Second-harmonic generation is of paramount importance in several fields of science and technology, including frequency conversion, self-referencing of frequency combs, nonlinear spectroscopy and pulse characterization. Advanced functionalities are enabled by modulation of the harmonic generation efficiency, which can be achieved with electrical or all-optical triggers. Electrical control of the harmonic generation efficiency offers large modulation depth at the cost of low switching speed, by contrast to all-optical nonlinear devices, which provide high speed and low modulation depth. Here we demonstrate all-optical modulation of second-harmonic generation in MoS₂ with a modulation depth of close to 100% and speed limited only by the fundamental pulse duration. This result arises from a combination of D_3h crystal symmetry and the deep subwavelength thickness of the sample, it can therefore be extended to the whole family of transition metal dichalcogenides to provide great flexibility in the design of advanced nonlinear optical devices such as high-speed integrated frequency converters, broadband autocorrelators for ultrashort pulse characterization, and tunable nanoscale holograms.

Triggered by advances in atomic-layer exfoliation and growth techniques, along with the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or a few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals now constitute a broad research field expanding in multiple directions through the combination of layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary subset of those directions, where 2D materials contribute remarkable nonlinearities, long-lived and ultraconfined polaritons, strong excitons, topological and chiral effects, susceptibility to external stimuli, accessibility, robustness, and a completely new range of photonic materials based on layer stacking, gating, and the formation of moiré patterns. These properties are being leveraged to develop applications in electro-optical modulation, light emission and detection, imaging and metasurfaces, integrated optics, sensing, and quantum physics across a broad spectral range extending from the far-infrared to the ultraviolet, as well as enabling hybridization with spin and momentum textures of electronic band structures and magnetic degrees of freedom. The rapid expansion of photonics with 2D materials as a dynamic research arena is yielding breakthroughs, which this Roadmap summarizes while identifying challenges and opportunities for future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

Optical communication can be revolutionized by encoding data into the orbital angular momentum of light beams. However, state-of-the-art approaches for dynamic control of complex optical wavefronts are mainly based on liquid crystal spatial light modulators or miniaturized mirrors, which suffer from intrinsically slow (µs-ms) response times. Here, we experimentally realize a hybrid meta-optical system that enables complex control of the wavefront of light with pulse-duration limited dynamics. Specifically, by combining ultrafast polarization switching in a WSe₂ monolayer with a dielectric metasurface, we demonstrate second harmonic beam deflection and structuring of orbital angular momentum on the femtosecond timescale. Our results pave the way to robust encoding of information for free space optical links, while reaching response times compatible with real-world telecom applications.

In monolayer transition metal dichalcogenides, time-reversal symmetry—combined with broken space-inversion symmetry—defines the spin–valley degree of freedom. As such, the engineering and control of time-reversal symmetry by optical or magnetic fields constitutes the foundation of valleytronics. Here we propose a new approach for the detection of broken time-reversal symmetry and valley imbalance in monolayer WSe₂ based on second-harmonic generation. At room temperature, our method can selectively probe a net valley imbalance generated by ultrafast, coherent and valley-exclusive optical Stark and Bloch–Siegert effects. This work demonstrates the potential and unique capabilities of nonlinear optics as a probe of broken time-reversal symmetry as well as a tool for ultrafast and non-destructive valleytronic operations.

With conventional electronics reaching performance and size boundaries, all‐optical processes have emerged as ideal building blocks for high speed and low power consumption devices. A promising approach in this direction is provided by valleytronics in atomically thin semiconductors, where light‐matter interaction allows to write, store, and read binary information into the two energetically degenerate but non‐equivalent valleys. Here, nonlinear valleytronics in monolayer WSe₂ is investigated and show that an individual ultrashort pulse with a photon energy tuned to half of the optical band‐gap can be used to simultaneously excite (by coherent optical Stark shift) and detect (by a rotation in the polarization of the emitted second harmonic) the valley population.