TY - JOUR
T1 - Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH3CH2NH3)4Pb3Br10-xClx
AU - Mao, Lingling
AU - Wu, Yilei
AU - Stoumpos, Constantinos C.
AU - Traore, Boubacar
AU - Katan, Claudine
AU - Even, Jacky
AU - Wasielewski, Michael R.
AU - Kanatzidis, Mercouri G.
N1 - Funding Information:
This work was supported by the Department of Energy, Office of Science, Basic Energy Sciences, under Grant SC0012541. Y.W. thanks the Fulbright Scholars Program for a Graduate Research Fellowship and gratefully acknowledges support of a Ryan Fellowship from the NU International Institute for Nanotechnology (IIN). Use of the Advanced Photon Source at Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The work at ISCR is supported by Agence Nationale pour la Recherche (TRANSHYPERO project).
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/8/30
Y1 - 2017/8/30
N2 - 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.
AB - 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.
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U2 - 10.1021/jacs.7b06143
DO - 10.1021/jacs.7b06143
M3 - Article
C2 - 28745881
AN - SCOPUS:85028645718
VL - 139
SP - 11956
EP - 11963
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 34
ER -