Fieldatkins1026

The existence of various quasiparticles of polarons because of electron-boson couplings plays important roles in determining electron transport in titanium dioxide (TiO2), which affects a wealth of physical properties from catalysis to interfacial superconductivity. In addition to the well-defined Fröhlich polarons whose electrons are dressed by the phonon clouds, it has been theoretically predicted that electrons can also couple to their own plasmonic oscillations, namely, the plasmonic polarons. Here we experimentally demonstrate the formation of plasmonic polarons in highly doped anatase TiO2 using angle-resolved photoemission spectroscopy. Our results show that the energy separation of plasmon-loss satellites follows a dependence on √n, where n is the electron density, manifesting the characteristic of plasmonic polarons. The spectral functions enable to quantitatively evaluate the strengths of electron-plasmon and electron-phonon couplings, respectively, providing an effective approach for characterizing the interplays among different bosonic modes in the complicate many-body interactions.One particularly fascinating vision for charge-operated devices is the controlled assembly of structures from single surface-deposited molecules. Here, we report on the assembly of linear clusters that consist of phthalocyanine (H2Pc) molecules on a Ag(111) surface. The molecules are imaged as well as manipulated with a low-temperature scanning tunneling microscope (STM). Upon deprotonation of every second H2Pc, the resulting HPc molecule exhibits an isomeric bistability which can be used as inputs in logic gates. Combining our STM measurements with density functional theory calculations we show that the HPc isomers exhibit a repulsive electrostatic interaction with adjacent H2Pc molecules which, due to the asymmetric charge distribution on HPc, results in a counterclockwise or clockwise molecule tilt of the latter, thereby defining the logic 0 and 1 of the output. It is shown that information can be relayed along molecule chains over distances equivalent to at least nine molecules.An imino-phosphanamide ligand, [NHIiPr2Me2P(Ph)NH-2,6- i Pr2C6H3] (LH), containing two different N-substituents was prepared by the direct reaction of the lithium salt of N-heterocyclic imine (NHI) with phenylchloro-2,6-diisopropylphenyl phosphanamine, PhP(Cl)NH-2,6- i Pr2-C6H3. Reaction of LH with Y(N(SiMe3)2)3 afforded the heteroleptic complex, [LY(N(SiMe3)2)2] (1), by elimination of HN(SiMe3)2. Compound 1 was characterized by multinuclear NMR and X-ray crystallography. In the complex, the Y(III) center was found to be tetracoordinate in a distorted tetrahedral geometry. The ligand, imino-phosphanamidinate, [L]-, functions in a chelating manner, and its coordination to Y(III) results in a distorted 4-membered YPN2 ring. As a proof of principle of its activity, 1 was used as a precatalyst for the hydroboration of various aldehydes and ketones using HBpin as the hydrogen source. The hydroboration reaction was rapid and clean even with low catalyst loadings (0.01-0.1 mol %). In addition, a very good functional group tolerance was observed in these reactions.Hybrid electronic materials combine inorganic metals and semiconductors with π-conjugated polymers. The orientation of the polymer molecules in relation to the inorganic components is crucial for electrical material properties and device performance, but little is known of the configuration of π-conjugated polymers that bind to inorganic surfaces. Highly curved surfaces are common when using nanoscale components, for example, metal nanocrystal cores covered with conductive polymers. It is important to understand their effect on molecular arrangement. Here, we compare the molecular structures and electrical conductivities of well-defined nanoscale gold spheres and rods with shells of the covalently bound polythiophene PTEBS (poly[2-(3-thienyl)-ethyloxy-4-butylsulfonate]). We prepared aqueous sinter-free inks from the particles and printed them. The particles formed highly conductive films immediately after drying. Films with spherical metal cores consistently had 40% lower conductivities than films based on nanorods. Raman and X-ray photoelectron spectroscopy revealed differences in the gold-sulfur bonds of PTEBS on rods and spheres. The fractions of bond sulfur groups implied differences in the alignment of PTEBS with the surface. selleck More polymer molecules were bound in an edge-on configuration on spheres than on rods, where almost all polymers aligned "face-on" with the metal surface. This leads to different interface resistances gold-polythiophene-gold interfaces between rods with π-π-tacked face-on PTEBS apparently foster electron transport along the surface-normal direction, while edge-on PTEBS does not. Molecular confinement thus increases the conductivity of hybrid inks based on highly curved nanostructures.Controllable wetting surfaces play a significant role in numerous applications such as smart liquid manipulation, lab-on-a-chip, drug delivery, liquid robot, and so on. A novel type of magnetically controllable isotropic/anisotropic slippery surface was prepared by femtosecond laser ablation. The slippery liquid-infused porous surface (SLIPS) can be switched between an isotropic smooth state and an anisotropic groove state by the magnetic field. The relationship between the sliding property of the SLIPS and the magnetic flux density, water droplet volume, microgroove width, and microgroove height are systematically studied. Passively flexible movement on the isotropic SLIPS and actively directional movement on the anisotropic SLIPS of water droplets were realized. This work provides a fresh understanding of the controllable isotropic/anisotropic SLIPS and reveals great potential in versatile applications which are related to magnetically controllable smart liquid manipulation.Enhancement of parallel (x-y plane) dielectric permittivity of confined fluids has been shown previously. However, a theoretical model that explains this enhancement is lacking thus far. In this study, using statistical-mechanical theories and molecular dynamics simulations, we show an explicit relation between the parallel dielectric permittivity, density variations, and dipolar correlations for protic and aprotic fluids confined in slit-like channels. We analyze the importance of dipolar correlations on enhancement of parallel dielectric permittivity inside large channels and extreme confinements. In large channels, beyond the interfacial region, dipolar correlations exhibit bulk-like behavior. Under extreme confinement, the correlations become stronger to the extent that they give rise to a giant increase in the parallel dielectric permittivity. This sudden increase in dielectric permittivity can be a signature of a liquid transition into higher-ordered structures and has important consequences for understanding ion transport, molecular dissociation, and chemical reactions inside nanoconfined environments.