Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides
Abstract Multicomponent oxides, such as many minerals and high entropy oxides, show promise as materials for protection in extreme environments. Similar to other phononically dominated materials, the spectrum of vibrational carriers and phonon scattering heavily influences thermal transport in multi...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-58345-w |
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| author | William T. Riffe Saman Zare Kristyn D. Ardrey Victor K. Champagne Milena Milich Kyungtae Lee Mahboobe Jassas Sara Makarem Elizabeth J. Opila David R. Clarke Prasanna V. Balachandran Patrick E. Hopkins |
| author_facet | William T. Riffe Saman Zare Kristyn D. Ardrey Victor K. Champagne Milena Milich Kyungtae Lee Mahboobe Jassas Sara Makarem Elizabeth J. Opila David R. Clarke Prasanna V. Balachandran Patrick E. Hopkins |
| author_sort | William T. Riffe |
| collection | DOAJ |
| description | Abstract Multicomponent oxides, such as many minerals and high entropy oxides, show promise as materials for protection in extreme environments. Similar to other phononically dominated materials, the spectrum of vibrational carriers and phonon scattering heavily influences thermal transport in multi-cation oxides. In this work, we experimentally and computationally investigate the nature of phonon scattering and thermal transport in a series of single and multi-cation rare earth sesquioxides and zirconates. A reduction in thermal conductivity was observed from the single to multi-cation oxides, which is directly correlated to measured optical mode lifetimes. Via spectroscopic ellipsometry, we observe red shifting of the optical modes from local bonding distortion. Density functional theory calculation was used to evaluate how bonding distortions influence the phononic scattering rate observed through modal broadening and reduced thermal conductivity. Compared to single-cation oxides, the multi-cation oxides, especially those with larger cation size variance, exhibited lower effective coordination number and greater bond distortion. |
| format | Article |
| id | doaj-art-dfd4738e538844ea8de3fc4d2989b5db |
| institution | DOAJ |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-dfd4738e538844ea8de3fc4d2989b5db2025-08-20T03:06:52ZengNature PortfolioNature Communications2041-17232025-04-0116111210.1038/s41467-025-58345-wBroadband optical phonon scattering reduces the thermal conductivity of multi-cation oxidesWilliam T. Riffe0Saman Zare1Kristyn D. Ardrey2Victor K. Champagne3Milena Milich4Kyungtae Lee5Mahboobe Jassas6Sara Makarem7Elizabeth J. Opila8David R. Clarke9Prasanna V. Balachandran10Patrick E. Hopkins11Department of Materials Science and Engineering, University of VirginiaDepartment of Mechanical and Aerospace Engineering, University of VirginiaDepartment of Materials Science and Engineering, University of VirginiaSchool of Engineering and Applied Sciences, Harvard UniversityDepartment of Mechanical and Aerospace Engineering, University of VirginiaDepartment of Materials Science and Engineering, University of VirginiaDepartment of Mechanical and Aerospace Engineering, University of VirginiaDepartment of Materials Science and Engineering, University of VirginiaDepartment of Materials Science and Engineering, University of VirginiaSchool of Engineering and Applied Sciences, Harvard UniversityDepartment of Materials Science and Engineering, University of VirginiaDepartment of Materials Science and Engineering, University of VirginiaAbstract Multicomponent oxides, such as many minerals and high entropy oxides, show promise as materials for protection in extreme environments. Similar to other phononically dominated materials, the spectrum of vibrational carriers and phonon scattering heavily influences thermal transport in multi-cation oxides. In this work, we experimentally and computationally investigate the nature of phonon scattering and thermal transport in a series of single and multi-cation rare earth sesquioxides and zirconates. A reduction in thermal conductivity was observed from the single to multi-cation oxides, which is directly correlated to measured optical mode lifetimes. Via spectroscopic ellipsometry, we observe red shifting of the optical modes from local bonding distortion. Density functional theory calculation was used to evaluate how bonding distortions influence the phononic scattering rate observed through modal broadening and reduced thermal conductivity. Compared to single-cation oxides, the multi-cation oxides, especially those with larger cation size variance, exhibited lower effective coordination number and greater bond distortion.https://doi.org/10.1038/s41467-025-58345-w |
| spellingShingle | William T. Riffe Saman Zare Kristyn D. Ardrey Victor K. Champagne Milena Milich Kyungtae Lee Mahboobe Jassas Sara Makarem Elizabeth J. Opila David R. Clarke Prasanna V. Balachandran Patrick E. Hopkins Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides Nature Communications |
| title | Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides |
| title_full | Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides |
| title_fullStr | Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides |
| title_full_unstemmed | Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides |
| title_short | Broadband optical phonon scattering reduces the thermal conductivity of multi-cation oxides |
| title_sort | broadband optical phonon scattering reduces the thermal conductivity of multi cation oxides |
| url | https://doi.org/10.1038/s41467-025-58345-w |
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