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Title: Enhanced yield-mobility products in hybrid halide Ruddlesden–Popper compounds with aromatic ammonium spacers

Abstract

We show hybrid halide Ruddlesden–Popper compounds are related to three-dimensional hybrid AMX3 perovskites (e.g. where A is a monovalent cation, M is a divalent metal cation, and X is a halogen) with the general formula L2An–1MnX3n+1 where L is a monovalent spacer cation. The crystal structure comprises perovskite-like layers separated by organic cation spacers. Here two Ruddlesden–Popper compounds with a conjugated cation, 2-(4-biphenyl)ethylammonium (BPEA) prepared by solvothermal and solvent evaporation techniques are reported. The structures of the two compounds: (BPEA)2PbI4 and (BPEA)2(CH3NH3)Pb2I7, were solved by X-ray crystallography. The aromatic rings of the BPEA groups are well-separated in the organic layers leading to optical properties comparable to n = 1 and 2 hybrid halide Ruddlesden–Popper compounds with simpler alkyl ammonium cations. The ambient stability of both compounds over time was also confirmed by powder X-ray diffraction. Finally, the transient photoconductance, measured by time-resolved microwave conductivity, show that the compounds have maximum yield-mobility products respectively of 0.07 cm2 V–1 s–1 and 1.11 cm2 V–1 s–1 for (BPEA)2PbI4 and (BPEA)2(CH3NH3)Pb2I7, both slightly enhanced over what has been measured for compounds with simpler (n-butylammonium) spacer cations.

Authors:
ORCiD logo [1];  [2];  [2];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of California, Santa Barbara, CA (United States). Dept. of Materials
  2. Univ. of California, Santa Barbara, CA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Univ. of California, Santa Barbara, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1594803
Alternate Identifier(s):
OSTI ID: 1560335
Grant/Contract Number:  
SC0012541; DMR-1720256
Resource Type:
Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 48; Journal Issue: 37; Journal ID: ISSN 1477-9226
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Venkatesan, Naveen R., Mahdi, Ali, Barraza, Brian, Wu, Guang, Chabinyc, Michael L., and Seshadri, Ram. Enhanced yield-mobility products in hybrid halide Ruddlesden–Popper compounds with aromatic ammonium spacers. United States: N. p., 2019. Web. doi:10.1039/C9DT03074C.
Venkatesan, Naveen R., Mahdi, Ali, Barraza, Brian, Wu, Guang, Chabinyc, Michael L., & Seshadri, Ram. Enhanced yield-mobility products in hybrid halide Ruddlesden–Popper compounds with aromatic ammonium spacers. United States. doi:10.1039/C9DT03074C.
Venkatesan, Naveen R., Mahdi, Ali, Barraza, Brian, Wu, Guang, Chabinyc, Michael L., and Seshadri, Ram. Thu . "Enhanced yield-mobility products in hybrid halide Ruddlesden–Popper compounds with aromatic ammonium spacers". United States. doi:10.1039/C9DT03074C. https://www.osti.gov/servlets/purl/1594803.
@article{osti_1594803,
title = {Enhanced yield-mobility products in hybrid halide Ruddlesden–Popper compounds with aromatic ammonium spacers},
author = {Venkatesan, Naveen R. and Mahdi, Ali and Barraza, Brian and Wu, Guang and Chabinyc, Michael L. and Seshadri, Ram},
abstractNote = {We show hybrid halide Ruddlesden–Popper compounds are related to three-dimensional hybrid AMX3 perovskites (e.g. where A is a monovalent cation, M is a divalent metal cation, and X is a halogen) with the general formula L2An–1MnX3n+1 where L is a monovalent spacer cation. The crystal structure comprises perovskite-like layers separated by organic cation spacers. Here two Ruddlesden–Popper compounds with a conjugated cation, 2-(4-biphenyl)ethylammonium (BPEA) prepared by solvothermal and solvent evaporation techniques are reported. The structures of the two compounds: (BPEA)2PbI4 and (BPEA)2(CH3NH3)Pb2I7, were solved by X-ray crystallography. The aromatic rings of the BPEA groups are well-separated in the organic layers leading to optical properties comparable to n = 1 and 2 hybrid halide Ruddlesden–Popper compounds with simpler alkyl ammonium cations. The ambient stability of both compounds over time was also confirmed by powder X-ray diffraction. Finally, the transient photoconductance, measured by time-resolved microwave conductivity, show that the compounds have maximum yield-mobility products respectively of 0.07 cm2 V–1 s–1 and 1.11 cm2 V–1 s–1 for (BPEA)2PbI4 and (BPEA)2(CH3NH3)Pb2I7, both slightly enhanced over what has been measured for compounds with simpler (n-butylammonium) spacer cations.},
doi = {10.1039/C9DT03074C},
journal = {Dalton Transactions},
number = 37,
volume = 48,
place = {United States},
year = {2019},
month = {9}
}

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    journal, December 1999

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    • DOI: 10.1021/jz500858a

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    • Tsai, Hsinhan; Nie, Wanyi; Blancon, Jean-Christophe
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    • DOI: 10.1038/nature18306

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    • Mitzi, David B.
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    journal, March 2013


    Phase Stability and Diffusion in Lateral Heterostructures of Methyl Ammonium Lead Halide Perovskites
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    • ACS Applied Materials & Interfaces, Vol. 11, Issue 28
    • DOI: 10.1021/acsami.9b06069

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    journal, January 2016

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    • DOI: 10.1039/c5ee02733k

    Understanding the Role of Cesium and Rubidium Additives in Perovskite Solar Cells: Trap States, Charge Transport, and Recombination
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    • Advanced Energy Materials, Vol. 8, Issue 16
    • DOI: 10.1002/aenm.201703057

    Stability Issues on Perovskite Solar Cells
    journal, November 2015


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    journal, June 2015


    Quantitative analysis of time-resolved microwave conductivity data
    journal, November 2017

    • Reid, Obadiah G.; Moore, David T.; Li, Zhen
    • Journal of Physics D: Applied Physics, Vol. 50, Issue 49
    • DOI: 10.1088/1361-6463/aa9559

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    • DOI: 10.1021/jp406706u

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    journal, May 2016


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    journal, January 2001

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    • IBM Journal of Research and Development, Vol. 45, Issue 1
    • DOI: 10.1147/rd.451.0029

    Characterization of the Valence and Conduction Band Levels of n = 1 2D Perovskites: A Combined Experimental and Theoretical Investigation
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    • DOI: 10.1038/nnano.2016.110

    Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors
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    • Stoumpos, Constantinos C.; Cao, Duyen H.; Clark, Daniel J.
    • Chemistry of Materials, Vol. 28, Issue 8, p. 2852-2867
    • DOI: 10.1021/acs.chemmater.6b00847

    Phase Engineering in Quasi-2D Ruddlesden–Popper Perovskites
    journal, April 2018


    Hybrid Dion–Jacobson 2D Lead Iodide Perovskites
    journal, February 2018

    • Mao, Lingling; Ke, Weijun; Pedesseau, Laurent
    • Journal of the American Chemical Society, Vol. 140, Issue 10
    • DOI: 10.1021/jacs.8b00542

    Vertically Oriented 2D Layered Perovskite Solar Cells with Enhanced Efficiency and Good Stability
    journal, July 2017


    Dimensionality and Interface Engineering of 2D Homologous Perovskites for Boosted Charge-Carrier Transport and Photodetection Performances
    journal, May 2017


    Electrons, Excitons, and Phonons in Two-Dimensional Hybrid Perovskites: Connecting Structural, Optical, and Electronic Properties
    journal, February 2018


    Preparation and characterization of layered lead halide compounds
    journal, March 1991

    • Calabrese, J.; Jones, N. L.; Harlow, R. L.
    • Journal of the American Chemical Society, Vol. 113, Issue 6, p. 2328-2330
    • DOI: 10.1021/ja00006a076

    Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells
    journal, September 2016


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