Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites

Li, Tianyang; Chen, Xihan; Wang, Xiaoming; Lu, Haipeng; Yan, Yanfa; Beard, Matthew C.; Mitzi, David B.

doi:10.1021/acsenergylett.9b02490

Title: Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites

Abstract

Hybrid organic-inorganic lead halide perovskites have shown promising results as active layers in light-emitting diodes, typically utilizing the near-monochromatic, free exciton emission. Some perovskite compounds, however, show broad-band emission that is more intense than the free exciton counterpart. In this study, we show that the light emission properties of Ruddlesden-Popper hybrid perovskites PEA₂MA_n-1Pb_nI_3n+1 (PEA = phenethylammonium, MA = methylammonium) can be tuned by Sn alloying and are highly sensitive to Sn %. With increasing dimensionality, the broad-band emission quantum yield decreases drastically, from 23% in n = 1 to <1% for the n = 3 compound. Using density functional theory calculations and transient reflectance spectroscopy, the broad emission is identified as originating from self-trapped excitons. A dynamic picture of the formation process is also presented, for which ultrafast (<5 ps) hole-trapping at the Sn site is the first step, followed by electron localization from Coulombic interaction. These findings are particularly valuable for designing perovskite materials with intense room-temperature broad-band emission for solid-state lighting applications.

Authors:

Li, Tianyang ^[1];

^[2];

^[3];

^[2];

^[3];

^[2];

^[1]

Duke Univ., Durham, NC (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Toledo, OH (United States)

Publication Date:: Fri Dec 27 00:00:00 EST 2019

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1593084

Report Number(s):: NREL/JA-5900-75462
Journal ID: ISSN 2380-8195

Grant/Contract Number:: AC36-08GO28308

Resource Type:: Accepted Manuscript

Journal Name:: ACS Energy Letters

Additional Journal Information:: Journal Volume: 5; Journal ID: ISSN 2380-8195

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; white light emission; hybrid perovskite; transient reflectance

Citation Formats


                    Li, Tianyang, Chen, Xihan, Wang, Xiaoming, Lu, Haipeng, Yan, Yanfa, Beard, Matthew C., and Mitzi, David B. Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites.  United States: N. p., 2019. 
Web.  doi:10.1021/acsenergylett.9b02490.

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                    Li, Tianyang, Chen, Xihan, Wang, Xiaoming, Lu, Haipeng, Yan, Yanfa, Beard, Matthew C., & Mitzi, David B. Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites.  United States.  https://doi.org/10.1021/acsenergylett.9b02490

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                    Li, Tianyang, Chen, Xihan, Wang, Xiaoming, Lu, Haipeng, Yan, Yanfa, Beard, Matthew C., and Mitzi, David B. Fri .  
"Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites".  United States.  https://doi.org/10.1021/acsenergylett.9b02490.  https://www.osti.gov/servlets/purl/1593084.

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@article{osti_1593084,

  title        = {Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites},

  author       = {Li, Tianyang and Chen, Xihan and Wang, Xiaoming and Lu, Haipeng and Yan, Yanfa and Beard, Matthew C. and Mitzi, David B.},

  abstractNote = {Hybrid organic-inorganic lead halide perovskites have shown promising results as active layers in light-emitting diodes, typically utilizing the near-monochromatic, free exciton emission. Some perovskite compounds, however, show broad-band emission that is more intense than the free exciton counterpart. In this study, we show that the light emission properties of Ruddlesden-Popper hybrid perovskites PEA2MAn-1PbnI3n+1 (PEA = phenethylammonium, MA = methylammonium) can be tuned by Sn alloying and are highly sensitive to Sn %. With increasing dimensionality, the broad-band emission quantum yield decreases drastically, from 23% in n = 1 to <1% for the n = 3 compound. Using density functional theory calculations and transient reflectance spectroscopy, the broad emission is identified as originating from self-trapped excitons. A dynamic picture of the formation process is also presented, for which ultrafast (<5 ps) hole-trapping at the Sn site is the first step, followed by electron localization from Coulombic interaction. These findings are particularly valuable for designing perovskite materials with intense room-temperature broad-band emission for solid-state lighting applications.},

  doi          = {10.1021/acsenergylett.9b02490},

  journal      = {ACS Energy Letters},

  number       = ,

  volume       = 5,

  place        = {United States},

  year         = {Fri Dec 27 00:00:00 EST 2019},

  month        = {Fri Dec 27 00:00:00 EST 2019}

}

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Title: Origin of Broad-Band Emission and Impact of Structural Dimensionality in Tin-Alloyed Ruddlesden–Popper Hybrid Lead Iodide Perovskites

Abstract

Citation Formats

Halide Perovskite Photovoltaics: Background, Status, and Future Prospects journal, March 2019

Synthetic Approaches for Halide Perovskite Thin Films journal, November 2018

Tuning the Luminescence of Layered Halide Perovskites journal, January 2019

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Self-Assembly of Broadband White-Light Emitters journal, January 2014

Intrinsic White-Light Emission from Layered Hybrid Perovskites journal, September 2014

Tunable White-Light Emission in Single-Cation-Templated Three-Layered 2D Perovskites (CH 3 CH 2 NH 3 ) 4 Pb 3 Br 10– x Cl x journal, August 2017

Structural Diversity in White-Light-Emitting Hybrid Lead Bromide Perovskites journal, September 2018

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Atomistic Mechanism of Broadband Emission in Metal Halide Perovskites journal, January 2019

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Isoelectronic Donors and Acceptors journal, August 1966

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Excited states of excitons bound to nitrogen pairs in GaP journal, January 1977

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Selecting between two transition states by which water oxidation intermediates decay on an oxide surface journal, August 2019

Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals journal, August 2018

Halide Perovskite Photovoltaics: Background, Status, and Future Prospects
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Synthetic Approaches for Halide Perovskite Thin Films
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Self-Assembly of Broadband White-Light Emitters
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