0000000000185422
AUTHOR
H. J. Schöpe
A compact apparatus for mass selective resonance ionization spectroscopy in a buffer gas cell
Abstract An ultra-sensitive laser spectroscopic method for the investigation of transuranium nuclides has been developed based on resonance ionization in an argon buffer gas cell. This method has been combined with ion-guide extraction and mass selective direct detection of the resonantly ionized atoms. Using argon as a buffer gas, recoils of fusion reactions can be thermalized even at low pressure. The differential pumping system consists of only one roots pump and two turbo molecular pumps. The set-up has been tested with 243 Am evaporated from a filament located inside the optical gas cell. Resonance ionization is performed using a two-step excitation with an excimer-dye-laser combinatio…
Opaline Hydrogels: Polycrystalline Body-Centered-Cubic Bulk Material with an in Situ Variable Lattice Constant
Opaline hydrogels were produced as a polycrystalline bulk material with a body-centered-cubic (bcc) structure by immobilization of self-ordered charged colloidal particles crystallized under equilibrium conditions in a poly(acrylamide) matrix. The final size of a polycrystalline sample is about 7 cm3; a single crystal is up to several millimeters in length. The crystal size is tunable by varying the amount of photoinitiator and the hydrogel volume change due to swelling. The resulting photonic crystals are of high quality, showing high-order reflections. These hydrogels show a reversible shift of the diffraction Bragg peak wavelength depending on external conditions due to swelling or shrin…
Radiation detected resonance ionization spectroscopy on208Tl and242fAm
An ultra-sensitive laser spectroscopic method has been developed for the hyperfine spectroscopy of short-lived isotopes far off stability produced by heavy ion induced nuclear reactions at very weak intensity (> 1/s). It is based on resonance ionization spectroscopy in a buffer gas cell with radiation detection of the ionization process (RADRIS). As a first on-line application of RADRIS optical spectroscopy at242fAm fission isomers is in progress at the low target production rate of 10/s. The resonance ionization has been performed in two steps utilizing an excimer dye laser combination with a repetition rate of 300 Hz. The first resonant step proceeds through terms which correspond to wave…
Charged colloidal model systems under confinement in slit geometry: a new setup for optical microscopic studies.
A new experimental setup for optical microscopic studies of charged colloidal model systems under confinement between two flat walls is presented. The measurement cell consists of optically flat quartz substrates attached to piezo actuators. Those facilitate fast and flexible adjustment of the confining geometry. Optionally, the local cell height can be quantitatively controlled by in situ interferometric measurements. Proper choice of materials guarantees sufficient chemical inertia against contamination with salt ions. For efficient preparation of charged colloidal suspensions under strongly deionized conditions, the cell can be connected to a conventional pump circuit including a mixed b…
A Multipurpose Instrument To Measure the Vitreous Properties of Charged Colloidal Solids
We present a new high-precision light-scattering setup to study the properties of colloidal solids. It combines static light scattering, dynamic light scattering, and torsional resonance spectroscopy with a flexible and reliable preparational procedure. All three experiments can be performed quasi-simultaneously on the same mechanically undisturbed sample. Thus, unequivocal identification of glassy behavior in a comprehensive characterization dependent on interaction parameters becomes possible. A detailed description of the mechanics is given. We thoroughly tested the new apparatus on dilute colloidal samples and against commercial reference instruments. We performed a first systematic ser…
Optical experiments on a crystallizing hard-sphere–polymer mixture at coexistence
We report on the crystallization kinetics in an entropically attractive colloidal system using a combination of time resolved scattering methods and microscopy. Hard sphere particles are polystyrene microgels swollen in a good solvent (radius a=380nm, starting volume fraction 0.534) with the short ranged attractions induced by the presence of short polymer chains (radius of gyration rg = 3nm, starting volume fraction 0.0224). After crystallization, stacking faulted face centred cubic crystals coexist with about 5% of melt remaining in the grain boundaries. From the Bragg scattering signal we infer the amount of crystalline material, the average crystallite size and the number density of cry…
Crystal nucleation versus vitrification in charged colloidal suspensions
We investigated the solidification behaviour of thoroughly deionised aqueous suspensions of polystyrene latex spheres by various optical scattering methods. We found a dramatic increase in the nucleation rate densities with increasing particle number density. Crystalline and nanocrystalline samples showed two relaxation processes on widely separated time scales. For an index-matched suspension of perfluorinated particles an amorphous state was accessible with the glass-typical signature of frozen long-time relaxation. From our results we propose a route into the amorphous state different to that observed in hard-sphere suspensions. It seems that in charged-sphere systems the increased nucle…
Crystallization in suspensions of hard spheres: a Monte Carlo and molecular dynamics simulation study
The crystallization of a metastable melt is one of the most important non-equilibrium phenomena in condensed matter physics, and hard sphere colloidal model systems have been used for several decades to investigate this process by experimental observation and computer simulation. Nevertheless, there is still an unexplained discrepancy between the simulation data and experimental nucleation rate densities. In this paper we examine the nucleation process in hard spheres using molecular dynamics and Monte Carlo simulation. We show that the crystallization process is mediated by precursors of low orientational bond-order and that our simulation data fairly match the experimental data sets.
Charged colloidal particles in a charged wedge: do they go in or out?
Using real-space microscopy experiments, theory and computer simulation, we study the behaviour of highly charged colloidal particles which are confined between two highly charged plates forming a wedge geometry. Under low salt conditions it is experimentally observed that colloidal particles accumulate in the cusp of a wedge to form dense fluid or crystalline ordered structures. This behaviour is found for various cell geometries, salt concentrations and gravitational strengths, and even stays stable when additional convection is present in the system. An effort is made to understand this effect qualitatively on the basis of linear screening theory. For a single macro-ion, linear screening…
Residual order in amorphous dry films of polymer latices: indications of an influence of particle interaction
Abstract We report small angle X-ray scattering and atomic force microscopy measurements on macroscopically thick, dry films of polymer latex particles. While the surface of dried droplets has long range order due to layering effects, the overall bulk structure is amorphous. This holds for both low charge polymethylmetacrylate particles and for highly charged polystyrene particles with additional stabilisation with sodiumdodecylsurfate. In the latter case, however, considerable amounts of residual crystal-like order is observed.
Frustration of structural fluctuations upon equilibration of shear melts
Abstract We report on the formation of amorphous solids from aquaeous suspensions of charged colloidal spheres. Comprehensive light scattering and microscopic studies show that in these systems the nucleation rate density continuously increases to very high values. At the highest particle densities of 47.5 μm −3 (packing fraction Φ =0.146) an amorphous state is observed of only short range order, finite static shear modulus and frozen long time dynamics. This state is composed of a piling of––as we propose pre-critical––nuclei. Differences from the Hard Sphere case are discussed in some detail. There the arrest of density fluctuations is observed and described by Mode Coupling scenarios. In…
Crystalline multilayers of charged colloids in soft confinement: experiment versus theory.
We combine real-space experiments and lattice sum calculations to investigate the phase diagram of charged colloidal particles under soft confinement. In the experiments we explore the equilibrium phase diagram of charged colloidal spheres in aqueous suspensions confined between two parallel charged walls at low background salt concentrations. Motivated by the experiments, we perform lattice sum minimizations to predict the crystalline ground state of point-like Yukawa particles which are exposed to a soft confining wall potential. In the multilayered crystalline regime, we obtain good agreement between the experimental and numerical findings: upon increasing the density we recover the sequ…
Properties of mixed colloidal crystals
We prepared colloidal crystals from aqueous suspensions of spherical, charged polystyrene spheres under deionised conditions. Using a home-built multipurpose light scattering apparatus we measured the static structure factor, the static shear modulus and the intermediate scattering function. In addition we also monitored also the conductivity as a function of the composition and the particle number density. For the mixture investigated the data are well described assuming the formation of randomly substituted body-centered-cubic crystals.
Nucleation and crystal growth in a suspension of charged colloidal silica spheres with bi-modal size distribution studied by time-resolved ultra-small-angle X-ray scattering
A suspension of charged colloidal silica spheres exhibiting a bi-modal size distribution of particles, thereby mimicking a binary mixture, was studied using time-resolved ultra-small-angle synchrotron X-ray scattering (USAXS). The sample, consisting of particles of diameters d(A) = (104.7 ± 9.0) nm and d(B) = (88.1 ± 7.8) nm (d(A)/d(B) ≈ 1.2), and with an estimated composition A(0.6(1))B(0.4(1)), was studied with respect to its phase behaviour in dependance of particle number density and interaction, of which the latter was modulated by varying amounts of added base (NaOH). Moreover, its short-range order in the fluid state and its eventual solidification into a long-range ordered colloidal…
Observation of optical Smith-Purcell radiation at an electron beam energy of 855 MeV.
Smith-Purcell radiation, generated when a beam of charged particles passes close to the surface of a diffraction grating, has been studied in the visible spectral range at wavelengths of 360 and 546 nm with the low emittance 855 MeV electron beam of the Mainz Microtron MAMI. The beam focused to a spot size of $4 \ensuremath{\mu}\mathrm{m}$ (full width at half maximum) passed over optical diffraction gratings of echelle profiles with blaze angles of $0.8\ifmmode^\circ\else\textdegree\fi{}, 17.27\ifmmode^\circ\else\textdegree\fi{},$ and $41.12\ifmmode^\circ\else\textdegree\fi{}$ and grating periods of 0.833 and $9.09 \ensuremath{\mu}\mathrm{m}.$ Taking advantage of the specific emission chara…
An Improved Empirical Relation to Determine the Particle Number Density of Fluid-Like Ordered Charge-Stabilized Suspensions
Polystyrene as an archetypal charge-stabilized colloid model system was used in this work under well defined preparation conditions. A continuous preparation technique was used to control the suspension parameters salt concentration c and particle number density n. Measurements of n were performed using both conductivity in the completely deionized state and static light scattering. We found a significant deviation between the position of the first maximum of the static structure factor qmax=2π/L and an estimate identifying the relevant length scale L with the average inter-particle distance d¯=n−1/3. Instead, qmax was observed to follow the relation qmax=(2.20±0.03)π/d¯, which is equivalen…
Photoemission of spinpolarized electrons from strained GaAsP
Strained layer GaAs.95P.05 photo cathodes are presented, which emit electron beams spinpolarized to a degree of P = 75% typically. Quantum yields around QE = 0.4% are observed routinely. The figure of merit P2 × QE = 2.3 × 10−3 is comparable to that of the best strained layer cathodes reported in literature. The optimum wavelength of irradiating light around 830 nm is in convenient reach of Ti:sapphire lasers or diode lasers respectively. The cathodes are produced using MOCVD-techniques. A GaAs.55P.45-GaAs.85P.15 superlattice structure prevents the migration of dislocations from the substrate and bottom layers to the strained overlayer. The surface is protected by an arsenic layer so that n…
Qualitative characterisation of effective interactions of charged spheres on different levels of organisation using Alexander’s renormalised charge as reference
Abstract Effective interactions are conveniently determined from experimental or numerical data by fitting a Debye–Huckel potential with an effective charge Z ∗ and an effective electrolyte concentration c ∗ as free parameters. In this contribution we numerically solved the Poisson–Boltzmann equation to obtain the so-called renormalised charge Z PBC ∗ . For sufficiently large bare charge Z one finds a saturation of Z ∗ which scales as Z ∗ = A a / λ B , where a is the particle radius, λ B the Bjerrum length and A a proportionality factor of order (8–10). The saturation value increases with increased total micro-ion concentration and shows a shallow minimum as a function of packing fraction. …
Colloidal crystallization in the quasi-two-dimensional induced by electrolyte gradients.
We investigated driven crystal formation events in thin layers of sedimented colloidal particles under low salt conditions. Using optical microscopy, we observe particles in a thermodynamically stable colloidal fluid to move radially converging towards cation exchange resin fragments acting as seed particles. When the local particle concentration has become sufficiently large, subsequently crystallization occurs. Brownian dynamics simulations of a 2D system of purely repulsive point-like particles exposed to an attractive potential, yield strikingly similar scenarios, and kinetics of accumulation and micro-structure formation. This offers the possibility of flexibly designing and manufactur…
First observation of a resonance ionization signal on242mAm fission isomers
The feasibility of a hyperfine spectroscopy on242mAm fission isomers has been demonstrated at the low target production rate of 10/s. The experimental method employed is based on resonance ionization spectroscopy in a buffer gas cell with detection of the ionization process by means of the fission decay of the isomers. The resonance ionization has been performed in two steps, utilizing an excimer dye laser combination with a repetition rate of 300 Hz. The first resonant step proceeds through theJ=7/2 term at 21440.35 cm−1, which has been excited with the tuncable dye laser beam of a wavelength of 466.28 nm, the second non-resonant step is achieved with the 351 nm radiation of the excimer la…
Transition radiation in the x-ray region from a low emittance 855 MeV electron beam
A quasi-monochromatic hard x-ray beam with a photon energy of 33 keV has been produced from transition radiation (TR) at the Mainz Microtron MAMI. The radiator was a stack of 30 polyimide foils of 25 μm thickness and 75 μm separation and the monochromator a highly-oriented pyrolytic graphite crystal. The intrinsic bandwidth was measured with a critical absorption technique to be 100 eV. On the basis of these experiments a photon flux of 4⋅109/mm2s over an illuminated area of 5.7×125 mm2 can be expected from an optimized beryllium radiator at a beam current of 100 μA. At the K-absorption edge of titanium at 5 keV narrow band transition radiation has been observed from a stack of four foils o…