3 research outputs found
A Supercooled Spin Liquid State in the Frustrated Pyrochlore Dy2Ti2O7
A "supercooled" liquid develops when a fluid does not crystallize upon
cooling below its ordering temperature. Instead, the microscopic relaxation
times diverge so rapidly that, upon further cooling, equilibration eventually
becomes impossible and glass formation occurs. Classic supercooled liquids
exhibit specific identifiers including microscopic relaxation times diverging
on a Vogel-Tammann-Fulcher (VTF) trajectory, a Havriliak-Negami (HN) form for
the dielectric function, and a general Kohlrausch-Williams-Watts (KWW) form for
time-domain relaxation. Recently, the pyrochlore Dy2Ti2O7 has become of
interest because its frustrated magnetic interactions may, in theory, lead to
highly exotic magnetic fluids. However, its true magnetic state at low
temperatures has proven very difficult to identify unambiguously. Here we
introduce high-precision, boundary-free magnetization transport techniques
based upon toroidal geometries and gain a fundamentally new understanding of
the time- and frequency-dependent magnetization dynamics of Dy2Ti2O7. We
demonstrate a virtually universal HN form for the magnetic susceptibility, a
general KWW form for the real-time magnetic relaxation, and a divergence of the
microscopic magnetic relaxation rates with precisely the VTF trajectory. Low
temperature Dy2Ti2O7 therefore exhibits the characteristics of a supercooled
magnetic liquid; the consequent implication is that this translationally
invariant lattice of strongly correlated spins is evolving towards an
unprecedented magnetic glass state, perhaps due to many-body localization of
spin.Comment: Version 2 updates: added legend for data in Figures 4A and 4B;
corrected equation reference in caption for Figure 4
Common glass-forming spin-liquid state in the pyrochlore magnets Dy2Ti2O7 and Ho2Ti2O7
Despite a well-ordered pyrochlore crystal structure and strong magnetic interactions between the Dy3+ or Ho3+ ions, no long-range magnetic order has been detected in the pyrochlore titanates Ho2Ti2O7 and Dy2Ti2O7. To explore the actual magnetic phase formed by cooling these materials, we measure their magnetization dynamics using toroidal, boundary-free magnetization transport techniques. We find that the dynamical magnetic susceptibility of both compounds has the same distinctive phenomenology, which is indistinguishable in form from that of the dielectric permittivity of dipolar glass-forming liquids. Moreover, Ho2Ti2O7 and Dy2Ti2O7 both exhibit microscopic magnetic relaxation times that increase along the super-Arrhenius trajectories analogous to those observed in glass-forming dipolar liquids. Thus, upon cooling below about 2 K, Dy2Ti2O7 and Ho2Ti2O7 both appear to enter the same magnetic state exhibiting the characteristics of a glass-forming spin liquid