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The interplay between magnetism and quantum effects has motivated several thermoelectric studies on iron‐telluride yet with little insight on the anomalous features in transport properties near magnetostructural transition temperature (≈70 K). A detailed investigation is carried out on Fe1.1Te by characterizing magnetic, heat capacity, galvanomagnetic, and thermoelectric transport properties to understand the electronic, magnetic, and structural origin of those anomalies. The magnetic susceptibility indicates a bicollinear stripe and short‐range ordering in the antiferromagnetic and paramagnetic domains, respectively. Hall conductivity and transverse magnetoresistance reveal a multicarrier transport impacted by spin fluctuations and magnons. Contributions from phonon‐drag and magnon‐drag are evaluated to understand the origin of the broad peak in antiferromagnetic thermopower. The peak at ≈50 K and the insignificant entropy contribution from the magnonic heat capacity support the phonon‐drag as the origin. The field‐dependent enhancement of thermal conductivity must be associated with field‐dependent spin‐phonon coupling modification. The field‐induced thermopower reduction can be attributed to the suppression of magnons or paramagnons, as evidenced by the magnetic susceptibility data. Above 70 K, the thermal conductivity drops sharply due to the structural change modifying phonon modes. Understanding these properties originated from the spin, and quantum effects are instrumental for designing high‐performance spin‐driven thermoelectrics.
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Designing Spin‐Crossover Systems to Enhance Thermopower and Thermoelectric Figure‐of‐Merit in Paramagnetic Materials
Thermoelectric materials, capable of converting temperature gradients into electrical power, have been traditionally limited by a trade‐off between thermopower and electrical conductivity. This study introduces a novel, broadly applicable approach that enhances both the spin‐driven thermopower and the thermoelectric figure‐of‐merit (zT) without compromising electrical conductivity, using temperature‐driven spin crossover. Our approach, supported by both theoretical and experimental evidence, is demonstrated through a case study of chromium doped‐manganese telluride, but is not confined to this material and can be extended to other magnetic materials. By introducing dopants to create a high crystal field and exploiting the entropy changes associated with temperature‐driven spin crossover, we achieved a significant increase in thermopower, by approximately 136 μV K−1, representing more than a 200% enhancement at elevated temperatures within the paramagnetic domain. Our exploration of the bipolar semiconducting nature of these materials reveals that suppressing bipolar magnon/paramagnon‐drag thermopower is key to understanding and utilizing spin crossover‐driven thermopower. These findings, validated by inelastic neutron scattering, X‐ray photoemission spectroscopy, thermal transport, and energy conversion measurements, shed light on crucial material design parameters. We provide a comprehensive framework that analyzes the interplay between spin entropy, hopping transport, and magnon/paramagnon lifetimes, paving the way for the development of high‐performance spin‐driven thermoelectric materials.
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- Award ID(s):
- 2110603
- PAR ID:
- 10535495
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- ENERGY & ENVIRONMENTAL MATERIALS
- Volume:
- 8
- Issue:
- 1
- ISSN:
- 2575-0356
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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