Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials

Shin, Donghyeop; Saparov, Bayrammurad; Mitzi, David B.

doi:10.1002/aenm.201602366

Title: Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials

Abstract

Application of zinc‐blende‐related chalcogenide absorbers such as CdTe and Cu(In,Ga)Se ₂ (CIGSe) has enabled remarkable advancement in laboratory‐ and commercial‐scale thin‐film photovoltaic performance; however concerns remain regarding the toxicity (CdTe) and scarcity (CIGSe/CdTe) of the constituent elements. Recently, kesterite‐based Cu ₂ ZnSn(S,Se) ₄ (CZTSSe) materials have emerged as attractive non‐toxic and earth‐abundant absorber candidates. Despite the similarities between CZTSSe and CIGSe/CdTe, the record power conversion efficiency of CZTSSe solar cells (12.6%) remains significantly lower than that of CIGSe (22.6%) and CdTe (22.1%) devices, with the performance gap primarily being attributed to cationic disordering and associated band tailing. To capture the promise of kesterite‐like materials as prospective “drop‐in” earth‐abundant replacements for closely‐related CIGSe, current research has focused on several key directions to control disorder, including: (i) examination of the interaction between processing conditions and atomic site disorder, (ii) isoelectronic cation substitution to introduce ionic size mismatch, and (iii) structural diversification beyond the zinc‐blende‐type coordination environment. In this review, recent efforts targeting accurate identification and engineering of anti‐site disorder in kesterite‐based CZTSSe are considered. Lessons learned from CZTSSe are applied to other complex chalcogenide semiconductors, in an effort to develop promising pathways to avoid anti‐site disordering and associated band tailing in futuremore »« less

Authors:

Shin, Donghyeop ^[1]; Saparov, Bayrammurad ^[1]; Mitzi, David B. ^[1]

Department of Mechanical Engineering and Materials Science Duke University Durham NC 27708 USA, Department of Chemistry Duke University Durham NC 27708 USA

Publication Date:: Fri Jan 13 00:00:00 EST 2017

Sponsoring Org.:: USDOE

OSTI Identifier:: 1400611

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Advanced Energy Materials

Additional Journal Information:: Journal Name: Advanced Energy Materials Journal Volume: 7 Journal Issue: 11; Journal ID: ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Shin, Donghyeop, Saparov, Bayrammurad, and Mitzi, David B. Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials.  Germany: N. p., 2017. 
Web.  doi:10.1002/aenm.201602366.

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                    Shin, Donghyeop, Saparov, Bayrammurad, & Mitzi, David B. Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials.  Germany.  https://doi.org/10.1002/aenm.201602366

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                    Shin, Donghyeop, Saparov, Bayrammurad, and Mitzi, David B. Fri .  
"Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials".  Germany.  https://doi.org/10.1002/aenm.201602366.

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@article{osti_1400611,

  title        = {Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials},

  author       = {Shin, Donghyeop and Saparov, Bayrammurad and Mitzi, David B.},

  abstractNote = {Application of zinc‐blende‐related chalcogenide absorbers such as CdTe and Cu(In,Ga)Se 2 (CIGSe) has enabled remarkable advancement in laboratory‐ and commercial‐scale thin‐film photovoltaic performance; however concerns remain regarding the toxicity (CdTe) and scarcity (CIGSe/CdTe) of the constituent elements. Recently, kesterite‐based Cu 2 ZnSn(S,Se) 4 (CZTSSe) materials have emerged as attractive non‐toxic and earth‐abundant absorber candidates. Despite the similarities between CZTSSe and CIGSe/CdTe, the record power conversion efficiency of CZTSSe solar cells (12.6%) remains significantly lower than that of CIGSe (22.6%) and CdTe (22.1%) devices, with the performance gap primarily being attributed to cationic disordering and associated band tailing. To capture the promise of kesterite‐like materials as prospective “drop‐in” earth‐abundant replacements for closely‐related CIGSe, current research has focused on several key directions to control disorder, including: (i) examination of the interaction between processing conditions and atomic site disorder, (ii) isoelectronic cation substitution to introduce ionic size mismatch, and (iii) structural diversification beyond the zinc‐blende‐type coordination environment. In this review, recent efforts targeting accurate identification and engineering of anti‐site disorder in kesterite‐based CZTSSe are considered. Lessons learned from CZTSSe are applied to other complex chalcogenide semiconductors, in an effort to develop promising pathways to avoid anti‐site disordering and associated band tailing in future high‐performance earth‐abundant photovoltaic technologies.},

  doi          = {10.1002/aenm.201602366},

  journal      = {Advanced Energy Materials},

  number       = 11,

  volume       = 7,

  place        = {Germany},

  year         = {Fri Jan 13 00:00:00 EST 2017},

  month        = {Fri Jan 13 00:00:00 EST 2017}

}

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Crystal Structures of Photovoltaic Chalcogenides, an Intricate Puzzle to Solve: the Cases of CIGSe and CZTS Materials
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Chen, Shiyou; Walsh, Aron; Gong, Xin-Gao
Advanced Materials, Vol. 25, Issue 11
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Gürel, Tanju; Sevik, Cem; Çağın, Tahir
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Photovoltaic Materials and Devices Based on the Alloyed Kesterite Absorber (Ag_xCu_1-_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

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Title: Defect Engineering in Multinary Earth‐Abundant Chalcogenide Photovoltaic Materials

Abstract

Citation Formats

Cu 2 ZnSnSe 4 Thin-Film Solar Cells by Thermal Co-evaporation with 11.6% Efficiency and Improved Minority Carrier Diffusion Length journal, December 2014

Solvothermal synthesis of highly crystallized quaternary chalcogenide Cu2FeSnS4 particles journal, July 2013

Strategies to increase CdTe solar-cell voltage journal, May 2007

Band tail recombination limit to the output voltage of amorphous silicon solar cells journal, April 1982

Crystal and electronic band structure of Cu2ZnSnX4 (X=S and Se) photovoltaic absorbers: First-principles insights journal, January 2009

Solar cell efficiency tables (version 48): Solar cell efficiency tables (version 48) journal, June 2016

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal, September 1976

A Detrimental Reaction at the Molybdenum Back Contact in Cu 2 ZnSn(S,Se) 4 Thin-Film Solar Cells journal, November 2012

Solution Processed Cu 2 CoSnS 4 Thin Films for Photovoltaic Applications journal, July 2014

Earth Abundant Element Cu 2 Zn(Sn 1− x Ge x )S 4 Nanocrystals for Tunable Band Gap Solar Cells: 6.8% Efficient Device Fabrication journal, May 2011

Preparation of the Ag–Zn–Sn–S quaternary photoelectrodes using chemical bath deposition for photoelectrochemical applications journal, May 2014

High-performance photovoltaic perovskite layers fabricated through intramolecular exchange journal, May 2015

Redetermination of the crystal structure of copper(I) tetrathiovanadate (sulvanite), CU3VS4 journal, April 1998

Raman scattering and disorder effect in Cu 2 ZnSnS 4 journal, March 2013

Phase relations in the quasi-binary Cu2GeS3–ZnS and quasi-ternary Cu2S–Zn(Cd)S–GeS2 systems and crystal structure of Cu2ZnGeS4 journal, July 2005

Far infrared studies on stannite and wurtzstannite type compounds journal, January 1991

Synthesis and properties of colloidal Cu2 CdSnS4 nanocrystals: Synthesis and properties of colloidal Cu2 CdSnS4 nanocrystals journal, February 2012

Solution-phase Synthesis of Stannite-type Ag2ZnSnS4 Nanoparticles for Application to Photoelectrode Materials journal, September 2012

Defect physics of the CuInSe 2 chalcopyrite semiconductor journal, April 1998

Anisotropy of the spectroscopy properties of the wurtz-stannite Cu2ZnGeS4 single crystals journal, November 2011

Effects of heavy alkali elements in Cu(In,Ga)Se 2 solar cells with efficiencies up to 22.6% journal, July 2016

Band offsets and optical bowings of chalcopyrites and Zn‐based II‐VI alloys journal, September 1995

Over 9% Efficient Kesterite Cu 2 ZnSnS 4 Solar Cell Fabricated by Using Zn 1- x Cd x S Buffer Layer journal, April 2016

Crystal structures of low- and high-temperature modifications of Cu2CdGeSe4 journal, December 2002

Direct evidence of void passivation in Cu(InGa)(SSe) 2 absorber layers journal, February 2015

The Role of Sodium as a Surfactant and Suppressor of Non-Radiative Recombination at Internal Surfaces in Cu 2 ZnSnS 4 journal, August 2014

Structural, thermodynamical and optical properties of Cu2-II-IV-VI4 quaternary compounds journal, April 2005

A vision for crystalline silicon photovoltaics journal, January 2006

Tetrahedral quaternary chalcogenides of the type Cu2IIIVS4(Se4) journal, May 1974

The Ag2S–ZnS–GeS2 system: Phase diagram, glass-formation region and crystal structure of Ag2ZnGeS4 journal, June 2010

The Long-Wavelength Edge of Photographic Sensitivity and of the Electronic Absorption of Solids journal, December 1953

Status and Potential of CdTe Solar-Cell Efficiency journal, July 2015

Properties of Cu(In,Ga)Se 2 solar cells with new record efficiencies up to 21.7% : Properties of Cu(In,Ga)Se journal, December 2014

Optoelectronic and material properties of nanocrystal-based CZTSe absorbers with Ag-alloying journal, February 2016

Optical constants of Cu2ZnGeS4 bulk crystals journal, November 2010

Can we improve the record efficiency of CdS/CdTe solar cells? journal, September 2006

Generalized Kohn-Sham schemes and the band-gap problem journal, February 1996

Cu 2 Sn 1- x Ge x S 3 ( x = 0.17) Thin-Film Solar Cells with High Conversion Efficiency of 6.0% journal, April 2013

Neutron Diffraction and X-ray Absorption Fine Structure Evidence for Local Lattice Distortions and Aperiodic Antisite Substitution in Cu 2 ZnSnS 4 Nanoparticles journal, October 2014

Cu 2 ZnSnS 4 Thin Film Solar Cells Utilizing Sulfurization of Metallic Precursor Prepared by Simultaneous Sputtering of Metal Targets journal, January 2011

Cu 3 NbS 4 journal, July 2005

Theory of band tails in heavily doped semiconductors journal, July 1992

Bonds, bands, and band gaps in tetrahedrally bonded ternary compounds: The role of group V lone pairs journal, April 2014

Development of CZTS-based thin film solar cells journal, February 2009

In-depth resolved Raman scattering analysis for the identification of secondary phases: Characterization of Cu2ZnSnS4 layers for solar cell applications journal, May 2011

Doping limits in II–VI compounds — Challenges, problems and solutions journal, January 1998

Investigation of combinatorial coevaporated thin film Cu 2 ZnSnS 4 . I. Temperature effect, crystalline phases, morphology, and photoluminescence journal, May 2014

Improvement of voltage deficit of Ge-incorporated kesterite solar cell with 12.3% conversion efficiency journal, September 2016

First-principles calculations for point defects in solids journal, March 2014

Tutorial: Defects in semiconductors—Combining experiment and theory journal, May 2016

Cu2MnMIVS4 (MIV = Si, Ge, Sn) — analysis of crystal structures and tetrahedra volumes of normal tetrahedral compounds journal, January 2005

Effect of post-sulfurization on the composition, structure and optical properties of Cu2ZnSnS4 thin films deposited by sputtering from a single quaternary target journal, January 2013

Photoluminescence characterization of a high-efficiency Cu 2 ZnSnS 4 device journal, October 2013

Disorder and the Optical-Absorption Edge of Hydrogenated Amorphous Silicon journal, November 1981

Synthesis and Characterization of Nanostructured Stannite Cu2ZnSnSe4 and Ag2ZnSnSe4 for Thermoelectric Applications journal, April 2015

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

Cu 2 SnS 3 thin-film solar cells fabricated by sulfurization from NaF/Cu/Sn stacked precursor journal, April 2015

Potential fluctuations in Cu2ZnSnSe4 solar cells studied by temperature dependence of quantum efficiency curves journal, August 2010

From kesterite to stannite photovoltaics: Stability and band gaps of the Cu 2 (Zn,Fe)SnS 4 alloy journal, January 2014

Structural aspects of adamantine like multinary chalcogenides journal, May 2007

Computational Techniques book, April 2013

Why are kesterite solar cells not 20% efficient? journal, May 2013

Temperature dependent band-gap energy for Cu2ZnSnSe4: A spectroscopic ellipsometric study journal, November 2014

Band structures of Cu2ZnSnS4 and Cu2ZnSnSe4 from many-body methods journal, June 2011

Single-crystal structure refinement of enargite [Cu3AsS4] journal, November 1994

Properties and structure of a ‐SiC:H for high‐efficiency a ‐Si solar cell journal, July 1982

Multicomponent tetrahedral compounds for solar cells journal, July 1977

The current status and future prospects of kesterite solar cells: a brief review: Kesterite solar cells journal, January 2016

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

Reversible order-disorder related band gap changes in Cu 2 ZnSn(S,Se) 4 via post-annealing of solar cells measured by electroreflectance journal, December 2014

Absence of Diffusion in Certain Random Lattices journal, March 1958

The crystal structure of kesterite type compounds: A neutron and X-ray diffraction study journal, June 2011

Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag 2 ZnSnSe 4 Absorber journal, August 2016

Solution-Based Preparation of Cu 2 ZnSn(S,Se) 4 for Solar Cells—Comparison of SnSe 2 and Elemental Se as Chalcogen Source journal, March 2015

Plasmons, photoluminescence, and band‐gap narrowing in very heavily doped n ‐GaAs journal, July 1990

Defect physics of the kesterite thin-film solar cell absorber Cu2ZnSnS4 journal, January 2010

Phase equilibria in the Cu2S–ZnS–SnS2 system journal, April 2004

Cu ₂ ZnSnSe ₄ Thin-Film Solar Cells by Thermal Co-evaporation with 11.6% Efficiency and Improved Minority Carrier Diffusion Length
journal, December 2014

Solvothermal synthesis of highly crystallized quaternary chalcogenide Cu2FeSnS4 particles
journal, July 2013

Strategies to increase CdTe solar-cell voltage
journal, May 2007

Band tail recombination limit to the output voltage of amorphous silicon solar cells
journal, April 1982

Crystal and electronic band structure of Cu2ZnSnX4 (X=S and Se) photovoltaic absorbers: First-principles insights
journal, January 2009

Solar cell efficiency tables (version 48): Solar cell efficiency tables (version 48)
journal, June 2016

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

A Detrimental Reaction at the Molybdenum Back Contact in Cu ₂ ZnSn(S,Se) ₄ Thin-Film Solar Cells
journal, November 2012

Solution Processed Cu ₂ CoSnS ₄ Thin Films for Photovoltaic Applications
journal, July 2014

Earth Abundant Element Cu ₂ Zn(Sn _{1− x} Ge _x )S ₄ Nanocrystals for Tunable Band Gap Solar Cells: 6.8% Efficient Device Fabrication
journal, May 2011

Preparation of the Ag–Zn–Sn–S quaternary photoelectrodes using chemical bath deposition for photoelectrochemical applications
journal, May 2014

High-performance photovoltaic perovskite layers fabricated through intramolecular exchange
journal, May 2015

Redetermination of the crystal structure of copper(I) tetrathiovanadate (sulvanite), CU3VS4
journal, April 1998

Raman scattering and disorder effect in Cu ₂ ZnSnS ₄
journal, March 2013

Phase relations in the quasi-binary Cu2GeS3–ZnS and quasi-ternary Cu2S–Zn(Cd)S–GeS2 systems and crystal structure of Cu2ZnGeS4
journal, July 2005

Far infrared studies on stannite and wurtzstannite type compounds
journal, January 1991

Synthesis and properties of colloidal Cu₂ CdSnS₄ nanocrystals: Synthesis and properties of colloidal Cu₂ CdSnS₄ nanocrystals
journal, February 2012

Solution-phase Synthesis of Stannite-type Ag₂ZnSnS₄ Nanoparticles for Application to Photoelectrode Materials
journal, September 2012

Defect physics of the ${CuInSe}_{2}$ chalcopyrite semiconductor
journal, April 1998

Anisotropy of the spectroscopy properties of the wurtz-stannite Cu2ZnGeS4 single crystals
journal, November 2011

Effects of heavy alkali elements in Cu(In,Ga)Se ₂ solar cells with efficiencies up to 22.6%
journal, July 2016

Band offsets and optical bowings of chalcopyrites and Zn‐based II‐VI alloys
journal, September 1995

Over 9% Efficient Kesterite Cu ₂ ZnSnS ₄ Solar Cell Fabricated by Using Zn _1- _x Cd _x S Buffer Layer
journal, April 2016

Crystal structures of low- and high-temperature modifications of Cu2CdGeSe4
journal, December 2002

Direct evidence of void passivation in Cu(InGa)(SSe) ₂ absorber layers
journal, February 2015

The Role of Sodium as a Surfactant and Suppressor of Non-Radiative Recombination at Internal Surfaces in Cu ₂ ZnSnS ₄
journal, August 2014

Structural, thermodynamical and optical properties of Cu2-II-IV-VI4 quaternary compounds
journal, April 2005

A vision for crystalline silicon photovoltaics
journal, January 2006

Tetrahedral quaternary chalcogenides of the type Cu2IIIVS4(Se4)
journal, May 1974

The Ag2S–ZnS–GeS2 system: Phase diagram, glass-formation region and crystal structure of Ag2ZnGeS4
journal, June 2010

The Long-Wavelength Edge of Photographic Sensitivity and of the Electronic Absorption of Solids
journal, December 1953

Status and Potential of CdTe Solar-Cell Efficiency
journal, July 2015

Properties of Cu(In,Ga)Se ₂ solar cells with new record efficiencies up to 21.7% : Properties of Cu(In,Ga)Se
journal, December 2014

Optoelectronic and material properties of nanocrystal-based CZTSe absorbers with Ag-alloying
journal, February 2016

Optical constants of Cu2ZnGeS4 bulk crystals
journal, November 2010

Can we improve the record efficiency of CdS/CdTe solar cells?
journal, September 2006

Generalized Kohn-Sham schemes and the band-gap problem
journal, February 1996

Cu ₂ Sn _{1- x} Ge _x S ₃ ( x = 0.17) Thin-Film Solar Cells with High Conversion Efficiency of 6.0%
journal, April 2013

Neutron Diffraction and X-ray Absorption Fine Structure Evidence for Local Lattice Distortions and Aperiodic Antisite Substitution in Cu ₂ ZnSnS ₄ Nanoparticles
journal, October 2014

Cu ₂ ZnSnS ₄ Thin Film Solar Cells Utilizing Sulfurization of Metallic Precursor Prepared by Simultaneous Sputtering of Metal Targets
journal, January 2011

Cu ₃ NbS ₄
journal, July 2005

Theory of band tails in heavily doped semiconductors
journal, July 1992

Bonds, bands, and band gaps in tetrahedrally bonded ternary compounds: The role of group V lone pairs
journal, April 2014

Development of CZTS-based thin film solar cells
journal, February 2009

In-depth resolved Raman scattering analysis for the identification of secondary phases: Characterization of Cu2ZnSnS4 layers for solar cell applications
journal, May 2011

Doping limits in II–VI compounds — Challenges, problems and solutions
journal, January 1998

Investigation of combinatorial coevaporated thin film Cu ₂ ZnSnS ₄ . I. Temperature effect, crystalline phases, morphology, and photoluminescence
journal, May 2014

Improvement of voltage deficit of Ge-incorporated kesterite solar cell with 12.3% conversion efficiency
journal, September 2016

First-principles calculations for point defects in solids
journal, March 2014

Tutorial: Defects in semiconductors—Combining experiment and theory
journal, May 2016

Cu2MnMIVS4 (MIV = Si, Ge, Sn) — analysis of crystal structures and tetrahedra volumes of normal tetrahedral compounds
journal, January 2005

Effect of post-sulfurization on the composition, structure and optical properties of Cu2ZnSnS4 thin films deposited by sputtering from a single quaternary target
journal, January 2013

Photoluminescence characterization of a high-efficiency Cu ₂ ZnSnS ₄ device
journal, October 2013

Disorder and the Optical-Absorption Edge of Hydrogenated Amorphous Silicon
journal, November 1981

Synthesis and Characterization of Nanostructured Stannite Cu₂ZnSnSe₄ and Ag₂ZnSnSe₄ for Thermoelectric Applications
journal, April 2015

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

Cu ₂ SnS ₃ thin-film solar cells fabricated by sulfurization from NaF/Cu/Sn stacked precursor
journal, April 2015

Potential fluctuations in Cu2ZnSnSe4 solar cells studied by temperature dependence of quantum efficiency curves
journal, August 2010

From kesterite to stannite photovoltaics: Stability and band gaps of the Cu ₂ (Zn,Fe)SnS ₄ alloy
journal, January 2014

Structural aspects of adamantine like multinary chalcogenides
journal, May 2007

Computational Techniques
book, April 2013

Why are kesterite solar cells not 20% efficient?
journal, May 2013

Temperature dependent band-gap energy for Cu2ZnSnSe4: A spectroscopic ellipsometric study
journal, November 2014

Band structures of Cu2ZnSnS4 and Cu2ZnSnSe4 from many-body methods
journal, June 2011

Single-crystal structure refinement of enargite [Cu3AsS4]
journal, November 1994

Properties and structure of a ‐SiC:H for high‐efficiency a ‐Si solar cell
journal, July 1982

Multicomponent tetrahedral compounds for solar cells
journal, July 1977

The current status and future prospects of kesterite solar cells: a brief review: Kesterite solar cells
journal, January 2016

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

Reversible order-disorder related band gap changes in Cu ₂ ZnSn(S,Se) ₄ via post-annealing of solar cells measured by electroreflectance
journal, December 2014

Absence of Diffusion in Certain Random Lattices
journal, March 1958

The crystal structure of kesterite type compounds: A neutron and X-ray diffraction study
journal, June 2011

Photovoltaic Device with over 5% Efficiency Based on an n-Type Ag ₂ ZnSnSe ₄ Absorber
journal, August 2016

Solution-Based Preparation of Cu ₂ ZnSn(S,Se) ₄ for Solar Cells—Comparison of SnSe ₂ and Elemental Se as Chalcogen Source
journal, March 2015

Plasmons, photoluminescence, and band‐gap narrowing in very heavily doped n ‐GaAs
journal, July 1990

Defect physics of the kesterite thin-film solar cell absorber Cu₂ZnSnS₄
journal, January 2010

Phase equilibria in the Cu2S–ZnS–SnS2 system
journal, April 2004

Solvothermal synthesis and tunable bandgap of Cu2(Zn1−xCox)SnS4 and Cu2(Fe1−xCox)SnS4 nanocrystals
journal, October 2015

The crystal structure of Cu ₃ PSe ₄ and other ternary normal tetrahedral structure compounds with composition 1 ₃ 56 ₄
journal, December 1972

Band tails, entropy, and equilibrium defects in hydrogenated amorphous silicon
journal, August 1987