Light-Induced Transient Polarization Reversal in Rhombohedrally Stacked Bilayer Transition Metal Dichalcogenides via an Electronic Mechanism

Abstract

Light-induced sliding ferroelectricity in two-dimensional van der Waals materials enables polarization control via relative layer motion. However, polarization switching occurs on the time scale of shear modes (tens of ps) and requires very large fluences, potentially damaging the samples. Here, using constrained density functional theory and many-body real-time simulations, we demonstrate an ultrafast electronic reversal of the total out-of-plane polarization sign in the photoexcited state, without requiring interlayer sliding, in rhombohedrally stacked transition-metal dichalcogenide bilayers. The polarization changes sign relative to its initial ground-state value at moderate fluences and within $\sim$ 200 fs, about 50 times faster than the typical shear-mode period. The ultrafast switching is driven by a rearrangement of localized dipoles around the tungsten sites. We establish a novel general mechanism for electronic control of low-dimensional ferroelectrics common to all polar multilayers having type II band alignment. Our work has direct implications for ultrahigh-speed volatile optical memory operating on sub-ps time scales.

References in corpus (22)

• SciPy 1.0--Fundamental Algorithms for Scientific Computing in Python
• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Phonons and related properties of extended systems from density-functional perturbation theory
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Optimized norm-conserving Vanderbilt pseudopotentials
• Pseudopotentials for high-throughput DFT calculations
• Thermal Contraction and Disordering of the Al(110) Surface
• Stacking-engineered ferroelectricity in bilayer boron nitride
• Precision and efficiency in solid-state pseudopotential calculations
• Interfacial Ferroelectricity by van-der-Waals Sliding
• Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides
• Interfacial ferroelectricity in marginally twisted 2D semiconductors
• Density functional perturbation theory for gated two-dimensional heterostructures: Theoretical developments and application to flexural phonons in graphene
• Light-induced emergent phenomena in 2D materials and topological materials
• Ultrafast reversal of the ferroelectric polarization
• Cumulative Polarization Coexisting with Conductivity at Interfacial Ferroelectrics
• Ultrafast dynamics of the low frequency shear mode in $1{\mathrm{T}}^{\prime }-\mathrm{MoT}{\mathrm{e}}_2$
• EPIq : an open-source software for the calculation of electron-phonon interaction related properties
• Ultrafast Laser Ablation, Intrinsic Threshold, and Nanopatterning of Monolayer Molybdenum Disulfide
• Large photo-induced tuning of ferroelectricity in sliding ferroelectrics
• Light-Induced Nonthermal Phase Transition to the Topological Crystalline Insulator State in SnSe
• Nonequilibrium Photocarrier and Phonon Dynamics from First Principles: a Unified Treatment of Carrier-Carrier, Carrier-Phonon, and Phonon-Phonon Scattering