Magnetic order and Li-diffusion in the 1/3-filled Kagome layers of antiperovskite Lithium-ion battery materials (Li$_2$Fe)SO and (Li$_2$Fe)SeO

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Autori principali: Seewald, F., Schulze, T., Gräßler, N., Carstens, F. L., Singer, L., Mohamed, M. A. A., Hampel, S., Büchner, B., Klingeler, R., Klauss, H. -H., Grafe, H. -J.
Natura: Preprint
Pubblicazione: 2025
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author Seewald, F.
Schulze, T.
Gräßler, N.
Carstens, F. L.
Singer, L.
Mohamed, M. A. A.
Hampel, S.
Büchner, B.
Klingeler, R.
Klauss, H. -H.
Grafe, H. -J.
author_facet Seewald, F.
Schulze, T.
Gräßler, N.
Carstens, F. L.
Singer, L.
Mohamed, M. A. A.
Hampel, S.
Büchner, B.
Klingeler, R.
Klauss, H. -H.
Grafe, H. -J.
contents The recently discovered lithium-rich antiperovskites (Li$_2$Fe)SeO and (Li$_2$Fe)SO host lithium and iron ions on the same atomic position which octahedrally coordinates to central oxygens. In a cubic antiperovskite these sites form Kagome planes stacked along the <111> directions which triangular motifs induce high geometric frustration in the diluted magnetic sublattice for antiferromagnetic interactions. Despite their compelling properties as high-capacity Li-ion battery cathode materials, very little is known about the electronic and magnetic properties of lithium-rich antiperovskites. We report static magnetization, Mössbauer, and NMR studies on both compounds. Our data reveal a Pauli paramagnetic-like behaviour, a long-range antiferromagnetically ordered ground state below 50 K and a regime of short-range magnetic correlations up to 100 K. Our results are consistent with a random Li-Fe distribution on the shared lattice position. In addition, Li-hopping is observed above 200 K with an activation energy of E$_a$ = 0.47 eV. Overall, our data elucidate static magnetism in a disordered magnetically frustrated and presumably semimetallic system with thermally induced ion diffusion dynamics.
format Preprint
id arxiv_https___arxiv_org_abs_2504_19603
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Magnetic order and Li-diffusion in the 1/3-filled Kagome layers of antiperovskite Lithium-ion battery materials (Li$_2$Fe)SO and (Li$_2$Fe)SeO
Seewald, F.
Schulze, T.
Gräßler, N.
Carstens, F. L.
Singer, L.
Mohamed, M. A. A.
Hampel, S.
Büchner, B.
Klingeler, R.
Klauss, H. -H.
Grafe, H. -J.
Materials Science
The recently discovered lithium-rich antiperovskites (Li$_2$Fe)SeO and (Li$_2$Fe)SO host lithium and iron ions on the same atomic position which octahedrally coordinates to central oxygens. In a cubic antiperovskite these sites form Kagome planes stacked along the <111> directions which triangular motifs induce high geometric frustration in the diluted magnetic sublattice for antiferromagnetic interactions. Despite their compelling properties as high-capacity Li-ion battery cathode materials, very little is known about the electronic and magnetic properties of lithium-rich antiperovskites. We report static magnetization, Mössbauer, and NMR studies on both compounds. Our data reveal a Pauli paramagnetic-like behaviour, a long-range antiferromagnetically ordered ground state below 50 K and a regime of short-range magnetic correlations up to 100 K. Our results are consistent with a random Li-Fe distribution on the shared lattice position. In addition, Li-hopping is observed above 200 K with an activation energy of E$_a$ = 0.47 eV. Overall, our data elucidate static magnetism in a disordered magnetically frustrated and presumably semimetallic system with thermally induced ion diffusion dynamics.
title Magnetic order and Li-diffusion in the 1/3-filled Kagome layers of antiperovskite Lithium-ion battery materials (Li$_2$Fe)SO and (Li$_2$Fe)SeO
topic Materials Science
url https://arxiv.org/abs/2504.19603