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Title: Highly Efficient Broad-Band Luminescence Involving Organic and Inorganic Molecules in a Zero-Dimensional Hybrid Lead Chloride

Abstract

The photophysical mechanism of ultrabright visible light emission in the zero-dimensional (0D) hybrid organic–inorganic material (HOIM), (DETA)PbCl5·H2O (DETA = diethylenetriammonium), has been studied. This compound exhibits efficient room-temperature bluish white-light (WL) emission, corroborated by a high photoluminescence quantum yield (PLQY) value of 36.8 % and a Commission Internationale de l’Eclairage (CIE) color coordinates of (0.18, 0.17). Optical investigations reveal that broad-band emission containing multiple emission centers originates from both the fluorescence of the organic molecules DETA and self-trapped excitons within the [Pb2Cl10]6– inorganic bioctahedral dimers. Furthermore, an enhanced PLQY of up to 40.3% with an adjusted pure WL emission (CIE of (0.33, 0.34)) and a remarkable color rendering index of 90 was achieved through the incorporation of Mn2+ within (DETA)PbCl5·H2O. Our findings aid in understanding the photophysical properties of 0D HOIMs and preparation of new families of highly emissive materials for solid-state lighting applications.

Authors:
 [1];  [1];  [2]; ORCiD logo [3];  [1]
  1. Univ. of Oklahoma, Norman, OK (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States). Scintillation Materials Research Center
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1566979
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 36; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Low-dimensional halides; hybrid organic-inorganic halides; Broadband emission; Excitons; DFT calculations; Mn doping

Citation Formats

Yangui, Aymen, Roccanova, Rachel, Wu, Yuntao, Du, Mao-Hua, and Saparov, Bayrammurad. Highly Efficient Broad-Band Luminescence Involving Organic and Inorganic Molecules in a Zero-Dimensional Hybrid Lead Chloride. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.9b05509.
Yangui, Aymen, Roccanova, Rachel, Wu, Yuntao, Du, Mao-Hua, & Saparov, Bayrammurad. Highly Efficient Broad-Band Luminescence Involving Organic and Inorganic Molecules in a Zero-Dimensional Hybrid Lead Chloride. United States. https://doi.org/10.1021/acs.jpcc.9b05509
Yangui, Aymen, Roccanova, Rachel, Wu, Yuntao, Du, Mao-Hua, and Saparov, Bayrammurad. 2019. "Highly Efficient Broad-Band Luminescence Involving Organic and Inorganic Molecules in a Zero-Dimensional Hybrid Lead Chloride". United States. https://doi.org/10.1021/acs.jpcc.9b05509. https://www.osti.gov/servlets/purl/1566979.
@article{osti_1566979,
title = {Highly Efficient Broad-Band Luminescence Involving Organic and Inorganic Molecules in a Zero-Dimensional Hybrid Lead Chloride},
author = {Yangui, Aymen and Roccanova, Rachel and Wu, Yuntao and Du, Mao-Hua and Saparov, Bayrammurad},
abstractNote = {The photophysical mechanism of ultrabright visible light emission in the zero-dimensional (0D) hybrid organic–inorganic material (HOIM), (DETA)PbCl5·H2O (DETA = diethylenetriammonium), has been studied. This compound exhibits efficient room-temperature bluish white-light (WL) emission, corroborated by a high photoluminescence quantum yield (PLQY) value of 36.8 % and a Commission Internationale de l’Eclairage (CIE) color coordinates of (0.18, 0.17). Optical investigations reveal that broad-band emission containing multiple emission centers originates from both the fluorescence of the organic molecules DETA and self-trapped excitons within the [Pb2Cl10]6– inorganic bioctahedral dimers. Furthermore, an enhanced PLQY of up to 40.3% with an adjusted pure WL emission (CIE of (0.33, 0.34)) and a remarkable color rendering index of 90 was achieved through the incorporation of Mn2+ within (DETA)PbCl5·H2O. Our findings aid in understanding the photophysical properties of 0D HOIMs and preparation of new families of highly emissive materials for solid-state lighting applications.},
doi = {10.1021/acs.jpcc.9b05509},
url = {https://www.osti.gov/biblio/1566979}, journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 36,
volume = 123,
place = {United States},
year = {Tue Aug 13 00:00:00 EDT 2019},
month = {Tue Aug 13 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 42 works
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Figures / Tables:

Figure 1 Figure 1: Optical microscope images of as-prepared single crystal of (DETA)PbCl5.H2O under (a) ambient light and (b) 325 nm UV irradiation, showing the bright bluish-WL emission at room temperature. (c) Projection of crystal structure of (DETA)PbCl5.H2O along the crystallographic a-axis. Yellow, pink, blue, black, blue, turquoise and grey spheres representmore » Pb, Cl, C, N, O, and H atoms, respectively. The edge sharing [Pb2Cl10]6- bioctahedra are emphasized in green.« less

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Works referencing / citing this record:

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Additive-assisted synthesis and optoelectronic properties of (CH 3 NH 3 ) 4 Bi 6 I 22
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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.