Nonempirical hyper-generalized-gradient functionals constructed from the Lieb-Oxford bound

A simple and completely general representation of the exact exchange-correlation functional of density-functional theory is derived from the universal Lieb-Oxford bound, which holds for any Coulomb-interacting system. This representation leads to an alternative point of view on popular hybrid functionals, providing a rationale for why they work and how they can be constructed. A similar representation of the exact correlation functional allows to construct fully nonempirical hyper-generalized-gradient approximations (HGGAs), radically departing from established paradigms of functional construction. Numerical tests of these HGGAs for atomic and molecular correlation energies and molecular atomization energies show that even simple HGGAs match or outperform state-of-the-art correlation functionals currently used in solid-state physics and quantum chemistry.

Lower Bounds on the Exchange-Correlation Energy in Reduced Dimensions

Bounds on the exchange-correlation energy of many-electron systems are derived and tested. By using universal scaling properties of the electron-electron interaction, we obtain the exponent of the bounds in three, two, one, and quasione dimensions. From the properties of the electron gas in the dilute regime, the tightest estimate to date is given for the numerical prefactor of the bound, which is crucial in practical applications. Numerical tests on various low-dimensional systems are in line with the bounds obtained and give evidence of an interesting dimensional crossover between two and one dimensions.

Limit on the diffuse flux of ultrahigh energy tau neutrinos with the surface detector of the Pierre Auger Observatory

Data collected at the Pierre Auger Observatory are used to establish an upper limit on the diffuse flux of tau neutrinos in the cosmic radiation. Earth-skimming nu(tau) may interact in the Earth's crust and produce a tau lepton by means of charged-current interactions. The tau lepton may emerge from the Earth and decay in the atmosphere to produce a nearly horizontal shower with a typical signature, a persistent electromagnetic component even at very large atmospheric depths. The search procedure to select events induced by tau decays against the background of normal showers induced by cosmic rays is described. The method used to compute the exposure for a detector continuously growing with time is detailed. Systematic uncertainties in the exposure from the detector, the analysis, and the involved physics are discussed. No tau neutrino candidates have been found. For neutrinos in the energy range 2x10(17) eV < E(nu)< 2x10(19) eV, assuming a diffuse spectrum of the form E(nu)(-2), data collected between 1 January 2004 and 30 April 2008 yield a 90% confidence-level upper limit of E(nu)(2)dN(nu tau)/dE(nu)< 9x10(-8) GeV cm(-2) s(-1) sr(-1).

Can quantum mechanics fool the cosmic censor?

We revisit the mechanism for violating the weak cosmic-censorship conjecture (WCCC) by overspinning a nearly-extreme charged black hole. The mechanism consists of an incoming massless neutral scalar particle, with low energy and large angular momentum, tunneling into the hole. We investigate the effect of the large angular momentum of the incoming particle on the background geometry and address recent claims that such a backreaction would invalidate the mechanism. We show that the large angular momentum of the incident particle does not constitute an obvious impediment to the success of the overspinning quantum mechanism, although the induced backreaction turns out to be essential to restoring the validity of the WCCC in the classical regime. These results seem to endorse the view that the ""cosmic censor"" may be oblivious to processes involving quantum effects.

Kondo screening regimes of a quantum dot with a single Mn ion

We study the Kondo and transport properties of a quantum dot with a single magnetic Mn ion connected to metallic leads. By employing a numerical renormalization group technique we show that depending on the value of ferromagnetic coupling strength between the local electronic spin and the magnetic moment of the Mn, two distinct Kondo regimes exist. In the weak-coupling limit, the system can be found in a completely screened Kondo state describing a local magnetic moment decoupled from the rest of the system. In contrast, in the strong-coupling regime the quantum dot spin and the local magnetic moment form a single large-spin entity partially Kondo screened. A crossover between these two regimes can be suitably tuned by varying the tunnel coupling between the quantum dot and the leads. The model investigated here is also suitable to study magnetic molecules adsorbed on a metallic surface. The rich phenomenology of these systems is reflected in the conductance across the system.

Energy transfer upconversion determination by thermal-lens and Z-scan techniques in Nd(3+)-doped laser materials

The Z-scan and thermal-lens techniques have been used to obtain the energy transfer upconversion parameter in Nd(3+)-doped materials. A comparison between these methods is done, showing that they are independent and provide similar results. Moreover, the advantages and applicability of each one are also discussed. The results point to these approaches as valuable alternative methods because of their sensitivity, which allows measurements to be performed in a pump-power regime without causing damage to the investigated material. (C) 2009 Optical Society of America

Partial magnetic ordering and crystal structure of the ludwigites Co(2)FeO(2)BO(3) and Ni(2)FeO(2)BO(3)

We present an extensive study of the structural, magnetic, and thermodynamic properties of the two heterometallic oxyborates: Co(2)FeO(2)BO(3) and Ni(2)FeO(2)BO(3). This has been carried out through x-ray diffraction at room temperature (RT) and 150 K, dc and ac magnetic susceptibilities, and specific-heat experiments in single crystals above 2 K. The magnetic properties of these iron ludwigites are discussed in comparison with those of the other two known homometallic ludwigites: Fe(3)O(2)BO(3) and Co(3)O(2)BO(3). In both ludwigites now studied we have found that the magnetic ordering of the Fe(3+) ions occurs at temperatures very near to which they order in Fe(3)O(2)BO(3). A freezing of the divalent ions (Co and Ni) is observed at lower temperatures. Our x-ray diffraction study of both ludwigites at RT and 150 K showed very small ionic disorder in apparent contrast with the freezing of the divalent ion spins. The structural transition that occurs in homometallic Fe(3)O(2)BO(3) has not been found in the present mixed ludwigites in the temperature range investigated.

Reverse engineering in many-body quantum physics: Correspondence between many-body systems and effective single-particle equations

The mapping, exact or approximate, of a many-body problem onto an effective single-body problem is one of the most widely used conceptual and computational tools of physics. Here, we propose and investigate the inverse map of effective approximate single-particle equations onto the corresponding many-particle system. This approach allows us to understand which interacting system a given single-particle approximation is actually describing, and how far this is from the original physical many-body system. We illustrate the resulting reverse engineering process by means of the Kohn-Sham equations of density-functional theory. In this application, our procedure sheds light on the nonlocality of the density-potential mapping of density-functional theory, and on the self-interaction error inherent in approximate density functionals.

Analytical results on Muller's ratchet effect in growing populations

Fontanari introduced [Phys. Rev. Lett. 91, 218101 (2003)] a model for studying Muller's ratchet phenomenon in growing asexual populations. They studied two situations, either including a death probability for each newborn or not, but were able to find analytical (recursive) expressions only in the no-decay case. In this Brief Report a branching process formalism is used to find recurrence equations that generalize the analytical results of the original paper besides confirming the interesting effects their simulations revealed.

Redetermination of 1-benzyl-3-furoyl-1-phenylthiourea

The title compound, C(19)H(16)N(2)O(2)S, was synthesized from furoyl isothiocyanate and N-benzylaniline in dry acetone and the structure redetermined. The structure [Otazo-Sanchez et al. (2001). J. Chem. Soc. Perkin Trans. 2, pp. 2211-2218] has been re-determined in order to establish the intramolecular and intermolecular interactions. The thiourea group is in the thioamide form. The thiourea group makes a dihedral angle of 29.2 (6)degrees with the furoyl group. In the crystal structure, molecules are linked by intermolecular C-H center dot center dot center dot O interactions, forming one-dimensional chains along the a axis. An intramolecular N-H center dot center dot center dot O hydrogen bond is also present.

Nonlinear refraction and absorption through phase transition in a Nd:SBN laser crystal

Time-resolved Z-scan measurements were performed in a Nd(3+)-doped Sr(0.61)Ba(0.39)Nb(2)O(6) laser crystal through ferroelectric phase transition. Both the differences in electronic polarizability (Delta alpha(p)) and cross section (Delta sigma) of the neodymium ions have been found to be strongly modified in the surroundings of the transition temperature. This observed unusual behavior is concluded to be caused by the remarkable influence that the structural changes associated to the ferro-to-paraelectric phase transition has on the 4f -> 5d transition probabilities. The maximum polarizability change value Delta alpha(p)=1.2x10(-25) cm(3) obtained at room temperature is the largest ever measured for a Nd(3+)-doped transparent material.

Physical signatures of discontinuities of the time-dependent exchange-correlation potential

The exact exchange-correlation (XC) potential in time-dependent density-functional theory (TDDFT) is known to develop steps and discontinuities upon change of the particle number in spatially confined regions or isolated subsystems. We demonstrate that the self-interaction corrected adiabatic local-density approximation for the XC potential has this property, using the example of electron loss of a model quantum well system. We then study the influence of the XC potential discontinuity in a real-time simulation of a dissociation process of an asymmetric double quantum well system, and show that it dramatically affects the population of the resulting isolated single quantum wells. This indicates the importance of a proper account of the discontinuities in TDDFT descriptions of ionization, dissociation or charge transfer processes.

Synergistic interaction between gold nanoparticles and nickel phthalocyanine in layer-by-layer (LbL) films: evidence of constitutional dynamic chemistry (CDC)

The concept of constitutional dynamic chemistry (CDC) based on the control of non-covalent interactions in supramolecular structures is promising for having a large impact on nanoscience and nanotechnology if adequate nanoscale manipulation methods are used. In this study, we demonstrate that the layer-by-layer (LbL) technique may be used to produce electroactive electrodes with ITO coated by tetrasulfonated nickel phthalocyanine (NiTsPc) alternated with poly(allylamine hydrochloride) (PAH) incorporating gold nanoparticles (AuNP), in which synergy has been achieved in the interaction between the nanoparticles and NiTsPc. The catalytic activity toward hydrogen peroxide (H(2)O(2)) in multilayer films was investigated using cyclic voltammetry, where oxidation of H(2)O(2) led to increased currents in the PAH-AuNP/NiTsPc films for the electrochemical processes associated with the phthalocyanine ring and nickel at 0.52 and 0.81 V vs. SCE, respectively, while for PAH/NiTsPc films (without AuNP) only the first redox process was affected. In control experiments we found out that the catalytic activity was not solely due to the presence of AuNP, but rather to the nanoparticles inducing NiTsPc supramolecular structures that favored access to their redox sites, thus yielding strong charge transfer. The combined effects of NiTsPc and AuNP, which could only be observed in nanostructured LbL films, point to another avenue to pursue within the CDC paradigm.

Intermediate motions and dipolar couplings as studied by Lee-Goldburg cross-polarization NMR: Hartmann-Hahn matching profiles

In this article, we evaluate the use of simple Lee-Goldburg cross-polarization (LG-CP) NMR experiments for obtaining quantitative information of molecular motion in the intermediate regime. In particular, we introduce the measurement of Hartmann-Hahn matching profiles for the assessment of heteronuclear dipolar couplings as well as dynamics as a reliable and robust alternative to the more common analysis of build-up curves. We have carried out dynamic spin dynamics simulations in order to test the method's sensitivity to intermediate motion and address its limitations concerning possible experimental imperfections. We further demonstrate the successful use of simple theoretical concepts, most prominently Anderson-Weiss (AW) theory, to analyze the data. We further propose an alternative way to estimate activation energies of molecular motions, based upon the acquisition of only two LG-CP spectra per temperature at different temperatures. As experimental tests, molecular jumps in imidazole methyl sulfonate, trimethylsulfoxonium iodide, and bisphenol A polycarbonate were investigated with the new method.

Thermal lens and interferometric method for glass transition and thermo physical properties measurements in Nd(2)O(3) doped sodium zincborate glass

In this work the time resolved thermal lens method is combined with interferometric technique, the thermal relaxation calorimetry, photoluminescence and lifetime measurements to determine the thermo physical properties of Nd(2)O(3) doped sodium zincborate glass as a function of temperature up to the glass transition region. Thermal diffusivity, thermal conductivity, fluorescence quantum efficiency, linear thermal expansion coefficient and thermal coefficient of electronic polarizability were determined. In conclusion, the results showed the ability of thermal lens and interferometric methods to perform measurements very close to the phase transition region. These techniques provide absolute values for the measured physical quantities and are advantageous when low scan rates are required. (c) 2008 Optical Society of America