Nanoscale Gaps Research Articles

Miniature hemispherical shell resonator with large-scale effective electrodes based on piezoelectric drive mechanism

Miniature resonators with three-dimensional curved surface are mostly driven by electrostatic capacitive. However, it is quite difficult to fabricate a curved surface electrostatic resonator with large-scale effective electrodes. This paper presents the first miniature hemispherical shell resonator with large-scale effective electrodes based on piezoelectric drive mechanism. The vibrating body and electrodes of the piezoelectric resonator are easily integrated without micro-scale or nano-scale narrow capacitive gap. Vibration experiment and finite element analysis both reveal that there exist seven significant vibration modes between 10 kHz and 100 kHz. Mode shape validation is also carried out by measuring the vibration velocity of upper perimeter and lateral perimeter with laser doppler vibrometer. Special vibration characteristics of each vibration mode are described in detail, based on which the resonator may be used for many specific applications. Compared with common electrostatic resonators, even smaller drive voltage applied to the piezoelectric resonator may produce larger vibration displacement at atmosphere. According to the experiment results, the resonator may provide a new way of realizing high performance three-dimensional miniature devices for communication and inertial navigation applications.

Intense radiative heat transport across a nano-scale gap

In this paper, we analyze the radiative heat transport in layered structures. The analysis is based on our prior description of the spectrum of thermally excited waves in systems with a heat flux. The developed method correctly predicts results for all known special cases for both large and closing gaps. Numerical examples demonstrate the applicability of our approach to the calculation of the radiative heat transport coefficient across various layered structures.

Survey of plasmonic gaps tuned at sub-nanometer scale in self-assembled arrays

Creating nanoscale and sub-nanometer gaps between noble metal nanoparticles is critical for the applications of plasmonics and nanophotonics. To realize simultaneous attainments of both the optical spectrum and the gap size, the ability to tune these nanoscale gaps at the sub-nanometer scale is particularly desirable. Many nanofabrication methodologies, including electron beam lithography, self-assembly, and focused ion beams, have been tested for creating nanoscale gaps that can deliver significant field enhancement. Here, we survey recent progress in both the reliable creation of nanoscale gaps in nanoparticle arrays using self-assemblies and in the in-situ tuning techniques at the sub-nanometer scale. Precisely tunable gaps, as we expect, will be good candidates for future investigations of surface-enhanced Raman scattering, non-linear optics, and quantum plasmonics.

Layered reduced graphene oxide with nanoscale interlayer gaps as a stable host for lithium metal anodes.

Metallic lithium is a promising anode candidate for future high-energy-density lithium batteries. It is a light-weight material, and has the highest theoretical capacity (3,860 mAh g(-1)) and the lowest electrochemical potential of all candidates. There are, however, at least three major hurdles before lithium metal anodes can become a viable technology: uneven and dendritic lithium deposition, unstable solid electrolyte interphase and almost infinite relative dimension change during cycling. Previous research has tackled the first two issues, but the last is still mostly unsolved. Here we report a composite lithium metal anode that exhibits low dimension variation (∼20%) during cycling and good mechanical flexibility. The anode is composed of 7 wt% 'lithiophilic' layered reduced graphene oxide with nanoscale gaps that can host metallic lithium. The anode retains up to ∼3,390 mAh g(-1) of capacity, exhibits low overpotential (∼80 mV at 3 mA cm(-2)) and a flat voltage profile in a carbonate electrolyte. A full-cell battery with a LiCoO2 cathode shows good rate capability and flat voltage profiles.

Field emitters with nanoscale tips based on Mo oxide fabricated by electrochemical methods

Field emitters with nanoscale tips and a fabrication technique using a nanoscale gap are described. Each fabrication technique makes it possible to form emitters on a meter-scale glass substrate. The emitter has a configuration with one side gate to reduce the electron scattering losses at the counter electrode to improve the emission efficiency. All thin film layers constituting the emitter are fabricated by plasma-enhanced chemical vapor deposition and sputtering deposition. Nanoscale tips are formed between a shallow gap less than 7 nm deep by the joule heating of a Mo complex oxide, which is produced by the electro chemical etching of a deposited Mo layer. To our knowledge, this is the first work that shows a uniform efficiency of 5% or more achieved at an anode voltage of 10 kV and an operation voltage of 23 V.

Radiative heat conductances between dielectric and metallic parallel plates with nanoscale gaps.

Recent experiments have demonstrated that radiative heat transfer between objects separated by nanometre-scale gaps considerably exceeds the predictions of far-field radiation theories. Exploiting this near-field enhancement is of great interest for emerging technologies such as near-field thermophotovoltaics and nano-lithography because of the expected increases in efficiency, power conversion or resolution in these applications. Past measurements, however, were performed using tip-plate or sphere-plate configurations and failed to realize the orders of magnitude increases in radiative heat currents predicted from near-field radiative heat transfer theory. Here, we report 100- to 1,000-fold enhancements (at room temperature) in the radiative conductance between parallel-planar surfaces at gap sizes below 100 nm, in agreement with the predictions of near-field theories. Our measurements were performed in vacuum gaps between prototypical materials (SiO2-SiO2, Au-Au, SiO2-Au and Au-Si) using two microdevices and a custom-built nanopositioning platform, which allows precise control over a broad range of gap sizes (from <100 nm to 10 μm). Our experimental set-up will enable systematic studies of a variety of near-field-based thermal phenomena, with important implications for thermophotovoltaic applications, that have been predicted but have defied experimental verification.

Ultrashort broadband polarization beam splitter based on a combined hybrid plasmonic waveguide

We propose an ultracompact broadband polarization beam splitter (PBS) based on a combined hybrid plasmonic waveguide (HPW). The proposed PBS separates transverse-electric (TE) and transverse-magnetic (TM) modes using a bent lower HPW with vertical nanoscale gaps and a straight upper HPW with a horizontal nanoscale gap, respectively, without relying on an additional coupling region. This design considerably reduces the length of the PBS to the submicron scale (920 nm, the shortest PBS reported to date) while offering polarization extinction ratios (PERs) of ~19 dB (~18 dB) and insertion losses (ILs) of ~0.6 dB (~0.3 dB) for the TE (TM) mode over an extremely broad band of 400 nm (from λ = 1300 nm to 1700 nm, covering entirely second and third telecom windows). The length of the designed PBS can be reduced further to 620 nm while still offering PERs of 15 dB, realizing a densely photonic integrated circuit. Considering the fabrication tolerance, the designed PBS allows for large geometrical deviations of ±20 nm while restricting PER variations to within 1 dB, except for those in the nanoscale gaps smaller than 10nm. Additionally, we also address the input and ouput coupling efficiencies of the proposed PBS.

Effect of temperature on the viscoelastic properties of nano-confined liquid mixtures.

The behaviour of fluids confined in nanoscale gaps plays a central role in molecular science and nanofluidics, with applications ranging from biological function to multiscale printing, osmosis and filtration, lab-on-chip technology and friction reduction. Here atomic force microscopy is used to shear five different mixtures of hexadecane and squalane confined between the tip apex and atomically flat graphite. The shearing amplitudes are typically <2 nm, hence reflecting highly localised information at the interface. The evolution of each mixture's viscoelastic properties is studied as a function of temperature, between 20 °C and 100 °C. The results, complemented by sub-nanometre resolution images of the interface, show that spatial organisation of the liquid molecules at the surface of graphite largely dominates the measurements. Squalane presents a higher effective affinity for the surface by forming a robust self-assembled layer in all mixtures. This results in a step-like change of the viscous and elastic response of the confined liquid as the confining pressure increases. In contrast, measurements in pure hexadecane show a continuous and linear increase in the apparent viscosity with pressure at all temperatures. This is interpreted as a more fragile interfacial layer and images show that it can be completely removed at high temperatures. Depending on the mixture composition, measurements can be strongly location-dependent which suggests molecular clustering and nanoscale phase separation at the interface.

Silver nanoparticle functionalized glass fibers for combined surface-enhanced Raman scattering spectroscopy (SERS)/surface-assisted laser desorption/ionization (SALDI) mass spectrometry via plasmonic/thermal hot spots.

We presented the fabrication of a silver nanoparticle (Ag NP) functionalized glass fiber (Ag-GF) substrate for combined surface-enhanced Raman scattering spectroscopy (SERS)/surface-assisted laser desorption/ionization (SALDI) mass spectrometry. Ag NPs were immobilized onto the surface of glass fibers through a simple sputter deposition process. The SERS and SALDI activities strongly depended on the nanostructures of the deposited Ag NPs on the GFs. The closely-packed Ag NPs with a size of 20-50 nm and an inter-particle nanoscale gap of less than 10 nm were effective for the simultaneously enhanced SERS/SALDI substrate via plasmonic/thermal "hot spots", while the interconnected continuous Ag film reduced both the SERS/SALDI activities. The SERS enhanced factor (EFSERS) and SALDI enhanced factor (EFSALDI) were newly proposed. Finally, the concentration-dependent signal intensities of SERS and SALD-MS of sulfur compounds using an identical Ag NP-GF substrate were examined, and the linear dependence relationship in the log-log plot was demonstrated for the combined quantitative SERS/SALDI-MS analysis.

Mechanism of the activation process for the formation of a surface-conduction electron-emitter

The major role of the chemical reaction between a silica substrate and deposited carbon in the activation process for the formation of a surface-conduction electron emitter (SCE) is investigated. The SCE emits electrons by the tunneling effect when an electric field is applied across a nanoscale gap. The nanogap is spontaneously formed by the activation process, wherein a pulse voltage is applied between a pair of electrodes, which are separated by a narrow gap inside a vacuum chamber in the presence of hydrocarbons. At the gap, two elemental processes compete; the deposition of carbon by the electron-induced decomposition of hydrocarbons and the consumption of carbon by reaction with the silica substrate. The balance of the dynamics of the two processes, which simply depends on the temperature at the gap, is responsible for the spontaneous determination of the width of the nanogap. The calculation based on the model that involves the two competitive processes agrees with the experimental results on the activation process.

Hierarchical Nanoflowers on Nanograss Structure for a Non-wettable Surface and a SERS Substrate.

Hierarchical nanostructures of CuO nanoflowers on nanograss were investigated for self-cleaning and surface plasmonic applications. We achieved the hierarchical nanostructures using one-step oxidation process by controlling the formation of flower-like nanoscale residues (nanoflowers) on CuO nanograss. While the nanograss structure of CuO has a sufficient roughness for superhydrophobic characteristics, the additional hierarchy of nanoflowers on nanograss leads to a semi-reentrant structure with a high repellency even for a very small droplet (10 nL) of low surface tension liquid such as 25 % ethanol (~35 mN/m), thus providing non-wettable and self-cleaning properties. Furthermore, the CuO hierarchical nanostructure serves as a substrate for surface-enhanced Raman spectroscopy (SERS). Both of the CuO nanograss and nanoflower provide many nanoscale gaps that act as hot-spots for surface-enhanced Raman signal of 4-mercaptopyridine (4-Mpy), thus enabling a non-destructive detection in a short analysis time with relatively simple preparation of sample. Especially, the CuO nanoflower has larger number of hot-spots at the nanogaps from floral leaf-like structures, thus leading to three times higher Raman intensity than the CuO nanograss. These multifunctional results potentially provide a path toward cost-effective fabrication of a non-wettable surface for self-maintenance applications and a SERS substrate for sensing applications.Electronic supplementary materialThe online version of this article (doi:10.1186/s11671-015-1214-7) contains supplementary material, which is available to authorized users.

Flexible thin-film black gold membranes with ultrabroadband plasmonic nanofocusing for efficient solar vapour generation.

Solar steam generation has been achieved by surface plasmon heating with metallic nanoshells or nanoparticles, which have inherently narrow absorption bandwidth. For efficient light-to-heat conversion from a wider solar spectrum, we employ adiabatic plasmonic nanofocusing to attain both polarization-independent ultrabroadband light absorption and high plasmon dissipation loss. Here we demonstrate large area, flexible thin-film black gold membranes, which have multiscale structures of varying metallic nanoscale gaps (0–200 nm) as well as microscale funnel structures. The adiabatic nanofocusing of self-aggregated metallic nanowire bundle arrays produces average absorption of 91% at 400–2,500 nm and the microscale funnel structures lead to average reflection of 7% at 2.5–17 μm. This membrane allows heat localization within the few micrometre-thick layer and continuous water provision through micropores. We efficiently generate water vapour with solar thermal conversion efficiency up to 57% at 20 kW m−2. This new structure has a variety of applications in solar energy harvesting, thermoplasmonics and related technologies.

Coupled T-Shaped Optical Antennas with Two Resonances Localized in a Common Nanogap

Resonant optical antennas with nanoscale gaps are of high interest due to their ability to enhance electric fields in localized subdiffraction-limited volumes. They are especially attractive for coupling with quantum emitters. One challenge for applications that exhibit a spectral shift is to fabricate nanoantennas that provide two distinct resonances at the excitation and emission frequency, respectively. We propose a coupled T-shaped nanoantenna structure that provides independently controllable resonances with a common electromagnetic hot spot in the antenna gap. We demonstrate the fabrication of such structures and investigate experimentally and theoretically their spatial, time-integrated spectral- and polarization-dependent electromagnetic field properties. The nanoantennas exhibit two resonances with unique spectral and polarization responses. The resonance wavelengths are independently tailored by varying the geometry of individual T-shaped antennas.

Hierarchically arranged helical fibre actuators driven by solvents and vapours.

Mechanical responsiveness in many plants is produced by helical organizations of cellulose microfibrils. However, simple mimicry of these naturally occurring helical structures does not produce artificial materials with the desired tunable actuations. Here, we show that actuating fibres that respond to solvent and vapour stimuli can be created through the hierarchical and helical assembly of aligned carbon nanotubes. Primary fibres consisting of helical assemblies of multiwalled carbon nanotubes are twisted together to form the helical actuating fibres. The nanoscale gaps between the nanotubes and micrometre-scale gaps among the primary fibres contribute to the rapid response and large actuation stroke of the actuating fibres. The compact coils allow the actuating fibre to rotate reversibly. We show that these fibres, which are lightweight, flexible and strong, are suitable for a variety of applications such as energy-harvesting generators, deformable sensing springs and smart textiles.

Near-Field Thermal Radiation between Metasurfaces

Evanescent waves induced by thermal fluctuations can tunnel through nanoscale gap spacing, leading to super-Planckian thermal radiation. However, investigations of near-field thermal radiation of macroscopic objects have been limited to simple planar or effectively planar geometries until recently. Based on exact formulations including the scattering theory and Green’s function method, patterning thin films into 1D and 2D metasurfaces is found to increase the radiative heat flux by more than 1 order of magnitude in a certain range of thicknesses. The underlying mechanism of this counterintuitive phenomenon lies in the excitation of hyperbolic modes supporting high local density of states for broad frequency and k-space regimes. The radiative heat flux of a 2D metasurface increases monotonically with the thickness, while the heat flux of a 1D metasurface is not so sensitive to the thickness and is surprisingly higher than that of its 2D counterparts. The stark difference is attributed to the rapid-decay su...

Matching Nanoantenna Field Confinement to FRET Distances Enhances Förster Energy Transfer Rates.

Förster resonance energy transfer (FRET) is widely applied in chemistry, biology, and nanosciences to assess distances on sub-10 nm scale. Extending the range and applicability of FRET requires enhancement of the fluorescence energy transfer at a spatial scale comparable to the donor-acceptor distances. Plasmonic nanoantennas are ideal to concentrate optical fields at a nanoscale fully matching the FRET distance range. Here, we present a resonant aluminum nanogap antenna tailored to enhance single molecule FRET. A 20 nm gap confines light into a nanoscale volume, providing a field gradient on the scale of the donor-acceptor distance, a large 10-fold increase in the local density of optical states, and strong intensity enhancement. With our dedicated design, we obtain 20-fold enhancement on the fluorescence emission of donor and acceptor dyes, and most importantly up to 5-fold enhancement of the FRET rate for donor-acceptor separations of 10 nm. We also provide a thorough framework of the fluorescence photophysics occurring in the nanoscale gap volume. The presented enhancement of energy transfer flow at the nanoscale opens a yet unexplored facet of the various advantages of optical nanoantennas and provides a new strategy toward biological applications of single molecule FRET at micromolar concentrations.

Gap Plasmon Resonance in a Suspended Plasmonic Nanowire Coupled to a Metallic Substrate.

We present an experimental demonstration of nanoscale gap plasmon resonators that consist of an individual suspended plasmonic nanowire (NW) over a metallic substrate. Our study demonstrates that the NW supports strong gap plasmon resonances of various gap sizes including single-nanometer-scale gaps. The obtained resonance features agree well with intuitive resonance models for near- and far-field regimes. We also illustrate that our suspended NW geometry is capable of constructing plasmonic coupled systems dominated by quasi-electrostatics.

Carbon Electrode-Molecule Junctions: A Reliable Platform for Molecular Electronics.

The development of reliable approaches to integrate individual or a small collection of molecules into electrical nanocircuits, often termed "molecular electronics", is currently a research focus because it can not only overcome the increasing difficulties and fundamental limitations of miniaturization of current silicon-based electronic devices, but can also enable us to probe and understand the intrinsic properties of materials at the atomic- and/or molecular-length scale. This development might also lead to direct observation of novel effects and fundamental discovery of physical phenomena that are not accessible by traditional materials or approaches. Therefore, researchers from a variety of backgrounds have been devoting great effort to this objective, which has started to move beyond simple descriptions of charge transport and branch out in different directions, reflecting the interdisciplinarity. This Account exemplifies our ongoing interest and great effort in developing efficient lithographic methodologies capable of creating molecular electronic devices through the combination of top-down micro/nanofabrication with bottom-up molecular assembly. These devices use nanogapped carbon nanomaterials (such as single-walled carbon nanotubes (SWCNTs) and graphene), with a particular focus on graphene, as point contacts formed by electron beam lithography and precise oxygen plasma etching. Through robust amide linkages, functional molecular bridges terminated with diamine moieties are covalently wired into the carboxylic acid-functionalized nanogaps to form stable carbon electrode-molecule junctions with desired functionalities. At the macroscopic level, to improve the contact interface between electrodes and organic semiconductors and lower Schottky barriers, we used SWCNTs and graphene as efficient electrodes to explore the intrinsic properties of organic thin films, and then build functional high-performance organic nanotransistors with ultrahigh responsivities. At the molecular level, to form robust covalent bonds between electrodes and molecules and improve device stability, we developed a reliable system to immobilize individual molecules within a nanoscale gap of either SWCNTs or graphene through covalent amide bond formation, thus affording two classes of carbon electrode-molecule single-molecule junctions. One unique feature of these devices is the fact that they contain only one or two molecules as conductive elements, thus forming the basis for building new classes of chemo/biosensors with ultrahigh sensitivity. We have used these approaches to reveal the dependence of the charge transport of individual metallo-DNA duplexes on π-stacking integrity, and fabricate molecular devices capable of realizing label-free, real-time electrical detection of biological interactions at the single-event level, or switching their molecular conductance upon exposure to external stimuli, such as ion, pH, and light. These investigations highlight the unique advantages and importance of these universal methodologies to produce functional carbon electrode-molecule junctions in current and future researches toward the development of practical molecular devices, thus offering a reliable platform for molecular electronics and the promise of a new generation of multifunctional integrated circuits and sensors.

Theoretical Study of Hybrid Guided Modes in a Multilayer Symmetrical Planar Plasmonic Waveguide

We presented a comprehensive theoretical study of the hybrid guided mode in a multilayer symmetrical planar plasmoinc waveguide, which is constructed with a thin film metal layer symmetrically sandwiched by three dielectric low/high/low-index layers. The seven-layer planar plasmonic structure can support super long-range plasmonic modes with strong subwavelength confinement in the low-index gap layer. We derived the dispersion equations for the guided mode and characterized the hybrid guided mode based on our derived analytical expressions. We explained how the variations in the thickness of the low-index gap and high-index cladding could change the types of the hybrid mode from strong surface plasmon polariton (SPP)-like mode, to SPP-dielectric waveguide (DW)-like mode, and further to strong-DW-like mode. We also found that by tailoring the geometric dimensions of the waveguide, the plasmonic mode of the multilayer structure can be optimized with the strongest mode confinement at the nanoscale gap. The combination of tight light confinement and long-range propagation length makes the seven-layer plasmonic waveguide an excellent candidate for applications in chip-scale plasmonic integrated circuits. The presented theoretical analysis shall be very useful in the design and optimization of active and passive nanoplasmonic devices.

Near-field thermal radiation between doped silicon plates at nanoscale gaps

Radiative heat transfer can be significantly enhanced via photon tunneling through a nanometer-scale gap to the point that it exceeds the blackbody limit. Here we report quantitative measurements of the near-field thermal radiation between doped-Si plates ($\text{width}\phantom{\rule{0.28em}{0ex}}=\phantom{\rule{0.28em}{0ex}}480\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\text{m}$ and $\text{length}\phantom{\rule{0.28em}{0ex}}=\phantom{\rule{0.28em}{0ex}}1.34\phantom{\rule{0.28em}{0ex}}\mathrm{cm}$). A novel MEMS-based platform enables us to maintain doped-Si plates at nanoscale gap distances that cannot be achieved by other methods. The measured radiative heat transfer coefficient was found to be 2.91 times greater than the blackbody limit at a 400-nm vacuum gap.