Surface and bulk effects of K in Cu1-xKxIn1-yGaySe2 solar cells

Muzzillo, Christopher P.; Anderson, Timothy J.

doi:10.1016/j.solmat.2017.12.038

Title: Surface and bulk effects of K in Cu_1-xK_xIn_1-yGa_ySe₂ solar cells

Abstract

Two strategies for enhancing photovoltaic (PV) performance in chalcopyrite solar cells were investigated: Cu_1-xK_xIn_1-yGa_ySe₂ absorbers with low K content (K/(K+Cu), or x ~ 0.07) distributed throughout the bulk, and CuIn_1-yGa_ySe₂ absorbers with KIn_1-yGa_ySe₂ grown on their surfaces. Distributing K throughout the bulk absorbers improved power conversion efficiency, open-circuit voltage (VOC) and fill factor (FF) for Ga/(Ga+In) of 0, 0.3 and 0.5. Surface KIn_1-yGa_ySe₂ and bulk x ~ 0.07 Cu_1-xK_xIn_1-yGa_ySe₂ films with Ga/(Ga+In), or y of 0.3 and 0.5 also had improved efficiency, VOC, and FF, relative to CuIn_1-yGa_ySe₂ baselines. On the other hand, y ~ 1 absorbers did not benefit from K introduction. Similar to Cu_1-xK_xInSe₂, the formation of Cu_1-xK_xGaSe₂ alloys was favored at low temperatures and high Na supply by the substrate, relative to the formation of mixed-phase CuGaSe₂ + KGaSe₂. KIn_1-yGa_ySe₂ alloys were grown for the first time, as evidenced by X-ray diffraction and ultraviolet/visible spectroscopy. For all Ga/(Ga+In) compositions, the surface KIn_1-yGa_ySe₂ absorbers had superior PV performance in buffered and buffer-free devices. However, the bulk x ~ 0.07 absorbers only outperformed the baselines in buffered devices. The data demonstrate that KIn_1-yGa_ySe₂ passivates the surface of CuIn_1-yGa_ySe₂ to increase efficiency, VOC, and FF, while bulk Cu_1-xK_xIn_1-yGa_ySe₂ absorbers withmore »« less

Authors:

Muzzillo, Christopher P. ^[1]; Anderson, Timothy J. ^[2]

Univ. of Florida, Gainesville, FL (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Univ. of Florida, Gainesville, FL (United States)

Publication Date:: Fri Dec 29 00:00:00 EST 2017

Research Org.:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

OSTI Identifier:: 1417137

Alternate Identifier(s):: OSTI ID: 1548886

Report Number(s):: NREL/JA-5K00-70736
Journal ID: ISSN 0927-0248

Grant/Contract Number:: AC36-08GO28308

Resource Type:: Accepted Manuscript

Journal Name:: Solar Energy Materials and Solar Cells

Additional Journal Information:: Journal Volume: 179; Journal Issue: C; Journal ID: ISSN 0927-0248

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; Cu(In,Ga)Se2; chalcopyrite; potassium; passivation; (Cu,K)GaSe2; K(In,Ga)Se2

Citation Formats


                    Muzzillo, Christopher P., and Anderson, Timothy J. Surface and bulk effects of K in Cu1-xKxIn1-yGaySe2 solar cells.  United States: N. p., 2017. 
Web.  doi:10.1016/j.solmat.2017.12.038.

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                    Muzzillo, Christopher P., & Anderson, Timothy J. Surface and bulk effects of K in Cu1-xKxIn1-yGaySe2 solar cells.  United States.  https://doi.org/10.1016/j.solmat.2017.12.038

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                    Muzzillo, Christopher P., and Anderson, Timothy J. Fri .  
"Surface and bulk effects of K in Cu1-xKxIn1-yGaySe2 solar cells".  United States.  https://doi.org/10.1016/j.solmat.2017.12.038.  https://www.osti.gov/servlets/purl/1417137.

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@article{osti_1417137,

  title        = {Surface and bulk effects of K in Cu1-xKxIn1-yGaySe2 solar cells},

  author       = {Muzzillo, Christopher P. and Anderson, Timothy J.},

  abstractNote = {Two strategies for enhancing photovoltaic (PV) performance in chalcopyrite solar cells were investigated: Cu1-xKxIn1-yGaySe2 absorbers with low K content (K/(K+Cu), or x ~ 0.07) distributed throughout the bulk, and CuIn1-yGaySe2 absorbers with KIn1-yGaySe2 grown on their surfaces. Distributing K throughout the bulk absorbers improved power conversion efficiency, open-circuit voltage (VOC) and fill factor (FF) for Ga/(Ga+In) of 0, 0.3 and 0.5. Surface KIn1-yGaySe2 and bulk x ~ 0.07 Cu1-xKxIn1-yGaySe2 films with Ga/(Ga+In), or y of 0.3 and 0.5 also had improved efficiency, VOC, and FF, relative to CuIn1-yGaySe2 baselines. On the other hand, y ~ 1 absorbers did not benefit from K introduction. Similar to Cu1-xKxInSe2, the formation of Cu1-xKxGaSe2 alloys was favored at low temperatures and high Na supply by the substrate, relative to the formation of mixed-phase CuGaSe2 + KGaSe2. KIn1-yGaySe2 alloys were grown for the first time, as evidenced by X-ray diffraction and ultraviolet/visible spectroscopy. For all Ga/(Ga+In) compositions, the surface KIn1-yGaySe2 absorbers had superior PV performance in buffered and buffer-free devices. However, the bulk x ~ 0.07 absorbers only outperformed the baselines in buffered devices. The data demonstrate that KIn1-yGaySe2 passivates the surface of CuIn1-yGaySe2 to increase efficiency, VOC, and FF, while bulk Cu1-xKxIn1-yGaySe2 absorbers with x ~ 0.07 enhance efficiency, VOC, and FF by some other mechanism.},

  doi          = {10.1016/j.solmat.2017.12.038},

  journal      = {Solar Energy Materials and Solar Cells},

  number       = C,

  volume       = 179,

  place        = {United States},

  year         = {Fri Dec 29 00:00:00 EST 2017},

  month        = {Fri Dec 29 00:00:00 EST 2017}

}

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https://doi.org/10.1063/1.2149166
Investigation of CdZnS Buffer Layers on the Performance of CuInGaSe2 and CuGaSe2 Solar Cells

Conference Song, J ; Li, S S ; Chen, L ; ...

Cu(In,Ga)Se{sub 2} (CIGS) and CuGaSe{sub 2} (CGS) solar cells were fabricated using Cd{sub 1-x}Zn{sub x}S (CdZnS) buffer layers prepared by chemical bath deposition (CBD) with relative Zn compositions in the CBD bath values of X{sub bath} = 0 (i.e., pure CdS), 0.1, 0.2, 0.3, 0.4, and 0.5. The cell performance parameters of CIGS and CGS films treated with a KCN solution were investigated and compared to cells without KCN treatment. It was found that absorber films treated with KCN etching prior to the buffer CBD step show an improved cell performance for both the CIGS and CGS cells deposited withmore »« less
Review of grain interior, grain boundary, and interface effects of K in CIGS solar cells: Mechanisms for performance enhancement

Journal Article Muzzillo, Christopher P. - Solar Energy Materials and Solar Cells

Introducing K into Cu(In,Ga)(Se,S)₂ (CIGS) absorbers has led to recent world record power conversion efficiencies for thin film polycrystalline solar cells. In this work, the diverse phenomena associated with K in CIGS were reviewed, and overarching mechanisms were identified. The effects of K depend on its distribution among grain interiors (GIs), grain boundaries (GBs), and interfaces. High substrate Na and low temperature favor GI K incorporation, while low Na and high temperature favor segregation of K at GBs. Depositing KInSe₂ (or KIn_1-yGaySe₂) by co-evaporation or KF post-deposition treatment onto CIGS reduces buffer interface recombination in the final solar cells. KInSe₂more »« less
Cited by 73
https://doi.org/10.1016/j.solmat.2017.07.006

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Title: Surface and bulk effects of K in Cu1-xKxIn1-yGaySe2 solar cells

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Citation Formats

Potassium-induced surface modification of Cu(In,Ga)Se2 thin films for high-efficiency solar cells journal, November 2013

Improved Photocurrent in Cu(In,Ga)Se 2 Solar Cells: From 20.8% to 21.7% Efficiency with CdS Buffer and 21.0% Cd-Free journal, September 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

Compositional investigation of potassium doped Cu(In,Ga)Se 2 solar cells with efficiencies up to 20.8% : Compositional investigation of potassium doped Cu(In,Ga)Se journal, February 2014

Efficiency enhancement of Cu(In,Ga)Se 2 thin-film solar cells by a post-deposition treatment with potassium fluoride : Efficiency enhancement of Cu(In,Ga)Se journal, July 2013

Investigation of the effect of potassium on Cu(In,Ga)Se 2 layers and solar cells journal, May 2015

Enhanced Performance in Cu(In,Ga)Se<inline-formula><tex-math>$_{\bf 2}$</tex-math></inline-formula> Solar Cells Fabricated by the Two-Step Selenization Process With a Potassium Fluoride Postdeposition Treatment journal, November 2014

Unveiling the effects of post-deposition treatment with different alkaline elements on the electronic properties of CIGS thin film solar cells journal, January 2014

Defect formation in Cu(In,Ga)Se 2 thin films due to the presence of potassium during growth by low temperature co-evaporation process journal, November 2013

Features of KF and NaF Postdeposition Treatments of Cu(In,Ga)Se 2 Absorbers for High Efficiency Thin Film Solar Cells journal, August 2015

Effects of Sodium and Potassium on the Photovoltaic Performance of CIGS Solar Cells journal, January 2017

New world record Cu(In, Ga)(Se, S)2 thin film solar cell efficiency beyond 22% conference, June 2016

Improved CIGS modules by KF post deposition treatment and reduced cell-to-module losses conference, June 2016

Effect of potassium fluoride post-deposition treatment on Cu(In,Ga)Se2 thin films and solar cells fabricated onto sodalime glass substrates journal, October 2016

Revealing Surface Modifications of Potassium-Fluoride-Treated Cu(In,Ga)Se 2 : A Study of Material Structure, Chemistry, and Photovoltaic Performance journal, July 2016

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

High-efficiency Cu(In,Ga)Se2 solar cells journal, July 2017

Beneficial effect of post-deposition treatment in high-efficiency Cu(In,Ga)Se2 solar cells through reduced potential fluctuations journal, August 2016

Effects of the incorporation of alkali elements on Cu(In,Ga)Se2 thin film solar cells journal, December 2016

Method for a High-Rate Solution Deposition of Zn(O,S) Buffer Layer for High-Efficiency Cu(In,Ga)Se 2 -Based Solar Cells journal, September 2016

Na-Diffusion Enhanced p-type Conductivity in Cu(In,Ga)Se 2 : A New Mechanism for Efficient Doping in Semiconductors journal, August 2016

Hybrid-Functional Calculations on the Incorporation of Na and K Impurities into the CuInSe 2 and CuIn 5 Se 8 Solar-Cell Materials journal, October 2015

Recent progress in nanoelectrical characterizations of CdTe and Cu(In, Ga)Se2 conference, June 2016

Notice of Removal In-situ and ex-situ characterizations of CIGS solar cells with KF post deposition treatment conference, June 2017

First-principles study on alkali-metal effect of Li, Na, and K in CuInSe 2 and CuGaSe 2 journal, July 2015

NaF/KF post-deposition treatments and their influence on the structure of Cu(In, Ga)Se2 absorber surfaces conference, June 2016

Potassium Postdeposition Treatment-Induced Band Gap Widening at Cu(In,Ga)Se 2 Surfaces – Reason for Performance Leap? journal, December 2015

Investigation of the potassium fluoride post deposition treatment on the CIGSe/CdS interface using hard X-ray photoemission spectroscopy – a comparative study journal, January 2016

Experimental indication for band gap widening of chalcopyrite solar cell absorbers after potassium fluoride treatment journal, August 2014

First-principles calculations of Na and K impurities in CuInSe2 and their effect on Cd incorporation conference, June 2016

A closer look at initial CdS growth on high-efficiency Cu(In, Ga)Se2 absorbers using surface-sensitive methods conference, June 2016

Alkali-Templated Surface Nanopatterning of Chalcogenide Thin Films: A Novel Approach Toward Solar Cells with Enhanced Efficiency journal, April 2015

Notice of Removal Co-evaporated KInSe2: A fast alternative to KF post deposition treatment in high efficiency Cu(In,Ga)Se2 thin film solar cells conference, June 2017

CIGS thin-film solar cells and modules on enamelled steel substrates journal, May 2012

Interfacial Alkali Diffusion Control in Chalcopyrite Thin-Film Solar Cells journal, July 2014

Influence of post-deposition selenium supply on Cu(In,Ga)Se 2 -based solar cell properties journal, May 2015

Surface modification of CIGS film by annealing and its effect on the band structure and photovoltaic properties of CIGS solar cells journal, January 2015

The impact of alkali elements on the degradation of CIGS solar cells: Degradation of CIGS solar cells journal, April 2015

Properties of Cu1−x K x InSe2 alloys journal, April 2016

Chemistry of K in Cu(In,Ga)Se2 photovoltaic absorbers: Effects of temperature on Cu-K-In-Se films journal, December 2017

Surface and bulk effects of K in highly efficient Cu1-xKxInSe2 solar cells journal, October 2018

Synthesis and Structures of Ternary Chalcogenides of Aluminum and Gallium with Stacking Faults: KMQ2 (M=Al, Ga; Q=Se, Te) journal, February 2000

Crystal data for CuGaSe2 journal, April 1977

The effect of Ga content on the selenization of co-evaporated CuGa/In films and their photovoltaic performance conference, June 2014

Differences between CuGa/In and Cu/Ga/In films for selenization conference, June 2015

Review of grain interior, grain boundary, and interface effects of K in CIGS solar cells: Mechanisms for performance enhancement journal, December 2017

Preparation and Characterization of Copper Gallium Diselenide Thin Films from the Solgel-Derived Precursors journal, October 2013

Recrystallization of Cu(In,Ga)Se2 thin films studied by X-ray diffraction journal, July 2013

XPS investigation of surface secondary phase segregation in CIGS thin film conference, June 2011

Control of secondary phase segregations during CuGaSe2 thin-film growth journal, July 2002

Sodium induced secondary phase segregations in CuGaSe2 thin films journal, November 2001

Na incorporation into Cu(In,Ga)Se 2 thin-film solar cell absorbers deposited on polyimide: Impact on the chemical and electronic surface structure journal, February 2012

Effects of Na on the electrical and structural properties of CuInSe2 journal, May 1999

Optical functions and electronic structure of CuInSe 2 , CuGaSe 2 , CuInS 2 , and CuGaS 2 journal, January 2001

K 2 MM‘ 3 Se 6 (M = Cu, Ag; M‘ = Ga, In), A New Series of Metal Chalcogenides with Chain−Sublayer−Chain Slabs: ∞ 1 [M‘Se 4 ]− ∞ 2 [(MSe 4 )(M‘Se 4 )]− ∞ 1 [M‘Se 4 ] journal, January 2003

Synthesis, structure, physical properties, and electronic structure of KGaSe2 journal, August 2012

Crystal structure of pentapotassium tetraselenidogallate(III), K 5 GaSe 4 journal, January 1991

Crystal structure of hexapotassium di- μ -selenido-bis(diselenidogallate), K 6 Ga 2 Se 6 journal, January 1991

Record 1.0 V open-circuit voltage in wide band gap chalcopyrite solar cells journal, July 2017

Revealing the beneficial role of K in grain interiors, grain boundaries, and at the buffer interface for highly efficient CuInSe 2 solar cells journal, June 2018

Title: Surface and bulk effects of K in Cu_1-xK_xIn_1-yGa_ySe₂ solar cells

Potassium-induced surface modification of Cu(In,Ga)Se2 thin films for high-efficiency solar cells
journal, November 2013

Improved Photocurrent in Cu(In,Ga)Se ₂ Solar Cells: From 20.8% to 21.7% Efficiency with CdS Buffer and 21.0% Cd-Free
journal, September 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

Compositional investigation of potassium doped Cu(In,Ga)Se ₂ solar cells with efficiencies up to 20.8% : Compositional investigation of potassium doped Cu(In,Ga)Se
journal, February 2014

Efficiency enhancement of Cu(In,Ga)Se ₂ thin-film solar cells by a post-deposition treatment with potassium fluoride : Efficiency enhancement of Cu(In,Ga)Se
journal, July 2013

Investigation of the effect of potassium on Cu(In,Ga)Se 2 layers and solar cells
journal, May 2015

Enhanced Performance in Cu(In,Ga)Se<inline-formula><tex-math>$_{\bf 2}$</tex-math></inline-formula> Solar Cells Fabricated by the Two-Step Selenization Process With a Potassium Fluoride Postdeposition Treatment
journal, November 2014

Unveiling the effects of post-deposition treatment with different alkaline elements on the electronic properties of CIGS thin film solar cells
journal, January 2014

Defect formation in Cu(In,Ga)Se ₂ thin films due to the presence of potassium during growth by low temperature co-evaporation process
journal, November 2013

Features of KF and NaF Postdeposition Treatments of Cu(In,Ga)Se ₂ Absorbers for High Efficiency Thin Film Solar Cells
journal, August 2015

Effects of Sodium and Potassium on the Photovoltaic Performance of CIGS Solar Cells
journal, January 2017

New world record Cu(In, Ga)(Se, S)2 thin film solar cell efficiency beyond 22%
conference, June 2016

Improved CIGS modules by KF post deposition treatment and reduced cell-to-module losses
conference, June 2016

Effect of potassium fluoride post-deposition treatment on Cu(In,Ga)Se2 thin films and solar cells fabricated onto sodalime glass substrates
journal, October 2016

Revealing Surface Modifications of Potassium-Fluoride-Treated Cu(In,Ga)Se ₂ : A Study of Material Structure, Chemistry, and Photovoltaic Performance
journal, July 2016

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

High-efficiency Cu(In,Ga)Se2 solar cells
journal, July 2017

Beneficial effect of post-deposition treatment in high-efficiency Cu(In,Ga)Se2 solar cells through reduced potential fluctuations
journal, August 2016

Effects of the incorporation of alkali elements on Cu(In,Ga)Se2 thin film solar cells
journal, December 2016

Method for a High-Rate Solution Deposition of Zn(O,S) Buffer Layer for High-Efficiency Cu(In,Ga)Se ₂ -Based Solar Cells
journal, September 2016

Na-Diffusion Enhanced p-type Conductivity in Cu(In,Ga)Se ₂ : A New Mechanism for Efficient Doping in Semiconductors
journal, August 2016

Hybrid-Functional Calculations on the Incorporation of Na and K Impurities into the CuInSe ₂ and CuIn ₅ Se ₈ Solar-Cell Materials
journal, October 2015

Recent progress in nanoelectrical characterizations of CdTe and Cu(In, Ga)Se2
conference, June 2016

Notice of Removal In-situ and ex-situ characterizations of CIGS solar cells with KF post deposition treatment
conference, June 2017

First-principles study on alkali-metal effect of Li, Na, and K in CuInSe ₂ and CuGaSe ₂
journal, July 2015

NaF/KF post-deposition treatments and their influence on the structure of Cu(In, Ga)Se2 absorber surfaces
conference, June 2016

Potassium Postdeposition Treatment-Induced Band Gap Widening at Cu(In,Ga)Se ₂ Surfaces – Reason for Performance Leap?
journal, December 2015

Investigation of the potassium fluoride post deposition treatment on the CIGSe/CdS interface using hard X-ray photoemission spectroscopy – a comparative study
journal, January 2016

Experimental indication for band gap widening of chalcopyrite solar cell absorbers after potassium fluoride treatment
journal, August 2014

First-principles calculations of Na and K impurities in CuInSe2 and their effect on Cd incorporation
conference, June 2016

A closer look at initial CdS growth on high-efficiency Cu(In, Ga)Se2 absorbers using surface-sensitive methods
conference, June 2016

Alkali-Templated Surface Nanopatterning of Chalcogenide Thin Films: A Novel Approach Toward Solar Cells with Enhanced Efficiency
journal, April 2015

Notice of Removal Co-evaporated KInSe2: A fast alternative to KF post deposition treatment in high efficiency Cu(In,Ga)Se2 thin film solar cells
conference, June 2017

CIGS thin-film solar cells and modules on enamelled steel substrates
journal, May 2012

Interfacial Alkali Diffusion Control in Chalcopyrite Thin-Film Solar Cells
journal, July 2014

Influence of post-deposition selenium supply on Cu(In,Ga)Se 2 -based solar cell properties
journal, May 2015

Surface modification of CIGS film by annealing and its effect on the band structure and photovoltaic properties of CIGS solar cells
journal, January 2015

The impact of alkali elements on the degradation of CIGS solar cells: Degradation of CIGS solar cells
journal, April 2015

Properties of Cu1−x K x InSe2 alloys
journal, April 2016

Chemistry of K in Cu(In,Ga)Se2 photovoltaic absorbers: Effects of temperature on Cu-K-In-Se films
journal, December 2017

Surface and bulk effects of K in highly efficient Cu1-xKxInSe2 solar cells
journal, October 2018

Synthesis and Structures of Ternary Chalcogenides of Aluminum and Gallium with Stacking Faults: KMQ2 (M=Al, Ga; Q=Se, Te)
journal, February 2000

Crystal data for CuGaSe2
journal, April 1977

The effect of Ga content on the selenization of co-evaporated CuGa/In films and their photovoltaic performance
conference, June 2014

Differences between CuGa/In and Cu/Ga/In films for selenization
conference, June 2015

Review of grain interior, grain boundary, and interface effects of K in CIGS solar cells: Mechanisms for performance enhancement
journal, December 2017

Preparation and Characterization of Copper Gallium Diselenide Thin Films from the Solgel-Derived Precursors
journal, October 2013

Recrystallization of Cu(In,Ga)Se2 thin films studied by X-ray diffraction
journal, July 2013

XPS investigation of surface secondary phase segregation in CIGS thin film
conference, June 2011

Control of secondary phase segregations during CuGaSe2 thin-film growth
journal, July 2002

Sodium induced secondary phase segregations in CuGaSe2 thin films
journal, November 2001

Na incorporation into Cu(In,Ga)Se ₂ thin-film solar cell absorbers deposited on polyimide: Impact on the chemical and electronic surface structure
journal, February 2012

Effects of Na on the electrical and structural properties of CuInSe2
journal, May 1999

Optical functions and electronic structure of ${CuInSe}_{2},$ ${CuGaSe}_{2},$ ${CuInS}_{2},$ and ${CuGaS}_{2}$
journal, January 2001

K ₂ MM‘ ₃ Se ₆ (M = Cu, Ag; M‘ = Ga, In), A New Series of Metal Chalcogenides with Chain−Sublayer−Chain Slabs: _∞ ¹ [M‘Se ₄ ]− _∞ ² [(MSe ₄ )(M‘Se ₄ )]− _∞ ¹ [M‘Se ₄ ]
journal, January 2003

Synthesis, structure, physical properties, and electronic structure of KGaSe2
journal, August 2012

Crystal structure of pentapotassium tetraselenidogallate(III), K ₅ GaSe ₄
journal, January 1991

Crystal structure of hexapotassium di- μ -selenido-bis(diselenidogallate), K ₆ Ga ₂ Se ₆
journal, January 1991

Record 1.0 V open-circuit voltage in wide band gap chalcopyrite solar cells
journal, July 2017

Revealing the beneficial role of K in grain interiors, grain boundaries, and at the buffer interface for highly efficient CuInSe ₂ solar cells
journal, June 2018