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Abstract
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.
Keywords
spin crossover
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thermoelectric materials
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thermopower enhancement
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paramagnons
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magnons
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Md Mobarak Hossain Polash, Matthew Stone, Songxue Chi, Daryoosh Vashaee.
Designing Spin-Crossover Systems to Enhance Thermopower and Thermoelectric Figure-of-Merit in Paramagnetic Materials.
Energy & Environmental Materials, 2025, 8(1): e12822 DOI:10.1002/eem2.12822
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2024 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.
