The Heusler-derived multiferroic alloy Ni${}_{50-x}$Co${}_x$Mn${}_{40}$Sn${}_{10}$ has recently been shown to exhibit, at just above room temperature, a highly reversible martensitic phase transformation with an unusually large magnetization change. In this work the nature of the magnetic ordering above and below this transformation has been studied in detail in the critical composition range $x$ $=$ 6–8 via temperature-dependent (5–600 K) magnetometry and small-angle neutron scattering (SANS). We observe fairly typical paramagnetic to long-range-ordered ferromagnetic phase transitions on cooling to 420–430 K, with the expected critical spin fluctuations, followed by first-order martensitic phase transformations to a nonferromagnetic state below 360–390 K. The static magnetization reveals complex magnetism in this low-temperature nonferromagnetic phase, including a Langevin-like field dependence, distinct spin freezing near 60 K, and significant exchange bias effects, consistent with superparamagnetic blocking of ferromagnetic clusters of nanoscopic dimensions. We demonstrate that these spin clusters, whose existence has been hypothesized in a variety of martensitic alloys exhibiting competition between ferromagnetic and antiferromagnetic exchange interactions, can be directly observed by SANS. The scattering data are consistent with a liquidlike spatial distribution of interacting magnetic clusters with a mean center-to-center spacing of 12 nm. Considering the behavior of the superparmagnetism, cooling-field and temperature-dependent exchange bias, and magnetic SANS, we discuss in detail the physical form and origin of these spin clusters, their intercluster interactions, the nature of the ground-state magnetic ordering in the martensitic phase, and the implications for our understanding of such alloy systems.

Years of intensive work on perovskite manganites has led to a detailed understanding of the phenomena that emerge from competition between the electronic and lattice degrees of freedom in these correlated electron systems. It is well understood that the related cobaltites provide an additional spin-state degree of freedom. Here, we use the magnetic properties of a particular cobaltite, ${\text{Pr}}_{1-x}{\text{Sr}}_x{\text{CoO}}_3$, to demonstrate the vital role played by a further ingredient often negligible in manganites; magnetocrystalline anisotropy. ${\text{Pr}}_{1-x}{\text{Sr}}_x{\text{CoO}}_3$ exhibits an anomalous “double magnetic transition” that cannot be ascribed to a spin-state transition or the usual charge/orbital/antiferromagnetic ordering and has thus far evaded explanation. We show that this is actually due to a coupled structural/magnetocrystalline anisotropy transition driven, in this case, by Pr-O hybridization. The results point to the existence of a distinct class of phenomena in the cobaltites due to the unique interplay between structure and magnetic anisotropy.

In recent years it has become clear that complex oxides provide an exceptional platform for the discovery of new physics as well as a considerable challenge to our understanding of correlated electrons. The tendency of these materials to display nanoscale electronic and magnetic inhomogeneity is a good example. Here, we have applied a variety of experimental techniques to investigate this magneto-electronic phase separation in a model system —the doped cobaltite La_1−xSr_xCoO₃. Comparing experimental data over a wide range of doping with statistical simulations, we conclude that the magneto-electronic inhomogeneity is driven solely by inevitable local compositional fluctuations at nanoscopic length scales. The phase separation is thus doping fluctuation-driven rather than electronically driven, meaning that more complex electronic phase separation models are not required to understand the observed phenomena in this material.

A potentially new kind of glass transition may exist among phase-separated regions in ${\text{La}}_{0.215}{\text{Pr}}_{0.41}{\text{Ca}}_{3/8}{\text{MnO}}_3$. We have observed a very large damping of ultrasonic waves in the dynamically phase-segregated state of this material. This damping is connected to the motion of structural interfaces at megahertz frequencies, which is a much faster time scale than that of magnetic relaxation effects. At lower temperatures, the dynamics of the phase-separated state freeze at the glass transition. Our observations link the onset of this freezing to a sudden decrease in mobility of interfaces between structurally dissimilar phase-segregated regions.

We report an evolution of an all-digital ultrasonic pulse technique for measurements of elastic constants of solids. An unambiguous analytical procedure is described for determining the correct time delay of echoes without any need for actual echo overlap. We also provide a simple procedure for making corrections for transducer-bond-induced phase shifts. The precision of a measurement made with this system at ambient temperature exceeds one part in 107 without the use of mixers, gates, time delays, and other complications normally associated with such measurements.