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Title: Realization of BaZrS3 chalcogenide perovskite thin films for optoelectronics

Abstract

BaZrS3 is a prototypical chalcogenide perovskite, an emerging class of unconventional semiconductor. Recent results on powder samples reveal that it is a material with a direct band gap of 1.7–1.8 eV, a very strong light-matter interaction, and a high chemical stability. Due to the lack of quality thin films, however, many fundamental properties of chalcogenide perovskites remain unknown, hindering their applications in optoelectronics. In this work, we report the fabrication of BaZrS3 thin films, by sulfurization of oxide films deposited by pulsed laser deposition. We show that these films are n-type with carrier densities in the range of 1019-1020 cm-3. Depending on the processing temperature, the Hall mobility ranges from 2.1 to 13.7 cm2/Vs. The absorption coefficient is > 105 cm-1 at photon energy >1.97 eV. Temperature dependent conductivity measurements suggest shallow donor levels. By assuring that BaZrS3 is a promising candidate, these results potentially unleash the family of chalcogenide perovskites for optoelectronics such as photodetectors, photovoltaics, and light emitting diodes.

Authors:
 [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3];  [4];  [1];  [1]; ORCiD logo [5]; ORCiD logo [3];  [1];  [6]; ORCiD logo [1];  [4];  [1];  [7]; ORCiD logo [1]
  1. State Univ. of New York (SUNY), Buffalo, NY (United States)
  2. Taiyuan Normal Univ. (China)
  3. Southern Univ. of Science & Technology, Shenzhen (China)
  4. Xi'an Jiaotong Univ. (China)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Chinese Academy of Sciences (CAS), Shanghai (China)
  7. Rensselaer Polytechnic Inst., Troy, NY (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF); Natural Science Foundation of China (NSFC)
OSTI Identifier:
1648108
Alternate Identifier(s):
OSTI ID: 1694277
Report Number(s):
LA-UR-20-24151
Journal ID: ISSN 2211-2855
Grant/Contract Number:  
89233218CNA000001; CBET-1510121; CBET-1510948; MRI-1229208; EE0007364; 11774365
Resource Type:
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 68; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; material science; chalcogenide perovskite; absorption coefficient; Hall effect; carrier mobility; defects

Citation Formats

Wei, Xiucheng, Hui, Haolei, Zhao, Chuan, Deng, Chenhua, Han, Mengjiao, Yu, Zhonghai, Sheng, Aaron, Roy, Pinku, Chen, Aiping, Lin, Junhao, Watson, David F., Sun, Yi-Yang, Thomay, Tim, Yang, Sen, Jia, Quanxi, Zhang, Shengbai, and Zeng, Hao. Realization of BaZrS3 chalcogenide perovskite thin films for optoelectronics. United States: N. p., 2019. Web. doi:10.1016/j.nanoen.2019.104317.
Wei, Xiucheng, Hui, Haolei, Zhao, Chuan, Deng, Chenhua, Han, Mengjiao, Yu, Zhonghai, Sheng, Aaron, Roy, Pinku, Chen, Aiping, Lin, Junhao, Watson, David F., Sun, Yi-Yang, Thomay, Tim, Yang, Sen, Jia, Quanxi, Zhang, Shengbai, & Zeng, Hao. Realization of BaZrS3 chalcogenide perovskite thin films for optoelectronics. United States. https://doi.org/10.1016/j.nanoen.2019.104317
Wei, Xiucheng, Hui, Haolei, Zhao, Chuan, Deng, Chenhua, Han, Mengjiao, Yu, Zhonghai, Sheng, Aaron, Roy, Pinku, Chen, Aiping, Lin, Junhao, Watson, David F., Sun, Yi-Yang, Thomay, Tim, Yang, Sen, Jia, Quanxi, Zhang, Shengbai, and Zeng, Hao. Fri . "Realization of BaZrS3 chalcogenide perovskite thin films for optoelectronics". United States. https://doi.org/10.1016/j.nanoen.2019.104317. https://www.osti.gov/servlets/purl/1648108.
@article{osti_1648108,
title = {Realization of BaZrS3 chalcogenide perovskite thin films for optoelectronics},
author = {Wei, Xiucheng and Hui, Haolei and Zhao, Chuan and Deng, Chenhua and Han, Mengjiao and Yu, Zhonghai and Sheng, Aaron and Roy, Pinku and Chen, Aiping and Lin, Junhao and Watson, David F. and Sun, Yi-Yang and Thomay, Tim and Yang, Sen and Jia, Quanxi and Zhang, Shengbai and Zeng, Hao},
abstractNote = {BaZrS3 is a prototypical chalcogenide perovskite, an emerging class of unconventional semiconductor. Recent results on powder samples reveal that it is a material with a direct band gap of 1.7–1.8 eV, a very strong light-matter interaction, and a high chemical stability. Due to the lack of quality thin films, however, many fundamental properties of chalcogenide perovskites remain unknown, hindering their applications in optoelectronics. In this work, we report the fabrication of BaZrS3 thin films, by sulfurization of oxide films deposited by pulsed laser deposition. We show that these films are n-type with carrier densities in the range of 1019-1020 cm-3. Depending on the processing temperature, the Hall mobility ranges from 2.1 to 13.7 cm2/Vs. The absorption coefficient is > 105 cm-1 at photon energy >1.97 eV. Temperature dependent conductivity measurements suggest shallow donor levels. By assuring that BaZrS3 is a promising candidate, these results potentially unleash the family of chalcogenide perovskites for optoelectronics such as photodetectors, photovoltaics, and light emitting diodes.},
doi = {10.1016/j.nanoen.2019.104317},
journal = {Nano Energy},
number = ,
volume = 68,
place = {United States},
year = {Fri Nov 22 00:00:00 EST 2019},
month = {Fri Nov 22 00:00:00 EST 2019}
}

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Works referenced in this record:

Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013

  • Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J.
  • Nature, Vol. 501, Issue 7467, p. 395-398
  • DOI: 10.1038/nature12509

Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013

  • Burschka, Julian; Pellet, Norman; Moon, Soo-Jin
  • Nature, Vol. 499, Issue 7458, p. 316-319
  • DOI: 10.1038/nature12340

Long-Range Balanced Electron- and Hole-Transport Lengths in Organic-Inorganic CH3NH3PbI3
journal, October 2013


Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013

  • Stranks, S. D.; Eperon, G. E.; Grancini, G.
  • Science, Vol. 342, Issue 6156, p. 341-344
  • DOI: 10.1126/science.1243982

Compositional engineering of perovskite materials for high-performance solar cells
journal, January 2015

  • Jeon, Nam Joong; Noh, Jun Hong; Yang, Woon Seok
  • Nature, Vol. 517, Issue 7535
  • DOI: 10.1038/nature14133

The light and shade of perovskite solar cells
journal, August 2014


Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals
journal, January 2015


Interface engineering of highly efficient perovskite solar cells
journal, July 2014


Impact of microstructure on local carrier lifetime in perovskite solar cells
journal, April 2015


Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009

  • Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo
  • Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051
  • DOI: 10.1021/ja809598r

Ferroelectricity and Giant Magnetocapacitance in Perovskite Rare-Earth Manganites
journal, June 2004


Multiferroics progress and prospects in thin films
journal, January 2007

  • Ramesh, R.; Spaldin, Nicola A.
  • Nature Materials, Vol. 6, Issue 1, p. 21-29
  • DOI: 10.1038/nmat1805

Multiferroicity: the coupling between magnetic and polarization orders
journal, July 2009


Multiferroics: Different ways to combine magnetism and ferroelectricity
journal, November 2006


Multiferroicity due to charge ordering
journal, October 2008


Untersuchungen �ber tern�re Chalkogenide. XI. Versuche zur Darstellung von Thioperowskiten
journal, January 1957

  • Hahn, Harry; Mutschke, Ursula
  • Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 288, Issue 5-6
  • DOI: 10.1002/zaac.19572880505

Sulphides with the GdFeO 3 structure
journal, October 1980

  • Lelieveld, R.; IJdo, D. J. W.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 36, Issue 10
  • DOI: 10.1107/S056774088000845X

Synthesis of BaZrS3 by short time reaction at lower temperatures
journal, August 2001


Synthesis, structure, and electronic and physical properties of the two SrZrS3 modifications
journal, September 2005


Raman and Infrared Spectra of BaTiS3 and BaNbS3
journal, March 1992


Vibrational spectra of barium-zirconium sulfides
journal, May 1993


Chalcogenide Perovskites for Photovoltaics
journal, December 2014

  • Sun, Yi-Yang; Agiorgousis, Michael L.; Zhang, Peihong
  • Nano Letters, Vol. 15, Issue 1
  • DOI: 10.1021/nl504046x

Bandgap Control via Structural and Chemical Tuning of Transition Metal Perovskite Chalcogenides
journal, December 2016


Chalcogenide perovskites – an emerging class of ionic semiconductors
journal, April 2016


Material Design of Green-Light-Emitting Semiconductors: Perovskite-Type Sulfide SrHfS 3
journal, March 2019

  • Hanzawa, Kota; Iimura, Soshi; Hiramatsu, Hidenori
  • Journal of the American Chemical Society, Vol. 141, Issue 13
  • DOI: 10.1021/jacs.8b13622

Stability and Band-Gap Tuning of the Chalcogenide Perovskite BaZrS 3 in Raman and Optical Investigations at High Pressures
journal, October 2017


Giant optical anisotropy in a quasi-one-dimensional crystal
journal, June 2018


Alloying and Defect Control within Chalcogenide Perovskites for Optimized Photovoltaic Application
journal, January 2016


Insights on the Synthesis, Crystal and Electronic Structures, and Optical and Thermoelectric Properties of Sr 1– x Sb x HfSe 3 Orthorhombic Perovskite
journal, June 2018


Machine Learning Augmented Discovery of Chalcogenide Double Perovskites for Photovoltaics
journal, March 2019

  • L. Agiorgousis, Michael; Sun, Yi‐Yang; Choe, Duk‐Hyun
  • Advanced Theory and Simulations, Vol. 2, Issue 5
  • DOI: 10.1002/adts.201800173

Sulfide perovskites for solar energy conversion applications: computational screening and synthesis of the selected compound LaYS 3
journal, January 2017

  • Kuhar, Korina; Crovetto, Andrea; Pandey, Mohnish
  • Energy & Environmental Science, Vol. 10, Issue 12
  • DOI: 10.1039/C7EE02702H

Oxygen-vacancy ordering as a fatigue mechanism in perovskite ferroelectrics
journal, June 2000

  • Scott, J. F.; Dawber, Matthew
  • Applied Physics Letters, Vol. 76, Issue 25
  • DOI: 10.1063/1.126786

Microscopic study of oxygen-vacancy defects in ferroelectric perovskites
journal, June 1998


CaMnO2.5 and Ca2MnO3.5: New oxygen-defect perovskite-type oxides
journal, August 1982

  • Poeppelmeier, K. R.; Leonowicz, M. E.; Longo, J. M.
  • Journal of Solid State Chemistry, Vol. 44, Issue 1, p. 89-98
  • DOI: 10.1016/0022-4596(82)90404-2

The oxygen defect perovskite BaLa4Cu5O13.4, a metallic conductor
journal, June 1985


Effect of substituting of S for O: The sulfide perovskite BaZrS 3 investigated with density functional theory
journal, June 2009


Protons in Oxysulfides, Oxysulfates, and Sulfides: A First-Principles Study of La 2 O 2 S, La 2 O 2 SO 4 , SrZrS 3 , and BaZrS 3
journal, October 2015

  • Polfus, Jonathan M.; Norby, Truls; Bredesen, Rune
  • The Journal of Physical Chemistry C, Vol. 119, Issue 42
  • DOI: 10.1021/acs.jpcc.5b08278

Charge-Carrier Mobilities in Metal Halide Perovskites: Fundamental Mechanisms and Limits
journal, June 2017


Coulomb gap and low temperature conductivity of disordered systems
journal, February 1975


Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013

  • Burschka, Julian; Pellet, Norman; Moon, Soo-Jin
  • Nature, Vol. 499, Issue 7458, p. 316-319
  • DOI: 10.1038/nature12340

The synthesis and crystal structures of some alkaline earth titanium and zirconium sulfides
journal, February 1963


Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013

  • Stranks, S. D.; Eperon, G. E.; Grancini, G.
  • Science, Vol. 342, Issue 6156, p. 341-344
  • DOI: 10.1126/science.1243982