Guerreroebsen3867

Silicon nitride (SiN) mechanical resonators with high quality mechanical properties are attractive for fundamental research and applications. However, it is challenging to maintain these mechanical properties while achieving strong coupling to an electrical circuit for efficient on-chip integration. Here, we present a SiN drum resonator covered with an aluminum thin film, enabling large capacitive coupling to a suspended top-gate. Implementing the full electrical measurement scheme, we demonstrate a high quality factor ∼104 (comparable to that of bare drums at room temperature) and present our ability to detect ∼10 mechanical modes at low temperature. The drum resonator is also coupled to a microwave cavity, so that we can perform optomechanical sideband pumping with a fairly good coupling strength G and demonstrate mechanical parametric amplification. This SiN drum resonator design provides efficient electrical integration and exhibits promising features for exploring mode coupling and signal processing.The combination of palladium catalysis and thermal cycloaddition is shown to transform tricyclic aziridines into complex, stereodefined tetracyclic products in a single step. This highly unusual cascade process involves a diverted Tsuji-Trost sequence leading to a surprisingly facile intramolecular Diels-Alder reaction. The starting materials are accessible on multigram scales from the photochemical rearrangement of simple pyrroles. The tetracyclic amine products can be further elaborated through routine transformations, highlighting their potential as scaffolds for medicinal chemistry.Interaction of surface adsorbate vibration and intraband electron absorption in nanocrystals has been reported to affect the photophysical properties of both nanocrystals and surface adsorbates and may affect the performance of hybrid photocatalysts composed of semiconductor nanocrystals and molecular catalysts. Here, by combining ultrafast transient visible and IR spectroscopic measurements, we report the observation of Fano resonances between the intraband transition of the photogenerated electrons in CdS and CdSe nanocrystals and CO stretching vibrational modes of adsorbed molecular catalysts, [Fe2(cbdt)(CO)6] (FeFe; cbdt = 1-carboxyl-benzene-2,3-dithiolate), a molecular mimic for the active site of FeFe-hydrogenase. The occurrence of Fano resonances is independent of nanocrystal types (rods vs dots) or charge transfer character between the nanocrystal and FeFe, and is likely a general feature of nanocrystal and molecular catalyst hybrid systems. click here These results provide new insights into the fundamental interactions in these hybrid assemblies for artificial photosynthesis.The development of stable and efficient electrocatalysts is of key importance for the establishment of a sustainable society. The activity of a metal electrocatalyst is determined by its electrochemically active surface area and intrinsic activity, which can be increased using highly porous structures and heteroatomic doping, respectively. Herein, we propose a general strategy of generating mesopores and residual oxygen in metal electrocatalysts by reduction of metastable metal oxides using Ag2O3 electrodeposited onto carbon paper as a model system and demonstrating that the obtained multipurpose porous Ag electrocatalyst has high activity for the electroreduction of O2 and CO2. The presence of mesopores and residual oxygen is confirmed by electrochemical and spectroscopic techniques, and quantum mechanical simulations prove the importance of residual oxygen for electrocatalytic activity enhancement. Thus, the adopted strategy is concluded to allow the synthesis of highly active metal catalysts with controlled mesoporosity and residual oxygen content.Materials enabling impact-energy absorption of high-velocity projectiles are of great interest for applications like aerospace. In such a frame, shear thickening fluids were found very useful. Here, we investigated nanorheological properties of neat and aqueous polyelectrolytes of low molecular weights containing poly([2-(methacryloyloxy) ethyl] trimethyl ammonium) as polycations and poly(acrylamide-co-acrylic acid) as polyanions. Results were compared with pure water. We employed nonequilibrium molecular dynamics with the SLLOD algorithm to compute the viscosity at various shear rates. Systems containing polyelectrolytes exhibit shear thickening. The analysis of molecular configurations revealed a strong disruption of the ionic structure and more clusters with smaller sizes on increasing the shear rate. Potential energies showed that shear thickening originates from an increase in intramolecular and van der Waals interactions resulting from the increasing difficultly of polyelectrolyte-based systems to relax at high shear rates. Our method and findings underscore the importance of accounting for the molecular scale in the design of materials absorbing the impact energy efficiently.Photoredox-catalyzed C-O bond formation reactions are reported. The decarboxylative esterification reaction allows the conversion of a variety of arylacetic acids into the corresponding benzyl carboxylates. Furthermore, the use of (diacetoxyiodo)benzene allows the conversion of the benzylic C-H bond through hydrogen atom transfer. The reactions were applied to the divergent transformation of pharmaceuticals via decarboxylative or C-H esterification reactions.Photobioelectrocatalysis (PBEC) adopts the sophistication and sustainability of photosynthetic units to convert solar energy into electrical energy. However, the electrically insulating outer membranes of photosynthetic units hinder efficient extracellular electron transfer from photosynthetic redox centers to an electrode in photobioelectrocatalytic systems. Among the artificial redox-mediating approaches used to enhance electrochemical communication at this biohybrid interface, conducting redox polymers (CRPs) are characterized by high intrinsic electric conductivities for efficient charge transfer. A majority of these CRPs constitute peripheral redox pendants attached to a conducting backbone by a linker. The consequently branched CRPs necessitate maintaining synergistic interactions between the pendant, linker, and backbone for optimal mediator performance. Herein, an unbranched, metal-free CRP, polydihydroxy aniline (PDHA), which has its redox moiety embedded in the polymer mainchain, is used as an exogenous redox mediator and an immobilization matrix at the biohybrid interface.