Confinement effects of mandrel degradation in ICF target fabrication.

Understanding and further regulating the degradation of mandrel materials is a key aspect of target fabrication in inertial confinement fusion (ICF). Here, a quasi-one-dimensional confinement model is developed using a series of single-walled carbon nanotubes with varying diameters (Dm), and the degradation of poly-α-methylstyrene (PAMS) as a typical mandrel material is investigated under such confined conditions by using the combined method of quantum mechanics and molecular mechanics. In comparison to the isolated system, the calculations show that confinement can decrease or increase the energy barriers of PAMS degradation, which directly depends on Dm. Following which a clear exponential relationship between the degradation rate of PAMS and its own density is derived, indicating that the density of PAMS can be used to regulate mandrel degradation. This work highlights the important effects of confinement on degradation and provides a valuable reference for further development of polymer degradation technologies in ICF target fabrication and other fields.

Synthesis, Hole Doping, and Electrical Properties of a Semiconducting Azatriangulene-Based Covalent Organic Framework.

Two-dimensional covalent organic frameworks (2D COFs) containing heterotriangulenes have been theoretically identified as semiconductors with tunable, Dirac-cone-like band structures, which are expected to afford high charge-carrier mobilities ideal for next-generation flexible electronics. However, few bulk syntheses of these materials have been reported, and existing synthetic methods provide limited control of network purity and morphology. Here, we report transimination reactions between benzophenone-imine-protected azatriangulenes (OTPA) and benzodithiophene dialdehydes (BDT), which afforded a new semiconducting COF network, OTPA-BDT. The COFs were prepared as both polycrystalline powders and thin films with controlled crystallite orientation. The azatriangulene nodes are readily oxidized to stable radical cations upon exposure to an appropriate p-type dopant, tris(4-bromophenyl)ammoniumyl hexachloroantimonate, after which the network's crystallinity and orientation are maintained. Oriented, hole-doped OTPA-BDT COF films exhibit electrical conductivities of up to 1.2 × 10-1 S cm-1, which are among the highest reported for imine-linked 2D COFs to date.

Design of Surface Plasmon Resonance-Based D-Type Double Open-Loop Channels PCF for Temperature Sensing.

Here, we document a D-type double open-loop channel floor plasmon resonance (SPR) photonic crystal fiber (PCF) for temperature sensing. The grooves are designed on the polished surfaces of the pinnacle and backside of the PCF and covered with a gold (Au) film, and stomata are distributed around the PCF core in a progressive, periodic arrangement. Two air holes between the Au membrane and the PCF core are designed to shape a leakage window, which no longer solely averts the outward diffusion of Y-polarized (Y-POL) core mode energy, but also sets off its coupling with the Au movie from the leakage window. This SPR-PCF sensor uses the temperature-sensitive property of Polydimethylsiloxane (PDMS) to reap the motive of temperature sensing. Our lookup effects point out that these SPR-PCF sensors have a temperature sensitivity of up to 3757 pm/°C when the temperature varies from 5 °C to 45 °C. In addition, the maximum refractive index sensitivity (RIS) of the SPR-PCF sensor is as excessive as 4847 nm/RIU. These proposed SPR-PCF temperature sensors have an easy nanostructure and proper sensing performance, which now not solely improve the overall sensing performance of small-diameter fiber optic temperature sensors, but also have vast application prospects in geo-logical exploration, biological monitoring, and meteorological prediction due to their remarkable RIS and exclusive nanostructure.

Synthesis of Uranium Single Atom from Radioactive Wastewater for Enhanced Water Dissociation and Hydrogen Evolution.

As a common nuclide in radioactive wastewater, uranium (U) is generally treated by landfill, which induces the massive abandonment of uranium resources. In this work, a pulse voltammetry method for the synthesis of U single atoms on MoS2 (U/MoS2 ) nanosheets from radioactive wastewater for the electrocatalytic alkaline hydrogen evolution reaction (HER) is reported. The mass loading of U single atoms is facilely controlled with high selectivity for coexisting ions in radioactive wastewater. In the electrolyte of 1 m of KOH, U/MoS2 nanosheets with 5.2% of U single atoms exhibit relatively low overpotentials of 72 mV at 10 mA cm-2 . The mechanistic study reveals that the HER on U/MoS2 includes the water dissociation on U single atoms to form OH* and H transfer from OH* to adjacent S-edge atoms. This procedure exhibits decreased activation energy for transition state in water dissociation and optimized Gibbs free energy for H* adsorption.

Side-chain engineering for high degradation performance of mandrel materials in ICF target fabrication.

The exploration of mandrel materials with superior degradation performance to the traditionally adopted hydrocarbon polymer of poly-α-methylstyrene (PAMS), has always been an important pursuit for fabricating high-quality inertial confinement fusion (ICF) targets. Here, we propose a method to enhance the degradation performance of mandrel material based on side-chain engineering. A series of hydrocarbon cyclic functional groups, including cyclopentane, cyclopentadiene, naphthalene and azulene, are used to replace the benzene ring on the side chain of PAMS to form new polymer structures. The results show that the degradation performance of structures can be largely regulated by different side chains. In particular, one of the naphthalene-substituted structures has similar properties to PAMS, but the required degradation condition is lower. Furthermore, the reaction rate calculations indicate that this structure is expected to be synthesized experimentally. This work provides a direction for side-chain engineering for research into the key technology of ICF target fabrication in the future.

Entropy-driven catalytic reaction-induced hairpin structure switching for fluorometric detection of uranyl ions.

An ultra-sensitive and "turn-on" method is demonstrated for the determination of uranyl ion. The assay is based on hairpin-to-DNAzyme structure switching that is induced by an entropy-driven catalytic reaction. An UO22+-specific DNAzyme is cleaved by UO22+ to produce a DNA fragment. This fragment initiates the entropy-driven catalytic reaction to produce a large number of a sequence "R". The sequence R initiates the circular cleavage of FAM-labeled hairpins by switching the hairpin to Mg2+-specific DNAzyme structure. This causes the recovery of green fluorescence. The method works in the 20 pM to 800 pM concentration range and the limit of detection is 4 pM. Graphical abstract Entropy driven catalytic reaction induced hairpin structure switching for fluorometric detection of uranyl ions.

A Tunable Plasmonic Refractive Index Sensor with Nanoring-Strip Graphene Arrays.

In the present study, we design a tunable plasmonic refractive index sensor with nanoring-strip graphene arrays. The calculations prove that the nanoring-strip have two transmission dips. By changing the strip length L of the present structure, we find that the nanoring-strip graphene arrays have a wide range of resonances (resonance wavelength increases from 17.73 µm to 28.15 µm). When changing the sensing medium refractive index nmed, the sensitivity of mode A and B can reach 2.97 µm/RIU and 5.20 µm/RIU. By changing the doping level ng, we notice that the transmission characteristics can be tuned flexibly. Finally, the proposed sensor also shows good angle tolerance for both transverse magnetic (TM) and transverse electric (TE) polarizations. The proposed nanoring-strip graphene arrays along with the numerical results could open a new avenue to realize various tunable plasmon devices and have a great application prospect in biosensing, detection, and imaging.

Laser emission from flash ignition of Zr/Al nanoparticles.

We report the first laser emission from flash ignition of Zr/Al nanoparticles with the addition of strong oxidizer KClO4 using Nd: YAG as a laser medium. The mixture Zr/Al/Kp-45 (mass ratio = 33%Zr: 33%Al: 34%KClO4) has the highest brightness temperature Tb = 4615 K and the adiabatic flame temperature Tf = 4194 K with the duration of 20 ms. At 1064 nm we measured a maximum output energy of 702.5 mJ with the duration of nearly 10 ms by using only 100 mg mixture with an output coupler (transmission T = 10%). Further optimizing the concentration cavity and increasing the mixture content will yield much higher efficiency and output energy.

Effect of boundary continuity on nanosecond laser damage of nodular defects in high-reflection coatings.

Two types of engineered nodules in Ta2O5/SiO2 high-reflection coatings were prepared using electron beam evaporation and an ion-assisted deposition processes to facilitate poor and good boundary continuity, respectively. The influence of nodular boundary continuity on their nanosecond laser damage characteristics was investigated through experimental studies, combined with 3D finite-difference time domain simulations and photo-thermal micro-characterizations. Better boundary continuity led to improved mechanical stability and higher ejection fluence of nodules, in accordance with the thermomechanical damage model. In contrast, the ejected nodules that initially had better boundary continuity exhibited higher localized absorption and lower damage growth fluence, which is attributed to the creation of mechanically induced electronic defects or stronger electric field intensity enhancement at the ejected nodules.

[An Analysis of Combustion Emission Spectrum and Combustion Products of KClO4/Zr in the Quartz Tubes].

Aiming at understanding the light radiation properties of KClO4/Zr combusting under different conditions, emission spectrum and combustion products for KClO4/Zr combusting in open air and closed quartz tubes were studied respectively. Energy distribution of the light radiation signal and the emission intensity evolution with time were measured with fiber optic spectrometer, and photo-diode and oscilloscope. Spectral efficiency within (590±10), (750±10) and (808±10) nm were analyzed respectively according to the obtained flame emission spectrum. Morphology of the combustion products of KClO4/Zr were observed with scanning electronic microscopy (SEM). Results showed that the flame emission spectrum of KClO4/Zr distributed within the visible and near infrared width wave band, whiel the strongest radiation appeared within 730 nm to 820 nm band. When burning in closed quartz tubes, detected combustion emission spectrum intensity decreased significantly with the decrease in size of the tube. Also, the energy distribution of the emission spectrum showed different variation trends, and to deal with flame emission spectrum distribution, as the change of volume of quartz tubes, (590±10), (750±10) and (808±10) nm bands' spectral efficiency are also present different change rules. Generally, increasing the diameter of the quarts tube favored the increase of the effective light radiation energy detected outside of the tube, and decreasing the diameter of the quartz tubes favored the peak emission intensity of KClO4/Zr. With the increase of tube diameter, KClO4 burning more fully, the product particle size is smaller; the morphology is the rule of the globular. And the change of tube length is not too large effect in the reaction results.

Depolymerization of Free-Radical Polymers with Spin Migrations.

The mechanism of depolymerization is one of the most essential issues in chemical engineering and materials science. In this work, we investigate the depolymerization reactions of three typical free-radical poly(alpha-methylstyrene) tetramers by using first-principles density functional theory. The calculated results show that these reactions all need to overcome the energy barriers in the range of 0.58 to 0.77 eV, and that breaking the C-C bond at the chain end leads to the dissociation of alpha-methylstyrene monomers from the polymers. Electronic-structure analysis indicates that the reactions occur easily at the CR3 unsaturated end, and that the frontier molecular orbitals that participate in the reactions are mainly localized at the unsaturated ends. Meanwhile, spin population analysis presents the unique net spin-transfer process in free-radical depolymerization reactions. We hope the current findings can contribute to understanding the free-radical depolymerization mechanism and help guide future experiments.

The influence of edge and corner evolution on plasmon properties and resonant edge effect in gold nanoplatelets.

In this paper a simulation of the properties of surface plasmons on gold nanoplatelets with various cross-sections inscribed in a circle and an investigation of their field distributions to assign multiple SPRs are described. The manipulated propagation can be obtained through the evolution of edges and corners. Furthermore, the particle morphology and the associated spectral positions alone do not uniquely reflect the important details of the local field distribution or the resonance modes. The plasmon modes were investigated and found to be mainly excited along the edges and in the side and sloped side surfaces. The strong field distributions can generally be found around the corners and how the plasmons transmit through the corners to adjacent edges was also investigated. Besides the plasmons excited along the edges as were found for the triangular nanoplatelets, plasmons were excited in the interior region of the triangular surfaces and were also investigated. Despite this in the infrared region, plasmon modes were found to be along the edges for the hexagonal nanoplatelets. Also, it can be seen that the change of nanoplatelet thickness can support different plasmon modes ranging from dipolar resonance mode to quadrupole resonance mode. The thickness far below the skin depth can display complex plasmon modes along the edges and on the side and sloping side surfaces as well as the strong coupling between the top and bottom surfaces. The observed plasmon resonance modes in this simulation reflect the interference of all these contributions including the plasmons along the edges and on the side surfaces. This is an essential step towards a thorough understanding of plasmon modes and the effect of edge and corner evolution in polygonous nanoplatelets.

Hydrogen spillover mechanism on covalent organic frameworks as investigated by ab initio density functional calculation.

The hydrogen spillover mechanism, including the H chemisorption, diffusion, and H(2) associative desorption on the surface of COFs and H atoms migration from metal catalyst to COFs, have been studied via density functional theory (DFT) calculation. The results described herein show that each sp(2) C atom on COFs' surface can adsorb one H atom with the bond length d(C-H) between 1.11 and 1.14 Å, and the up-down arrangement of the adsorbed H atoms is the most stable configuration. By counting the chemisorption binding sites for these COFs, we can predict the saturation storage densities. High hydrogen storage densities show that the gravimetric uptakes of COFs are in the range of 5.13-6.06 wt%. The CI-NEB calculations reveal that one H atom diffusing along the C-C path on HHTP surface should overcome the 1.41-2.16 eV energy barrier. We chose tetrahedral Pt(4) cluster and HHTP as the representative catalyst and substrate, respectively, to study the H migration from metal cluster to COFs. At most, two H atoms can migrate from Pt(4) cluster to HHTP substrate. The migration reaction is an endothermic process, undergoing an activation barrier of 1.87 eV and 0.57 eV for the first and second H migration process, respectively. Three types of H(2) associative desorption from hydrogenated COFs were studied: (I) the two H adatoms recombining to one H(2) molecule with a recombination barrier of 4.28 eV, (II) the abstraction of adsorbed H atoms by gas-phase hydrogen atoms through ER type recombination reactions with a recombination barrier of 1.05 eV, (III) the H(2) desorption through the reverse spillover mechanism with an energy barrier of 2.90 eV.

Bulk synthesis of monodisperse magnetic FeNi3 nanopowders by flow levitation method.

In this work, a novel bulk synthesis method for monodisperse FeNi3 nanoparticles was developed by flow levitation method (FL). The Fe and Ni vapours ascending from the high temperature levitated droplet was condensed by cryogenic Ar gas under atmospheric pressure. X-ray diffraction was used to identify and characterize the crystal phase of prepared powders exhibiting a FeNi3 phase. The morphology and size of nanopowders were observed by transmission electron microscopy (TEM). The chemical composition of the nanoparticles was determined with energy dispersive spectrometer (EDS). The results indicated that the FeNi3 permalloy powders are nearly spherical-shaped with diameter about 50-200 nm. Measurement of the magnetic property of nanopowders by a superconducting quantum interference device (SQUID, Quantum Design MPMS-7) showed a symmetric hysteresis loop of ferromagnetic behavior with coercivity of 220 Oe and saturation magnetization of 107.17 emu/g, at 293 K. At 5 K, the obtained saturation magnetization of the sample was 102.16 emu/g. The production rate of FeNi3 nanoparticles was estimated to be about 6 g/h. This method has great potential in mass production of FeNi3 nannoparticles.

[Study on the preparation and properties of novel silica microporous antireflective coating by sol-gel process].

Silica sol was prepared by acid catalyzed sol-gel process using tetraethylorthosilicate (TEOS) as precursor and dimethyldietoxysilane (DDS) as pore-forming agent. A novel kind of monolayer microporous silica anti-reflective (AR) coating was obtained on K9 glass substrate by dip-coating technique and then heat treated at 500 degrees C. The effects of different DDS/TEOS molar ratios on refractive index, transmittance and hardness were investigated. A positive correlation was found between the transmittance and the DDS/TEOS molar ratio due to the increasing porosity. The maximum transmittance can reach 99.7% with the molar ratio of DDS/TEOS rising to 1 : 1. Meanwhile, the refractive index was found quite close to the ideal value 1.22. Nevertheless, higher molar ratio will lead to a bad film-forming property. On the other hand, the hardness of the coatings decreased with the DDS increasing but still remained more than 2 h when the transmittance reached highest. Besides, these coatings exhibit a well abrasion-resistance and excellent adhesivity. The maximum transmittance was only dropped by 0.071% and 0.112% after abrasion for 500 and 1 000 times respectively. Accelerated corrosion tests indicated that the transmittance of traditional coatings rapidly fell down to the substrate level (-92%) after immersion for 5 min, while the transmittance of our novel coating almost linearly decreased and was kept 93.2% after 56 min. In other words, the environment-resistance of our novel silica AR coating is ten times higher than that of traditional ones. The promotions of the coating performances benefit from its micropore structure (-0. 4 nm) with which water molecule can be effectively prevented. With its high transmittance, good mechanical properties and high environment-resistance, this kind of novel coating has a potential application in the field of solar glass modification to improve its anti-reflective properties.

Ultra-Wideband High-Efficiency Solar Absorber and Thermal Emitter Based on Semiconductor InAs Microstructures.

Since the use of chemical fuels is permanently damaging the environment, the need for new energy sources is urgent for mankind. Given that solar energy is a clean and sustainable energy source, this study investigates and proposes a six-layer composite ultra-wideband high-efficiency solar absorber with an annular microstructure. It achieves this by using a combination of the properties of metamaterials and the quantum confinement effects of semiconductor materials. The substrate is W-Ti-Al2O3, and the microstructure is an annular InAs-square InAs film-Ti film combination. We used Lumerical Solutions' FDTD solution program to simulate the absorber and calculate the model's absorption, field distribution, and thermal radiation efficiency (when it is used as a thermal emitter), and further explored the physical mechanism of the model's ultra-broadband absorption. Our model has an average absorption of 95.80% in the 283-3615 nm band, 95.66% in the 280-4000 nm band, and a weighted average absorption efficiency of 95.78% under AM1.5 illumination. Meanwhile, the reflectance of the model in the 5586-20,000 nm band is all higher than 80%, with an average reflectance of 94.52%, which has a good thermal infrared suppression performance. It is 95.42% under thermal radiation at 1000 K. It has outstanding performance when employed as a thermal emitter as well. Additionally, simulation results show that the absorber has good polarization and incidence angle insensitivity. The model may be applied to photodetection, thermophotovoltaics, bio-detection, imaging, thermal ion emission, and solar water evaporation for water purification.

Plasmoid ejection and secondary current sheet generation from magnetic reconnection in laser-plasma interaction.

Reconnection of the self-generated magnetic fields in laser-plasma interaction was first investigated experimentally by Nilson et al. [Phys. Rev. Lett. 97, 255001 (2006)] by shining two laser pulses a distance apart on a solid target layer. An elongated current sheet (CS) was observed in the plasma between the two laser spots. In order to more closely model magnetotail reconnection, here two side-by-side thin target layers, instead of a single one, are used. It is found that at one end of the elongated CS a fanlike electron outflow region including three well-collimated electron jets appears. The (>1 MeV) tail of the jet energy distribution exhibits a power-law scaling. The enhanced electron acceleration is attributed to the intense inductive electric field in the narrow electron dominated reconnection region, as well as additional acceleration as they are trapped inside the rapidly moving plasmoid formed in and ejected from the CS. The ejection also induces a secondary CS.

GCMC investigation into adamantane-based aromatic frameworks with diamond-like structure as high-capacity hydrogen storage materials.

A new class of 3D adamantane-based aromatic framework (AAF) with diamond-like structure was computationally designed with the aid of density functional theory (DFT) calculation and molecular mechanics (MM) methods. The hydrogen storage capacities of these AAFs were studied by the method of grand canonical Monte Carlo (GCMC) simulations. The calculated pore sizes of three AAFs reveal that AAF-1 and AAF-2 belong to microporous materials, while AAF-3 is a member of mesoporous materials. The GCMC results reveal that at 77 K and 100 bar, AAF-3 exhibits the highest gravimetric hydrogen uptake of 29.50 wt%, while AAF-1 shows the highest volumetric hydrogen uptake of 63.04 g L(-1). In particular, the gravimetric hydrogen uptake of AAF-3 reaches the Department of Energy's target of 6 wt% at room temperature. The extraordinary performances of these new AAFs in hydrogen storage have made them enter the list of top hydrogen storage materials up to now.

[Study of density functional theory for surface-enhanced Raman spectra of furfural].

In the present paper, DFT method at the B3LYP/6-31+G* * (C, H, O)/LANL2DZ(Ag) level was used to optimize molecular configurations of furfural. Based on the optimized structure, the normal Raman spectrum (NRS) of FUR and the surface-enhanced Raman spectrum (SERS) of FUR adsorbed on Ag, Ag2 and Ag4 were all calculated, which were compared with the experimental values. The calculation results indicated that a good conformity was found between the computed and the experimental results. The results of furfural adsorbed on Ag4 were more approximate to the ever reported experimental date than those of furfural adsorbed on Ag and Ag2. At the end, detailed analysis of the Raman spectrum and more comprehensive assignments of the vibration mode for furfural were studied by the software of GaussView. The data of the SERS by comparing with the one of NRS show that furfural molecule and Ag atoms interact with each other. And we suppose that the molecular plane with the ring of adsorbed furfural molecule is vertically orientated to the silver surface. The work in this paper offers a theory evidence for detection and trace analysis of drinks containing furfural.

[Surface-enhanced raman spectra of thymine calculated by DFT and ab inition HF].

In the present paper, B3LYP (Becke's three-parameter hybrid method with the Lee, Yang, and Parr gradient corrected correlation functional) and HF (Hartree-Fock) methods at 6-31+G* * (C, H, N, O)/LANL2DZ(Ag) level were used to optimize molecular configurations of thymine. Base on the optimized structure, the normal Raman spectrum (NRS) of thymine and the surface-enhanced Raman spectrum (SERS) of thymine adsorbed on Ag and Ag2 were calculated, which were compared with the experimental values. The calculation results indicated that the result of the DFT for NRS was more approximate to the ever reported experimental date than those of HF results. A better conformity of SERS was found between the HF computed and the experimental results. At the end, detailed analysis of the Raman spectrum and more comprehensive assignments of the vibration mode for thymine were studied by the software of GaussView.