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Abstract We demonstrate shear‐printed layered photonic films with vivid structural coloration from bio‐derived cellulose nanocrystals and highly aligned Ti3C2TxMXene nanoflakes. These ultrathin films (700–1500 nm) show high light transmittance above 40% in the visible range. In reflectance mode, however, the films appear vividly colored and iridescent due to the multiple distinct photonic bandgaps in the visible and near‐infrared ranges, which are rarely observed in CNC composites. The structural coloration is controlled by the stacking of MXene nanoscale‐thin layers separated by the thicker cellulose nanocrystals matrix, as confirmed by photonic simulations. The unique combination of distinctly different optical appearances in transmittance and reflectance modes occurs in films printed with just a few layers. This is because of the molecularly smooth interfaces and the high refractive contrast between bio‐based and inorganic phases, which result in a concurrence of constructive and destructive interference. These lamellar biophotonic films open the possibilities for advanced radiative cooling, camouflaging, multifunctional capacitors, and optical filtration applications, while the cellulose nanocrystals matrix strengthens their flexibility, robustness, and facilitates sustainability.more » « less
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Abstract Natural polymers, particularly plant‐derived nanocelluloses, self‐organize into hierarchical structures, enabling mechanical robustness, bright iridescence, emission, and polarized light reflection. These biophotonic properties are facilitated by the assembly of individual components during evaporation, such as cellulose nanocrystals (CNCs), which exhibit a left‐handed helical pitch in a chiral nematic state. This work demonstrates how optically active films with pre‐programmed opposite handedness (left or right) can be constructed via shear‐induced twisted printing with clockwise and counter‐clockwise shearing vectors. The resulting large‐area thin films are transparent yet exhibit pre‐determined mirror‐symmetrical optical activity, enabling the distinction of absorbed and emitted circularly polarized light. This processing method allows for sequential printing of thin and ultrathin films with twisted layered organization and on‐demand helicity. The complex light polarization behavior is due to step‐like changes in linear birefringence within each deposited layer and circular birefringence, different from that of conventional CNC films as revealed with Muller matrix analysis. Furthermore, intercalating an achiral organic dye into printed structures induces circularly polarized luminescence while preserving high transmittance and controlled handedness. These results suggest that twisted sequential printing can facilitate the construction of chiroptical metamaterials with tunable circular polarization, absorption, and emission for optical filters, encryption, photonic coatings, and chiral sensors.more » « less
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Abstract Ultra-thin films of low damping ferromagnetic insulators with perpendicular magnetic anisotropy have been identified as critical to advancing spin-based electronics by significantly reducing the threshold for current-induced magnetization switching while enabling new types of hybrid structures or devices. Here, we have developed a new class of ultra-thin spinel structure Li0.5Al1.0Fe1.5O4(LAFO) films on MgGa2O4(MGO) substrates with: 1) perpendicular magnetic anisotropy; 2) low magnetic damping and 3) the absence of degraded or magnetic dead layers. These films have been integrated with epitaxial Pt spin source layers to demonstrate record low magnetization switching currents and high spin-orbit torque efficiencies. These LAFO films on MGO thus combine all of the desirable properties of ferromagnetic insulators with perpendicular magnetic anisotropy, opening new possibilities for spin based electronics.more » « less
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Perovskite chalcogenides are gaining substantial interest as an emerging class of semiconductors for optoelectronic applications. High-quality samples are of vital importance to examine their inherent physical properties. We report the successful crystal growth of the model system, BaZrS 3 and its Ruddlesden–Popper phase Ba 3 Zr 2 S 7 by a flux method. X-ray diffraction analyses showed the space group of Pnma with lattice constants of a = 7.056(3) Å, b = 9.962(4) Å, and c = 6.996(3) Å for BaZrS 3 and P 4 2 / mnm with a = 7.071(2) Å, b = 7.071(2) Å, and c = 25.418(5) Å for Ba 3 Zr 2 S 7 . Rocking curves with full width at half maximum of 0.011° for BaZrS 3 and 0.027° for Ba 3 Zr 2 S 7 were observed. Pole figure analysis, scanning transmission electron microscopy images, and electron diffraction patterns also establish the high quality of the grown crystals. The octahedral tilting in the corner-sharing octahedral network is analyzed by extracting the torsion angles.more » « less
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