Long-wavelength correlations in ferromagnetic titanate pyrochlores as revealed by small-angle neutron scattering

Abstract

We have carried out small angle neutron scattering measurements on single crystals of two members of the family of cubic rare-earth titanate pyrochlores that display ferromagnetic Curie-Weiss susceptibilities,Yb$_2$Ti$_2$O$_7$ and Ho$_2$Ti$_2$O$_7$. Ho$_2$Ti$_2$O$_7$ is established as displaying a prototypical classical dipolar spin ice ground state, while Yb$_2$Ti$_2$O$_7$ has been purported as a candidate for a quantum spin ice ground state. While both materials have been well studied with neutron scattering techniques, neither has been previously explored in single crystal form with small angle neutron scattering (SANS). Our results for Yb$_2$Ti$_2$O$_7$ show distinct SANS features below its $\Theta_{CW}$$\sim$ 0.50 K, with rods of diffuse scattering extending along $\langle 111 \rangle$ directions in reciprocal space, off-rod scattering which peaks in temperature near $\Theta_{CW}$, and quasi-Bragg scattering at very small angles which correlates well with T$_C$ $\sim$ 0.26 K. The quasi-Bragg scattering corresponds to finite extent ferromagnetic domains $\sim$ 140 \AA$~$ across, at the lowest temperatures. We interpret the $\langle 111\rangle$ rods of diffuse scattering as arising from domain boundaries between the finite-extent ferromagnetic domains. In contrast the SANS signal in Ho$_2$Ti$_2$O$_7$ is isotropic within the (HHL) plane around $\textbf{Q}$=0. However the strength of this overall SANS signal has a temperature dependence resembling that of the magnetic heat capacity, with a peak near 3 K. Below the break between the field-cooled and the zero-field cooled susceptibility in Ho$_2$Ti$_2$O$_7$ at $\sim$ 0.60 K, the SANS signal is very low, approaching zero.