Godfreywells1597
In contrast, other scar states we find are product states, which could be easily prepared experimentally. The dimension of scar subspace is directly controlled by the choice of group G and can be made exponentially large.The stereoselective β-C(sp2)-H arylation of various acyclic enamides with arylsilanes via Rh(III)-catalyzed cross-coupling reaction was illustrated. The methodology was characterized by extraordinary efficacy and stereoselectivity, a wide scope of substrates, good functional group tolerance, and the adoption of environmentally friendly arylsilanes. The utility of this present method was evidenced by the gram-scale synthesis and further elaboration of the product. In addition, Rh(III)-catalyzed C-H activation is considered to be the critical step in the reaction mechanism.The hydrophilic/hydrophobic interactions of water are important in biological and chemical self-assembly phenomena. Water clusters in hydrophobic environments exhibit a unique morphology. Their process of formation and nonpolar properties have been extensively studied, but no direct experimental evidence has been available until now. This study provides spectroscopic evidence for the transformation of water to nonpolar configuration via clustering. Although individual water molecules form hydrogen bonds with the hydroxyl protons of n-hexanol when codissolved in a nonpolar solvent (toluene-d8), the water clusters are comprised solely of hydrogen bonds between water molecules and do not form hydrogen bonds with the hydroxyl protons of n-hexanol. This behavior indicates that the water clusters are nonpolar rather than polar. This study reports the first example of nonpolar water configuration produced via a liquid-state clustering. This property is a common and important interfacial phenomenon of water in chemistry, biology, materials science, geology, and meteorology.It is promising yet challenging to develop efficient methods to separate nanoparticles (NPs) with nanochannel devices. Herein, in order to guide and develop the separation method, the thermodynamic mechanism of NP penetration into solvent-filled nanotubes is investigated by using classical density functional theory. The potential of mean force (PMF) is calculated to evaluate the thermodynamic energy barrier for NP penetration into nanotubes. The accuracy of the theory is validated by comparing it with parallel molecular dynamics simulation. By examining the effects of nanotube size, solvent density, and substrate wettability on the PMF, we find that a large tube, a low bulk solvent density, and a solvophilic substrate can boost the NP penetration into nanotubes. In addition, it is found that an hourglass-shaped entrance can effectively improve the NP penetration efficiency compared with a square-shaped entrance. Furthermore, the minimum separation density of NPs in solution is identified, below which the NP penetration into nanotubes requires an additional driving force. Our findings provide fundamental insights into the thermodynamic barrier for NP penetration into nanotubes, which may provide theoretical guidance for separating two components using microfluidics.Halide double perovskites are an interesting alternative to Pb-containing counterparts as active materials in optoelectronic devices. Low-dimensional double perovskites are fabricated by introducing large organic cations, resulting in organic/inorganic architectures with one or more inorganic octahedra layers separated by organic cations. Here, we synthesized layered double perovskites based on 3D Cs2AgBiBr6, consisting of double (2L) or single (1L) inorganic octahedra layers, using ammonium cations of different sizes and chemical structures. DSSCrosslinker Temperature-dependent Raman spectroscopy revealed phase transition signatures in both inorganic lattice and organic moieties by detecting variations in their vibrational modes. Changes in the conformational arrangement of the organic cations to an ordered state coincided with a phase transition in the 1L systems with the shortest ammonium moieties. Significant changes of photoluminescence intensity observed around the transition temperature suggest that optical properties may be affected by the octahedral tilts emerging at the phase transition.The asymmetric synthesis of chiral benzo-ring containing compounds through enantioselective intramolecular arylation of unbiased methylene C(sp3)-H bonds was reported. Judicious choice of non-C2-symmetric chiral phosphoric acid (CPA) ligand is crucial for the high reactivity and enantioselectivity. The slight decrease in enantioselectivity at the late stage of the reaction was attributed to the hydrolysis of CPA ligands to the corresponding BINOL.In parallel to the burgeoning field of soft electronics, soft plasmonics focuses on the design and fabrication of plasmonic structures supported on elastomers and to understand how their properties respond to mechanical deformations. Here, we report on a partial ligand-stripping strategy to fabricate elastomer-supported gold nanobipyramid (NBP) plasmene nanosheets. Unlike spherelike building blocks, NBP-building blocks display complex orientation-dependent plasmonic responses to external strains. By collecting polarized plasmonic resonance spectra in conjunction with electrostatic eigenmode modeling, we reveal simultaneous changes in interparticle spacing and spatial orientations of NBP building blocks under mechanical strains. Such changes are directly related to initial NBP packing orders. Further analysis of strain sensitivities for various NBP plasmenes indicated that plasmonic spectra of ∼45° oriented samples are mostly susceptible to strain at acute polarized angles. The results presented may enable novel applications in future soft optoelectronic devices in sensing, encryption, and data storage.An efficient and straightforward gold-catalyzed protocol for the synthesis of 2-substituted 4-oxo-4-arylbutanal derivatives from commercially available or easily accessible alkynes and vinylsulfoxide substrates has been developed. Extension of the methodology to the use of 1-cycloalkenyl sulfoxides allowed the facile synthesis of five-, six-, and seven-membered-ring cycloalkyl-1-one backbone. Subsequently, the tetrahydrocycloalkyl[b]pyrrole derivatives, which are found in many active pharmaceutical ingredients, were isolated in good yields. Mechanistic investigation highlighted a [3,3]-sigmatropic rearrangement of a sulfonium intermediate in this process.