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Controlling the phases of matter is a central task in condensed matter physics and materials science. In 2D magnets, manipulating spin orientation is of great significance in the context of the Mermin–Wagner theorem. Herein, a systematic study of temperature‐ and pressure‐dependent magnetic properties up to 1 GPa in van der Waals CrPS4 is reported. Owing to the temperature‐dependent change of the...
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