Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2 mNH3)(CH3NH3)n-1PbnI3 n+1 (m = 4-9; N = 1-4)

Xiaotong Li, Justin Hoffman, Weijun Ke, Michelle Chen, Hsinhan Tsai, Wanyi Nie, Aditya D. Mohite, Mikaël Kepenekian, Claudine Katan, Jacky Even, Michael R Wasielewski, Constantinos C. Stoumpos, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

Low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4-9; n = 1-4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer (n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7-9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series (n = 1-4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer (n = 2), 2.01 eV for three-layer (n = 3), and 1.90 eV for four-layer (n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher-m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displaying both vertical and parallel layer orientation, as confirmed by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. The vertical layer orientation for the (NH3C8H16NH3)(CH3NH3)2Pb3I10 member results in the best thermal, light, and air stability within this series, thus showing excellent potential for solar cell applications.

Original languageEnglish
Pages (from-to)12226-12238
Number of pages13
JournalJournal of the American Chemical Society
Volume140
Issue number38
DOIs
Publication statusPublished - Sep 26 2018

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Ions
Optical band gaps
X ray scattering
X-Ray Diffraction
Glass
Cations
Solar cells
Multilayers
Casting
Carbon
Hot Temperature
Positive ions
Air
X-Rays
Single crystals
Light
X ray diffraction
Thin films
Incidence
Substrates

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2 mNH3)(CH3NH3)n-1PbnI3 n+1 (m = 4-9; N = 1-4). / Li, Xiaotong; Hoffman, Justin; Ke, Weijun; Chen, Michelle; Tsai, Hsinhan; Nie, Wanyi; Mohite, Aditya D.; Kepenekian, Mikaël; Katan, Claudine; Even, Jacky; Wasielewski, Michael R; Stoumpos, Constantinos C.; Kanatzidis, Mercouri G.

In: Journal of the American Chemical Society, Vol. 140, No. 38, 26.09.2018, p. 12226-12238.

Research output: Contribution to journalArticle

Li, Xiaotong ; Hoffman, Justin ; Ke, Weijun ; Chen, Michelle ; Tsai, Hsinhan ; Nie, Wanyi ; Mohite, Aditya D. ; Kepenekian, Mikaël ; Katan, Claudine ; Even, Jacky ; Wasielewski, Michael R ; Stoumpos, Constantinos C. ; Kanatzidis, Mercouri G. / Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2 mNH3)(CH3NH3)n-1PbnI3 n+1 (m = 4-9; N = 1-4). In: Journal of the American Chemical Society. 2018 ; Vol. 140, No. 38. pp. 12226-12238.
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abstract = "Low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4-9; n = 1-4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer (n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7-9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series (n = 1-4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer (n = 2), 2.01 eV for three-layer (n = 3), and 1.90 eV for four-layer (n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher-m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displaying both vertical and parallel layer orientation, as confirmed by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. The vertical layer orientation for the (NH3C8H16NH3)(CH3NH3)2Pb3I10 member results in the best thermal, light, and air stability within this series, thus showing excellent potential for solar cell applications.",
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AU - Hoffman, Justin

AU - Ke, Weijun

AU - Chen, Michelle

AU - Tsai, Hsinhan

AU - Nie, Wanyi

AU - Mohite, Aditya D.

AU - Kepenekian, Mikaël

AU - Katan, Claudine

AU - Even, Jacky

AU - Wasielewski, Michael R

AU - Stoumpos, Constantinos C.

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N2 - Low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4-9; n = 1-4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer (n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7-9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series (n = 1-4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer (n = 2), 2.01 eV for three-layer (n = 3), and 1.90 eV for four-layer (n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher-m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displaying both vertical and parallel layer orientation, as confirmed by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. The vertical layer orientation for the (NH3C8H16NH3)(CH3NH3)2Pb3I10 member results in the best thermal, light, and air stability within this series, thus showing excellent potential for solar cell applications.

AB - Low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4-9; n = 1-4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer (n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7-9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series (n = 1-4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer (n = 2), 2.01 eV for three-layer (n = 3), and 1.90 eV for four-layer (n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher-m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displaying both vertical and parallel layer orientation, as confirmed by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. The vertical layer orientation for the (NH3C8H16NH3)(CH3NH3)2Pb3I10 member results in the best thermal, light, and air stability within this series, thus showing excellent potential for solar cell applications.

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