Quantum and thermal spin relaxation in diluted spin ice: Dy(2-x)MxTi2O7 (M = Lu, Y)

We have studied the low temperature a.c. magnetic susceptibility of the diluted spin ice compound Dy(2-x)MxTi2O7, where the magnetic Dy ions on the frustrated pyrochlore lattice have been replaced with non-magnetic ions, M = Y or Lu. We examine a broad range of dilutions, 0 <= x <= 1.98, and we find that the T ~ 16 K freezing is suppressed for low levels of dilution but re-emerges for x > 0.4 and persists to x = 1.98. This behavior can be understood as a non-monotonic dependence of the quantum spin relaxation time with dilution. The results suggest that the observed spin freezing is fundamentally a single spin process which is affected by the local environment, rather than the development of spin-spin correlations as earlier data suggested.Comment: 26 pages, 9 figure

Quantum-Classical Reentrant Relaxation Crossover in Dy2Ti2O7 Spin-Ice

We have studied spin relaxation in the spin ice compound Dy2Ti2O7 through measurements of the a.c. magnetic susceptibility. While the characteristic spin relaxation time is thermally activated at high temperatures, it becomes almost temperature independent below Tcross ~ 13 K, suggesting that quantum tunneling dominates the relaxation process below that temperature. As the low-entropy spin ice state develops below Tice ~ 4 K, the spin relaxation time increases sharply with decreasing temperature, suggesting the emergence of a collective degree of freedom for which thermal relaxation processes again become important as the spins become highly correlated

Low Temperature Spin Freezing in Dy2Ti2O7 Spin Ice

We report a study of the low temperature bulk magnetic properties of the spin ice compound Dy2Ti2O7 with particular attention to the (T < 4 K) spin freezing transition. While this transition is superficially similar to that in a spin glass, there are important qualitative differences from spin glass behavior: the freezing temperature increases slightly with applied magnetic field, and the distribution of spin relaxation times remains extremely narrow down to the lowest temperatures. Furthermore, the characteristic spin relaxation time increases faster than exponentially down to the lowest temperatures studied. These results indicate that spin-freezing in spin ice materials represents a novel form of magnetic glassiness associated with the unusual nature of geometrical frustration in these materials.Comment: 24 pages, 8 figure

Magnetisation Studies of Geometrically Frustrated Antiferromagnets SrLn2O4, with Ln = Er, Dy and Ho

We present the results of susceptibility \chi(T) and magnetisation M(H) measurements performed on single crystal samples of the rare-earth oxides SrLn2O4 (Ln = Er, Dy and Ho). The measurements reveal the presence of magnetic ordering transition in SrHo2O4 at 0.62 K and confirm that SrEr2O4 orders magnetically at 0.73 K, while in SrDy2O4 such a transition is absent down to at least 0.5 K. The observed ordering temperatures are significantly lower than the Curie-Weiss temperatures, \theta_{CW}, obtained from the high-temperature linear fits to the 1/\chi(T) curves, which implies that these materials are subject to geometric frustration. Strong anisotropy found in the \chi(T) curves for a field applied along the different crystallographic directions is also evident in the M(H) curves measured both above and below the ordering temperatures. For all three compounds the magnetisation plateaux at approximately one third of the magnetisation saturation values can be seen for certain directions of applied field, which is indicative of field-induced stabilisation of a collinear {\it two-up one-down} structure.Comment: 6 pages, 6 figure

Recent advances in unveiling active sites in molybdenum sulfide-based electrocatalysts for the hydrogen evolution reaction

Hydrogen has received significant attention as a promising future energy carrier due to its high energy density and environmentally friendly nature. In particular, the electrocatalytic generation of hydrogen fuel is highly desirable to replace current fossil fuel-dependent hydrogen production methods. However, to achieve widespread implementation of electrocatalytic hydrogen production technology, the development of highly active and durable electrocatalysts based on Earth-abundant elements is of prime importance. In this context, nanostructured molybdenum sulfides (MoS x ) have received a great deal of attention as promising alternatives to precious metal-based catalysts. In this focus review, we summarize recent efforts towards identification of the active sites in MoS x -based electrocatalysts for the hydrogen evolution reaction (HER). We also discuss recent synthetic strategies for the engineering of catalyst structures to achieve high active site densities. Finally, we suggest ongoing and future research challenges in the design of advanced MoS x -based HER electrocatalysts

Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution

Low-cost, layered transition-metal dichalcogenides (MX_2) based on molybdenum and tungsten have attracted substantial interest as alternative catalysts for the hydrogen evolution reaction (HER). These materials have high intrinsic per-site HER activity; however, a significant challenge is the limited density of active sites, which are concentrated at the layer edges. Here we unravel electronic factors underlying catalytic activity on MX_2 surfaces, and leverage the understanding to report group-5 MX_2 (H-TaS_2 and H-NbS_2) electrocatalysts whose performance instead mainly derives from highly active basal-plane sites, as suggested by our first-principles calculations and performance comparisons with edge-active counterparts. Beyond high catalytic activity, they are found to exhibit an unusual ability to optimize their morphology for enhanced charge transfer and accessibility of active sites as the HER proceeds, offering a practical advantage for scalable processing. The catalysts reach 10 mA cm^(−2) current density at an overpotential of ∼50–60 mV with a loading of 10–55 μg cm^(−2), surpassing other reported MX2 candidates without any performance-enhancing additives