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Chirality is a geometric property describing the lack of mirror symmetry. This unique feature enables photonic spin-selectivity in light–matter interaction, which is of great significance in stereochemistry, drug development, quantum optics, and optical polarization control. The versatile control of optical geometry renders optical metamaterials as an effective platform for engineered chiral properties at prescribed spectral regimes. Unfortunately, geometry-imposed restrictions only allow one circular polarization state of photons to effectively interact with chiral meta-structures. This limitation motivates the idea of discovering alternative techniques for dynamically reconfiguring the chiroptical responses of metamaterials in a fast and facile manner. Here, we demonstrate an approach that enables optical, sub-picosecond conversion of achiral meta-structures to transient chiral media in the visible regime with desired handedness upon the inhomogeneous generation of plasmonic hot electrons. As a proof of concept, we utilize linearly polarized laser pulse to demonstrate near-complete conversion of spin sensitivity in an achiral meta-platform—a functionality yet achieved in a non-mechanical fashion. Owing to the generation, diffusion, and relaxation dynamics of hot electrons, the demonstrated technique for all-optical creation of chirality is inherently fast, opening new avenues for ultrafast spectro-temporal construction of chiral platforms with on-demand spin-selectivity. 

Understanding the ultrafast excitation and transport dynamics of plasmon-driven hot carriers is critical to the development of optoelectronics, photochemistry, and solar-energy harvesting. However, the ultrashort time and length scales associated with the behavior of these highly out-of-equilibrium carriers have impaired experimental verification of ab initio quantum theories. Here, we present an approach to studying plasmonic hot-carrier dynamics that analyzes the temporal waveform of coherent terahertz bursts radiated by photo-ejected hot carriers from designer nano-antennas with a broken symmetry. For ballistic carriers ejected from gold antennas, we find an ~11-femtosecond timescale composed of the plasmon lifetime and ballistic transport time. Polarization- and phase-sensitive detection of terahertz fields further grant direct access to their ballistic transport trajectory. Our approach opens explorations of ultrafast carrier dynamics in optically excited nanostructures. 

Abstract 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. 

Abstract 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.