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Title: PbI2 Nanocrystal Growth by Atomic Layer Deposition from Pb(tmhd)2 and HI

Abstract

Atomic layer deposition (ALD) allows for fine control over the thickness, stoichiometry, and structural defects of materials. ALD provides a suitable route to deposit lead halides, which can further be converted to perovskites for photovoltaics, photoemission, and photodetection, among other applications. Deposition of lead halides by ALD has already begun to be explored; however, the precursors used in published processes are highly hazardous, require expensive fabrication processes, or contain impurities that can jeopardize the optoelectronic properties of metal halide perovskites after conversion. In this work, we deposited lead iodide (PbI2) by a facile ALD process involving only two readily accessible and low-cost precursors. PbI2 nanocrystals were grown on soda-lime glass (SLG), silicon dioxide support grids, and silicon wafer substrates and provided the groundwork for further investigation into developing lead halide perovskite processes by ALD. Further, the ALD-grown PbI2 was characterized by annular dark-field scanning transmission electron microscopy (ADF-STEM), atomic force microscopy (AFM), high resolution transmission electron microscopy (HRTEM), X-ray fluorescence (XRF), and X-ray photoemission spectroscopy (XPS), among other methods. This work presents the first step to synthesize lead halide perovskites with atomic control for applications such as interfacial layers in photovoltaics and for deposition in microcavities for lasing.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [3];  [3];  [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. Georgia Institute of Technology, Atlanta, GA (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Georgia Tech Graduate Assistance in Areas of National Need (GAANN); USDOD; Micron Foundation; Goizueta Foundation
OSTI Identifier:
1901700
Alternate Identifier(s):
OSTI ID: 1888291
Report Number(s):
BNL-223402-2022-JAAM
Journal ID: ISSN 0897-4756; 173598
Grant/Contract Number:  
AC02-06CH11357; SC0012704; ECCS-1542174
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 34; Journal Issue: 6; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Atomic layer deposition; Deposition; Nanocrystals; Precursors; Thin films

Citation Formats

Vagott, Jacob N., Bairley, Kathryn, Hidalgo, Juanita, Perini, Carlo A. R., Castro-Méndez, Andrés-Felipe, Lombardo, Sarah, Lai, Barry, Zhang, Lihua, Kisslinger, Kim, Kacher, Josh, and Correa-Baena, Juan-Pablo. PbI2 Nanocrystal Growth by Atomic Layer Deposition from Pb(tmhd)2 and HI. United States: N. p., 2022. Web. doi:10.1021/acs.chemmater.1c03093.
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Vagott, Jacob N., Bairley, Kathryn, Hidalgo, Juanita, Perini, Carlo A. R., Castro-Méndez, Andrés-Felipe, Lombardo, Sarah, Lai, Barry, Zhang, Lihua, Kisslinger, Kim, Kacher, Josh, & Correa-Baena, Juan-Pablo. PbI2 Nanocrystal Growth by Atomic Layer Deposition from Pb(tmhd)2 and HI. United States. https://doi.org/10.1021/acs.chemmater.1c03093
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Vagott, Jacob N., Bairley, Kathryn, Hidalgo, Juanita, Perini, Carlo A. R., Castro-Méndez, Andrés-Felipe, Lombardo, Sarah, Lai, Barry, Zhang, Lihua, Kisslinger, Kim, Kacher, Josh, and Correa-Baena, Juan-Pablo. Tue . "PbI2 Nanocrystal Growth by Atomic Layer Deposition from Pb(tmhd)2 and HI". United States. https://doi.org/10.1021/acs.chemmater.1c03093. https://www.osti.gov/servlets/purl/1901700.
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@article{osti_1901700,
title = {PbI2 Nanocrystal Growth by Atomic Layer Deposition from Pb(tmhd)2 and HI},
author = {Vagott, Jacob N. and Bairley, Kathryn and Hidalgo, Juanita and Perini, Carlo A. R. and Castro-Méndez, Andrés-Felipe and Lombardo, Sarah and Lai, Barry and Zhang, Lihua and Kisslinger, Kim and Kacher, Josh and Correa-Baena, Juan-Pablo},
abstractNote = {Atomic layer deposition (ALD) allows for fine control over the thickness, stoichiometry, and structural defects of materials. ALD provides a suitable route to deposit lead halides, which can further be converted to perovskites for photovoltaics, photoemission, and photodetection, among other applications. Deposition of lead halides by ALD has already begun to be explored; however, the precursors used in published processes are highly hazardous, require expensive fabrication processes, or contain impurities that can jeopardize the optoelectronic properties of metal halide perovskites after conversion. In this work, we deposited lead iodide (PbI2) by a facile ALD process involving only two readily accessible and low-cost precursors. PbI2 nanocrystals were grown on soda-lime glass (SLG), silicon dioxide support grids, and silicon wafer substrates and provided the groundwork for further investigation into developing lead halide perovskite processes by ALD. Further, the ALD-grown PbI2 was characterized by annular dark-field scanning transmission electron microscopy (ADF-STEM), atomic force microscopy (AFM), high resolution transmission electron microscopy (HRTEM), X-ray fluorescence (XRF), and X-ray photoemission spectroscopy (XPS), among other methods. This work presents the first step to synthesize lead halide perovskites with atomic control for applications such as interfacial layers in photovoltaics and for deposition in microcavities for lasing.},
doi = {10.1021/acs.chemmater.1c03093},
journal = {Chemistry of Materials},
number = 6,
volume = 34,
place = {United States},
year = {Tue Mar 08 00:00:00 EST 2022},
month = {Tue Mar 08 00:00:00 EST 2022}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acs.chemmater.1c03093
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