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This article shows experimentally that an external electric field affects the velocity of the longitudinal acoustic phonons (vLA), thermal conductivity (κ), and diffusivity (D) in a bulk lead zirconium titanate–based ferroelectric. Phonon conduction dominates κ, and the observations are due to changes in the phonon dispersion, not in the phonon scattering. This gives insight into the nature of the thermal fluctuations in ferroelectrics, namely, phonons labeled ferrons that carry heat and polarization. It also opens the way for phonon-based electrically driven all-solid-state heat switches, an enabling technology for solid-state heat engines. A quantitative theoretical model combining piezoelectric strain and phonon anharmonicity explains the field dependence ofvLA, κ, andDwithout any adjustable parameters, thus connecting thermodynamic equilibrium properties with transport properties. The effect is four times larger than previously reported effects, which were ascribed to field-dependent scattering of phonons.
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Two stage decoherence of optical phonons in long oligomers
Molecular vibrations are generally responsible for chemical energy transport and dissipation in molecular systems. This transport is fast and efficient if energy is transferred by optical phonons in periodic oligomers, but its efficiency is limited by decoherence emerging due to anharmonic interactions with acoustic phonons. Using a general theoretical model, we show that in the most common case of the optical phonon band being narrower than the acoustic bands, decoherence takes place in two stages. The faster stage involves optical phonon multiple forward scattering due to absorption and emission of transverse acoustic phonons, i.e., collective bending modes with a quadratic spectrum; the transport remains ballistic and the speed can be altered. The subsequent slower stage involves phonon backscattering in multiphonon processes involving two or more acoustic phonons resulting in a switch to diffusive transport. If the initially excited optical phonon possesses a relatively small group velocity, then it is accelerated in the first stage due to its transitions to states propagating faster. This theoretical expectation is consistent with the recent measurements of optical phonon transport velocity in alkane chains, increasing with increasing the chain length.
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- Award ID(s):
- 2201027
- PAR ID:
- 10611632
- Publisher / Repository:
- AIP
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 161
- Issue:
- 9
- ISSN:
- 0021-9606
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1063/5.0222580
