Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission

Xiaotong Li, Peijun Guo, Mikaël Kepenekian, Ido Hadar, Claudine Katan, Jacky Even, Constantinos C. Stoumpos, Richard D Schaller, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Two-dimensional (2D) halide perovskites exhibit excellent potential for optoelectronics because of their outstanding physical properties and structural diversity. White-light emission is one property of 2D perovskites that originates from self-trapped excitons (STE) in the highly distorted structures. The so-called (110)-oriented 2D perovskites are generally distorted and believed to be good candidates for white-light emitting devices. Here, we report (110)-oriented 2D perovskites, C 4 N 2 H 12 PbX 4 (X = I, Br, Cl), templated by the small cyclic diammonium cation, 3-aminopyrrolidinium (3APr). Structural characterization by single-crystal X-ray diffraction reveals that the distortion of the inorganic part of the structures is influenced by the stereochemical conformation of the cation between the perovskite layers. The experimental bandgaps follow the trend I < Br < Cl (2.56 eV, 3.29 eV, 3.85 eV, respectively). Density functional theory calculations reveal a weak but significant electronic band dispersion along the stacking axis, suggesting a non-negligible interlayer electronic coupling caused by the short proximity of adjacent inorganic layers. The high level of distortion results in the emergence of white-light emission, rarely seen in iodide perovskites, as well as the bromide and chloride isostructural analogues, which provides perfect platform to compare the broad emission mechanism for all three halides. The bromide and chloride perovskites show longer lifetimes and higher color rendering index (CRI) (83 and 85), relevant to solid-state lighting. Temperature-dependent PL measurements confirm that the broad emission comes from different STE mechanism for different halides, with the peak broadening persisting even at low temperature for the chloride compound.

Original languageEnglish
Pages (from-to)3582-3590
Number of pages9
JournalChemistry of Materials
Volume31
Issue number9
DOIs
Publication statusPublished - May 14 2019

Fingerprint

Light emission
Excitons
Cations
Chlorides
Positive ions
Bromides
Optoelectronic devices
Perovskite
Density functional theory
Conformations
Energy gap
Physical properties
Lighting
Single crystals
Iodides
Color
X ray diffraction
Temperature
LDS 751

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

Cite this

Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission. / Li, Xiaotong; Guo, Peijun; Kepenekian, Mikaël; Hadar, Ido; Katan, Claudine; Even, Jacky; Stoumpos, Constantinos C.; Schaller, Richard D; Kanatzidis, Mercouri G.

In: Chemistry of Materials, Vol. 31, No. 9, 14.05.2019, p. 3582-3590.

Research output: Contribution to journalArticle

Li, Xiaotong ; Guo, Peijun ; Kepenekian, Mikaël ; Hadar, Ido ; Katan, Claudine ; Even, Jacky ; Stoumpos, Constantinos C. ; Schaller, Richard D ; Kanatzidis, Mercouri G. / Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission. In: Chemistry of Materials. 2019 ; Vol. 31, No. 9. pp. 3582-3590.
@article{1c087dffb499441293160d9a5198f4c6,
title = "Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission",
abstract = "Two-dimensional (2D) halide perovskites exhibit excellent potential for optoelectronics because of their outstanding physical properties and structural diversity. White-light emission is one property of 2D perovskites that originates from self-trapped excitons (STE) in the highly distorted structures. The so-called (110)-oriented 2D perovskites are generally distorted and believed to be good candidates for white-light emitting devices. Here, we report (110)-oriented 2D perovskites, C 4 N 2 H 12 PbX 4 (X = I, Br, Cl), templated by the small cyclic diammonium cation, 3-aminopyrrolidinium (3APr). Structural characterization by single-crystal X-ray diffraction reveals that the distortion of the inorganic part of the structures is influenced by the stereochemical conformation of the cation between the perovskite layers. The experimental bandgaps follow the trend I < Br < Cl (2.56 eV, 3.29 eV, 3.85 eV, respectively). Density functional theory calculations reveal a weak but significant electronic band dispersion along the stacking axis, suggesting a non-negligible interlayer electronic coupling caused by the short proximity of adjacent inorganic layers. The high level of distortion results in the emergence of white-light emission, rarely seen in iodide perovskites, as well as the bromide and chloride isostructural analogues, which provides perfect platform to compare the broad emission mechanism for all three halides. The bromide and chloride perovskites show longer lifetimes and higher color rendering index (CRI) (83 and 85), relevant to solid-state lighting. Temperature-dependent PL measurements confirm that the broad emission comes from different STE mechanism for different halides, with the peak broadening persisting even at low temperature for the chloride compound.",
author = "Xiaotong Li and Peijun Guo and Mika{\"e}l Kepenekian and Ido Hadar and Claudine Katan and Jacky Even and Stoumpos, {Constantinos C.} and Schaller, {Richard D} and Kanatzidis, {Mercouri G}",
year = "2019",
month = "5",
day = "14",
doi = "10.1021/acs.chemmater.9b01511",
language = "English",
volume = "31",
pages = "3582--3590",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "9",

}

TY - JOUR

T1 - Small Cyclic Diammonium Cation Templated (110)-Oriented 2D Halide (X = I, Br, Cl) Perovskites with White-Light Emission

AU - Li, Xiaotong

AU - Guo, Peijun

AU - Kepenekian, Mikaël

AU - Hadar, Ido

AU - Katan, Claudine

AU - Even, Jacky

AU - Stoumpos, Constantinos C.

AU - Schaller, Richard D

AU - Kanatzidis, Mercouri G

PY - 2019/5/14

Y1 - 2019/5/14

N2 - Two-dimensional (2D) halide perovskites exhibit excellent potential for optoelectronics because of their outstanding physical properties and structural diversity. White-light emission is one property of 2D perovskites that originates from self-trapped excitons (STE) in the highly distorted structures. The so-called (110)-oriented 2D perovskites are generally distorted and believed to be good candidates for white-light emitting devices. Here, we report (110)-oriented 2D perovskites, C 4 N 2 H 12 PbX 4 (X = I, Br, Cl), templated by the small cyclic diammonium cation, 3-aminopyrrolidinium (3APr). Structural characterization by single-crystal X-ray diffraction reveals that the distortion of the inorganic part of the structures is influenced by the stereochemical conformation of the cation between the perovskite layers. The experimental bandgaps follow the trend I < Br < Cl (2.56 eV, 3.29 eV, 3.85 eV, respectively). Density functional theory calculations reveal a weak but significant electronic band dispersion along the stacking axis, suggesting a non-negligible interlayer electronic coupling caused by the short proximity of adjacent inorganic layers. The high level of distortion results in the emergence of white-light emission, rarely seen in iodide perovskites, as well as the bromide and chloride isostructural analogues, which provides perfect platform to compare the broad emission mechanism for all three halides. The bromide and chloride perovskites show longer lifetimes and higher color rendering index (CRI) (83 and 85), relevant to solid-state lighting. Temperature-dependent PL measurements confirm that the broad emission comes from different STE mechanism for different halides, with the peak broadening persisting even at low temperature for the chloride compound.

AB - Two-dimensional (2D) halide perovskites exhibit excellent potential for optoelectronics because of their outstanding physical properties and structural diversity. White-light emission is one property of 2D perovskites that originates from self-trapped excitons (STE) in the highly distorted structures. The so-called (110)-oriented 2D perovskites are generally distorted and believed to be good candidates for white-light emitting devices. Here, we report (110)-oriented 2D perovskites, C 4 N 2 H 12 PbX 4 (X = I, Br, Cl), templated by the small cyclic diammonium cation, 3-aminopyrrolidinium (3APr). Structural characterization by single-crystal X-ray diffraction reveals that the distortion of the inorganic part of the structures is influenced by the stereochemical conformation of the cation between the perovskite layers. The experimental bandgaps follow the trend I < Br < Cl (2.56 eV, 3.29 eV, 3.85 eV, respectively). Density functional theory calculations reveal a weak but significant electronic band dispersion along the stacking axis, suggesting a non-negligible interlayer electronic coupling caused by the short proximity of adjacent inorganic layers. The high level of distortion results in the emergence of white-light emission, rarely seen in iodide perovskites, as well as the bromide and chloride isostructural analogues, which provides perfect platform to compare the broad emission mechanism for all three halides. The bromide and chloride perovskites show longer lifetimes and higher color rendering index (CRI) (83 and 85), relevant to solid-state lighting. Temperature-dependent PL measurements confirm that the broad emission comes from different STE mechanism for different halides, with the peak broadening persisting even at low temperature for the chloride compound.

UR - http://www.scopus.com/inward/record.url?scp=85065710158&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85065710158&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.9b01511

DO - 10.1021/acs.chemmater.9b01511

M3 - Article

AN - SCOPUS:85065710158

VL - 31

SP - 3582

EP - 3590

JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 9

ER -