resonances. [5,6] A collective excitation (SLR) possesses a reduced linewidth as compared to the excitation of the LSPRs in nanoparticle ensembles. [1][2][3][4] Thus, SLRs can provide high quality-factor metasurfaces with substantial impact in nanophotonic and sensing applications. [1][2][3][4] Oblique incidence on planar metasurfaces constructed of an array of split-ring resonators showed that SLRs can also selectively respond to the handedness of circularly polarized light, causing sharp lattice-mode assisted extrinsic circular dichroism. [7,8] The spectral position of these SLRs can be tuned by the angle of incidence, leading to the emergence of extrinsic chiral surface lattice resonances. [9][10][11][12] Strong optical activity can also result from plasmonic 3D nanostructures without mirror symmetry. However, SLRs from arrays of 3D building-blocks with intrinsic chirality remain unexplored, but promise decreased losses and enhanced optical activity. [1,13] The fabrication of chiral 3D nanostructures is challenging for both, bottom-up and top-down methods. [14][15][16] Recently, the excitation of SLRs was seen in self-assembled, large area colloidal systems. [17,18] Such systems offer the possibility for fast manufacturing and covering large-areas on different substrate materials. [19] Colloid-based materials allow for embedding of nanoparticle arrays into flexible free-standing polymer films, [20] enabling the design of mechanically tunable [21] and stimuliresponsive hydrogel membranes. [22] Here, we use colloidal lithography [23][24][25] to fabricate arrays of 3D crescents with a selective response to the handedness of incident circularly polarized light, and we experimentally demonstrate handedness-dependent (chiral) SLRs at normal incidence. Colloidal lithography [23][24][25] is an experimentally simple and fast process to fabricate 3D chiral plasmonic nanostructures. [26][27][28] However, a necessary condition to observe SLRs in such nanostructure arrays is that their lattice constant must be in the range of the wavelength of the LSPRs of the individual nanostructures. [1][2][3][4] For objects with resonances in the near-infrared, such as, for example, split ring resonators, this requires large interparticle distances approaching the micrometer range. For conventional colloidal lithography processes, which depend on the controlled shrinkage of a polymer particle matrix, such distances are not easily achievable. [12,[28][29][30] Therefore, we use core-shell particles with rigid cores (silica) and soft, deformable polymer shells. [31,32] The particles selfassemble into hexagonally ordered monolayers at the air/water Collective excitation of periodic arrays of metallic nanoparticles by coupling localized surface plasmon resonances to grazing diffraction orders leads to surface lattice resonances with narrow line width. These resonances may find numerous applications in optical sensing and information processing. Here, a new degree of freedom of surface lattice resonances is experimentally investigated by dem...

Particle interactions, from pronounced dipolar plasmon coupling to noncoupling in colloidal monolayers with interparticle distances of hundreds of nanometers, are demonstrated. Macroscopically sized, hexagonal monolayers with exceptionally high degrees of order are fabricated in one step. Time controls the interparticle spacing and no further processing is required.

Periodic arrays of plasmonic nanostructures can support surface lattice resonances emerging from coupling between localized and diffractive modes. This allows the confinement of light at the nanometer scale with significantly increased resonance lifetimes as compared to those of purely localized modes. Here, we demonstrate that self‐assembly of plasmonic hybrid nanoparticles allows the simple and fast fabrication of periodic plasmonic monolayers featuring macroscopic dimensions and easily controllable lattice spacings. Electromagnetic coupling between diffractive and localized modes is significantly enhanced when the arrays are embedded in a homogeneous refractive index environment. This is realized through spin‐coating of a polymer film on top of the colloidal monolayer. Narrow surface lattice resonances are detected by far‐field extinction spectroscopy while optical microscopy reveals a homogeneous coupling strength on cm‐sized substrates. The surface lattice resonance position is changed by manipulation of the refractive index of the polymer film through the immersion into different organic solvents. Capitalizing on the thermoresponsive behavior of the polymer film we modulate the surface lattice resonance by temperature in a fully reversible, dynamic manner. The findings demonstrate the potential of colloidal self‐assembly as a bottom‐up approach for the fabrication of future nanophotonic devices.

Heterogeneous catalysis with supported nanoparticles (NPs) is a highly active field of research. However, the efficient stabilization of NPs without deteriorating their catalytic activity is challenging. By combining top-down (coaxial electrospinning) and bottom-up (crystallization-driven self-assembly) approaches, we prepared patchy nonwovens with functional, nanometer-sized patches on the surface. These patches can selectively bind and efficiently stabilize gold nanoparticles (AuNPs). The use of these AuNP-loaded patchy nonwovens in the alcoholysis of dimethylphenylsilane led to full conversion under comparably mild conditions and in short reaction times. The absence of gold leaching or a slowing down of the reaction even after ten subsequent cycles manifests the excellent reusability of this catalyst system. The flexibility of the presented approach allows for easy transfer to other nonwoven supports and catalytically active NPs, which promises broad applicability.