Emergence of Spin Ice freezing in Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$

TL;DR

This study investigates how Mn substitution in Dy2Ti2O7 alters spin ice freezing temperatures and magnetic interactions, revealing enhanced ferromagnetism and thermally induced spin relaxations in Dy2Ti1.8Mn0.2O7.

Contribution

It demonstrates that Mn doping shifts spin freezing temperatures higher and enhances ferromagnetic interactions in Dy2Ti2O7, providing insights into tuning spin ice behavior.

Findings

Spin freezing temperature T_i shifts from 3 K to 5 K with Mn doping.

Enhanced ferromagnetic interactions observed in Mn-doped compound.

Crystal field phonon coupling emerges at higher temperature in Mn-doped sample.

Abstract

We herein present the spin freezing dynamics of stuffed polycrystalline compound Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$. In Dy$_2$Ti$_2$O$_7$, spin freezes with ice-like spin relaxations at a temperature around 3 K (T$_i$) along with another spin freezing at a temperature around 0.7 K (T\textless T$_i$). These relaxations can be observed prominently with an application of varying DC magnetic field bias and applied AC-field. We show here that with fractional inclusion of Mn at the Ti site in Dy$_2$Ti$_2$O$_7$, there is a significant shift in these temperatures. In Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$ the T$_i$ shifts to a higher temperature around 5 K and freezing belonging to T\textless T$_i$ shifts to 2.5 K without any application of external DC Bias and/or AC-field. The inclusion of Mn at Ti site also enhances the ferromagnetic interaction for Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$ as compared to Dy$_2$Ti$_2$O$_7$. Arrhenius fit of freezing temperature with frequency for Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$ shows that these spin relaxations at T$_i$ and T\textless T$_i$ are thermally induced. Low-temperature structural change in lattice parameters and crystal field phonon coupling has been studied using synchrotron x-ray diffraction. Debye-Gruineisen analysis of temperature-dependent lattice volume shows the emergence of crystal field phonon coupling at a much higher temperature (70 K) in Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$ in contrast to 40 K in Dy$_2$Ti$_2$O$_7$. These findings make Dy$_2$Ti$_{1.8}$Mn$_{0.2}$O$_7$ a suitable system to explore the application of the spin ice phenomenon at a workable temperature.