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High performance thermal management is of great significance to the data security and working stability of magnetic devices with broad applications from sensing to data storage and spintronics, where there would exist coupling between the spin and phonon (lattice vibrations). However, the knowledge of the spin effect on thermal transport is lacking. Here, we report that the thermal conductivity of monolayer CrI 3 is more than two orders of magnitude enhanced by the spin–lattice coupling. Fundamental understanding is achieved by analyzing the coupling among electronic, magnetic and phononic properties based on the orbital projected electronic structure and spin density. The bond angles and atomic positions are substantially changed due to the spin–lattice coupling, making the structure more stiff and more symmetric, and lead to the weaker phonon anharmonicity, and thus the enhanced thermal conductivity. This study uncovers the giant effect of spin–lattice coupling on the thermal transport, which would deepen our understanding on thermal transport and shed light on future research of thermal transport in magnetic materials.more » « less
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