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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
A MnSb2(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 theA site generates the compound (Ba0.38Sr0.14Ca0.16Eu0.16Yb0.16)MnSb2(denoted asA 5MnSb2), giving access to a polar structure with a space group that is not present in any of the parent compounds.A 5MnSb2is an entropy-stabilized phase that preserves its linear band dispersion despite considerable lattice disorder. Although bothA 5MnSb2andA MnSb2have quasi-two-dimensional crystal structures, the two-dimensional Dirac states in the pristineA MnSb2evolve 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. -
We synthesized single crystals for Mn2-xZnxSb (0 ≤ x ≤ 1) 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.more » « lessFree, publicly-accessible full text available October 1, 2024
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Abstract Recent advances in 2D magnetism have heightened interest in layered magnetic materials due to their potential for spintronics. In particular, layered semiconducting antiferromagnets exhibit intriguing low‐dimensional semiconducting behavior with both charge and spin as carrier controls. However, synthesis of these compounds is challenging and remains rare. Here, first‐principles based high‐throughput search is conducted to screen potentially stable mixed metal phosphorous trichalcogenides (MM′P2X6, where M and M′are transition metals and X is a chalcogenide) that have a wide range of tunable bandgaps and interesting magnetic properties. Among the potential candidates, a stable semiconducting layered magnetic material, CdFeP2Se6, that exhibits a short‐range antiferromagnetic order at
T N = 21 K with an indirect bandgap of 2.23 eV is successfully synthesized . This work suggests that high‐throughput screening assisted synthesis can be an effective method for layered magnetic materials discovery. -
Abstract Superior infrared nonlinear optical (NLO) crystals are in urgent demand in the development of lasers and optical technologies for communications and computing. The critical challenge is to find a crystal with large non‐resonant phase‐matchable NLO coefficients and high laser damage threshold (LDTs) simultaneously, which however scale inversely. This work reports such a material, MgSiP2,that exhibits a large second harmonic generation (SHG) coefficient of
d 14≈d 36= 89 ± 5 pm V−1at 1550 nm fundamental wavelength, surpassing the commercial NLO crystals AgGaS2, AgGaSe2, and ZnGeP2. First principles theory reveals the polarizability and geometric arrangement of the [SiP4] tetrahedral units as the origin of this large nonlinear response. Remarkably, it also exhibits a high LDT value of 684 GW cm−2, which is six times larger than ZnGeP2and three times larger than CdSiP2. It has a wide transparency window of 0.53–10.35 µm, allowing broadband tunability. Further, it is Type I and Type II phase‐matchable with large effective SHG coefficients ofd eff,I≈80.2 pm V−1andd eff,II≈73.4 pm V−1. The outstanding properties of MgSiP2make it a highly attractive candidate for optical frequency conversion in the infrared.