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The suppression of ferroquadrupolar order in TmVO$_4$ in a magnetic field is well-described by the transverse field Ising model, enabling detailed studies of critical dynamics near the quantum phase transition. We describe nuclear magnetic resonance measurements in pure and Y-doped single crystals. The non-Kramers nature of the ground state doublet leads to a unique form of the hyperfine coupling that exclusively probes the transverse field susceptibility. Our results show that this quantity diverges at the critical field, in contrast to the mean-field prediction. Furthermore, we find evidence for quantum critical fluctuations present near Tm-rich regions in Y-doped crystals at levels beyond which long-range order is suppressed, suggesting the presence of quantum Griffiths phases., Comment: 13 pages, 6 figures

A major obstacle to understanding high-Tc cuprates is that superconductivity precludes observing normal-state properties at low temperatures. One prime example is the normal-state spin susceptibility: although its decrease upon cooling far above Tc typifies pseudogap behavior, its behavior at low temperatures is generally unknown. Here, our measurements in high magnetic fields expose the spin susceptibility of YBa2Cu3Oy down to low temperatures. Even though superconductivity is suppressed by the field, we uncover two thermally-activated contributions alongside a residual susceptibility at T=0 due to gapless excitations. We relate these two distinct gaps to short-range charge-density waves and to the formation of spin singlets similar to those found in certain quantum spin systems. These phenomena thus collectively contribute to the pseudogap in the spin susceptibility at low temperature, supplementing short-lived antiferromagnetism known to initiate pseudogap behavior at high temperatures. We therefore propose that the pseudogap should be regarded as a composite property.

Using spin-echo Nuclear Magnetic Resonance in the model Transverse-Field Ising system TmVO$_4$, we show that low frequency quantum fluctuations at the quantum critical point have a very different effect on $^{51}$V nuclear-spins than classical low-frequency noise or fluctuations that arise at a finite temperature critical point. Spin-echos filter out the low frequency classical noise but not the quantum fluctuations. This allows us to directly visualize the quantum critical fan and demonstrate the persistence of quantum fluctuations at the critical coupling strength in TmVO$_4$ to high temperatures in an experiment that remains transparent to finite temperature classical phase transitions. These results show that while dynamical decoupling schemes can be quite effective in eliminating classical noise in a qubit, a quantum critical environment may lead to rapid entanglement and decoherence., Comment: 10 pages, 5 figures

When superconductivity is suppressed by high magnetic fields in La2-xSrxCuO4, striped antiferromagnetic (AFM) order becomes the magnetic ground state of the entire pseudogap regime, up to its end at the doping p* [M. Frachet, I. Vinograd et al., Nat. Phys. 16, 1064 (2020)]. Glass-like freezing of this state is detected in 139La NMR measurements of the spin-lattice relaxation rate 1/T1. Here, we present a quantitative analysis of 1/T1 data in the hole-doping range p=x=0.12-0.171, based on the Bloembergen-Purcell-Pound (BPP) theory, modified to include statistical distribution of parameters arising from strong spatial inhomogeneity. We observe spin fluctuations to slow down at temperatures T near the onset of static charge order and, overall, the effect of the field B may be seen as equivalent to strengthening stripe order by approaching p=0.12 doping. In details however, our analysis reveals significant departure from usual field-induced magnetic transitions. The continuous growth of the amplitude of the fluctuating moment with increasing B suggests a nearly-critical state in the B->0 limit, with very weak quasi-static moments possibly confined in small areas like vortex cores. Further, the nucleation of spin order in the vortex cores is shown to account quantitatively for both the value and the p dependence of a field scale characterizing bulk spin freezing. The correlation time of the fluctuating moment appears to depend exponentially on B/T (over the investigated range). This explains the timescale dependence of various experimental manifestations, including why, for transport measurements, the AFM moments may be considered static over a considerable range of B and T. These results make the high-field magnetic ground state up to p* an integral part of the discussion on putative quantum criticality.

TmVO$_{4}$ exhibits ferroquadrupolar order of the Tm 4f electronic orbitals at low temperatures, and is a model system for Ising nematicity that can be tuned continuously to a quantum phase transition via magnetic fields along the $c$-axis. Here we present $^{51}$V nuclear magnetic resonance data in magnetic fields perpendicular to the $c$-axis in a single crystal that has been carefully cut by a plasma focused ion beam to an ellipsoidal shape to minimize the inhomogeneity of the internal demagnetization field. The resulting dramatic increase in spectral resolution enabled us to resolve the anisotropy of the electric field gradient and to measure the magnetic and quadrupolar relaxation channels separately. Perpendicular magnetic fields nominally do not couple to the low energy degrees of freedom, but we find a significant nonlinear contribution for sufficiently large fields that give rise to a rich phase diagram. The in-plane magnetic field can act either as an effective transverse or longitudinal field to the Ising nematic order, depending on the orientation relative to the principle axes of the quadrupole order, and leads to a marked in-plane anisotropy in both relaxation channels. We find that the small in-plane transverse fields initially enhance the ferroquadrupolar ordering temperature but eventually suppress the long-range order. We tentatively ascribe this behavior to the competing effects of field-induced mixing of higher energy crystal field states and the destabilizing effects of field-induced quantum fluctuations., Comment: 15 pages, 13 figures

We investigate the effectiveness of the Inverse Laplace Transform (ILT) analysis method to extract the distribution of relaxation rates from nuclear magnetic resonance data with stretched exponential relaxation. Stretched-relaxation is a hallmark of a distribution of relaxation rates, and an analytical expression exists for this distribution for the case of a spin-1/2 nucleus. We compare this theoretical distribution with those extracted via the ILT method for several values of the stretching exponent and at different levels of experimental noise. The ILT accurately captures the distributions for $\beta \lesssim 0.7$, and for signal to noise ratios greater than $\sim 40$; however the ILT distributions tend to introduce artificial oscillatory components. We further use the ILT approach to analyze stretched relaxation for spin $I>1/2$ and find that the distributions are accurately captured by the theoretical expression for $I=1/2$. Our results provide a solid foundation to interpret distributions of relaxation rates for general spin $I$ in terms of stretched exponential fits., Comment: 10 pages, 10 figures

TmVO$_4$ exhibits ferroquadrupolar order below 2.15 K with a well-isolated non-Kramers ground state doublet, and is a model system to understand Ising nematic order. We present $^{51}$V nuclear magnetic resonance data as a function of field orientation in a single crystal. Although the spectra are well understood in terms of direct dipolar hyperfine couplings, the spin lattice relaxation rate exhibits strong anisotropy that cannot be understood in terms of magnetic fluctuations. We find that the spin lattice relaxation rate scales with the shear elastic constant associated with the ferroquadrupole phase transition, suggesting that quadrupole (nematic) fluctuations dominate the spin lattice relaxation for in-plane fields., Comment: 7 pages, 5 figures

In order to identify the mechanism responsible for the formation of charge-density waves (CDW) in cuprate superconductors, it is important to understand which aspects of the CDW's microscopic structure are generic and which are material-dependent. Here, we show that, at the local scale probed by NMR, long-range CDW order in YBa2Cu3Oy is unidirectional with a commensurate period of three unit cells (lambda = 3b), implying that the incommensurability found in X-ray scattering is ensured by phase slips (discommensurations). Furthermore, NMR spectra reveal a predominant oxygen character of the CDW with an out-of-phase relationship between certain lattice sites but no specific signature of a secondary CDW with lambda = 6b associated with a putative pair-density wave. These results shed light on universal aspects of the cuprate CDW. In particular, its spatial profile appears to generically result from the interplay between an incommensurate tendency at long length scales, possibly related to properties of the Fermi surface, and local commensuration effects, due to electron-electron interactions or lock-in to the lattice., Comment: Original submission (revised version available upon request)

We report $^{77}$Se NMR data in the normal and superconducting states of a single crystal of FeSe for several different field orientations. The Knight shift is suppressed in the superconducting state for in-plane fields, but does not vanish at zero temperature. For fields oriented out of the plane, little or no reduction is observed below $T_c$. These results reflect spin-singlet pairing emerging from a nematic state with large orbital susceptibility and spin-orbit coupling. The spectra and spin-relaxation rate data reveal electronic inhomogeneity that is enhanced in the superconducting state, possibly arising from enhanced density of states in the vortex cores. Despite the spin polarization of these states, there is no evidence for antiferromagnetic fluctuations., Comment: 6 pages, 4 figures

High-$T_{\rm{c}}$ cuprate superconductors host spin, charge and lattice instabilities. In particular, in the antiferromagnetic glass phase, over a large doping range, lanthanum based cuprates display a glass-like spin freezing with antiferromagnetic correlations. Previously, sound velocity anomalies in La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) for hole doping $p\geq 0.145$ were reported and interpreted as arising from a coupling of the lattice to the magnetic glass [Frachet, Vinograd et al., Nat. Phys. 16, 1064-1068 (2020)]. Here we report both sound velocity and attenuation in LSCO $p=0.12$, i.e. at a doping level for which the spin freezing temperature is the highest. Using high magnetic fields and comparing with nuclear magnetic resonance (NMR) measurements, we confirm that the anomalies in the low temperature ultrasound properties of LSCO are produced by a coupling between the lattice and the spin glass. Moreover, we show that both sound velocity and attenuation can be simultaneously accounted for by a simple phenomenological model originally developed for canonical spin glasses. Our results point towards a strong competition between superconductivity and spin freezing, tuned by the magnetic field. A comparison of different acoustic modes suggests that the slow spin fluctuations have a nematic character., Comment: 12 pages, 8 figures

The transferred hyperfine interaction between nuclear and electron spins in an heavy fermion material depends on the hybridization between the $f$-electron orbitals and those surrounding a distant nucleus. In CeMIn$_5$ (M=Rh, Ir, Co), both the hyperfine coupling to the two indium sites as well as the crystalline electric field at the Ce are strongly dependent on the transition metal. We measure a series of CeRh$_{1-x}$Ir$_x$In$_5$ crystals and find that the hyperfine coupling reflects the orbital anisotropy of the ground state Ce 4$f$ wavefunction. These findings provide direct proof that the localized to itinerant transition is dominated by hybridization out of the Ce-In plane in this system., Comment: 10 pages, 11 figures

The effect of hydrostatic pressure (P) on charge density waves (CDW) in YBa2Cu3Oy has recently been controversial. Using NMR, we find that both the short-range CDW in the normal state and the long-range CDW in high fields are, at most, slightly weakened at P=1.9 GPa. This result is in contradiction with x-ray scattering results finding complete suppression of the CDW at ~1 GPa and we discuss possible explanations of this discrepancy. Quantitative analysis, however, shows that the NMR data is not inconsistent with a disappearance of the CDW on a larger pressure scale, typically ~10-20 GPa. We also propose a simple model reconciling transport data with such a hypothesis, provided the pressure-induced change in doping is taken into account. We conclude that it is therefore possible that most of the spectacular increase in Tc upon increasing pressure up to ~15~GPa arises from a concomitant decrease of CDW strength.

The value of the upper critical field Hc2, a fundamental characteristic of the superconducting state, has been subject to strong controversy in high-Tc copper-oxides. Since the issue has been tackled almost exclusively by macroscopic techniques so far, there is a clear need for local-probe measurements. Here, we use 17O NMR to measure the spin susceptibility $\chi_{spin}$ of the CuO2 planes at low temperature in charge ordered YBa2Cu3Oy. We find that $\chi_{spin}$ increases (most likely linearly) with magnetic field H and saturates above field values ranging from 20 to 40 T. This result is consistent with Hc2 values claimed by G. Grissonnanche et al. [Nat. Commun. 5, 3280 (2014)] and with the interpretation that the charge-density-wave (CDW) reduces Hc2 in underdoped YBa2Cu3Oy. Furthermore, the absence of marked deviation in $\chi_{spin}(H)$ at the onset of long-range CDW order indicates that this Hc2 reduction and the Fermi-surface reconstruction are primarily rooted in the short-range CDW order already present in zero field, not in the field-induced long-range CDWorder. Above Hc2, the relatively low values of $\chi_{spin}$ at T=2 K show that the pseudogap is a ground-state property, independent of the superconducting gap., Comment: To appear