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Abstract:

The honeycomb-lattice system $\alpha \text{−}{\mathrm{RuI}}_3$ is isostructural to the widely studied $\alpha \text{−}{\mathrm{RuCl}}_3$ compound which was identified as a potential Kitaev system but exhibits, instead of spin liquid behavior, a magnetically ordered zigzag ground state which sets in below 14 K. Here we show experimentally that, in contrast, the spins in $\alpha \text{−}{\mathrm{RuI}}_3$ remain dynamic down to at least 50 mK. We study the spin dynamics using muon-spin relaxation methods and determine the presence of low-frequency fluctuations which are characteristic of a two-dimensional system.

Abstract:

The kagome lattice of spin-1/2 copper atoms in herbertsmithite is conjectured to sustain a quantum spin liquid state with spinon quasiparticles. Ideally, the kagome crystal planes are each separated by a plane of spinless zinc atoms. However, in real crystals, some spin-1/2 copper atoms substitute randomly onto these inter-kagome zinc sites. Here we reconceptualize such ‘impurity’ atoms as quantum witness spins whose dynamics is designed to probe the spin liquid state. We then introduce spin noise spectroscopy to measure the frequency and temperature dependence of witness spin dynamics, demonstrating that their phenomenology is consistent with extensive interactions between witness spins mediated by propagation of spinons through a quantum spin liquid. Ultimately, a sharp transition occurs at around 260 mK, below which the properties of both spin noise and magnetic susceptibility suggest that the witness spins form a spin glass phase. Among the theoretical models considered, we demonstrate that our observations are only consistent with spinon-mediated interactions between witness spins by either a Z2 or U(1) quantum spin liquid, with the former model more closely matching the data. Our work demonstrates that quantum mechanical witness spins may now conceivably be used as a widely applicable probe of quantum spin liquid physics.

Abstract:

Dynamical heterogeneity, in which transitory local fluctuations occur in the conformation and dynamics of constituent particles, is widely hypothesized to be essential to the evolution of supercooled liquids into the structural glass state. Yet its microscopic spatiotemporal phenomenology is challenging to detect directly in molecular glass forming liquids. Because recent theoretical advances predict that corresponding dynamical heterogeneity could occur in supercooled magnetic monopole fluids (Proc. Nat. Acad. Sci. 112, 8549 (2015)), we searched for such phenomena in Dy2Ti2O7. By measuring its microsecond-resolved spontaneous magnetization fluctuations M(t, T) we detected a sharp bifurcation in monopole noise characteristics below T≈1,500 mK, with the appearance of powerful spontaneous monopole current bursts. This intense dynamics emerges upon entering the supercooled monopole fluid regime, reaches maximum strength near T≈750 mK and then collapses along with coincident loss of ergodicity approaching Tg≈250 mK. Moreover, when the four-point dynamical susceptibility χ4(τ, T) is determined directly from temperature dependence of correlations in M(t, T), it evolves as predicted when dynamical heterogeneity is present, revealing its simultaneously and rapidly escalating length and time scales, ξ(T) and τ4(T). This overall phenomenology greatly expands our empirical knowledge of supercooled monopole fluids and, more generally, demonstrates techniques for detection of the time sequence, magnitude, statistics, and correlations of dynamical heterogeneity, access to which may greatly accelerate fundamental vitrification studies.

Abstract:

We present a first-principles investigation of the spin-ice state in Dy2Ti2O7 using a magnetic source-free exchange and correlation (xc) functional, implemented in the Castep electronic-structure code. By comparing results from the conventional local spin-density approximation, we show that a spin-ice state in Dy2Ti2O7 can be reliably obtained by removing the magnetic sources from the xc contributions to the potential, and we contrast this against the computed ground states of other frustrated pyrochlore magnets.