Extension of the Coulomb–Hole–Hartree–Fock theory to molecules

The Coulomb–Hole–Hartree–Fock method introduced by E. Clementi in the early 1960s and reparametrized more recently by S. Chakraworty and E. Clementi to compute the correlated electronic energy in atomic systems, is here extended to compute molecules. The new parametrization is obtained empirically by fitting first and second atomic ionization potentials from He to Ca and a few diatomic molecules. The present formulation makes use of either one or more determinants in order to ensure proper dissociation products, following the early proposal of G.C. Lie and E. Clementi in the context of density functional computations for molecular systems. The new formulation is tested against the dissociation energies of a large number of molecules and it is found satisfactory. © 1995 John Wiley & Sons, Inc.     

Microscopic imaging of slow flow and diffusion: a pulsed field gradient stimulated echo sequence combined with turbo spin echo imaging.

In this paper we present a pulse sequence that combines a displacement-encoded stimulated echo with rapid sampling of k-space by means of turbo spin echo imaging. The stimulated echo enables the use of long observation times between the two pulsed field gradients that sample q-space completely. Propagators, constructed with long observation times, could discriminate slowly flowing protons from diffusing protons, as shown in a phantom in which a plug flow with linear velocity of 50microm/s could clearly be distinguished from stationary water. As a biological application the apparent diffusion constant in longitudinal direction of a transverse image of a maize plant stem had been measured as a function of observation time. Increasing contrast in the apparent diffusion constant image with increasing observation times were caused by differences in plant tissue: although the plant stem did not take up any water, the vascular bundles, concentrated in the outer ring of the stem, could still be discerned because of their longer unrestricted diffusional pathways for water in the longitudinal direction compared to cells in the parenchymal tissue. In the xylem region of a tomato pedicel flowing water could be distinguished from a large amount of stationary water. Linear flow velocities up to 0.67 mm/s were measured with an observation time of 180 ms.     

0.7 and 3 T MRI and Sap Flow in Intact Trees: Xylem and Phloem in Action

Dedicated magnetic resonance imaging (MRI) hardware is described that allows imaging of sap flow in intact trees with a maximal trunk diameter of 4 cm and height of several meters. This setup is used to investigate xylem and phloem flow in an intact tree quantitatively. Due to the fragile gradients in pressure present in both xylem and phloem, methods to study xylem and phloem transport must be minimally invasive. MRI flow imaging by means of this hardware certainly fulfils this condition. Flow is quantified in terms of (averaged) velocity, volume flow (flux) and flow conducting area, either in imaging mode or as a nonspatially resolved total. Results obtained for one tree, imaged at two different field strengths (0.7 and 3 T), are compared. An overall shortening of observed T ₂ values is manifest going from 0.7 to 3 T. Although some susceptibility artefacts may be present at 3 T, the results are still reliable and the gain in sensitivity results in shorter measurement time (or higher signal-to-noise ratio) with respect to the 0.7 T system. The results demonstrate that by use of dedicated hardware, xylem and phloem flow and its mutual interaction, can be studied in intact trees in relation to the water balance and in response to environmental (stress) conditions. Authors' address: Henk Van As, Laboratory of Biophysics, Wageningen University, Drejenlaan 3, 6703 HA Wageningen, The Netherlands     

Elucidating the Supramolecular Copolymerization of N- and C-Centered Benzene-1,3,5-Tricarboxamides: The Role of Parallel and Antiparallel Packing of Amide Groups in the Copolymer Microstructure

An in-depth study of the supramolecular copolymerization behavior of N- and C-centered benzene-1,3,5-tricarboxamides (N- and C-BTAs) has been conducted in methylcyclohexane and in the solid state. The connectivity of the amide groups in the BTAs differs, and mixing N- and C-BTAs results in supramolecular copolymers with a blocky microstructure in solution. The blocky microstructure results from the formation of weaker and less organized, antiparallel hydrogen bonds between N- and C-BTAs. In methylcyclohexane, the helical threefold hydrogen-bonding network present in C- and N-BTAs is retained in the mixtures. In the solid state, in contrast, the hydrogen bonds of pure BTAs as well as their mixtures organize in a sheet-like pattern, and in the mixtures long-range order is lost. Drop-casting to kinetically trap the solution microstructures shows that C-BTAs retain the helical hydrogen bonds, but N-BTAs immediately adopt the sheet-like pattern, a direct consequence of the lower stabilization energy of the helical hydrogen bonds. In the copolymers, the stability of the helical aggregates depends on the copolymer composition, and helical aggregates are only preserved when a high amount of C-BTAs is present. The method outlined here is generally applicable to elucidate the copolymerization behavior of supramolecular monomers both in solution as well as in the solid state.     

Normal-incidence reflectance of optimized W /B(4) C x-ray multilayers in the range 1.4 nm < l > 2.4 nm

We have fabricated W/B(4)C multilayers having periods in the range d = 0.8-1.2 nm and measured their soft-x-ray performance near normal incidence in the wavelength range 1.4相似文献   

Observation of two-magnon bound states in the two-leg ladders of (Ca,La)(14)Cu(24)O(41)

Phonon-assisted two-magnon absorption is studied in the spin- 1/2 two-leg ladders of (Ca,La)(14)Cu(24)O(41) for E parallel c (legs) and E parallel a (rungs). We verify the theoretically predicted existence of two-magnon singlet bound states, which give rise to peaks at approximately equal to 2140 and 2800 cm(-1). The two-magnon continuum is observed at approximately equal to 4000 cm(-1). Two different theoretical approaches (Jordan-Wigner fermions and perturbation theory) describe the data very well for J parallel approximately equal to 1020-1100 cm(-1), J parallel/J perpendicular approximately equal to 1-1.2. At high energies, the magnetic contribution to sigma(omega) is strikingly similar in the ladders and in the undoped high-T(c) cuprates, which emphasizes the importance of strong quantum fluctuations in the latter.