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 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.Comment: 9 pages, 5 figures (with Supplemental Material), to appear in Physical Review Letter

One-dimensional quantum antiferromagnetism in the p−p-orbital CsO2_2 compound revealed by electron paramagnetic resonance

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.Comment: 6 pages, 3 figure

Neutron diffraction investigation of the H-T phase diagram above the longitudinal incommensurate phase of BaCo2V2O8

The quasi-one-dimensional antiferromagnetic Ising-like compound BaCo2V2O8 has been shown to be describable by the Tomonaga-Luttinger liquid theory in its gapless phase induced by a magnetic field applied along the Ising axis. Above 3.9 T, this leads to an exotic field-induced low-temperature magnetic order, made of a longitudinal incommensurate spin-density wave, stabilized by weak interchain interactions. By single-crystal neutron diffraction we explore the destabilization of this phase at a higher magnetic field. We evidence a transition at around 8.5 T towards a more conventional magnetic structure with antiferromagnetic components in the plane perpendicular to the magnetic field. The phase diagram boundaries and the nature of this second field-induced phase are discussed with respect to previous results obtained by means of nuclear magnetic resonance and electron spin resonance, and in the framework of the simple model based on the Tomonaga-Luttinger liquid theory, which obviously has to be refined in this complex system.Comment: 7 pages, 5 figure

Symmetric and antisymmetric exchange anisotropies in quasi-one-dimensional CuSe2_2O5_5 as revealed by ESR

We present an electron spin resonance (ESR) study of single-crystalline spin chain-system CuSe$_2$O$_5$ in the frequency range between 9 GHz and 450 GHz. In a wide temperature range above the N\'{e}el temperature $T_N=17$ K we observe strong and anisotropic frequency dependence of a resonance linewidth. Although sizeable interchain interaction $J_{IC}\approx 0.1 J$ ($J$ is the intrachain interaction) is present in this system, the ESR results agree well with the Oshikawa-Affleck theory for one-dimensional $S=1/2$ Heisenberg antiferromagnet. This theory is used to extract the anisotropies present in CuSe$_2$O$_5$. We find that the symmetric anisotropic exchange $J_c=(0.04 \pm 0.01) \:J$ and the antisymmetric Dzyaloshinskii-Moriya (DM) interaction $D=(0.05\pm 0.01)\:J$ are very similar in size in this system. Staggered-field susceptibility induced by the presence of the DM interaction is witnessed in the macroscopic susceptibility anisotropy.Comment: 8 pages, 7 figures, 2 tables, published in Phys. Rev.

Antiferromagnetic fluctuations in the normal state of LiFeAs

We present a detailed study of 75As NMR Knight shift and spin-lattice relaxation rate in the normal state of stoichiometric polycrystalline LiFeAs. Our analysis of the Korringa relation suggests that LiFeAs exhibits strong antiferromagnetic fluctuations, if transferred hyperfine coupling is a dominant interaction between 75As nuclei and Fe electronic spins, whereas for an on-site hyperfine coupling scenario, these are weaker, but still present to account for our experimental observations. Density-functional calculations of electric field gradient correctly reproduce the experimental values for both 75As and 7Li sites.Comment: 5 pages, 3 figures, thoroughly revised version with refined experimental data, accepted for publication as a Rapid Communication in Physical Review B

Giant magnetic-field dependence of the coupling between spin Tomonaga-Luttinger liquids in BaCo2V2O8

We use nuclear magnetic resonance to map the complete low-temperature phase diagram of the antiferromagnetic Ising-like spin-chain system BaCo2V2O8 as a function of the magnetic field applied along the chains. In contrast to the predicted crossover from the longitudinal incommensurate phase to the transverse antiferromagnetic phase, we find a sequence of three magnetically ordered phases between the critical fields 3.8 T and 22.8 T. Their origin is traced to the giant magnetic-field dependence of the total effective coupling between spin chains, extracted to vary by a factor of 24. We explain this novel phenomenon as emerging from the combination of nontrivially coupled spin chains and incommensurate spin fluctuations in the chains treated as Tomonaga-Luttinger liquids.Comment: 6 pages, 3 figure