Browse Articles

Sequential addition of cations increases photoluminescence quantum yield of metal nanoclusters near unity

AbstractPhotoluminescence is one of the most intriguing properties of metal nanoclusters derived from their molecular-like electronic structure, however, achieving high photoluminescence quantum yield (PLQY) of metal core-dictated fluorescence remains a formidable challenge. Here, we report efficient suppression of the total structural vibrations and rotations, and management of the pathways and rates of the electron transfer dynamics to boost a near-unity absolute PLQY, by decorating progressive addition of cations. Specifically, with the sequential addition of Zn2+, Ag+, and Tb3+ into the 3-mercaptopropionic acids capped Au nanoclusters (NCs), the low-frequency vibration of the metal core progressively decreases from 144.0, 55.2 to 40.0 cm−1, and the coupling strength of electrons-high-frequency vibration related to surface motifs gradually diminishes from 40.2, 30.5 to 14.4 meV. Moreover, introducing cation additives significantly reduces electron transfer time from 40, 27 to 12 ps in the pathway from staple motifs to the metal core. This benefits from the shrinkage of the total structure that speeds up the shell-core electron transition, and in particular, the Tb3+ provides a hopping platform for the excited electrons as their intrinsic ladder-like energy level structure. As a result, it allows a remarkable enhancement in PLQY, from 51.2%, 83.4%, up to 99.5%.

Time-varying 3D optical torque via a single beam

The role of direct air capture in achieving climate-neutral aviation

Abstract Growing demand for air travel and limited scalable solutions pose significant challenges to the mitigation of aviation’s climate change impact. Direct air capture (DAC) may gain prominence due to its versatile applications for either carbon removal (direct air carbon capture and storage, DACCS) or synthetic fuel production (direct air carbon capture and utilization, DACCU). Through a comprehensive and time-dynamic techno-economic assessment, we explore the conditions for synthetic fuels from DACCU to become cost-competitive with an emit-and-remove strategy based on DACCS under 2050 CO 2 and climate neutrality targets. We find that synthetic fuels could achieve climate neutrality at lower cost than an emit-and-remove strategy due to their ability to cost-effectively mitigate contrails. Under demand reductions, contrail avoidance, and CO 2 neutrality targets the cost advantage of synthetic fuels weakens or disappears. Low electricity cost (€0.02 kWh -1 ) and high fossil kerosene prices (€0.9 l -1 ) can favor synthetic fuels’ cost-competitiveness even under these conditions. Strategic interventions, such as optimal siting and the elimination of fossil fuel subsidies, can thus favor a shift away from fossil-reliant aviation.

Engineered hypoxia-responsive albumin nanoparticles mediating mitophagy regulation for cancer therapy

Cryo-EM structure of an activated GPR4–Gs signaling complex

CF2H-synthon enables asymmetric radical difluoroalkylation for synthesis of chiral difluoromethylated amines

Tailoring pyridine bridged chalcogen-concave molecules for defects passivation enables efficient and stable perovskite solar cells

Influence of aluminium distribution on the diffusion mechanisms and pairing of [Cu(NH3)2]+ complexes in Cu-CHA

AbstractThe performance of Cu-exchanged chabazite (Cu-CHA) for the ammonia-assisted selective catalytic reduction of NOx (NH3-SCR) depends critically on the presence of paired $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + complexes. Here, a machine-learning force field augmented with long-range Coulomb interactions is developed to investigate the effect of Al-distribution and Cu-loading on the mobility and pairing of $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + complexes. Performing unbiased and constrained molecular dynamics simulations, we obtain unique information inaccessible to first-principle calculations and experiments. The free energy barrier for $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + diffusion between CHA-cages depends sensitively on both the local and distant Al-distribution. Importantly, certain Al-distributions and arrangements of neighboring $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + and $${{{{{\rm{NH}}}}}_{4}}^{+}$$ NH 4 + cations make paired $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + complexes exothermic with respect to separated configurations. Our results suggest that the NH3-SCR activity can be enhanced by increasing the Cu-loading and Al-content. The dynamic interplay between $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + and $${{{{{\rm{NH}}}}}_{4}}^{+}$$ NH 4 + diffusion is crucial for the $${[{{{\rm{Cu}}}}{({{{{\rm{NH}}}}}_{3})}_{2}]}^{+}$$ [ Cu ( NH 3 ) 2 ] + mobility and stresses the need to explore large systems including long-range Coulomb interactions when studying diffusion of charged species in zeolites.

A membrane-targeted photoswitch restores physiological ON/OFF responses to light in the degenerate retina

The art and science of translucent color organic solar cells

Northern Scandinavian mountains supported by a low-grade eclogitic crustal keel

Inhibited peroxidase activity of peroxiredoxin 1 by palmitic acid exacerbates nonalcoholic steatohepatitis in male mice

Evolution of Omicron lineage towards increased fitness in the upper respiratory tract in the absence of severe lung pathology

Abstract The emergence of the Omicron lineage represented a major genetic drift in SARS-CoV-2 evolution. This was associated with phenotypic changes including evasion of pre-existing immunity and decreased disease severity. Continuous evolution within the Omicron lineage raised concerns of potential increased transmissibility and/or disease severity. To address this, we evaluate the fitness and pathogenesis of contemporary Omicron variants XBB.1.5, XBB.1.16, EG.5.1, and JN.1 in the upper (URT) and lower respiratory tract (LRT). We compare in vivo infection in Syrian hamsters with infection in primary human nasal and lung epithelium cells and assess differences in transmissibility, antigenicity, and innate immune activation. Omicron variants replicate efficiently in the URT but display limited pathology in the lungs compared to previous variants and fail to replicate in human lung organoids. JN.1 is attenuated in both URT and LRT compared to other Omicron variants and fails to transmit in the male hamster model. Our data demonstrate that Omicron lineage evolution has favored increased fitness in the URT.

Two-component system GrpP/GrpQ promotes pathogenicity of uropathogenic Escherichia coli CFT073 by upregulating type 1 fimbria

CRISPR-Hybrid: A CRISPR-Mediated Intracellular Directed Evolution Platform for RNA Aptamers

Tailoring industrial enzymes for thermostability and activity evolution by the machine learning-based iCASE strategy

Overrated energy storage performances of dielectrics seriously affected by fringing effect and parasitic capacitance

mosGILT antibodies interfere with Plasmodium sporogony in Anopheles gambiae

AbstractPlasmodium, the causative agents of malaria, are obtained by mosquitoes from an infected human. Following Plasmodium acquisition by Anopheles gambiae, mosquito gamma-interferon-inducible lysosomal thiol reductase (mosGILT) plays a critical role in its subsequent sporogony in the mosquito. A critical location for this development is the midgut, a tissue we show expresses mosGILT. Using membrane-feeding and murine infection models, we demonstrate that antibodies against mosGILT reduce the number of P. falciparum and P. berghei oocysts in the midgut and the infection prevalence of both species in the mosquito. mosGILT antibodies act in the mosquito midgut, specifically impacting the Plasmodium oocyst stage. Targeting mosGILT can therefore interfere with the Plasmodium life cycle in the mosquito and potentially serve as a transmission-blocking vaccine.

An intelligent hybrid-fabric wristband system enabled by thermal encapsulation for ergonomic human-machine interaction

Believed Gender Differences in Social Preferences

Abstract While there is a vast (and mixed) literature on gender differences in social preferences, little is known about believed gender differences in social preferences. Using data from 15 studies and 8,979 individuals, we find that women are believed to be more generous and more equality-oriented than men. This believed gender gap is robust across a wide range of contexts that vary in terms of strategic considerations, selfish motives, fairness concepts, and payoffs. Yet this believed gender gap is largely inaccurate. Consistent with models of associative memory, specifically the role of similarity and interference, the believed gender gap is correlated with recalled prior life experiences from similar contexts and significantly affected by an experience that may interfere with the recall process of prior memories, even though this interfering experience should not affect the beliefs of perfect-memory Bayesians. Application studies further reveal that believed gender differences extend to the household (i.e., beliefs about contributions to the home, family, and upbringing of children), the workplace (i.e., beliefs about equal pay), and policy views (i.e., beliefs about redistribution, equal access to education, healthcare, and affordable housing).