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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 (κ) is highly desired. Herein, by combining thermal transport measurements with density functional theory calculations, this study demonstrates low κ down to 1 W m−1 K−1 in a typical vdW ferromagnet Cr2Si2Te6. In the paramagnetic state, development of magnetic fluctuations way above Tc = 33 K strongly reduces κ via spin‐phonon scattering, leading to low κ ≈ 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 κ below ≈2 W m−1 K−1, which will be three times larger if magnetic scatterings are absent. Application of magnetic fields strongly suppresses the spin‐phonon scattering, giving rise to large enhancements of κ. This study's calculations well capture these complex behaviors of κ by taking the temperature‐ and magnetic‐field‐dependent spin‐phonon scattering into account. Realization of low κ, which is easily tunable by magnetic fields in Cr2Si2Te6, may further promote spincaloritronic applications of vdW magnets. This study's theoretical approach may also provide a generic understanding of spin‐phonon scattering, which appears to play important roles in various systems. [ABSTRACT FROM AUTHOR]

The electron–phonon coupling (EPC) in semiconductors is typically much weaker than phonon–phonon scattering and its effect on lattice thermal conductivity κl has long been considered negligible. Herein, using first‐principle calculations, it is discovered that the EPC can be significant or even dominant over the intrinsic phonon–phonon scattering via doping in 2D semiconductor hexagonal boron phosphorus (h‐BP). Filling electron pocket till van Hove singularity gradually strengthens the EPC and consequently diminishes the room‐temperature κl by 25% and 80% for monolayer and bilayer h‐BP, respectively. Strikingly, at high doping levels, the EPC drives phonon transport in bilayer h‐BP to an anomalous regime where κl becomes nearly temperature (T) independent deviated from the intrinsic 1/T trend. This distinctive behavior is governed by the joint effects of horizontal mirror symmetry breaking, and weak phonon–phonon scattering stemming from the predominance of normal processes. Further considering electronic contributions, the abnormal T‐independent thermal conductivity is still reserved, thereby facilitating the experimental exploration of EPC effect on κl. This study unveils the exotic thermal transport phenomenon in one‐atom‐thick 2D semiconductors and offers a unique avenue to manipulate heat flow by externally controlling the EPC, which calls for future experimental verification. [ABSTRACT FROM AUTHOR]

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 (κ) is highly desired. Herein, by combining thermal transport measurements with density functional theory calculations, this study demonstrates low κ down to 1 W m−1 K−1 in a typical vdW ferromagnet Cr2Si2Te6. In the paramagnetic state, development of magnetic fluctuations way above Tc = 33 K strongly reduces κ via spin‐phonon scattering, leading to low κ ≈ 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 κ below ≈2 W m−1 K−1, which will be three times larger if magnetic scatterings are absent. Application of magnetic fields strongly suppresses the spin‐phonon scattering, giving rise to large enhancements of κ. This study's calculations well capture these complex behaviors of κ by taking the temperature‐ and magnetic‐field‐dependent spin‐phonon scattering into account. Realization of low κ, which is easily tunable by magnetic fields in Cr2Si2Te6, may further promote spincaloritronic applications of vdW magnets. This study's theoretical approach may also provide a generic understanding of spin‐phonon scattering, which appears to play important roles in various systems. [ABSTRACT FROM AUTHOR]