Evidence for a dynamical ground state in the frustrated pyrohafnate Tb2Hf2O7

We report the physical properties of Tb2Hf2O7 based on ac magnetic susceptibility \chi_ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H), and heat capacity C_p(T) measurements combined with muon spin relaxation (\muSR) and neutron powder diffraction measurements. No evidence for long-range magnetic order is found down to 0.1 K. However, \chi_ac(T) data present a frequency-dependent broad peak (near 0.9 K at 16 Hz) indicating slow spin dynamics. The slow spin dynamics is further evidenced from the \muSR data (characterized by a stretched exponential behavior) which show persistent spin fluctuations down to 0.3 K. The neutron powder diffraction data collected at 0.1 K show a broad peak of magnetic origin (diffuse scattering) but no magnetic Bragg peaks. The analysis of the diffuse scattering data reveals a dominant antiferromagnetic interaction in agreement with the negative Weiss temperature. The absence of long-range magnetic order and the presence of slow spin dynamics and persistent spin fluctuations together reflect a dynamical ground state in Tb2Hf2O7.Comment: 11 pages and 8 figure

Magnetic interactions and spin dynamics in the bond-disordered pyrochlore fluoride NaCaCo2_2F7_7

We report high-frequency/high-field electron spin resonance (ESR) and high-field magnetization studies on single crystals of the bond-disordered pyrochlore NaCaCo$_2$F$_7$. Frequency- and temperature-dependent ESR investigations above the freezing temperature $T_f \sim 2.4$ K reveal the coexistence of two distinct magnetic phases. A cooperative paramagnetic phase, evidenced by a gapless excitation mode, is found as well as a spin-glass phase developing below 20 K which is associated with a gapped low-energy excitation. Effective $g$-factors close to 2 are obtained for both modes in line with pulsed high-field magnetization measurements which show an unsaturated isotropic behavior up to 58 T at 2 K. In order to describe the field-dependent magnetization in high magnetic fields, we propose an empirical model accounting for highly anisotropic ionic $g$-tensors expected for this material and taking into account the strongly competing interactions between the spins which lead to a frustrated ground state. As a detailed quantitative relation between effective $g$-factors as determined from ESR and the local $g$-tensors obtained by neutron scattering [Ross et al., Phys. Rev. B 93, 014433 (2016)] is still sought after, our work motivates further theoretical investigations of the low-energy excitations in bond-disordered pyrochlores.Comment: 9 pages, 6 figure

Freezing of molecular rotation in a paramagnetic crystal studied by 31^{31}P NMR

We present a detailed $^{31}$P nuclear magnetic resonance (NMR) study of the molecular rotation in the compound [Cu(pz)$_{2}$(2-HOpy)$_{2}$](PF$_{6}$)$_{2}$, where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. Here, a freezing of the PF$_6$ rotation modes is revealed by several steplike increases of the temperature-dependent second spectral moment, with accompanying broad peaks of the longitudinal and transverse nuclear spin-relaxation rates. An analysis based on the Bloembergen-Purcell-Pound (BPP) theory quantifies the related activation energies as $E_{a}/k_{B}$ = 250 and 1400 K. Further, the anisotropy of the second spectral moment of the $^{31}$P absorption line was calculated for the rigid lattice, as well as in the presence of several sets of PF$_6$ reorientation modes, and is in excellent agreement with the experimental data. Whereas the anisotropy of the frequency shift and enhancement of nuclear spin-relaxation rates is driven by the molecular rotation with respect to the dipole fields stemming from the Cu ions, the second spectral moment is determined by the intramolecular interaction of nuclear $^{19}$F and $^{31}$P moments in the presence of the distinct rotation modes.Comment: 9 pages, 5 figures; additionally 2 pages with 3 figures of supplemental material; typos corrected, references added, supplemental material adde

Field-tunable Berezinskii-Kosterlitz-Thouless correlations in a Heisenberg magnet

We report the manifestation of field-induced Berezinskii-Kosterlitz-Thouless (BKT) correlations in the weakly coupled spin-1/2 Heisenberg layers of the molecular-based bulk material [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$. Due to the moderate intralayer exchange coupling of $J/k_\mathrm{B} = 6.8$ K, the application of laboratory magnetic fields induces a substantial $XY$ anisotropy of the spin correlations. Crucially, this provides a significant BKT regime, as the tiny interlayer exchange $J^\prime / k_\mathrm{B} \approx 1$ mK only induces 3D correlations upon close approach to the BKT transition with its exponential growth in the spin-correlation length. We employ nuclear magnetic resonance and $\mu^{+}$SR measurements to probe the spin correlations that determine the critical temperatures of the BKT transition as well as that of the onset of long-range order. Further, we perform stochastic series expansion quantum Monte Carlo simulations based on the experimentally determined model parameters. Finite-size scaling of the in-plane spin stiffness yields excellent agreement of critical temperatures between theory and experiment, providing clear evidence that the nonmonotonic magnetic phase diagram of [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ is determined by the field-tuned $XY$ anisotropy and the concomitant BKT physics.Comment: 10 pages, 7 figure

Berezinskii—Kosterlitz—Thouless correlations in copper-based quasi-2D spin systems (Review Article)

We present an overview of selected copper-based quasi-2D square-lattice spin-1/2 materials with an easy-plane anisotropy, providing the possibility to study emergent Berezinskii-Kosterlitz-Thouless (BKT) correlations. In particular, in those materials with a comparatively small exchange coupling, the effective XY anisotropy of the low-temperature spin correlations can be controlled by an applied magnetic field, yielding a systematic evolution of the BKT correlations. In cases where the residual interlayer correlations are small enough, dynamical BKT correlations in the critical regime may be observed experimentally, whereas the completion of the genuine BKT transition is preempted by the onset of long-range order. © 2023 Author(s)

Magnetization beyond the Ising limit of Ho2Ti2O7

International audienceWe report that the local Ising anisotropy in pyrochlore oxides-the crucial requirement for realizing the spin-ice state-can be broken by means of high magnetic fields. For the case of the well-established classical spin-ice compound Ho2Ti2O7 the magnetization exceeds the angle-dependent saturation value of the Ising limit using ultrahigh fields up to 120 T. However, even under such extreme magnetic fields full saturation cannot be achieved. Crystal-electric-field calculations reveal that a level crossing for two of the four ion positions leads to magnetization steps at 55 and 100 T. In addition, we show that by using a field sweep rate in the range of the spin-relaxation time the dynamics of the spin system can be probed. Exclusively at 25 ns/T, a new peak of the susceptibility appears around 2 T. We argue, this signals the crossover between spin-ice and polarized correlations

Magnetization beyond the Ising limit of Ho2Ti2O7

International audienceWe report that the local Ising anisotropy in pyrochlore oxides-the crucial requirement for realizing the spin-ice state-can be broken by means of high magnetic fields. For the case of the well-established classical spin-ice compound Ho2Ti2O7 the magnetization exceeds the angle-dependent saturation value of the Ising limit using ultrahigh fields up to 120 T. However, even under such extreme magnetic fields full saturation cannot be achieved. Crystal-electric-field calculations reveal that a level crossing for two of the four ion positions leads to magnetization steps at 55 and 100 T. In addition, we show that by using a field sweep rate in the range of the spin-relaxation time the dynamics of the spin system can be probed. Exclusively at 25 ns/T, a new peak of the susceptibility appears around 2 T. We argue, this signals the crossover between spin-ice and polarized correlations