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Abstract

The magnetic response of antiferromagnetic CsO2, coming from the p-orbital S = 1/2 spins of anionic O-2(-) molecules, is followed by Cs-133 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 O-2(-) 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.