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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

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.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Duke Univ., Durham, NC (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Univ. of Toledo, OH (United States)
Publication Date:
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 = {2019},
month = {12}
}
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https://doi.org/10.1021/acsenergylett.9b02490
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