Liquid-Liquid Phase Transition Drives Intra-chloroplast Cargo Sorting.

In eukaryotic cells, organelle biogenesis is pivotal for cellular function and cell survival. Chloroplasts are unique organelles with a complex internal membrane network. The mechanisms of the migration of imported nuclear-encoded chloroplast proteins across the crowded stroma to thylakoid membranes are less understood. Here, we identified two Arabidopsis ankyrin-repeat proteins, STT1 and STT2, that specifically mediate sorting of chloroplast twin arginine translocation (cpTat) pathway proteins to thylakoid membranes. STT1 and STT2 form a unique hetero-dimer through interaction of their C-terminal ankyrin domains. Binding of cpTat substrate by N-terminal intrinsically disordered regions of STT complex induces liquid-liquid phase separation. The multivalent nature of STT oligomer is critical for phase separation. STT-Hcf106 interactions reverse phase separation and facilitate cargo targeting and translocation across thylakoid membranes. Thus, the formation of phase-separated droplets emerges as a novel mechanism of intra-chloroplast cargo sorting. Our findings highlight a conserved mechanism of phase separation in regulating organelle biogenesis.

The DnaJ proteins DJA6 and DJA5 are essential for chloroplast iron-sulfur cluster biogenesis.

Fe-S clusters are ancient, ubiquitous and highly essential prosthetic groups for numerous fundamental processes of life. The biogenesis of Fe-S clusters is a multistep process including iron acquisition, sulfur mobilization, and cluster formation. Extensive studies have provided deep insights into the mechanism of the latter two assembly steps. However, the mechanism of iron utilization during chloroplast Fe-S cluster biogenesis is still unknown. Here we identified two Arabidopsis DnaJ proteins, DJA6 and DJA5, that can bind iron through their conserved cysteine residues and facilitate iron incorporation into Fe-S clusters by interactions with the SUF (sulfur utilization factor) apparatus through their J domain. Loss of these two proteins causes severe defects in the accumulation of chloroplast Fe-S proteins, a dysfunction of photosynthesis, and a significant intracellular iron overload. Evolutionary analyses revealed that DJA6 and DJA5 are highly conserved in photosynthetic organisms ranging from cyanobacteria to higher plants and share a strong evolutionary relationship with SUFE1, SUFC, and SUFD throughout the green lineage. Thus, our work uncovers a conserved mechanism of iron utilization for chloroplast Fe-S cluster biogenesis.

User-Friendly Multifunctional Red-Emissive Carbon Dots for Rapid Cell Nucleus Staining via Targeting Nuclear Proteins.

Cytoarchitectural staining is of great importance in disease diagnosis and cell biology research. This study developed user-friendly multifunctional red-emissive carbon dots (R-CDs) for rapid cell nucleus staining via targeting nuclear proteins. R-CDs, simply prepared by electrochemical treatment of 1,2,4-benzenetriamine, exhibit strong emission at 635 nm when excited at 507 nm. The R-CDs can rapidly stain the nucleus of human SH-SY5Y, HepG2, and HUH-7 cells with a high signal-to-noise ratio owing to fluorescence enhancement after entering the nucleus. Compared to conventional cytosolic dyes such as Hoechst and DAPI, R-CDs are cheaper, more highly dispersed in water, and more stable (requiring no stringent storage conditions). The R-CDs show stable optical properties with insignificant photobleaching over 7 days and salt resistance up to 2 M of NaCl. More importantly, R-CDs, possessing a positive charge, allow rapid staining of live cells (3 min) and dead cells (10 s) in saline. According to kinetic variation, R-CDs can distinguish live cells from dead cells. Staining exhibits high efficiency in onion epidermal cells, Aspergillus niger, Caenorhabditis elegans, and human spermatozoa. The mechanism for efficient staining is based on their fast accumulation in the nucleus due to their small size and positive charge and strong interaction with nuclear proteins at amino acid residues of histidine and arginine, resulting in fluorescence enhancement by dozens of times. The developed R-CDs do not bind to DNA and would not cause genetic damage and will find various safe applications in biological and medical fields.

The translocon protein FtsHi1 is an ATP-dependent DNA/RNA helicase that prevents R-loop accumulation in chloroplasts.

R-loops, three-stranded nucleic acid structures consisting of a DNA: RNA hybrid and displaced single-stranded DNA, play critical roles in gene expression and genome stability. How R-loop homeostasis is integrated into chloroplast gene expression remains largely unknown. We found an unexpected function of FtsHi1, an inner envelope membrane-bound AAA-ATPase in chloroplast R-loop homeostasis of Arabidopsis thaliana. Previously, this protein was shown to function as a component of the import motor complex for nuclear-encoded chloroplast proteins. However, this study provides evidence that FtsHi1 is an ATP-dependent helicase that efficiently unwinds both DNA-DNA and DNA-RNA duplexes, thereby preventing R-loop accumulation. Over-accumulation of R-loops could impair chloroplast transcription but not necessarily genome integrity. The dual function of FtsHi1 in both protein import and chloroplast gene expression may be important to coordinate the biogenesis of nuclear- and chloroplast-encoded subunits of multi-protein photosynthetic complexes. This study suggests a mechanical link between protein import and R-loop homeostasis in chloroplasts of higher plants.

Electromagnetically induced transparency enabled by quasi-bound states in the continuum modulated by epsilon-near-zero materials.

Highly tunable electromagnetically induced transparency (EIT) with high-quality-factor (Q-factor) excited by combining with the quasi-bound states in the continuum (quasi-BIC) resonances is crucial for many applications. This paper describes all-dielectric metasurface composed of silicon cuboid etched with two rectangular holes into a unit cell and periodically arranged on a SiO2 substrate. By breaking the C2 rotational symmetry of the unit cell, a high-Q factor EIT and double quasi-BIC resonant modes are excited at 1224.3, 1251.9 and 1299.6 nm with quality factors of 7604, 10064 and 15503, respectively. We show that the EIT resonance is caused by destructive interference between magnetic dipole resonances and quasi-BIC dominated by electric quadrupole. Toroidal dipole (TD) and electric quadrupole (EQ) dominate the other two quasi-BICs. The EIT window can be successfully modulated with transmission intensity from 90% to 5% and modulation depths ranging from -17 to 24 dB at 1200-1250 nm by integrating the metasurface with an epsilon-near-zero (ENZ) material indium tin oxide (ITO) film. Our findings pave the way for the development of applications such as optical switches and modulators with many potential applications in nonlinear optics, filters, and multichannel biosensors.

(3+1)-dimensional Pearcey-Gaussian wave packet with arbitrary velocity driven by flying focus.

The group velocity (GV) modulation of space-time wave packets (STWPs) along the transverse and longitudinal directions in free space is constrained by various factors. To surmount this limitation, a technique called "flying focus" has been developed, which enables the generation of laser pulses with dynamic focal points that can propagate at arbitrary velocities independent of GV. In this Letter, we propose a (3+1)-dimensional Pearcey-Gauss wave packet based on the "flying focus" technique, which exhibits superluminal propagation, transverse focus oscillation, and longitudinal periodic autofocusing. By selecting appropriate parameters, we can flexibly manipulate the position, the size, and the number of focal points- or make the wave packet follow a desired trajectory. This work may pave the way for the advancement of space-time structured light fields.

Concave Gold Nanocubes Exhibit Growth-Etching Behavior: Unexpected Morphological Transformations.

Chemical equilibrium stands as a fundamental principle governing the dynamics of chemical systems. However, it may become intricate when it refers to nanomaterials because of their unique properties. Here, we invesitigated concave gold nanocubes (CGNs) subjected to an akaline Au3+/H2O2 solution, which exhibit both etching and growth in a monotonic solution. When CGNs were subjected to an increasingly alkaline Au3+/H2O2 solution, their dimensions increased from 107 to 199 nm and then decreased to 125 nm. Transmission electron microscopy (TEM) demonstrated that their morphology undergoes intricate alternations from concave to mutibranch and finally to concave again. Real-time ultraviolet-visible spectroscopy and time-dependent TEM also demonstrated reduction first and then oxidation in one solution. Among the nanomaterials, the obtained carpenterworm-like gold nanoparticles revealed the best catalytic performance in p-nitrophenol reduction by NaBH4, with a chemical rate that continues to increase until the reaction reaches completion. Growth leading to atomic dislocation, distortion, and exposure on nanoparticles and the redox of H2O2 plausibly account for the further etching due to the Ostwald ripening effect. Our study may spur more interest in the tuning of the properties, engineering, investigation, and design of new kinds of nanomaterials.

Description of a pathogenic strain of Aeromonas dhakensis isolated from Ancherythroculter nigrocauda in an inland region of China.

Aeromonas dhakensis is reported as an emerging pathogenic species within the genus Aeromonas and is widely distributed in tropical coastal areas. This study provided a detailed description and characterization of a strain of A. dhakensis (202108B1) isolated from diseased Ancherythroculter nigrocauda in an inland region of China. Biochemical tests identified the isolate at the genus level, and the further molecular analysis of concatenated housekeeping gene sequences revealed that the strain belonged to the species A. dhakensis. The isolated A. dhakensis strain was resistant to five antibiotics, namely, penicillin, ampicillin, clindamycin, cephalexin, and imipenem, while it was susceptible to or showed intermediate resistance to most of the other 15 tested antibiotics. The isolated strain of A. dhakensis caused acute hemorrhagic septicemia and tissue damage in artificially infected A. nigrocauda, with a median lethal dose of 7.76 × 104 CFU/fish. The genome size of strain 202108B1 was 5 043 286 bp, including 1 chromosome and 4 plasmids. This is the first detailed report of the occurrence of infection caused by an A. dhakensis strain causing infection in an aquaculture system in inland China, providing important epidemiological data on this potential pathogenic species.

Size Dependence of Gold Nanorods for Efficient and Rapid Photothermal Therapy.

In recent years, gold nanomaterials have become a hot topic in photothermal tumor therapy due to their unique surface plasmon resonance characteristics. The effectiveness of photothermal therapy is highly dependent on the shape and size of gold nanoparticles. In this work, we investigate the photothermal therapeutic effects of four different sizes of gold nanorods (GNRs). The results show that the uptake of short GNRs with aspect ratios 3.3-3.5 by cells is higher than that of GNRs with aspect ratios 4-5.5. Using a laser with single pulse energy as low as 28 pJ laser for 20 s can induce the death of liver cancer cells co-cultured with short GNRs. Long GNRs required twice the energy to achieve the same therapeutic effect. The dual-temperature model is used to simulate the photothermal response of intracellular clusters irradiated by a laser. It is found that small GNRs are easier to compact because of their morphological characteristics, and the electromagnetic coupling between GNRs is better, which increases the internal field enhancement, resulting in higher local temperature. Compared with a single GNR, GNR clusters are less dependent on polarization and wavelength, which is more conducive to the flexible selection of excitation laser sources.

Surface Charge Effects for the Hydrogen Evolution Reaction on Pt(111) Using a Modified Grand-Canonical Potential Kinetics Method.

Surface charges of catalysts have important influences on the thermodynamics and kinetics of electrochemical reactions. Herein, we develop a modified version of the grand-canonical potential kinetics (GCP-K) method based on density functional theory (DFT) calculations to explore the effect of surface charges on reaction thermodynamics and kinetics. Using the hydrogen evolution reaction (HER) on the Pt(111) surface as an example, we show how to track the change of surface charge in a reaction and how to analyze its influence on the kinetics. Grand-canonical calculations demonstrate that the optimum hydrogen adsorption energy on Pt under the standard hydrogen electrode condition (SHE) is around -0.2 eV, rather than 0 eV established under the canonical ensemble, due to the high density of surface negative charges. By separating the surface charges that can freely exchange with the external electron reservoir, we obtain a Tafel barrier that is in good agreement with the experimental result. During the Tafel reaction, the net electron inflow into the catalyst leads to a stabilization of canonical energy and a destabilization of the charge-dependent grand-canonical component. This study provides a practical method for obtaining accurate grand-canonical reaction energetics and analyzing the surface charge induced changes.

Tuning Geometric Chirality in Metallic and Hybrid Nanostructures by Controlled Nanoscale Crystal Symmetry Breaking.

Understanding and controlling chirality in inorganic crystalline materials at the nanoscale is crucial in elucidating fundamental chirality-dependent physical and chemical processes as well as advancing new technological prospects, but significant challenges remain due to the lack of material control. Here, we have developed a facile and general bottom-up synthetic strategy for achieving chiral plasmonic Au nanostructures, including nanocubes and nanorods with fine chirality control. The underlying chiral mechanism enabled by the chiral boundary morphology is substantiated by theoretical modeling and finite element method (FEM) simulation. Because of the robustness of induced handedness and their small size, these as-synthesized chiral nanostructures can be further employed as building blocks toward the formation of complex chiral nanostructures. We have demonstrated a new class of chiral hybrid metal-semiconductor nanostructures that can allow integration of chirality with other properties and functionalities. All of these together have paved the way to engineer nanoscale inorganic chirality and thus study various emerging chirality-entangled effects with practical technological applications.

Highly efficient enhancement and extension of focusing ability for ring Pearcey beam by means of dual-region parabolic trajectory offset modulation.

It is a highly significant area of research to investigate how to effectively enhance the focusing ability of abruptly auto-focusing beams (AAFBs) while extending the focal length. We introduce a dual-region parabolic trajectory offset modulation to auto-focusing ring Pearcey beams (RPBs), presenting a novel, to the best of our knowlege, approach to extend the focal length while greatly enhancing their auto-focusing capabilities. Unlike directly introducing a linear chirp, which inevitably shortens the focal length to enhance the auto-focusing ability and allows only single focusing in the RPBs, our scheme can achieve a multi-focusing effect. Furthermore, we have experimentally generated such a beam, verifying our theoretical predictions. Our findings offer promising possibilities for generating optical bottles, trapping multiple particles periodically, and enhancing free-space optical communication capabilities.

Electronegativity principle for hydrogen evolution activity using first-principles calculations.

The catalytic activity of a heterogeneous catalyst is routinely described by the Sabatier principle using molecule/proton adsorption energy ΔGH as the thermodynamic descriptor. This descriptor, however, fails in quantitatively tracking the reaction rate due to the lack of charge transfer information during a reaction. Herein, we use density functional theory (DFT) calculations combining both canonical and grand-canonical ensembles to report a positive correlation between reaction kinetics and interfacial charge transfer for the hydrogen evolution reaction (HER). The Sabatier relationship for the HER catalysts exhibits a large dispersion in the canonical calculation but an improved linearity under the grand-canonical ensemble, indicating that surface charges are indeed important. This charge effect can be well captured by the Mulliken electronegativity χ of a catalyst because the reaction barrier shows a linear dependence on χ for a wide range of catalysts. Specifically, a catalyst with lower electronegativity exhibits a lower barrier and thus a faster reaction rate. This electronegativity principle is reaction route and pH independent and is founded on the thermoneutral requirement on ΔGH.

Substantial impact of surface charges on electrochemical reaction kinetics on S vacancies of MoS2 using grand-canonical iteration method.

The surface charges of catalysts have intricate influences on the thermodynamics and kinetics of electrochemical reactions. Herein, we develop a grand-canonical iteration method based on density functional theory calculations to explore the effect of surface charges on reaction kinetics beyond the traditional Butler-Volmer picture. Using the hydrogen evolution reaction on S vacancies of MoS2 as an example, we show how to track the change of surface charge in a reaction and to analyze its influence on the kinetics. Protons adsorb on S vacancies in a tough and charge-insensitive water splitting manner, which explains the observed large Tafel slope. Grand-canonical calculations report an unanticipated surface charge-induced change of the desorption pathway from the Heyrovsky route to a Volmer-Tafel route. During an electrochemical reaction, a net electron inflow into the catalyst may bring two effects, i.e., stabilization of the canonical energy and destabilization of the charge-dependent grand-canonical part. On the contrary, a net outflow of electrons from the catalyst can reverse the two effects. This surface charge effect has substantial impacts on the overpotential and the Tafel slope. We suggest that the surface charge effect is universal for all electrochemical reactions and significant for those involving interfacial proton transfers.

An approach for accessibility assessment and vulnerability analysis of national multimodal transport systems.

A series of ambitious accessibility-oriented policies have been launched in the world, which center around improving accessibility via the national multimodal transport systems including road, airline, and railway. The national multimodal transport accessibility assessment is one of the "basic" analyses for the design and implementation of these policies, whereas existing national-scale accessibility studies either focus on single-mode or two-mode transport or ignore the schedule-dependent nature of railway and airline. This article models the integrated road, railway, airline, and walking transport as a four-layer network with the consideration of their interdependencies. An algorithm is then developed to accurately assess the travel time-based accessibility on the four-layer network with the consideration of the daily schedule of trains and flights. The proposed approach is applied to map accessibility to 363 cities in mainland China and analyze the optimal travel modes. In addition, this article investigates the travel time-based vulnerability of the national multimodal transport system in mainland China under the extreme storm recently occurred in Zhengzhou (July 2021). The findings in this work provide insightful suggestions for transport planners to design the national multimodal transport systems and for stakeholders to schedule travels.

Resilience patterns of urban road networks under the worst-case localized disruptions.

Recent events, including COVID-19, extreme floods, and explosion accidents, commonly induced localized closures and disruptions of urban road networks (URNs), resulting in significant impacts on human mobility and socio-economic activities. Existing studies on URN resilience to those events mainly took few cases for empirical studies, limiting our understanding on the URN resilience patterns across different cities. By conducting a large-scale nationwide resilience analysis of URNs in 363 cities in mainland China, this study attempts to uncover the resilience patterns of URNs against the worst-case single (SLDs) and multiple localized disruptions (MLDs). Results show that the distance from the worst-case SLD to the city center would be less than 5 km in 62.3% cities, as opposed to more than 15 km in 14.3% cities. Moreover, the average road network resilience of cities in western China could be 7% and 13% smaller than that of the eastern cities under the worst-case SLDs and MLDs, respectively. This inequality in the worst-case resilience is partly attributable to variations in urban socio-economic, infrastructure-related, and topographic factors. These findings could inspire nationwide pre-disaster mitigation strategies to cope with localized disruptions and help transfer insights for mitigation strategies against disruptive events across cities.

Boundary effects on topological characteristics of urban road networks.

Urban road networks (URNs), as simplified views and important components of cities, have different structures, resulting in varying levels of transport efficiency, accessibility, resilience, and many socio-economic indicators. Thus, topological characteristics of URNs have received great attention in the literature, while existing studies have used various boundaries to extract URNs for analysis. This naturally leads to the question of whether topological patterns concluded using small-size boundaries keep consistent with those uncovered using commonly adopted administrative boundaries or daily travel range-based boundaries. This paper conducts a large-scale empirical analysis to reveal the boundary effects on 22 topological metrics of URNs across 363 cities in mainland China. Statistical results show that boundaries have negligible effects on the average node degree, edge density, orientation entropy of road segments, and the eccentricity for the shortest or fastest routes, while other metrics including the clustering coefficient, proportion of high-level road segments, and average edge length together with route-related metrics such as average angular deviation show significant differences between road networks extracted using different boundaries. In addition, the high-centrality components identified using varied boundaries show significant differences in terms of their locations, with only 21%-28% of high-centrality nodes overlapping between the road networks extracted using administrative and daily travel range-based boundaries. These findings provide useful insights to assist urban planning and better predict the influence of a road network structure on the movement of people and the flow of socio-economic activities, particularly in the context of rapid urbanization and the ever-increasing sprawl of road networks.

Enrichment, bioaccumulation and human health assessment of organochlorine pesticides in sediments and edible fish of a plateau lake.

The organochlorine pesticides (OCPs) are with features of persistence, high toxicity, bioaccumulation and adverse impact on ecosystems and human beings. Although OCPs pollutions have been observed in the plateau lakes, comprehensive understandings in the distribution characteristics and human health risks of OCPs in these valuable but fragile ecosystems are limited. We here investigated the distribution, bioaccumulation process and health risks of OCPs in the Jianhu lake, a representative plateau lake in China. The endrin ketone, endrin aldehyde and heptachlor were the most dominant species in surface and columnar sediments. Their total contents ranged between 0 ~ 1.92 × 103 ng·g-1. The distribution of OCPs in sediment cores combined with chronology information indicated that the fast accumulation of OCPs happened during the last decades. Combining the distribution features of OCPs in different sources with mixing model results of carbon isotope (δ13C), farming area was identified as the main source (46%), and the OCPs were transported to lake by inflow-rivers (37%). The enrichment of OCPs in sediments caused considerable bioaccumulation of OCPs in local fish (∑OCPs 0-3199.93 ng·g-1, dw) with the bio-sediment accumulation factor (BSAF) ranging from ND to 9.41. Moreover, growing time was another key factor governing the accumulation in specific species (Carassius auratus and Cyprinus carpio). Eventually, the carcinogenic risk index (CRI) and exposure risk index (ERI) of the endrin category and aldrin exceeded the reference value, indicating relatively high health risks through consumption of fish. Overall, this study systematically illustrated the bioaccumulation process and health risks of OCPs in the typical plateau lake, providing theoretical support for the better protection of this kind of lakes.

An RNA Chaperone-Like Protein Plays Critical Roles in Chloroplast mRNA Stability and Translation in Arabidopsis and Maize.

A key characteristic of chloroplast gene expression is the predominance of posttranscriptional control via numerous nucleus-encoded RNA binding factors. Here, we explored the essential roles of the S1-domain-containing protein photosynthetic electron transfer B (petB)/ petD Stabilizing Factor (BSF) in the stabilization and translation of chloroplast mRNAs. BSF binds to the intergenic region of petB-petD, thereby stabilizing 3' processed petB transcripts and stimulating petD translation. BSF also binds to the 5' untranslated region of petA and activates its translation. BSF displayed nucleic-acid-melting activity in vitro, and its absence induces structural changes to target RNAs in vivo, suggesting that BSF functions as an RNA chaperone to remodel RNA structure. BSF physically interacts with the pentatricopeptide repeat protein Chloroplast RNA Processing 1 (AtCRP1) and the ribosomal release factor-like protein Peptide chain Release Factor 3 (PrfB3), whose established RNA ligands overlap with those of BSF. In addition, PrfB3 stimulated the RNA binding ability of BSF in vitro. We propose that BSF and PrfB3 cooperatively reduce the formation of secondary RNA structures within target mRNAs and facilitate AtCRP1 binding. The translation activation function of BSF for petD is conserved in Arabidopsis (Arabidopsis thaliana) and maize (Zea mays), but that for petA operates specifically in Arabidopsis. Our study sheds light on the mechanisms by which RNA binding proteins cooperatively regulate mRNA stability and translation in chloroplasts.

First Results from the Taiwan Axion Search Experiment with a Haloscope at 19.6 µeV.

This Letter reports on the first results from the Taiwan Axion Search Experiment with a Haloscope, a search for axions using a microwave cavity at frequencies between 4.707 50 and 4.798 15 GHz. Apart from the nonaxion signals, no candidates with a significance of more than 3.355 were found. The experiment excludes models with the axion-two-photon coupling |g_{aγγ}|≳8.1×10^{-14} GeV^{-1}, a factor of eleven above the benchmark Kim-Shifman-Vainshtein-Zakharov model, in the mass range 19.4687