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Engineering magnetism in layered magnets could result in novel phenomena related to two-dimensional (2D) magnetism, which can be useful for fundamental research and practical applications. Extensive doping efforts such as substitution and intercalation have been adopted to tune antiferromagnetic (AFM) properties in M2P2X6 compounds. The substitutional doping in this material family has mainly focused on bimetallic substitution. Recently, the metal substitution can also be extended to more than two metal elements, leading to medium and high-entropy alloys (MEAs and HEAs), which are fairly underexplored in layered magnetic systems including M2P2X6. In this work, we explored the magnetic properties of the previously unreported Cu- and Cr-substituted Ni2P2S6 i.e., CuxNi2(1-x)CrxP2S6. Our study reveals a relatively systematic evolution of AFM phases with substitution than that observed in traditional bimetallic substitution in M2P2X6. Furthermore, the Cu and Cr substitutions in Ni2P2S6 are found to enhance the ferromagnetic (FM) correlation, which is also accompanied by a possible weak FM phase at low temperatures for the intermediate compositions from 0.32 to 0.80. Our work provides a strategy to establish ferromagnetism in AFM M2P2X6 that can also be used for property tuning in other layered magnets.

Recently, layered materials transition metal thiophosphate MPX3 (M = transition metals, X = S or Se) have gained significant attention because of their rich magnetic, optical, and electronic properties. Specifically, the diverse magnetic structures and the robustness of magnetism in the two-dimensional limit have made them prominent candidates to study two-dimensional magnetism. Numerous efforts such as substitutions and interlayer intercalations have been made to tune the properties of these materials, which has greatly deepened the understanding of the underlying mechanisms that govern the properties. In this work, we focus on modifying the magnetism of Ising-type antiferromagnet FePS3 using electrochemical lithium intercalation. Our work unveils the effectiveness of electrochemical intercalation as a controllable tool to modulating magnetism, including tuning magnetic ordering temperature and inducing low temperature spin-glass state, offering an approach for implementing this material into applications.

Magnetotransport, the response of electrical conduction to external magnetic field, acts as an important tool to reveal fundamental concepts behind exotic phenomena and plays a key role in enabling spintronic applications. Magnetotransport is generally sensitive to magnetic field orientations. In contrast, efficient and isotropic modulation of electronic transport, which is useful in technology applications such as omnidirectional sensing, is rarely seen, especially for pristine crystals. Here we propose a strategy to realize extremely strong modulation of electron conduction by magnetic field which is independent of field direction. GdPS, a layered antiferromagnetic semiconductor with resistivity anisotropies, supports a field-driven insulator-to-metal transition with a paradoxically isotropic gigantic negative magnetoresistance insensitive to magnetic field orientations. This isotropic magnetoresistance originates from the combined effects of a near-zero spin-orbit coupling of Gd3+-based half-filling f-electron system and the strong on-site f-d exchange coupling in Gd atoms. Our results not only provide a novel material system with extraordinary magnetotransport that offers a missing block for antiferromagnet-based ultrafast and efficient spintronic devices, but also demonstrate the key ingredients for designing magnetic materials with desired transport properties for advanced functionalities., Comment: 44 pages, 18 figures

Magnetic topological semimetals LnSbTe (Ln = Lanthanide) have attracted intensive attention because of the presence of interplay between magnetism, topological, and electron correlations depending on the choices of magnetic Ln elements. Recently, varying Sb-Te composition has been found to effectively control the electronic and magnetic states in LnSbxTe$_{2-x}$. With this motivation, we report the evolution of magnetic properties with Sb-Te substitution in NdSb$_x$Te$_{2-x+\delta}$. Our work reveals the interesting non-monotonic change in magnetic ordering temperature with varying composition stoichiometry. In addition, reducing the Sb content x drives the reorientation of moments from in-plane (ab-plane) to out-of-plane (c-axis) direction that results in the distinct magnetic structures for two end compounds NdTe$_2$ ($x = 0$) and NdSbTe ($x = 1$). Furthermore, the moment orientation in NdSb$_x$Te$_{2-x+\delta}$ is also found to be strongly tunable upon application of weak magnetic field, leading to rich magnetic phases depending on the composition stoichiometry, temperature, and magnetic field. Such strong tuning of magnetism in this material establishes it as a promising platform for investigating tunable topological states and correlated topological physics., Comment: 35 pages, 5 figures

Tuning magnetic properties in layered magnets is an important route to realize novel phenomenon related to two-dimensional (2D) magnetism. Recently, tuning antiferromagnetic (AFM) properties through substitution and intercalation techniques have been widely studied in MPX3 compounds. Interesting phenomena, such as diverse AFM structures and even the signatures of ferrimagnetism, have been reported. However, long-range ferromagnetic (FM) ordering has remained elusive. In this work, we explored the magnetic properties of the previously unreported Cr-substituted NiPS3. We found that Cr substitution is extremely efficient in controlling spin orientation in NiPS3. Our study reveals a field-induced spin polarization in lightly (9%) Cr-substituted NiPS3, which is likely attributed to the attenuation of AFM interactions and magnetic anisotropy due to Cr doping. Our work provides a possible strategy to achieve FM phase in AFM MPX3, which could be useful for investigating 2D magnetism as well as potential device applications.

Spintronics, an evolving interdisciplinary field at the intersection of magnetism and electronics, explores innovative applications of electron charge and spin properties for advanced electronic devices. The topological Hall effect, a key component in spintronics, has gained significance due to emerging theories surrounding noncoplanar chiral spin textures. This study focuses on Mn2-xZnxSb, a material crystalizing in centrosymmetric space group with rich magnetic phases tunable by Zn contents. Through comprehensive magnetic and transport characterizations, we found that the high-Zn (x>0.6) samples display THE which is enhanced with decreasing temperature, while THE in the low-Zn (x<0.6) samples show an opposite trend. The coexistence of those distinct temperature dependences for THE suggests very different magnetic interactions/structure for different compositions and underscores the strong coupling between magnetism and transport in Mn2-xZnxSb. Our findings contribute to understanding topological magnetism in centrosymmetric tetragonal lattices, establishing Mn2-xZnxSb as a unique platform for exploring tunable transport effects and opening avenues for further exploration in the realm of spintronics., Comment: 23 pages, 6 Figures, Accepted

Recent development in two-dimensional (2D) magnetic materials have motivated the search for new van der Waals magnetic materials, especially Ising-type magnets with strong magnetic anisotropy. Fe-based MPX3 (M = transition metal, X = chalcogen) compounds such as FePS3 and FePSe3 both exhibit an Ising-type magnetic order, but FePSe3 receives much less attention compared to FePS3. This work focuses on establishing the strategy to engineer magnetic anisotropy and exchange interactions in this less-explored compound. Through chalcogen and metal substitutions, the magnetic anisotropy is found to be immune against S substitution for Se whereas tunable only with heavy Mn substitution for Fe. In particular, Mn substitution leads to a continuous rotation of magnetic moments from the out-of-plane direction towards in-plane. Furthermore, the magnetic ordering temperature displays non-monotonic doping dependence for both chalcogen and metal substitutions but due to different mechanisms. These findings provide deeper insight into the Ising-type magnetism in this important van der Waals material, shedding light on the study of other Ising-type magnetic systems as well as discovering novel 2D magnets for potential applications in spintronics.

We synthesized single crystals for Mn2-xZnxSb and studied their magnetic and electronic transport properties. This material system displays rich magnetic phase tunable with temperature and Zn composition. In addition, two groups of distinct magnetic and electronic properties, separated by a critical Zn composition of x = 0.6, are discovered. The Zn-less samples are metallic and characterized by a resistivity jump at the magnetic ordering temperature, while the Zn-rich samples lose metallicity and show a metal-to-insulator transition-like feature tunable by magnetic field. Our findings establish Mn2-xZnxSb as a promising material platform that offers opportunities to study how the coupling of spin, charge, and lattice degrees of freedom governs interesting transport properties in 2D magnets, which is currently a topic of broad interest., Comment: 23 pages, 5 figures, Figures are at the end of the manuscript

Topological magnetism typically appears in noncentrosymmetric compounds or compounds with geometric frustration. Here we report the effective tuning of magnetism in centrosymmetric tetragonal Mn2-xZnxSb by Zn substitution. The magnetism is found to be closely coupled to the transport properties, giving rise to to a very large topological hall effect is possibly associated with topological magnetism. Our finding suggests Mn2-xZnxSb is a candidate material for the centrosymmetric tetragonal topological magnetic system, offers opportunities for studying and tuning spin textures and developing near room temperature spin-based devices., Comment: 15 pages, 4 Figures and already published in Physical Review B

The ZrSiS family of compounds hosts various exotic quantum phenomena due to the presence of both topological nonsymmorphic Dirac fermions and nodal-line fermions. In this material family, the LnSbTe (Ln= lanthanide) compounds are particularly interesting owing to the intrinsic magnetism from magnetic Ln which leads to new properties and quantum states. In this work, the authors focus on the previously unexplored compound SmSbTe. The studies reveal a rare combination of a few functional properties in this material, including antiferromagnetism with possible magnetic frustration, electron correlation enhancement, and Dirac nodal-line fermions. These properties enable SmSbTe as a unique platform to explore exotic quantum phenomena and advanced functionalities arising from the interplay between magnetism, topology, and electronic correlations., Comment: 23 pages, 5 figures

ZrSiS-type materials represent a large material family with unusual coexistence of topological nonsymmorphic Dirac fermions and nodal-line fermions. As a special group of ZrSiS-family, LnSbTe (Ln = Lanthanide rare earth) compounds provide a unique opportunity to explore new quantum phases due to the intrinsic magnetism induced by Ln. Here we report the single crystal growth and characterization of NdSbTe, a previously unexplored LnSbTe compound. NdSbTe has an antiferromagnetic ground state with field-driven metamagnetic transitions similar to other known LnSbTe, but exhibits distinct enhanced electronic correlations characterized by large a Sommerfeld coefficient of 115 mJ/mol $K^2$, which is the highest among the known LnSbTe compounds. Furthermore, our transport studies have revealed the coupling with magnetism and signatures of Kondo localization. All these findings establish NdSbTe as a new platform for observing novel phenomena arising from the interplay between magnetism, topology, and electron correlations.