Gapped and gapless short range ordered magnetic states with $(\frac{1}{2},\frac{1}{2},\frac{1}{2})$ wavevectors in the pyrochlore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+\delta}$

TL;DR

This study investigates how slight variations in composition affect magnetic states in Tb$_{2+x}$Ti$_{2-x}$O$_{7+ delta}$, revealing robust short-range antiferromagnetic spin ice order under field cooling, independent of specific heat anomalies.

Contribution

It demonstrates that the gapped short-range antiferromagnetic spin ice state is robust across different compositions and is not directly linked to the specific heat anomaly.

Findings

Short-range AF spin ice order observed under field cooling in samples with different x.

The C$_P$ anomaly is confined to x between 0 and 0.01.

The magnetic order is not correlated with the specific heat phase transition.

Abstract

Recent low temperature heat capacity (C$_P$) measurements on polycrystalline samples of the pyrochlore antiferromagnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+\delta}$ have shown a strong sensitivity to the precise Tb concentration $x$, with a large anomaly exhibited for $x \sim 0.005$ at $T_C \sim 0.5$ K and no such anomaly and corresponding phase transition for $x \le 0$. We have grown single crystal samples of Tb$_{2+x}$Ti$_{2-x}$O$_{7+\delta}$, with approximate composition $x=-0.001, +0.0042$, and $+0.0147$, where the $x=0.0042$ single crystal exhibits a large C$_P$ anomaly at $T_C$=0.45 K, but neither the $x=-0.001$ nor the $x=+0.0147$ single crystals display any such anomaly. We present new time-of-flight neutron scattering measurements on the $x=-0.001$ and the $x=+0.0147$ samples which show strong $\left(\frac{1}{2},\frac{1}{2},\frac{1}{2}\right)$ quasi-Bragg peaks at low temperatures characteristic of short range antiferromagnetic spin ice (AFSI) order at zero magnetic field but only under field-cooled conditions, as was previously observed in our $x = 0.0042$ single crystal. These results show that the strong $\left(\frac{1}{2},\frac{1}{2},\frac{1}{2}\right)$ quasi-Bragg peaks and gapped AFSI state at low temperatures under field cooled conditions are robust features of Tb$_2$Ti$_2$O$_7$, and are not correlated with the presence or absence of the C$_P$ anomaly and phase transition at low temperatures. Further, these results show that the ordered state giving rise to the C$_P$ anomaly is confined to $0 \leq x \leq 0.01$ for Tb$_{2+x}$Ti$_{2-x}$O$_{7+\delta}$, and is not obviously connected with conventional order of magnetic dipole degrees of freedom.