Structural Color 3D Printing By Shrinking Photonic Crystals

The rings, spots and stripes found on some butterflies, Pachyrhynchus weevils, and many chameleons are notable examples of natural organisms employing photonic crystals to produce colorful patterns. Despite advances in nanotechnology, we still lack the ability to print arbitrary colors and shapes in all three dimensions at this microscopic length scale. Commercial nanoscale 3D printers based on two-photon polymerization are incapable of patterning photonic crystal structures with the requisite ~300 nm lattice constant to achieve photonic stopbands/ bandgaps in the visible spectrum and generate colors. Here, we introduce a means to produce 3D-printed photonic crystals with a 5x reduction in lattice constants (periodicity as small as 280 nm), achieving sub-100-nm features with a full range of colors. The reliability of this process enables us to engineer the bandstructures of woodpile photonic crystals that match experiments, showing that observed colors can be attributed to either slow light modes or stopbands. With these lattice structures as 3D color volumetric elements (voxels), we printed 3D microscopic scale objects, including the first multi-color microscopic model of the Eiffel Tower measuring only 39-microns tall with a color pixel size of 1.45 microns. The technology to print 3D structures in color at the microscopic scale promises the direct patterning and integration of spectrally selective devices, such as photonic crystal-based color filters, onto free-form optical elements and curved surfaces

Silicon Nanoantenna Mix Arrays for a Trifecta of Quantum Emitter Enhancements

Dielectric nanostructures have demonstrated optical antenna effects due to Mie resonances. Preliminary investigations on dielectric nanoantennas have been carried out for a trifecta of enhancements, i.e., simultaneous enhancements in absorption, emission directionality and radiative decay rates of quantum emitters. However, these investigations are limited by fragile substrates or low Purcell factor, which is extremely important for exciting quantum emitters electrically. In this paper, we present a Si mix antenna array to achieve the trifecta enhancement of ~1200 fold with a Purcell factor of ~47. The antenna design incorporates ~10 nm gaps within which fluorescent molecules strongly absorb the pump laser energy through a resonant mode. In the emission process, the antenna array increases the radiative decay rates of the fluorescence molecules via Purcell effect and provides directional emission through a separate mode. This work could lead to novel CMOS compatible platforms for enhancing fluorescence for biological and chemical applications.Comment: 20 pages, 4 figure

Nuclear Magnetic Resonance Observation of α‑Synuclein Membrane Interaction by Monitoring the Acetylation Reactivity of Its Lysine Side Chains

The interaction between α-synuclein (αS) protein and lipid membranes is key to its role in synaptic vesicle homeostasis and plays a role in initiating fibril formation, which is implicated in Parkinson’s disease. The natural state of αS inside the cell is generally believed to be intrinsically disordered, but chemical cross-linking experiments provided evidence of a tetrameric arrangement, which was reported to be rich in α-helical secondary structure based on circular dichroism (CD). Cross-linking relies on chemical modification of the protein’s Lys C^ε amino groups, commonly by glutaraldehyde, or by disuccinimidyl glutarate (DSG), with the latter agent preferred for cellular assays. We used ultra-high-resolution homonuclear decoupled nuclear magnetic resonance experiments to probe the reactivity of the 15 αS Lys residues toward <i>N</i>-succinimidyl acetate, effectively half the DSG cross-linker, which results in acetylation of Lys. The intensities of both side chain and backbone amide signals of acetylated Lys residues provide direct information about the reactivity, showing a difference of a factor of 2.5 between the most reactive (K6) and the least reactive (K102) residue. The presence of phospholipid vesicles decreases reactivity of most Lys residues by up to an order of magnitude at high lipid:protein stoichiometries (500:1), but only weakly at low ratios. The decrease in Lys reactivity is found to be impacted by lipid composition, even for vesicles that yield similar αS CD signatures. Our data provide new insight into the αS–bilayer interaction, including the pivotal state in which the available lipid surface is limited. Protection of Lys C^ε amino groups by αS–bilayer interaction will strongly impact quantitative interpretation of DSG cross-linking experiments

Monomeric Aβ^1–40 and Aβ^1–42 Peptides in Solution Adopt Very Similar Ramachandran Map Distributions That Closely Resemble Random Coil

The pathogenesis of Alzheimer’s disease is characterized by the aggregation and fibrillation of amyloid peptides Aβ^1–40 and Aβ^1–42 into amyloid plaques. Despite strong potential therapeutic interest, the structural pathways associated with the conversion of monomeric Aβ peptides into oligomeric species remain largely unknown. In particular, the higher aggregation propensity and associated toxicity of Aβ^1–42 compared to that of Aβ^1–40 are poorly understood. To explore in detail the structural propensity of the monomeric Aβ^1–40 and Aβ^1–42 peptides in solution, we recorded a large set of nuclear magnetic resonance (NMR) parameters, including chemical shifts, nuclear Overhauser effects (NOEs), and <i>J</i> couplings. Systematic comparisons show that at neutral pH the Aβ^1–40 and Aβ^1–42 peptides populate almost indistinguishable coil-like conformations. Nuclear Overhauser effect spectra collected at very high resolution remove assignment ambiguities and show no long-range NOE contacts. Six sets of backbone <i>J</i> couplings (³<i>J</i>_HNHα, ³<i>J</i>_C′C′, ³<i>J</i>_C′Hα, ¹<i>J</i>_HαCα, ²<i>J</i>_NCα, and ¹<i>J</i>_NCα) recorded for Aβ^1–40 were used as input for the recently developed MERA Ramachandran map analysis, yielding residue-specific backbone ϕ/ψ torsion angle distributions that closely resemble random coil distributions, the absence of a significantly elevated propensity for β-conformations in the C-terminal region of the peptide, and a small but distinct propensity for α_L at K28. Our results suggest that the self-association of Aβ peptides into toxic oligomers is not driven by elevated propensities of the monomeric species to adopt β-strand-like conformations. Instead, the accelerated disappearance of Aβ NMR signals in D₂O over H₂O, particularly pronounced for Aβ^1–42, suggests that intermolecular interactions between the hydrophobic regions of the peptide dominate the aggregation process

Low-Threshold near-Infrared GaAs–AlGaAs Core–Shell Nanowire Plasmon Laser

We demonstrate plasmonic lasing from metal–organic chemical vapor deposition (MOCVD)-grown GaAs–AlGaAs core–shell nanowires (NWs) with subdiffraction limit diameters of ∼150 nm placed directly on a silver thin film. The absence of a low-index dielectric spacer layer between the NW and the metal layer allows for surface plasmon polariton (SPP) lasing using a nonhybridized plasmonic mode. Unlike previously reported plasmonic NW lasers using the fundamental SPP mode, we demonstrate for the first time plasmonic NW lasing under pulsed optical excitation by using the higher order SPP mode. The higher order mode allows us to alleviate the high losses associated with the fundamental plasmonic mode. We observed lasing at temperatures up to 125 K. Our demonstration of a plasmonic laser based on GaAs emitting in the near-infrared region will be useful for the on-chip integration of nanophotonic and electronic devices and the development of GaAs-based plasmonic devices

Printing Beyond sRGB Color Gamut by Mimicking Silicon Nanostructures in Free-Space

Localized optical resonances in metallic nanostructures have been increasingly used in color printing, demonstrating unprecedented resolution but limited in color gamut. Here, we introduce a new nanostructure design, which broadens the gamut while retaining print resolution. Instead of metals, silicon nanostructures that exhibit localized magnetic and electric dipole resonances were fabricated on a silicon substrate coated with a Si₃N₄ index matching layer. Index matching allows a suppression of substrate effects, thus enabling Kerker’s conditions to be met, that is, sharpened transitions in the reflectance spectra leading to saturated colors. This nanostructure design achieves a color gamut superior to sRGB, and is compatible with CMOS processes. The presented design could enable compact high-resolution color displays and filters, and the use of a Si₃N₄ antireflection coating can be readily extended to designs with nanostructures fabricated using other high-index materials

Miniaturizing Color-Sensitive Photodetectors via Hybrid Nanoantennas towards Sub-micron Dimensions

Digital camera sensors utilize color filters on photodiodes to achieve color selectivity. As color filters and photosensitive silicon layers are separate elements, these sensors suffer from optical cross-talk, which sets limits to the minimum pixel size. In this paper, we report hybrid silicon-aluminum nanostructures in the extreme limit of zero distance between color filters and sensors. This design could essentially achieve sub micron pixel dimensions and minimize the optical cross-talk originated from tilt illuminations. The designed hybrid silicon-aluminum nanostructure has dual functionalities. Crucially, it supports a hybrid Mie-plasmon resonance of magnetic dipole to achieve the color-selective light absorption, generating electron hole pairs. Simultaneously, the silicon-aluminum interface forms a Schottky barrier for charge separation and photodetection. This design could potentially replace the traditional dye based filters for camera sensors at ultra-high pixel densities with advanced functionalities in sensing polarization and directionality, as well as UV selectivity via interband plasmons of silicon.Comment: 32 pages, 4 Figures (main text), 7 Figures (supplementary