High-speed tracking of single particles is a gateway to understanding physical, chemical, and biological processes at the nanoscale. It is also a major experimental challenge, particularly for small, nanometer-scale particles. Although methods such as confocal or fluorescence microscopy offer both high spatial resolution and high signal-to-background ratios, the fluorescence emission lifetime limits the measurement speed, while photobleaching and thermal diffusion limit the duration of measurements. Here we present a tracking method based on elastic light scattering that enables long-duration measurements of nanoparticle dynamics at rates of thousands of frames per second. We contain the particles within a single-mode silica fiber having a subwavelength, nanofluidic channel and illuminate them using the fiber's strongly confined optical mode. The diffusing particles in this cylindrical geometry are continuously illuminated inside the collection focal plane. We show that the method can track unlabeled dielectric particles as small as 20 nm as well as individual cowpea chlorotic mottle virus (CCMV) virions-26 nm in size and 4.6 megadaltons in mass-at rates of over 3 kHz for durations of tens of seconds. Our setup is easily incorporated into common optical microscopes and extends their detection range to nanometer-scale particles and macromolecules. The ease-of-use and performance of this technique support its potential for widespread applications in medical diagnostics and micro total analysis systems.
In binary aluminosilicate liquids and glasses, heterogeneity on intermediate length scale is a crucial factor for optical fiber performance, determining the lower limit of optical attenuation and Rayleigh scattering, but also clustering and precipitation of optically active dopants, for example, in the fabrication of high-power laser gain media. Here, we consider the low-frequency vibrational modes of such materials for assessing structural heterogeneity on molecular scale. We determine the vibrational density of states VDoS g(ω) using low-temperature heat capacity data. From correlation with low-frequency Raman spectroscopy, we obtain the Raman coupling coefficient. Both experiments allow for the extraction of the average dynamic correlation length as a function of alumina content. We find that this value decreases from about 3.9 nm to 3.3 nm when mildly increasing the alumina content from zero (vitreous silica) to 7 mol%. At the same time, the average inter-particle distance increases slightly due to the presence of oxygen tricluster species. In accordance with Loewensteinian dynamics, this proves that mild alumina doping increases structural homogeneity on molecular scale.
The increasing fields of applications for modern optical fibers present great challenges to the material properties and the processing technology of fiber optics. This paper gives an overview of the capabilities and limitations of established vapor deposition fiber preform technologies, and discusses new techniques for improved and extended doping properties in fiber preparation. In addition, alternative fabrication technologies are discussed, such as a powder-based process (REPUSIL) and an optimized glass melting method to overcome the limits of conventional vapor deposition methods concerning the volume fabrication of rare earth (RE)-doped quartz and high silica glasses. The new preform technologies are complementary with respect to enhanced RE solubility, the adjustment of nonlinear fiber properties, and the possibility of hybrid fiber fabrication. The drawing technology is described based on the requirements of specialty fibers such as adjusted preform and fiber diameters, varying coating properties, and the microstructuring of fiber configurations as low as in the nanometer range.
Guiding light inside the hollow cores of microstructured optical fibers is a major research field within fiber optics. However, most of current fibers reveal limited spectral operation ranges between the mid-visible and the infrared and rely on complicated microstructures. Here we report on a new type of hollow-core fiber, showing for the first time distinct transmission windows between the deep ultraviolet and the near infrared. The fiber, guiding in a single mode, operates by the central core mode being anti-resonant to adjacent modes, leading to a novel modified tunneling leaky mode. The fiber design is straightforward to implement and reveals beneficial features such as preselecting the lowest loss mode (Gaussian-like or donut-shaped mode). Fibers with such a unique combination of attributes allow accessing the extremely important deep-UV range with Gaussian-like mode quality and may pave the way for new discoveries in biophotonics, multispectral spectroscopy, photo-initiated chemistry or ultrashort pulse delivery.
Metal-organic frameworks (Mofs) are intriguing host materials in composite electrolytes due to their ability for tailoring host-guest interactions by chemical tuning of the Mof backbone. Here, we introduce particularly high sodium ion conductivity into the zeolitic imidazolate framework ZIF-8 by impregnation with the sodium-salt-containing ionic liquid (iL) (na 0.1 eMiM 0.9)tfSi. We demonstrate an ionic conductivity exceeding 2 × 10 −4 S • cm −1 at room temperature, with an activation energy as low as 0.26 eV, i.e., the highest reported performance for room temperature na +-related ion conduction in Mof-based composite electrolytes to date. partial amorphization of the Zif-backbone by ball-milling results in significant enhancement of the composite stability towards exposure to ambient conditions, up to 20 days. While the introduction of network disorder decelerates IL exudation and interactions with ambient contaminants, the ion conductivity is only marginally affected, decreasing with decreasing crystallinity but still maintaining superionic behavior. This highlights the general importance of 3D networks of interconnected pores for efficient ion conduction in MOF/IL blends, whereas pore symmetry is a less stringent condition. Crystalline metal-organic frameworks (MOFs) consist of metal nodes as coordination centers and organic linkers which self-assemble to form a three-dimensional network. Chemical tailoring of both the inorganic node and the organic linker enables property design for a wide range of applications such as gas storage, gas separation, catalysis and ion conduction 1,2. An alternative route to tune the properties of a given MOF is post-synthetic modification, for example, by applying pressure, temperature or other exogenous stimuli 3. Depending on stimulus intensity, such post-treatment can lead to structural collapse and solid-state amorphization of the framework 4-7. The formation of amorphous MOFs through solid-solid transitions (or, similarly, through quenching of MOF-liquids) is of particular interest due to the distinct variations in chemical, mechanical and physical properties which can be obtained as a result of structural disorder 8. Amorphization of MOFs can be achieved via different techniques, including pressure-induced structural collapse, ball-milling, melt-quenching, hot-pressing, and re-melting 8-10. Of these, ball-milling, or mechanosynthesis, which can also be used to synthesize crystalline MOFs, is the most universally applicable route. The low minimum shear moduli of MOFs have previously been shown to be responsible for facile collapse of systems such as UiO-66 ([Zr 6 O 4 (OH) 4 (1,4-BDC) 6 ], BDC = benzenedicarboxylate) 11. Using calcein as a model drug incorporated into crystalline UiO-66, it was demonstrated that amorphization via ball-milling leads to delayed release of the guest molecule: the timescale of release was increased from ~2 days in the crystalline structure to one month in the amorphous composite as a result of structural collapse 12. Here, we investigate how st...
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