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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:

An emerging concept for identification of different types of spin liquids [C. Broholm et al., Science 367, eaay0668 (2020)] is through the use of spontaneous spin noise [S. Chatterjee, J. F. Rodriguez-Nieva, E. Demler, Phys. Rev. B 99, 104425 (2019)]. Here, we develop spin noise spectroscopy for spin liquid studies by considering Ca10Cr7O28, a material hypothesized to be either a quantum or a spiral spin liquid (SSL). By enhancing techniques introduced for magnetic monopole noise studies [R. Dusad et al., Nature 571, 234–239 (2019)], we measure the time and temperature dependence of spontaneous flux Φ(t, T) and thus magnetization M(t, T) of Ca10Cr7O28 samples. The resulting power spectral density of magnetization noise SMω, T reveals intense spin fluctuations with SMω, T∝ω-α(T) and 0.84

Abstract:

A recent advance in the study of emergent magnetic monopoles was the discovery that monopole motion is restricted to dynamical fractal trajectories [J. N. Hallén et al., Science 378, 1218 (2022)], thus explaining the characteristics of magnetic monopole noise spectra [R. Dusad et al., Nature 571, 234 (2019); A. M. Samarakoon et al., Proc. Natl. Acad. Sci. U.S.A. 119, e2117453119 (2022)]. Here, we apply this novel theory to explore the dynamics of field-driven monopole currents, finding them composed of two quite distinct transport processes: initially swift fractal rearrangements of local monopole configurations followed by conventional monopole diffusion. This theory also predicts a characteristic frequency dependence of the dissipative loss angle for AC field–driven currents. To explore these novel perspectives on monopole transport, we introduce simultaneous monopole current control and measurement techniques using SQUID-based monopole current sensors. For the canonical material Dy2Ti2O7, we measure Φ(t), the time dependence of magnetic flux threading the sample when a net monopole current J(t) = Φ̇ (t)∕0 is generated by applying an external magnetic field B0(t). These experiments find a sharp dichotomy of monopole currents, separated by their distinct relaxation time constants before and after t ~600 μs from monopole current initiation. Application of sinusoidal magnetic fields B0(t) = Bcos(t) generates oscillating monopole currents whose loss angle ( f ) exhibits a characteristic transition at frequency f ≈ 1.8 kHz over the same temperature range. Finally, the magnetic noise power is also dichotomic, diminishing sharply after t ~600 μs. This complex phenomenology represents an unprecedented form of dynamical heterogeneity generated by the interplay of fractionalization and local spin configurational symmetry.

Abstract:

Spin-orbit Mott insulators composed of t_{2g}^{4} transition metal ions may host excitonic magnetism due to the condensation of spin-orbital J=1 triplons. Prior experiments suggest that the 4d antiferromagnet Ca_{2}RuO_{4} embodies this notion, but a J=0 nonmagnetic state as a basis of the excitonic picture remains to be confirmed. We use Ru L_{3}-edge resonant inelastic x-ray scattering to reveal archetypal J multiplets with a J=0 ground state in the cubic compound K_{2}RuCl_{6}, which are well described within the LS-coupling scheme. This result highlights the critical role of unquenched orbital moments in 4d-electron compounds and calls for investigations of quantum criticality and excitonic magnetism on various crystal lattices.