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At least 1,045 records · Page 58

Preparation of porous nitrogen-doped titanium dioxide microspheres and a study of their photocatalytic, antibacterial and electrochemical activities

Graphical abstract: Porous N-doped TiO{sub 2} microspheres were prepared for the first time via plasma technique. The sample exhibited better photocatalytic activity, photoinduced inactivation activity and better electrochemical activity than those of TiO{sub 2} microspheres and P25. Display Omitted Highlights: ► Porous N-doped TiO{sub 2} microspheres were prepared via nitrogen plasma technique. ► Plasma treatment did not affect the porous structure of the TiO{sub 2} microspheres. ► With the plasma treatment, the N contents in the samples increased. ► Their photocatalytic, antibacterial and electrochemical activities were studied. -- Abstract: Nitrogen-doped titanium dioxide (N-doped TiO{sub 2}) microspheres with porous structure were prepared via the nitrogen-assisted glow discharge plasma technique at room temperature for the first time. The samples were characterized by X-ray diffraction, scanning electron microscopy, nitrogen adsorption–desorption measurement, UV–Vis diffuse reflectance spectra, photoluminescence spectroscopy and X-ray photoelectron spectroscopy. The results indicated that the plasma treatment did not affect the porous structure of the TiO{sub 2} microspheres. With the plasma treatment, the N contents in the samples increased. During the photocatalytic degradation of methylene blue under simulative sunlight irradiation, the sample after plasma treatment for 60 min (N-TiO{sub 2}-60) exhibited higher photocatalytic activity than those of the TiO{sub 2} microspheres, P25 and other N-doped TiO{sub 2} microspheres. Furthermore, the N-TiO{sub 2}-60 showed excellent antibacterial activities towards Escherichia coli under visible irradiation. These should be attributed to the enhancement of the visible light region absorption for TiO{sub 2} after N-doping. Electrochemical data demonstrated that the N-doping not only enhanced the electrochemical activity of TiO{sub 2}, but also improved the reversibility of Li insertion/extraction reactions and the rate behavior of TiO{sub 2} during charge–discharge cycles.

36 MATERIALS SCIENCE↗

Ambient pressure synthesis and characterization of layered honeycomb Li 2 PdO 3

Single-phase polycrystalline Li 2 PdO 3 has been synthesized at 640°C in oxygen for the first time under ambient pressure. X-ray and neutron diffraction analyses show that the sample possesses a monoclinic layered structure belonging to the C2/m space group. Rietveld refinements of neutron powder diffraction data indicate ~10% Li–Pd site exchange and DIFFaX modelling manifest ~2% stacking faults present within LiPd 2 layers. A band gap of ~2.23 eV was calculated for the golden Li 2 PdO 3 using absorbance measurements. Thermogravimetric analysis of the sample shows that Li 2 PdO 3 is stable up to 730°C under oxygen. Here a Curie tail is observed at low temperature magnetic measurements (T < 50K), yielding an effective moment of 0.038 μ B , possibly due to spin ½ impurities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large-area borophene sheets on sacrificial Cu(111) films promoted by recrystallization from subsurface boron

Borophene, an atomically thin covalently bonded boron sheet, has attracted great attention as a novel quantum material because of its structural tunability and potential utilization in flexible and transparent electronics. So far, borophene has been synthesized on silver or copper single crystals, but these substrates are small, very expensive, and unsuitable for study of transport properties or electronics applications. Here, we report synthesis of borophene on nanometer-scale thick Cu(111) films grown on sapphire. We have developed a process of enlarging faceted borophene islands, by repeated submersion of boron into copper at high temperature and resurfacing and re-crystallization at lower temperature. This discovery was enabled by real-time feedback from low-energy electron microscopy and diffraction. We demonstrate synthesis of borophene as faceted micrometer-size monocrystal islands or as full-monolayer sheets. The process is scalable to wafer size; moreover, Cu films could be sacrificed and sapphire reused. Our work opens the door for new experiments and brings applications one step closer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Following the dynamics of matter with femtosecond precision using the X-ray streaking method

X-ray Free Electron Lasers (FELs) can produce extremely intense and very short pulses, down to below 10 femtoseconds (fs). Among the key applications are ultrafast time-resolved studies of dynamics of matter by observing responses to fast excitation pulses in a pump-probe manner. Detectors with sufficient time resolution for observing these processes are not available. Therefore, such experiments typically measure a sample's full dynamics by repeating multiple pump-probe cycles at different delay times. This conventional method assumes that the sample returns to an identical or very similar state after each cycle. Here we describe a novel approach that can provide a time trace of responses following a single excitation pulse, jitter-free, with fs timing precision. We demonstrate, in an X-ray diffraction experiment, how it can be applied to the investigation of ultrafast irreversible processes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nonstationary oscillations in gyrotrons revisited

Development of gyrotrons requires careful understanding of different regimes of gyrotron oscillations. It is known that in the planes of the generalized gyrotron variables: cyclotron resonance mismatch and dimensionless current or cyclotron resonance mismatch and dimensionless interaction length complicated alternating sequences of regions of stationary, periodic, automodulation, and chaotic oscillations exist. In the past, these regions were investigated on the supposition that the transit time of electrons through the interaction space is much shorter than the cavity decay time. This assumption is valid for short and/or high diffraction quality resonators. However, in the case of long and/or low diffraction quality resonators, which are often utilized, this assumption is no longer valid. In such a case, a different mathematical formalism has to be used for studying nonstationary oscillations. One example of such a formalism is described in the present paper.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Surface acoustic wave propagation in graphene film

Surface acoustic wave (SAW) propagation in a graphene film on the surface of piezoelectric crystals was studied at the BESSY II synchrotron radiation source. Talbot effect enabled the visualization of the SAW propagation on the crystal surface with the graphene film in a real time mode, and high-resolution x-ray diffraction permitted the determination of the SAW amplitude in the graphene/piezoelectric crystal system. The influence of the SAW on the electrical properties of the graphene film was examined. It was shown that the changing of the SAW amplitude enables controlling the magnitude and direction of current in graphene film on the surface of piezoelectric crystals.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Probing polymer crystallization at processing-relevant cooling rates with synchrotron radiation

Processing of polymeric materials to produce any kind of goods, from films to complex objects, involves application of flow fields on the polymer melt, accompanied or followed by its rapid cooling. Typically, polymers solidify at cooling rates which span over a wide range, from a few to hundreds of °C/s. A novel method to probe polymer crystallization at processing-relevant cooling rates is proposed. Using a custom-built quenching device, thin polymer films are ballistically cooled from the melt at rates between approximately 10 and 200 °C/s. Thanks to highly brilliant synchrotron radiation and to state-of-the-art X-ray detectors, the crystallization process is followed in real-time, recording about 20 wide angle X-ray diffraction patterns per second while monitoring the instantaneous sample temperature. The method is applied to a series of industrially relevant polymers, such as isotactic polypropylene, its copolymers and virgin and nucleated polyamide-6. Their crystallization behaviour during rapid cooling is discussed, with particular attention to the occurrence of polymorphism, which deeply impact material’s properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The phase-contrast imaging instrument at the matter in extreme conditions endstation at LCLS

Here, we describe the phase-contrast imaging instrument at the Matter in Extreme Conditions (MEC) endstation of the Linac Coherent Light Source. The instrument can image phenomena with a spatial resolution of a few hundreds of nanometers and at the same time reveal the atomic structure through X-ray diffraction, with a temporal resolution better than 100 fs. It was specifically designed for studies relevant to high-energy-density science and can monitor, e.g., shock fronts, phase transitions, or void collapses. This versatile instrument was commissioned last year and is now available to the MEC user community.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Spall and subsequent recompaction of copper under shock loading

Research was undertaken to study spall and subsequent recompaction of oxygen-free high-thermal-conductivity copper using a single-stage large-bore light gas gun capable of planar impacts. Gun experiments were conducted that produced an initial spall in the target with a subsequent recompaction of the spall damage/layer by the use of layered impactors. Symmetric spall experiments at similar conditions were also conducted as a control to the recompaction experiments. Photonic Doppler velocimetry was used to obtain the velocity history of the target’s back surface; these velocity histories were analyzed, and the results were compared to numerical simulations. After recovery of selected samples, the microstructure was analyzed using optical imaging microscopy and electron backscatter diffraction. Recompaction waves were clearly observed in the time-resolved data obtained at the back surface of the targets. Two different series of experiments were performed to understand the effect of damage morphology on the stress required for spall recompaction. In the initial series, the peak pressure of the first shock was systematically increased to alter the amount of damage in the material. While in the second series, the peak pressure of the second shock was increased, keeping the magnitude of the first shock relatively constant to understand the effect of peak stress on the recompaction process. Findings clearly show that recompaction results in a perturbed band of the microstructure at the location of the expected spall plane in all cases except where the peak stress of the second shock is lower than the critical value.

, recompaction↗

Ultrafast sorting: Excimeric π–π stacking distinguishes pyrene-N-methylacetamide isomers on the ultrafast time scale

Pyrene based molecules are inclined to form excimers through self-association upon photoexcitation. In this work, the pyrene core is functionalized with N-methylacetamide group at the position 1 or 2, to develop pyren-1-methylacetamide (PyMA1) and pyren-2- methylacetamide (PyMA2), respectively. The introduction of methylacetamide group was believed to help having hydrogen bonded excimers in close aggregation. Upon photoexcitation, PyMA1 and PyMA2, at 1.0mM in toluene, have formed predominantly static and dynamic excimers, respectively. The transient absorption (TA) measurements over fs-ps regime (fs-TA) showed that the formation of static excimers is an ultrafast process (~560fs) whereas, the dynamic excimers formed in much slower time scale (~65ps). Finally, single crystal X-ray diffraction studies show that for PyMA2 the overlap between the pyrene moieties (~42%) are better than PyMA1 (~17%) in ground state at 80K, which also reflected in the respective lifetimes and population percentages of excimers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Light-activated Gigahertz Ferroelectric Domain Dynamics

Using time- and spatially-resolved hard X-ray diffraction microscopy, the striking structural and electrical dynamics upon optical excitation of a single crystal of BaTiO 3 are simultaneously captured on sub-nanoseconds and nanoscale within individual ferroelectric domains and across walls. A large emergent photo-induced electric field of up to 20 million volts per meter is discovered in a surface layer of the crystal, which then drives polarization and lattice dynamics that are dramatically distinct in a surface layer versus bulk regions. A dynamical phase-field modeling (DPFM) method is developed that reveals the microscopic origin of these dynamics, leading to GHz polarization and elastic waves travelling in the crystal with sonic speeds and spatially varying frequencies. The advance of spatiotemporal imaging and dynamical modeling tools open opportunities of disentangling ultrafast processes in complex mesoscale structures such as ferroelectric domains

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Improved Spatial Resolution Achieved by Chromatic Intensity Interferometry

Interferometers are widely used in imaging technologies to achieve enhanced spatial resolution, but require that the incoming photons be indistinguishable. In previous work, we built and analyzed color erasure detectors which expand the scope of intensity interferometry to accommodate sources of different colors. Here we demonstrate experimentally how color erasure detectors can achieve improved spatial resolution in an imaging task, well beyond the diffraction limit. Utilizing two 10.9 mm-aperture telescopes and a 0.8 m baseline, we measure the distance between a 1063.6 nm source and a 1064.4 nm source separated by 4.2 mm at a distance of 1.43 km, which surpasses the diffraction limit of a single telescope by about 40 times. Moreover, chromatic intensity interferometry allows us to recover the phase of the Fourier transform of the imaged objects – a quantity that is, in the presence of modest noise, inaccessible to conventional intensity interferometry.

74 ATOMIC AND MOLECULAR PHYSICS↗

Solid state reduction of nickelate thin films

The square-planar nickelates are a class of superconductors analogous to the cuprates and promise to provide insight into the pairing mechanism in high-temperature superconducting oxides. The parent phase of doped superconducting films is NdNiO 2 , which is prepared by reducing 3 + Ni in NdNiO 3 films. In this paper, we develop an ultrahigh vacuum reduction method using aluminum deposited on top of the 3 + nickelates and monitor the reduction process in real time through in situ crystal truncation rod measurements and diffraction x-ray absorption near edge spectroscopy measurements across the Ni K edge. Further, we establish a relation between Ni valence and the lattice constant of NdNiO 3-x and show that the process can precisely control the oxygen content in the films. Finally, we extend the reduction process to quintuple square-planar nickelates.

36 MATERIALS SCIENCE↗

Lifetimes and spatio-temporal response of protein crystals in intense X-ray microbeams

Serial synchrotron-based crystallography using intense microfocused X-ray beams, fast-framing detectors and protein microcrystals held at 300 K promises to expand the range of accessible structural targets and to increase overall structure-pipeline throughputs. To explore the nature and consequences of X-ray radiation damage under microbeam illumination, the time-, dose- and temperature-dependent evolution of crystal diffraction have been measured with maximum dose rates of 50 MGy s −1 . At all temperatures and dose rates, the integrated diffraction intensity for a fixed crystal orientation shows non-exponential decays with dose. Non-exponential decays are a consequence of non-uniform illumination and the resulting spatial evolution of diffracted intensity within the illuminated crystal volume. To quantify radiation-damage lifetimes and the damage state of diffracting crystal regions, a revised diffraction-weighted dose (DWD) is defined and it is shown that for Gaussian beams the DWD becomes nearly independent of actual dose at large doses. An apparent delayed onset of radiation damage seen in some intensity–dose curves is in fact a consequence of damage. Intensity fluctuations at high dose rates may arise from the impulsive release of gaseous damage products. Accounting for these effects, data collection at the highest dose rates increases crystal radiation lifetimes near 300 K (but not at 100 K) by a factor of ∼1.5–2 compared with those observed at conventional dose rates. Improved quantification and modeling of the complex spatio-temporal evolution of protein microcrystal diffraction in intense microbeams will enable more efficient data collection, and will be essential in improving the accuracy of structure factors and structural models.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Finite-frequency modeling of regional tropospheric infrasound using realistic atmospheres and terrain

Infrasonic waves have been observed to propagate to regional (greater than 15 km) distances through the troposphere. Infrasound propagation in the geometric acoustics approximation has shown that realistic terrain can scatter acoustic energy from tropospheric ducts; however, ray methods cannot intrinsically capture finite-frequency behavior such as diffraction. A two-dimensional finite-difference time-domain (FDTD) method has been developed to solve linearized equations for infrasound propagation with realistic terrain. Acoustic wave propagation over 100 km with both flat terrain and a Gaussian hill was first simulated in order to compare finite-frequency propagation with ray predictions. The effects of realistic terrain and atmospheres on infrasound signals from a 2012 surface explosion at the Utah Testing and Training Range are then investigated. Propagation through the troposphere is suggested by array processing results, but eigenrays are not predicted due to weak to nonexistent ducting conditions. FDTD modeling suggests that the inclusion of terrain and finite frequency effects helps explain much of the observed signal in a realistic scenario. Furthermore, these results suggest that geometric acoustics may underestimate propagation through the troposphere, and that recorded waveforms at regional distances may be noticeably affected by terrain.

58 GEOSCIENCES↗

Do analogs of the Hoyle state exist in {sup 16}O?

The root-mean-square radii of short-lived 0{sup +}-states in {sup 16}O were obtained for the first time from an analysis of α+{sup 16}O diffraction scattering. Data on elastic and inelastic α+{sup 16}O scattering were analyzed on the basis of the modified diffraction model in the range of projectile energies between a few tens of MeV units to 400 MeV. No case of a significant enhancement of the radius with respect to its ground-state value was observed. In particular, this concerns the 15.1-MeV 0{sub 6}{sup +} state, which lies near the threshold for breakup to four alpha particles and for which we did not confirm a giant radius predicted by the alpha-particle-condensate model. This result disproves the hypothesis that the {sup 16}O nucleus in the 0{sub 6}{sup +} state has a rarefied structure and appears to be an analog of the known Hoyle state at 7.65 MeV (0{sub 2}{sup +}) in {sup 12}C.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗