One-dimensional quantum antiferromagnetism in the $p-$orbital CsO$_2$ compound revealed by electron paramagnetic resonance

TL;DR

This study uses electron paramagnetic resonance to reveal one-dimensional quantum antiferromagnetic behavior in the $p$-orbital CsO$_2$ compound, confirming the formation of spin-1/2 chains and analyzing their quantum properties.

Contribution

It provides the first detailed EPR analysis of the $p$-orbital CsO$_2$ compound, demonstrating quantum antiferromagnetic chains and characterizing their Tomonaga-Luttinger liquid behavior.

Findings

EPR signal appears below structural transition at 61 K

Antiferromagnetic resonance observed below 8.3 K

TLL exponent determined as K=0.48

Abstract

Recently it was proposed that the orbital ordering of $\pi_{x,y}^*$ molecular orbitals in the superoxide CsO$_2$ compound leads to the formation of spin-1/2 chains below the structural phase transition occuring at $T_{\rm{s1}}=61$~K on cooling. Here we report a detailed X-band electron paramagnetic resonance (EPR) study of this phase in CsO$_2$ powder. The EPR signal appears as a broad line below $T_{\rm{s1}}$, which is replaced by the antiferromagnetic resonance below the N\'{e}el temperature $T_{\rm N}=8.3$~K. The temperature dependence of the EPR linewidth between $T_{\rm{s1}}$ and $T_{\rm{N}}$ agrees with the predictions for the one-dimensional Heisenberg antiferromagnetic chain of $S=1/2$ spins in the presence of symmetric anisotropic exchange interaction. Complementary analysis of the EPR lineshape, linewidth and the signal intensity within the Tomonaga-Luttinger liquid (TLL) framework allows for a determination of the TLL exponent $K=0.48$. Present EPR data thus fully comply with the quantum antiferromagnetic state of spin-1/2 chains in the orbitally ordered phase of CsO$_2$, which is, therefore, a unique $p-$orbital system where such a state could be studied.