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Phase-change materials (PCMs) offer a compelling platform for active metaoptics, owing to their large index contrast and fast yet stable phase transition attributes. Despite recent advances in phase-change metasurfaces, a fully integrable solution that combines pronounced tuning measures, i.e., efficiency, dynamic range, speed, and power consumption, is still elusive. Here, we demonstrate an in situ electrically driven tunable metasurface by harnessing the full potential of a PCM alloy, Ge₂Sb₂Te₅(GST), to realize non-volatile, reversible, multilevel, fast, and remarkable optical modulation in the near-infrared spectral range. Such a reprogrammable platform presents a record eleven-fold change in the reflectance (absolute reflectance contrast reaching 80%), unprecedented quasi-continuous spectral tuning over 250 nm, and switching speed that can potentially reach a few kHz. Our scalable heterostructure architecture capitalizes on the integration of a robust resistive microheater decoupled from an optically smart metasurface enabling good modal overlap with an ultrathin layer of the largest index contrast PCM to sustain high scattering efficiency even after several reversible phase transitions. We further experimentally demonstrate an electrically reconfigurable phase-change gradient metasurface capable of steering an incident light beam into different diffraction orders. This work represents a critical advance towards the development of fully integrable dynamic metasurfaces and their potential for beamforming applications.

Ultrafast optical switching in plasmonic platforms relies on the third‐order Kerr nonlinearity, which is tightly linked to the dynamics of hot carriers in nanostructured metals. Although extensively utilized, a fundamental understanding on the dependence of the switching dynamics upon optical resonances has often been overlooked. Here, all‐optical control of resonance bands in a hybrid photonic‐plasmonic crystal is employed as an empowering technique for probing the resonance‐dependent switching dynamics upon hot carrier formation. Differential optical transmission measurements reveal an enhanced switching performance near the anti‐crossing point arising from strong coupling between local and nonlocal resonance modes. Furthermore, entangled with hot‐carrier dynamics, the nonlinear correspondence between optical resonances and refractive index change results in tailorable dispersion of recovery speeds which can notably deviate from the characteristic lifetime of hot carriers. The comprehensive understanding provides new protocols for optically characterizing hot‐carrier dynamics and optimizing resonance‐based all‐optical switches for operations across the visible spectrum.

Atomically thin transition metal dichalcogenides (TMDs) in their excited states can serve as exceptionally small building blocks for active optical platforms. In this scheme, optical excitation provides a practical approach to control light‐TMD interactions via the photocarrier generation, in an ultrafast manner. Here, it is demonstrated that via a controlled generation of photocarriers the second‐harmonic generation (SHG) from a monolayer MoS₂crystal can be substantially modulated up to ≈55% within a timeframe of ≈250 fs, a set of performance characteristics that showcases the promise of low‐dimensional materials for all‐optical nonlinear data processing. The combined experimental and theoretical study suggests that the large SHG modulation stems from the correlation between the second‐order dielectric susceptibility χ⁽²⁾and the density of photoexcited carriers in MoS₂. Indeed, the depopulation of the conduction band electrons, at the vicinity of the high‐symmetryK/K′points of MoS₂, suppresses the contribution of interband electronic transitions in the effective χ⁽²⁾of the monolayer crystal, enabling the all‐optical modulation of the SHG signal. The strong dependence of the second‐order optical response on the density of photocarriers reveals the promise of time‐resolved nonlinear characterization as an alternative route to monitoring carrier dynamics in excited states of TMDs.

The optical Kerr nonlinearity of plasmonic metals provides enticing prospects for developing reconfigurable and ultracompact all‐optical modulators. In nanostructured metals, the coherent coupling of light energy to plasmon resonances creates a nonequilibrium electron distribution at an elevated electron temperature that gives rise to significant Kerr optical nonlinearities. Although enhanced nonlinear responses of metals facilitate the realization of efficient modulation devices, the intrinsically slow relaxation dynamics of the photoexcited carriers, primarily governed by electron–phonon interactions, impedes ultrafast all‐optical modulation. Here, femtosecond (≈190 fs) all‐optical modulation in plasmonic systems via the activation of relaxation pathways for hot electrons at the interface of metals and electron acceptor materials, following an on‐resonance excitation of subradiant lattice plasmon modes, is demonstrated. Both the relaxation kinetics and the optical nonlinearity can be actively tuned by leveraging the spectral response of the plasmonic design in the linear regime. The findings offer an opportunity to exploit hot‐electron‐induced nonlinearities for design of self‐contained, ultrafast, and low‐power all‐optical modulators based on plasmonic platforms.