Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics: Compositional Control of Dimensionality and Optoelectronic Properties

Narendra Pai; Manjunath Chatti; Sebastian O. Fürer; Andrew D. Scully; Sonia R. Raga; Nitish Rai; Boer Tan; Anthony S.R. Chesman; Zhou Xu; Kevin J. Rietwyk; Saripally Sudhaker Reddy; Yvonne Hora; Gaveshana A. Sepalage; Nadja Glück; Monica Lira-Cantú; Udo Bach; Alexandr N. Simonov

doi:10.1002/aenm.202201482

Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics: Compositional Control of Dimensionality and Optoelectronic Properties

Narendra Pai, Manjunath Chatti, Sebastian O. Fürer, Andrew D. Scully, Sonia R. Raga, Nitish Rai, Boer Tan, Anthony S.R. Chesman, Zhou Xu, Kevin J. Rietwyk, Saripally Sudhaker Reddy, Yvonne Hora, Gaveshana A. Sepalage, Nadja Glück, Monica Lira-Cantú, Udo Bach, Alexandr N. Simonov

Research output: Contribution to journal › Article › peer-review

33 Scopus citations

Abstract

The search for lead-free alternatives to lead-halide perovskite photovoltaic materials resulted in the discovery of copper(I)-silver(I)-bismuth(III) halides exhibiting promising properties for optoelectronic applications. The present work demonstrates a solution-based synthesis of uniform Cu_xAgBiI₄₊_x thin films and scrutinizes the effects of x on the phase composition, dimensionality, optoelectronic properties, and photovoltaic performance. Formation of pure 3D CuAgBiI₅ at x = 1, 2D Cu₂AgBiI₆ at x = 2, and a mix of the two at 1 < x < 2 is demonstrated. Despite lower structural dimensionality, Cu₂AgBiI₆ has broader optical absorption with a direct bandgap of 1.89 ± 0.05 eV, a valence band level at -5.25 eV, improved carrier lifetime, and higher recombination resistance as compared to CuAgBiI₅. These differences are mirrored in the power conversion efficiencies of the CuAgBiI₅ and Cu₂AgBiI₆ solar cells under 1 sun of 1.01 ± 0.06% and 2.39 ± 0.05%, respectively. The latter value is the highest reported for this class of materials owing to the favorable film morphology provided by the hot-casting method. Future performance improvements might emerge from the optimization of the Cu₂AgBiI₆ layer thickness to match the carrier diffusion length of ≈40–50 nm. Nonencapsulated Cu₂AgBiI₆ solar cells display storage stability over 240 days.

Original language	English
Article number	2201482
Journal	Advanced Energy Materials
Volume	12
Issue number	32
DOIs	https://doi.org/10.1002/aenm.202201482
State	Published - 25 Aug 2022
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2022 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.

Funding

The authors are highly grateful to Dr. Jiangfeng Lu (Wuhan University of Technology) for invaluable discussions, Mr. Philippe Holzhey (Oxford University) for assistance with PL measurements, Mr. D. Vowles (Monash University) for assistance with EBIC experiments, and to the Monash Centre for Electron Microscopy and Monash X-ray Platform for providing access to their characterization facilities used for some parts of this work. The authors acknowledge funding of this work by the Australian Government through the Australian Centre for Advanced Photovoltaics (ACAP), the Australian Renewable Energy Agency (ARENA), and the Australian Research Council through the Centre of Excellence in Exciton Science (CE170100026) and Future Fellowship to ANS (FT200100317). Responsibility for the views, information, or advice expressed herein is not accepted by the Australian Government. SRR acknowledges the support from “laCaixa” Foundation (ID 100010434; LCF/BQ/PI20/11760024). Open access publishing facilitated by Monash University, as part of the Wiley – Monash University agreement via the Council of Australian University Librarians. The authors are highly grateful to Dr. Jiangfeng Lu (Wuhan University of Technology) for invaluable discussions, Mr. Philippe Holzhey (Oxford University) for assistance with PL measurements, Mr. D. Vowles (Monash University) for assistance with EBIC experiments, and to the Monash Centre for Electron Microscopy and Monash X‐ray Platform for providing access to their characterization facilities used for some parts of this work. The authors acknowledge funding of this work by the Australian Government through the Australian Centre for Advanced Photovoltaics (ACAP), the Australian Renewable Energy Agency (ARENA), and the Australian Research Council through the Centre of Excellence in Exciton Science (CE170100026) and Future Fellowship to ANS (FT200100317). Responsibility for the views, information, or advice expressed herein is not accepted by the Australian Government. SRR acknowledges the support from “laCaixa” Foundation (ID 100010434; LCF/BQ/PI20/11760024).

Funders	Funder number
Australian University Librarians
Wiley – Monash University
Australian Centre for Advanced Photovoltaics
Australian Research Council
Monash University
Australian Renewable Energy Agency
Wuhan University of Technology
Centre of Excellence in Exciton Science	FT200100317, CE170100026
laCaixa” Foundation	100010434, LCF/BQ/PI20/11760024

Keywords

Cu AgBiI
CuAgBiI
solar cells
thin film

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/aenm.202201482

Cite this

Pai, N., Chatti, M., Fürer, S. O., Scully, A. D., Raga, S. R., Rai, N., Tan, B., Chesman, A. S. R., Xu, Z., Rietwyk, K. J., Reddy, S. S., Hora, Y., Sepalage, G. A., Glück, N., Lira-Cantú, M., Bach, U., & Simonov, A. N. (2022). Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics: Compositional Control of Dimensionality and Optoelectronic Properties. Advanced Energy Materials, 12(32), Article 2201482. https://doi.org/10.1002/aenm.202201482

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title = "Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics: Compositional Control of Dimensionality and Optoelectronic Properties",

abstract = "The search for lead-free alternatives to lead-halide perovskite photovoltaic materials resulted in the discovery of copper(I)-silver(I)-bismuth(III) halides exhibiting promising properties for optoelectronic applications. The present work demonstrates a solution-based synthesis of uniform CuxAgBiI4+x thin films and scrutinizes the effects of x on the phase composition, dimensionality, optoelectronic properties, and photovoltaic performance. Formation of pure 3D CuAgBiI5 at x = 1, 2D Cu2AgBiI6 at x = 2, and a mix of the two at 1 < x < 2 is demonstrated. Despite lower structural dimensionality, Cu2AgBiI6 has broader optical absorption with a direct bandgap of 1.89 ± 0.05 eV, a valence band level at -5.25 eV, improved carrier lifetime, and higher recombination resistance as compared to CuAgBiI5. These differences are mirrored in the power conversion efficiencies of the CuAgBiI5 and Cu2AgBiI6 solar cells under 1 sun of 1.01 ± 0.06% and 2.39 ± 0.05%, respectively. The latter value is the highest reported for this class of materials owing to the favorable film morphology provided by the hot-casting method. Future performance improvements might emerge from the optimization of the Cu2AgBiI6 layer thickness to match the carrier diffusion length of ≈40–50 nm. Nonencapsulated Cu2AgBiI6 solar cells display storage stability over 240 days.",

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author = "Narendra Pai and Manjunath Chatti and F{\"u}rer, {Sebastian O.} and Scully, {Andrew D.} and Raga, {Sonia R.} and Nitish Rai and Boer Tan and Chesman, {Anthony S.R.} and Zhou Xu and Rietwyk, {Kevin J.} and Reddy, {Saripally Sudhaker} and Yvonne Hora and Sepalage, {Gaveshana A.} and Nadja Gl{\"u}ck and Monica Lira-Cant{\'u} and Udo Bach and Simonov, {Alexandr N.}",

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Pai, N, Chatti, M, Fürer, SO, Scully, AD, Raga, SR, Rai, N, Tan, B, Chesman, ASR, Xu, Z, Rietwyk, KJ, Reddy, SS, Hora, Y, Sepalage, GA, Glück, N, Lira-Cantú, M, Bach, U & Simonov, AN 2022, 'Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics: Compositional Control of Dimensionality and Optoelectronic Properties', Advanced Energy Materials, vol. 12, no. 32, 2201482. https://doi.org/10.1002/aenm.202201482

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T1 - Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics

T2 - Compositional Control of Dimensionality and Optoelectronic Properties

AU - Pai, Narendra

AU - Chatti, Manjunath

AU - Fürer, Sebastian O.

AU - Scully, Andrew D.

AU - Raga, Sonia R.

AU - Rai, Nitish

AU - Tan, Boer

AU - Chesman, Anthony S.R.

AU - Xu, Zhou

AU - Rietwyk, Kevin J.

AU - Reddy, Saripally Sudhaker

AU - Hora, Yvonne

AU - Sepalage, Gaveshana A.

AU - Glück, Nadja

AU - Lira-Cantú, Monica

AU - Bach, Udo

AU - Simonov, Alexandr N.

PY - 2022/8/25

Y1 - 2022/8/25

N2 - The search for lead-free alternatives to lead-halide perovskite photovoltaic materials resulted in the discovery of copper(I)-silver(I)-bismuth(III) halides exhibiting promising properties for optoelectronic applications. The present work demonstrates a solution-based synthesis of uniform CuxAgBiI4+x thin films and scrutinizes the effects of x on the phase composition, dimensionality, optoelectronic properties, and photovoltaic performance. Formation of pure 3D CuAgBiI5 at x = 1, 2D Cu2AgBiI6 at x = 2, and a mix of the two at 1 < x < 2 is demonstrated. Despite lower structural dimensionality, Cu2AgBiI6 has broader optical absorption with a direct bandgap of 1.89 ± 0.05 eV, a valence band level at -5.25 eV, improved carrier lifetime, and higher recombination resistance as compared to CuAgBiI5. These differences are mirrored in the power conversion efficiencies of the CuAgBiI5 and Cu2AgBiI6 solar cells under 1 sun of 1.01 ± 0.06% and 2.39 ± 0.05%, respectively. The latter value is the highest reported for this class of materials owing to the favorable film morphology provided by the hot-casting method. Future performance improvements might emerge from the optimization of the Cu2AgBiI6 layer thickness to match the carrier diffusion length of ≈40–50 nm. Nonencapsulated Cu2AgBiI6 solar cells display storage stability over 240 days.

AB - The search for lead-free alternatives to lead-halide perovskite photovoltaic materials resulted in the discovery of copper(I)-silver(I)-bismuth(III) halides exhibiting promising properties for optoelectronic applications. The present work demonstrates a solution-based synthesis of uniform CuxAgBiI4+x thin films and scrutinizes the effects of x on the phase composition, dimensionality, optoelectronic properties, and photovoltaic performance. Formation of pure 3D CuAgBiI5 at x = 1, 2D Cu2AgBiI6 at x = 2, and a mix of the two at 1 < x < 2 is demonstrated. Despite lower structural dimensionality, Cu2AgBiI6 has broader optical absorption with a direct bandgap of 1.89 ± 0.05 eV, a valence band level at -5.25 eV, improved carrier lifetime, and higher recombination resistance as compared to CuAgBiI5. These differences are mirrored in the power conversion efficiencies of the CuAgBiI5 and Cu2AgBiI6 solar cells under 1 sun of 1.01 ± 0.06% and 2.39 ± 0.05%, respectively. The latter value is the highest reported for this class of materials owing to the favorable film morphology provided by the hot-casting method. Future performance improvements might emerge from the optimization of the Cu2AgBiI6 layer thickness to match the carrier diffusion length of ≈40–50 nm. Nonencapsulated Cu2AgBiI6 solar cells display storage stability over 240 days.

KW - Cu AgBiI

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KW - thin film

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Solution Processable Direct Bandgap Copper-Silver-Bismuth Iodide Photovoltaics: Compositional Control of Dimensionality and Optoelectronic Properties

Abstract

Bibliographical note

Funding

Keywords

UN SDGs

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