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The chemically synthesizable quantum emitters such as quantum dots (QDs), fluorescent nanodiamonds (FNDs), and organic fluorescent dyes can be integrated with an easy-to-craft quantum nanophotonic device, which would be readily developed by non-lithographic solution process. As a representative example, the solution dipping or casting of such soft quantum emitters on a flat metal layer and subsequent drop-casting of plasmonic nanoparticles can afford the quantum emitter-coupled plasmonic nanocavity (referred to as a nanoparticle-on-mirror (NPoM) cavity), allowing us for exploiting various quantum mechanical behaviors of light–matter interactions such as quantum electrodynamics (QED), strong coupling (e.g., Rabi splitting), and quantum mirage. This versatile, yet effective soft quantum nanophotonics would be further benefitted from a deterministic control over the positions and orientations of each individual quantum emitter, particularly at the molecule level of resolution. In this review, we will argue that DNA nanotechnology can provide a gold vista toward this end. A collective set of exotic characteristics of DNA molecules, including Watson-Crick complementarity and helical morphology, enables reliable grabbing of quantum emitters at the on-demand position and steering of their directors at the single molecular level. More critically, the recent advances in large-scale integration of DNA origami have pushed the reliance on the distinctly well-formed single device to the regime of the ultra-scale device arrays, which is critical for promoting the practically immediate applications of such soft quantum nanophotonics.

The chemically synthesizable quantum emitters such as quantum dots (QDs), fluorescent nanodiamonds (FNDs), and organic fluorescent dyes can be integrated with an easy-to-craft quantum nanophotonic device, which would be readily developed by non-lithographic solution process. As a representative example, the solution dipping or casting of such soft quantum emitters on a flat metal layer and subsequent drop-casting of plasmonic nanoparticles can afford the quantum emitter-coupled plasmonic nanocavity (referred to as a nanoparticle-on-mirror (NPoM) cavity), allowing us for exploiting various quantum mechanical behaviors of light–matter interactions such as quantum electrodynamics (QED), strong coupling (e.g., Rabi splitting), and quantum mirage. This versatile, yet effective soft quantum nanophotonics would be further benefitted from a deterministic control over the positions and orientations of each individual quantum emitter, particularly at the molecule level of resolution. In this review, we will argue that DNA nanotechnology can provide a gold vista toward this end. A collective set of exotic characteristics of DNA molecules, including Watson-Crick complementarity and helical morphology, enables reliable grabbing of quantum emitters at the on-demand position and steering of their directors at the single molecular level. More critically, the recent advances in large-scale integration of DNA origami have pushed the reliance on the distinctly well-formed single device to the regime of the ultra-scale device arrays, which is critical for promoting the practically immediate applications of such soft quantum nanophotonics. [ABSTRACT FROM AUTHOR]

All‐dielectric nanoparticles (NPs) with high (>3.0) or moderate (1.7–3.0) refractive indices have become fundamental to meta‐optics, as they enable low‐loss, low‐heating, and quenching‐free magnetodielectric Mie resonances, which are difficult to achieve by use of plasmonic counterparts. However, a scalable and versatile synthetic route for such magnetodielectric NPs retaining high uniformity, roundness, and robustness has remained elusive. Thus, soft self‐assembly still represents an underutilized method in the optical engineer's toolset, which in turn limits the accessible range of meta‐optics. Herein, a gram‐scale and versatile synthesis of dielectric colloidal Mie resonators is presented, in which selenous acid precursors are converted into highly uniform, crystalline colloids by a low demand reaction. These crystalline selenium (c‐Se) colloids enable strong electric and magnetic resonances due to their moderate refractive index (2.8–3.2 at optical frequencies), while simultaneously satisfying the requirements of high uniformity, roundness, and robustness. Even with these exotic properties, c‐Se colloids are successfully self‐assembled into various all‐dielectric meta‐optics systems including (i) metafluids exhibiting directional scattering, (ii) metamolecules with nanogap‐dielectric resonances, and (iii) metacrystals with magnetodielectric bandgaps. The design space of all‐dielectric meta‐optics will be greatly expanded by utilizing soft self‐assembly of c‐Se colloids. Highly uniform, robust, and scalable high‐index selenium colloids are successfully synthesized under mild conditions. With explicit demonstration of selenium colloids self‐assembled into various platforms including metafluids, metamolecules, and metacrystals, selenium colloids are proven to serve as general building block for "soft" meta‐optics. [ABSTRACT FROM AUTHOR]

This study demonstrates the developments of self-assembled optical metasurfaces to overcome inherent limitations in polarization density (P) and high refractive indices (n) within naturally occurring materials. The Maxwellian macroscopic description establishes a link between P and n, revealing a static limit in natural materials, restricting n to ≈4.0 at optical frequencies. Previously, it is accepted that self-assembly enables the creation of nanogaps between metallic nanoparticles (NPs), boosting capacitive enhancement of P and resultant exceptionally high n at optical frequencies. The work focuses on assembling gold (Au) NPs into a closely packed monolayer by rationally designing the polymeric ligand to balance attractive and repulsive forces, in that polymeric brush-mediated self-assembly of the close-packed Au NP monolayer is robustly achieved over a large-area. The resulting monolayer of Au nanospheres (NSs), nanooctahedras (NOs), and nanocubes (NCs) exhibits high macroscopic integrity and crystallinity, sufficiently enough for pushing n to record-high regimes. The systematic comparisons between each differently shaped Au NP monolayers elucidate the significance of capacitive coupling in achieving an unnaturally high n. The achieved n of 10.12 at optical frequencies stands as a benchmark, highlighting the potential of polyhedral Au NPs in advancing optical metasurfaces., (© 2024 The Author(s). Small published by Wiley‐VCH GmbH.)