Talleynygaard2059

Here, we describe the rhodium-catalyzed bridged (3+2) cycloaddition cascade reactions of N-sulfonyl-1,2,3-triazoles, which allowed the efficient diastereoselective construction of various functionalized and synthetically challenging bridged ring systems. This simple, direct transformation had a broad substrate scope and excellent functional group tolerance. The highly strained polycyclic bicyclo[2.2.2]octa[b]indole core of fruticosine was synthesized efficiently using this methodology.The Landsberg limit represents the ultimate efficiency limit of solar energy harvesting. Reaching this limit requires the use of nonreciprocal elements. The existing device configurations for attaining the Landsberg limit, however, are very complicated. Here, we introduce the concept of a nonreciprocal multijunction solar cell and show that such a cell can reach the Landsberg limit in the idealized situation where an infinite number of layers are used. We also show that such a nonreciprocal multijunction cell outperforms a standard reciprocal multijunction cell for a finite number of layers. Our work significantly simplifies the device configuration required to reach the ultimate limit of solar energy conversion and points to a pathway toward using nonreciprocity to improve solar energy harvesting.Inspired by the brain, future computation depends on creating a neuromorphic device that is energy-efficient for information processing and capable of sensing and learning. The current computation-chip platform is not capable of self-power and neuromorphic functionality; therefore, a need exists for a new platform that provides both. This Perspective illustrates potential transparent photovoltaics as a platform to achieve scalable, multimodal sensory, self-sustainable neural systems (e.g., visual cortex, nociception, and electronic skin). We present herein a strategy to harvest solar power using a transparent photovoltaic device that provides neuromorphic functionality to implement versatile, sustainable, integrative, and practical applications. The proposed solid-inorganic heterostructure platform is indispensable for achieving a variety of biosensors, sensory systems, neuromorphic computing, and machine learning.The therapeutic effects of Δ9-tetrahydrocannabinol (Δ9-THC) can be enhanced by modifications of the pentyl moiety at C-3. The engineering of Cannabis sativa olivetolic acid cyclase and tetraketide synthase with F24I and L190G substitutions, respectively, in the biosynthesis of Δ9-THC serves as a platform for the generation of resorcylic acids up to 6-undecylresorcylic acid. These results provide insights into the development of THC analogs with chemically distinct acyl moieties at C-3.Using light scattering (LS), small-angle X-ray scattering (SAXS), and coarse-grained Monte Carlo (MC) simulations, we studied the self-interactions of two monoclonal antibodies (mAbs), PPI03 and PPI13. With LS measurements, we obtained the osmotic second virial coefficient, B22, and the molecular weight, Mw, of the two mAbs, while with SAXS measurements, we studied the mAbs' self-interaction behavior in the high protein concentration regime up to 125 g/L. Through SAXS-derived coarse-grained representations of the mAbs, we performed MC simulations with either a one-protein or a two-protein model to predict B22. By comparing simulation and experimental results, we validated our models and obtained insights into the mAbs' self-interaction properties, highlighting the role of both ion binding and charged patches on the mAb surfaces. Our models provide useful information about mAbs' self-interaction properties and can assist the screening of conditions driving to colloidal stability.In this paper, we consider drops that are subjected to a gradually increasing lateral force and follow the stages of the motion of the drops. We show that the first time a drop slides as a whole is when the receding edge of the drop is pulled by the advancing edge (the advancing edge drags the receding edge). The generality of this phenomenon includes sessile and pendant drops and spans over various chemically and topographically different cases. Because this observation is true for both pendant and sessile cases, we exclude hydrostatic pressure as its reason. Instead, we explain it in terms of the wetting adaptation and interfacial modulus, that is, the difference in the energies of the solid interface at the advancing and receding edges. At the receding edge, a slight motion exposes to the air a recently wetted solid surface whose molecules had reoriented to the liquid and will take time to reorient back to the air. This results in a high surface energy at the solid-air interface which pulls on the triple line, that is, inhibits the motion of the receding edge. On the other hand, at the advancing edge, a slight advancement does not change the nature of the solid interfacial molecules outside the drop, and the advancing side's sliding can continue. Moreover, the solid molecules under the drop at the advancing edge take time to reorient, and hence, their configuration is not yet adapted for the liquid and therefore not adapted for retention of the advancing edge. selleck chemical Therefore, in sliding-drop experiments, the advancing edge moves before the receding one, typically a few times before the receding edge moves. For the same reason, the last motion of the receding edge usually happens as a result of the advancing edge pulling on it.The hydration of ketones is known to occur in condensed phases, but it is not considered to be favorable in the gas phase due to restricted water content. We report the first evidence of geminal diol formation upon ketone hydration in the gas phase, obtained through the investigation of the interactions of cyclooctanone with water using broadband rotational spectroscopy. Oxygen-atom exchange between water and cyclooctanone was observed for two isomers of cyclooctanone-H2O and two isomers of cyclooctanone-(H2O)2. All complexes were unambiguously identified from the analysis of the rotational spectrum of the parent species and all their 13C and 18O isotopologues, and their heavy-atom substitution and effective structures were determined as well as their binding interactions. The production of gem-diols from gas-phase hydration of ketones has implications for atmospheric chemistry and opens a new channel for secondary aerosol formation.Lead-based halide perovskite nanocrystals (NCs) are recognized as emerging emissive materials with superior photoluminescence (PL) properties. However, the toxicity of lead and the swift chemical decomposition under atmospheric moisture severely hinder their commercialization process. Herein, we report the first colloidal synthesis of lead-free Cs4CuIn2Cl12 layered double perovskite NCs via a facile moisture-assisted hot-injection method stemming from relatively nontoxic precursors. Although moisture is typically detrimental to NC synthesis, we demonstrate that the presence of water molecules in Cs4CuIn2Cl12 synthesis enhances the PL quantum yield (mainly in the near-UV range), induces a morphological transformation from 3D nanocubes to 2D nanoplatelets, and converts the dark transitions to radiative transitions for the observed self-trapped exciton relaxation. This work paves the way for further studies on the moisture-assisted synthesis of novel lead-free halide perovskite NCs for a wide range of applications.Apolipoprotein B-100 (apo B-100) is the protein moiety of both low- and very-low-density lipoproteins, whose role is crucial to cholesterol and triglyceride transport. Aiming at the molecular dynamics' details of apo B-100, scarcely studied, we performed elastic and quasi-elastic incoherent neutron scattering (EINS, QENS) experiments combining different instruments and time scales. Similar to classical membrane proteins, the solubilization results in remaining detergent, here Nonidet P-40 (NP40). Therefore, we propose a framework for QENS studies of protein-detergent complexes, with the introduction of a combined model, including the experimental apo B-100/NP40 ratio. Relying on the simultaneous analysis of all QENS amplitudes, this approach is sensitive enough to separate both contributions. Its application identified two points (i) apo B-100 slow dynamics and (ii) the acceleration of NP40 dynamics in the presence of apo B-100. Direct translation of the exposed methodology now makes the investigation of more membrane proteins by neutron spectroscopy achievable.Nonfullerene, a small molecular electron acceptor, has substantially improved the power conversion efficiency of organic photovoltaics (OPVs). However, the large structural freedom of π-conjugated polymers and molecules makes it difficult to explore with limited resources. Machine learning, which is based on rapidly growing artificial intelligence technology, is a high-throughput method to accelerate the speed of material design and process optimization; however, it suffers from limitations in terms of prediction accuracy, interpretability, data collection, and available data (particularly, experimental data). This recognition motivates the present Perspective, which focuses on utilizing the experimental data set for ML to efficiently aid OPV research. This Perspective discusses the trends in ML-OPV publications, the NFA category, and the effects of data size and explanatory variables (fingerprints or Mordred descriptors) on the prediction accuracy and explainability, which broadens the scope of ML and would be useful for the development of next-generation solar cell materials.Ab initio coupled-cluster, electron propagator, and Møller-Plesset second-order perturbation theory calculations are utilized to analyze the low-lying electronic states of several metal-doped B20. In the ground state, the presently focused AB20/EB20 (A = Li, Na, and K; E = Mg and Ca) consist of charge-separated A+B20-/E2+B202- frameworks. The excited electronic states of AB20 and EB20+ were analyzed by computing the vertical electron attachment energies (VEAEs) of AB20+ and EB202+. In several excited states, the radical electron is predominantly localized on the B20 frames, which are counterparts of the low-lying states of bare B20-. A variety of basis sets were tested on obtaining VEAEs, and the aug-cc-pVDZ/A,E d-aug-cc-pVDZ/B combination provided the best accuracy-efficiency compromise on them. Furthermore, this work analyzes the Rydberg-like excited states of AB20 and EB20+ and will serve as a guide for future studies on similar metal-doped boron systems.Due to chlorodifluoromethane's (CHClF2, HCFC-22) dual environmental impact on climate change and ozone depletion, its emissions have attracted international attention. In this study, a set of national-provincial-gridded (1° × 1°) emission estimation methods were built and applied to obtain the national, provincial, and gridded emission inventories in China in 1990-2019. In addition, the HCFC-22 emission reduction potential of different emission scenarios was analyzed. The results show that China's HCFC-22 emissions reached a peak in 2017 and that the cumulative emissions in 1990-2019 were 1576.8 (1348.2-1819.0) kt (equivalent to 86.7 kt CFC-11 and 2854.1 Mt CO2). China's HCFC-22 emissions in the east were higher than those in the west, and the emissions in the south were higher than those in the north. Under the control of the Montreal Protocol, China will reduce the cumulative emissions of 17 840.8 kt (avoiding 0.08° of global warming by 2056) in 2020-2056. If the disposal refrigerant can be effectively recycled in the future, the HCFC-22 emission reduction in this period will reach 18 020.