4.8 Article

Anomalous Defect Dependence of Thermal Conductivity in Epitaxial WO3 Thin Films

Journal

ADVANCED MATERIALS
Volume 31, Issue 43, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201903738

Keywords

defects; electrolyte gating; lattice volume; thermal conductivity; WO3

Funding

  1. Solid State Solar-Thermal Energy Conversion Center (S3TEC), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001299]
  2. MRSEC Program of the National Science Foundation [DMR-1419807]
  3. National Science Foundation [ECS-0335765]
  4. National Research Foundation of Korea [2016R1A5A1008184, 2018R1A2A2A14079326]
  5. National Institute of Supercomputing and Network/Korea Institute of Science and Technology Information with supercomputing resources [KSC-2017-C3-0005]
  6. National Research Foundation of Korea [2018R1A2A2A14079326] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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Lattice defects typically reduce lattice thermal conductivity, which has been widely exploited in applications such as thermoelectric energy conversion. Here, an anomalous dependence of the lattice thermal conductivity on point defects is demonstrated in epitaxial WO3 thin films. Depending on the substrate, the lattice of epitaxial WO3 expands or contracts as protons are intercalated by electrolyte gating or oxygen vacancies are introduced by adjusting growth conditions. Surprisingly, the observed lattice volume, instead of the defect concentration, plays the dominant role in determining the thermal conductivity. In particular, the thermal conductivity increases significantly with proton intercalation, which is contrary to the expectation that point defects typically lower the lattice thermal conductivity. The thermal conductivity can be dynamically varied by a factor of approximate to 1.7 via electrolyte gating, and tuned over a larger range, from 7.8 to 1.1 W m(-1) K-1, by adjusting the oxygen pressure during film growth. The electrolyte-gating-induced changes in thermal conductivity and lattice dimensions are reversible through multiple cycles. These findings not only expand the basic understanding of thermal transport in complex oxides, but also provide a path to dynamically control the thermal conductivity.

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