Phonon-modulated magnetic interactions and spin Tomonaga-Luttinger liquid in the p-orbital antiferromagnet CsO2

Abstract

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 occuring at Ts1=61 K on cooling. Above Ts1, 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 Ts1, 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.

9 pages, 5 figures (with Supplemental Material), to appear in Physical Review Letters

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• A new high-temperature quantum spin liquid with polaron spins
• Observation of two types of anyons in the Kitaev honeycomb magnet
• Experimental signatures of quantum and topological states in frustrated magnetism
• Dichotomy between Attractive and Repulsive Tomonaga-Luttinger Liquids in Spin Ladders
• Instabilities of Spin-Liquid States in a Quantum Kagome Antiferromagnet
• Temperature dependence of the NMR relaxation rate 1/T_1 for quantum spin chains
• Dynamical response and dimensional crossover for spatially anisotropic antiferromagnets
• Superconductivity in the regime of attractive interactions in the Tomonaga-Luttinger liquid
• Magnetism and high-magnetic field magnetization in alkali superoxide CsO2
• Spin-dimer ground state driven by consecutive charge and orbital ordering transitions in the anionic mixed-valence compound Rb${}_4$O${}_6$
• Spin-gap formation due to spin-Peierls instability in $\pi$-orbital-ordered NaO${}_2$
• Antiferromagnetic structure of alkali metal superoxide CsO${}_2$
• The crystal and magnetic structure of cesium superoxide
• Spin-Orbital Ordering in Alkali Superoxides