Candidate Quantum Spin Liquid in the Ce\textsuperscript{3+} Pyrochlore Stannate Ce2_2Sn2_2O7_7

We report the low temperature magnetic properties of Ce$_2$Sn$_2$O$_7$, a rare-earth pyrochlore. Our susceptibility and magnetization measurements show that due to the thermal isolation of a Kramers doublet ground state, Ce$_2$Sn$_2$O$_7$ has Ising-like magnetic moments of $\sim1.18$ $\mu_\mathrm{B}$. The magnetic moments are confined to the local trigonal axes, as in a spin ice, but the exchange interactions are antiferromagnetic. Below 1 K the system enters a regime with antiferromagnetic correlations. In contrast to predictions for classical $\langle 111 \rangle$-Ising spins on the pyrochlore lattice, there is no sign of long-range ordering down to 0.02 K. Our results suggest that Ce$_2$Sn$_2$O$_7$ features an antiferromagnetic liquid ground state with strong quantum fluctuations.Comment: 6 pages, 4 figure

Palmer-Chalker correlations in the XY pyrochlore antiferromagnet Er2Sn2O7

\ersn\, is considered, together with \erti, as a realization of the XY antiferromagnet on the pyrochlore lattice. We present magnetization measurements confirming that \ersn\, does not order down to 100 mK but exhibits a freezing below 200 mK. Our neutron scattering experiments evidence the strong XY character of the \er moment and point out the existence of short range correlations in which the magnetic moments are in peculiar configurations, the Palmer-Chalker states, predicted theoretically for an XY pyrochlore antiferromagnet with dipolar interactions. Our estimation of the \ersn\, parameters confirm the role of the latter interactions on top of relatively weak and isotropic exchange couplings

Magnetic structure and dynamics of a strongly one-dimensional cobaltII^{II} metal-organic framework

We investigate the magnetism of the Co$^{II}_4$(OH)$_2$(C$_1$$_0$H$_1$$_6$O$_4$)$_3$ metal-organic framework which displays complex inorganic chains separated from each other by distances of 1 to 2 nm, and which orders at ~5.4 K. The zero-field magnetic structure is determined using neutron powder diffraction: it is mainly antiferromagnetic but posseses a ferromagnetic component along the $\textbf{c}$-axis. This magnetic structure persists in presence of a magnetic field. Ac susceptibility measurements confirm the existence of a single thermally activated regime over 7 decades in frequency ($E/k_B\approx64 K$) whereas time-dependent relaxation of the magnetization after saturation in an external field leads to a two times smaller energy barrier. These experiments probe the slow dynamics of domain walls within the chains: we propose that the ac measurements are sensitive to the motion of existing domain walls within the chains, while the magnetization measurements are governed by the creation of domain walls.Comment: 12 pages, 14 figure

Candidate quantum spin ice in the pyrochlore Pr2_2Hf2_2O7_7

We report the low temperature magnetic properties of the pyrochlore Pr$_2$Hf$_2$O$_7$. Polycrystalline and single-crystal samples are investigated using time-of-flight neutron spectroscopy and macroscopic measurements, respectively. The crystal-field splitting produces a non-Kramers doublet ground state for Pr$^{3+}$, with Ising-like anisotropy. Below 0.5 K ferromagnetic correlations develop, which suggests that the system enters a spin ice-like state associated with the metamagnetic behavior observed at $\mu_0H_c\sim2.4$~T. In this regime, the development of a discrete inelastic excitation in the neutron spectra indicates the appearance of spin dynamics which are likely related to cooperative quantum fluctuations.Comment: 7 pages, 5 figures, 1 tabl

Magnetisation process in Er2Ti2O7 and Tb2Ti2O7 at very low temperature

We present a model which accounts for the high field magnetisation at very low temperature in two pyrochlore frustrated systems, Er2Ti2O7 and Tb2Ti2O7. The two compounds present very different ground states: Er2Ti2O7, which has a planar crystal field anisotropy, is an antiferromagnet with T_N=1.2K, whereas Tb2Ti2O7 is expected to have Ising character and shows no magnetic ordering down to 0.05K, being thus labelled a ``spin liquid''. Our model is a mean field self-consistent calculation involving the 4 rare earth sites of a tetrahedron, the building unit of the pyrochlore lattice. It includes the full crystal field hamiltonian, the infinite range dipolar interaction and anisotropic nearest neighbour exchange described by a 3-component tensor. For Er2Ti2O7, we discuss the equivalence of our treatment of the exchange tensor, taken to be diagonal in a frame linked to a rare earth - rare earth bond, with the pseudo-spin hamiltonian recently developped for Kramers doublets in a pyrochlore lattice. In Tb2Ti2O7, an essential ingredient of our model is a symmetry breaking developping at very low temperature. We compare its prediction for the isothermal magnetisation with that of ``the quantum spin ice'' model

Antiferro-quadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7

We present an experimental study of the quantum spin ice candidate pyrochlore coumpound \przr\ by means of magnetization measurements, specific heat and neutron scattering up to 12 T and down to 60 mK. When the field is applied along the $[111]$ and $[1\bar{1}0]$ directions, ${\bf k}=0$ field induced structures settle in. We find that the ordered moment rises slowly, even at very low temperature, in agreement with macroscopic magnetization. Interestingly, for $H \parallel [1\bar{1}0]$, the ordered moment appears on the so called $\alpha$ chains only. The spin excitation spectrum is essentially {\it inelastic} and consists in a broad flat mode centered at about 0.4 meV with a magnetic structure factor which resembles the spin ice pattern. For $H \parallel [1\bar{1}0]$ (at least up to 2.5 T), we find that a well defined mode forms from this broad response, whose energy increases with $H$, in the same way as the temperature of the specific heat anomaly. We finally discuss these results in the light of mean field calculations and propose a new interpretation where quadrupolar interactions play a major role, overcoming the magnetic exchange. In this picture, the spin ice pattern appears shifted up to finite energy because of those new interactions. We then propose a range of acceptable parameters for \przr\, that allow to reproduce several experimental features observed under field. With these parameters, the actual ground state of this material would be an antiferroquadrupolar liquid with spin-ice like excitations

Strong quantum fluctuations due to competition between magnetic phases in a pyrochlore iridate

We report neutron diffraction measurements of the magnetic structures in two pyrochlore iridates, Yb2Ir2O7 and Lu2Ir2O7. Both samples exhibit the all-in-all-out magnetic structure on the Ir4+ sites below TN~ 150,K, with a low temperature moment of around 0.45 muB/Ir. Below 2\,K, the Yb moments in Yb2Ir2O7 begin to order ferromagnetically. However, even at 40 mK the ordered moment is only 0.57(3)muB/Yb, well below the saturated moment of the ground state doublet of Yb3+ (1.9 muB/Yb), deduced from magnetization measurements and from a refined model of the crystal field environment, and also significantly smaller than the ordered moment of Yb in Yb2Ti2O7 (0.9 muB/Yb). A mean-field analysis shows that the reduced moment on Yb is a consequence of enhanced phase competition caused by coupling to the all-in-all-out magnetic order on the Ir sublattice.Comment: 14 pages, 10 figures, resubmitted to PR

Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb2+x_{2+x}Ti2−x_{2-x}O7+y_{7+y}

While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it.Comment: Main text: 7 pages, 3 figures ; Supplemental Material: 6 pages, 2 figure

Geometric Frustration on the Trillium Lattice in a Magnetic Metal-Organic Framework

In the dense metal-organic framework Na[Mn(HCOO)3], Mn2+ ions (S = $5\over2$) occupy the nodes of a ‘trillium’ net. We show that the system is strongly magnetically frustrated: the Neel transition is suppressed well ´ below the characteristic magnetic interaction strength; short-range magnetic order persists far above the Neel ´ temperature; and the magnetic susceptibility exhibits a pseudo-plateau at $1\over3$-saturation magnetisation. A simple model of nearest-neighbour Heisenberg antiferromagnetic and dipolar interactions accounts quantitatively for all observations, including an unusual 2-k magnetic ground-state. We show that the relative strength of dipolar interactions is crucial to selecting this particular ground-state. Geometric frustration within the classical spin liquid regime gives rise to a large magnetocaloric response at low applied fields that is degraded in powder samples as a consequence of the anisotropy of dipolar interactions