Aging and memory properties of topologically frustrated magnets

The model 2d kagome system (H3O)Fe3(SO4)2(OH)6 and the 3d pyrochlore Y2Mo2O7 are two well characterized examples of low-disordered frustrated antiferromagnets which rather then condensing into spin liquid have been found to undergo a freezing transition with spin glass-like properties. We explore more deeply the comparison of their properties with those of spin glasses, by the study of characteristic rejuvenation and memory effects in the non-stationary susceptibility. While the pyrochlore shows clear evidence for these non-trivial effects, implying temperature selective aging, that is characteristic of a wide hierarchical distribution of equilibration processes, the kagome system does n not show clearly these effects. Rather, it seems to evolve towards the same final state independently of temperature.Comment: submitted for the proceedings of the 46th MMM conference (Seattle, 2001

Superconducting properties of the pyrochlore oxide Cd2Re2O7

We report the superconducting properties of the pyrochlore oxide Cd2Re2O7. The bulk superconducting transition temperature Tc is about 1.0 K, and the upper critical field Hc2 determined by the measurement of specific heat under magnetic fields is 0.29 T. The superconducting coherence length is estimated to be 34 nm. Specific heat data measured on single crystals suggest that the superconducting gap of Cd2Re2O7 is nodeless.Comment: 6 pages, 6 figures, 1 table, to be published in J. Chem. Phys. Solid

Magnetic and Thermodynamic Properties of the Collective Paramagnet-Spin Liquid Pyrochlore Tb2Ti2O7

In a recent letter [Phys. Rev. Lett. {\bf 82}, 1012 (1999)] it was found that the Tb$^{3+}$ magnetic moments in the Tb$_2$Ti$_2$O$_7$ pyrochlore lattice of corner-sharing tetrahedra remain in a {\it collective paramagnetic} state down to 70mK. In this paper we present results from d.c. magnetic susceptibility, specific heat data, inelastic neutron scattering measurements, and crystal field calculations that strongly suggest that (1) the Tb$^{3+}$ ions in Tb$_2$Ti$_2$O$_7$ possess a moment of approximatively 5$\mu_{\rm B}$, and (2) the ground state $g-$tensor is extremely anisotropic below a temperature of $O(10^0)$K, with Ising-like Tb$^{3+}$ magnetic moments confined to point along a local cubic $$diagonal (e.g. towards the middle of the tetrahedron). Such a very large easy-axis Ising like anisotropy along a$$ direction dramatically reduces the frustration otherwise present in a Heisenberg pyrochlore antiferromagnet. The results presented herein underpin the conceptual difficulty in understanding the microscopic mechanism(s) responsible for Tb$_2$Ti$_2$O$_7$ failing to develop long-range order at a temperature of the order of the paramagnetic Curie-Weiss temperature $\theta_{\rm CW} \approx -10^1$K. We suggest that dipolar interactions and extra perturbative exchange coupling(s)beyond nearest-neighbors may be responsible for the lack of ordering of Tb$_2$Ti$_2$O$_7$.Comment: 8 POSTSCRIPT figures included. Submitted to Physical Review B. Contact: [email protected]

Structural and Magnetic Properties of Pyrochlore Solid Solutions (Y,Lu)2Ti2-x(Nb,Ta)xO7+/-y

The synthesis and characterization of the pyrochlore solid solutions, Y2Ti2-xNbxO7-y, Lu2Ti2-xNbxO7-y, Y2Ti2-xTaxO7-y and Lu2TiTaO7-y (-0.4<y<0.5), is described. Synthesis at 1600 C, and 10-5 Torr yields oxygen deficiency in all systems. All compounds are found to be paramagnetic and semiconducting, with the size of the local moments being less, in some cases substantially less, than the expected value for the number of nominally unpaired electrons present. Thermogravimetric analysis (TGA) shows that all compounds can be fully oxidized while retaining the pyrochlore structure, yielding oxygen rich pyrochlores as white powders. Powder neutron diffraction of Y2TiNbO7-based samples was done. Refinement of the data for oxygen deficient Y2TiNbO6.76 indicates the presence of a distribution of oxygen over the 8b and 48f sites. Refinement of the data for oxygen rich Y2TiNbO7.5 shows these sites to be completely filled, with an additional half filling of the 8a site. The magnetic and TGA data strongly suggest a preference for a Ti3+/(Nb,Ta)5+ combination, as opposed to Ti4+/(Nb,Ta)4+, in this pyrochlore family. In addition, the evidence clearly points to Ti3+ as the source of the localized moments, with no evidence for localized Nb4+ moments.Comment: Accepted to Journal of Solid State Chemistr

Frustration effects in magnetic molecules

Besides being a fascinating class of new materials, magnetic molecules provide the opportunity to study concepts of condensed matter physics in zero dimensions. This contribution will exemplify the impact of molecular magnetism on concepts of frustrated spin systems. We will discuss spin rings and the unexpected rules that govern their low-energy behavior. Rotational bands, which are experimentally observed in various molecular magnets, provide a useful, simplified framework for characterizing the energy spectrum, but there are also deviations thereof with far-reaching consequences. It will be shown that localized independent magnons on certain frustrated spin systems lead to giant magnetization jumps, a new macroscopic quantum effect. In addition a frustration-induced metamagnetic phase transitions will be discussed, which demonstrates that hysteresis can exist without anisotropy. Finally, it is demonstrated that frustrated magnetic molecules could give rise to an enhanced magnetocaloric effect.Comment: 6 pages, 4 figures; submitted to J. Low. Temp. Phys.; proceedings of the Sixth International Symposium on Crystalline Organic Metals, Superconductors, and Ferromagnets (ISCOM

Static Critical Behavior of the Spin-Freezing Transition in the Geometrically Frustrated Pyrochlore Antiferromagnet Y2Mo2O7

Some frustrated pyrochlore antiferromagnets, such as Y2Mo2O7, show a spin-freezing transition and magnetic irreversibilities below a temperature Tf similar to what is observed nonlinear magnetization measurements on Y2Mo2O7 that provide strong evidence that there is an underlying thermodynamic phase transition at Tf, which is characterized by critical exponents \gamma \approx 2.8 and \beta \approx 0.8. These values are typical of those found in random spin glasses, despite the fact that the level of random disorder in Y2Mo2O7 is immeasurably small.Comment: Latex file, calls for 4 encapsulated postscript figures (included). Submitted to Phys. Rev. Letters

Manifestation of geometric frustration on magnetic and thermodynamic properties of pyrochlores Sm2X2O7Sm_2X_2O_7 (X=Ti, Zr)

We present here magnetization, specific heat and Raman studies on single-crystalline specimens of the first pyrochlore member $Sm_2Ti_2O_7$ of the rare-earth titanate series. Its analogous compound $Sm_2Zr_2O_7$ in the rare-earth zirconate series is also investigated in the polycrystalline form. The Sm spins in $Sm_2Ti_2O_7$ remain unordered down to at least T = 0.5 K. The absence of magnetic ordering is attributed to very small values of exchange ($\theta_{cw} ~ -0.26 K$) and dipolar interaction ($\mu_{eff} ~ 0.15 \mu_B$) between the $Sm^{3+}$ spins in this pyrochlore. In contrast, the pyrochlore $Sm_2Zr_2O_7$ is characterized by a relatively large value of Sm-Sm spin exchange ($\theta_{cw} ~ - 10 K$); however, long-range ordering of the $Sm^{3+}$ spins is not established at least down to T = 0.67 K, due to frustration of the $Sm^{3+}$ spins on the pyrochlore lattice. The ground state of $Sm^{3+}$ ions in both pyrochlores is a well-isolated Kramer's doublet. The higher-lying crystal field excitations are observed in the low-frequency region of the Raman spectra of the two compounds recorded at T = 10 K. At higher temperatures, the magnetic susceptibility of $Sm_2Ti_2O_7$ shows a broad maximum at T = 140 K while that of $Sm_2Zr_2O_7$ changes monotonically. Whereas $Sm_2Ti_2O_7$ is a promising candidate for investigating spin-fluctuations on a frustrated lattice as indicated by our data, the properties of $Sm_2Zr_2O_7$ seem to conform to a conventional scenario where geometrical frustration of the spin exclude their long-range ordering.Comment: 24 pages, 6 figures, Accepted for publication in Phys. Rev.