Chiral nano-or metamaterials and surfaces enable striking photonic properties, such as negative refractive index and superchiral light, driving promising applications in novel optical components, nanorobotics, and enhanced chiral molecular interactions with light. In characterizing chirality, although nonlinear chiroptical techniques are typically much more sensitive than their linear optical counterparts, separating true chirality from anisotropy is a major challenge. Here, we report the first observation of optical activity in second-harmonic hyper-Rayleigh scattering (HRS). We demonstrate the effect in a 3D isotropic suspension of Ag nanohelices in water. The effect is 5 orders of magnitude stronger than linear optical activity and is well pronounced above the multiphoton luminescence background. Because of its sensitivity, isotropic environment, and straightforward experimental geometry, HRS optical activity constitutes a fundamental experimental breakthrough in chiral photonics for media including nanomaterials, metamaterials, and chemical molecules.

Recent advances in nonlinear optics, hot electrons for renewable energy (e.g., solar cells and water‐splitting), acousto‐optics, nanometalworking, nanorobotics, steam generation, and photothermal cancer therapy are reviewed here. In all these areas, one of the key enabling properties is the ability of metallic nanoparticles to harvest and control light at the subwavelength scale by supporting coherent electronic oscillations, called localized surface plasmon resonances (LSPRs). Various physical properties and potential areas of application emerge depending on the decay mechanism of the LSPR and, especially, depending on the considered timescale. The field of plasmonics has mainly been associated with manipulating electromagnetic near‐fields at the nanoscale, where absorption is an obstacle. However, plasmonic absorption leads to a stream of temperature‐related phenomena that have only recently attracted significant attention. The goal of this review is to highlight exciting new areas of research (such as nanorobotics, nanometalworking, or acousto‐optical techniques) and to survey the most recent progress in more established areas (such as hot electrons, photothermal therapy, and plasmonic steam generation). To set each research area in context, the text is organized around the thermal cycle of the nanoparticles.

Linear optical methods of determining the chirality of organic and inorganic materials have relied on weak chiral optical (chiroptical) effects. Nonlinear chiroptical characterization holds the potential of much greater sensitivity and smaller interaction volumes. However, suitable materials on which to perform measurements have been lacking for decades. Here, we present the first nonlinear chiroptical characterization of crystallographic chirality in gold helicoids (≈150 nm size) and core/shell helicoids with the newly discovered hyper-Rayleigh scattering optical activity (HRS OA) technique. The observed chiroptical signal is, on average, originating from between ≈0.05 and ≈0.13 helicoids, i.e., less than a single nanoparticle. The measured HRS OA ellipticities reach ≈3°, for a concentration ≈10 9 times smaller than that of chiral molecules with similar nonlinear chiroptical response. These huge values indicate that the helicoids are excellent candidates for future nonlinear chiroptical materials and applications.

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ombinatorial nanochemistry allows tens to millions of mixtures to be produced in a single process 1,2 , generating large chemical libraries [3][4][5][6][7] and making implementation of artificial intelligence algorithms possible. Following the rapid development of chiral nanostructures [8][9][10][11][12][13] , such synthetic and analytical platforms can be applied to the high-throughput assessment of enzyme mimics, contrast agents, antibiotic agents, drug delivery vehicles, as well as other applications of these bioinspired materials. These analyses should be carried out in microplates of 1,536, 3,456 or 9,600 wells, with sample volumes as small as, and smaller than, 1 µl (ref.