Understanding the anomalous dispersion of doubly ionized carbon plasmas near 47 nm

Over the last several years we have predicted and observed plasmas with an index of refraction greater than 1 in the soft X-ray regime. These plasmas are usually a few times ionized and have ranged from low-Z carbon plasmas to mid-Z tin plasmas. Our main calculational tool has been the average-atom code. We have recently observed C²⁺ plasmas with an index of refraction greater than 1 at a wavelength of 46.9 nm (26.44 eV). In this paper we compare the average-atom method, AVATOMKG, against two more detailed methods, OPAL and CAK, for calculating the index of refraction for the carbon plasmas and discuss the different approximations used. We present experimental measurements of carbon plasmas that display this anomalous dispersion phenomenon. It is shown that the average-atom calculation is a good approximation when the strongest lines dominate the dispersion. However, when weaker lines make a significant contribution, the more detailed calculations such as OPAL and CAK are essential. During the next decade X-ray free electron lasers and other X-ray sources will be available to probe a wider variety of plasmas at higher densities and shorter wavelengths so understanding the index of refraction in plasmas will be even more essential. With the advent of tunable X-ray lasers the frequency-dependent interferometer measurements of the index of refraction may enable us to determine the absorption coefficients and lineshapes and make detailed comparisons against our atomic physics codes.     

Temporal and spectral behavior of sub-picosecond laser-created X-ray sources from low- to moderate-Z elements

We report on a set of experiments in which solid targets of different atomic numbers (Z) were irradiated with laser pulses of time durations ranging from 300 fs to 33 ps, and energies up to 26 J. The time-resolved X-ray emission in the 7.6–8.1 Å spectral range was measured using an ultra-fast X-ray streak camera coupled with a conical Bragg crystal. In this way we were able to follow the dramatic modification of the spectral features as a function of the laser duration. The features evolve from a “ns-type” emission, characterized by narrow and well-defined spectral lines, to very broad spectral features, due not only to the Stark broadening but also to the proliferation of satellites lines. The measured spectra also show strong time dependence, which allows us to follow the time evolution of the hydrodynamic parameters. We then compare the derived parameter with the CHIVAS hydro-radiative simulations. The experimental results are also compared with the AVERROES/TRANSPEC collisional-radiative code, and with precise spectral line shape calculations (PPP and PrismSPECT). The results seem to indicate regimes of interaction where hot electrons play an important role on spectral line formation.     

Bow shocks formed by plasma collisions in laser irradiated semi-cylindrical cavities

The formation of shocks in plasmas created by short pulse laser irradiation (λ = 800 nm, I ≈ 1 × 10¹² W cm^?2) of semi-cylindrical cavities of different materials was studied combining visible and soft X-ray laser interferometry with simulations. The plasma rapidly converges near the axis to form a dense bright plasma focus. Later in time a long lasting bow shock is observed to develop outside the cavity, that is shown to arise from the collision of plasmas originating from within the cavity and the surrounding flat walls of the target. The shock is sustained for tens of nanoseconds by the continuous arrival of plasma ablated from the target walls. The plasmas created from the heavier target materials evolve more slowly, resulting in increased shock lifetimes.     

Isochoric heating of reduced mass targets by ultra-intense laser produced relativistic electrons

We present measurements of the chlorine K-alpha emission from reduced mass targets, irradiated with ultra-high intensity laser pulses. Chlorinated plastic targets with diameters down to 50 μm and mass of a few 10^?8 g were irradiated with up to 7 J of laser energy focused to intensities of several 10¹⁹ W/cm². The conversion of laser energy to K-alpha radiation is measured, and high-resolution spectra that allow observation of line shifts are observed, indicating isochoric heating of the target up to 18 eV. A zero-dimensional 2-temperature equilibration model, combined with electron impact K-shell ionization and post processed spectra from collisional radiative calculations reproduces the observed K-alpha yields and line shifts, and shows the importance of target expansion due to the hot electron pressure.     

Fabrication of nano-sized Ca(OH)2 with excellent adsorption ability for N2O4

Uniform nano-sized calcium hydroxide (Ca(OH)₂) monocrystal powder was synthesized from calcium oxide in a surfactant solution via a digestion method by decreasing the surface tension of the reaction system to control the growth of crystalline Ca(OH)₂. The Ca(OH)₂ monocrystal powder samples were characterized by means of scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), and Fourier transform-infrared spectroscopy (FT-IR). The NO_x adsorption ability of the samples was evaluated, and the influence of various types and concentrations of surfactants on powder agglomeration and then the specific surface area in the precipitation process were studied. The specific surface area of the samples was found as high as 58 m²/g and 92 m²/g and the particle size, 300–400 nm and 200–300 nm in the presence of 10 wt% PEG600 and 0.086 mL/L SDS at a reaction time of 5 h, respectively. The product has an exceptionally strong adsorption ability for NO_x, which makes it a highly promising adsorbent for emission control and air purification.     

Plasma emission spectroscopy of solids irradiated by intense XUV pulses from a free electron laser

The FLASH XUV-free electron laser has been used to irradiate solid samples at intensities of the order 10¹⁶ W cm^?2 at a wavelength of 13.5 nm. The subsequent time integrated XUV emission was observed with a grating spectrometer. The electron temperature inferred from plasma line ratios was in the range 5–8 eV with electron density in the range 10²¹–10²² cm^?3. These results are consistent with the saturation of absorption through bleaching of the L-edge by intense photo-absorption reported in an earlier publication.     

Solvent-less synthesis of zinc oxide nanostructures from Zn(salen) as precursor and their optical properties

ZnO nanoparticles, 10–20 nm in size, were synthesized by heat treatment in air at 500 °C for 5 h., using [N,N′-bis(salicylaldehydo) ethylene diamine]zinc(II), i.e., Zn(salen), as precursor, which was obtained by a solvent-free solid–solid reaction. Heat-treated products were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, and transmission electron microscopy. Room temperature photoluminescence spectra of ZnO nanostructures are dominated by green emission attributed to oxygen vacancy related donor–acceptor transition.     

Diagnosing laser-driven,shock-heated foam target with Al absorption spectroscopy on OMEGA EP

Results on diagnoses of laser-driven, shock-heated foam plasma with time-resolved Al 1s-2p absorption spectroscopy are reported. Experiments were carried out to produce a platform for the study of relativistic electron transport. In cone-guided Fast Ignition (FI), relativistic electrons generated by a high-intensity, short-pulse igniter beam must be transported through a cone tip to an imploded core. Transport of the energetic electrons could be significantly affected by the temperature-dependent resistivity of background plasmas. The experiment was conducted using four UV beams of the OMEGA EP laser at the Laboratory For Laser Energetics. One UV beam (1.2 kJ, 3.5 ns square) was used to launch a shock wave into a foam package target, consisting of 200 mg/cm³ CH foam with aluminum dopant and a solid plastic container surrounding the foam layer. The other three UV beams with the total energy of 3.2 kJ in 2.5 ns pulse duration were tightly focused onto a Sm dot target to produce a point X-ray source in the energy range of 1.4–1.6 keV. The quasi-continuous X ray signal was transmitted through the shock-heated Al-doped, foam layer and recorded with an X-ray streak camera. The measured 1s-2p Al absorption features were analyzed using an atomic physics code FLYCHK. Electron temperature of 40 eV inferred from the spectral analysis is consistent with 2-D DRACO Radiation-hydrodynamic simulations.     

Hydrothermal preparation of nanocrystalline ZnO2

A green hydrothermal method was proposed for the synthesis of nanocrystalline ZnO₂, using Zn₅(CO₃)₂(OH)₆ powder and 6 vol% H₂O₂ aqueous solution as the starting materials. Characterization results from X-ray diffraction, Raman, high resolution transmission electron microscopy and selected area electron diffraction revealed that the products synthesized at 80–120 °C for 6–18 h were pure cubic phase ZnO₂ nanocrystals. Room temperature photoluminescence spectra of the as-synthesized ZnO₂ nanocrystals displayed a wide and strong emission band in the visible region of about 525–570 nm upon laser excitation at 325 nm, which may have originated from their surface state and other crystal defects.     

Measurements of emission spectra from hot,dense germanium plasma in short pulse laser experiments

Heating of thin foil targets by an high power laser at intensities of 10¹⁷–10¹⁹ W/cm² has been studied as a method for producing high temperature, high density samples to investigate X-ray opacity and equation of state. The targets were plastic (parylene-N) foils with a microdot made of a mixture of germanium and titanium buried at depth of 1.5 μm. The L-shell spectra from the germanium and the K-shell spectra from the titanium were taken using crystal spectrometers recording onto film and an ultra fast X-ray streak camera coupled to a conical focussing crystal with a time resolution of 1 ps. The conditions in the microdot were inferred by comparing the measured spectra to synthetic spectra produced by the time-dependent collisional–radiative (CR) models FLY and FLYCHK. The data were also compared to simulated spectra from a number of opacity codes assuming local thermodynamic equilibrium (LTE). Temperature and density gradients were taken into account in the comparisons. The sample conditions were inferred from the CR modelling using FLYCHK to be 800 ± 100 eV and 1.5 ± 0.5 g/cc. The best fit to the LTE models was at a temperature 20% lower than with the CR model. Though the sample departs from LTE significantly useful spectral comparisons can still be made. The results and comparisons are discussed along with improvements to the experimental technique to achieve conditions closer to LTE.     

Hard X-ray spectroscopy of inner-shell K transitions generated by MeV electron propagation from intense picosecond laser focal spots

The propagation of energetic electrons from the focal spots of intense picosecond laser pulses was studied using targets consisting of planar foils and fine metal wires. High-resolution K-shell spectra of elements with atomic numbers in the range 46–74 (Pd to W) and with energies from 21 keV to 69 keV were recorded by a Cauchois-type spectrometer using a curved transmission crystal. The K-shell spectra resulted from the collisional ionization of 1 s electrons by energetic electrons that were generated in the laser focal spot and propagated into the planar foil region beyond the focal spot or into the metal wires adjacent to an irradiated wire. The lateral spread of the energetic electrons from the focal spot was determined from the source broadening of the K spectral lines and from the relative intensities of the K spectra from an irradiated wire and neighboring wires of different metals. The propagation distances up to 1 mm in a variety of materials indicated electron energies up to 1 MeV were generated in the laser focal spot. Inhibited propagation in an electrically insulating material was observed that results from a weak return current and incomplete space charge neutralization.     

Microwave-hydrothermal preparation of a graphene/hierarchy structure MnO2 composite for a supercapacitor

Graphene/hierarchy structure manganese dioxide (GN/MnO₂) composites were synthesized using a simple microwave-hydrothermal method. The properties of the prepared composites were analyzed using field emission scanning electron microscopy (FE-SEM), X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) measurements. The electrochemical performances of the composites were analyzed using cyclic voltammetry, electrochemical impedance spectrometry (EIS), and chronopotentiometry. The results showed that GN/MnO₂ (10 wt% graphene) displayed a specific capacitance of 244 F/g at a current density of 100 mA/g. An excellent cyclic stability was obtained with a capacity retention of approximately 94.3% after 500 cycles in a 1 mol/L Li₂SO₄ solution. The improved electrochemical performance is attributed to the hierarchy structure of the manganese dioxide, which can enlarge the interface between the active materials and the electrolyte. The preparation route provides a new approach for hierarchy structure graphene composites; this work could be readily extended to the preparation of other graphene-based composites with different structures for use in energy storage devices.     

Low-frequency conductivity in the average-atom approximation

The quantum-mechanical average-atom model is reviewed and applied to determine scattering phase shifts, mean-free paths, and relaxation times in warm-dense plasmas. Static conductivities σ are based on an average-atom version of the Ziman formula. Applying linear response to the average-atom model leads to an average-atom version of the Kubo–Greenwood formula for the frequency-dependent conductivity σ(ω). The free–free contribution to σ(ω) is found to diverge as 1/ω² at low frequencies; however, considering effects of multiple scattering leads to a modified version of σ(ω) that is finite and reduces to the Ziman formula at ω = 0. The resulting average-atom version of the Kubo–Greenwood formula satisfies the conductivity sum rule. The dielectric function ε(ω) and the complex index of refraction n(ω) + iκ(ω) are inferred from σ(ω) using dispersion relations. Applications to anomalous dispersion in laser-produced plasmas are discussed.     

Observation and analysis of near-surface atmospheric aerosol optical properties in urban Beijing

Year-round measurements of the mass concentration and optical properties of fine aerosols (PM_2.5) from June 2009 to May 2010 at an urban site in Beijing were analyzed. The annual mean values of the PM_2.5 mass concentration, absorption coefficient (Ab), scattering coefficient (Sc) and single scattering albedo (SSA) at 525 nm were 67 ± 66 μg/m³, 64 ± 62 Mm⁻¹, 360 ± 405 Mm⁻¹ and 0.82 ± 0.09, respectively. The bulk mass absorption efficiency and scattering efficiency of the PM_2.5 at 525 nm were 0.78 m²/g and 5.55 m²/g, respectively. The Ab and Sc showed a similar diurnal variation with a maximum at night and a minimum in the afternoon, whereas SSA displayed an opposite diurnal pattern. Significant increases in the Ab and Sc were observed in pollution episodes caused by the accumulation of pollutants from both local and regional sources under unfavorable weather conditions. Aerosol loadings in dust events increased by several times in the spring, which had limited effects on the Ab and Sc due to the low absorption and scattering efficiency of dust particles. The frequency of haze days was the highest in autumn because of the high aerosol absorption and scattering under unfavorable weather conditions. The daily PM_2.5 concentration should be controlled to a level lower than 64 μg/m³ to prevent the occurrence of haze days according to its exponentially decreased relationship with visibility.     

X-ray spectral measurements and collisional-radiative modeling of hot,gold plasmas at the omega laser

M-Band and L-Band Gold spectra between 3 and 5 keV and 8 and 13 keV, respectively, have been recorded by a photometrically calibrated crystal spectrometer. The spectra were emitted from the plasma in the laser deposition region of a ‘hot hohlraum’. This is a reduced-scale hohlraum heated with ≈9 kJ of 351 nm light in a 1 ns square pulse at the OMEGA laser. The space- and time-integrated spectra included L-Band line emission from Co-like to Ne-like gold. The three L-Band line features were identified to be the 3s → 2p, 3d_5/2 → 2p_3/2 and 3d_3/2 → 2p_1/2 transitions at ≈9 keV, ≈10 keV and ≈13 keV, respectively. M-Band 5f → 3d, 4d → 3p, and 4p → 3s transition features from Fe-like to P-like gold were also recorded between 3 and 5 keV. Modeling from the radiation–hydrodynamics code LASNEX, the collisional-radiative codes FLYCHK and SCRAM, and the atomic structure code FAC were used to model the plasma and generate simulated spectra for comparison with the recorded spectra. Through these comparisons, we have determined the average electron temperature of the emitting plasma to be between 6.0 and 6.5 keV. The electron temperatures predicted by LASNEX appear to be too large by a factor of about 1.5.     

Fourier analysis of X-ray micro-diffraction profiles to characterize laser shock peened metals

X-ray micro-diffraction profiles using a synchrotron light source were analyzed via Fourier transformation for single crystal Aluminum and Copper samples subjected to micro-scale laser shock peening. Specifically, the asymmetric and broadened diffraction profiles registered across the shock peen region were observed and analyzed by classic Warren and Averbach (W–A) method [Warren, B.E., Averbach, B.L., 1950. The effect of cold-work distortion on X-ray patterns. Journal of Applied Physics 21, 595–599] and modified W–A method [Ungar, T., Borbely, A., 1996. The effect of dislocation contrast on X-ray line broadening: A new approach to line profile analysis. Applied Physics Letters 69, 3173–3175]. Average strain deviation, mosaic size and dislocation density were estimated for the first time with a spatial resolution of 5 μm. The results compare well with the simulation results obtained from FEM analysis and from electron backscatter diffraction (EBSD) measurements. Differences in response caused by different materials and crystalline orientations (1 1 0 and 0 0 1) were also studied.     

Preparation and electrochemical performance of carbon-coated LiFePO4/LiMnPO4-positive material for a Li-ion battery

Lithium iron phosphate (LiFePO₄)/lithium manganese phosphate (LiMnPO₄)-positive material was successfully prepared through ball milling and high-temperature sintering using manganese acetate, lithium hydroxide, ammonium dihydrogen phosphate, and ferrous oxalate as raw materials. The as-prepared samples were characterized by X-ray diffraction, transmission electron microscopy, scanning electron microscopy, a constant current charge–discharge test, cyclic voltammetry, and electrochemical impedance spectroscopy. The effects of lithium iron phosphate coating were also discussed. Because of its special core–shell structure, the as-prepared LiMn_0.7Fe_0.3PO₄–LiFePO₄–C exhibits excellent electrochemical performance. The discharge capacity reached 136.6 mAh/g and the specific discharge energy reached 506.9 Wh/kg at a rate of 0.1 C.     

Microwave-assisted polyol synthesis of LiMnPO4/C and its use as a cathode material in lithium-ion batteries

We synthesized LiMnPO₄/C with an ordered olivine structure by using a microwave-assisted polyol process in 2:15 (v/v) water–diethylene glycol mixed solvents at 130 °C for 30 min. We also studied how three surfactants—hexadecyltrimethylammonium bromide, polyvinylpyrrolidone k30 (PVPk30), and polyvinylpyrrolidone k90 (PVPk90)—affected the structure, morphology, and performance of the prepared samples, characterizing them by using X-ray diffraction, scanning electron microscopy, transmission electron microscopy, charge/discharge tests, and electrochemical impedance spectroscopy. All the samples prepared with or without surfactant had orthorhombic structures with the Pnmb space group. Surfactant molecules may have acted as crystal-face inhibitors to adjust the oriented growth, morphology, and particle size of LiMnPO₄. The microwave effects could accelerate the reaction and nucleation rates of LiMnPO₄ at a lower reaction temperature. The LiMnPO₄/C sample prepared with PVPk30 exhibited a flaky structure coated with a carbon layer (∼2 nm thick), and it delivered a discharge capacity of 126 mAh/g with a capacity retention ratio of ∼99.9% after 50 cycles at 1C. Even at 5C, this sample still had a high discharge capacity of 110 mAh/g, demonstrating good rate performance and cycle performance. The improved performance of LiMnPO₄ likely came from its nanoflake structure and the thin carbon layer coating its LiMnPO₄ particles. Compared with the conventional polyol method, the microwave-assisted polyol method had a much lower reaction time.     

Effects of multi-dopants (Zn and Ho) in stabilizing spinel structure for cathode materials in lithium rechargeable batteries—Novel chelated sol–gel synthesis

Multi-doped spinels, namely LiMn₂O₄ and LiZn_xHo_yMn_2−x−yO₄ (x = 0.10–0.18; y = 0.02–0.10), for use as cathode materials for lithium-ion rechargeable batteries were synthesized via sol–gel method, using lauric acid as the chelating agent, to obtain micron-sized particles. The physical properties of the synthesized samples were investigated using differential thermal analysis, Fourier-transform infrared spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy, energy-dispersive X-ray analysis, and electrochemical methods. XRD showed that LiMn₂O₄ and LiZn_xHo_yMn_2−x−yO₄ have high degrees of crystallinity and good phase purities. The SEM images of LiMn₂O₄ showed an ice-cube morphology with particles of size 1 μm. Charge–discharge studies showed that undoped LiMn₂O₄ delivered the discharge capacity of 124 mA h/g with coulombic efficiency of 95% during the first cycle, whereas doped spinels delivered discharge capacities of 125, 120, and 127 mA h/g in the first cycle with coulombic efficiencies of 96%, 91%, and 91%, respectively.