Search

We report an extensive high-field study of atacamite Cu$_2$Cl(OH)$_3$, a material realization of quantum sawtooth chains with weak interchain couplings, in continuous and pulsed magnetic fields up to 58 T. In particular, we have mapped the entropy landscape for fields as high as 35 T and have identified a field-induced quantum critical point at 21.9(1) T for $\mathbf{H} \parallel c$ axis. The quantum critical point separates field regions with and without magnetic order, evidenced by our thermodynamic study and $^1$H nuclear magnetic resonance spectroscopy, but lies far below full saturation of the magnetization. Corroborated by numerical results using density-matrix renormalization group (DMRG) calculations, we find this behavior associated with a decoupling of the sawtooth chain into two magnetic subsystems consisting of a spin-$1/2$ antiferromagnetic Heisenberg chain (backbone of the sawtooth chain) in the presence of an exchange field produced by the remaining field-polarized spins.

Two triangular lattice antiferromagnets Sr$_3$Co(Nb,Ta)$_2$O$_9$ with an effective $j_{\rm eff}=1/2$ of Co$^{2+}$ are synthesized and their magnetic properties are investigated via magnetization and heat capacity measurements. The leading in-plane antiferromagnetic exchange coupling is estimated to be $J/k_{\rm B} \simeq 4.7$ K and 5.8 K, respectively. Both the compounds feature two-step magnetic transitions at low temperatures [($T_{\rm N1} \simeq 1.47$ K and $T_{\rm N2} \simeq 1.22$ K) and ($T_{\rm N1} \simeq 0.88$ K and $T_{\rm N2} \simeq 0.67$ K), respectively], driven by weak easy-axis anisotropy. Under magnetic field Sr$_3$CoNb$_2$O$_9$ evinces a plateau at $1/3$ magnetization. Interestingly, the high field magnetization of Sr$_3$CoTa$_2$O$_9$ reveals an exotic regime (between $H_{\rm S1}$ and $H_{\rm S2}$), below the fully polarized state in which the heat capacity at low temperatures is governed by a power law ($C_{\rm p} \propto T^{\alpha}$) with a reduced exponent $\alpha \simeq 2$. These results demonstrate an unusual field induced state with gapless excitations in the strongly frustrated magnet Sr$_3$CoTa$_2$O$_9$. The complete $T-H$ phase diagram is discussed for both the compounds., Comment: 12 pages, 7 figures, 2 tables

We report the structural and magnetic properties of a new spin-$\frac12$ antiferromagnet NaZnVOPO$_4$(HPO$_4$) studied via x-ray diffraction, magnetic susceptibility, high-field magnetization, specific heat, and $^{31}$P nuclear magnetic resonance (NMR) measurements, as well as density-functional band-structure calculations. While thermodynamic properties of this compound are well described by the $J_1-J_2$ square-lattice model, \textit{ab initio} calculations suggest a significant deformation of the spin lattice. From fits to the magnetic susceptibility we determine the averaged nearest-neighbor and second-neighbor exchange couplings of $\bar J_1\simeq -1.3$ K and $\bar J_2\simeq 5.6$ K, respectively. Experimental saturation field of 15.3\,T is consistent with these estimates if 20\% spatial anisotropy in $J_1$ is taken into account. Specific heat data signal the onset of a magnetic long-range order at $T_{\rm N} \simeq 2.1$ K, which is further supported by a sharp peak in the NMR spin-lattice relaxation rate. The NMR spectra mark the superposition of two P lines due to two noneqivalent P sites where the broad line with the strong hyperfine coupling and short $T_1$ is identified as the P(1) site located within the magnetic planes, while the narrow line with the weak hyperfine coupling and long $T_1$ is designated as the P(2) site located between the planes., Comment: 13 pages, 11 figures

We set forth the structural and magnetic properties of the frustrated spin-$5/2$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$ examined via x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements on the polycrystalline sample. No structural distortion was detected from the temperature-dependant x-ray diffraction down to 12.5 K, except a systematic lattice contraction. The magnetic susceptibility at high temperatures agrees well with the high-temperature series expansion for a spin-$5/2$ isotropic triangular lattice antiferromagnet with an average exchange coupling of $J/k_{\rm B} \simeq 1.8$ K rather than a one-dimensional spin-$5/2$ chain model. This value of the exchange coupling is consistently reproduced by the saturation field of the pulse field magnetization data. It undergoes a magnetic long-range-order at $T_{\rm N} \simeq 10.4$ K. Neutron diffraction experiments elucidate a collinear antiferromagnetic ordering below $T_{\rm N}$ with the propagation vector $k = (1,0,0)$. An intermediate value of frustration ratio ($f \simeq 3.6$) reflects moderate frustration in the compound which is corroborated by a reduced ordered magnetic moment of $\sim 1.52$ $\mu_{\rm B}$ at 1.6 K, compared to its classical value ($5 \mu_{\rm B}$). Magnetic isotherms exhibit a change of slope envisaging a field induced spin-flop transition at $H_{\rm SF}\simeq3.2$ T. The magnetic field vs temperature phase diagram clearly unfold three distinct phase regimes, reminiscent of a frustrated magnet with in-plane (XY-type) anisotropy., Comment: 11 pages, 11 figures, 1 table

We report on a comprehensive characterization of the newly synthesized Cu$^{2+}$-based molecular magnet [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ (CuPOF), where pz = C$_4$H$_4$N$_2$ and 2-HOpy = C$_5$H$_4$NHO. From a comparison of theoretical modeling to results of bulk magnetometry, specific heat, $\mu^+$SR, ESR, and NMR spectroscopy, this material is determined as an excellent realization of the 2D square-lattice $S=1/2$ antiferromagnetic Heisenberg model with a moderate intraplane nearest-neighbor exchange coupling of $J/k_\mathrm{B} = 6.80(5)$ K, and an extremely small interlayer interaction of about 1 mK. At zero field, the bulk magnetometry reveals a temperature-driven crossover of spin correlations from isotropic to $XY$ type, caused by the presence of a weak intrinsic easy-plane anisotropy. A transition to long-range order, driven by the low-temperature $XY$ anisotropy under the influence of the interlayer coupling, occurs at $T_\mathrm{N} = 1.38(2)$ K, as revealed by $\mu^+$SR. In applied magnetic fields, our $^1$H-NMR data reveal a strong increase of the magnetic anisotropy, manifested by a pronounced enhancement of the transition temperature to commensurate long-range order at $T_\mathrm{N} =2.8$ K and 7 T., Comment: 14 pages, 8 figures, as well as 10 pages and 18 figures of supplemental material

We report the synthesis and characterization of a new quantum magnet [2-[Bis(2-hydroxybenzyl)aminomethyl]pyridine]Ni(II)-trimer (BHAP-Ni3) in single-crystalline form. Our combined experimental and theoretical investigations reveal an exotic spin state that stabilizes a robust 2/3 magnetization plateau between 7 and 20 T in an external magnetic field. AC-susceptibility measurements show the absence of any magnetic order/glassy state down to 60 mK. The magnetic ground state is disordered and specific-heat measurements reveal the gapped nature of the spin excitations. Most interestingly, our theoretical modeling suggests that the 2/3 magnetization plateau emerges due to the interplay between antiferromagnetic Heisenberg and biquadratic exchange interactions within nearly isolated spin $S$ = 1 triangles.

We 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 Ho$_2$Ti$_2$O$_7$ the magnetization exceeds the angle-dependent saturation value of the Ising limit using ultra-high 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 cross-over between spin-ice and polarized correlations., Comment: 7 pages, 4 figures, accepted for publication in Phys. Rev. B

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 figures

By use of ultrasound studies we resolved magneto-acoustic quantum oscillation deep into the mixed state of the multiband nonmagnetic superconductor YNi2B2C. Below the upper critical field, only a very weak additional damping appears that can be well explained by the field inhomogeneity caused by the flux-line lattice in the mixed state. This is clear evidence for no or a vanishingly small gap for one of the bands, namely, the spheroidal alpha band. This contrasts de Haas--van Alphen data obtained by use of torque magnetometry for the same sample, with a rapidly vanishing oscillation signal in the mixed state. This points to a strongly distorted flux-line lattice in the latter case that, in general, can hamper a reliable extraction of gap parameters by use of such techniques., Comment: 6 pages, 6 figures

Physical properties of a pyrohafnate compound Pr2Hf2O7 have been investigated by ac magnetic susceptibility \chi_ ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements on polycrystalline as well as single crystal samples combined with high-resolution synchrotron x-ray diffraction (XRD) for structural characterization and inelastic neutron scattering (INS) to determine the crystal field energy level scheme and wave functions. Synchrotron XRD data confirm the ordered cubic pyrochlore (Fd-3m) structure without any noticeable site mixing or oxygen deficiency. No clear evidence of long range magnetic ordering is observed down to 90 mK, however the \chi_ac(T) evinces slow spin dynamics revealed by a frequency dependent broad peak associated with spin freezing. The INS data reveal the expected five well defined magnetic excitations due to crystal field splitting of the J = 4 ground state multiplet of the Pr^3+. The crystal field parameters and ground state wavefunction of Pr^3+ have been determined. The Ising anisotropic nature of magnetic ground state is inferred from the INS as well as \chi(T) and M(H) data. Together these properties make Pr2Hf2O7 a candidate compound for quantum spin-ice behavior., Comment: 12 pages, 10 figures, 2 tables

We report evidence for multiband transport and an insulating low-temperature normal state in superconducting K$_{0.50}$Na$_{0.24}$Fe$_{1.52}$Se$_{2}$ with $T_{c}\approx 20$ K. The temperature-dependent upper critical field, $H_{c2}$, is well described by a two-band BCS model. The normal-state resistance, accessible at low temperatures only in pulsed magnetic fields, shows an insulating logarithmic temperature dependence as $T \rightarrow 0$ after superconductivity is suppressed. This is similar as for high-$T_{c}$ copper oxides and granular type-I superconductors, suggesting that the superconductor-insulator transition observed in high magnetic fields is related to intrinsic nanoscale phase separation., Comment: 5 pages, 4 figures

We report on the emergence of an Electronic Griffiths Phase (EGP) in the doped semiconductor FeSb$_{2}$, predicted for disordered insulators with random localized moments in the vicinity of a metal-insulator transition (MIT). Magnetic, transport, and thermodynamic measurements of Fe(Sb$_{1-x}$Te$_{x}$)$_{2}$ single crystals show signatures of disorder-induced non-Fermi liquid behavior and a Wilson ratio expected for strong electronic correlations. The EGP states are found on the metallic boundary, between the insulating state ($x = 0$) and a long-range albeit weak magnetic order ($x \geq 0.075$)., Comment: 5 pages, 4 figures

The Weyl semimetal NbP was found to exhibit topological Fermi arcs and exotic magneto-transport properties. Here, we report on magnetic quantum-oscillation measurements on NbP and construct the 3D Fermi surface with the help of band-structure calculations. We reveal a pair of spin-orbit-split electron pockets at the Fermi energy and a similar pair of hole pockets, all of which are strongly anisotropic. The Fermi surface well explains the linear magnetoresistance observed in high magnetic fields by the quantum-limit scenario. The Weyl points that are located in the $k_z \approx \pi/c$ plane are found to exist 5 meV above the Fermi energy. Therefore, we predict that the chiral anomaly effect can be realized in NbP by electron doping to drive the Fermi energy to the Weyl points., Comment: 5 pages, 4 figures and 1 table

The normal-state in-plane resistivity below the zero-field superconducting transition temperature $T_c$ and the upper critical field Hc2 were measured by suppressing superconductivity in pulsed magnetic fields for K0.70Fe1.46Se1.85Te0.15. The normal-state resistivity $\rho_{ab}$ is found to increase logarithmically with decrasing temperature as $\frac{T}{T_c}\rightarrow 0$. Similar to granular metals, our results suggest that a superconductor - insulator transition below zero-field T$_{c}$ may be induced in high magnetic fields. This is related to the intrinsic real-space phase-separated states common to all inhomogeneous superconductors., Comment: 6 pages, 4 figures

We present a comprehensive macroscopic thermodynamic study of the quasi-one-dimensional (1D) $s = \tfrac{1}{2}$ frustrated spin-chain system linarite. Susceptibility, magnetization, specific heat, magnetocaloric effect, magnetostriction, and thermal-expansion measurements were performed to characterize the magnetic phase diagram. In particular, for magnetic fields along the b axis five different magnetic regions have been detected, some of them exhibiting short-range-order effects. The experimental magnetic entropy and magnetization are compared to a theoretical modelling of these quantities using DMRG and TMRG approaches. Within the framework of a purely 1D isotropic model Hamiltonian, only a qualitative agreement between theory and the experimental data can be achieved. Instead, it is demonstrated that a significant symmetric anisotropic exchange of about 10% is necessary to account for the basic experimental observations, including the 3D saturation field, and which in turn might stabilize a triatic (three-magnon) multipolar phase., Comment: 20 pages, 17 figures

We report on an investigation of optical properties of multiferroic CoCr$_{2}$O$_{4}$ at terahertz frequencies in magnetic fields up to 30 T. Below the ferrimagnetic transition (94 K), the terahertz response of CoCr$_{2}$O$_{4}$ is dominated by a magnon mode, which shows a steep magnetic-field dependence. We ascribe this mode to an exchange resonance between two magnetic sublattices with different $g$-factors. In the framework of a simple two-sublattice model (the sublattices are formed by Co$^{2+}$ and Cr$^{3+}$ ions), we find the inter-sublattice coupling constant, $\lambda = - (18 \pm 1)$ K, and trace the magnetization for each sublattice as a function of field. We show that the Curie temperature of the Cr$^{3+}$ sublattice, $\Theta_{2}$ = $(49 \pm 2)$ K, coincides with the temperature range, where anomalies of the dielectric and magnetic properties of CoCr$_{2}$O$_{4}$ have been reported in literature., Comment: accepted to PRB

We have measured the magnetization and specific heat of multiferroic CoCr2O4 in magnetic fields up to 14 T. The high-field magnetization measurements indicate a new phase transition at T* = 5 - 6 K. The phase between T* and the lock-in transition at 15 K is characterized by magnetic irreversibility. At higher magnetic fields, the irreversibility increases. Specific-heat measurements confirm the transition at T*, and also show irreversible behavior. We construct a field-temperature phase diagram of CoCr2O4., Comment: 4 pages

We present a detailed study in the paramagnetic regime of the frustrated $s$ = 1/2 spin-compound linarite, PbCuSO$_4$(OH)$_2$, with competing ferromagnetic nearest-neighbor and antiferromagnetic next-nearest-neighbor exchange interactions. Our data reveal highly anisotropic values for the saturation field along the crystallographic main directions, with $\sim$ 7.6, $\sim$ 10.5 and $\sim$ 8.5\,T for the $a$, $b$, and $c$ axes, respectively. In the paramagnetic regime, this behavior is explained mainly by the anisotropy of the \textit{g}-factor but leaving room for an easy-axis exchange anisotropy. Within the isotropic $J_1$-$J_2$ spin model our experimental data are described by various theoretical approaches yielding values for the exchange interactions $J_1$ $\sim$ -100\,K and $J_2$ $\sim$ 36\,K. These main intrachain exchange integrals are significantly larger as compared to the values derived in two previous studies in the literature and shift the frustration ratio $\alpha = J_2/|J_1|$ $\approx$ 0.36 of linarite closer to the 1D critical point at 0.25. Electron spin resonance (ESR) and nuclear magnetic resonance (NMR) measurements further prove that the static susceptibility is dominated by the intrinsic spin susceptibility. The Knight shift as well as the broadening of the linewidth in ESR and NMR at elevated temperatures indicate a highly frustrated system with the onset of magnetic correlations far above the magnetic ordering temperature $T_\mathrm{N}$ = 2.75(5)\,K, in agreement with the calculated exchange constants., Comment: 18 pages, 18 figures

We report on high-field magnetization, specific-heat and electron spin resonance (ESR) studies of the quasi-two-dimensional spin-1/2 Heisenberg antiferromagnet [Cu(pyz)2(HF2)]PF6. The frequency-field diagram of ESR modes below TN = 4.38 K is described in the frame of the meanfield theory, confirming a collinear magnetic structure with an easy-plane anisotropy. The obtained results allowed us to determine the anisotropy/exchange interaction ratio, A/J = 0.003, and the upper limit for the inter/intra-plane exchange-interaction ratio, J'/J = 1/16. It is argued that despite the onset of 3D long-range magnetic ordering the magnetic properties of this material (including high-magnetic-field magnetization and non-monotonic field dependence of the Neel temperature) are strongly affected by two-dimensional spin correlations., Comment: 5 pages, 7 figures

We have investigated the evolution of ferromagnetic order in the correlated metal URhGe (Curie temperature $T_{\rm C} = $9.5 K) by chemical substitution of Ru, Co and Si. Polycrystalline samples URh$_{1-x}$Ru$_x$Ge ($x \leq $0.6), URh$_{1-x}$Co$_x$Ge ($x \leq $0.9) and URhGe$_{1-x}$Si$_x$ ($x \leq $0.2) have been prepared and the magnetic properties have been investigated by magnetization and transport experiments. In the case of Ru doping, $T_{\rm C}$ initially increases, but then decreases linearly as a function of $x$ and is completely suppressed for $x_{\rm cr} \approx 0.38$. The Curie temperature in the URh$_{1-x}$Co$_x$Ge series has a broad maximum $T_{\rm C} = 20$ K near $x=0.6$ and then drops to 8 K for $x=0.9$. In the case of Si doping $T_{\rm C}$ stays roughly constant. We conclude that the alloy systems URh$_{1-x}$Ru$_x$Ge and URh$_{1-x}$Co$_x$Ge are interesting candidates to study the ferromagnetic instability., Comment: 15 pages, 12 figures; revised & shortened version

We have studied the pressure dependence of the magnetization of single crystalline CeSi_1.81. At ambient pressure ferromagnetism develops below T_C = 9.5 Below ~ 5 K an additional shoulder in low-field hysteresis loops and a metamagnetic crossover around 4 T suggest the appearance of an additional magnetic modulation to the ferromagnetic state. The suppression of the magnetic order in CeSi_1.81 as function of temperature at ambient pressure and as function of pressure at low temperature are in remarkable qualitative agreement. The continuous suppression of the ordered moment at p ~ 13.1 kbar suggests the existence of a ferromagnetic quantum critical point in this material., Comment: 9 pages, 9 figures, to be published in Physical Review B

We show that the superconductivity observed recently in the weak itinerant ferromagnet ZrZn2 [C. Pfleiderer et al., Nature (London) 412, 58 (2001)] is due to remnants of a superconducting layer induced by spark erosion. Results of resistivity, susceptibility, specific heat and surface analysis measurements on high-quality ZrZn2 crystals show that cutting by spark erosion leaves a superconducting surface layer. The resistive superconducting transition is destroyed by chemically etching a layer of 5 microns from the sample. No signature of superconductivity is observed in rho(T) of etched samples at the lowest current density measured, J=675 Am-2, and at T < 45 mK. EDX analysis shows that spark-eroded surfaces are strongly Zn depleted. The simplest explanation of our results is that the superconductivity results from an alloy with higher Zr content than ZrZn2., Comment: Final published version

We report a study of the ferromagnetism of ZrZn$_{2}$, the most promising material to exhibit ferromagnetic quantum criticality, at low temperatures $T$ as function of pressure $p$. We find that the ordered ferromagnetic moment disappears discontinuously at $p_c$=16.5 kbar. Thus a tricritical point separates a line of first order ferromagnetic transitions from second order (continuous) transitions at higher temperature. We also identify two lines of transitions of the magnetisation isotherms up to 12 T in the $p-T$ plane where the derivative of the magnetization changes rapidly. These quantum phase transitions (QPT) establish a high sensitivity to local minima in the free energy in ZrZn$_{2}$, thus strongly suggesting that QPT in itinerant ferromagnets are always first order.