Search results for "Clusters"
showing 10 items of 1274 documents
Atomically Precise, Thiolated Copper–Hydride Nanoclusters as Single-Site Hydrogenation Catalysts for Ketones in Mild Conditions
2019
Copper-hydrides are known catalysts for several technologically important reactions such as hydrogenation of CO, hydroamination of alkenes and alkynes, and chemoselective hydrogenation of unsaturated ketones to unsaturated alcohols. Stabilizing copper-based particles by ligand chemistry to nanometer scale is an appealing route to make active catalysts with optimized material economy; however, it has been long believed that the ligand-metal interface, particularly if sulfur-containing thiols are used as stabilizing agent, may poison the catalyst. We report here a discovery of an ambient-stable thiolate-protected copper-hydride nanocluster [Cu25H10(SPhCl2)18]3- that readily catalyzes hydrogen…
Ab initiocalculations of theFcenters in MgF2bulk and on the (001) surface
2012
We present and discuss the results of atomic and electronic structure calculations of the F centers in MgF2 bulk and on the (001) surface. The calculations are based on the B3PW Hartree–Fock and density functional theory hybrid exchange-correlation functional. Most of the electronic density of a missing fluorine ion is localized in the bulk vacancy and a little bit less—in a surface vacancy. It is shown that the electronic F center is a deep donor. The lattice distortion and defect formation energy on the neutral (001) surface and in the bulk are also compared.
Time-dependent effects in the nonsequential ionization of helium at various wavelengths
2000
Calculations of the double ionization of a model 1D helium atom interacting with an intense short laser pulse are presented. A substantial signature of nonsequential double ionization is found for all the wavelengths that are considered, from 248 nm to 1064 nm, provided that sufficiently short pulses are employed. We show how one can modify the size of the “knee” structure of the double ionization yield curve by varying the laser pulse duration. The underlying mechanism of the correlated double electron ejection is investigated and discussed.
Highly Robust but Surface-Active: N-Heterocyclic Carbene-Stabilized Au25 Nanocluster as a Homogeneous Catalyst
2019
<div> <div> <div> <p>Surface organic ligands play a critical role in stabilizing atomically precise metal nanoclusters in solutions. However, it is still challenging to prepare highly robust ligated metal nanoclusters that are surface-active for liquid-phase catalysis without any pre-treatment. Herein, we report a novel N-heterocyclic carbine-stabilized Au25 nanocluster with high thermal and air stabilities as a homogenous catalyst for cycloisomerization of alkynyl amines to indoles. The nanocluster, characterized as [Au25(iPr2-bimy)10Br7]2+ (iPr2-bimy=diisopropyl-benzilidazolium) (1), was synthesized by direct reduction of AuSMe2Cl and iPr2- bimyAuBr with NaBH4 in o…
Hydrogen adsorption on the ZnO $(1\bar{1}00)$ surface: ab initio hybrid density functional linear combination of atomic orbitals calculations
2014
Hydrogen atoms unavoidably presented in ZnO samples or thin films during their synthesis considerably affect electrical conductivity. Results of first principles hybrid functional linear combination of atomic orbitals calculations are discussed for hydrogen atoms incorporated in bulk or adsorbed upon non-polar ZnO (1¯ 100) surfaces. The energy of H incorporation, atomic relaxation, electronic density redistribution and modification of the electronic structure are compared for both surface adsorption and bulk absorption. It is shown that hydrogen forms a strong bonding with the surface O ions (Eads = 2.7eV) whereas its incorporation into bulk is energetically quite unfavorable. Hydrogen adso…
Photoelectron emission induced by low temperature hydrogen plasmas
2018
Experimental results of low temperature hydrogen plasma induced photoelectron emission measurements comparing two different plasma heating methods are summarized. By exposing the samples to the vacuum ultraviolet radiation of a filament-driven multi-cusp arc discharge ion source and a 2.45 GHz microwave-driven ion source, it has been measured that the total photoelectron emission from various metal surfaces is on the order of 1 A per kW of plasma heating power, which can be increased by a factor of 2–3.5 with a thin layer of alkali metal. The possible effects of the photoelectrons on the plasma sheath structure are studied with a 1D collisionless model extended to include the contribution o…
DFT studies of OH-functionalized open-ended zigzag, armchair, and chiral single wall carbon nanotubes
2011
The functionalization of single-wall carbon nanotubes (SWCNTs) by attaching various molecules or molecular groups to the exterior walls or tips has attracted much attention, because it offers a possible way to modify their electronic, chemical, optical and mechanical properties. In this contribution the results of DFT studies of pristine and OH-modified open-ended zigzag (9,0), armchair (5,5) and chiral (8,2) nanotubes are reported. The calculations have been performed for partially and fully functionalized at one end model SWCNTs with dangling bonds saturated with hydrogen atoms and a nonadditive dependence of attachment energy on the number of substituents was observed.
Self-Passivating Edge Reconstructions of Graphene
2008
Planar reconstruction patterns at the zigzag and armchair edges of graphene were investigated with density functional theory. It was unexpectedly found that the zigzag edge is metastable and a planar reconstruction spontaneously takes place at room temperature. The reconstruction changes electronic structure and self-passivates the edge with respect to adsorption of atomic hydrogen from molecular atmosphere.
Local electronic structure rearrangements and strong anharmonicity in YH3 under pressures up to 180 GPa
2021
The authors acknowledge the ESRF program committee (Grenoble, France) for the opportunity to perform XAFS and XRD measurements. We are grateful to Prof. Dr Marek Tkacz from the Institute of Physical Chemistry, PAS Kasprzaka 44/52, 01-224 Warsaw, Poland, for high quality YH3 samples and to Dr. José A. Flores-Livas for a fruitful discussion. A.P.M. and A.A.I. acknowledge the Russian Foundation for the Basic Research (grant No 18-02-40001_mega) for financial support. J.P., A.K., and I.P. would like to thank the support of the Latvian Council of Science project No. lzp-2018/2-0353. ISSP UL acknowledge the European Union’s Horizon 2020 Framework Programme H2020-WIDESPREAD-01-20l 6-2017-TeamingPh…
Ionization potential of aluminum clusters
1998
Structure, electronic structure, and ionization potential of aluminum clusters of 2–23 atoms are studied with a total energy method based on the density-functional theory. The calculated adiabatic ionization potentials agree remarkably well with the data from threshold photoionization measurements. The analysis of results gives insight into hybridization effects in the smallest clusters as well as reveals certain clusters that exhibit a clear jellium-type shell structure. An explanation of the experimental results in the size region of 12–23 atoms is given in terms of coexisting, competing icosahedral, decahedral, and fcc-based clusters. @S0163-1829~98!00228-8#