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Main Authors: Xu, Mingyu, Wang, Haozhe, Koirala, Krishna Prasad, Melnick, Corey, Peng, Cheng, González-Rivas, Mario U., Lu, Jiaqi, Wang, Le, Engelhard, Mark H., Du, Yingge, Ke, Xianglin, Green, Robert J., Hallas, Alannah M., Li, Jie, Kotliar, Gabriel, Xie, Weiwei
Format: Preprint
Published: 2024
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Online Access:https://arxiv.org/abs/2410.18826
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author Xu, Mingyu
Wang, Haozhe
Koirala, Krishna Prasad
Melnick, Corey
Peng, Cheng
González-Rivas, Mario U.
Lu, Jiaqi
Wang, Le
Engelhard, Mark H.
Du, Yingge
Ke, Xianglin
Green, Robert J.
Hallas, Alannah M.
Li, Jie
Kotliar, Gabriel
Xie, Weiwei
author_facet Xu, Mingyu
Wang, Haozhe
Koirala, Krishna Prasad
Melnick, Corey
Peng, Cheng
González-Rivas, Mario U.
Lu, Jiaqi
Wang, Le
Engelhard, Mark H.
Du, Yingge
Ke, Xianglin
Green, Robert J.
Hallas, Alannah M.
Li, Jie
Kotliar, Gabriel
Xie, Weiwei
contents The interplay between crystal electric field splitting of d states and Hund's rule exchange energy in cobalt-based perovskites offers a promising avenue for inducing spin-state transitions. This study reports a new body-centered tetragonal (BCT) phase of BaCoO$_3$ (BCT-BaCoO$_3$), synthesized under high pressure (15 GPa) and high temperature (1200 °C) conditions. BCT-BaCoO$_3$ adopts a double perovskite structure of EuTiO$_3$-type (space group I4/mcm, #140), confirmed by high-resolution scanning transmission electron microscopy. X-ray photoelectron spectroscopy reveals a rare Co$^{4+}$ valence state. Magnetization and X-ray absorption measurements reveal a low-spin to high-spin transition that takes place between 200 and 300 K. While spin crossovers are relatively common among common oxides, the one observed in BCT-BaCoO$_3$ is remarkable in that it proceeds in the opposite direction from conventional spin transitions. BCT-BaCoO$_3$ exhibits a low-spin (S = 1/2) state at high temperatures and transitions to a high-spin (S = 5/2) state at low temperatures. Within the high-spin state, hard ferromagnetic order onsets at T$_C$ = 107 K. Electrical resistivity indicates weak magnetoresistance and insulating behavior. Overall, BCT-BaCoO$_3$ presents an exceptional model for the exploration of spin-state transitions and the study of Co spin states in cobalt-based perovskites.
format Preprint
id arxiv_https___arxiv_org_abs_2410_18826
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Tetragonal BaCoO$_3$: A Co$^{4+}$ Ferromagnetic Mott Insulator with Inverted Spin Crossover
Xu, Mingyu
Wang, Haozhe
Koirala, Krishna Prasad
Melnick, Corey
Peng, Cheng
González-Rivas, Mario U.
Lu, Jiaqi
Wang, Le
Engelhard, Mark H.
Du, Yingge
Ke, Xianglin
Green, Robert J.
Hallas, Alannah M.
Li, Jie
Kotliar, Gabriel
Xie, Weiwei
Materials Science
The interplay between crystal electric field splitting of d states and Hund's rule exchange energy in cobalt-based perovskites offers a promising avenue for inducing spin-state transitions. This study reports a new body-centered tetragonal (BCT) phase of BaCoO$_3$ (BCT-BaCoO$_3$), synthesized under high pressure (15 GPa) and high temperature (1200 °C) conditions. BCT-BaCoO$_3$ adopts a double perovskite structure of EuTiO$_3$-type (space group I4/mcm, #140), confirmed by high-resolution scanning transmission electron microscopy. X-ray photoelectron spectroscopy reveals a rare Co$^{4+}$ valence state. Magnetization and X-ray absorption measurements reveal a low-spin to high-spin transition that takes place between 200 and 300 K. While spin crossovers are relatively common among common oxides, the one observed in BCT-BaCoO$_3$ is remarkable in that it proceeds in the opposite direction from conventional spin transitions. BCT-BaCoO$_3$ exhibits a low-spin (S = 1/2) state at high temperatures and transitions to a high-spin (S = 5/2) state at low temperatures. Within the high-spin state, hard ferromagnetic order onsets at T$_C$ = 107 K. Electrical resistivity indicates weak magnetoresistance and insulating behavior. Overall, BCT-BaCoO$_3$ presents an exceptional model for the exploration of spin-state transitions and the study of Co spin states in cobalt-based perovskites.
title Tetragonal BaCoO$_3$: A Co$^{4+}$ Ferromagnetic Mott Insulator with Inverted Spin Crossover
topic Materials Science
url https://arxiv.org/abs/2410.18826