Designing Spin‐Crossover Systems to Enhance Thermopower and Thermoelectric Figure‐of‐Merit in Paramagnetic Materials

Polash, Md Mobarak Hossain; Stone, Matthew; Chi, Songxue; Vashaee, Daryoosh

doi:10.1002/eem2.12822

Designing Spin‐Crossover Systems to Enhance Thermopower and Thermoelectric Figure‐of‐Merit in Paramagnetic Materials

Journal Article · Thu Aug 22 00:00:00 EDT 2024 · ENERGY & ENVIRONMENTAL MATERIALS

DOI:https://doi.org/10.1002/eem2.12822· OSTI ID:2586977

Polash, Md Mobarak Hossain ^[1]; Stone, Matthew ^[2]; Chi, Songxue ^[2]; ^[1]

North Carolina State University, Raleigh, NC (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Air Force Office of Scientific Research; National Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2586977

Journal Information:: ENERGY & ENVIRONMENTAL MATERIALS, Journal Name: ENERGY & ENVIRONMENTAL MATERIALS Journal Issue: 1 Vol. 8; ISSN 2575-0356

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Designing Spin‐Crossover Systems to Enhance Thermopower and Thermoelectric Figure‐of‐Merit in Paramagnetic Materials

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