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Enantiomers are chiral isomers in which the isomer's structure itself and its mirror image cannot be superimposed on each other. Enantiomer selective sensing is critical as enantiomers exhibit distinct functionalities to their mirror image. Discriminating between enantiomers by optical methods has been widely used as these techniques provide nondestructive characterization, however, they are constrained by the intrinsically small chirality of the molecules. Here, a method to effectively discriminate chiral analytes in the nonlinear regime is demonstrated, which is facilitated by an upconverting chiral plasmonic metamaterial. The different handedness of the chiral molecules interacts with the chiral metamaterial platform, which leads to a change in the circular dichroism of the chiral metamaterial in the near‐infrared region. The contrast of the circular dichroism is identified by the upconverted signal in the visible region.

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.