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Tunable Pseudocapacitance in 3D TiO2−δ Nanomembranes Enabling Superior Lithium Storage Performance

Nanostructured TiO2 of different polymorphs, mostly prepared by hydro/solvothermal methods, have been extensively studied for more than a decade as anode materials in lithium ion batteries. Enormous efforts have been devoted to improving the electrical conductivity and lithium ion diffusivity in chemically synthesized TiO2 nanostructures. In this work we demonstrate that 3D Ti3+-self-doped TiO2 (TiO2-δ) nanomembranes, which are prepared by physical vapor deposition combined with strain-released rolled-up technology, have a great potential to address several of the long-standing challenges associated with TiO2 anodes. The intrinsic electrical conductivity of the TiO2 layer can be significantly improved by the in situ generated Ti3+, and the amorphous, thin TiO2 nanomembrane provides a shortened Li+ diffusion pathway. The fabricated material shows a favorable electrochemical reaction mechanism for lithium storage. Further, post-treatments are employed to adjust the Ti3+ concentration and crystallinity degree in TiO2 nanomembranes, providing an opportunity to investigate the important influences of Ti3+ self-doping and amorphous structures on the electrochemical processes. With these experiments, the pseudocapacitance contributions in TiO2 nanomembranes with different crystallinity degree are quantified and verified by an in-depth kinetics analysis. Additionally, an ultrathin metallic Ti layer can be included, which further improves the lithium storage properties of the TiO2, giving rise to the state-of-the-art capacity (200 mAh g-1 at 1 C), excellent rate capability (up to 50 C), and ultralong lifetime (for 5000 cycles at 10 C, with an extraordinary retention of 100%) of TiO2 anodes.

Silver nanovoid arrays for surface-enhanced Raman scattering.

Highly ordered silver nanovoid arrays are fabricated on porous anodic alumina membranes to produce robust and cost-efficient surface-enhanced Raman scattering (SERS) substrates. Plasmonic tunability can be accomplished by adjusting the topography with different anode voltages. Evenly distributed plasmonic fields, high average enhancement factor, and excellent ambient stability due to the natural protective layer are some of the unique advantages, and the silver nanovoid arrays are applicable to sensing devices.

Facile design of ultra-thin anodic aluminum oxide membranes for the fabrication of plasmonic nanoarrays

Ultra-thin anodic aluminum oxide (AAO) membranes are efficient templates for the fabrication of patterned nanostructures. Herein, a three-step etching method to control the morphology of AAO is described. The morphological evolution of the AAO during phosphoric acid etching is systematically investigated and a nonlinear growth mechanism during unsteady-state anodization is revealed. The thickness of the AAO can be quantitatively controlled from ∼100 nm to several micrometers while maintaining the tunablity of the pore diameter. The AAO membranes are robust and readily transferable to different types of substrates to prepare patterned plasmonic nanoarrays such as nanoislands, nanoclusters, ultra-small nanodots, and core-satellite superstructures. The localized surface plasmon resonance from these nanostructures can be easily tuned by adjusting the morphology of the AAO template. The custom AAO template provides a platform for the fabrication of low-cost and large-scale functional nanoarrays suitable for fundamental studies as well as applications including biochemical sensing, imaging, photocatalysis, and photovoltaics.

VO2/TiN Plasmonic Thermochromic Smart Coatings for Room‐Temperature Applications

Vanadium dioxide/titanium nitride (VO2 /TiN) smart coatings are prepared by hybridizing thermochromic VO2 with plasmonic TiN nanoparticles. The VO2 /TiN coatings can control infrared (IR) radiation dynamically in accordance with the ambient temperature and illumination intensity. It blocks IR light under strong illumination at 28 °C but is IR transparent under weak irradiation conditions or at a low temperature of 20 °C. The VO2 /TiN coatings exhibit a good integral visible transmittance of up to 51% and excellent IR switching efficiency of 48% at 2000 nm. These unique advantages make VO2 /TiN promising as smart energy-saving windows.

Localized Surface Plasmons Selectively Coupled to Resonant Light in Tubular Microcavities.

Vertical gold nanogaps are created on microtubular cavities to explore the coupling between resonant light supported by the microcavities and surface plasmons localized at the nanogaps. Selective coupling of optical axial modes and localized surface plasmons critically depends on the exact location of the gold nanogap on the microcavities, which is conveniently achieved by rolling up specially designed thin dielectric films into three-dimensional microtube cavities. The coupling phenomenon is explained by a modified quasipotential model based on perturbation theory. Our work reveals the coupling of surface plasmon resonances localized at the nanoscale to optical resonances confined in microtubular cavities at the microscale, implying a promising strategy for the investigation of light-matter interactions.

Spin–orbit coupling of light in asymmetric microcavities

When spinning particles, such as electrons and photons, undergo spin–orbit coupling, they can acquire an extra phase in addition to the well-known dynamical phase. This extra phase is called the geometric phase (also known as the Berry phase), which plays an important role in a startling variety of physical contexts such as in photonics, condensed matter, high-energy and space physics. The geometric phase was originally discussed for a cyclically evolving physical system with an Abelian evolution, and was later generalized to non-cyclic and non-Abelian cases, which are the most interesting fundamental subjects in this area and indicate promising applications in various fields. Here, we enable optical spin–orbit coupling in asymmetric microcavities and experimentally observe a non-cyclic optical geometric phase acquired in a non-Abelian evolution. Our work is relevant to fundamental studies and implies promising applications by manipulating photons in on-chip quantum devices.

Controlled Patterning of Plasmonic Dimers by Using an Ultrathin Nanoporous Alumina Membrane as a Shadow Mask

We report on design and fabrication of patterned plasmonic dimer arrays by using an ultrathin anodic aluminum oxide (AAO) membrane as a shadow mask. This strategy allows for controllable fabrication of plasmonic dimers where the location, size, and orientation of each particle in the dimer pairs can be independently tuned. Particularly, plasmonic dimers with ultrasmall nanogaps down to the sub-10 nm scale as well as a large dimer density up to 1.0 × 1010 cm-2 are fabricated over a centimeter-sized area. The plasmonic dimers exhibit significant surface-enhanced Raman scattering (SERS) enhancement with a polarization-dependent behavior, which is well interpreted by finite-difference time-domain (FDTD) simulations. Our results reveal a facile approach for controllable fabrication of large-area dimer arrays, which is of fundamental interest for plasmon-based applications in surface-enhanced spectroscopy, biochemical sensing, and optoelectronics.

Hybridization of photon-plasmon modes in metal-coated microtubular cavities

The coupling of resonant light and surface plasmons in metal layer coated optical microcavities results in the formation of hybrid photon-plasmon modes. Here, we comprehensively investigate the hybridization mechanism of photon-plasmon modes based on opto-plasmonic microtubular cavities. By changing the cavity structure and the metal layer thickness, weakly, moderately and strongly hybridized resonant modes are demonstrated depending on the photon-plasmon coupling strength. An effective potential approach is applied to illustrate the hybridization of photon-plasmon modes relying on the competition between light confinement by the cavity wall and the potential barrier introduced by the metal layer. Our work reveals the basic physical mechanisms for the generation of hybrid modes in metal-coated whispering-gallery-mode microcavities, and is of importance for the study of enhanced light-matter interactions and potential sensing applications.

Tunable fluorescence from patterned silver nano-island arrays for sensitive sub-cell imaging

Surface-enhanced fluorescence, a burgeoning technique in biological detection, provides largely enhanced fluorescence signal by exciting localized surfaces plasmons resonance with fluorescent dyes. Nanostructure and surroundings brings great impact on the emission signal, however, insufficient physics about the process limits further improvement on the nanostructure design. In this study, optical properties of Rhodamin-6G molecules on patterned silver nano-island arrays are tailored by precisely controlling the distance between the dyes and silver arrays. The fluorescence signal depends on the distance and the largest enhancement of 10 folds is achieved when the distance is 10 nm. The results are theoretically corroborated by finite difference time domain simulation and applied to cytoskeleton fluorescence imaging using phalloidin–fluorescein isothiocyanate. Our study provides insights into the physical mechanisms associated with the fluorescence enhancement and quenching, and our experiments suggest potential applications to high-sensitivity sub-cell imaging.

In Situ Generation of Plasmonic Nanoparticles for Manipulating Photon–Plasmon Coupling in Microtube Cavities

In situ generation of silver nanoparticles for selective coupling between localized plasmonic resonances and whispering-gallery modes (WGMs) is investigated by spatially resolved laser dewetting on microtube cavities. The size and morphology of the silver nanoparticles are changed by adjusting the laser power and irradiation time, which in turn effectively tune the photon-plasmon coupling strength. Depending on the relative position of the plasmonic nanoparticles spot and resonant field distribution of WGMs, selective coupling between the localized surface plasmon resonances (LSPRs) and WGMs is experimentally demonstrated. Moreover, by creating multiple plasmonic-nanoparticle spots on the microtube cavity, the field distribution of optical axial modes is freely tuned due to multicoupling between LSPRs and WGMs. The multicoupling mechanism is theoretically investigated by a modified quasipotential model based on perturbation theory. This work provides an in situ fabrication of plasmonic nanoparticles on three-dimensional microtube cavities for manipulating photon-plasmon coupling which is of interest for optical tuning abilities and enhanced light-matter interactions.