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Intramolecular Oxa-Michael Reactions of Aldols Generated from Enones and Isatins to Afford Spirooxindole Tetrahydropyrans
Get PDFSpirooxindole derivatives are found in bioactive natural products and are used in drug discovery and related research. Here, acid-catalyzed diastereoselective intramolecular oxa-Michael cyclization reactions of β-hydroxyenones generated from enones and isatin derivatives that afford spirooxindole tetrahydropyranes are reported. The major diastereomers of the products of these reactions were previously difficult to access by the amine-catalyzed hetero-Diels-Alder reactions of enones with isatins. With the use of enantiomerically enriched forms of the starting materials in the reactions, enantiomerically enriched spirooxindole tetrahydropyranes that retained the enantiopurities of the starting materials were obtained.journal articl
Evolution of a multifunctional trait: shared effects of foraging ecology and thermoregulation on beak morphology, with consequences for song evolution
Get PDFWhile morphological traits are often associated with multiple functions, it remains unclear how evolution balances the selective effects of different functions. Birds' beaks function not only in foraging but also in thermoregulating and singing, among other behaviours. Studies of beak evolution abound, however, most focus on a single function. Hence, we quantified relative contributions of different functions over an evolutionary timescale. We measured beak shape using geometric morphometrics and compared this trait with foraging behaviour, climatic variables and song characteristics in a phylogenetic comparative study of an Australasian radiation of songbirds (Meliphagidae). We found that both climate and foraging behaviour were significantly correlated with the beak shape and size. However, foraging ecology had a greater effect on shape, and climate had a nearly equal effect on size. We also found that evolutionary changes in beak morphology had significant consequences for vocal performance: species with elongate-shaped beaks sang at higher frequencies, while species with large beaks sang at a slower pace. The evolution of the avian beak exemplifies how morphological traits can be an evolutionary compromise among functions, and suggests that specialization along any functional axis may increase ecological divergence or reproductive isolation along others.journal articl
Stable Nickel(I) Complexes with Electron-Rich, Sterically-Hindered, Innocent PNP Pincer Ligands
Get PDFThe electronic and steric properties of a new class of electron-rich and sterically hindered tertamethylated PNP pincer ligands (Me4PNPR = 2,6-bisRdialkylphosphino)propylipyridine with R = Pr-i, Bu-t) are discussed. Introducing the methyl groups on the pincer arm prevents dearomatization of the pincer framework and increases the bulkiness and electron-donating capacity of the ligand. Highly reactive Ni-I species are thus prevented from dimerizing and can be analyzed by a wide variety of spectroscopic methods. X-ray diffraction study shows that steric bulk has an important influence on the resulting geometric and spectroscopic properties of the Ni-I complexes. Complexes S and 6, which contain Pr-i groups on the phosphorus atoms, show a very rare seesaw geometry around the metal center, while Bu-t complexes 7 and 8 show a distorted square-planar geometry. Computational analysis reveals that the SOMO for all complexes has a d(x)(-y)(2)(2) character with the spin density mostly residing on the nickel.journal articl
Driving Interactions Efficiently in a Composite Few-Body System
Get PDFWe study how to efficiently control an interacting few-body system consisting of three harmonically trapped bosons. Specifically, we investigate the process of modulating the inter-particle interactions to drive an initially non-interacting state to a strongly interacting one, which is an eigenstate of a chosen Hamiltonian. We also show that for unbalanced subsystems, where one can individually control the different inter- and intra-species interactions, complex dynamics originate when the symmetry of the ground state is broken by phase separation. However, as driving the dynamics too quickly can result in unwanted excitations of the final state, we optimize the driven processes using shortcuts to adiabaticity, which are designed to reduce these excitations at the end of the interaction ramp, ensuring that the target eigenstate is reached.journal articl
Psychiatric-disorder-related behavioral phenotypes and cortical hyperactivity in a mouse model of 3q29 deletion syndrome
Get PDF3q29 microdeletion, a rare recurrent copy number variant (CNV), greatly confers an increased risk of psychiatric disorders, such as schizophrenia and autism spectrum disorder (ASD), as well as intellectual disability. However, disease-relevant cellular phenotypes of 3q29 deletion syndrome remain to be identified. To reveal the molecular and cellular etiology of 3q29 deletion syndrome, we generated a mouse model of human 3q29 deletion syndrome by chromosome engineering, which achieved construct validity. 3q29 deletion (Df/+) mice showed reduced body weight and brain volume and, more importantly, impaired social interaction and prepulse inhibition. Importantly, the schizophrenia-related impaired prepulse inhibition was reversed by administration of antipsychotics. These findings are reminiscent of the growth defects and neuropsychiatric behavioral phenotypes in patients with 3q29 deletion syndrome and exemplify that the mouse model achieves some part of face validity and predictive validity. Unbiased whole-brain imaging revealed that neuronal hyperactivation after a behavioral task was strikingly exaggerated in a restricted region of the cortex of Df/+ mice. We further elucidated the cellular phenotypes of neuronal hyperactivation and the reduction of parvalbumin expression in the cortex of Df/+ mice. Thus, the 3q29 mouse model provides invaluable insight into the disease-causative molecular and cellular pathology of psychiatric disorders.journal articl
Dewetting Metal Nanofilms—Effect of Substrate on Refractive Index Sensitivity of Nanoplasmonic Gold
Get PDFThe localized surface plasmon resonance (LSPR) sensitivity of metal nanostructures is strongly dependent on the interaction between the supporting substrate and the metal nanostructure, which may cause a change in the local refractive index of the metal nanostructure. Among various techniques used for the development of LSPR chip preparation, solid-state dewetting of nanofilms offers fast and cost effective methods to fabricate large areas of nanostructures on a given substrate. Most of the previous studies have focused on the effect of the size, shape, and inter-particle distance of the metal nanostructures on the LSPR sensitivity. In this work, we reveal that the silicon-based supporting substrate influences the LSPR associated refractive index sensitivity of gold (Au) nanostructures designed for sensing applications. Specifically, we develop Au nanostructures on four different silicon-based ceramic substrates (Si, SiO2, Si3N4, SiC) by thermal dewetting process and demonstrate that the dielectric properties of these ceramic substrates play a key role in the LSPR-based refractive index (RI) sensitivity of the Au nanostructures. Among these Si-supported Au plasmonic refractive index (RI) sensors, the Au nanostructures on the SiC substrates display the highest average RI sensitivity of 247.80 nm/RIU, for hemispherical Au nanostructures of similar shapes and sizes. Apart from the significance of this work towards RI sensing applications, our results can be advantageous for a wide range of applications where sensitive plasmonic substrates need to be incorporated in silicon based optoelectronic devices.journal articl
Review of the Arabian Crematogaster Lund (Hymenoptera, Formicidae), synoptic list, distribution, and description of two new species from Oman and Saudi Arabia
Get PDFThe genus Crematogaster is one of the most species-rich and widespread groups of ants. Despite their often-high local abundance and important ecological interactions, the taxonomy of the genus is fragmentary and in great need of modern revisionary studies. As a first step towards a revision for the Arabian fauna of Crematogaster, a review of all known species with synoptic species accounts is provided. Seventeen species are recognized and illustrated from the Arabian Peninsula, of which two new species are described: C. jacindae Sharaf & Hita Garcia, sp. nov. from the Dhofar Governorate, Oman, and C. gryllsi Sharaf & Hita Garcia, sp. nov. from the Kingdom of Saudi Arabia (KSA) based on the worker caste. Crematogaster jacindae sp. nov. is easily separated from the remainder of the Arabian Crematogaster fauna due to its complete lack of propodeal spines, slit-shaped propodeal spiracles, and its distinct bicoloration, whereas C. gryllsi sp. nov. is readily distinguished by its unlobed postpetiolar dorsum. Furthermore, new country records are presented: C. acaciae Forel for the KSA and Yemen, and C. delagoensis Forel and C. jehovae Forel for the KSAC. antaris for Qatar, whereas C. luctans Forel is excluded from the Arabian fauna. In addition, on the basis of morphological examination of original type material, C. affabilis Forel is proposed as junior synonym of C. chiarinii Mayr, and C. striaticeps is elevated to species rank stat. nov. Furthermore, a new identification key for the Arabian species is provided, as well as distribution maps for all species.journal articl
Purely Elastic Fluid–Structure Interactions in Microfluidics: Implications for Mucociliary Flows
Get PDFFluid-structure interactions lie at the heart of the complex, and often highly coordinated, motions of actively driven microscale biological systems (e.g., translating cilia, flagella, and motile cells). Due to the highly viscoelastic nature of most relevant biological fluids and the small length scales involved, the viscous and inertial forces in such flows are dominated by elasticity. However, elastic effects are often overlooked in studies seeking to address phenomena like the synchronization of beating cilia. In this study, unique microfluidic experiments are presented to demonstrate that inertia-free viscoelastic flows can lead to highly regular beating of an immersed (passive) flexible structure, herein named "purely-elastic" fluid-structure interaction. It is also shown how two such flexible structures can achieve an extraordinary degree of synchronization, with a correlation coefficient approaching unity. The synchronization is a result of the generation of localized elastic stresses in the fluid that effectively link the two objects. These purely elastic interactions may be important to consider toward developing a complete understanding of the motions of microscale biological systems.journal articl
Specific Recognition of Promoter G-Quadruplex DNAs by Small Molecule Ligands and Light-up Probes
Get PDFG-Quadruplexes (G4s) are four-stranded nucleic acid structures whose underlying G-rich sequences are present across the chromosome and transcriptome. These highly structured elements are known to regulate many key biological functions such as replication, transcription, translation, and genomic stability, thereby providing an additional layer of gene regulation. G4s are structurally dynamic and diverse, and they can fold into numerous topologies. They are potential targets for small molecules, which can modulate their functions. To this end, myriad classes of small molecules have been developed and studied for their ability to bind and stabilize these unique structures. Though many of them can selectively target G4s over duplex DNA, only a few of them can distinguish one G4 topology from others. Design and development of G4-specific ligands are challenging owing to the subtle structural variations among G4 structures. However, screening assays and computational methods have identified a few classes of ligands that preferentially or specifically target the G4 topology of interest over others. This review focuses on the small molecules and fluorescent probes that specifically target human promoter G4s associated with oncogenes. Targeting promoter G4s could circumvent the issues such as undruggability and development of drug resistance associated with the protein targets. The ligands discussed here highlight that development of G4-specific ligands is an achievable goal in spite of the limited structural data available. The future goal is to pursue the development of G4-specific ligands endowed with drug-like properties for G4-based therapeutics and diagnostics.journal articl
Recent Progress of All‐Bromide Inorganic Perovskite Solar Cells
Get PDFInorganic perovskite solar cells (PSCs) have attracted enormous attention during the past 5 years. Many advanced strategies and techniques have been developed for fabricating inorganic PSCs with improved efficiency and stability to realize commercial applications. CsPbBr3 is one of the representative materials of inorganic perovskites and has demonstrated excellent stability against thermal and high humidity environmental conditions. The power conversion efficiency of CsPbBr3-based PSCs has increased significantly from 5.95% in 2015 to 10.91%, and the storage stability under moisture (approximate to 80% relative humidity) and heat (approximate to 80 degrees C) is more than 2000 h. The outstanding performance of CsPbBr3 PSCs shows great potential in light-to-electricity conversion applications. In this review, recent developments of CsPbBr3-based PSCs including the physico-chemical as well as optoelectronic properties, processing techniques for fabricating CsPbBr3 films, derivative phase structures, efficiency, and stability of devices are reviewed and discussed. Finally, the challenges and outlook of CsPbBr3 PSCs for future research directions are outlined.journal articl