Concomitant formation of protocells and prebiotic compounds under a plausible early Earth atmosphere.

Revealing the origin of life and unambiguously detecting fossil remains of the earliest organisms are closely related aspects of the same scientific research. The synthesis of prebiotic molecular building blocks of life and the first compartmentalization into protocells have been considered two events apart in time, space, or both. We conducted lightning experiments in borosilicate reactors filled with a mixture of gases mimicking plausible geochemical conditions of early Earth.

Evidence for a metal-bosonic insulator-superconductor transition in compressed sulfur.

The abrupt drop of resistance to zero at a critical temperature is a key signature of the current paradigm of the metal-superconductor transition. However, the emergence of an intermediate bosonic insulating state characterized by a resistance peak preceding the onset of the superconducting transition has challenged this traditional understanding. Notably, this phenomenon has been predominantly observed in disordered or chemically doped low-dimensional systems, raising intriguing questions about the generality of the effect and its underlying fundamental physics.

Genesis and regulation of C-terminal cyclic imides from protein damage.

C-Terminal cyclic imides are posttranslational modifications that can arise from spontaneous intramolecular cleavage of asparagine or glutamine residues resulting in a form of irreversible protein damage. These protein damage events are recognized and removed by the E3 ligase substrate adapter cereblon (CRBN), indicating that these aging-related modifications may require cellular quality control mechanisms to prevent deleterious effects. However, the factors that determine protein or peptide susceptibility to C-terminal cyclic imide formation or their effect on protein stability have not been explored in detail.

A hybrid meta on-top functional for multiconfiguration pair-density functional theory.

Multiconfiguration pair-density functional theory (MC-PDFT) was proposed a decade ago, but it is still in the early stage of density functional development. MC-PDFT uses functionals that are called on-top functionals; they depend on the density and the on-top pair density. Most MC-PDFT calculations to date have been unoptimized translations of generalized gradient approximations (GGAs) of Kohn-Sham density functional theory (KS-DFT).

Liquid-nano-liquid interface-oriented anisotropic encapsulation.

Emulsion interface engineering has been widely employed for the synthesis of nanomaterials with various morphologies. However, the instability of the liquid-liquid interface and uncertain interfacial interactions impose significant limitations on controllable fabrications. Here, we developed a liquid-nano-liquid interface-oriented anisotropic encapsulation strategy for fabricating asymmetric nanohybrids.

Pseudogap in electron-doped cuprates: Strong correlation leading to band splitting.

The pseudogap phenomena have been a long-standing mystery of the cuprate high-temperature superconductors. The pseudogap in the electron-doped cuprates has been attributed to band folding due to antiferromagnetic (AFM) long-range order or short-range correlation. We performed an angle-resolved photoemission spectroscopy study of the electron-doped cuprates PrLaCeCuO showing spin-glass, disordered AFM behaviors, and superconductivity at low temperatures and, by measurements with fine momentum cuts, found that the gap opens on the unfolded Fermi surface rather than the AFM Brillouin zone boundary.

Integrating climate and physical constraints into assessments of net capture from direct air capture facilities.

Limiting climate change to targets enshrined in the Paris Agreement will require both deep decarbonization of the energy system and the deployment of carbon dioxide removal at potentially large scale (gigatons of annual removal). Nations are pursuing direct air capture to compensate for inertia in the expansion of low-carbon energy systems, decarbonize hard-to-abate sectors, and address legacy emissions. Global assessments of this technology have failed to integrate factors that affect net capture and removal cost, including ambient conditions like temperature and humidity, as well as emission factors of electricity and natural gas systems.

Electron transfer in polysaccharide monooxygenase catalysis.

Polysaccharide monooxygenase (PMO) catalysis involves the chemically difficult hydroxylation of unactivated C-H bonds in carbohydrates. The reaction requires reducing equivalents and will utilize either oxygen or hydrogen peroxide as a cosubstrate. Two key mechanistic questions are addressed here: 1) How does the enzyme regulate the timely and tightly controlled electron delivery to the mononuclear copper active site, especially when bound substrate occludes the active site? and 2) How does this electron delivery differ when utilizing oxygen or hydrogen peroxide as a cosubstrate? Using a computational approach, potential paths of electron transfer (ET) to the active site copper ion were identified in a representative AA9 family PMO from (PMO9E).

Advancing the Mechanosensitivity of Atropisomeric Diarylethene Mechanophores through a Lever-Arm Effect.

Understanding structure-mechanical activity relationships (SMARs) in polymer mechanochemistry is essential for the rational design of mechanophores with desired properties, yet SMARs in noncovalent mechanical transformations remain relatively underexplored. In this study, we designed a subset of diarylethene mechanophores based on a lever-arm hypothesis and systematically investigated their mechanical activity toward a noncovalent-yet-chemical conversion of atropisomer stereochemistry. Results from Density functional theory (DFT) calculations, single-molecule force spectroscopy (SMFS) measurements, and ultrasonication experiments collectively support the lever-arm hypothesis and confirm the exceptional sensitivity of chemo-mechanical coupling in these atropisomers.

PM2.5 Speciation chemicals and Neonatal Respiratory Distress Syndrome (RDS): Uncovering the Interactions of Maternal Health, Environmental metal pollutants, and Sociodemographic Factors.

Objective: To assess factors influencing Neonatal Respiratory Distress Syndrome (RDS) risk, incorporating maternal demographics, behaviors, medical conditions, pregnancy-related factors, and PM2.5 speciation pollutants exposures.

Methods: Using Florida de-identified birth records, logistic regression analyses were conducted to assess associations between maternal exposure to PM2.

Dual-Anion-Rich Polymer Electrolytes for High-Voltage Solid-State Lithium Metal Batteries.

Solid polymer electrolytes (SPEs) are promising candidates for lithium metal batteries (LMBs) owing to their safety features and compatibility with lithium metal anodes. However, the inferior ionic conductivity and electrochemical stability of SPEs hinder their application in high-voltage solid-state LMBs (HVSSLMBs). Here, a strategy is proposed to develop a dual-anion-rich solvation structure by implementing ferroelectric barium titanate (BTO) nanoparticles (NPs) and dual lithium salts into poly(vinylidene fluoride) (PVDF)-based SPEs for HVSSLMBs.

Voices of Nanomedicine: Blueprint Guidelines for Collaboration in Addressing Global Unmet Medical Needs.

The "" under this Perspective underline the importance of interdisciplinary collaboration and partnerships across several disciplines, such as medical science and technology, medicine, bioengineering, and computational approaches, in bridging the gap between research, manufacturing, and clinical applications. Effective communication is key to bridging team gaps, enhancing trust, and resolving conflicts, thereby fostering teamwork and individual growth toward shared goals. Drawing from the success of the COVID-19 vaccine development, we advocate the application of similar collaborative models in other complex health areas such as nanomedicine and biomedical engineering.

Enhancing air quality predictions in Chile: Integrating ARIMA and Artificial Neural Network models for Quintero and Coyhaique cities.

In this comprehensive analysis of Chile's air quality dynamics spanning 2016 to 2021, the utilization of data from the National Air Quality Information System (SINCA) and its network of monitoring stations was undertaken. Quintero, Puchuncaví, and Coyhaique were the focal points of this study, with the primary objective being the construction of predictive models for sulfur dioxide (SO2), fine particulate matter (PM2.5), and coarse particulate matter (PM10).

Deciphering the Energy Transfer Mechanism Across Metal Halide Perovskite-Phthalocyanine Interfaces.

Energy transfer processes in nanohybrids are at the focal point of conceptualizing, designing, and realizing novel energy-harvesting systems featuring nanocrystals that absorb photons and transfer their energy unidirectionally to surface-immobilized functional dyes. Importantly, the functionality of these dyes defines the ultimate application. Herein, CsPbBr perovskite nanocrystals (NCs) are interfaced with zinc phthalocyanine (ZnPc) dyes featuring carboxylic acid.

Analyzing Atomic Interactions in Molecules as Learned by Neural Networks.

While machine learning (ML) models have been able to achieve unprecedented accuracies across various prediction tasks in quantum chemistry, it is now apparent that accuracy on a test set alone is not a guarantee for robust chemical modeling such as stable molecular dynamics (MD). To go beyond accuracy, we use explainable artificial intelligence (XAI) techniques to develop a general analysis framework for atomic interactions and apply it to the SchNet and PaiNN neural network models. We compare these interactions with a set of fundamental chemical principles to understand how well the models have learned the underlying physicochemical concepts from the data.

Precise Sizing and Collision Detection of Functional Nanoparticles by Deep Learning Empowered Plasmonic Microscopy.

Single nanoparticle analysis is crucial for various applications in biology, materials, and energy. However, precisely profiling and monitoring weakly scattering nanoparticles remains challenging. Here, it is demonstrated that deep learning-empowered plasmonic microscopy (Deep-SM) enables precise sizing and collision detection of functional chemical and biological nanoparticles.

Skin-Integrated Electrogenetic Regulation of Vasculature for Accelerated Wound Healing.

Neo-vascularization plays a key role in achieving long-term viability of engineered cells contained in medical implants used in precision medicine. Moreover, strategies to promote neo-vascularization around medical implants may also be useful to promote the healing of deep wounds. In this context, a biocompatible, electroconductive borophene-poly(ε-caprolactone) (PCL) 3D platform is developed, which is called VOLT, to support designer cells engineered with a direct-current (DC) voltage-controlled gene circuit that drives secretion of vascular endothelial growth factor A (VEGFA).

Evaluation of Larger Side-Group Functionalities and the Side/End-Group Interplay in Ritonavir-Like Inhibitors of CYP3A4.

A new series of 13 ritonavir-like inhibitors of human drug-metabolizing CYP3A4 was rationally designed to study the R side-group and R end-group interplay when the R side-group is represented by phenyl. Spectral, functional, and structural characterization showed no improvement in the binding affinity and inhibitory potency of R/R-phenyl inhibitors upon elongation and/or fluorination of R-Boc (tert-butyloxycarbonyl) or its replacement with benzenesulfonyl. When R is pyridine, the impact of R-phenyl-to-indole/naphthalene substitution was multidirectional and highly dependent on side-group stereo configuration.

Theoretical Understanding of Photoluminescence and Singlet Oxygen Quantum Yields in a Few Halogenated Fluorescein Dyes.

Visible-light absorbing metal-free organic dyes are of increasing demand for various optoelectronic applications because of their great structure-function tunability through chemical means. Several dyes also show huge potential in triplet photosensitization, generating reactive singlet oxygen. Understanding the structure-property relationships of many well-known fluorescein dyes is of paramount importance in designing next-generation energy efficient dyes, which is currently limited.

Large enhancement of ferroelectric properties of perovskite oxides via nitrogen incorporation.

Perovskite oxides have a wide variety of physical properties that make them promising candidates for versatile technological applications including nonvolatile memory and logic devices. Chemical tuning of those properties has been achieved, to the greatest extent, by cation-site substitution, while anion substitution is much less explored due to the difficulty in synthesizing high-quality, mixed-anion compounds. Here, nitrogen-incorporated BaTiO thin films have been synthesized by reactive pulsed-laser deposition in a nitrogen growth atmosphere.

Redesigning protonic ceramic electrochemical cells to lower the operating temperature.

Protonic ceramic electrochemical cells (PCECs) can operate at intermediate temperatures (450° to 600°C) for power generation and hydrogen production. However, the operating temperature is still too high to revolutionize ceramic electrochemical cell technology. Lowering the operating temperature to <450°C will enable a wider material choice and reduce system costs.

Molecular dynamics at immune synapse lipid rafts influence the cytolytic behavior of CAR T cells.

Chimeric antigen receptor T cells (CART) targeting CD19 through CD28.ζ signaling induce rapid lysis of leukemic blasts, contrasting with persistent tumor control exhibited by 4-1BB.ζ-CART.

Sequential Targeting Chondroitin Sulfate-Bilirubin Nanomedicine Attenuates Osteoarthritis via Reprogramming Lipid Metabolism in M1 Macrophages.

The infiltration and excessive polarization of M1 macrophages contribute to the induction and persistence of low-grade inflammation in joint-related degenerative diseases such as osteoarthritis (OA). The lipid metabolism dysregulation promotes M1 macrophage polarization by coordinating the compensatory pathways of the inflammatory and oxidative stress responses. Here, a self-assembling, licofelone-loaded nanoparticle (termed LCF-CSBN), comprising chondroitin sulfate and bilirubin joined by an ethylenediamine linker, is developed to selectively reprogram lipid metabolism in macrophage activation.

High-Resolution Mapping of Photocatalytic Activity by Diffusion-Based and Tunneling Modes of Photo-Scanning Electrochemical Microscopy.

Semiconductor nanomaterials and nanostructured interfaces have important technological applications, ranging from fuel production to electrosynthesis. Their photocatalytic activity is known to be highly heterogeneous, both in an ensemble of nanomaterials and within a single entity. Photoelectrochemical imaging techniques are potentially useful for high-resolution mapping of photo(electro)catalytic active sites; however, the nanoscale spatial resolution required for such experiments has not yet been attained.