Spin-phonon scattering-induced low thermal conductivity in a van der Waals layered ferromagnet Cr$_2$Si$_2$Te$_6$

Layered van der Waals (vdW) magnets are prominent playgrounds for developing magnetoelectric, magneto-optic and spintronic devices. In spintronics, particularly in spincaloritronic applications, low thermal conductivity ($\kappa$) is highly desired. Here, by combining thermal transport measurements with density functional theory calculations, we demonstrate low $\kappa$ down to 1 W m$^{-1}$ K$^{-1}$ in a typical vdW ferromagnet Cr$_2$Si$_2$Te$_6$. In the paramagnetic state, development of magnetic fluctuations way above $T_\mathrm{c}=$ 33 K strongly reduces $\kappa$ via spin-phonon scattering, leading to low $\kappa \sim$ 1 W m$^{-1}$ K$^{-1}$ over a wide temperature range, in comparable to that of amorphous silica. In the magnetically ordered state, emergence of resonant magnon-phonon scattering limits $\kappa$ below $\sim$ 2 W m$^{-1}$ K$^{-1}$, which would be three times larger if magnetic scatterings were absent. Application of magnetic fields strongly suppresses the spin-phonon scattering, giving rise to large enhancements of $\kappa$. Our calculations well capture these complex behaviours of $\kappa$ by taking the temperature- and magnetic-field-dependent spin-phonon scattering into account. Realization of low $\kappa$ which is easily tunable by magnetic fields in Cr$_2$Si$_2$Te$_6$, may further promote spincaloritronic applications of vdW magnets. Our theoretical approach may also provide a generic understanding of spin-phonon scattering, which appears to play important roles in various systems.
Comment: 14 pages, 6 figures, accepted for publication in Advanced Functional Materials