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Abstract Optical manipulation of coherent phonon frequency in two-dimensional (2D) materials could advance the development of ultrafast phononics in atomic-thin platforms. However, conventional approaches for such control are limited to doping, strain, structural or thermal engineering. Here, we report the experimental observation of strong laser-polarization control of coherent phonon frequency through time-resolved pump-probe spectroscopic study of van der Waals (vdW) materials Fe 3 GeTe 2 . When the polarization of the pumping laser with tilted incidence is swept between in-plane and out-of-plane orientations, the frequencies of excited phonons can be monotonically tuned by as large as 3% (~100 GHz). Our first-principles calculations suggest the strong planar and vertical inter-atomic interaction asymmetry in layered materials accounts for the observed polarization-dependent phonon frequencies, as in-plane/out-of-plane polarization modifies the restoring force of the lattice vibration differently. Our work provides insightful understanding of the coherent phonon dynamics in layered vdW materials and opens up new avenues to optically manipulating coherent phonons. 

Abstract The interplay between chirality and magnetism generates a distinct physical process, the magneto-chiral effect, which enables one to develop functionalities that cannot be achieved solely by any of the two. Such a process is universal with the breaking of parity-inversion and time-reversal symmetry simultaneously. However, the magneto-chiral effect observed so far is weak when the matter responds to photons, electrons, or phonons. Here we report the first observation of strong magneto-chiral response to excitons in a twisted bilayer tungsten disulfide with the amplitude of excitonic magneto-chiral (ExMCh) anisotropy reaches a value of ~4%. We further found the ExMCh anisotropy features with a spectral splitting of ~7 nm, precisely the full-width at half maximum of the excitonic chirality spectrum. Without an externally applied strong magnetic field, the observed ExMCh effect with a spontaneous magnetic moment from the ferromagnetic substrate of thulium iron garnet at room temperature is favorable for device applications. The unique ExMCh processes provide a new pathway to actively control magneto-chiral applications in photochemical reactions, asymmetric synthesis, and drug delivery. 

Engineering the electronic band structure of material systems enables the unprecedented exploration of new physical properties that are absent in natural or as-synthetic materials. Half metallicity, an intriguing physical property arising from the metallic nature of electrons with singular spin polarization and insulating for oppositely polarized electrons, holds a great potential for a 100% spin-polarized current for high-efficiency spintronics. Conventionally synthesized thin films hardly sustain half metallicity inherited from their 3D counterparts. A fundamental challenge, in systems of reduced dimensions, is the almost inevitable spin-mixed edge or surface states in proximity to the Fermi level. Here, we predict electric field-induced half metallicity in bilayer A-type antiferromagnetic van der Waals crystals (i.e., intralayer ferromagnetism and interlayer antiferromagnetism), by employing density functional theory calculations on vanadium diselenide. Electric fields lift energy levels of the constituent layers in opposite directions, leading to the gradual closure of the gap of singular spin-polarized states and the opening of the gap of the others. We show that a vertical electrical field is a generic and effective way to achieve half metallicity in A-type antiferromagnetic bilayers and realize the spin field effect transistor. The electric field-induced half metallicity represents an appealing route to realize 2D half metals and opens opportunities for nanoscale highly efficient antiferromagnetic spintronics for information processing and storage.