Phonon-Modulated Magnetic Interactions and Spin Tomonaga-Luttinger Liquid in the p-Orbital Antiferromagnet CsO2

The magnetic response of antiferromagnetic CsO2, coming from the p-orbital S=1/2 spins of anionic O2(-) molecules, is followed by 133Cs nuclear magnetic resonance across the structural phase transition occurring at T(s1)=61  K on cooling. Above T(s1), where spins form a square magnetic lattice, we observe a huge, nonmonotonic temperature dependence of the exchange coupling originating from thermal librations of O2(-) molecules. Below T(s1), where antiferromagnetic spin chains are formed as a result of p-orbital ordering, we observe a spin Tomonaga-Luttinger-liquid behavior of spin dynamics. These two interesting phenomena, which provide rare simple manifestations of the coupling between spin, lattice, and orbital degrees of freedom, establish CsO2 as a model system for molecular solids.