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Phonon-Polaritonic Bowtie Nanoantennas: Controlling Infrared Thermal Radiation at the Nanoscale
A conventional thermal emitter exhibits a broad emission spectrum with a peak wavelength depending upon the operation temperature. Recently, narrowband thermal emission was realized with periodic gratings or single microstructures of polar crystals supporting distinct optical modes. Here, we exploit the coupling of adjacent phonon-polaritonic nanostructures, demonstrating experimentally that the nanometer-scale gaps can control the thermal emission frequency while retaining emission line widths as narrow as 10 cm-1. This was achieved by using deeply subdiffractional bowtie-shaped silicon carbide nanoantennas. Infrared far-field reflectance spectroscopy, near-field optical nanoimaging, and full-wave electromagnetic simulations were employed to prove that the thermal emission originates from strongly localized surface phonon-polariton resonances of nanoantenna structures. The observed narrow emission line widths and exceptionally small modal volumes provide new opportunities for the user-design of near- and far-field radiation patterns for advancements in infrared spectroscopy, sensing, signaling, communications, coherent thermal emission, and infrared photodetection. © 2017 American Chemical Society.
Giant faraday rotation through ultra-small Fe0n clusters in superparamagnetic FeO-SiO2 vitreous films
Magnetooptical (MO) glasses and, in particular, Faraday rotators are becoming key components in lasers and optical information processing, light switching, coding, filtering, and sensing. The common design of such Faraday rotator materials follows a simple path: high Faraday rotation is achieved by maximizing the concentration of paramagnetic ion species in a given matrix material. However, this approach has reached its limits in terms of MO performance; hence, glass‐based materials can presently not be used efficiently in thin film MO applications. Here, a novel strategy which overcomes this limitation is demonstrated. Using vitreous films of xFeO·(100 − x)SiO2, unusually large Faraday rotation has been obtained, beating the performance of any other glassy material by up to two orders of magnitude. It is shown that this is due to the incorporation of small, ferromagnetic clusters of atomic iron which are generated in line during laser deposition and rapid condensation of the thin film, generating superparamagnetism. The size of these clusters underbids the present record of metallic Fe incorporation and experimental verification in glass matrices.
Tuning the spin coherence time of Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes by advanced ESR pulse protocols
We have investigated with the pulsed ESR technique at X- and Q-band frequencies the coherence and relaxation of Cu spins S = 1/2 in single crystals of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opba)] (1%) in the host lattice of [n-Bu4N]2[Ni(opba)] (99%, opba = o-phenylenebis(oxamato)) and of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opbon-Pr2)] (1%) in the host lattice of [n-Bu4N]2[Ni(opbon-Pr2)] (99%, opbon-Pr2 = o-phenylenebis(N(propyl)oxamidato)). For that we have measured the electron spin dephasing time Tm at different temperatures with the two-pulse primary echo and with the special Carr–Purcell–Meiboom–Gill (CPMG) multiple microwave pulse sequence. Application of the CPMG protocol has led to a substantial increase of the spin coherence lifetime in both complexes as compared to the primary echo results. It shows the efficiency of the suppression of the electron spin decoherence channel in the studied complexes arising due to spectral diffusion induced by a random modulation of the hyperfine interaction with the nuclear spins. We argue that this method can be used as a test for the relevance of the spectral diffusion for the electron spin decoherence. Our results have revealed a prominent role of the opba4– and opbon-Pr24– ligands for the dephasing of the Cu spins. The presence of additional 14N nuclei and protons in [Cu(opbon-Pr2)]2– as compared to [Cu(opba)]2– yields significantly shorter Tm times. Such a detrimental effect of the opbon-Pr24− ligands has to be considered when discussing a potential application of the Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes as building blocks of more complex molecular structures in prototype spintronic devices. Furthermore, in our work we propose an improved CPMG pulse protocol that enables elimination of unwanted echoes that inevitably appear in the case of inhomogeneously broadened ESR spectra due to the selective excitation of electron spins.
Mechanochemistry-assisted synthesis of hierarchical porous carbons applied as supercapacitors
A solvent-free synthesis of hierarchical porous carbons is conducted by a facile and fast mechanochemical reaction in a ball mill. By means of a mechanochemical ball-milling approach, we obtained titanium(IV) citrate-based polymers, which have been processed via high temperature chlorine treatment to hierarchical porous carbons with a high specific surface area of up to 1814 m2 g−1 and well-defined pore structures. The carbons are applied as electrode materials in electric double-layer capacitors showing high specific capacitances with 98 F g−1 in organic and 138 F g−1 in an ionic liquid electrolyte as well as good rate capabilities, maintaining 87% of the initial capacitance with 1 M TEA-BF4 in acetonitrile (ACN) and 81% at 10 A g−1 in EMIM-BF4.
A PDF Test-Set for Well-Formedness Validation in JHOVE - The Good, the Bad and the Ugly
Digital preservation and active software stewardship are both cyclical processes. While digital preservation strategies have to be reevaluated regularly to ensure that they still meet technological and organizational requirements, software needs to be tested with every new release to ensure that it functions correctly. JHOVE is an open source format validation tool which plays a central role in many digital preservation workflows and the PDF module is one of its most important features. Unlike tools such as Adobe PreFlight or veraPDF which check against requirements at profile level, JHOVE’s PDF-module is the only tool that can validate the syntax and structure of PDF files. Despite JHOVE’s widespread and long-standing adoption, the underlying validation rules are not formally or thoroughly tested, leading to bugs going undetected for a long time. Furthermore, there is no ground-truth data set which can be used to understand and test PDF validation at the structural level. The authors present a corpus of light-weight files designed to test the validation criteria of JHOVE’s PDF module against “well-formedness”. We conclude by measuring the code coverage of the test corpus within JHOVE PDF validation and by feeding detected inconsistencies of the PDF-module back into the open source development process.
Electrically-Pumped Wavelength-Tunable GaAs Quantum Dots Interfaced with Rubidium Atoms
We demonstrate the first wavelength-tunable electrically pumped source of nonclassical light that can emit photons with wavelength in resonance with the D2 transitions of 87Rb atoms. The device is fabricated by integrating a novel GaAs single-quantum-dot light-emitting diode (LED) onto a piezoelectric actuator. By feeding the emitted photons into a 75 mm long cell containing warm 87Rb vapor, we observe slow-light with a temporal delay of up to 3.4 ns. In view of the possibility of using 87Rb atomic vapors as quantum memories, this work makes an important step toward the realization of hybrid-quantum systems for future quantum networks.
(Metallo)porphyrins for potential materials science applications
The bottom-up approach to replace existing devices by molecular-based systems is a subject that attracts permanently increasing interest. Molecular-based devices offer not only to miniaturize the device further, but also to benefit from advanced functionalities of deposited molecules. Furthermore, the molecules itself can be tailored to allow via their self-assembly the potential fabrication of devices with an application potential, which is still unforeseeable at this time. Herein, we review efforts to use discrete (metallo)porphyrins for the formation of (sub)monolayers by surface-confined polymerization, of monolayers formed by supramolecular recognition and of thin films formed by sublimation techniques. Selected physical properties of these systems are reported as well. The application potential of those ensembles of (metallo)porphyrins in materials science is discussed.
The influence of the in-plane lattice constant on the superconducting transition temperature of FeSe0.7Te0.3 thin films
Epitaxial Fe(Se,Te) thin films were prepared by pulsed laser deposition on (La0.18Sr0.82)(Al0.59Ta0.41)O3 (LSAT), CaF2-buffered LSAT and bare CaF2 substrates, which exhibit an almost identical in-plane lattice parameter. The composition of all Fe(Se,Te) films were determined to be FeSe0.7Te0.3 by energy dispersive X-ray spectroscopy, irrespective of the substrate. Albeit the lattice parameters of all templates have comparable values, the in-plane lattice parameter of the FeSe0.7Te0.3 films varies significantly. We found that the superconducting transition temperature (Tc) of FeSe0.7Te0.3 thin films is strongly correlated with their a-axis lattice parameter. The highest Tc of over 19 K was observed for the film on bare CaF2 substrate, which is related to unexpectedly large in-plane compressive strain originating mostly from the thermal expansion mismatch between the FeSe0.7Te0.3 film and the substrate.
Germania and alumina dopant diffusion and viscous flow effects at preparation of doped optical fibers
We report on germania and alumina dopant profile shift effects at preparation of compact optical fibers using packaging methods (Stack-and-Draw method, Rod-in-Tube (RiT) technique). The sintering of package hollow volume by viscous flow results in a shift of the core-pitch ratio in all-solid microstructured fibers. The ratio is increased by about 5% in the case of a hexagonal package. The shift by diffusion effects of both dopants is simulated for typical slow speed drawing parameters. Thermodynamic approximations of surface dissociation of germania doped silica suggest the need of an adequate undoped silica barrier layer to prevent an undesired bubble formation at fiber drawing. In contrast, alumina doping does not estimate critical dissociation effects with vaporous aluminium oxide components. We report guide values of diffusion length of germania and alumina for the drawing process by kinetic approximation. The germania diffusion involves a small core enlargement, typically in the sub-micrometer scale. Though, the alumina diffusion enlarges it by a few micrometers. A drawn pure alumina preform core rod transforms to an amorphous aluminosilicate core with a molar alumina concentration of only about 50% and a non-gaussian concentration profile.
Synthesis, spectroscopic characterization and thermogravimetric analysis of two series of substituted (metallo)tetraphenylporphyrins
Subsequent treatment of H2TPP(CO2H)4 (tetra(p-carboxylic acid phenyl)porphyrin, 1) with an excess of oxalyl chloride and HNR2 afforded H2TPP(C(O)NR2)4 (R = Me, 2; iPr, 3) with yields exceeding 80%. The porphyrins 2 and 3 could be converted to the corresponding metalloporphyrins MTPP(C(O)NR2)4 (R = Me/iPr for M = Zn (2a, 3a); Cu (2b, 3b); Ni (2c, 3c); Co (2d, 3d)) by the addition of 3 equiv of anhydrous MCl2 (M = Zn, Cu, Ni, Co) to dimethylformamide solutions of 2 and 3 at elevated temperatures. Metalloporphyrins 2a–d and 3a–d were obtained in yields exceeding 60% and have been, as well as 2 and 3, characterized by elemental analysis, electrospray ionization mass spectrometry (ESIMS) and IR and UV–vis spectroscopy. Porphyrins 2, 2a–d and 3, 3a–d are not suitable for organic molecular beam deposition (OMBD), which is attributed to their comparatively low thermal stability as determined by thermogravimetric analysis (TG) of selected representatives.