White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites

Lingling Mao; Yilei Wu; Konstantinos Stoumpos; Michael R. Wasielewski; Mercouri G. Kanatzidis

doi:10.1021/jacs.7b01312

White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites

Lingling Mao, Yilei Wu, Konstantinos Stoumpos, Michael R. Wasielewski, Mercouri G. Kanatzidis^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

561 Scopus citations

Abstract

Hybrid inorganic-organic perovskites are developing rapidly as high performance semiconductors. Recently, two-dimensional (2D) perovskites were found to have white-light, broadband emission in the visible range that was attributed mainly to the role of self-trapped excitons (STEs). Here, we describe three new 2D lead bromide perovskites incorporating a series of bifunctional ammonium dications as templates which also emit white light: (1) α-(DMEN)PbBr ₄ (DMEN = 2-(dimethylamino)ethylamine), which adopts a unique corrugated layered structure in space group Pbca with unit cell a = 18.901(4) Å, b = 11.782(2) Å, and c = 23.680(5) Å (2) (DMAPA)PbBr ₄ (DMAPA = 3-(dimethylamino)-1-propylamine), which crystallizes in P2 ₁ /c with a = 10.717(2) Å, b = 11.735(2) Å, c = 12.127(2) Å, and β = 111.53(3)° and (3) (DMABA)PbBr ₄ (DMABA = 4-dimethylaminobutylamine), which adopts Aba2 with a = 41.685(8) Å, b = 23.962(5) Å, and c = 12.000(2) Å. Photoluminescence (PL) studies show a correlation between the distortion of the "PbBr ₆ " octahedron in the 2D layer and the broadening of PL emission, with the most distorted structure having the broadest emission (183 nm full width at half-maximum) and longest lifetime (τ _avg = 1.39 ns). The most distorted member α-(DMEN)PbBr ₄ exhibits white-light emission with a color rendering index (CRI) of 73 which is similar to a fluorescent light source and correlated color temperature (CCT) of 7863 K, producing "cold" white light.

Original language	English (US)
Pages (from-to)	5210-5215
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	139
Issue number	14
DOIs	https://doi.org/10.1021/jacs.7b01312
State	Published - Apr 12 2017

Funding

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).

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.7b01312

Cite this

@article{799ed44ecd6d425184fa9a727a63c89f,

title = "White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites",

abstract = " Hybrid inorganic-organic perovskites are developing rapidly as high performance semiconductors. Recently, two-dimensional (2D) perovskites were found to have white-light, broadband emission in the visible range that was attributed mainly to the role of self-trapped excitons (STEs). Here, we describe three new 2D lead bromide perovskites incorporating a series of bifunctional ammonium dications as templates which also emit white light: (1) α-(DMEN)PbBr 4 (DMEN = 2-(dimethylamino)ethylamine), which adopts a unique corrugated layered structure in space group Pbca with unit cell a = 18.901(4) {\AA}, b = 11.782(2) {\AA}, and c = 23.680(5) {\AA} (2) (DMAPA)PbBr 4 (DMAPA = 3-(dimethylamino)-1-propylamine), which crystallizes in P2 1 /c with a = 10.717(2) {\AA}, b = 11.735(2) {\AA}, c = 12.127(2) {\AA}, and β = 111.53(3)° and (3) (DMABA)PbBr 4 (DMABA = 4-dimethylaminobutylamine), which adopts Aba2 with a = 41.685(8) {\AA}, b = 23.962(5) {\AA}, and c = 12.000(2) {\AA}. Photoluminescence (PL) studies show a correlation between the distortion of the {"}PbBr 6 {"} octahedron in the 2D layer and the broadening of PL emission, with the most distorted structure having the broadest emission (183 nm full width at half-maximum) and longest lifetime (τ avg = 1.39 ns). The most distorted member α-(DMEN)PbBr 4 exhibits white-light emission with a color rendering index (CRI) of 73 which is similar to a fluorescent light source and correlated color temperature (CCT) of 7863 K, producing {"}cold{"} white light. ",

author = "Lingling Mao and Yilei Wu and Konstantinos Stoumpos and Wasielewski, {Michael R.} and Kanatzidis, {Mercouri G.}",

note = "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). Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

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AU - Wu, Yilei

AU - Stoumpos, Konstantinos

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). Publisher Copyright: © 2017 American Chemical Society.

PY - 2017/4/12

Y1 - 2017/4/12

N2 - Hybrid inorganic-organic perovskites are developing rapidly as high performance semiconductors. Recently, two-dimensional (2D) perovskites were found to have white-light, broadband emission in the visible range that was attributed mainly to the role of self-trapped excitons (STEs). Here, we describe three new 2D lead bromide perovskites incorporating a series of bifunctional ammonium dications as templates which also emit white light: (1) α-(DMEN)PbBr 4 (DMEN = 2-(dimethylamino)ethylamine), which adopts a unique corrugated layered structure in space group Pbca with unit cell a = 18.901(4) Å, b = 11.782(2) Å, and c = 23.680(5) Å (2) (DMAPA)PbBr 4 (DMAPA = 3-(dimethylamino)-1-propylamine), which crystallizes in P2 1 /c with a = 10.717(2) Å, b = 11.735(2) Å, c = 12.127(2) Å, and β = 111.53(3)° and (3) (DMABA)PbBr 4 (DMABA = 4-dimethylaminobutylamine), which adopts Aba2 with a = 41.685(8) Å, b = 23.962(5) Å, and c = 12.000(2) Å. Photoluminescence (PL) studies show a correlation between the distortion of the "PbBr 6 " octahedron in the 2D layer and the broadening of PL emission, with the most distorted structure having the broadest emission (183 nm full width at half-maximum) and longest lifetime (τ avg = 1.39 ns). The most distorted member α-(DMEN)PbBr 4 exhibits white-light emission with a color rendering index (CRI) of 73 which is similar to a fluorescent light source and correlated color temperature (CCT) of 7863 K, producing "cold" white light.

AB - Hybrid inorganic-organic perovskites are developing rapidly as high performance semiconductors. Recently, two-dimensional (2D) perovskites were found to have white-light, broadband emission in the visible range that was attributed mainly to the role of self-trapped excitons (STEs). Here, we describe three new 2D lead bromide perovskites incorporating a series of bifunctional ammonium dications as templates which also emit white light: (1) α-(DMEN)PbBr 4 (DMEN = 2-(dimethylamino)ethylamine), which adopts a unique corrugated layered structure in space group Pbca with unit cell a = 18.901(4) Å, b = 11.782(2) Å, and c = 23.680(5) Å (2) (DMAPA)PbBr 4 (DMAPA = 3-(dimethylamino)-1-propylamine), which crystallizes in P2 1 /c with a = 10.717(2) Å, b = 11.735(2) Å, c = 12.127(2) Å, and β = 111.53(3)° and (3) (DMABA)PbBr 4 (DMABA = 4-dimethylaminobutylamine), which adopts Aba2 with a = 41.685(8) Å, b = 23.962(5) Å, and c = 12.000(2) Å. Photoluminescence (PL) studies show a correlation between the distortion of the "PbBr 6 " octahedron in the 2D layer and the broadening of PL emission, with the most distorted structure having the broadest emission (183 nm full width at half-maximum) and longest lifetime (τ avg = 1.39 ns). The most distorted member α-(DMEN)PbBr 4 exhibits white-light emission with a color rendering index (CRI) of 73 which is similar to a fluorescent light source and correlated color temperature (CCT) of 7863 K, producing "cold" white light.

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White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites

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CCDC 1963064: Experimental Crystal Structure Determination

CCDC 1963065: Experimental Crystal Structure Determination

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White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites

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ASJC Scopus subject areas

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CCDC 1963064: Experimental Crystal Structure Determination

CCDC 1963065: Experimental Crystal Structure Determination

CCDC 1963066: Experimental Crystal Structure Determination

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