Nano-compositional imaging of the lanthanum silicide system at THz wavelengths.

Terahertz scattering-type scanning near-field optical microscopy (THz-sSNOM) provides a noninvasive way to probe the low frequency conductivity of materials and to characterize material compositions at the nanoscale. However, the potential capability of atomic compositional analysis with THz nanoscopy remains largely unexplored. Here, we perform THz near-field imaging and spectroscopy on a model rare-earth alloy of lanthanum silicide (La-Si) which is known to exhibit diverse compositional and structural phases. We identify subwavelength spatial variations in conductivity that is manifested as alloy microstructures down to much less than 1 µm in size and is remarkably distinct from the surface topography of the material. Signal contrasts from the near-field scattering responses enable mapping the local silicon/lanthanum content differences. These observations demonstrate that THz-sSNOM offers a new avenue to investigate the compositional heterogeneity of material phases and their related nanoscale electrical as well as optical properties.

Complex Magnetism of Lanthanide Intermetallics and the Role of their Valence Electrons: Ab Initio Theory and Experiment.

We explain a profound complexity of magnetic interactions of some technologically relevant gadolinium intermetallics using an ab initio electronic structure theory which includes disordered local moments and strong f-electron correlations. The theory correctly finds GdZn and GdCd to be simple ferromagnets and predicts a remarkably large increase of Curie temperature with a pressure of +1.5 K kbar(-1) for GdCd confirmed by our experimental measurements of +1.6 K kbar(-1). Moreover, we find the origin of a ferromagnetic-antiferromagnetic competition in GdMg manifested by noncollinear, canted magnetic order at low temperatures. Replacing 35% of the Mg atoms with Zn removes this transition, in excellent agreement with long-standing experimental data.

Anomalous Schottky specific heat and structural distortion in ferromagnetic PrAl2.

Unique from other rare earth dialuminides, PrAl(2) undergoes a cubic to tetragonal distortion below T = 30 K in a zero magnetic field, but the system recovers its cubic symmetry upon the application of an external magnetic field of 10 kOe via a lifting of the 4f crystal field splitting. The nuclear Schottky specific heat in PrAl(2) is anomalously high compared to that of pure Pr metal. First principles calculations reveal that the 4f crystal field splitting in the tetragonally distorted phase of PrAl(2) underpins the observed unusual low temperature phenomena.

Controlling magnetism of a complex metallic system using atomic individualism.

When the complexity of a metallic compound reaches a certain level, a specific location in the structure may be critically responsible for a given fundamental property of a material while other locations may not play as much of a role in determining such a property. The first-principles theory has pinpointed a critical location in the framework of a complex intermetallic compound--Gd(5)Ge(4)--that resulted in a controlled alteration of the magnetism of this compound using precise chemical tools.

Magnetostructural behavior in the non-centrosymmetric compound Nd7Pd3.

A systematic study of the physical properties and microscopic magnetism of Nd7Pd3 compound, which in the paramagnetic state crystallizes in the non-centrosymmetric hexagonal Th7Fe3-type structure (hP20-P63 mc; with a = 10.1367(1) Å and c = 6.3847(1) Å at 300 K), confirms multiple magnetic ordering transitions that occur upon cooling. Antiferromagnetic transition is observed at T N = 37 K, which is followed by ferromagnetic transformation at T C = 33 K. The first-order magnetic transition at T C is magnetoelastic: it involves a change of crystal symmetry from P63 mc to Cmc21 and leads to anisotropic changes of the unit cell parameters. While the antiferromagnetic structure is symmetry allowed in P63 mc, the ferromagnetic structure with magnetic moments along the a-direction of the original hexagonal unit cell induces the first order transition to Cmc21. Density functional theory calculations confirm the experimentally observed ground state with the a-axis as the easy magnetization direction.

Non-hysteretic first-order phase transition with large latent heat and giant low-field magnetocaloric effect.

First-order magnetic transitions (FOMTs) with a large discontinuity in magnetization are highly sought in the development of advanced functional magnetic materials. Isosymmetric magnetoelastic FOMTs that do not perturb crystal symmetry are especially rare, and only a handful of material families, almost exclusively transition metal-based, are known to exhibit them. Yet, here we report a surprising isosymmetric FOMT in a rare-earth intermetallic, Eu2In. What makes this transition in Eu2In even more remarkable is that it is associated with a large latent heat and an exceptionally high magnetocaloric effect in low magnetic fields, but with tiny lattice discontinuities and negligible hysteresis. An active role of the Eu-5d and In-4p states and a rather unique electronic structure borne by In to Eu charge transfer, altogether result in an unusual exchange mechanism that both sets the transition in motion and unveils an approach toward developing specific magnetic functionalities ad libitum.

Crystal, magnetic, calorimetric and electronic structure investigation of GdScGe1-x Sb x compounds.

Experimental investigations of crystal structure, magnetism and heat capacity of compounds in the pseudoternary GdScGe-GdScSb system combined with density functional theory projections have been employed to clarify the interplay between the crystal structure and magnetism in this series of RTX materials (R = rare-earth, [Formula: see text] = transition metal and X = p-block element). We demonstrate that the CeScSi-type structure adopted by GdScGe and CeFeSi-type structure adopted by GdScSb coexist over a limited range of compositions [Formula: see text]. Antimony for Ge substitutions in GdScGe result in an anisotropic expansion of the unit cell of the parent that is most pronounced along the c axis. We believe that such expansion acts as the driving force for the instability of the double layer CeScSi-type structure of the parent germanide. Extensive, yet limited Sb substitutions [Formula: see text] lead to a strong reduction of the Curie temperature compared to the GdScGe parent, but without affecting the saturation magnetization. With a further increase in Sb content, the first compositions showing the presence of the CeFeSi-type structure of the antimonide, [Formula: see text], coincide with the appearance of an antiferromagnetic phase. The application of a finite magnetic field reveals a jump in magnetization toward a fully saturated ferromagnetic state. This antiferro-ferromagnetic transformation is not associated with a sizeable latent heat, as confirmed by heat capacity measurements. The electronic structure calculations for [Formula: see text] indicate that the key factor in the conversion from the ferromagnetic CeScSi-type to the antiferromagnetic CeFeSi-type structure is the disappearance of the induced magnetic moments on Sc. For the parent antimonide, heat capacity measurements indicate an additional transition below the main antiferromagnetic transition.