Lattice dielectric response of CdCu{3}Ti{4}O{12} and of CaCu{3}Ti{4}O{12} from first principles

Structural, vibrational, and lattice dielectric properties of CdCu{3}Ti{4}O{12} are studied using density-functional theory within the local spin-density approximation, and the results are compared with those computed previously for CaCu{3}Ti{4}O{12}. Replacing Ca with Cd is found to leave many calculated quantities largely unaltered, although significant differences do emerge in zone-center optical phonon frequencies and mode effective charges. The computed phonon frequencies of CdCu{3}Ti{4}O{12} are found to be in excellent agreement with experiment, and the computed lattice contribution to the intrinsic static dielectric constant (~60) also agrees exceptionally well with a recent optical absorption experiment. These results provide further support for a picture in which the lattice dielectric response is essentially conventional, suggesting an extrinsic origin for the anomalous low-frequency dielectric response recently observed in both materials.Comment: 5 pages; uses REVTEX macros. Also available at http://www.physics.rutgers.edu/~dhv/preprints/lh_cdct/index.htm

The 2-Channel Kondo Model I: Review of Experimental Evidence for its Realization in Metal Nanoconstrictions

Certain zero-bias anomalies (ZBAs) in the voltage, temperature and magnetic field dependence of the conductance $G(V,T,H)$ of quenched Cu point contacts have previously been interpreted to be due to non-magnetic 2-channel Kondo (2CK) scattering from near-degenerate atomic two-level tunneling systems (Ralph and Buhrman, 1992; Ralph et al. 1994), and hence to represent an experimental realization of the non-Fermi-liquid physics of the T=0 fixed point of the 2-channel Kondo model. In this, the first in a series of three papers (I,II,III) devoted to 2-channel Kondo physics, we present a comprehensive review of the quenched Cu ZBA experiments and their 2CK interpretation, including new results on ZBAs in constrictions made from Ti or from metallic glasses. We first review the evidence that the ZBAs are due to electron scattering from stuctural defects that are not static, but possess internal dynamics. In order to distinguish between several mechanisms proposed to explain the experiments, we then analyze the scaling properties of the conductance at low temperature and voltage and extract from the data a universal scaling function $\Gamma(v)$. The theoretical calculation of the corresponding scaling function within the 2CK model is the subject of papers II and III. The main conclusion of our work is that the properties of the ZBAs, and most notably their scaling behavior, are in good agreement with the 2CK model and clearly different from several other proposed mechanisms.Comment: 35 pages RevTeX, 19 encapsulated postscript figures; this final published version features two additional authors, an additional section reviewing recent experiments on Ti nanoconstrictions that agree very well with the 2-channel Kondo model, 6 new figures (and is much shorter the previous 53 page version, due to reformatting

Use of the Generalized Gradient Approximation in Pseudopotential Calculations of Solids

We present a study of the equilibrium properties of $sp$-bonded solids within the pseudopotential approach, employing recently proposed generalized gradient approximation (GGA) exchange correlation functionals. We analyze the effects of the gradient corrections on the behavior of the pseudopotentials and discuss possible approaches for constructing pseudopotentials self-consistently in the context of gradient corrected functionals. The calculated equilibrium properties of solids using the GGA functionals are compared to the ones obtained through the local density approximation (LDA) and to experimental data. A significant improvement over the LDA results is achieved with the use of the GGA functionals for cohesive energies. For the lattice constant, the same accuracy as in LDA can be obtained when the nonlinear coupling between core and valence electrons introduced by the exchange correlation functionals is properly taken into account. However, GGA functionals give bulk moduli that are too small compared to experiment.Comment: 15 pages, latex, no figure

Redox-driven changes in porewater chemistry in the unsaturated zone of the chalk aquifer beneath unlined cattle slurry lagoons

Farm waste stores such as cattle slurry lagoons are widespread in the UK and many overly important aquifers. Stores can be serious risks to water quality because they are important sources of N species, organic C and pathogenic microbes. At two sites on the Chalk aquifer of southern England, inclined boreholes were drilled and cored to obtain aquifer material from directly beneath unlined slurry stores. Vertical boreholes were also drilled adjacent to the slurry stores to determine any lateral movement of contaminants. Interstitial porewaters were analysed for major and minor ions and S isotopes. At the second site, unsaturated zone gases were sampled from the inclined hole. Infiltration of slurry into the unsaturated zone caused significantly elevated concentrations of metals such as Cu and Ni at both sites. Sulphate reduction was occurring at Site 1, as evidenced by SO4 concentrations decreasing from 150 to 50 mg/l and enhanced ratios of delta(34)S-SO4 and delta(18)O-SO4. Ammomum-N also leaches along with dissolved organic C which were found 17 m below ground surface at concentrations up to 400 and 260 mg/l, respectively. Contaminant concentrations were similar in the porewaters from both the inclined and vertical boreholes. At Site 2, higher contaminant concentrations were found in the inclined borehole compared with the vertical borehole. Organic C concentrations were considerably lower than at Site 1, ranging from 10 to 70 mg/l. Ammonium-N concentrations reached a maximum concentration of 25 mg/l. however NO3-N concentrations were up to 500 mg/l and SO4 concentrations were generally higher than Site 1. Data for N-2/Ar and delta(15)N-N-2 from the gas samplers show a peak of 102 and 2.2parts per thousand, respectively. at 14 m below ground level indicating denitrification was taking place. Evidence from delta(34)S- SO4 and delta(18)O-SO4 suggest that some SO4 reduction was taking place simultaneously. From CH4 and NH3 detected at depth it is suggested that slurry contamination. emanating from early use of the store, has passed through the top 18 m of the unsaturated zone at Site 2. The presence of high concentrations of NO3 and lower concentrations of organic C suggests that this lagoon has formed a relatively impermeable seal at its base within the first few years of its lifetime. The anoxic conditions at both sites may have mobilised U from N-P-K fertilisers. Both sites are continuing to impact on the porewater chemistry and pose a risk of groundwater contamination