Abstract
Understanding and controlling microscopic heat transfer mechanisms in solids is critical to material design in numerous technological applications. Yet, the current understanding of thermal transport in semiconductors and insulators is limited by the difficulty in directly measuring individual phonon lifetimes and mean free paths, and studying their dependence on the microscopic state of the material. Here we report our measurements of microscopic phonon scattering rates in AgBiSe2, which exhibits a controllable, reversible change directly linked to microstructure evolution near a reversible structural phase transition, that directly impacts the thermal conductivity. We demonstrate a steplike doubling of phonon scattering rates resultant from the cation disordering at the structural transition. To rationalize the neutron scattering data, we leverage a stepwise approach to account for alterations to the thermal conductivity that are imparted by distinct scattering mechanisms. These results highlight the potential of tunable microstructures housed in a stable crystal matrix to provide a practical route to tailor phonon scattering to optimize thermal transport properties.
| Original language | English |
|---|---|
| Article number | 105402 |
| Journal | Physical Review Materials |
| Volume | 4 |
| Issue number | 10 |
| DOIs | |
| State | Published - Oct 12 2020 |
Bibliographical note
Publisher Copyright:© 2020 American Physical Society.
Funding
J.N. wishes to acknowledge useful discussions with N. P. Luciano and J. Ma, technical support from D. Dunning, S. Elorfi, and E. Huckabay, and manuscript reviews by L. Lindsey and M. B. Stone. Neutron scattering measurements and analysis (J.N., C.L, O.D.) were supported as part of the S3TEC EFRC, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0001299. First-principles simulations (D.B.) were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under the Early Career Award No. DE-SC0016166 (PI O.D.) Thermal conductivity modeling (JD) and thermal measurements (TLA) were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Award No. DE-SC0019299. Sample synthesis (A.F.M.) was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. H.W. was supported by the Propulsion Materials program of Vehicle Technology Office under EERE. The research at Oak Ridge National Laboratory was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. Theoretical calculations were performed using resources of the National Energy Research Scientific Computing Center, a US DOE Office of Science User Facility supported by the Office of Science of the US Department of Energy under Contract No. DE-AC02-05CH11231. We acknowledge the support of the National Institute of Standards and Technology, US Department of Commerce, in providing the neutron research facilities used in this work.
| Funders | Funder number |
|---|---|
| S3TEC EFRC | |
| Scientific User Facilities Division | |
| U.S. Department of Energy | DE-AC02-05CH11231 |
| National Institute of Standards and Technology | |
| U.S. Department of Commerce | |
| Office of Science | |
| Office of Energy Efficiency and Renewable Energy | |
| Basic Energy Sciences | DE-SC0001299 |
| Division of Materials Sciences and Engineering | DE-SC0019299, DE-SC0016166 |
| National Energy Research Scientific Computing Center |