Generating a pure spin current using electrons, which have degrees of freedom beyond spin, such as electric charge and valley index, presents challenges. In response, we propose a mechanism based on intervalley exciton dynamics in arc-shaped strained transition metal dichalcogenides (TMDs) to achieve the exciton spin Hall effect in an electrically insulating regime, without the need for an external electric field. The interplay between strain gradients and strain-induced pseudomagnetic fields results in a net Lorentz force on long-lived intervalley excitons in WSe2, carrying nonzero spin angular momentum. This process generates an exciton-mediated pure spin Hall current, resulting in opposite-sign spin accumulations and local magnetization on the two sides of the single-layer arc-shaped TMD. We demonstrate that the magnetic field induced by spin accumulation, at approximately ∼mT, can be detected using techniques such as superconducting quantum interference magnetometry or spatially resolved magneto-optical Faraday and Kerr rotations.

In this theoretical investigation, we analyze light-induced nonlinear spin Hall currents in a gated single-layer 1T′-WTe₂, flowing transversely to the incident laser polarization direction. Our study encompasses the exploration of the second and third-order rectified spin Hall currents using an effective low-energy Hamiltonian and employing the Kubo's formalism. We extend our analysis to a wide frequency range spanning both transparent and absorbing regimes, investigating the influence of light frequency below and above the optical band gap. Additionally, we investigate the influence of an out-of-plane gate potential on the system, disrupting inversion symmetry and effectively manipulating both the strength and sign of nonlinear spin Hall responses. We predict a pronounced third-order spin Hall current relative to its second-order counterpart. The predicted nonlinear spin currents show strong anisotropic dependence on the laser polarization angle. The outcomes of our study contribute to a generalized framework for nonlinear response theory within the spin channel will impact the development of emerging field of opto-spintronic.

Twisting bilayer sheets of graphene have been proven to be an efficient way to manipulate the electronic Dirac-like properties, resulting in flat bands at magic angles. Inspired by the electronic model, we develop a continuum model for the lattice dynamics of twisted bilayer graphene and we show that a remarkable band flattening applies to almost all the high-frequency in-plane lattice vibration modes, including the valley Dirac phonon, valley optical phonon, and zone-center optical phonon bands. Utilizing an approximate approach, we estimate small but finite magic angles at which a vanishing phonon bandwidth is expected. In contrast to the electronic case, the existence of a restoring potential prohibits the emergence of a magic angle in a more accurate modeling. The predicted phonon band flattening is highly tunable by the twist angle and this strong dependence is directly accessible by spectroscopic tools.

The generation of entangled photons by spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing (SFWM) attracted enormous interest in the field of quantum optics. Depending on applications, entangled photon sources prioritize either bandwidth (e.g. for quantum imaging) or brightness (e.g. for quantum key distribution). Layered materials offer unique advantages for both. They have already been used to realize thinnest SPDC sources [1], which, like other layered materials such as transition-metal dichalcogenides (TMDs) [2], offer nearly unlimited bandwidth thanks to relaxed phase-matching constraints. Further, their easy integration on photonic platforms is promising for bright on-chip entangled photon sources. In this context, SPDC-based solutions are limited by phase-matching, whereas SFWM would be an almost phase-matching-free process, as pump, idler, and signal photons can be generated at similar wavelengths, thus propagating at the same group velocity in integrated devices. Moreover, exploiting excitonic resonances could enhance FWM even more. However, to date, experiments with resonant FWM in TMDs have been limited to signals in the visible [3], which is unsuitable for integrated photonics and telecom systems due to reabsorption during propagation in the photonic device.

The Faraday Discussion 'From optical to THz control of materials' was held in London, UK, and online on the 23rd, 24th, and 25th May 2022. The meeting brought together established and early-career scientists, postgraduate students, scientific editors, and industrial researchers in the field of spectroscopy and materials science from over ten different countries interested in exploring the physical properties of materials at ultrafast timescales driven by optical and THz excitations. This conference report provides highlights of this meeting and we give summaries of the presentations including the introductory lecture, all the papers discussed, and the concluding remarks.

Coherent engineering of landscape potential in crystalline materials is a rapidly evolving research field. Ultrafast optical pulses can manipulate low-frequency shear phonons in van der Waals layered materials through the dynamical dressing of electronic structure and photoexcited carrier density. In this work, we provide a diagrammatic formalism for nonlinear Raman force and implement it to shear phonon dynamics in bilayer graphene. We predict a controllable splitting of double degenerate shear phonon modes due to light-induced phonon mixing and renormalization according to a coherent nonlinear Raman force mechanism. Intriguingly, we obtain a light-induced shear phonon softening that facilitates structural instability at a critical field amplitude for which the shear phonon frequency vanishes. The phonon splitting and instability strongly depend on the laser intensity, frequency, chemical potential, and temperature of photoexcited electrons. This study motivates future experimental investigation of the optical fine tuning and regulation of shear phonons and layer stacking order in layered van der Waals materials.

Electronic states and their dynamics are of critical importance for electronic and optoelectronic applications. Here, various relevant electronic states in monolayer MoS2, such as multiple excitonic Rydberg states and free-particle energy bands are probed with a high relative contrast of up to ≥200 via broadband (from ≈1.79 to 3.10 eV) static third-harmonic spectroscopy (THS), which is further supported by theoretical calculations. Moreover, transient THS is introduced to demonstrate that third-harmonic generation can be all-optically modulated with a modulation depth exceeding ≈94% at ≈2.18 eV, providing direct evidence of dominant carrier relaxation processes associated with carrier–exciton and carrier–phonon interactions. The results indicate that static and transient THS are not only promising techniques for the characterization of monolayer semiconductors and their heterostructures, but also a potential platform for disruptive photonic and optoelectronic applications, including all-optical modulation and imaging.

Using a diagrammatic scheme, we study the acoustoelectric effects in two-dimensional (2D) hexagonal Dirac materials due to the sound-induced pseudogauge field. We analyze both uniform and spatially dispersive currents in response to copropagating and counterpropagating sound waves, respectively. In addition to the longitudinal acoustoelectric current, we obtain an exotic transverse charge current flowing perpendicular to the sound propagation direction owing to the interplay of transverse and longitudinal gauge field components jT∝ALA∗T. In contrast to the almost isotropic directional profile of the longitudinal uniform current, a highly anisotropic transverse component jT∼sin(6θ) is achieved that stems from the inherited threefold symmetry of the hexagonal lattice. However, both longitudinal and transverse parts of the dispersive current are predicted to be strongly anisotropic ∼sin2(3θ) or cos2(3θ). We quantitatively estimate the pseudogauge field contribution to the acoustoelectric current that can be probed in future experiments in graphene and other 2D hexagonal Dirac materials.

A single layer of the 1T' phase of WTe2 provides a rich platform for exotic physical properties such as the nonlinear Hall effect and high-temperature quantum spin Hall transport. Utilizing a continuum model and the diagrammatic method, we calculate the second harmonic conductivity of monolayer 1T'-WTe2 modulated by an external vertical electric field and electron doping. We obtain a finite helicity and Faraday rotation for the second harmonic signal in response to linearly polarized incident light in the presence of time-reversal symmetry. The second harmonic signal's helicity is highly controllable by altering the bias potential and serves as an optical indicator of the nonlinear Hall current. Our study motivates future experimental investigation of the helicity spectroscopy of two-dimensional materials.

Hexagonal two-dimensional materials with broken inversion symmetry (as BN or transition metal dichalcogenides) are known to sustain chiral phonons with finite angular momentum, adding a further useful degree of freedom to the extraordinary entangled (electrical, optical, magnetic, and mechanical) properties of these compounds. However, because of lattice symmetry constraints, such chiral modes are constrained to the corners of the Brillouin zone, allowing little freedom for manipulating the chiral features. In this paper, we show how the application of uniaxial strain leads to the existence of unique chiral modes in the vicinity of the zone center. We also show that such strain-induced chiral modes, unlike the ones pinned at the K points, can be efficiently manipulated by modifying the strain itself, which determines the position of these modes in the Brillouin zone. The present paper results add a technique for the engineering of the quantum properties of two-dimensional lattices.