Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)

doi:10.1021/jacs.8b07712

Title: Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH₃C_mH_2mNH₃)(CH₃NH₃)_n-1Pb_nI_3n+1 (m = 4–9; n = 1–4)

Abstract

We report that 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 (NH₃C_mH_2mNH₃)(CH₃NH₃)_n-1Pb_nI_3n+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 displayingmore »« less

Authors:

Li, Xiaotong ^[1]; Hoffman, Justin ^[2];

^[1];

^[3];

^[4];

^[5];

^[6];

^[1];

^[1]

Northwestern Univ., Evanston, IL (United States)
Northwestern Univ., Evanston, IL (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Rice Univ., Houston, TX (United States)
Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) (France)
Univ Rennes, INSA Rennes, CNRS, Institut FOTON (France)

Publication Date:: 2018-08-31

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Laboratory Directed Research and Development (LDRD) Program

OSTI Identifier:: 1506004

Report Number(s):: LA-UR-19-20437
Journal ID: ISSN 0002-7863

Grant/Contract Number:: 89233218CNA000001; SC0012704; AC52-06NA25396; SC0001059; FOA-0001647-1544; AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 140; Journal Issue: 38; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    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., and Kanatzidis, Mercouri G. Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4).  United States: N. p., 2018. 
        Web.  doi:10.1021/jacs.8b07712.

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                    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, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4).  United States.  doi:10.1021/jacs.8b07712.

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                    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., and Kanatzidis, Mercouri G. Fri .  
        "Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)".  United States.  doi:10.1021/jacs.8b07712.  https://www.osti.gov/servlets/purl/1506004.

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@article{osti_1506004,

  title        = {Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)},

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

  abstractNote = {We report that 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. Lastly, 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.},

  doi          = {10.1021/jacs.8b07712},

  journal      = {Journal of the American Chemical Society},

  number       = 38,

  volume       = 140,

  place        = {United States},

  year         = {2018},

  month        = {8}

}

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DOI: 10.1021/jacs.8b07712

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Cited by: 52 works

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CCDC 1869670: Experimental Crystal Structure Determination
dataset, January 2018

Xiaotong, Li,; Justin, Hoffman,; Weijun, Ke,
Cambridge Crystallographic Data Centre
DOI: 10.5517/ccdc.csd.cc20rjy8

CCDC 1869671: Experimental Crystal Structure Determination
dataset, January 2018

Xiaotong, Li,; Justin, Hoffman,; Weijun, Ke,
Cambridge Crystallographic Data Centre
DOI: 10.5517/ccdc.csd.cc20rjz9

CCDC 1869672: Experimental Crystal Structure Determination
dataset, January 2018

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Cambridge Crystallographic Data Centre
DOI: 10.5517/ccdc.csd.cc20rk0c

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Xiaotong, Li,; Justin, Hoffman,; Weijun, Ke,
Cambridge Crystallographic Data Centre
DOI: 10.5517/ccdc.csd.cc20rk1d

CCDC 1869674: Experimental Crystal Structure Determination
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Cambridge Crystallographic Data Centre
DOI: 10.5517/ccdc.csd.cc20rk2f

CCDC 1869675: Experimental Crystal Structure Determination
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Xiaotong, Li,; Justin, Hoffman,; Weijun, Ke,
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DOI: 10.5517/ccdc.csd.cc20rk3g

Hybrid Halide Perovskites: Discussions on Terminology and Materials
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Compositional Control in 2D Perovskites with Alternating Cations in the Interlayer Space for Photovoltaics with Efficiency over 18%
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Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites
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DOI: 10.1002/ange.201910701

Mechanosynthesis, Optical, and Morphological Properties of MA, FA, Cs-SnX ₃ (X = I, Br) and Phase-Pure Mixed-Halide MASnI _x Br ₃ _{- x} Perovskites: Mechanosynthesis, Optical, and Morphological Properties of MA, FA, Cs-SnX ₃ (X = I, Br) and Phase-Pure Mixed-Halide MASnI _x Br ₃ _{- x} Perovskites
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European Journal of Inorganic Chemistry, Vol. 2019, Issue 22
DOI: 10.1002/ejic.201801506

Pure Bromide‐Based Perovskite Nanoplatelets for Blue Light‐Emitting Diodes
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DOI: 10.1002/smtd.201900196

Oriented and Uniform Distribution of Dion–Jacobson Phase Perovskites Controlled by Quantum Well Barrier Thickness
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Zheng, Yiting; Niu, Tingting; Qiu, Jian
Solar RRL, Vol. 3, Issue 9
DOI: 10.1002/solr.201900090

The Role of Diammonium Cation on the Structural and Optoelectronic Properties in 3D Cesium–Formamidinium Mixed‐Cation Perovskite Solar Cells
journal, May 2019

Xu, Xiuwen; Xie, Yue-Min; Ma, Yuhui
Solar RRL, Vol. 3, Issue 8
DOI: 10.1002/solr.201900140

Interlayer Cross‐Linked 2D Perovskite Solar Cell with Uniform Phase Distribution and Increased Exciton Coupling
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Recent advances in controlling the crystallization of two-dimensional perovskites for optoelectronic device
journal, May 2019

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Frontiers of Physics, Vol. 14, Issue 5
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Searching for stability at lower dimensions: current trends and future prospects of layered perovskite solar cells
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Title: Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH3CmH2mNH3)(CH3NH3)n-1PbnI3n+1 (m = 4–9; n = 1–4)

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Citation Formats

CCDC 1869670: Experimental Crystal Structure Determination dataset, January 2018

CCDC 1869671: Experimental Crystal Structure Determination dataset, January 2018

CCDC 1869672: Experimental Crystal Structure Determination dataset, January 2018

CCDC 1869673: Experimental Crystal Structure Determination dataset, January 2018

CCDC 1869674: Experimental Crystal Structure Determination dataset, January 2018

CCDC 1869675: Experimental Crystal Structure Determination dataset, January 2018

Hybrid Halide Perovskites: Discussions on Terminology and Materials journal, October 2019

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Ruddlesden–Popper Perovskites: Synthesis and Optical Properties for Optoelectronic Applications journal, October 2019

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Title: Two-Dimensional Halide Perovskites Incorporating Straight Chain Symmetric Diammonium Ions, (NH₃C_mH_2mNH₃)(CH₃NH₃)_n-1Pb_nI_3n+1 (m = 4–9; n = 1–4)

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dataset, January 2018

CCDC 1869673: Experimental Crystal Structure Determination
dataset, January 2018

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CCDC 1869675: Experimental Crystal Structure Determination
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