Archerfrye0460

Optically induced magnetic resonances in nonmagnetic media have unlocked magnetic light-matter interactions and led to new technologies in many research fields. Previous proposals for the levitation of nanoscale particles without structured illumination have worked on the basis of epsilon-near-zero surfaces or anisotropic materials, but these materials carry with them significant fabrication difficulties. We report the optical levitation of a magnetic dipole over a wide range of realistic materials, including bulk metals, thereby relieving these difficulties. The repulsion is independent of surface losses, and we propose an experiment to detect this force which consists of a core-shell nanoparticle, exhibiting a magnetic resonance, in close proximity to a gold substrate under plane wave illumination. We anticipate the use of this phenomenon in new nanomechanical devices.Incorporating functional atomic sites in graphene is essential for realizing advanced two-dimensional materials. Doping graphene with nitrogen offers the opportunity to tune its chemical activity with significant charge redistribution occurring between molecules and substrate. The necessary atomic scale understanding of how this depends on the spatial distribution of dopants, as well as their positions relative to the molecule, can be provided by scanning tunneling microscopy. Here we show that a noncovalently bonded molecule such as CoPc undergoes a variable charge transfer when placed on N-doped graphene; on a nitrogen pair, it undergoes a redox reaction with an integral charge transfer whereas a lower fractional charge transfer occurs over a single nitrogen. Thus, the charge state of molecules can be tuned by suitably tailoring the conformation of dopant atoms.Enhancement of the discharge capacity of lithium-oxygen batteries (LOBs) while maintaining a high cell voltage is an important challenge to overcome to achieve an ideal energy density. Both the cell voltage and discharge capacity of an LOB could be controlled by employing a binary solvent electrolyte composed of dimethyl sulfoxide (DMSO) and acetonitrile (MeCN), whereby an energy density 3.2 times higher than that of the 100 vol % DMSO electrolyte was obtained with an electrolyte containing 50 vol % of DMSO. The difference in the solvent species that preferentially solvates Li+ and that which controls the adsorption-desorption equilibrium of the discharge reaction intermediate, LiO2, on the cathode/electrolyte interface provides these unique properties of the binary solvent electrolyte. Combined spectroscopic and electrochemical analysis have revealed that the solvated complex of Li+ and the environment of the cathode/electrolyte interface were the determinants of the cell voltage and discharge capacity, respectively.A stereoselective annulation protocol was developed to construct dihydrofuranoindoles from readily available starting materials. In the presence of a bifunctional squaramide, the Friedel-Crafts alkylation/annulation cascade process occurred smoothly to provide dihydrofuranoindoles in 26-95% isolated yields exclusively as trans-diastereomers (38-99% ee). This catalytic protocol was compatible with a range of structurally distinct hydroxyindoles bearing the hydroxyl group at different positions, providing four kinds of dihydrofuranoindoles. Moreover, gram-scale synthesis and further synthetic manipulation of the product were also demonstrated.The production of zinc-containing nanostructures has a large variety of applications. WP1130 Using electron beam techniques to degrade organometallic molecules for that purpose is perhaps one of the most versatile methods. In this work, we investigate the scattering of low-energy (3 eV. The mechanisms for electron capture and then molecular dissociation are discussed in terms of density functional theory studies.The fungal metabolite illudinine is prepared in seven steps and ca. 55% overall yield from dimedone using an "open and shut" (ring-opening and ring-closing) strategy. Tandem ring-opening fragmentation and olefination of dimedone establishes alkyne and vinylarene functionality linked by a neopentylene tether. Oxidative cycloisomerization then provides the illudinine framework. The key innovation in this second-generation synthesis of illudinine is the use of the nitrile functional group, rather than an ester, as the functional precursor to the carboxylic acid of illudinine. The small, linear nitrile (C≡N) is associated with improved selectivity, π-conjugation, and reactivity at multiple points in the synthetic sequence relative to the carboxylic acid ester. Preliminary assays indicate that illudinine and several related synthetic analogues are monoamine oxidase inhibitors, which is the first reported indication of biological activity associated with this natural product. Illudinine was found to inhibit monoamine oxidase B (MAO-B) with an IC50 of 18 ± 7.1 μM in preliminary assays.In the framework of a multistep mechanism in which environmental motion triggers comparatively faster elementary electron-transfer steps and stabilizes hole-transfer products, microscopic coherence is crucial for rationalizing the observed yield ratios of oxidative damage to DNA. Interference among probability amplitudes of indistinguishable electron-transfer paths is able to drastically change the final outcome of charge transport, even in DNA oligomers constituted by similar building blocks, and allows for reconciling apparently discordant experimental observations. link2 Properly tailored DNA oligomers appear to be a promising workbench for studying tunneling in the presence of dissipation at the macroscopic level.Light-induced oxidative damage of DNA by 1O2 generated from photoexcited C60 was observed at the single-molecule level by atomic force microscopy (AFM) imaging. Two types of DNA origami with uniform morphologies were immobilized on a mica surface and used as DNA substrates. Upon visible light irradiation (528 nm) in the presence of a C60 aqueous solution, the morphology changes of DNA origami substrates were observed by time-lapse AFM imaging at the single-molecule level by tracking a discrete DNA molecule. The origami showed nicked and flattened morphologies with relaxed features caused by the covalent cleavage of the DNA strands. link3 The involvement of 1O2 in the on-surface DNA damage was clearly confirmed by AFM experiments in the presence of a 1O2 quencher and ESR measurements with a spin-trapping agent for 1O2. This study is the first example of single-molecule observation of oxidative damage of DNA by AFM with corresponding morphology changes in a photocontrolled and time-dependent manner by 1O2 generated catalytically from photoexcited C60.The NH3-mediated selective catalytic reduction (NH3-SCR) of NOx over Cu-ion-exchanged chabazite (Cu-CHA) catalysts is the basis of the technology for abatement of NOx from diesel vehicles. A crucial step in this reaction is the activation of oxygen. Under conditions for low-temperature NH3-SCR, oxygen only reacts with CuI ions, which are present as mobile CuI diamine complexes [CuI(NH3)2]+. To determine the structure and reactivity of the species formed by oxidation of these CuI diamine complexes with oxygen at 200 °C, we have followed this reaction, using a Cu-CHA catalyst with a Si/Al ratio of 15 and 2.6 wt% Cu, by X-ray absorption spectroscopies (XANES and EXAFS) and diffuse reflectance UV-Vis spectroscopy, with the support of DFT calculations and advanced EXAFS wavelet transform analysis. The results provide unprecedented direct evidence for the formation of a [Cu2(NH3)4O2]2+ mobile complex with a side-on μ-η2,η2-peroxo diamino dicopper(II) structure, accounting for 80-90% of the total Cu content. These [Cu2(NH3)4O2]2+ are completely reduced to [CuI(NH3)2]+ at 200 °C in a mixture of NO and NH3. Some N2 is formed as well, which suggests the role of the dimeric complexes in the low-temperature NH3-SCR reaction. The reaction of [Cu2(NH3)4O2]2+ complexes with NH3 leads to a partial reduction of the Cu without any formation of N2. The reaction with NO results in an almost complete reduction to CuI, under the formation of N2. This indicates that the low-temperature NH3-SCR reaction proceeds via a reaction of these complexes with NO.Readily available 1,2-amino alcohols provide the framework for a new generation of chiral carboxylic acid catalysts that rival the acidity of the widely used chiral phosphoric acid catalyst (S)-TRIP. Covalently linked thiourea sites stabilize the carboxylate conjugate bases of these catalysts via anion-binding, an interaction that is largely responsible for the low pKa values. The utility of the new catalysts is illustrated in the context of challenging [4 + 2] cycloadditions of salicylaldehyde-derived acetals with homoallylic and bishomoallylic alcohols, providing polycyclic chromanes in a highly enantioselective fashion.The fragmentation dynamics of water in a superexcited state play an important role in the ionosphere of the planets and in the photodissociation region (PDR) of the planetary nebula. In this Letter, we experimentally study the fragmentation dynamics of H2O with the energy above its ionization potential initiated by vacuum ultraviolet free-electron laser pulses. The experimental results indicate that the binary fragmentation channels H + OH and the triple channels O + 2H both present at 96.4 nm photolysis. Electronically excited OH super-rotors (v = 0, N ≥ 36, or v = 1, N ≥ 34), with the internal energy just above the OH (A) dissociation energy, are observed for the first time, which are only supported by the large centrifugal barriers. An absolute cross section of these super-rotors is estimated to be 0.7(±0.3) × 10-18 cm2. The tunnelling rates of these extremely rotationally excited states are also analyzed. This work shows a spectacular example of energy transfer from a photon to fragment rotation through photodissociation.The combination of Al nanoparticles (ANPs) and hydrogen peroxide (H2O2) can serve as environmentally friendly bipropellants and maximize the energetic benefits through harnessing heat release and chemical energy stored in H2. This work presents an atomic insight into the combustion mechanism of ANPs/H2O2. Two main paths, including the ANPs oxidation by H2O2 to produce H2 and Al oxides, and the catalytic decomposition of H2O2 on ANP surface to generate O2 and H2O, are confirmed to maintain the combustion. OH and HOO radicals as well as H2O, O2, H2, and Al oxides are detected as dominant intermediates and products therein. It is evidenced that higher temperature, smaller ANP size, and higher H2O2 concentration enhance the combustion. Moreover, atomic details show that the H desorption from ANPs/Al clusters is a critical step for both H2 production and ANP oxidation. In addition, microexplosion that has been confirmed in hot and dense O2 is not observed in H2O2, even with a high concentration, possibly due to a slower heat release. Besides, the observed excellent specific impulse of the ANP/H2O2 bipropellants could be attributed to the considerable H2 production, instead of heat release. This work is expected to present an overall atomic perspective about the combustion mechanism of ANP/H2O2 bipropellants.