Thermally enhanced magnon-phonon resonance in van der Waals antiferromagnet FePS3

Strong coupling between collective excitations provides a route to controlling quantum states of matter, yet its evolution under thermal fluctuations remains poorly understood. In the van der Waals antiferromagnet FePS3, strong magnon-phonon coupling is established at low temperatures. At the same time, recent terahertz experiments revealed the counterintuitive stabilization of a long-lived metastable magnetic state with an exceedingly long lifetime of 5 msec at the antiferromagnetic transition, not at the base temperature. This was attributed to a strongly coupled spin-lattice scenario, challenging the conventional wisdom that increased magnetic and thermal fluctuations near TN should be detrimental to the coherent control of a metastable phase. Thus it requires an independent examination for correct understanding. Using high-field Raman spectroscopy, we systematically investigate the temperature evolution of magnon-phonon coupling in FePS3. We observe a pronounced avoided crossing between magnon and phonon modes across a wide range of temperatures and find that the coupling strength remains remarkably robust with increasing temperatures. The zero-field magnon-phonon detuning decreases progressively with warming, driving the system toward resonance and thereby enhancing their hybridization near the transition temperature. This anomalous thermal evolution provides the crucial key to understanding the unusual terahertz-driven states recently reported in FePS3. More broadly, our results highlight van der Waals magnets as a promising platform for strong coupling among collective excitations and for controlling magnetic states through light-matter interactions.