Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO2

Benjamin A.D. Williamson; Thomas J. Featherstone; Sanjayan S. Sathasivam; Jack E.N. Swallow; Huw Shiel; Leanne A.H. Jones; Matthew J. Smiles; Anna Regoutz; Tien Lin Lee; Xueming Xia; Christopher Blackman; Pardeep K. Thakur; Claire J. Carmalt; Ivan P. Parkin; Tim D. Veal; David O. Scanlon

doi:10.1021/acs.chemmater.9b04845

Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO₂

Benjamin A.D. Williamson, Thomas J. Featherstone, Sanjayan S. Sathasivam, Jack E.N. Swallow, Huw Shiel, Leanne A.H. Jones, Matthew J. Smiles, Anna Regoutz, Tien Lin Lee, Xueming Xia, Christopher Blackman, Pardeep K. Thakur, Claire J. Carmalt, Ivan P. Parkin, Tim D. Veal^*, David O. Scanlon

^*Corresponding author for this work

Chemistry

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

Abstract

Transparent conducting oxides (TCOs) are ubiquitous in modern consumer electronics. SnO₂ is an earth abundant, cheaper alternative to In₂O₃ as a TCO. However, its performance in terms of mobilities and conductivities lags behind that of In₂O₃. On the basis of the recent discovery of mobility and conductivity enhancements in In₂O₃ from resonant dopants, we use a combination of state-of-the-art hybrid density functional theory calculations, high resolution photoelectron spectroscopy, and semiconductor statistics modeling to understand what is the optimal dopant to maximize performance of SnO₂-based TCOs. We demonstrate that Ta is the optimal dopant for high performance SnO₂, as it is a resonant dopant which is readily incorporated into SnO₂ with the Ta 5d states sitting ∼1.4 eV above the conduction band minimum. Experimentally, the band edge electron effective mass of Ta doped SnO₂ was shown to be 0.23m₀, compared to 0.29m₀ seen with conventional Sb doping, explaining its ability to yield higher mobilities and conductivities.

Original language	English
Pages (from-to)	1964-1973
Number of pages	10
Journal	Chemistry of Materials
Volume	32
Issue number	5
DOIs	https://doi.org/10.1021/acs.chemmater.9b04845
Publication status	Published - 10 Mar 2020

Bibliographical note

Funding Information:
This work was supported by the Engineering and Physical Sciences Research Council (EPSRC) [grant numbers EP/N01572X/1 and EP/N015800/1]. T.J.F., J.E.N.S., and M.J.S. acknowledge studentship support from the EPSRC Centre for Doctoral Training in New and Sustainable Photovoltaics (Grant No. EP/L01551X/1). H.S. studentship was funded by the EPSRC (Grant No. EP/N509693/1). L.A.H.J.’s studentship was funded by the EPSRC Doctoral Training Partnership (Grant No. EP/R513271/1). The authors thank Diamond Light source for providing beam time and facilities under proposals SI18195-1 and SI21431-1. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1) and to UCL for the provision of the Legion, Myriad, and Grace supercomputers. Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202, EP/R029431), this work used the ARCHER UK National Supercomputing Service ( http://www.archer.ac.uk ). D.O.S. and T.D.V. acknowledge membership of the Materials Design Network. NSG Group are acknowledged for useful discussions and for supplying glass substrates used in this work.

Publisher Copyright:
Copyright © 2020 American Chemical Society.

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering
Materials Chemistry

Access to Document

10.1021/acs.chemmater.9b04845

Cite this

Williamson, B. A. D., Featherstone, T. J., Sathasivam, S. S., Swallow, J. E. N., Shiel, H., Jones, L. A. H., Smiles, M. J., Regoutz, A., Lee, T. L., Xia, X., Blackman, C., Thakur, P. K., Carmalt, C. J., Parkin, I. P., Veal, T. D., & Scanlon, D. O. (2020). Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO₂. Chemistry of Materials, 32(5), 1964-1973. https://doi.org/10.1021/acs.chemmater.9b04845

@article{f9bec80fe8334e958ff565a3d43cea29,

title = "Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO2",

abstract = "Transparent conducting oxides (TCOs) are ubiquitous in modern consumer electronics. SnO2 is an earth abundant, cheaper alternative to In2O3 as a TCO. However, its performance in terms of mobilities and conductivities lags behind that of In2O3. On the basis of the recent discovery of mobility and conductivity enhancements in In2O3 from resonant dopants, we use a combination of state-of-the-art hybrid density functional theory calculations, high resolution photoelectron spectroscopy, and semiconductor statistics modeling to understand what is the optimal dopant to maximize performance of SnO2-based TCOs. We demonstrate that Ta is the optimal dopant for high performance SnO2, as it is a resonant dopant which is readily incorporated into SnO2 with the Ta 5d states sitting ∼1.4 eV above the conduction band minimum. Experimentally, the band edge electron effective mass of Ta doped SnO2 was shown to be 0.23m0, compared to 0.29m0 seen with conventional Sb doping, explaining its ability to yield higher mobilities and conductivities.",

author = "Williamson, {Benjamin A.D.} and Featherstone, {Thomas J.} and Sathasivam, {Sanjayan S.} and Swallow, {Jack E.N.} and Huw Shiel and Jones, {Leanne A.H.} and Smiles, {Matthew J.} and Anna Regoutz and Lee, {Tien Lin} and Xueming Xia and Christopher Blackman and Thakur, {Pardeep K.} and Carmalt, {Claire J.} and Parkin, {Ivan P.} and Veal, {Tim D.} and Scanlon, {David O.}",

note = "Funding Information: This work was supported by the Engineering and Physical Sciences Research Council (EPSRC) [grant numbers EP/N01572X/1 and EP/N015800/1]. T.J.F., J.E.N.S., and M.J.S. acknowledge studentship support from the EPSRC Centre for Doctoral Training in New and Sustainable Photovoltaics (Grant No. EP/L01551X/1). H.S. studentship was funded by the EPSRC (Grant No. EP/N509693/1). L.A.H.J.{\textquoteright}s studentship was funded by the EPSRC Doctoral Training Partnership (Grant No. EP/R513271/1). The authors thank Diamond Light source for providing beam time and facilities under proposals SI18195-1 and SI21431-1. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1) and to UCL for the provision of the Legion, Myriad, and Grace supercomputers. Via our membership of the UK{\textquoteright}s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202, EP/R029431), this work used the ARCHER UK National Supercomputing Service ( http://www.archer.ac.uk ). D.O.S. and T.D.V. acknowledge membership of the Materials Design Network. NSG Group are acknowledged for useful discussions and for supplying glass substrates used in this work. Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

month = mar,

day = "10",

doi = "10.1021/acs.chemmater.9b04845",

language = "English",

volume = "32",

pages = "1964--1973",

journal = "Chemistry of Materials",

issn = "0897-4756",

publisher = "American Chemical Society",

number = "5",

}

Williamson, BAD, Featherstone, TJ, Sathasivam, SS, Swallow, JEN, Shiel, H, Jones, LAH, Smiles, MJ, Regoutz, A, Lee, TL, Xia, X, Blackman, C, Thakur, PK, Carmalt, CJ, Parkin, IP, Veal, TD & Scanlon, DO 2020, 'Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO₂', Chemistry of Materials, vol. 32, no. 5, pp. 1964-1973. https://doi.org/10.1021/acs.chemmater.9b04845

TY - JOUR

T1 - Resonant Ta Doping for Enhanced Mobility in Transparent Conducting SnO2

AU - Williamson, Benjamin A.D.

AU - Featherstone, Thomas J.

AU - Sathasivam, Sanjayan S.

AU - Swallow, Jack E.N.

AU - Shiel, Huw

AU - Jones, Leanne A.H.

AU - Smiles, Matthew J.

AU - Regoutz, Anna

AU - Lee, Tien Lin

AU - Xia, Xueming

AU - Blackman, Christopher

AU - Thakur, Pardeep K.

AU - Carmalt, Claire J.

AU - Parkin, Ivan P.

AU - Veal, Tim D.

AU - Scanlon, David O.

N1 - Funding Information: This work was supported by the Engineering and Physical Sciences Research Council (EPSRC) [grant numbers EP/N01572X/1 and EP/N015800/1]. T.J.F., J.E.N.S., and M.J.S. acknowledge studentship support from the EPSRC Centre for Doctoral Training in New and Sustainable Photovoltaics (Grant No. EP/L01551X/1). H.S. studentship was funded by the EPSRC (Grant No. EP/N509693/1). L.A.H.J.’s studentship was funded by the EPSRC Doctoral Training Partnership (Grant No. EP/R513271/1). The authors thank Diamond Light source for providing beam time and facilities under proposals SI18195-1 and SI21431-1. We are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/P020194/1) and to UCL for the provision of the Legion, Myriad, and Grace supercomputers. Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202, EP/R029431), this work used the ARCHER UK National Supercomputing Service ( http://www.archer.ac.uk ). D.O.S. and T.D.V. acknowledge membership of the Materials Design Network. NSG Group are acknowledged for useful discussions and for supplying glass substrates used in this work. Publisher Copyright: Copyright © 2020 American Chemical Society.

PY - 2020/3/10

Y1 - 2020/3/10

N2 - Transparent conducting oxides (TCOs) are ubiquitous in modern consumer electronics. SnO2 is an earth abundant, cheaper alternative to In2O3 as a TCO. However, its performance in terms of mobilities and conductivities lags behind that of In2O3. On the basis of the recent discovery of mobility and conductivity enhancements in In2O3 from resonant dopants, we use a combination of state-of-the-art hybrid density functional theory calculations, high resolution photoelectron spectroscopy, and semiconductor statistics modeling to understand what is the optimal dopant to maximize performance of SnO2-based TCOs. We demonstrate that Ta is the optimal dopant for high performance SnO2, as it is a resonant dopant which is readily incorporated into SnO2 with the Ta 5d states sitting ∼1.4 eV above the conduction band minimum. Experimentally, the band edge electron effective mass of Ta doped SnO2 was shown to be 0.23m0, compared to 0.29m0 seen with conventional Sb doping, explaining its ability to yield higher mobilities and conductivities.

AB - Transparent conducting oxides (TCOs) are ubiquitous in modern consumer electronics. SnO2 is an earth abundant, cheaper alternative to In2O3 as a TCO. However, its performance in terms of mobilities and conductivities lags behind that of In2O3. On the basis of the recent discovery of mobility and conductivity enhancements in In2O3 from resonant dopants, we use a combination of state-of-the-art hybrid density functional theory calculations, high resolution photoelectron spectroscopy, and semiconductor statistics modeling to understand what is the optimal dopant to maximize performance of SnO2-based TCOs. We demonstrate that Ta is the optimal dopant for high performance SnO2, as it is a resonant dopant which is readily incorporated into SnO2 with the Ta 5d states sitting ∼1.4 eV above the conduction band minimum. Experimentally, the band edge electron effective mass of Ta doped SnO2 was shown to be 0.23m0, compared to 0.29m0 seen with conventional Sb doping, explaining its ability to yield higher mobilities and conductivities.

UR - http://www.scopus.com/inward/record.url?scp=85081935698&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.9b04845

DO - 10.1021/acs.chemmater.9b04845

M3 - Article

AN - SCOPUS:85081935698

SN - 0897-4756

VL - 32

SP - 1964

EP - 1973

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 5

ER -