We report broadband circular polarizers achieved by engineering the electromagnetic coupling between 3D meta-atoms in large-area arrays. The 3D meta-atoms are composed of bulk Au/Au nanocrystal (NC) bilayer helical arms, tailored in their number, length, and curvature through a one-step patterning process and postfabrication chemical and thermal treatments. By tuning the meta-atom array periodicity, hybridization originating from dipole− dipole and quadrupole−quadrupole interactions broadens the chiral response. We demonstrate circular polarizers operating at wavelengths spanning 2.5 to 5 μm, with a maximal transmission difference between left-and right-hand circularly polarized light of 43%.
Self-doping in nanocrystals allows accessing higher quantum states. The electrons occupying the lowest energy state of the conduction band form a metastable state that is very sensitive to the electrostatic potential of the surface. Here, we demonstrate that the high charge sensitivity of the self-doped HgSe colloidal quantum dot solid can be used for sensing three different targets with different phases through self-doped HgSe nanocrystal/ZnO thin-film transistors: the environmental gases (CO2 gas, NO gas, and H2S gas); mid-IR photon; and biothiol (l-cysteine) molecules. The self-doped quantum dot solid detects the targets through different mechanisms. The physisorption of the CO2 gas and the NO gas molecules, and the mid-IR photodetection show reversible processes, whereas the chemisorption of l-cysteine biothiol and H2S gas molecules shows irreversible processes. Considering the quenching of mid-IR intraband photoluminescence of the HgSe colloidal quantum dot solid by the vibrational mode of the CO2 gas molecule, sensing the CO2 gas could be involved in the electronic-to-vibrational energy transfer. The target molecules are quantitatively analyzed, and the limits of detection for CO2 and l-cysteine are 250 ppm and 10 nM, respectively, which are comparable to the performance of commercial detectors.
The process of dynamic self-organization of small building blocks is fundamental to the emergent function of living systems and is characteristic of their out-of-equilibrium homeostasis. The ability to control the interactions of synthetic particles in large groups could lead to the realization of analogous macroscopic robotic systems with microscopic complexity. Rotationally induced self-organization has been observed in biological systems and modeled theoretically, but studies of fast, autonomously moving synthetic rotors remain rare. Here, we report switchable, out-of-equilibrium hydrodynamic assembly and phase separation in suspensions of acoustically powered chiral microspinners. Semiquantitative modeling suggests that three-dimensionally (3D) complex spinners interact through viscous and weakly inertial (streaming) flows. The interactions between spinners were studied over a range of densities to construct a phase diagram, which included gaseous dimer pairing at low density, collective rotation and multiphase separation at intermediate densities, and ultimately jamming at high density. The 3D chirality of the spinners leads to self-organization in parallel planes, forming a three-dimensionally hierarchical system that goes beyond the 2D systems that have so far been modeled computationally. Dense mixtures of spinners and passive tracer particles also show active−passive phase separation. These observations are consistent with recent theoretical predictions of the hydrodynamic coupling between rotlets generated by autonomous spinners and provide an exciting experimental window to the study of colloidal active matter and microrobotic systems.
Colloidal noble metal nanoparticles (NPs) are composed of metal cores and organic or inorganic ligand shells. These NPs support size‐ and shape‐dependent plasmonic resonances. They can be assembled from dispersions into artificial metamolecules which have collective plasmonic resonances originating from coupled bright and dark optical electric and magnetic modes that form depending on the size and shape of the constituent NPs and their number, arrangement, and interparticle distance. NPs can also be assembled into extended 2D and 3D metamaterials that are glassy thin films or ordered thin films or crystals, also known as superlattices and supercrystals. The metamaterials have tunable optical properties that depend on the size, shape, and composition of the NPs, and on the number of NP layers and their interparticle distance. Interestingly, strong light‐matter interactions in superlattices form plasmon polaritons. Tunable interparticle distances allow designer materials with dielectric functions tailorable from that characteristic of an insulator to that of a metal, and serve as strong optical absorbers or scatterers, respectively. In combination with lithography techniques, these extended assemblies can be patterned to create subwavelength NP superstructures and form large‐area 2D and 3D metamaterials that manipulate the amplitude, phase, and polarization of transmitted or reflected light.
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