Self-consistent implementation of a nonlocal van der Waals density functional with a Gaussian basis set

Nearly all common density functional approximations fail to properly describe dispersion interactions responsible for binding in van der Waals complexes. Empirical corrections can fix some of the failures but cannot fully grasp the complex physics and may not be reliable for systems dissimilar to the fitting set. In contrast, the recently proposed nonlocal van der Waals density functional (vdW-DF) was derived from first principles, describes dispersion interactions in a seamless fashion, and yields the correct asymptotics. Implementation of this functional is somewhat cumbersome: Nonlocal dependence on the electron density requires numerical double integration over the space variables and functional derivatives are nontrivial. This paper shows how vdW-DF can be implemented self-consistently with Gaussian basis functions. The gradients of the energy with respect to nuclear displacements have also been derived and coded, enabling efficient geometry optimizations. We test the vdW-DF correlation functional in combination with several exchange approximations. We also study the sensitivity of the method to the basis set size and to the quality of the numerical quadrature grid. For weakly interacting systems, acceptable accuracy in semilocal exchange is achieved only with fine grids, whereas for nonlocal vdW-DF correlation even rather coarse grids are sufficient. The current version of vdW-DF is not well suited for pairing with Hartree-Fock exchange, leading to considerable overbinding.     

Improved hydrogen release from ammonia-borane with ZIF-8

The promotion for hydrogen release from ammonia-borane (AB) was observed in the presence of ZIF-8. Even at concentrations of ZIF-8 as low as 0.25 mol %, a reduction of the onset temperature for dehydrogenation accompanies an increase in both the rate and amount of hydrogen released from AB.     

Error analysis of free probability approximations to the density of States of disordered systems

Theoretical studies of localization, anomalous diffusion and ergodicity breaking require solving the electronic structure of disordered systems. We use free probability to approximate the ensemble-averaged density of states without exact diagonalization. We present an error analysis that quantifies the accuracy using a generalized moment expansion, allowing us to distinguish between different approximations. We identify an approximation that is accurate to the eighth moment across all noise strengths, and contrast this with perturbation theory and isotropic entanglement theory.     

Colorimetric detection of Escherichia coli using engineered bacteriophage and an affinity reporter system

Analytical and Bioanalytical Chemistry - Reporter phage systems have emerged as a promising technology for the detection of bacteria in foods and water. However, the sensitivity of these assays is...     

Numerical stability analysis for the explicit high-order finite difference analysis of rotationally symmetric shells

A numerical stability analysis has been formulated to accompany the already developed explicit high-order finite difference analysis of rotationally symmetric shells subjected to time-dependent impulsive loadings. This already developed analysis utilizes a constant nodal point spacing for the spatial finite difference mesh, with the governing field differential equations formulated in terms of the transverse, meridional, and circumferential displacements as the fundamental variables. The remaining quantities which enter into the natural boundary conditions at each edge of the shell are incorporated into the complete system of equations by defining those quantities at each boundary in terms of the displacements. Surface loadings and inertia forces in each of the three displacement directions of the shell have been considered in the governing equations. Ordinary finite difference representations are used for the time derivatives. All loadings and dependent variables in the circumferential direction of the shell are expressed in Fourier series expansions. The complete system of equations is solved implicitly for the first time increment, while explicit relations are used to determine the three primary displacements within the boundary edges of the shell for the second and succeeding time increments. Separate implicit solutions at each boundary are then used to determine the remaining unspecified primary variables on and outside the boundaries. Subsequently, the remaining primary variables within the boundary edges of the shell and all secondary variables are determined explicitly. Numerical stability (or instability) of numerical solutions for given choices of spatial and time increments is determined by evaluation of the eigenvalues of the explicit coefficient matrix and comparing the maximum eigenvalue with the requirements of a stability criterion developed before by the author. Solutions for typical shells and loadings together with results of stability analyses have been included, and comparisons of the stability requirements and solutions with the requirements and solutions based upon ordinary spatial finite difference representations are included.     

All Schatten spaces endowed with the Schur product are Q-algebras

We prove that the Banach algebra formed by the space of compact operators on a Hilbert space endowed with the Schur product is a quotient of a uniform algebra (also known as a Q-algebra). Together with a similar result of Pérez-García for the trace class, this completes the answer to a long-standing question of Varopoulos.     

The spectrum of α‐resolvable designs with block size four

Abstact: An α‐resolvable BIBD is a BIBD with the property that the blocks can be partitioned into disjoint classes such that every class contains each point of the design exactly α times. In this paper, we show that the necessary conditions for the existence of α‐resolvable designs with block size four are sufficient, with the exception of (α, ν, λ) = (2, 10, 2). © 2000 John Wiley & Sons, Inc. J Combin Designs 9: 1–16, 2001     

The existence,uniqueness, and instability of spherically symmetric solutions of a system of reaction—Diffusion equations

The system $\text{?x}\text{?t}\text{= Δx + F(x,y),}\text{?y}\text{?t}\text{= G(x,y)}$ is investigated, where x and y are scalar functions of time (t ? 0), and n space variables $\text{(ξ}{}_1\text{,…, ξ}{}_{\mathrm{n}}\text{), Δx ≡ ∑}{}_{\mathrm{i\; =\; 1}}{}^{\mathrm{n}}\text{?}{}^2\text{x}\text{?ξ}{}_{\mathrm{i}}{}^2$, and F and G are nonlinear functions. Under certain hypotheses on F and G it is proved that there exists a unique spherically symmetric solution $\text{(x(r),y(r)),}\text{where}\text{r = (ξ}{}_1{}^2\text{+ … + ξ}{}_{\mathrm{n}}{}^2\text{)}{}^{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}$, which is bounded for r ? 0 and satisfies x(0) >x₀, y(0) > y₀, x′(0) = 0, y′(0) = 0, and x′ < 0, y′ > 0, ?r > 0. Thus, (x(r), y(r)) represents a time independent equilibrium solution of the system. Further, the linearization of the system restricted to spherically symmetric solutions, around (x(r), y(r)), has a unique positive eigenvalue. This is in contrast to the case n = 1 (i.e., one space dimension) in which zero is an eigenvalue. The uniqueness of the positive eigenvalue is used in the proof that the spherically symmetric solution described is unique.     

Single-pass waveguide amplifiers in Er-Yb doped zinc polyphosphate glass fabricated with femtosecond laser pulses

We have investigated the direct fabrication of subsurface waveguide amplifiers in Er-Yb zinc polyphosphate glass by utilizing the relationship between the initial glass composition and the resulting changes to the network structure after modification by fs laser pulses. Waveguides, exhibiting internal gain of 1 dB/cm at 1.53 μm when pumped with 500 mW at 976 nm, were directly fabricated using a regenerative amplified Ti:sapphire 1 kHz, 180 fs laser system. Optical properties as well as insertion losses and internal gain are reported.