Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy

Aguiar, Jeffery A.; Erkan, Mehmet E.; Pruzan, Dennis S.; Nagaoka, Akira; Yoshino, Kenji; Moutinho, Helio; Al‐Jassim, Mowafak; Scarpulla, Michael A.

doi:10.1002/pssa.201600060

Title: Cation ratio fluctuations in Cu ₂ ZnSnS ₄ at the 20 nm length scale investigated by analytical electron microscopy

Abstract

Kesterite Cu ₂ ZnSn(S,Se) ₄ (CZTSSe) is a sustainable material for thin‐film photovoltaics with device efficiencies greater than 12% have been demonstrated. Despite similar crystal structure and polycrystalline film microstructures, there is widespread evidence for larger‐amplitude potential and bandgap fluctuations in CZTS than in the analogous Cu(In,Ga)Se ₂ (CIGSe) chalcopyrite material. This disorder is believed to account for a sizable part of the larger open‐circuit voltage ( V _OC ) deficit in CZTS devices, yet the detailed origins and length scales of these fluctuations have not been fully elucidated. Herein, we present a transmission electron microscopy study focusing on composition variation within bulk multicrystals of CZTS grown by the travelling heater method (THM). In these slow‐cooled, solution grown crystals we find direct evidence for spatial composition fluctuations of amplitude <1 at.% (∼5 × 10 ²⁰ cm ⁻³ ) and thus, explainable by point defects. However, rather than being homogeneously‐distributed we find a characteristic 20 nm length scale for these fluctuations, which sets a definite length scale for band gap and potential fluctuations. At Σ3 grain boundaries, we find no evidence of composition variation compared to the bulk. The finding highlights such variations reported at grain boundaries in polycrystalline thin‐films are direct consequences of processingmore »« less

Authors:

Aguiar, Jeffery A. ^[1]; Erkan, Mehmet E. ^[2]; Pruzan, Dennis S. ^[3]; Nagaoka, Akira ^[4]; Yoshino, Kenji ^[5]; Moutinho, Helio ^[1]; Al‐Jassim, Mowafak ^[1]; Scarpulla, Michael A. ^[6]

National Renewable Energy Laboratory Golden CO 80401 USA
Department of Electrical and Computer Engineering University of Utah UT 84112 USA
Department of Materials Science and Engineering University of Utah UT 84112 USA
Department of Materials Science and Engineering University of Utah UT 84112 USA, Department of Applied Physics and Electronic Engineering University of Miyazaki Miyazaki 889 2192 Japan
Department of Applied Physics and Electronic Engineering University of Miyazaki Miyazaki 889 2192 Japan
Department of Electrical and Computer Engineering University of Utah UT 84112 USA, Department of Materials Science and Engineering University of Utah UT 84112 USA

Publication Date:: Tue Apr 05 00:00:00 EDT 2016

Sponsoring Org.:: USDOE

OSTI Identifier:: 1400554

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Physica Status Solidi. A, Applications and Materials Science

Additional Journal Information:: Journal Name: Physica Status Solidi. A, Applications and Materials Science Journal Volume: 213 Journal Issue: 9; Journal ID: ISSN 1862-6300

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Aguiar, Jeffery A., Erkan, Mehmet E., Pruzan, Dennis S., Nagaoka, Akira, Yoshino, Kenji, Moutinho, Helio, Al‐Jassim, Mowafak, and Scarpulla, Michael A. Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy.  Germany: N. p., 2016. 
Web.  doi:10.1002/pssa.201600060.

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                    Aguiar, Jeffery A., Erkan, Mehmet E., Pruzan, Dennis S., Nagaoka, Akira, Yoshino, Kenji, Moutinho, Helio, Al‐Jassim, Mowafak, & Scarpulla, Michael A. Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy.  Germany.  https://doi.org/10.1002/pssa.201600060

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                    Aguiar, Jeffery A., Erkan, Mehmet E., Pruzan, Dennis S., Nagaoka, Akira, Yoshino, Kenji, Moutinho, Helio, Al‐Jassim, Mowafak, and Scarpulla, Michael A. Tue .  
"Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy".  Germany.  https://doi.org/10.1002/pssa.201600060.

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@article{osti_1400554,

  title        = {Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy},

  author       = {Aguiar, Jeffery A. and Erkan, Mehmet E. and Pruzan, Dennis S. and Nagaoka, Akira and Yoshino, Kenji and Moutinho, Helio and Al‐Jassim, Mowafak and Scarpulla, Michael A.},

  abstractNote = {Kesterite Cu 2 ZnSn(S,Se) 4 (CZTSSe) is a sustainable material for thin‐film photovoltaics with device efficiencies greater than 12% have been demonstrated. Despite similar crystal structure and polycrystalline film microstructures, there is widespread evidence for larger‐amplitude potential and bandgap fluctuations in CZTS than in the analogous Cu(In,Ga)Se 2 (CIGSe) chalcopyrite material. This disorder is believed to account for a sizable part of the larger open‐circuit voltage ( V OC ) deficit in CZTS devices, yet the detailed origins and length scales of these fluctuations have not been fully elucidated. Herein, we present a transmission electron microscopy study focusing on composition variation within bulk multicrystals of CZTS grown by the travelling heater method (THM). In these slow‐cooled, solution grown crystals we find direct evidence for spatial composition fluctuations of amplitude <1 at.% (∼5 × 10 20  cm −3 ) and thus, explainable by point defects. However, rather than being homogeneously‐distributed we find a characteristic 20 nm length scale for these fluctuations, which sets a definite length scale for band gap and potential fluctuations. At Σ3 grain boundaries, we find no evidence of composition variation compared to the bulk. The finding highlights such variations reported at grain boundaries in polycrystalline thin‐films are direct consequences of processing methods and not intrinsic properties of CZTS itself.},

  doi          = {10.1002/pssa.201600060},

  journal      = {Physica Status Solidi. A, Applications and Materials Science},

  number       = 9,

  volume       = 213,

  place        = {Germany},

  year         = {Tue Apr 05 00:00:00 EDT 2016},

  month        = {Tue Apr 05 00:00:00 EDT 2016}

}

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Title: Cation ratio fluctuations in Cu 2 ZnSnS 4 at the 20 nm length scale investigated by analytical electron microscopy

Abstract

Citation Formats

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

Electrically Benign Behavior of Grain Boundaries in Polycrystalline CuInSe 2 Films journal, December 2007

Transmission Electron Microscopy book, January 2009

How grain boundaries in Cu(In,Ga)Se 2 thin films are charged: Revisit journal, July 2012

Enhanced Conversion Efficiencies of Cu 2 ZnSnS 4 -Based Thin Film Solar Cells by Using Preferential Etching Technique journal, April 2008

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Structural and elemental characterization of high efficiency Cu2ZnSnS4 solar cells journal, January 2011

Thermally evaporated Cu2ZnSnS4 solar cells journal, October 2010

New world record efficiency for Cu(In,Ga)Se2 thin-film solar cells beyond 20% journal, January 2011

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

Growth of Cu2ZnSnS4 Single Crystal by Traveling Heater Method journal, November 2011

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

Contrasting the Material Chemistry of Cu 2 ZnSnSe 4 and Cu 2 ZnSnS (4- x ) Se x journal, February 2016

Evidence for a Neutral Grain-Boundary Barrier in Chalcopyrites journal, October 2006

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

Synthesis of Cu 2 ZnSnS 4 Nanocrystal Ink and Its Use for Solar Cells journal, August 2009

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

Effects of sodium on electrical properties in Cu 2 ZnSnS 4 single crystal journal, April 2014

Grain boundary segregation in Fe–Mn–C twinning-induced plasticity steels studied by correlative electron backscatter diffraction and atom probe tomography journal, January 2015

Multiwavelength excitation Raman scattering study of polycrystalline kesterite Cu 2 ZnSnS 4 thin films journal, January 2014

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Device characteristics of a 10.1% hydrazine-processed Cu2ZnSn(Se,S)4 solar cell: Characteristics of a 10.1% efficient kesterite solar cell journal, September 2011

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Symmetry-dependence of electronic grain boundary properties in polycrystalline CuInSe 2 thin films journal, October 2011

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Chemical etching of Cu2ZnSn(S,Se)4 monograin powder conference, June 2010

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High-resolution work function imaging of single grains of semiconductor surfaces journal, April 2002

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Entropy-Driven Clustering in Tetrahedrally Bonded Multinary Materials journal, March 2015

Thermodynamic Aspects of the Synthesis of Thin-Film Materials for Solar Cells journal, April 2012

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Title: Cation ratio fluctuations in Cu ₂ ZnSnS ₄ at the 20 nm length scale investigated by analytical electron microscopy

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

Electrically Benign Behavior of Grain Boundaries in Polycrystalline ${CuInSe}_{2}$ Films
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Transmission Electron Microscopy
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How grain boundaries in Cu(In,Ga)Se ₂ thin films are charged: Revisit
journal, July 2012

Enhanced Conversion Efficiencies of Cu ₂ ZnSnS ₄ -Based Thin Film Solar Cells by Using Preferential Etching Technique
journal, April 2008

Engineering Grain Boundaries in Cu ₂ ZnSnSe ₄ for Better Cell Performance: A First-Principle Study
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journal, January 2011

Thermally evaporated Cu2ZnSnS4 solar cells
journal, October 2010

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journal, January 2011

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

Development of CZTS-based thin film solar cells
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journal, February 2016

Evidence for a Neutral Grain-Boundary Barrier in Chalcopyrites
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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

Synthesis of Cu ₂ ZnSnS ₄ Nanocrystal Ink and Its Use for Solar Cells
journal, August 2009

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

Effects of sodium on electrical properties in Cu ₂ ZnSnS ₄ single crystal
journal, April 2014

Grain boundary segregation in Fe–Mn–C twinning-induced plasticity steels studied by correlative electron backscatter diffraction and atom probe tomography
journal, January 2015

Multiwavelength excitation Raman scattering study of polycrystalline kesterite Cu ₂ ZnSnS ₄ thin films
journal, January 2014

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

Epitaxial growth of CZTS on Si substrates investigated with electron backscatter diffraction
conference, June 2014

Device characteristics of a 10.1% hydrazine-processed Cu2ZnSn(Se,S)4 solar cell: Characteristics of a 10.1% efficient kesterite solar cell
journal, September 2011

Preparation of Cu2ZnSnS4 single crystals from Sn solutions
journal, February 2012

Chemical Insights into the Instability of Cu ₂ ZnSnS ₄ Films during Annealing
journal, October 2011

Interplay between surface preparation and device performance in CZTSSe solar cells: Effects of KCN and NH4OH etching
journal, May 2015

Symmetry-dependence of electronic grain boundary properties in polycrystalline CuInSe ₂ thin films
journal, October 2011

Growth of Cu2ZnSnSe4 single crystals from Sn solutions
journal, September 2012

Chemical etching of Cu2ZnSn(S,Se)4 monograin powder
conference, June 2010

Strategic review of secondary phases, defects and defect-complexes in kesterite CZTS–Se solar cells
journal, January 2015

Kesterites-a challenging material for solar cells: Kesterites-a challenging material for solar cells
journal, February 2012

High-resolution work function imaging of single grains of semiconductor surfaces
journal, April 2002

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

Entropy-Driven Clustering in Tetrahedrally Bonded Multinary Materials
journal, March 2015

Thermodynamic Aspects of the Synthesis of Thin-Film Materials for Solar Cells
journal, April 2012

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

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

Defect formation and phase stability of ${Cu}_{2} {ZnSnS}_{4}$ photovoltaic material
journal, March 2010

Growth and Raman scattering characterization of Cu2ZnSnS4 thin films
journal, February 2009

The path towards a high-performance solution-processed kesterite solar cell
journal, June 2011

Cu-Zn disorder and band gap fluctuations in Cu ₂ ZnSn(S,Se) ₄ : Theoretical and experimental investigations (Phys. Status Solidi B 2/2016)
journal, February 2016