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Abstract A recent publication by Wu and co‐workers demonstrated that the workhorse functional B3LYP tends to overemphasize the delocalization in antiaromatic molecules, leading to poor agreement between the calculated proton NMR values and the experimentally obtained numbers. Rather, they showed that the M11 functional affords the best agreement between theory and experiment. We have computationally re‐examined our previously published NICS‐XY scan data using M11‐determined geometries and find that, aside from the placement ofs‐indacene, the antiaromaticity trends for both sets of data are essentially identical. 

Abstract Herein we report the synthesis and characterization of four donor/acceptor‐fuseds‐indacenes via the late‐stage oxidation of a family of unsymmetrical benzofuran/benzothiophene‐s‐indacene regioisomers. A thorough study of their properties through experimental and computational analysis has revealed the effect of asymmetry on the molecular properties associated with antiaromaticity, as well as a strong correlation between antiaromaticity and intramolecular charge transfer (ICT). The strength of the charge transfer depends on the fusion orientation of the donor and acceptor motifs relative to thes‐indacene core. The two most antiaromatic oxidized isomers exhibit strong evidence of ICT with 30 and 40 nm solvatochromic shifts. 

Abstract Interfacial self‐assembly describes the directed organization of molecules and colloids at phase boundaries. Believed to be fundamental to the inception of primordial life, interfacial assembly is exploited by a myriad of eukaryotic and prokaryotic organisms to execute physiologic activities and maintain homeostasis. Inspired by these natural systems, chemists, engineers, and materials scientists have sought to harness the thermodynamic equilibria at phase boundaries to create multi‐dimensional, highly ordered, and functional nanomaterials. Recent advances in our understanding of the biophysical principles guiding molecular assembly at gas–solid, gas–liquid, solid–liquid, and liquid–liquid interphases have enhanced the rational design of functional bio‐nanomaterials, particularly in the fields of biosensing, bioimaging and biotherapy. Continued development of non‐canonical building blocks, paired with deeper mechanistic insights into interphase self‐assembly, holds promise to yield next generation interfacial bio‐nanomaterials with unique, and perhaps yet unrealized, properties. This article is categorized under:Nanotechnology Approaches to Biology > Nanoscale Systems in BiologyTherapeutic Approaches and Drug Discovery > Emerging Technologies 

The human colon is home to trillions of microorganisms that modulate gastrointestinal physiology. The understanding of how this gut ecosystem impacts human health, although evolving, is slowed by the lack of accessible tools suitable to studying complex host‐mucus‐microbe interactions. Here, a synthetic gel‐like material capable of recapitulating the varied structural, mechanical, and biochemical profiles of native human colonic mucus is reported to develop compositionally simple microbiome screening platforms with utility in microbiology and drug discovery. The viscous fibrillar material is realized through templated assembly of a fluorine‐rich amino acid at liquid‐liquid interphases. The fluorine‐assisted mucus surrogate (FAMS) can be decorated with mucins to serve as a habitat for microbial colonization and integrated with human colorectal cells to generate artificial mucosae, referred to as a microbiome organoid. Notably, FAMS are made with inexpensive and commercially available materials and can be generated using simple protocols and standard laboratory hardware. As a result, this platform can be broadly incorporated into various laboratory settings to advance probiotic research and inform in vivo approaches. If implemented into high throughput screening approaches, FAMS may represent a valuable tool to study compound metabolism and gut permeability, with an exemplary demonstration of this utility presented here. 

Abstract This paper explicates a solution to building correspondences between molecular-scale transcriptomics and tissue-scale atlases. This problem arises in atlas construction and cross-specimen/technology alignment where specimens per emerging technology remain sparse and conventional image representations cannot efficiently model the high dimensions from subcellular detection of thousands of genes. We address these challenges by representing spatial transcriptomics data as generalized functions encoding position and high-dimensional feature (gene, cell type) identity. We map onto low-dimensional atlas ontologies by modeling regions as homogeneous random fields with unknown transcriptomic feature distribution. We solve simultaneously for the minimizing geodesic diffeomorphism of coordinates through LDDMM and for these latent feature densities. We map tissue-scale mouse brain atlases to gene-based and cell-based transcriptomics data from MERFISH and BARseq technologies and to histopathology and cross-species atlases to illustrate integration of diverse molecular and cellular datasets into a single coordinate system as a means of comparison and further atlas construction.