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Title: Existence of a Size-Dependent Stokes Shift in CsPbBr 3 Perovskite Nanocrystals

Abstract

The existence of a size-dependent Stokes shift is observed in CsPbBr 3 perovskite nanocrystals for the first time. Stokes shifts range from ~100 to 30 meV for particles with edge lengths between ~4 and 12 nm, respectively.

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Univ. of Notre Dame, Notre Dame, IN (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Univ. of Notre Dame, IN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1364180
Alternate Identifier(s):
OSTI ID: 1425740
Grant/Contract Number:
SC0014334
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 2; Journal Issue: 7; Journal ID: ISSN 2380-8195
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

Brennan, Michael C., Zinna, Jessica, and Kuno, Masaru. Existence of a Size-Dependent Stokes Shift in CsPbBr3 Perovskite Nanocrystals. United States: N. p., 2017. Web. doi:10.1021/acsenergylett.7b00383.
Brennan, Michael C., Zinna, Jessica, & Kuno, Masaru. Existence of a Size-Dependent Stokes Shift in CsPbBr3 Perovskite Nanocrystals. United States. doi:10.1021/acsenergylett.7b00383.
Brennan, Michael C., Zinna, Jessica, and Kuno, Masaru. Wed . "Existence of a Size-Dependent Stokes Shift in CsPbBr3 Perovskite Nanocrystals". United States. doi:10.1021/acsenergylett.7b00383.
@article{osti_1364180,
title = {Existence of a Size-Dependent Stokes Shift in CsPbBr3 Perovskite Nanocrystals},
author = {Brennan, Michael C. and Zinna, Jessica and Kuno, Masaru},
abstractNote = {The existence of a size-dependent Stokes shift is observed in CsPbBr3 perovskite nanocrystals for the first time. Stokes shifts range from ~100 to 30 meV for particles with edge lengths between ~4 and 12 nm, respectively.},
doi = {10.1021/acsenergylett.7b00383},
journal = {ACS Energy Letters},
number = 7,
volume = 2,
place = {United States},
year = {Wed May 31 00:00:00 EDT 2017},
month = {Wed May 31 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acsenergylett.7b00383

Citation Metrics:
Cited by: 9works
Citation information provided by
Web of Science

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  • The existence of a size-dependent Stokes shift is observed in CsPbBr 3 perovskite nanocrystals for the first time. Stokes shifts range from ~100 to 30 meV for particles with edge lengths between ~4 and 12 nm, respectively.
  • A selective growth of gold (Au) nanoparticles on the corners of CsPbBr 3 nanocrystals (NCs) is made possible with the treatment of Au(III) salts such as Au(III) bromide and Au(III) chloride in solution. The surface bound oleylamine ligands not only stabilize NCs but also facilitate reduction of the Au(III) salts followed by nucleation of the Au nanoparticles on the corners of the perovskite NCs. The luminescence quantum yield of NCs is decreased when Au nanoparticles are formed on the corners of CsPbBr 3 NCs, suggesting interaction between the two systems. Formation of Au nanoparticles as well as an anion exchangemore » is seen when Au(III) bromide was replaced with Au(III) chloride as a precursor. This simple strategy of designing perovskite-gold hybrid nanostructures with good colloidal stability offers new opportunities to explore their photocatalytic properties.« less
  • A selective growth of gold (Au) nanoparticles on the corners of CsPbBr 3 nanocrystals (NCs) is made possible with the treatment of Au(III) salts such as Au(III) bromide and Au(III) chloride in solution. The surface bound oleylamine ligands not only stabilize NCs but also facilitate reduction of the Au(III) salts followed by nucleation of the Au nanoparticles on the corners of the perovskite NCs. The luminescence quantum yield of NCs is decreased when Au nanoparticles are formed on the corners of CsPbBr 3 NCs, suggesting interaction between the two systems. Formation of Au nanoparticles as well as an anion exchangemore » is seen when Au(III) bromide was replaced with Au(III) chloride as a precursor. This simple strategy of designing perovskite-gold hybrid nanostructures with good colloidal stability offers new opportunities to explore their photocatalytic properties.« less
  • All-inorganic cesium lead halide (CsPbX 3, X = Br , I ) perovskites could potentially provide comparable photovoltaic performance with enhanced stability compared to organic–inorganic lead halide species. However, small-bandgap cubic CsPbI3 has been difficult to study due to challenges forming CsPbI 3 in the cubic phase. Here, a low-temperature procedure to form cubic CsPbI 3 has been developed through a halide exchange reaction using films of sintered CsPbBr 3 nanocrystals. The reaction was found to be strongly dependent upon temperature, featuring an Arrhenius relationship. Additionally, film thickness played a significant role in determining internal film structure at intermediate reactionmore » times. Thin films (50 nm) showed only a small distribution of CsPbBr xI 3–x species, while thicker films (350 nm) exhibited much broader distributions. Furthermore, internal film structure was ordered, featuring a compositional gradient within film. Transient absorption spectroscopy showed the influence of halide exchange on the excited state of the material. In thicker films, charge carriers were rapidly transferred to iodide-rich regions near the film surface within the first several picoseconds after excitation. Furthermore, this ultrafast vectorial charge-transfer process illustrates the potential of utilizing compositional gradients to direct charge flow in perovskite-based photovoltaics.« less
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  • All-inorganic cesium lead halide (CsPbX 3, X = Br , I ) perovskites could potentially provide comparable photovoltaic performance with enhanced stability compared to organic–inorganic lead halide species. However, small-bandgap cubic CsPbI3 has been difficult to study due to challenges forming CsPbI 3 in the cubic phase. Here, a low-temperature procedure to form cubic CsPbI 3 has been developed through a halide exchange reaction using films of sintered CsPbBr 3 nanocrystals. The reaction was found to be strongly dependent upon temperature, featuring an Arrhenius relationship. Additionally, film thickness played a significant role in determining internal film structure at intermediate reactionmore » times. Thin films (50 nm) showed only a small distribution of CsPbBr xI 3–x species, while thicker films (350 nm) exhibited much broader distributions. Furthermore, internal film structure was ordered, featuring a compositional gradient within film. Transient absorption spectroscopy showed the influence of halide exchange on the excited state of the material. In thicker films, charge carriers were rapidly transferred to iodide-rich regions near the film surface within the first several picoseconds after excitation. Furthermore, this ultrafast vectorial charge-transfer process illustrates the potential of utilizing compositional gradients to direct charge flow in perovskite-based photovoltaics.« less