Ligand Field-Induced Exotic Dopant for Infrared Transparent Electrode: W in Rutile SnO2

Michitaka Fukumoto, Yasushi Hirose*, Benjamin A.D. Williamson, Shoichiro Nakao, Koji Kimura, Koichi Hayashi, Yuki Sugisawa, Daiichiro Sekiba, David O. Scanlon, Tetsuya Hasegawa

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Transparent conductive oxides (TCOs) exhibiting high near-infrared (NIR) transmittance are one of the key materials for highly efficient thin-film solar cells with widened spectral sensitivity. To realize excellent NIR transparency in a TCO film, developing a dopant providing high mobility (µ) carriers is quite important. Herein, it is demonstrated that W is a high-μ dopant in rutile SnO2, which is unexpected from the conventional strategy. A combination of electrical transport property measurements and hybrid density functional theory calculations reveals that W behaves as a singly charged donor (W5+) showing minimized ionized impurity scattering. This charge state is realized by the splitting of the W 5d t2g-states originating not only from the octahedral crystal field but also hybridization with the O 2p orbitals, whose contribution has not been considered in transition metal-doped TCOs. Hybridization between metal d orbital and O 2p orbitals would provide a new guide for designing a novel dopant of NIR transparent conductors.

Original languageEnglish
Article number2110832
Number of pages7
JournalAdvanced Functional Materials
Volume32
Issue number14
Early online date27 Dec 2021
DOIs
Publication statusPublished - 4 Apr 2022

Bibliographical note

Funding Information:
This work was partially supported by JSPS Grants-in-Aid for Transformative Research Areas (A) ”Hyper-Ordered Structures Science”: Grant Nos. 20H05878 and 20H05881, the Engineering and Physical Sciences Research Council (EPSRC) (Grant No. EP/ N01572X/1), and Nanotechnology Platform project by the Ministry of Education, Culture, Sports, Science and Technology of Japan (Grant Nos. JPMXP09A20UT0246 and JPMX09A20NM0084). The authors are grateful to the UK Materials and Molecular Modelling Hub for computational resources, which was partially funded by EPSRC (EP/P020194/ 1), and to UCL for provision of the Legion, Myriad, and Grace supercomputers. Via the membership in 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). B.A.D.W. would also like to acknowledge support from the Research Council of Norway (Project No. 275810). D.O.S. acknowledges the membership of the Materials Design Network. The XFH measurements were performed at the BL13XU of SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (Proposal No. 2020A0827). They thank Prof. Hiroyuki Matsuzaki, Dr. Hironori Tokuyama, and Dr. Takeyasu Yamagata of the University of Tokyo for their assistance in the Rutherford backscattering spectrometry measurements at MALT. The crystal structure in the graphical abstract image was drawn by VESTA. [50]

Publisher Copyright:
© 2021 Wiley-VCH GmbH.

Keywords

  • high mobility
  • ligand field splitting
  • near-infrared transparent conductors
  • SnO
  • solar cells

ASJC Scopus subject areas

  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics

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