Search for: All records

Understanding thermal transport in solid electrolytes is essential for improving the performance, reliability, and safety of all-solid-state batteries. Garnet-type lithium-ion conductors are promising candidates for solid electrolytes, yet their thermal-transport mechanisms remain poorly understood. Here, we connect the lattice and ion dynamics of single-crystal garnet-type ${\mathrm{Li}}_{6.5}$ ${\mathrm{La}}_3$ ${\mathrm{Zr}}_{1.5}$ ${\mathrm{Ta}}_{0.5}$ ${\mathrm{O}}_{12}$to its intrinsically low thermal conductivity. Our study reveals that the single crystals grown by the floating-zone method exhibit remarkably low glasslike thermal conductivity. Using first-principles calculations and inelastic-neutron-scattering measurements, we identify both the acoustic and numerous optical phonon modes, which stem from the complex crystal structure of the material. Notably, a low-energy optical branch exhibits an avoided crossing with acoustic phonons near 7 meV. These optical modes can enhance the scattering of heat-carrying acoustic phonons and reduce thermal conductivity. Furthermore, the calculated Grüneisen parameters are large, especially for the vibrational modes around 6 meV, indicating strong anharmonicity, with a noticeable contribution from lithium-ion vibrations. A two-channel thermal-transport model is employed to describe the weak temperature dependence of the thermal conductivity, which can be attributed to the substantial contribution of diffuson transport facilitated by the abundance of optical phonons and intrinsic anharmonicity. These results offer valuable insights into the thermal transport in a broad class of ionic conductors of interest for energy conversion and storage applications. 

Cobalt titanate, CoTiO3, is a honeycomb antiferromagnet recently confirmed experimentally to host Dirac magnons, topological spin-orbit excitons, and chiral phonons. Here, we investigate a magnon gap at the zone center which calls for a refined spin Hamiltonian. We propose a microscopic model for the magnon gap and attribute it to a lattice-distortion (phonon)-induced higher-order spin interaction. Strong magnetoelastic coupling in CoTiO3 is also evident in Raman spectra, in which the magnetic order exerts a stronger influence on phonons corresponding to in-plane ionic motions than those with out-of-plane motions. We further examine the evolution of the zone-center magnons in a high magnetic field up to 18.5 T via THz absorption spectroscopy measurements. Based on this field dependence, we propose a spin Hamiltonian that not only agrees with magnon dispersion measured by inelastic neutron scattering but also includes fewer exchange constants and a realistic anisotropy term. Our work highlights the broad implications of magnetoelastic coupling in the study of topologically protected bosonic excitations. 

The interplay of charge, spin, lattice, and orbital degrees of freedom in correlated materials often leads to rich and exotic properties. Recent studies have brought new perspectives to bosonic collective excitations in correlated materials. For example, inelastic neutron scattering experiments revealed non-trivial band topology for magnons and spin–orbit excitons (SOEs) in a quantum magnet CoTiO₃(CTO). Here, we report phonon properties resulting from a combination of strong spin–orbit coupling, large crystal field splitting, and trigonal distortion in CTO. Specifically, the interaction between SOEs and phonons endows chirality to two $E_g$phonon modes and leads to large phonon magnetic moments observed in magneto-Raman spectra. The remarkably strong magneto-phononic effect originates from the hybridization of SOEs and phonons due to their close energy proximity. While chiral phonons have been associated with electronic topology in some materials, our work suggests opportunities may arise by exploring chiral phonons coupled to topological bosons.