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Great Chiral Fluorescence from Optical Duality Silver Nanostructures Enabled by 3D Laser Printing

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 Added by Shichao Song
 Publication date 2020
  fields Physics
and research's language is English




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Featured by prominent flexibility and fidelity in producing sophisticated stereoscopic structures transdimensionally, three-dimensional (3D) laser printing technique has vastly extended the toolkit for delivering diverse functional devices. Yet chiral nanoemitters heavily resorting to artificial structures that manifest efficient emission and tightly confined light-mater interactions simultaneously remains alluring but dauntingly challenging for this technique at this moment. In this work, we assert the chiral photoluminescence is implemented from silver nanostructures of optical duality in one go via a twofold three-dimensional laser printing scheme. Such laser printing protocol allows the highly desired duality by simultaneously producing uniformly distributed fluorescent silver nanoclusters and aggregated plasmonic silver nanoparticles to tightly confine chiral interactions at the nanoscale. A helical emitter of 550 nm-helix-diameter as fabricated has seen a record-high luminescence anisotropic factor with the absolute value up to 0.58, which is two orders of magnitude greater than fluorescent chiral silver clusters. This method holds great promise for future versatile applications in chiroptical nanodevices.



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We present a comprehensive review of recent developments in the field of chiral plasmonics. Significant advances have been made recently in understanding the working principles of chiral plasmonic structures. With advances in micro- and nanofabrication techniques, a variety of chiral plasmonic nanostructures have been experimentally realized; these tailored chiroptical properties vastly outperform those of their molecular counterparts. We focus on chiral plasmonic nanostructures created using bottom-up approaches, which not only allow for rational design and fabrication but most intriguingly in many cases also enable dynamic manipulation and tuning of chiroptical responses. We first discuss plasmon-induced chirality, resulting from the interaction of chiral molecules with plasmonic excitations. Subsequently, we discuss intrinsically chiral colloids, which give rise to optical chirality owing to their chiral shapes. Finally, we discuss plasmonic chirality, achieved by arranging achiral plasmonic particles into handed configurations on static or active templates. Chiral plasmonic nanostructures are very promising candidates for real-life applications owing to their significantly larger optical chirality than natural molecules. In addition, chiral plasmonic nanostructures offer engineerable and dynamic chiroptical responses, which are formidable to achieve in molecular systems. We thus anticipate that the field of chiral plasmonics will attract further widespread attention in applications ranging from enantioselective analysis to chiral sensing, structural determination, and in situ ultrasensitive detection of multiple disease biomarkers, as well as optical monitoring of transmembrane transport and intracellular metabolism.
Chirality is an intriguing property of certain molecules, materials or artificial nanostructures, which allows them to interact with the spin angular momentum of the impinging light field. Due to their chiral geometry, they can distinguish between left- and right-hand circular polarization states or convert them into each other. Here, we introduce a novel approach towards optical chirality, which is observed in individual two-dimensional and geometrically mirror-symmetric nanostructures. In this scheme, the chiral optical response is induced by the chosen heterogeneous material composition of a particle assembly and the corresponding resonance behavior of the constituents it is built from, which breaks the symmetry of the system. As a proof of principle, we investigate such a structure composed of individual silicon and gold nanoparticles both experimentally as well as numerically. Our proposed concept constitutes a novel approach for designing two-dimensional chiral media tailored at the nanoscale.
A light field print (LFP) displays three-dimensional (3D) information to the naked-eye observer under ambient white light illumination. Changing perspectives of a 3D image are seen by the observer from varying angles. However, LFPs appear pixelated due to limited resolution and misalignment between their lenses and colour pixels. A promising solution to create high-resolution LFPs is through the use of advanced nanofabrication techniques. Here, we use two-photon polymerization lithography as a one-step nanoscale 3D printer to directly fabricate LFPs out of transparent resin. This approach produces simultaneously high spatial resolution (29 - 45 {mu}m) and high angular resolution (~ 1.6 {deg}) images with smooth motion parallax across 15 {times} 15 views. Notably, the smallest colour pixel consists of only a single nanopillar (~ 300 nm diameter). Our LFP signifies a step towards hyper-realistic 3D images that can be applied in print media and security tags for high-value goods.
Varying only the in-plane or out-of-plane dimensions of nanostructures produces a wide range of colourful elements in metasurfaces and thin films. However, achieving shades of grey and control of colour saturation remains challenging. Here, we introduce a hybrid approach to colour generation based on the tuning of nanostructure geometry in all three dimensions. Through two-photon polymerization lithography, we systematically investigated colour generation from the simple single nanopillar geometry made of low-refractive-index material; realizing grayscale and full colour palettes with control of hue, saturation, brightness through tuning of height, diameter, and periodicity of nanopillars. Arbitrary colourful and grayscale images were painted by mapping desired prints to precisely controllable parameters during 3D printing. We extend our understanding of the scattering properties of the low-refractive-index nanopillar to demonstrate grayscale inversion and colour desaturation, with steganography at the level of single nanopillars.
We demonstrate the first buried optical waveguides in diamond using focused femtosecond laser pulses. The properties of nitrogen vacancy centers are preserved in the waveguides, making them promising for diamond-based magnetometers or quantum information systems.
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