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