DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag2ZnSnSe4 Absorber

Abstract

The kesterite material Cu2ZnSn(S,Se)4 (CZTSSe) is an attractive earth–abundant semiconductor for photovoltaics. However, the power conversion efficiency is limited by a large density of I–II antisite defects, which cause severe band tailing and open–circuit voltage loss. Ag2ZnSnSe4 (AZTSe) is a promising alternative to CZTSSe with a substantially lower I–II antisite defect density and smaller band tailing. AZTSe is weakly n–type, and this study reports for the first time on how the carrier density is impacted by stoichiometry. Here, this study presents the first–ever photovoltaic device based on AZTSe, which exhibits an efficiency of 5.2%, which is the highest value reported for an n–type thin–film absorber. Due to the weakly n–type nature of the absorber, a new architecture is employed (SnO:F/AZTSe/MoO3/ITO) to replace conventional contacts and buffer materials. Using this platform, it is shown that the band tailing parameter in AZTSe more closely resembles that of CIGSe than CZTSSe, underscoring the strong promise of this absorber. In demonstrating the ability to collect photogenerated carriers from AZTSe, this study paves the way for novel thin–film heterojunction architectures where light absorption in the n–type device layer can supplement absorption in the p–type layer as opposed to producing a net optical loss.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [2];  [1]
  1. IBM T J Watson Research Center, Yorktown Heights, NY (United States)
  2. University of California, San Diego, CA (United States)
Publication Date:
Research Org.:
International Business Machines Corp., Armonk, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1533062
Alternate Identifier(s):
OSTI ID: 1401226
Grant/Contract Number:  
EE0006334
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 22; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Chemistry; Energy & Fuels; Materials Science; Physics; AZTSe; Band tailing; CZTSSe; Kesterite; N‐type

Citation Formats

Gershon, Talia, Sardashti, Kasra, Gunawan, Oki, Mankad, Ravin, Singh, Saurabh, Lee, Yun Seog, Ott, John A., Kummel, Andrew, and Haight, Richard. Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag2ZnSnSe4 Absorber. United States: N. p., 2016. Web. doi:10.1002/aenm.201601182.
Gershon, Talia, Sardashti, Kasra, Gunawan, Oki, Mankad, Ravin, Singh, Saurabh, Lee, Yun Seog, Ott, John A., Kummel, Andrew, & Haight, Richard. Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag2ZnSnSe4 Absorber. United States. https://doi.org/10.1002/aenm.201601182
Gershon, Talia, Sardashti, Kasra, Gunawan, Oki, Mankad, Ravin, Singh, Saurabh, Lee, Yun Seog, Ott, John A., Kummel, Andrew, and Haight, Richard. Mon . "Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag2ZnSnSe4 Absorber". United States. https://doi.org/10.1002/aenm.201601182. https://www.osti.gov/servlets/purl/1533062.
@article{osti_1533062,
title = {Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag2ZnSnSe4 Absorber},
author = {Gershon, Talia and Sardashti, Kasra and Gunawan, Oki and Mankad, Ravin and Singh, Saurabh and Lee, Yun Seog and Ott, John A. and Kummel, Andrew and Haight, Richard},
abstractNote = {The kesterite material Cu2ZnSn(S,Se)4 (CZTSSe) is an attractive earth–abundant semiconductor for photovoltaics. However, the power conversion efficiency is limited by a large density of I–II antisite defects, which cause severe band tailing and open–circuit voltage loss. Ag2ZnSnSe4 (AZTSe) is a promising alternative to CZTSSe with a substantially lower I–II antisite defect density and smaller band tailing. AZTSe is weakly n–type, and this study reports for the first time on how the carrier density is impacted by stoichiometry. Here, this study presents the first–ever photovoltaic device based on AZTSe, which exhibits an efficiency of 5.2%, which is the highest value reported for an n–type thin–film absorber. Due to the weakly n–type nature of the absorber, a new architecture is employed (SnO:F/AZTSe/MoO3/ITO) to replace conventional contacts and buffer materials. Using this platform, it is shown that the band tailing parameter in AZTSe more closely resembles that of CIGSe than CZTSSe, underscoring the strong promise of this absorber. In demonstrating the ability to collect photogenerated carriers from AZTSe, this study paves the way for novel thin–film heterojunction architectures where light absorption in the n–type device layer can supplement absorption in the p–type layer as opposed to producing a net optical loss.},
doi = {10.1002/aenm.201601182},
journal = {Advanced Energy Materials},
number = 22,
volume = 6,
place = {United States},
year = {Mon Aug 22 00:00:00 EDT 2016},
month = {Mon Aug 22 00:00:00 EDT 2016}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 89 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

A low-temperature order-disorder transition in Cu 2 ZnSnS 4 thin films
journal, January 2014

  • Scragg, Jonathan J. S.; Choubrac, Léo; Lafond, Alain
  • Applied Physics Letters, Vol. 104, Issue 4
  • DOI: 10.1063/1.4863685

The effect of Mo back contact ageing on Cu(In,Ga)Se 2 thin-film solar cells : Effect of Mo back contact ageing on CIGS solar cells
journal, March 2013

  • Salomé, Pedro M. P.; Fjallstrom, Viktor; Hultqvist, Adam
  • Progress in Photovoltaics: Research and Applications, Vol. 22, Issue 1
  • DOI: 10.1002/pip.2360

What is the bandgap of kesterite?
journal, December 2016


Electronic and elemental properties of the Cu 2 ZnSn(S,Se) 4 surface and grain boundaries
journal, January 2014

  • Haight, Richard; Shao, Xiaoyan; Wang, Wei
  • Applied Physics Letters, Vol. 104, Issue 3
  • DOI: 10.1063/1.4862791

Suns- V OC characteristics of high performance kesterite solar cells
journal, August 2014

  • Gunawan, Oki; Gokmen, Tayfun; Mitzi, David B.
  • Journal of Applied Physics, Vol. 116, Issue 8
  • DOI: 10.1063/1.4893315

Fabrication of Cu2ZnSnS4 films by sulfurization of Cu/ZnSn/Cu precursor layers in sulfur atmosphere for solar cells
journal, December 2011

  • Chalapathy, R. B. V.; Jung, Gwang Sun; Ahn, Byung Tae
  • Solar Energy Materials and Solar Cells, Vol. 95, Issue 12
  • DOI: 10.1016/j.solmat.2011.07.017

Design of I 2 –II–IV–VI 4 Semiconductors through Element Substitution: The Thermodynamic Stability Limit and Chemical Trend
journal, May 2014

  • Wang, Congcong; Chen, Shiyou; Yang, Ji-Hui
  • Chemistry of Materials, Vol. 26, Issue 11
  • DOI: 10.1021/cm500598x

Electronic Structure and Photocatalytic Water-Splitting Properties of Ag 2 ZnSn(S 1– x Se x ) 4
journal, December 2015

  • Jing, Tao; Dai, Ying; Ma, Xiangchao
  • The Journal of Physical Chemistry C, Vol. 119, Issue 50
  • DOI: 10.1021/acs.jpcc.5b09522

Grazing Incidence Cross-Sectioning of Thin-Film Solar Cells via Cryogenic Focused Ion Beam: A Case Study on CIGSe
journal, June 2016

  • Sardashti, Kasra; Haight, Richard; Anderson, Ryan
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 24
  • DOI: 10.1021/acsami.6b04214

Work function of fluorine doped tin oxide
journal, January 2011

  • Helander, M. G.; Greiner, M. T.; Wang, Z. B.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 29, Issue 1
  • DOI: 10.1116/1.3525641

Crystallographic and optical properties of (Cu, Ag)2ZnSnS4 and (Cu, Ag)2ZnSnSe4 solid solutions: Crystallographic and optical properties of (Cu, Ag)
journal, April 2015

  • Gong, Weiyan; Tabata, Takahiro; Takei, Koji
  • physica status solidi (c), Vol. 12, Issue 6, p. 700-703
  • DOI: 10.1002/pssc.201400343

Quantification of surface ZnSe in Cu2ZnSnSe4-based solar cells by analysis of the spectral response
journal, April 2014

  • Colombara, Diego; Robert, Erika Victoria Christiane; Crossay, Alexandre
  • Solar Energy Materials and Solar Cells, Vol. 123
  • DOI: 10.1016/j.solmat.2014.01.015

Work function recovery of air exposed molybdenum oxide thin films
journal, August 2012

  • Irfan, Irfan; James Turinske, Alexander; Bao, Zhenan
  • Applied Physics Letters, Vol. 101, Issue 9
  • DOI: 10.1063/1.4748978

Dye-Sensitized Solar Cells
journal, November 2010

  • Hagfeldt, Anders; Boschloo, Gerrit; Sun, Licheng
  • Chemical Reviews, Vol. 110, Issue 11
  • DOI: 10.1021/cr900356p

Formation of transparent and ohmic ZnO:Al/MoSe2 contacts for bifacial Cu(In,Ga)Se2 solar cells and tandem structures
journal, June 2005


Is the Cu/Zn Disorder the Main Culprit for the Voltage Deficit in Kesterite Solar Cells?
journal, March 2016

  • Bourdais, Stéphane; Choné, Christophe; Delatouche, Bruno
  • Advanced Energy Materials, Vol. 6, Issue 12
  • DOI: 10.1002/aenm.201502276

Work Function and Photothreshold of Layered Metal Dichalcogenides
journal, May 1994

  • Shimada, Toshihiro; Ohuchi, Fumio S.; Parkinson, Bruce A.
  • Japanese Journal of Applied Physics, Vol. 33, Issue Part 1, No. 5A
  • DOI: 10.1143/JJAP.33.2696

Thin‐film CdS/CdTe solar cell with 15.8% efficiency
journal, May 1993

  • Britt, J.; Ferekides, C.
  • Applied Physics Letters, Vol. 62, Issue 22
  • DOI: 10.1063/1.109629

A neutron diffraction study of the stannite-kesterite solid solution series [A neutron diffraction study of the stannite-kesterite solid solution series]
journal, February 2007


A parallel dipole line system
journal, February 2015

  • Gunawan, Oki; Virgus, Yudistira; Tai, Kong Fai
  • Applied Physics Letters, Vol. 106, Issue 6
  • DOI: 10.1063/1.4907931

Engineering Solar Cell Absorbers by Exploring the Band Alignment and Defect Disparity: The Case of Cu- and Ag-Based Kesterite Compounds
journal, October 2015

  • Yuan, Zhen-Kun; Chen, Shiyou; Xiang, Hongjun
  • Advanced Functional Materials, Vol. 25, Issue 43
  • DOI: 10.1002/adfm.201502272

Correlation between intrinsic defects and electrical properties in the high-quality Cu 2 ZnSnS 4 single crystal
journal, September 2013

  • Nagaoka, Akira; Miyake, Hideto; Taniyama, Tomoyasu
  • Applied Physics Letters, Vol. 103, Issue 11
  • DOI: 10.1063/1.4821279

Fabrication and Electronic Properties of CZTSe Single Crystals
journal, January 2015

  • Bishop, Douglas M.; McCandless, Brian E.; Haight, Richard
  • IEEE Journal of Photovoltaics, Vol. 5, Issue 1
  • DOI: 10.1109/JPHOTOV.2014.2363552

Electronically active defects in the Cu 2 ZnSn(Se,S) 4 alloys as revealed by transient photocapacitance spectroscopy
journal, October 2012

  • Miller, D. Westley; Warren, Charles W.; Gunawan, Oki
  • Applied Physics Letters, Vol. 101, Issue 14
  • DOI: 10.1063/1.4754834

MoO3/poly(9,9-dioctylfluorene-co-N-[4-(3-methylpropyl)]-diphenylamine) double-interlayer effect on polymer solar cells
journal, February 2010

  • Subbiah, Jegadesan; Kim, Do Young; Hartel, Michael
  • Applied Physics Letters, Vol. 96, Issue 6
  • DOI: 10.1063/1.3310013

Direct observation of Cu, Zn cation disorder in Cu 2 ZnSnS 4 solar cell absorber material using aberration corrected scanning transmission electron microscopy : Aberration corrected STEM in Cu, Zn cation disorder in CZTS
journal, September 2012

  • Mendis, Budhika G.; Shannon, Mervyn D.; Goodman, Max CJ
  • Progress in Photovoltaics: Research and Applications, Vol. 22, Issue 1
  • DOI: 10.1002/pip.2279

Cation Substitution of Solution-Processed Cu 2 ZnSnS 4 Thin Film Solar Cell with over 9% Efficiency
journal, July 2015

  • Su, Zhenghua; Tan, Joel Ming Rui; Li, Xianglin
  • Advanced Energy Materials, Vol. 5, Issue 19
  • DOI: 10.1002/aenm.201500682

Relationship between Cu 2 ZnSnS 4 quasi donor-acceptor pair density and solar cell efficiency
journal, November 2013

  • Gershon, Talia; Shin, Byungha; Gokmen, Tayfun
  • Applied Physics Letters, Vol. 103, Issue 19
  • DOI: 10.1063/1.4829920

Formation and characterisation of MoSe2 for Cu(In,Ga)Se2 based solar cells
journal, June 2005


The role of Ag in (Ag,Cu)2ZnSnS4 thin film for solar cell application
journal, March 2015


Extended antisite defects in tetrahedrally bonded semiconductors
journal, November 2015


Growth of void free Cu2ZnSnS4 (CZTS) thin films by sulfurization of stacked metallic precursor films
journal, June 2014


Band tailing and efficiency limitation in kesterite solar cells
journal, September 2013

  • Gokmen, Tayfun; Gunawan, Oki; Todorov, Teodor K.
  • Applied Physics Letters, Vol. 103, Issue 10
  • DOI: 10.1063/1.4820250

Classification of Lattice Defects in the Kesterite Cu 2 ZnSnS 4 and Cu 2 ZnSnSe 4 Earth-Abundant Solar Cell Absorbers
journal, February 2013


Fluorine Tin Oxide as an Alternative to Indium Tin Oxide in Polymer LEDs
journal, August 1998


Understanding the relationship between Cu 2 ZnSn(S,Se) 4 material properties and device performance
journal, November 2014

  • Gershon, Talia; Gokmen, Tayfun; Gunawan, Oki
  • MRS Communications, Vol. 4, Issue 4
  • DOI: 10.1557/mrc.2014.34

Beyond 11% Efficiency: Characteristics of State-of-the-Art Cu 2 ZnSn(S,Se) 4 Solar Cells
journal, August 2012

  • Todorov, Teodor K.; Tang, Jiang; Bag, Santanu
  • Advanced Energy Materials, Vol. 3, Issue 1
  • DOI: 10.1002/aenm.201200348

Photovoltaic Materials and Devices Based on the Alloyed Kesterite Absorber (AgxCu1-x)2 ZnSnSe4
journal, March 2016

  • Gershon, Talia; Lee, Yun Seog; Antunez, Priscilla
  • Advanced Energy Materials, Vol. 6, Issue 10, Article No. 1502468
  • DOI: 10.1002/aenm.201502468

Works referencing / citing this record:

Progress and Perspectives of Thin Film Kesterite Photovoltaic Technology: A Critical Review
journal, February 2019

  • Giraldo, Sergio; Jehl, Zacharie; Placidi, Marcel
  • Advanced Materials, Vol. 31, Issue 16
  • DOI: 10.1002/adma.201806692

Cation Substitution in Earth-Abundant Kesterite Photovoltaic Materials
journal, January 2018


Synergistic Effects of Double Cation Substitution in Solution-Processed CZTS Solar Cells with over 10% Efficiency
journal, October 2018

  • Hadke, Shreyash H.; Levcenko, Sergiu; Lie, Stener
  • Advanced Energy Materials, Vol. 8, Issue 32
  • DOI: 10.1002/aenm.201802540

Suppressed Deep Traps and Bandgap Fluctuations in Cu 2 CdSnS 4 Solar Cells with ≈8% Efficiency
journal, October 2019

  • Hadke, Shreyash; Levcenko, Sergiu; Sai Gautam, Gopalakrishnan
  • Advanced Energy Materials, Vol. 9, Issue 45
  • DOI: 10.1002/aenm.201902509

Metal@I 2 –II–IV–VI 4 core–shell nanocrystals: controlled synthesis by aqueous cation exchange for efficient photoelectrochemical hydrogen generation
journal, January 2018

  • Cheng, Xiaoyan; Liu, Jia; Feng, Jingwen
  • Journal of Materials Chemistry A, Vol. 6, Issue 25
  • DOI: 10.1039/c8ta03070g

Wide band gap kesterite absorbers for thin film solar cells: potential and challenges for their deployment in tandem devices
journal, January 2019

  • Vermang, Bart; Brammertz, Guy; Meuris, Marc
  • Sustainable Energy & Fuels, Vol. 3, Issue 9
  • DOI: 10.1039/c9se00266a

Heterovalent Ga 3+ doping in solution-processed Cu 2 ZnSn(S,Se) 4 solar cells for better optoelectronic performance
journal, January 2020

  • Du, Yachao; Tian, Qingwen; Huang, Jin
  • Sustainable Energy & Fuels, Vol. 4, Issue 4
  • DOI: 10.1039/c9se00705a

Analysis of loss mechanisms in Ag 2 ZnSnSe 4 Schottky barrier photovoltaics
journal, May 2017

  • Gershon, Talia; Gunawan, Oki; Gokmen, Tayfun
  • Journal of Applied Physics, Vol. 121, Issue 17
  • DOI: 10.1063/1.4982906

Structural, electrical, and optical properties of Ag 2 ZnSnSe 4 for photodetection application
journal, January 2019

  • Jiang, Yuhong; Yao, Bin; Jia, Jinhuan
  • Journal of Applied Physics, Vol. 125, Issue 2
  • DOI: 10.1063/1.5055895

Emerging inorganic solar cell efficiency tables (Version 1)
journal, July 2019

  • Wong, Lydia H.; Zakutayev, Andriy; Major, Jonathan D.
  • Journal of Physics: Energy, Vol. 1, Issue 3
  • DOI: 10.1088/2515-7655/ab2338

Doping and alloying of kesterites
journal, August 2019

  • Romanyuk, Yaroslav E.; Haass, Stefan G.; Giraldo, Sergio
  • Journal of Physics: Energy, Vol. 1, Issue 4
  • DOI: 10.1088/2515-7655/ab23bc

New Earth-Abundant Thin Film Solar Cells Based on Chalcogenides
journal, April 2019


New Earth-Abundant Thin Film Solar Cells Based on Chalcogenides
journal, April 2019