Novel Methods for Binding Disparate Materials

This project was intended to advance the science of surface bonding in order to provide the functionality demanded by target fabrication requirements, as well as similar needs in other fields of importance to LLNL. We have developed and demonstrated a very powerful capability, i.e. 'single molecule force spectroscopy', that allows the strength of individual chemical bonds to be measured. This project focused on long chain molecules that are covalently bound to surfaces on one end and have complementary reactive groups that have the potential for bridging between surfaces. In biological systems, long chain tethers provide the mechanism for adhesion between dissimilar surfaces, e.g. bacteria adhesion to cells, and were found useful for developing the methodology. Polymer tethers offer the means to bridge across finite surface roughness and have the potential of forming thin, well-characterized bonds on a variety of surfaces

Current density inhomogeneity throughout the thickness of superconducting films and its effect on their irreversible magnetic properties

We calculate the distribution of the current density $j$ in superconducting films along the direction of an external field applied perpendicular to the film plane. Our analysis reveals that in the presence of bulk pinning $j$ is inhomogeneous on a length scale of order the inter vortex distance. This inhomogeneity is significantly enhanced in the presence of surface pinning. We introduce new critical state model, which takes into account the current density variations throughout the film thickness, and show how these variations give rise to the experimentally observed thickness dependence of $$ and magnetic relaxation rate.Comment: RevTex, 9 PS figures. To appear in Phys. Rev.

Electrical Resistivity and Thermal Expansion Measurements of URu2Si2 under Pressure

We carried out simultaneous measurements of electrical resistivity and thermal expansion of the heavy-fermion compound URu2Si2 under pressure using a single crystal. We observed a phase transition anomaly between hidden (HO) and antiferromagnetic (AFM) ordered states at TM in the temperature dependence of both measurements. For the electrical resistivity, the anomaly at TM was very small compared with the distinct hump anomaly at the phase transition temperature T0 between the paramagnetic state (PM) and HO, and exhibited only a slight increase and decrease for the I // a-axis and c-axis, respectively. We estimated each excitation gap of HO, Delta_HO, and AFM, Delta_AFM, from the temperature dependence of electrical resistivity; Delta_HO and Delta_AFM have different pressure dependences from each other. On the other hand, the temperature dependence of thermal expansion exhibited a small anomaly at T0 and a large anomaly at TM. The pressure dependence of the phase boundaries of T0 and TM indicates that there is no critical end point and the two phase boundaries meet at the critical point.Comment: 4 pages, 4 figure

Nonlinearly Additive Forces in Multivalent Ligand Binding to a Single Protein Revealed with Force Spectroscopy

We present evidence of multivalent interactions between a single protein molecule and multiple carbohydrates at a pH where the protein can bind four ligands. The evidence is based not only on measurements of the force required to rupture the bonds formed between ConcanavalinA (ConA) and {alpha}-D-mannose, but also on an analysis of the polymer-extension force curves to infer the polymer architecture that binds the protein to the cantilever and the ligands to the substrate. We find that although the rupture forces for multiple carbohydrate connections to a single protein are larger than the rupture force for a single connection, they do not scale additively with increasing number. Specifically, the most common rupture forces are approximately 46, 66, and 85 pN, which we argue corresponds to 1, 2, and 3 ligands being pulled simultaneously from a single protein as corroborated by an analysis of the linkage architecture. As in our previous work polymer tethers allow us to discriminate between specific and non-specific binding. We analyze the binding configuration (i.e. serial versus parallel connections) through fitting the polymer stretching data with modified Worm-Like Chain (WLC) models that predict how the effective stiffness of the tethers is affected by multiple connections. This analysis establishes that the forces we measure are due to single proteins interacting with multiple ligands, the first force spectroscopy study that establishes single-molecule multivalent binding unambiguously

Pinning of spiral fluxons by giant screw dislocations in YBa_2Cu_3O_7 single crystals: Josephson analog of the fishtail effect

By using a highly sensitive homemade AC magnetic susceptibility technique, the magnetic flux penetration has been measured in YBa_2Cu_3O_7 single crystals with giant screw dislocations (having the structure of the Archimedean spirals) exhibiting a=3 spiral turnings, the pitch b=18.7 microns and the step height c=1.2nm (the last parameter is responsible for creation of extended weak-link structure around the giant defects). The magnetic field applied parallel to the surface enters winding around the weak-link regions of the screw in the form of the so-called spiral Josephson fluxons characterized by the temperature dependent pitch b_f(T). For a given temperature, a stabilization of the fluxon structure occurs when b_f(T) matches b (meaning an optimal pinning by the screw dislocations) and manifests itself as a pronounced low-field peak in the dependence of the susceptibility on magnetic field (applied normally to the surface) in the form resembling the high-field (Abrikosov) fishtail effect.Comment: see also http://www.jetpletters.ac.ru/ps/1886/article_28701.shtm

Neutron Scattering Study on Competition between Hidden Order and Antiferromagnetism in U(Ru_{1-x}Rh_x)_2Si_2 (x <= 0.05)

We have performed elastic and inelastic neutron scattering experiments on the solid solutions U(Ru_{1-x}Rh_x)_2Si_2 for the Ru rich concentrations: x=0, 0.01, 0.02, 0.025, 0.03, 0.04 and 0.05. Hidden order is suppressed with increasing x, and correspondingly the onset temperature T_m (~ 17.5 K at x=0) of weak antiferromagnetic (AF) Bragg reflection decreases. For x=0.04 and 0.05, no magnetic order is detected in the investigated temperature range down to 1.4 K. In the middle range, 0.02 <= x <= 0.03, we found that the AF Bragg reflection is strongly enhanced. At x=0.02, this takes place at ~ 7.7 K (=T_M), which is significantly lower than T_m (~ 13.7 K). T_M increases with increasing x, and seems to merge with T_m at x=0.03. If the AF state is assumed to be homogeneous, the staggered moment \mu_o estimated at 1.4 K increases from 0.02(2) \mu_B/U (x=0) to 0.24(1) \mu_B/U (x=0.02). The behavior is similar to that observed under hydrostatic pressure (\mu_o increases to ~ 0.25 \mu_B/U at 1.0 GPa), suggesting that the AF evolution induced by Rh doping is due to an increase in the AF volume fraction. We also found that the magnetic excitation observed at Q=(1,0,0) below T_m disappears as T is lowered below T_M.Comment: 4 pages, 4 figures, submitted to J. Phys. Soc. Jp

Effect of Pressure on Tiny Antiferromagnetic Moment in the Heavy-Electron Compound URu_2Si_2

We have performed elastic neutron-scattering experiments on the heavy-electron compound URu_2Si_2 for pressure P up to 2.8 GPa. We have found that the antiferrmagnetic (100) Bragg reflection below T_m ~ 17.5 K is strongly enhanced by applying pressure. For P < 1.1 GPa, the staggered moment mu_o at 1.4 K increases linearly from ~ 0.017(3) mu_B to ~ 0.25(2) mu_B, while T_m increases slightly at a rate ~ 1 K/GPa, roughly following the transition temperature T_o determined from macroscopic anomalies. We have also observed a sharp phase transition at P_c ~ 1.5 GPa, above which a 3D-Ising type of antiferromagnetic phase (mu_o ~ 0.4 mu_B) appears with a slightly reduced lattice constant.Comment: RevTeX, 4 pages, 4 eps figures, accepted for publication in Phys. Rev. Let

Fabrication of Beryllium Capsules with Copper-Doped Layers for NIF Targets: A Progress Report

The sputtering of beryllium (Be) has been used at LLNL for nearly 30 years in the fabrication of laser targets. Several years ago the prospect of using sputtering to fabricate spherical Be capsules for National Ignition Facility (NIF) targets began to be explored and a basic strategy was developed that involved sputtering down onto plastic mandrels bouncing in a pan. While this appears to be very straightforward in principle, in practice sputtering has been used almost exclusively to make thin films (&lt; 1 micron) on flat substrates. Thick films pose a significant challenge for sputtering while materials on spherical substrates are essentially unexplored. More recently, based on computational results, the point design for the first NIF ignition target capsule was specified as a Be capsule with Cu-doped layers of specific thickness, each layer with a different concentration of copper. While the work described here was motivated by the need to make the layered capsules, the primary progress on Be capsules has been the development of a more complete metallurgical understanding of the materials that are fabricated and the beginning of the exploration of the relationship between the sputter processing and microstructure of these spherical samples. At least two barriers to growth to full thickness (i.e. 170 microns) have been identified and efforts to overcome these barriers are underway

Point-contact spectroscopy on URu2_2Si2_2

Tunnel and point contact experiments have been made in a URu$_2$Si$_2$ single crystal along the c-axis. The experiments were performed changing temperature and contact size in a low temperature scanning tunneling microscope. A resonance develops at the Fermi level at $T\sim 60$ K. This resonance splits and becomes asymmetric when the 17.5 K phase transition is crossed. These results are consistent with the existence of Kondo like bound states of the U$^{4+}$ ionic configurations and the conduction electrons. Below the transition, these configurations are split by the development of quadrupolar ordering. The peak separation can be interpreted as a direct measurement of the order parameter. Measurements on a policrystalline UAu_2Si_2$ sample are also reported, with a comparative study of the behavior of both materials.Comment: 4 pages (Latex) + 2 postscript figure