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991.
Elodie Fernandes Lima;Thomas Bredow; 《Journal of computational chemistry》2024,45(32):2702-2709
The development of novel methods in solid-state quantum chemistry necessitates reliable reference data sets for their assessment. The most fundamental solid-state property of interest is the crystal structure, quantified by the lattice parameters. In the last decade, several studies were conducted to assess theoretical approaches based on the agreement of calculated lattice parameters with respect to experiment as a measure. However, most of these studies used a limited number of reference systems with high symmetry. The present work offers a more comprehensive reference benchmark denoted as Sol337LC, which consists of 337 inorganic compounds with 553 symmetry-inequivalent lattice parameters, representing every element of the periodic table for atomic numbers between 1 and 86, except noble gases, the radioactive elements and lanthanoids. The reference values were taken from earlier benchmarks and from measurements at very low temperature or extrapolation to 0 K. The experimental low-temperature lattice parameters were then corrected for zero-point energy effects via the quasi-harmonic approximation for direct comparison with quantum-chemical optimized structures. A selection of standard density functional approximations was assessed for their deviations from the experimental reference data. The calculations were performed with the crystal orbital program CRYSTAL23, applying optimized atom-centered basis sets of triple-zeta plus polarization quality. The SCAN functional family and the global hybrid functional PW1PW, augmented with the D3 dispersion correction, were found to provide closest agreement with the Sol337LC reference data. 相似文献
992.
Sónia O. Pereira Ana Barros‐Timmons Tito Trindade 《Particle & Particle Systems Characterization》2017,34(2)
The synthesis of core‐shell Au nanoparticles protected by an amphiphilic block copolymer is investigated by distinct reversible addition fragmentation chain transfer (RAFT) emulsion polymerization routes. The controlled polymerization of polymer shells onto Au nanoparticles is attempted by using the macroRAFT (MR) agent based on 2‐(dodecylthiocarbonothioylthio)‐2‐methylpropionic acid synthesized via RAFT polymerization of poly(ethylene glycol) methyl ether acrylate and exploring several approaches, which include (i) post‐modification; (ii) in situ synthesis and (iii) “grafting from” strategies. In the conditions investigated here all these strategies lead to Au polymer nanocomposites but morphological well‐defined core‐shell nanoparticles are only obtained by applying the “grafting from” strategy. In particular, conditions that promote chain extension from the MR agent adsorbed onto the Au nanoparticles are found necessary to obtain nanostructures with such morphological characteristics and that still show the localized surface plasmon resonance typical of colloidal Au nanoparticles. 相似文献
993.
Andreia T. Pereira António J. M. Ribeiro Pedro A. Fernandes Maria J. Ramos 《International journal of quantum chemistry》2017,117(18)
In recent years, there has been an increased interest in understanding the enzymatic mechanism of glycosidases resorting mostly to DFT and DFT/MM calculations. However, the performance of density functionals (DFs) is well known to be system and property dependent. Trends drawn from general studies, despite important to evaluate the quality of the DFs and to pave the way for the development of new DFs, may be misleading when applied to a single specific system/property. To overcome this issue, we carried out a benchmarking study of 40 DFs applied to the geometry optimization and to the electronic barrier height (E Barrier) and electronic energy of reaction (E R) of prototypical glycosidase‐catalyzed reactions. Additionally, we report calculations with SCC‐DFTB and four semiempirical MO methods applied to the same problem. We have used a universal molecular model for retaining glycosidases, comprising only a 22‐atoms system that mimics the active site and substrate. High accuracy reference geometries and energies were calculated at the CCSD(T)/CBS//MP2/aug‐cc‐pVTZ level of theory. Most DFs reproduce the reference geometries extremely well, with mean unsigned errors (MUE) smaller than 0.05 Å for bond lengths and 3° for bond angles. Among the DFs, wB97X‐D, CAM‐B3LYP, B3P86, and PBE1PBE have the best performance in geometry optimizations (MUE = 0.02 Å). Conversely, semiempirical MO and SCC‐DFTB methods yielded less accurate geometries (MUE between 0.09 and 0.17 Å). The inclusion of D3 correction has a small, but still relevant, influence in the geometry predicted by some DFs. Regarding E Barrier, 11 DFs (MPW1B95, CAM‐B3LYP, M06 ‐ 2X, PBE1PBE, wB97X ‐ D, B1B95, BMK, MN12 – SX, M05, M06, and M11) presented errors below 1 kcal.mol?1, in relation to the reference energy. Most of these functionals belong to the family of hybrid functionals (H‐GGA, HH‐GGA, and HM‐GGA), which shows a positive influence of HF exchange in the determination of E Barrier. The inclusion of D3 correction has not affected significantly the E Barrier and E R. The use of geometries at the accurate but expensive MP2/aug‐cc‐pVTZ level of theory has a small, albeit not insignificant, influence in the E Barrier when compared with energies calculated with geometries determined with the DFs (usually a few tenths of kcal.mol?1, with exceptions). In general, semiempirical MO methods and DFTB are associated with larger errors in the determination of E Barrier, with unsigned errors from 6.9 to 24.7 kcal.mol?1. 相似文献
994.
Humberto César Chaves Fernandes Davi Bibiano Brito 《International Journal of Infrared and Millimeter Waves》2007,28(8):651-661
Photonic band gap (PBG) crystals have been used as a perfectly reflecting substrate for many millimeter wave applications.
In this work the fin line directional coupler with substrate PBG was analyzed using the TTL - Transverse Transmission Line
- method. Compared to other full wave methods the TTL is an efficient tool to determine the coupler characteristics, making
possible a significant algebraic simplification of the equations involved in the process. In order to analyze this structure
the effective dielectric constant, the attenuation constant and the coupling were determined. The results obtained for this
application and the conclusions are presented.
This work was partially financed by CNPQ. 相似文献
995.
Chern GD Fernandes GE Chang RK Song Q Xu L Kneissl M Johnson NM 《Optics letters》2007,32(9):1093-1095
We present an efficient design for direct coupling between a spiral-shaped and a semicircle-shaped microcavity (micro-cavity) as an alternative to traditional evanescent wave coupling for planar integrated photonic technology. We observe the preservation of the high Q-value of the spiral oscillator when coupled to a semicircle under current injection using an AlGaAs single-quantum-well heterostructure. With slight alterations to the directly coupled micro-cavity configuration, such as coupling shape and overlap distance, the number of observed modes and output intensity are changed. AlGaAs and InGaN spiral-shaped microcavities have unidirectional emission normal to the spiral notch. 相似文献
996.
J.M.?FonsecaEmail author W.A.?Moura-Melo A.R.?Pereira 《The European Physical Journal B - Condensed Matter and Complex Systems》2013,86(11):481
By coating a three-dimensional topological insulator (TI) with a ferromagnetic filmsupporting an in-plane magnetic vortex, one breaks the time-reversal symmetry (TRS)without generating a mass gap. It rather yields electronic states bound to the vortexcenter which have different probabilities associated with each spin mode. In addition, itsassociate current (around the vortex center) is partially polarized with an energy gapseparating the most excited bound state from the scattered ones. Charged zero-modes alsoappear as fully polarized modes localized near the vortex center. From the magnetic pointof view, the observation of such a special current in a TI-magnet sandwich comes about asan alternative technique for detecting magnetic vortices in magnetic thin films. 相似文献
997.
998.
999.
J. P. B. Silva A. Khodorov A. Almeida J. Agostinho Moreira M. Pereira M. J. M. Gomes 《Applied Physics A: Materials Science & Processing》2014,116(3):1271-1280
In this work, Ba0.8Sr0.2TiO3 (BST) films were grown by pulse laser ablation on bare glass and platinized substrates. The crystalline phase was obtained with the help of laser-assisted annealing (LAA) at room temperature, in air environment. By adjusting LAA conditions, like frequency of the laser and number of shots, we were able to grow crack-free BST thin films with pure perovskite phase on bare glass and platinized substrates. The crystalline layer was found to be the same irrespective of the substrate used, c.a. 250 nm thick. The electric characteristics of the amorphous and LAA crystalline BST films deposited on platinized substrate were further studied and analyzed. While in amorphous films it was found that the oxygen defects are responsible for conduction, in LAA films the amorphous/crystalline interface layer plays an important role in current leakage. 相似文献
1000.
Lenneke WA van Hooijdonk Muhammad Ichwan Thomas F Dijkmans Theo G Schouten Marijke WA de Backer Roger AH Adan Fons J Verbeek Erno Vreugdenhil Carlos P Fitzsimons 《BMC neuroscience》2009,10(1):2-19