Search

Metal carbides, nitrides, or carbonitrides of early transition metals, better known as MXenes, possess notable structural, electrical, and magnetic properties. Analyzing electronic structures by calculating structural stability, band structure, density of states, Bader charge transfer, and work functions utilizing first principle calculations, we revealed that titanium nitride Mxenes, namely Ti$_2$N and Ti$_3$N$_2$, have excess anionic electrons in their pseudo-atomic structure inside the crystal lattice, making them MXene electrides. Bulk Ti$_3$N$_2$ has competing antiferromagnetic (AFM) and ferromagnetic(FM) configurations with slightly more stable AFM configurations, while the Ti$_2$N MXene is nonmagnetic. Although Ti$_3$N$_2$ favors AFM configurations with hexagonal crystal systems having $6/mmm$ point group symmetry, Ti$_3$N$_2$ does not support altermagnetism. The monolayer of the Ti$_3$N$_2$ MXene is a ferromagnetic electride. These unique properties of having non-nuclear interstitial anionic electrons in the electronic structure of titanium nitride MXene have not yet been reported in the literature. Density functional theory calculations show TiN is neither an electride, MXene, or magnetic.

In actinide systems, the 5f electrons experience a uniquely delicate balance of effects and interactions having similar energy scales, which are often difficult to properly disentangle. This interplay of factors such as the dual nature of 5f-states, strong electronic correlations, and strong spin-orbit coupling results in electronically unusual and intriguing behavior such as multi-k antiferromagnetic ordering, multipolar ordering, mott-physics, mixed valence configurations, and more. Despite the inherent allure of their exotic properties, the exploratory science of even the more basic, binary systems like the actinide oxides has been limited due to their toxicity, radioactivity, and reactivity. In this article, we provide an overview of the available synthesis techniques for selected binary actinide oxides, including the actinide dioxides, sesquioxides, and a selection of higher oxides. For these oxides, we also review and evaluate the current state of knowledge of their crystal structures and magnetic properties. In many aspects, substantial knowledge gaps exist in the current body of research on actinide oxides related to understanding their electronic ground states. Bridging these gaps is vital for improving not only a fundamental understanding of these systems but also of future nuclear technologies. To this end, we note the experimental techniques and necessary future investigations which may aid in better elucidating the nature of these fascinating systems.

The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unreported modulation vectors characterizing the ordered spin configuration which exhibit changes in magnitude and direction that are phase dependent. Between 5.9 and 7.6 K the additional modulation vector has a magnitude $Q$ =0.12 \AA$^{-1}$ and is primarily due to order of the Nd layers which contain a center of inversion. In this region of the phase diagram, the SANS measurements also identify a phase boundary at $\approx$1 T. An important feature of these modulation vectors is that they indicate the presence of nanometer length scale spin textures which are likely stabilized by frustrated Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions rather than a Dzyaloshinskii-Moriya (DM) exchange interaction., Comment: 16 pages, 15 figures

The experimental realization of magnetic skyrmions in centrosymmetric materials has been driven by theoretical understanding of how a delicate balance of anisotropy and frustration can stabilize topological spin structures in applied magnetic fields. Recently, the centrosymmetric material Gd$_{2}$PdSi$_{3}$ was shown to host a field-induced skyrmion phase, but the skyrmion stabilization mechanism remains unclear. Here, we employ neutron-scattering measurements on an isotopically-enriched polycrystalline Gd$_{2}$PdSi$_{3}$ sample to quantify the interactions that drive skyrmion formation. Our analysis reveals spatially-extended interactions in triangular planes that are consistent with an RKKY mechanism, and large ferromagnetic inter-planar magnetic interactions that are modulated by the Pd/Si superstructure. The skyrmion phase emerges from a zero-field helical magnetic order with magnetic moments perpendicular to the magnetic propagation vector, indicating that the magnetic dipolar interaction plays a significant role. Our experimental results establish an interaction space that can promote skyrmion formation, facilitating identification and design of centrosymmetric skyrmion materials., Comment: 5 pages, 5 figures

Polar materials can host a variety of topologically significant magnetic phases, which often emerge from a modulated magnetic ground state. Relatively few noncentrosymmetric tetragonal materials have been shown to host topological spin textures and new candidate materials are necessary to expand the current theoretical models. This manuscript reports on the anisotropic magnetism in the polar, tetragonal material NdCoGe$_3$ via thermodynamic and neutron diffraction measurements. The previously reported $H$-$T$ phase diagram is updated to include several additional phases, which exist for both $H$ = 0 and with an applied field H$\perp$ c. Neutron diffraction data reveal that the magnetic structures below $T_{N1}$ = 3.70 K and $T_{N2}$ = 3.50 K are incommensurate, with a ground state magnetic order that is incommensurate in all directions with the propagation vector $\vec{k}$ = (0.494, 0.0044, 0.385) at 1.8 K. A unique magnetic structure solution is not achievable, but the possible single and multi-$\vec{k}$ spin models are discussed. These results demonstrate that NdCoGe3 hosts complicated magnetic order derived from modulated magnetic moments., Comment: 11 pages, 10 figures

Spin-1/2 chains with alternating antiferromagnetic (AF) and ferromagnetic (FM) couplings exhibit quantum entanglement like the integer-spin Haldane chains and might be similarly utilized for quantum computations. Such alternating AF-FM chains have been proposed to be realized in the distorted honeycomb-lattice compound Na$_2$Cu$_2$TeO$_6$, but to confirm this picture a comprehensive understanding of the exchange interactions including terms outside of the idealized model is required. Here we employ neutron scattering to study the spin dynamics in Na$_2$Cu$_2$TeO$_6$ and accurately determine the coupling strengths through the random phase approximation and density functional theory (DFT) approaches. We find the AF and FM intrachain couplings are the dominant terms in the spin Hamiltonian, while the interchain couplings are AF but perturbative. This hierarchy in the coupling strengths and the alternating signs of the intrachain couplings can be understood through their different exchange paths. Our results establish Na$_2$Cu$_2$TeO$_6$ as a weakly-coupled alternating AF-FM chain compound and reveal the robustness of the gapped ground state in alternating chains under weak interchain couplings., Comment: 9 pages, 7 figures

Single crystals of Nd$_2$O$_3$ were grown and characterized using neutron scattering and thermodynamic measurements. Nd$_2$O$_3$ has long-range antiferromagnetic order below $T_{\rm N}$ = 0.55 K and specific heat measurements have demonstrated that a significant amount of the magnetic entropy is released above $T_{\rm N}$. Inelastic neutron scattering experiments reveal a magnetic mode(s) with little dispersion peaked at $\approx$ 0.37 meV that is of greatest intensity below $T_{\rm N}$ but persists above 2$T_{\rm N}$. This persistence of dynamic correlations is likely related to frustrated interactions associated with the nearly-ideal stacked triangular lattice geometry of $J_{\textrm{eff}}$ = 1/2 spins on Nd$^{3+}$ ions. The magnetization is observed to be strongly anisotropic at all temperatures due to crystal field effects, with easy-plane anisotropy observed. A non-compensated magnetic structure is inferred from the temperature-dependence of the magnetization when a magnetic field of sufficient strength is applied within the basal plane near $T_{\rm N}$, and the evolution of the long-range order is summarized in a temperature-field phase diagram., Comment: 11 pages

The magnetic excitation spectrum of the quantum magnet YbCl$_3$ is studied with inelastic neutron scattering. The spectrum exhibits an unusually sharp feature within a broad continuum, as well as conventional spin waves. By including both transverse and longitudinal channels of the neutron response, linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice reproduces all of the key features in the spectrum. In particular, the broad continuum corresponds to a two-magnon contribution from the longitudinal channel, while the sharp feature within this continuum is identified as a Van Hove singularity in the joint density of states, which indicates the two-dimensional nature of the two-magnon continuum. We term these singularities magneto-caustic features in analogy with caustic features in ray optics where focused envelopes of light are generated when light passes through or reflects from curved or distorted surfaces. The experimental demonstration of a sharp Van Hove singularity in a two-magnon continuum is important because analogous features in potential two-spinon continua could distinguish quantum spin liquids from merely disordered systems. These results establish YbCl$_3$ as a nearly ideal two-dimensional honeycomb lattice material hosting strong quantum effects in the unfrustrated limit., Comment: 17 pages, 5 figures

We report the discovery of Ce$_3$Ir$_4$Ge$_{13}$, a new Remeika phase compound with a complex array of structural, electronic, and magnetic properties. Our single crystal x-ray diffraction measurements show that Ce$_3$Ir$_4$Ge$_{13}$ forms in the tetragonally distorted $I4_1/amd$ space group. The electrical resistivity is almost temperature independent over three decades in temperature, from 0.4 K to 400 K, while the Hall coefficient measurements are consistent with a low-carrier semimetal. Magnetic susceptibility measurements reveal an effective moment of $\mu^{\text{exp}}_{\text{eff}} = 1.87 \mu_B$/Ce, suggesting that this material has a mixture of magnetic Ce$^{3+}$ and non-magnetic Ce$^{4+}$. Upon cooling, Ce$_3$Ir$_4$Ge$_{13}$ first enters a short range magnetically ordered state below $T_{\text{SRO}}=10$ K, marked by a deviation from Curie-Weiss behavior in susceptibility and a broad field-independent heat capacity anomaly. At lower temperatures, we observe a second, sharper peak in the heat capacity at $T^* = 1.7$ K, concurrent with a splitting of the field-cooled and zero-field-cooled susceptibilities. A small resistivity drop at $T^*$ suggests a loss of spin disorder scattering consistent with a magnetic ordering or spin freezing transition. Ce$_3$Ir$_4$Ge$_{13}$ is therefore a rare example of an inhomogeneous mixed valence compound with a complex array of thermodynamic and transport properties., Comment: 8 pages, 6 figures, accepted for publication in Phys. Rev. Materials

We study the correlated quantum magnet, YbCl$_3$, with neutron scattering, magnetic susceptibility, and heat capacity measurements. The crystal field Hamiltonian is determined through simultaneous refinements of the inelastic neutron scattering and magnetization data. The ground state doublet is well isolated from the other crystal field levels and results in an effective spin-1/2 system with local easy plane anisotropy at low temperature. Cold neutron spectroscopy shows low energy excitations that are consistent with nearest neighbor antiferromagnetic correlations of reduced dimensionality., Comment: main paper plus supplemental information

Co substituted Ni$_{1-x}$Co$_x$Br$_2$ (0 $\leq~x~\leq$ 1) single crystals were synthesized using vapor transport. The physical properties of the crystals were characterized by x-ray powder diffraction, magnetization, and specific heat measurements. Room temperature x-ray powder diffraction data indicate a change from the CdCl$_2$ structure type to the CdI$_2$ structure type occurs within 0.56 $<~x~<$ 0.76. NiBr$_2$ has a commensurate antiferromagnetic phase below $T_{\rm N} \approx$ 46 K and an incommensurate magnetic ground state below $T_{\rm IC} \approx$ 20 K. Both magnetic transitions are affected by cobalt substitution, and the incommensurate phase transition is present up to at least $x$ = 0.56. The evolution of magnetism has been studied as a function of cobalt content and is summarized in the temperature-composition phase diagram.

We show that Ce- and Yb-based Kondo-lattice ferromagnets order mainly along the magnetically hard direction of the ground state Kramers doublet determined by crystalline electric field (CEF). Here we argue that this peculiar phenomenon, that was believed to be rare, is instead the standard case. Moreover, it seems to be independent on the Curie temperature $T_\mathrm{C}$, crystalline structure, size of the ordered moment and type of ground state wave function. On the other hand, all these systems show the Kondo coherence maximum in the temperature dependence of the resistivity just above $T_\mathrm{C}$ which indicates a Kondo temperature of a few Kelvin. An important role of fluctuations is indicated by the non-mean-field like transition in specific heat measurements as well as by the suppression of this effect by a strong Ising-like anisotropy. We discuss possible theoretical scenarios.

Ferromagnetic Kondo lattice compounds are far less common than their antiferromagnetic analogs. In this work, we report the discovery of a new ferromagnetic Kondo lattice compound, YbIr3Ge7. Like almost all ferromagnetic Kondo lattice systems, YbIr3Ge7 shows magnetic order with moments aligned orthogonal to the crystal electric field (CEF) easy axis. YbIr3Ge7 is unique in that it is the only member of this class of compounds that crystallizes in a rhombohedral structure with a trigonal point symmetry of the magnetic site, and it lacks broken inversion symmetry at the local moment site. AC magnetic susceptibility, magnetization, and specific heat measurements show that YbIr3Ge7 has a Kondo temperature TK = 14 K and a Curie temperature TC = 2.4 K. Ferromagnetic order occurs along the crystallographic [100] hard CEF axis despite the large CEF anisotropy of the ground state Kramers doublet with a saturation moment along [001] almost four times larger than the one along [100]. This implies that a mechanism which considers the anisotropy in the exchange interaction to explain the hard axis ordering is unlikely. On the other hand, the broad second-order phase transition at TC favors a fluctuation-induced mechanism.

Inelastic neutron scattering experiments have been conducted to investigate the semimetal system Yb$_3$Ir$_4$Ge$_{13}$. No clear crystal-field-split levels were observed up to an excitation energy of 60 meV, while a magnetic excitation appears at low energy below approximately 3 meV. This excitation shows a short spatial correlation, and an energy spectrum is reproduced by an imaginary part of generalized magnetic susceptibility on the basis of a damped harmonic oscillator model. The magnetic excitation emerges simultaneously with an anomalous electrical-resistivity enhancement below 20 K. The close relationship between the magnetic and transport behaviors evidences that the semimetal carriers are scattered by magnetic fluctuation dominated by the Yb $4f$ state., Comment: 6 pages, 4 figures

The crystalline electric field (CEF) of Ce3+ in trigonal symmetry has recently become of some relevance, for instance, in the search of frustrated magnetic systems. Fortunately, it is one of the CEF case in which a manageable analytic solution can be obtained. Here, we present this solution for the general case, and use this result to determine the CEF scheme of the new compound CeIr3Ge7 with the help of T-dependent susceptibility and isothermal magnetization measurements. The resulting CEF parameters B20 = 34.4 K, B40 = 0.82 K and B43 = 67.3 K correspond to an exceptional large CEF splittings of the first and second excited levels, 374 K and 1398 K, and a large mixing between the +-|5/2> and the -+|1/2> states. This indicates a very strong easy plane anisotropy with an unusual small c-axis moment. Using the same general expressions, we show that the properties of the recently reported system CeCd3As3 can also be described by a similar CEF scheme, providing a much simpler explanation for its magnetic properties than the initial proposal. Moreover, a similar strong easy plane anisotropy has also been reported for the two compounds CeAuSn and CePdAl4Ge2, indicating that the CEF scheme elaborated here for CeIr3Ge7 corresponds to an exemplary case for Ce3+ in trigonal symmetry., Comment: 10 pages, 7 figures

Kondo-based semimetals and semiconductors are of extensive current interest as a viable platform for strongly correlated states. It is thus important to understand the routes towards such dilute-carrier correlated states. One established pathway is through Kondo effect in metallic non-magnetic analogues. Here we advance a new mechanism, through which Kondo-based semimetals develop out of conduction electrons with a low carrier-density in the presence of an even number of rare-earth sites. We demonstrate this effect by studying the Kondo material Yb3Ir4Ge13 along with its closed-f-shell counterpart, Lu3Ir4Ge13. Through magnetotransport, optical conductivity and thermodynamic measurements, we establish that the correlated semimetallic state of Yb3Ir4Ge13 below its Kondo temperature originates from the Kondo effect of a low carrier conduction-electron background. In addition, it displays fragile magnetism at very low temperatures, which, in turn, can be tuned to a non Fermi liquid regime through Lu-for-Yb substitution. These findings are connected with recent theoretical studies in simplified models. Our results open an entirely new venue to explore the strong correlation physics in a semimetallic environment.

CeIr$_3$Ge$_7$ is an antiferromagnetic metal with a remarkably low ordering temperature $T_{\rm N}$ = 0.63 K, while most Ce-based magnets order between 2 and 15 K. Thermodynamic and transport properties as a function of magnetic field or pressure do not show signatures of Kondo correlations, interaction competition, or frustration, as had been observed in a few antiferromagnets with comparably low or lower $T_{\rm N}$. The averaged Weiss temperature measured below 10 K is comparable to $T_{\rm N}$ suggesting that the RKKY exchange coupling is very weak in this material. The unusually low $T_{\rm N}$ in CeIr$_3$Ge$_7$ can therefore be attributed to the large Ce-Ce bond length of about 5.7 {\AA}, which is about 1.5 {\AA} larger than in the most Ce-based intermetallic systems., Comment: 4 figures

We report complex metamagnetic transitions in single crystals of the new low carrier Kondo antiferromagnet YbRh3Si7. Electrical transport, magnetization, and specific heat measurements reveal antiferromagnetic order at T_N = 7.5 K. Neutron diffraction measurements show that the magnetic ground state of YbRh3Si7 is a collinear antiferromagnet where the moments are aligned in the ab plane. With such an ordered state, no metamagnetic transitions are expected when a magnetic field is applied along the c axis. It is therefore surprising that high field magnetization, torque, and resistivity measurements with H||c reveal two metamagnetic transitions at mu_0H_1 = 6.7 T and mu_0H_2 = 21 T. When the field is tilted away from the c axis, towards the ab plane, both metamagnetic transitions are shifted to higher fields. The first metamagnetic transition leads to an abrupt increase in the electrical resistivity, while the second transition is accompanied by a dramatic reduction in the electrical resistivity. Thus, the magnetic and electronic degrees of freedom in YbRh3Si7 are strongly coupled. We discuss the origin of the anomalous metamagnetism and conclude that it is related to competition between crystal electric field anisotropy and anisotropic exchange interactions., Comment: 23 pages and 4 figures in the main text. 7 pages and 5 figures in the supplementary material