Terahertz field-induced metastable magnetization near criticality in FePS3

Abstract

Controlling the functional properties of quantum materials with light has emerged as a frontier of condensed-matter physics, leading to the discovery of various light-induced phases of matter, such as superconductivity, ferroelectricity, magnetism and charge density waves. However, in most cases, the photoinduced phases return to equilibrium on ultrafast timescales after the light is turned off, limiting their practical applications. Here we use intense terahertz pulses to induce a metastable magnetization with a remarkably long lifetime of more than 2.5 milliseconds in the van der Waals antiferromagnet FePS3. The metastable state becomes increasingly robust as the temperature approaches the antiferromagnetic transition point, suggesting that critical order parameter fluctuations play an important part in facilitating the extended lifetime. By combining first-principles calculations with classical Monte Carlo and spin dynamics simulations, we find that the displacement of a specific phonon mode modulates the exchange couplings in a manner that favours a ground state with finite magnetization near the Néel temperature. This analysis also clarifies how the critical fluctuations of the dominant antiferromagnetic order can amplify both the magnitude and the lifetime of the new magnetic state. Our discovery demonstrates the efficient manipulation of the magnetic ground state in layered magnets through non-thermal pathways using terahertz light and establishes regions near critical points with enhanced order parameter fluctuations as promising areas to search for metastable hidden quantum states.

33 pages, 4 figures

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Cited by in corpus (13)

• Time-domain study of coupled collective excitations in quantum materials
• Terahertz-field activation of polar skyrons
• Terahertz Control of Linear and Nonlinear Magno-Phononics
• Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets
• Simple THz phase retarder based on Mach-Zehnder interferometer for polarization control
• Modifying electronic and structural properties of 2D van der Waals materials via cavity quantum vacuum fluctuations: A first-principles QEDFT study
• Steady-states and response functions of the periodically driven O(N) scalar field theory
• Long-range magnetic order with disordered spin orientations in a high-entropy antiferromagnet
• Switching of an antiferromagnet controlled by spin canting in a laser-induced hidden phase
• Frequency renormalization and its effects in nonlinear phononics with $Q_R{Q}_{IR}^2$-type coupling
• Stabilization of zigzag order in NiPS${}_3$ via positive biquadratic interaction
• Ultrafast magnetic moment transfer and bandgap renormalization in monolayer FeCl${}_2$
• Van der Waals Antiferromagnets: From Early Discoveries to Future Directions in the 2D Limit