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Low dimensional magnetism has been powerfully boosted as a promising candidate for numerous applications. The stability of the long-range magnetic order is directly dependent on the electronic structure and the relative strength of the competing magnetic exchange constants. Here, we report a comparative pressure-dependent theoretical and experimental study of the electronic structure and exchange interactions of two-dimensional ferromagnets CrBr 3 and Cr 2 Ge 2 Te 6 . While CrBr 3 is found to be a Mott–Hubbard-like insulator, Cr 2 Ge 2 Te 6 shows a charge-transfer character due to the broader character of the Te 5p bands at the Fermi level. This different electronic behaviour is responsible for the robust insulating state of CrBr 3 , in which the magnetic exchange constants evolve monotonically with pressure, and the proximity to a metal–insulator transition predicted for Cr 2 Ge 2 Te 6 , which causes a non-monotonic evolution of its magnetic ordering temperature. We provide a microscopic understanding for the pressure evolution of the magnetic properties of the two systems. 

The lattice thermal conductivity (κ_ph) of metals and semimetals is limited by phonon‐phonon scattering at high temperatures and by electron‐phonon scattering at low temperatures or in some systems with weak phonon‐phonon scattering. Following the demonstration of a phonon band engineering approach to achieve an unusually high κ_phin semiconducting cubic‐boron arsenide (c‐BAs), recent theories have predicted ultrahigh κ_phof the semimetal tantalum nitride in the θ‐phase (θ‐TaN) with hexagonal tungsten carbide (WC) structure due to the combination of a small electron density of states near the Fermi level and a large phonon band gap, which suppress electron‐phonon and three‐phonon scattering, respectively. Here, measurements on the thermal and electrical transport properties of polycrystalline θ‐TaN converted from the ε phase via high‐pressure synthesis are reported. The measured thermal conductivity of the θ‐TaN samples shows weak temperature dependence above 200 K and reaches up to 90 Wm⁻¹K⁻¹, one order of magnitude higher than values reported for polycrystalline ε‐TaN and δ‐TaN thin films. These results agree with theoretical calculations that account for phonon scattering by 100 nm‐level grains and suggest κ_phincrease above the 249 Wm⁻¹K⁻¹value predicted for single‐crystal WC when the grain size of θ‐TaN is increased above 400 nm.