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Title: Single-Particle Spectroscopy as a Versatile Tool to Explore Lower-Dimensional Structures of Inorganic Perovskites

Abstract

The remarkable defect tolerant nature of inorganic cesium halide perovskites leading to near unity photoluminescence (PL) quantum yield (QY) and narrow emission linewidth across the entire visible spectrum, have provided a tantalizing platform for a development of a plethora of light-emitting applications. Recently, lower dimensional (2D, 1D, and 0D) perovskites have attracted further attention due to the enhanced thermal, photo and chemical stability as compared to their three-dimensional (3D) analogues. Combination of the external size quantization and internal octahedral organization provides a unique opportunity to study and harness “multidimensional” electronic properties engineered both on atomic scale and the nanoscale. However, crucial research to understand the elementary charge carrier dynamics in lower dimensional perovskites lags far behind the enormous effort to incorporate them into optoelectronic devices. In this Perspective, we provide a review of recent developments that focus on studies of the dynamics of excitonic complexes in Cs-based perovskite nanocrystals using single-particle time-resolved PL spectroscopy and photon correlation measurements. Single photon statistical studies not only offer the unprecedented level of detail to directly assess various recombination pathways but also provide insights into specifics of carrier’s localization. Further, we discuss the underlying physicochemical processes that govern PL emission and draw attention tomore » a number of attributes within this class of the materials, especially lower-dimensional perovskites that may indicate the common origin of the PL emission, as well as provide a route map for the vast unexplored territories where single particle spectroscopy can be a powerful tool to unravel crucial information.« less

Authors:
ORCiD logo [1];  [1];  [1];  [2]; ORCiD logo [2];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Texas at Dallas, Richardson, TX (United States)
  2. King Abdullah University of Science and Technology (KAUST), Thuwal (Saudi Arabia)
Publication Date:
Research Org.:
Univ. of Texas at Dallas, Richardson, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1831718
Grant/Contract Number:  
SC0010697
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 10; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Excitons; Nanocomposites; Perovskites; Recombination

Citation Formats

Bose, Riya, Zhou, Xiaohe, Guo, Tianle, Yang, Haoze, Yin, Jun, Mishra, Aditya, Slinker, Jason D., Bakr, Osman M., Mohammed, Omar F., and Malko, Anton V. Single-Particle Spectroscopy as a Versatile Tool to Explore Lower-Dimensional Structures of Inorganic Perovskites. United States: N. p., 2021. Web. doi:10.1021/acsenergylett.1c01604.
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Bose, Riya, Zhou, Xiaohe, Guo, Tianle, Yang, Haoze, Yin, Jun, Mishra, Aditya, Slinker, Jason D., Bakr, Osman M., Mohammed, Omar F., & Malko, Anton V. Single-Particle Spectroscopy as a Versatile Tool to Explore Lower-Dimensional Structures of Inorganic Perovskites. United States. https://doi.org/10.1021/acsenergylett.1c01604
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Bose, Riya, Zhou, Xiaohe, Guo, Tianle, Yang, Haoze, Yin, Jun, Mishra, Aditya, Slinker, Jason D., Bakr, Osman M., Mohammed, Omar F., and Malko, Anton V. Mon . "Single-Particle Spectroscopy as a Versatile Tool to Explore Lower-Dimensional Structures of Inorganic Perovskites". United States. https://doi.org/10.1021/acsenergylett.1c01604. https://www.osti.gov/servlets/purl/1831718.
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@article{osti_1831718,
title = {Single-Particle Spectroscopy as a Versatile Tool to Explore Lower-Dimensional Structures of Inorganic Perovskites},
author = {Bose, Riya and Zhou, Xiaohe and Guo, Tianle and Yang, Haoze and Yin, Jun and Mishra, Aditya and Slinker, Jason D. and Bakr, Osman M. and Mohammed, Omar F. and Malko, Anton V.},
abstractNote = {The remarkable defect tolerant nature of inorganic cesium halide perovskites leading to near unity photoluminescence (PL) quantum yield (QY) and narrow emission linewidth across the entire visible spectrum, have provided a tantalizing platform for a development of a plethora of light-emitting applications. Recently, lower dimensional (2D, 1D, and 0D) perovskites have attracted further attention due to the enhanced thermal, photo and chemical stability as compared to their three-dimensional (3D) analogues. Combination of the external size quantization and internal octahedral organization provides a unique opportunity to study and harness “multidimensional” electronic properties engineered both on atomic scale and the nanoscale. However, crucial research to understand the elementary charge carrier dynamics in lower dimensional perovskites lags far behind the enormous effort to incorporate them into optoelectronic devices. In this Perspective, we provide a review of recent developments that focus on studies of the dynamics of excitonic complexes in Cs-based perovskite nanocrystals using single-particle time-resolved PL spectroscopy and photon correlation measurements. Single photon statistical studies not only offer the unprecedented level of detail to directly assess various recombination pathways but also provide insights into specifics of carrier’s localization. Further, we discuss the underlying physicochemical processes that govern PL emission and draw attention to a number of attributes within this class of the materials, especially lower-dimensional perovskites that may indicate the common origin of the PL emission, as well as provide a route map for the vast unexplored territories where single particle spectroscopy can be a powerful tool to unravel crucial information.},
doi = {10.1021/acsenergylett.1c01604},
journal = {ACS Energy Letters},
number = 10,
volume = 6,
place = {United States},
year = {Mon Sep 27 00:00:00 EDT 2021},
month = {Mon Sep 27 00:00:00 EDT 2021}
}
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journal, July 2016

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Exciton-phonon coupling in a CsPbBr 3 single nanocrystal
journal, February 2018

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Controlling the influence of Auger recombination on the performance of quantum-dot light-emitting diodes
journal, October 2013

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Low‐Dimensional‐Networked Cesium Lead Halide Perovskites: Properties, Fabrication, and Applications
journal, June 2020

Trion Decay in Colloidal Quantum Dots
journal, March 2009

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Zero‐Dimensional Perovskite Nanocrystals for Efficient Luminescent Solar Concentrators
journal, May 2019

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2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications
journal, June 2015

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Dynamics of Charged Excitons and Biexcitons in CsPbBr 3 Perovskite Nanocrystals Revealed by Femtosecond Transient-Absorption and Single-Dot Luminescence Spectroscopy
journal, March 2017

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Memories in the photoluminescence intermittency of single cesium lead bromide nanocrystals
journal, January 2020

Synthesis and Localized Photoluminescence Blinking of Lead‐Free 2D Nanostructures of Cs 3 Bi 2 I 6 Cl 3 Perovskite
journal, July 2020

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2D layered all-inorganic halide perovskites: recent trends in their structure, synthesis and properties
journal, January 2020

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The Benefit and Challenges of Zero-Dimensional Perovskites
journal, June 2018

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Fluorescent Phase-Pure Zero-Dimensional Perovskite-Related Cs 4 PbBr 6 Microdisks: Synthesis and Single-Particle Imaging Study
journal, September 2017

Efficient Generation of Long-Lived Triplet Excitons in 2D Hybrid Perovskite
journal, December 2016

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Intrinsic Lead Ion Emissions in Zero-Dimensional Cs 4 PbBr 6 Nanocrystals
journal, November 2017

Trap States in Lead Iodide Perovskites
journal, January 2015

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Excitons and Biexciton Dynamics in Single CsPbBr 3 Perovskite Quantum Dots
journal, November 2018

Postsynthesis Transformation of Insulating Cs 4 PbBr 6 Nanocrystals into Bright Perovskite CsPbBr 3 through Physical and Chemical Extraction of CsBr
journal, September 2017

Perovskite CsPb 2 Br 5 Microplate Laser with Enhanced Stability and Tunable Properties
journal, November 2016

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Quantum Dot Light-Emitting Diodes Based on Inorganic Perovskite Cesium Lead Halides (CsPbX 3 )
journal, October 2015

Fluorescence Blinking and Photoactivation of All-Inorganic Perovskite Nanocrystals CsPbBr 3 and CsPbBr 2 I
journal, January 2016

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Surface Chemistry of All Inorganic Halide Perovskite Nanocrystals: Passivation Mechanism and Stability
journal, March 2018

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Lasing from Zero-Dimensional Perovskite and Optical Imaging Applications
journal, November 2019

Room Temperature Single-Photon Emission from Individual Perovskite Quantum Dots
journal, September 2015

Highly Emissive Multiexcitons in Steady-State Photoluminescence of Individual “Giant” CdSe/CdS Core/Shell Nanocrystals
journal, July 2010

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Highly Luminescent Cesium Lead Halide Perovskite Nanocrystals with Tunable Composition and Thickness by Ultrasonication
journal, September 2016

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Inorganic Halide Perovskites for Efficient Light-Emitting Diodes
journal, October 2015

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Coherent single-photon emission from colloidal lead halide perovskite quantum dots
journal, February 2019

Superparamagnetism of Green Emissive Cs 4 PbBr 6 Zero-Dimensional Perovskite Crystals
journal, June 2020

Excitation Intensity Dependence of Photoluminescence Blinking in CsPbBr 3 Perovskite Nanocrystals
journal, May 2018

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Mechanistic Investigation of the Defect Activity Contributing to the Photoluminescence Blinking of CsPbBr 3 Perovskite Nanocrystals
journal, November 2019

Efficient Luminescence from CsPbBr 3 Nanoparticles Embedded in Cs 4 PbBr 6
journal, August 2020

Fluorescence intermittency in single cadmium selenide nanocrystals
journal, October 1996

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  • Nature, Vol. 383, Issue 6603
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White-Light Emission from Layered Halide Perovskites
journal, February 2018

Cs 2 PbI 2 Cl 2 , All-Inorganic Two-Dimensional Ruddlesden–Popper Mixed Halide Perovskite with Optoelectronic Response
journal, August 2018

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Highly Emissive Self-Trapped Excitons in Fully Inorganic Zero-Dimensional Tin Halides
journal, July 2018

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Single Nonblinking CdTe Quantum Dots Synthesized in Aqueous Thiopropionic Acid
journal, November 2006

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Bright and Effectual Perovskite Light-Emitting Electrochemical Cells Leveraging Ionic Additives
journal, November 2019

Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure
journal, January 2016

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  • ACS Nano, Vol. 10, Issue 2
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