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1.
J Am Chem Soc ; 2024 Aug 20.
Article in English | MEDLINE | ID: mdl-39163142

ABSTRACT

How disorder affects magnetic ordering is always an intriguing question, and it becomes even more interesting in the recently rising high entropy oxides due to the extremely high disorder density. However, due to the lack of high-quality single crystal samples, the strong compositional disorder effect on magnetic transition has not been deeply investigated. In this work, we have successfully synthesized high-quality single crystalline high entropy spinel ferrites (Mg0.2Mn0.2Fe0.2Co0.2Ni0.2)xFe3-xO4. Our findings from high-temperature magnetization and neutron diffraction experiments showed ferrimagnetic transitions at 748, 694, and 674 K for x values of 1, 1.5, and 1.8, respectively. Notably, the magnetic transition almost showed no broadening for x values of 1 and 1.5, compared to Fe3O4. Extended X-ray absorption fine structure measurements provided insights into the elemental distribution among the octahedral and tetrahedral sites. The random distribution of elements across these sites reduced the formation of local clusters and short-range orders, enhancing sample homogeneity and preserving the sharpness of the magnetic transition, despite bond length variation. Our study not only marks the first successful synthesis of an HEO bulk single crystal exhibiting long-range magnetic order but also sheds light on the interaction between high configurational entropy and magnetic orderings. This opens new avenues for future research and applications of magnetic high entropy oxides.

2.
Phys Rev Lett ; 132(14): 146601, 2024 Apr 05.
Article in English | MEDLINE | ID: mdl-38640375

ABSTRACT

The layer-dependent Chern number (C) in MnBi_{2}Te_{4} is characterized by the presence of a Weyl semimetal state in the ferromagnetic coupling. However, the influence of a key factor, namely, the exchange coupling, remains unexplored. This study focuses on characterizing the C=2 state in MnBi_{2}Te_{4}, which is classified as a higher C state resulting from the anomalous n=0 Landau levels (LLs). Our findings demonstrate that the exchange coupling parameter strongly influences the formation of this Chern state, leading to a competition between the C=1 and 2 states. Moreover, the emergence of odd-even LL sequences, resulting from the breaking of LL degeneracy, provides compelling evidence for the strong exchange coupling strength. These findings highlight the significance of the exchange coupling in understanding the behavior of Chern states and LLs in magnetic quantum systems.

3.
Nat Commun ; 15(1): 2881, 2024 Apr 03.
Article in English | MEDLINE | ID: mdl-38570519

ABSTRACT

Achieving spin-pinning at the interface of hetero-bilayer ferromagnet/antiferromagnet structures in conventional exchange bias systems can be challenging due to difficulties in interface control and the weakening of spin-pinning caused by poor interface quality. In this work, we propose an alternative approach to stabilize the exchange interaction at the interface of an uncompensated antiferromagnet by utilizing a gradient of interlayer exchange coupling. We demonstrate this exchange interaction through a designed field training protocol in the odd-layer topological antiferromagnet MnBi2Te4. Our results reveal a remarkable field-trained exchange bias of up to ~ 400 mT, which exhibits high repeatability and can be easily reset by a large training field. Notably, this field-trained exchange bias effect persists even with zero-field initialization, presenting a stark contrast to the traditional field-cooled exchange bias. The highly tunable exchange bias observed in this single antiferromagnet compound, without the need for an additional magnetic layer, provides valuable insight into the exchange interaction mechanism. These findings pave the way for the systematic design of topological antiferromagnetic spintronics.

4.
Sci Adv ; 10(32): eadn5696, 2024 Aug 09.
Article in English | MEDLINE | ID: mdl-39121229

ABSTRACT

The indirect exchange interaction between local magnetic moments via surface electrons has been long predicted to bolster the surface ferromagnetism in magnetic topological insulators (MTIs), which facilitates the quantum anomalous Hall effect. This unconventional effect is critical to determining the operating temperatures of future topotronic devices. However, the experimental confirmation of this mechanism remains elusive, especially in intrinsic MTIs. Here, we combine time-resolved photoemission spectroscopy with time-resolved magneto-optical Kerr effect measurements to elucidate the unique electromagnetism at the surface of an intrinsic MTI MnBi2Te4. Theoretical modeling based on 2D Ruderman-Kittel-Kasuya-Yosida interactions captures the initial quenching of a surface-rooted exchange gap within a factor of two but overestimates the bulk demagnetization by one order of magnitude. This mechanism directly explains the sizable gap in the quasi-2D electronic state and the nonzero residual magnetization in even-layer MnBi2Te4. Furthermore, it leads to efficient light-induced demagnetization comparable to state-of-the-art magnetophotonic crystals, promising an effective manipulation of magnetism and topological orders for future topotronics.

5.
Nat Commun ; 15(1): 3532, 2024 Apr 26.
Article in English | MEDLINE | ID: mdl-38670964

ABSTRACT

Dirac and Weyl semimetals are a central topic of contemporary condensed matter physics, and the discovery of new compounds with Dirac/Weyl electronic states is crucial to the advancement of topological materials and quantum technologies. Here we show a widely applicable strategy that uses high configuration entropy to engineer relativistic electronic states. We take the AMnSb2 (A = Ba, Sr, Ca, Eu, and Yb) Dirac material family as an example and demonstrate that mixing of Ba, Sr, Ca, Eu and Yb at the A site generates the compound (Ba0.38Sr0.14Ca0.16Eu0.16Yb0.16)MnSb2 (denoted as A5MnSb2), giving access to a polar structure with a space group that is not present in any of the parent compounds. A5MnSb2 is an entropy-stabilized phase that preserves its linear band dispersion despite considerable lattice disorder. Although both A5MnSb2 and AMnSb2 have quasi-two-dimensional crystal structures, the two-dimensional Dirac states in the pristine AMnSb2 evolve into a highly anisotropic quasi-three-dimensional Dirac state triggered by local structure distortions in the high-entropy phase, which is revealed by Shubnikov-de Haas oscillations measurements.

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