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Blue lasers play a pivotal role in laser-based display, printing, manufacturing, data recording and medical technologies. Colloidal quantum dots (QDs) are solution-grown materials with strong, tunable emission covering the whole visible spectrum, but the development of QD lasers has largely relied on Cd-containing red-emitting QDs, with technologically viable blue QD lasers remaining out of reach. Here we report on the realization of tunable and robust lasing using low-toxicity blue-emitting ZnSe-ZnS core-shell QDs that are compact in size yet still feature suppressed Auger recombination and long optical gain lifetime approaching 1 ns. These characteristics allow us to handle the blue QDs like laser dyes for liquid-state amplified spontaneous emission and lasing. The blue QD laser is operated under quasi-continuous-wave excitation by solid-state nanosecond lasers. A Littrow-configuration cavity enables narrow linewidth (<0.2 nm), wavelength-tunable, coherent and stable laser outputs without circulating the solution. These results indicate the promise of ZnSe-ZnS QDs to fill the 'blue gap' of QD lasers and to replace less stable blue laser dyes for a multitude of applications., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Observation and understanding of fine-structure splitting of bright excitons in lead halide perovskite quantum dots (QDs) are crucial to their emerging applications in quantum light sources and exciton coherence manipulation. Recent studies demonstrate that ensemble-level polarization-resolved transient absorption spectroscopy can reveal the quantum beats arising from the coherence between two fine-structure levels. Here we report the observation of an extra fine-structure quantum coherence hidden in previous studies by using cryo-magnetic quantum beat spectroscopy. In ∼6 nm CsPbI 3 QDs, two splitting energies of 0.25 and 1.20 meV were observed at 1.7 K, which gradually increased to 0.74 and 1.55 meV, respectively, when a longitudinal magnetic field up to 7 T was applied. The field dependence allowed us to extract two distinct nominal Landé g -factors corresponding to QDs with different orientations with respect to the external field.

Coherent interaction between light fields and matter has led to many exotic physical phenomena, one of which is the Autler-Townes splitting originating from the optical Stark effect of a three-level system. It has been well documented for atoms, molecules, and low-dimensional, epitaxial-grown semiconductors but rarely for solution-processed samples. Here, we report on Autler-Townes splitting observed in CdSe nanoplatelets. The strong intersubband transition of these nanoplatelets situated in the near-infrared allows us to coherently drive it with femtosecond near-infrared pulses, and meanwhile, their strong interband transition in the visible records the resultant spectral changes. The splitting is most prominent with cross-polarized, linear pump-probe pulses, consistent with the orthogonal polarizations of interband and intersubband transition dipoles. When the nanoplatelets are driven from tilted incident angles, we observe anomalous spectral lineshapes arising from a competition between interband and intersubband drivings, which are nevertheless quantitatively captured by our dressed-state model simulation.

The clinical application of photodynamic therapy (PDT) is limited by oxygen-dependence and side effects caused by photosensitizer residues. Photoinitiators based on the H-abstraction reaction can address these challenges because they can generate alkyl radical-killing cells independently of oxygen and undergo rapid bleaching following H-abstraction. Nonetheless, the development of photoinitiators for PDT has been impeded by the absence of effective design strategies. Herein, we have developed aryl-ketone substituted cyanine (ACy-R), the first red-light triggered H-abstraction photoinitiators for hypoxic cancer therapy. These ACy-R molecules inherited the near-infrared absorption of cyanine dye, and aryl-ketone modification imparted H-abstraction capability. Experimental and quantum calculations revealed that modifying the electron-withdrawing groups of the aryl (e.g., ACy-5F) improved the contribution of the O atom to the photon excitation process promoting intersystem crossing and H-abstraction ability. Particularly, ACy-5F rapidly penetrated cells and enriched in the endoplasmic reticulum. Even under severe hypoxia, ACy-5F initiated red-light induced H-abstraction with intracellular biomolecules, inducing necroptosis and ferroptosis. Moreover, ACy-5F was degraded after H-abstraction, thus avoiding the side effects of long-term phototoxicity after therapy. This study not only provides a crucial molecular tool for hypoxic tumors therapy, but also presents a promising strategy for the development of multifunctional photosensitizers and photoinitiators., (© 2024 Wiley-VCH GmbH.)

Background: Foot-and-mouth disease virus (FMDV) is an important pathogen of the MicroRNA virus family. Infection of livestock can cause physical weakness, weight loss, reduced milk production, and a significant reduction in productivity for an extended period. It also causes a high mortality rate in young animals, seriously affecting livestock production. The host range of FMDV is mainly limited to cloven-hoofed animals such as cattle and sheep, while odd-toed ungulates such as horses and donkeys have natural resistance to FMDV. The mechanism underlying this resistance in odd-toed ungulates remains unclear., Objective: This study aimed to analyze the differences between FMDV-infected cattle and horses to provide valuable insights into the host-FMDV interaction mechanisms, thereby contributing to the control of foot-and-mouth disease and promoting the development of the livestock industry., Methods: We observed the distribution of integrins, which help FMDV enter host cells, in the nasopharyngeal tissues of cattle and horses using immunohistochemistry. Then, we employed high-throughput RNA sequencing (RNA-Seq) to study the changes in host gene expression in the nasopharyngeal epithelial tissues of cattle and horses after FMDV infection. We performed enrichment analysis of GO and KEGG pathways after FMDV infection and validated related genes through qPCR., Results: The immunohistochemical results showed that both cattle and horses had four integrin receptors that could assist FMDV entry into host cells. The transcriptome analysis revealed that after FMDV infection, pro-apoptotic genes such as caspase-3 (CASP3) and cytochrome C (CYCS) were upregulated in cattle, while apoptosis-inhibiting genes such as NAIP and BCL2A1 were downregulated. In contrast, the expression trend of related genes in horses was opposite to that in cattle. Additionally, autophagy-related genes such as beclin 1, ATG101, ATG4B, ATG4A, ATG13, and BCL2A1 were downregulated in cattle after FMDV infection, indicating that cattle did not clear the virus through autophagy. However, key autophagy genes including ATG1, ATG3, ATG9, ATG12, and ATG16L1 were significantly upregulated in horses after viral infection., Conclusion: Both water buffaloes and Mongolian horses express integrin receptors that allow FMDV entry into cells. Therefore, the resistance of Mongolian horses to FMDV may result from more changes in intracellular mechanisms, including processes such as autophagy and apoptosis. Significant differences were observed between water buffaloes and Mongolian horses in these processes, suggesting that these processes influence FMDV replication and synthesis., (© 2024 The Author(s). Veterinary Medicine and Science published by John Wiley & Sons Ltd.)

The detoxified pneumolysin derivative ΔA146Ply has been proven to have a direct anti-triple negative breast cancer effect by our group, but its work model remains unclear. In this study, we focused on its ability to inhibit triple-negative breast cancer metastasis. We found that ΔA146Ply suppressed the migration and invasion of triple-negative breast cancer cells by activating mannose receptor and toll-like receptor 4. Their activation triggers the activation of the mammalian target of rapamycin signalling, sequentially leading to autophagy, transforming growth factor-β1, and epithelial-mesenchymal transition inhibition. Furthermore, the combination of doxorubicin and ΔA146Ply significantly inhibited triple-negative breast cancer progression and prolonged survival in tumour-bearing mice. Taken together, our study provides an alternative microbiome-based mannose receptor-targeted therapy for triple-negative breast cancer and a novel theoretical and experimental basis for the downstream signalling pathway of the mannose receptor.

Intersubband transition was recently discovered in colloidal nanoplatelets, but the associated intersubband carrier relaxation dynamics remains poorly understood. In particular, it is crucial to selectively excite the intersubband transition and to follow the hot electron dynamics in the absence of valence-band holes. This is achieved herein by exciting the predoped electrons in CdSe/ZnS nanoplatelets using near-infrared femtosecond pulses and monitoring nonequilibrium electron dynamics using broad-band visible pulses. We find that the n = 2 electrons relax to the n = 1 subband and establish a Fermi-Dirac distribution within 200 fs, and finally reach an equilibrium with the lattice within a few ps. The cooling dynamics depend mainly on the excitation fluence but weakly on the doping density and the lattice temperature. These characteristics are well captured by our numerical simulation that explicitly accounts for the state occupation effect and optical phonon scattering.

Controlling the interplay between relaxation and charge/energy transfer processes in the excited states of photocatalysts is crucial for the performance of artificial photosynthesis. Metal-to-ligand charge-transfer triplet states ( 3 MLCT*) of ruthenium(II) complexes are broadly implemented for photocatalysis, but an effective means of managing the triplets for enhanced photocatalysis has been lacking. Herein, We proposed a strategy to considerably prolong the triplet excited-state lifetime by decorating a ruthenium(II) phosphine complex (RuP-1) with pendent polyaromatic hydrocarbons (PAHs). Systematic studies demonstrate that in RuP-4 decorated with anthracene, sub-picosecond electron transfer from anthracene to 3 MLCT* leads to a charge-separated state that can mediate the formation of the intra-ligand triplet state ( 3 IL) of anthracene, resulting in an exceptionally long excited-state up to several milliseconds. This triplet management strategy enables impressive photocatalytic reduction of CO 2 to CO with a turnover number (TON) of 404, an optimized quantum yield of 43 % and 100 % selectivity, which is the highest reported performance for mononuclear photocatalysts without additional photosensitizers. RuP-4 also catalyzes photochemical hydrogen generation under argon. This work opens up an avenue for regulating the excited-state charge/energy flow for the development of long-lived 3 IL multi-functional mononuclear photocatalysts to boost artificial photosynthesis., (© 2024 Wiley-VCH GmbH.)

Solution-processed colloidal nanocrystals of lead halide perovskites have been intensively investigated in recent years in the context of optoelectronic devices, during which time their quantum properties have also begun to attract attention. Their unmatched ease of synthetic tunability and unique structural, optical and electronic properties, in conjunction with the confinement of carriers in three dimensions, have motivated studies on observing and controlling coherent light-matter interaction in these materials for quantum information technologies. This Review outlines the recent efforts and achievements in this direction. Particularly notable examples are the observation of coherent single-photon emission, evidence for superfluorescence and the realization of room-temperature coherent spin manipulation for ensemble samples, which have not been achieved for prototypical colloidal CdSe nanocrystals that have been under investigation for decades. This Review aims to highlight these results, point out the challenges ahead towards realistic applications and bring together the efforts of multidisciplinary communities in this nascent field., (© 2024. Springer Nature Limited.)

High-efficiency generation of spin-triplet states in organic molecules is of great interest in diverse areas such as photocatalysis, photodynamic therapy, and upconversion photonics. Recent studies have introduced colloidal semiconductor nanocrystals as a new class of photosensitizers that can efficiently transfer their photoexcitation energy to molecular triplets. Here, we demonstrate that metallic Ag nanoparticles can also assist in the generation of molecular triplets in polycyclic aromatic hydrocarbons (PAHs), but not through a conventional sensitization mechanism. Instead, the triplet formation is mediated by charge-separated states resulting from hole transfer from photoexcited PAHs (anthracene and pyrene) to Ag nanoparticles, which is established through the rapid formation and subsequent decay of molecular anions revealed in our transient absorption measurements. The dominance of hole transfer over electron transfer, while both are energetically allowed, could be attributed to a Marcus inverted region of charge transfer. Owing to the rapid charge separation and the rapid spin-flip in metals, the triplet formation yields are remarkably high, as confirmed by their engagement in production of singlet oxygen with a quantum efficiency reaching 58.5%. This study not only uncovers the fundamental interaction mechanisms between metallic nanoparticles and organic molecules in both charge and spin degrees of freedom but also greatly expands the scope of triplet "sensitization" using inorganic nanomaterials for a variety of emerging applications.

Inhabiting some of the world's most inhospitable climatic regions, the Sunite Mongolian sheep generates average temperatures as low as 4.3 °C and a minimum temperature of -38.8 °C; in these environments, they make essential cold adaptations. In this regard, scapular fat tissues from Mongolian sheep were collected both in winter and summer for transcriptomic and proteomic analyses to identify genes related to adaptive thermogenesis. In the transcriptome analysis, 588 differentially expressed genes were identified to participate in smooth muscle activity and fat metabolism, as well as in nutrient regulation. There were 343 upregulated and 245 downregulated genes. GO and KEGG pathway analyses on these genes revealed their participation in regulating smooth muscle activity, metabolism of fats, and nutrients. Proteomic analysis showed the differential expression of 925 proteins: among them, there are 432 up- and 493 down-expressed proteins. These proteins are mainly involved in oxidative phosphorylation, respiratory chain complex assembly, and ATP production by electron transport. Furthermore, using both sets at a more detailed level of analysis revealed over-representation in gene ontology categories related to hormone signaling, metabolism of lipids, the pentose phosphate pathway, the TCA cycle, and especially the process of oxidative phosphorylation. The identified essential genes and proteins were further validated by quantitative real-time polymerase chain reaction and Western blotting, respectively; key metabolic network constriction was constructed. The present study emphasized the critical role of lipid turnover in scapular fat for thermogenic adaptation in Sunite sheep., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Direct reduction of unactivated alkyl halides for C(sp3)-N couplings under mild conditions presents a significant challenge in organic synthesis due to their low reduction potential. Herein, we introduce an in situ formed pyridyl-carbene-ligated copper (I) catalyst that is capable of abstracting halide atom and generating alkyl radicals for general C(sp3)-N couplings under visible light. Control experiments confirmed that the mono-pyridyl-carbene-ligated copper complex is the active species responsible for catalysis. Mechanistic investigations using transient absorption spectroscopy across multiple decades of timescales revealed ultrafast intersystem crossing (260 ps) of the photoexcited copper (I) complexes into their long-lived triplet excited states (>2 μs). The non-Stern-Volmer quenching dynamics of the triplets by unactivated alkyl halides suggests an association between copper (I) complexes and alkyl halides, thereby facilitating the abstraction of halide atoms via inner-sphere single electron transfer (SET), rather than outer-sphere SET, for the formation of alkyl radicals for subsequent cross couplings., (© 2024. The Author(s).)

The significant deposition of tail fat in sheep has a profound impact on the economic benefits of animal husbandry. Furthermore, increasing the litter size is a crucial means of enhancing economic benefits. The BMPR1B and T / Brachyury genes are considered major functional genes that could affect sheep litter size and tail bone number, respectively. In this study, we employed direct sequencing to identify specific mutations of the BMPR1B gene in Gobi short tail sheep and carried out genotyping using MassARRAY technology for each variant of both the BMPR1B and T genes. Significant associations were demonstrated between the c.687G>A mutation of BMPR1B and the litter size in both the Gobi short tail sheep and Ujimqin sheep breeds. Meanwhile, the g.30058882&#95;30058873GCAGATTAAAIndel mutation was significantly associated with the litter size in Gobi short tail sheep. These findings may provide valuable genetic markers for expanding sheep litter size. In addition, we also confirmed that the frequency of tail-bone-number-related T alleles was significantly higher in Gobi short tail sheep than in longer-tailed Ujimqin sheep.

Decreasing perovskite nanocrystal size increases radiative recombination due to the quantum confinement effect, but also increases the Auger recombination rate which leads to carrier imbalance in the emitting layers of electroluminescent devices. Here, we overcome this trade-off by increasing the exciton effective mass without affecting the size, which is realized through the trace Cd 2+ doping of formamidinium lead bromide perovskite nanocrystals. We observe an ~2.7 times increase in the exciton binding energy benefiting from a slight distortion of the [BX 6 ] 4- octahedra caused by doping in the case of that the Auger recombination rate is almost unchanged. As a result, bright color-saturated green emitting perovskite nanocrystals with a photoluminescence quantum yield of 96 % are obtained. Cd 2+ doping also shifts up the energy levels of the nanocrystals, relative to the Fermi level so that heavily n-doped emitters convert into only slightly n-doped ones; this boosts the charge injection efficiency of the corresponding light-emitting diodes. The light-emitting devices based on those nanocrystals reached a high external quantum efficiency of 29.4 % corresponding to a current efficiency of 123 cd A -1 , and showed dramatically improved device lifetime, with a narrow bandwidth of 22 nm and Commission Internationale de I'Eclairage coordinates of (0.20, 0.76) for color-saturated green emission for the electroluminescence peak centered at 534 nm, thus being fully compliant with the latest standard for wide color gamut displays., (© 2024 Wiley-VCH GmbH.)

All-inorganic metal halides with afterglow emission have attracted increasing attention due to their significantly longer afterglow duration and higher stability compared to their organic-inorganic hybrid counterparts. However, their afterglow colors have not yet reached the blue spectral region. Here, we report all-inorganic copper-doped Rb 2 AgBr 3 single crystals with ultralong blue afterglow (>300 s) by modulating defect states through doping engineering. The introduction of copper(I) ions into Rb 2 AgBr 3 facilitates the formation of bromine vacancies, thus increasing the density of trap states available for charge storage and enabling bright, persistent emission after ceasing the excitation. Moreover, cascade energy transfer between distinct emissive centers in the crystals results in ultra-broadband photoluminescence, not only covering the whole white light with near-unity quantum yield but also extending into the near-infrared region. This 'cocktail' of exotic light-emission properties, in conjunction with the excellent stability of copper-doped Rb 2 AgBr 3 crystals, allowed us to demonstrate their implementation to solid-state lighting, night vision, and intelligent anti-counterfeiting., (© 2024 Wiley-VCH GmbH.)

Competence development is essential for bacterial transformation since it enables bacteria to take up free DNA from the surrounding environment. The regulation of teichoic acid biosynthesis is tightly controlled during pneumococcal competence; however, the mechanism governing this regulation and its impact on transformation remains poorly understood. We demonstrated that a defect in lipoteichoic acid ligase (TacL)-mediated lipoteichoic acids (LTAs) biosynthesis was associated with impaired pneumococcal transformation. Using a fragment of tacL regulatory probe as bait in a DNA pulldown assay, we successfully identified several regulatory proteins, including ComE. Electrophoretic mobility shift assays revealed that phosphomimetic ComE, but not wild-type ComE, exhibited specific binding to the probe. DNase I footprinting assays revealed the specific binding sequences encompassing around 30 base pairs located 31 base pairs upstream from the start codon of tacL . Expression of tacL was found to be upregulated in the Δ comE strain, and the addition of exogenous competence-stimulating peptide repressed the tacL transcription in the wild-type strain but not the Δ comE mutant, indicating that ComE exerted a negative regulatory effect on the transcription of tacL . Mutation in the JH2 region of tacL upstream regulatory sequence led to increased LTAs abundance and displayed higher transformation efficiency. Collectively, our work identified the regulatory mechanisms that control LTAs biosynthesis during competence and thereby unveiled a repression mechanism underlying pneumococcal transformation., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2024 Yao, Wang, Song, Hu, Chen, Li, Liang, Wu, Xu, Wang, Zheng, Zhang, Yin, Yao and Wu.)

The properties of colloidal quantum-confined semiconductor nanocrystals (NCs), including zero-dimensional (0D) quantum dots, 1D nanorods, 2D nanoplatelets, and their heterostructures, can be tuned through their size, dimensionality, and material composition. In their photovoltaic and photocatalytic applications, a key step is to generate spatially separated and long-lived electrons and holes by interfacial charge transfer. These charge transfer properties have been extensively studied recently, which is the subject of this Review. The Review starts with a summary of the electronic structure and optical properties of 0D-2D nanocrystals, followed by the advances in wave function engineering, a novel way to control the spatial distribution of electrons and holes, through their size, dimension, and composition. It discusses the dependence of NC charge transfer on various parameters and the development of the Auger-assisted charge transfer model. Recent advances in understanding multiple exciton generation, decay, and dissociation are also discussed, with an emphasis on multiple carrier transfer. Finally, the applications of nanocrystal-based systems for photocatalysis are reviewed, focusing on the photodriven charge separation and recombination processes that dictate the function and performance of these materials. The Review ends with a summary and outlook of key remaining challenges and promising future directions in the field.

Excessive aggressive migration and invasion are important factors that increase the mortality of cancer patients. Matrix metalloproteinase 13 (MMP13) expression is positively correlated with lung cancer malignancy. However, the mechanism underlying an elevated MMP13 expression is not clearly defined. In this study, we demonstrated that hypoxia induced by CoCl 2 enhanced the expression of HIF1α, JAK2, STAT3 and MMP13 in A549 cells. A positive correlation between HIF1α and MMP13 expression was observed in lung adenocarcinoma patients. Mechanically, hypoxia upregulated HIF1α/JAK2/STAT3 signal axis, promoted transcription factor STAT3 to bind to MMP13 promoter region, and activated MMP13 transcription, finally promoted cell invasion and migration. However, stattic (STAT3 inhibitor) could reverse this effect caused by STAT3 in A549 cells. Together our data indicated that hypoxia might promote lung cancer cell migration and invasion through the HIF1α/JAK2/STAT3 axis by activating MMP13 transcription. MMP13 could be a promising therapeutic target for lung adenocarcinoma metastasis., (© 2023. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

Colloidal semiconductor nanoplatelets (NPLs) have emerged as low-cost and free-standing alternates of traditional quantum wells. The giant heavy- and light-hole splitting in NPLs allows for efficient optical spin injection. However, the electron spin lifetimes for prototypical CdSe NPLs are within a few picoseconds, likely limited by strong electron-hole exchange in these quantum- and dielectric-confined materials. Here how this hurdle can be overcome with engineered NPL-heterostructures is demonstrated. By constructing type-I CdSe/ZnS core/shell NPLs, dielectric screening inside the core is strongly enhanced, prolonging the electron spin polarization time (τ esp ) to over 30 ps (or 60 ps electron spin-flip time). Alternatively, by growing type-II CdSe/CdTe core/crown NPLs to spatially separate electron and hole wavefunctions, the electron-hole exchange is strongly suppressed, resulting in τ esp as long as 300 ps at room temperature. This study not only exemplifies how the well-established synthetic chemistry of colloidal heterostructures can aid in spin dynamics control but also establishes the feasibility of room-temperature coherent spin manipulation in colloidal NPLs., (© 2023 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Most of current metal halide materials, including all inorganic and organic-inorganic hybrids, are crystalline materials with poor workability and plasticity that limit their application scope. Here, we develop a novel class of materials termed polymeric metal halides (PMHs) through introducing polycations into antimony-based metal halide materials as A-site cations. A series of PMHs with orange-yellow broadband emission and large Stokes shift originating from inorganic self-trapped excitons are successfully prepared, which meanwhile exhibit the excellent processability and formability of polymers. The versatility of these PMHs is manifested as the broad choices of polycations, the ready extension to manganese- and copper-based halides, and the tolerance to molar ratios between polycations and metal halides in the formation of PMHs. The merger of polymer chemistry and inorganic chemistry thus provides a novel generic platform for the development of metal halide functional materials., (© 2024 Wiley-VCH GmbH.)

Magnetic impurity doping in semiconductors has emerged as an important strategy to endow exotic photophysical and magnetic properties. While most reported hosts are centrosymmetric semiconductors, doping magnetic ions into a noncentrosymmetric chiral semiconductor can offer additional control of photonic and spin polarization. In this work, we synthesized a Mn 2+ -doped chiral two-dimensional (2D) perovskite, Mn 2+ :( R -MPA) 2 PbBr 4 ( R -MPA + = R -methyl phenethylammonium). We found that the optical activity of chiral 2D perovskites is enhanced with an increased concentration of Mn 2+ ions. Additionally, efficient energy transfer from the chiral host to the Mn 2+ dopants is observed. This energy transfer process gives rise to circularly polarized luminescence from the excited state of Mn 2+ ( 4 T 1 → 6 A 1 ), exhibiting a photoluminescence quantum yield up to 24% and a dissymmetry factor of 11%. The exciton fine structures of undoped and Mn 2+ -doped ( R -MPA) 2 PbBr 4 are further studied through magnetic circular dichroism (MCD) spectroscopy. Our analysis shows that chiral organic cations lead to an exciton fine structure splitting energy as large as 5.0 meV, and the splitting is further increased upon Mn 2+ doping. Our results reveal the strong impacts of molecular chirality and magnetic dopants on the exciton structures of halide perovskites.

Colloidal quantum-dot (QD) lasing is normally achieved in close-packed solid-state films, as a high QD volume fraction is required for stimulated emission to outcompete fast Auger decay of optical-gain-active multiexciton states. Here a new type of liquid optical-gain medium is demonstrated, in which compact compositionally-graded QDs (ccg-QDs) that feature strong suppression of Auger decay are liquefied using a small amount of solvent. Transient absorption measurements of ccg-QD liquid suspensions reveal broad-band optical gain spanning a wide spectral range from 560 (green) to 675 nm (red). The gain magnitude is sufficient to realize a two-color amplified spontaneous emission (ASE) at 637 and 594 nm due to the band-edge (1S) and the excited-state (1P) transition, respectively. Importantly, the ASE regime is achieved using quasicontinuous excitation with nanosecond pulses. Furthermore, the ASE is highly stable under prolonged excitation, which stands in contrast to traditional dyes that exhibit strong degradation under identical excitation conditions. These observations point toward a considerable potential of high-density ccg-QD suspensions as liquid, dye-like optical gain media that feature readily achievable spectral tunability and stable operation under intense photoexcitation., (© 2023 Wiley-VCH GmbH.)

Lead halide perovskite quantum dots (QDs) have recently emerged as a promising material platform for quantum information processing owing to their strong light-matter interaction and relatively long-lived optical and spin coherences. In particular, the coherence of the fine-structure bright excitons is sustainable up to room temperature and can be observed even at an ensemble level. Here modulation of the polarization of these excitons in CsPbI 3 QDs and manipulation of their time-domain coherent dynamics using a longitudinal magnetic field are demonstrated. The manipulation is realized using femtosecond quantum beat spectroscopy performed with both circularly- and linearly-polarized pulses. The results are well captured by the density of matrix simulation and are picturized using a Bloch sphere. This study forms the basis for preparing arbitrary coherent superpositions of excitons in perovskite QDs for an array of quantum technologies under near-ambient conditions., (© 2023 Wiley-VCH GmbH.)

Background: Early microbial exposure is associate with protective allergic asthma. We have previously demonstrated that Streptococcus pneumoniae aminopeptidase N (PepN), one of the pneumococcal components, inhibits ovalbumin (OVA) -induced airway inflammation in murine models of allergic asthma, but the underlying mechanism was incompletely determined., Methods: BALB/c mice were pretreated with the PepN protein and exposed intranasally to HDM allergen. The anti-inflammatory mechanisms were investigated using depletion and adoptive transfer experiments as well as transcriptome analysis and isolated lung CD11c high macrophages., Results: We found pretreatment of mice with PepN promoted the proliferation of lung-resident F4/80 + CD11c high macrophages in situ but also mobilized bone marrow monocytes to infiltrate lung tissue that were then transformed into CD11 high macrophages. PepN pre-programmed the macrophages during maturation to an anti-inflammatory phenotype by shaping the metabolic preference for oxidative phosphorylation (OXPHOS) and also inhibited the inflammatory response of macrophages by activating AMP-activated protein kinase. Furthermore, PepN treated macrophages also exhibited high-level costimulatory signaling molecules which directed the differentiation into Treg., Conclusion: Our results demonstrated that the expansion of CD11c high macrophages in lungs and the OXPHOS metabolic bias of macrophages are associated with reduced allergic airway inflammation after PepN exposure, which paves the way for its application in preventing allergic asthma., (© 2023. The Author(s).)

Background: Carbapenem-resistant Acinetobacter baumannii (CRAB) has emerged as a predominant strain of healthcare-associated infections worldwide, particularly in intensive care units (ICUs). Therefore, it is imperative to study the molecular epidemiology of CRAB in the ICUs using multiple molecular typing methods to lay the foundation for the development of infection prevention and control strategies. This study aimed to determine the antimicrobial susceptibility profile, the molecular epidemiology and conduct homology analysis on CRAB strains isolated from ICUs., Methods: The sensitivity to various antimicrobials was determined using the minimum inhibitory concentration (MIC) method, Kirby-Bauer disk diffusion (KBDD), and E-test assays. Resistance genes were identified by polymerase chain reaction (PCR). Molecular typing was performed using multilocus sequence typing (MLST) and multiple-locus variable-number tandem repeat analysis (MLVA)., Results: Among the 79 isolates collected, they exhibited high resistance to various antimicrobials but showed low resistance to levofloxacin, trimethoprim-sulfamethoxazole, and tetracyclines. Notably, all isolates of A. baumannii were identified as multidrug-resistant A. baumannii (MDR-AB). The bla OXA-51-like , adeJ , and adeG genes were all detected, while the detection rates of bla OXA-23-like (97.5%), adeB (93.67%), bla ADC (93.67%), qacEΔ1-sul1 (84.81%) were higher; most of the Ambler class A and class B genes were not detected. MLST analysis on the 79 isolates identified five sequence types (STs), which belonged to group 3 clonal complexes 369. ST1145 Ox was the most frequently observed ST with a count of 56 out of 79 isolates (70.89%). MLST analysis for non-sensitive tigecycline isolates, which were revealed ST1145 Ox and ST1417 Ox as well. By using the MLVA assay, the 79 isolates could be grouped into a total of 64 distinct MTs with eleven clusters identified in them. Minimum spanning tree analysis defined seven different MLVA complexes (MCs) labeled MC1 to MC6 along with twenty singletons. The locus MLVA-AB&#95;2396 demonstrated the highest Simpson's diversity index value at 0.829 among all loci tested in this study while also having one of the highest variety of tandem repeat species., Conclusion: The molecular diversity and clonal affinities within the genomes of the CRAB strains were clearly evident, with the identification of ST1144 Ox , ST1658 Ox , and ST1646 Ox qaq representing novel findings., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2023 Xiong, Deng, Yang, Shen, Chen, Tian, Zha and Wu.)

Optical gain of colloidal quantum dots (QDs) is often attained in the multiexciton regime, which strongly complicates their lasing applications as the gain lifetime is limited by nonradiative Auger recombination occurring typically on the picosecond time scale. In principle, low-threshold gain can be achieved if the gain-active emission has a sizable red shift compared to the absorption. But, this mechanism has been rarely observed in typical QDs featuring small Stokes shift due to their weak electron-phonon coupling. Here, we report the observation of sub-single-exciton gain in CsPbI 3 and CsPbBr 3 perovskite QDs, which is unequivocally established through pinpointing the stimulated emission and biexciton absorption signatures using polarization-controlled femtosecond transient absorption spectroscopy. The soft lattice of perovskite QDs and hence strong electron-phonon coupling lead to two stimulated emission features from free and self-trapped excitons, respectively. In monodisperse QDs of varying sizes, the Stokes shift of the self-trapped exciton emission is sufficiently large to overcome the biexciton absorption loss and the inhomogeneous line width, enabling optical gain with average exciton occupancy down to <10%.

The electronic structure of halide perovskites is central to their carrier dynamics, enabling the excellent optoelectronic performance. However, the experimentally resolved transient absorption spectra exhibit large discrepancies from the commonly computed electronic structure by density functional theory. Using pseudocubic CsPbI 3 as a prototype example, here, it is unveiled with both ab initio molecular dynamics simulations and transmission electron microscopy that there exists pronounced dynamical lattice distortion in the form of disordered instantaneous octahedral tilting. Rigorous first-principles calculations reveal that the lattice distortion substantially alters the electronic band structure through renormalizing the band dispersions and the interband transition energies. Most notably, the electron and hole effective masses increase by 65% and 88%, respectively; the transition energy between the two highest valence bands decreases by about one half, agreeing remarkably well with supercontinuum transient-absorption measurements. This study further demonstrates how the resulting electronic structure modulates various aspects of the carrier dynamics such as carrier transport, hot-carrier relaxation, Auger recombination, and carrier multiplication in halide perovskites. The insights provide a pathway to engineer carrier transport and relaxation via lattice distortion, enabling the promise to achieve ultrahigh-efficiency photovoltaic devices., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

It is known that ribonucleotide reductase M2 (RRM2) could be induced by hepatitis B virus (HBV) via DNA damage response. However, whether RRM2 is a potential biomarker for diagnosing and monitoring liver fibrosis in chronic hepatitis B (CHB) patients is still unclear. In this study, CHB patients from GSE84044 (a transcriptome data from GEO data set) were downloaded and RRM2 was selected as a hub gene. Interestingly, a positive correlation was found between serum RRM2 and liver fibrosis stage. The similar results were found in CHB patients with normal alanine aminotransferase (ALT). Notably, RRM2 could effectively differentiate preliminary fibrosis from advanced fibrosis in CHB patients with/without normal ALT. In addition, RRM2 had a better performance in diagnosing liver fibrosis than two commonly used noninvasive methods (aspartate aminotransferase-to-platelet ratio index and fibrosis index based on the four factors), two classic fibrotic biomarkers (hyaluronic acid and type IV collagen) as well as Mac-2 binding protein glycosylation isomer, a known serum fibrosis marker. Moreover, CHB patients with high RRM2, who were associated with advanced fibrosis, had higher expressions of immune checkpoints. Overall, serum RRM2 may be a promising biomarker for diagnosing and monitoring liver fibrosis in CHB patients., (© 2023 Wiley Periodicals LLC.)

Background: Metformin is the most frequently prescribed medication for the treatment of type II diabetes mellitus and has played an anti-tumor potential in a variety of cancer types. Metformin can inhibit the growth of many cancer cells through various mechanisms, including ferroptosis. However, it is still unclear whether metformin can induce ferroptosis in lung cancer., Methods: This study evaluated the anti-tumor effect of metformin by detecting the levels of oxidative stress factors, the levels of ferrous ions, and the expression of ferroptosis-related genes in A549 and H1299 lung cancer cell lines treated with or without metformin., Results: The results showed that metformin treatment increased the levels of MDA, ROS and iron ions, while decreased the levels of GSH, T-SOD and CAT. Meanwhile, metformin treatment reduced the protein expression levels of Gpx4 and SLC7A11, Nrf2 and HO-1, while the addition of ferroptosis inhibitor ferrostatin-1 reversed the reduction., Conclusions: These results demonstrated that metformin exerts anti-tumor effects by inducing ferroptosis through the Nrf2/HO-1 signaling pathway in lung cancer cells, providing a theoretical basis for drug therapy of lung cancer patients., (© 2023. BioMed Central Ltd., part of Springer Nature.)

The ability to deliver electrons is vital for dye-based photocatalysts. Conventionally, the aromatic stacking-based charge-transfer complex increases photogenerated electron accessibility but decreases the energy of excited-state dyes. To circumvent this dilemma, here we show a strategy by tuning the stacking mode of dyes. By decorating naphthalene diimide with S-bearing branches, the S···S contact-linked naphthalene diimide string is created in coordination polymer, thereby enhancing electron mobility while simultaneously preserving competent excited-state reducing power. This benefit, along with in situ assembly between naphthalene diimide strings and exogenous reagent/reactant, improves the accessibility of short-lived excited states during consecutive photon excitation, resulting in greater efficiency in photoinduced electron-transfer activation of inert bonds in comparison to other coordination polymers with different dye-stacking modes. This heterogeneous approach is successfully applied in the photoreduction of inert aryl halides and the successive formation of C Ar -C/S/P/B bonds with potential pharmaceutical applications., (© 2023. The Author(s).)

Light-driven valorization conversion of CO 2 is an encouraging carbon-negative pathway that shifts energy-reliance from fossil fuels to renewables. Herein, a hierarchical urchin-like hollow-TiO 2 @CdS/ZnS (HTO@CdS/ZnS) Z-scheme hybrid synthesized by an in situ self-assembly strategy presents superior photocatalytic CO 2 -to-CO activity with nearly 100% selectivity. Specifically, benefitting from the reasonable architectural and interface design, as well as surface modification, this benchmarked visible-light-driven photocatalyst achieves a CO output of 62.2 μmol·h -1 and a record apparent quantum yield of 6.54% with the Co(bpy) 3 2+ (bpy = 2,2'-bipyridine) cocatalyst. It rivals all the incumbent selective photocatalytic conversion of CO 2 to CO in the CH 3 CN/H 2 O/TEOA reaction systems. Specifically, the addition of HTO and stabilized ZnS enables the photocatalyst to effectively upgrade optical and electrical performances, contributing to efficient light-harvesting and photogenerated carrier separation, as well as interfacial charge transfer. The tremendous enhancement of photocatalytic performance reveals the superiority of the Z-scheme heterojunction assembled from HTO and CdS/ZnS, featuring the inner electric field derived from the band bending of HTO@CdS/ZnS make CdS resistant to photocorrosion. This study allows access to inspire studies on rationally modeling and constructing diverse heterostructures for the storage and conversion of renewables and chemicals.

Epitaxial heterostructures of colloidal lead halide perovskite nanocrystals (NCs) with other semiconductors, especially the technologically important metal chalcogenides, can offer an unprecedented level of control in wavefunction design and exciton/charge carrier engineering. These NC heterostructures are ideal material platforms for efficient optoelectronics and other applications. Existing methods, however, can only yield heterostructures with random connections and distributions of the two components. The lack of epitaxial relation and uniform geometry hinders the structure-function correlation and impedes the electronic coupling at the heterointerface. This work reports the synthesis of uniform, epitaxially grown CsPbBr 3 /CdS Janus NC heterostructures with ultrafast charge separation across the electronically coupled interface. Each Janus NC contains a CdS domain that grows exclusively on a single {220} facet of CsPbBr 3 NCs. Varying reaction parameters allows for precise control in the sizes of each domain and readily modulates the optical properties of Janus NCs. Transient absorption measurements and modeling results reveal a type II band alignment, where photoexcited electrons rapidly transfer (within ≈9 picoseconds) from CsPbBr 3 to CdS. The promoted charge separation and extraction in epitaxial Janus NCs leads to photoconductors with drastically improved (approximately three orders of magnitude) responsivity and detectivity, which is promising for ultrasensitive photodetection., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Surface plasmon resonance-induced charge separation plays key roles in plasmon-related applications, especially in photocatalysis and photovoltaics. Plasmon coupling nanostructures exhibit extraordinary behaviors in hybrid states, phonon scattering, and ultrafast plasmon dephasing, but plasmon-induced charge separation in these materials remains unknown. Here, we design Schottky-free Au nanoparticle (NP)/NiO/Au nanoparticles-on-a-mirror plasmonic photocatalysts to support plasmon-induced interfacial hole transfer, evidenced by surface photovoltage microscopy at the single-particle level. In particular, we observe a nonlinear increase in charge density and photocatalytic performance with an increase in excitation intensity in plasmonic photocatalysts containing hot spots as a result of varying the geometry. Such charge separation increased the internal quantum efficiency by 14 times at 600 nm in catalytic reactions as compared to that of the Au NP/NiO without a coupling effect. These observations provide an improved understanding of charge transfer management and utilization by geometric engineering and interface electronic structure for plasmonic photocatalysis.

Strain engineering is an attractive strategy for improving the intrinsic catalytic performance of heterogeneous catalysts. Manipulating strain on the short-range atomic scale to the local structure of the catalytic sites is still challenging. Herein, we successfully achieved atomic strain modulation on ultrathin layered vanadium oxide nanoribbons by an ingenious intercalation chemistry method. When trace sodium cations were introduced between the V 2 O 5 layers (Na + -V 2 O 5 ), the V-O bonds were stretched by the atomically strained vanadium sites, redistributing the local charges. The Na + -V 2 O 5 demonstrated excellent photooxidation performance, which was approximately 12 and 14 times higher than that of pristine V 2 O 5 and VO 2 , respectively. Complementary spectroscopy analysis and theoretical calculations confirmed that the atomically strained Na + -V 2 O 5 had a high surficial charge density, improving the activation of oxygen molecules and contributing to the excellent photocatalytic property. This work provides a new approach for the rational design of strain-equipped catalysts for selective photooxidation reactions.

The rational steering and construction of efficient and stable atomic interfaces is highly desirable but rather challenging in solar energy conversion. Here, we report an in-situ oxygen impregnation strategy to build abundant atomic interfaces composed of homogeneous Ru and RuO x amorphous hybrid-mixture with ultrafast charge transfer, for solar hydrogen evolution with sacrificial agent free. Via in-situ synchrotron X-ray absorption and photoelectron spectroscopies, we can precisely track and identify the gradual formation of atomic interfaces towards homogeneous Ru-RuO x hybrid-structure at the atomic level. Benefiting from the abundant interfaces, the amorphous RuO x sites can intrinsically trap the photoexcited hole within an ultrafast process (<100 fs), and the amorphous Ru sites enable subsequent electron transfer (~1.73 ps). Hence, this hybrid-structure triggers long-lived charge-separated states, and results in a high hydrogen evolution rate of 60.8 μmol·h -1 . This design integrating the two sites fulfilled each half-reaction in a single hybrid-structure suggests potential guidelines towards efficient artificial photosynthesis., (© 2023. The Author(s).)

Manipulation of solid-state spin coherence is an important paradigm for quantum information processing. Current systems either operate at very low temperatures or are difficult to scale up. Developing low-cost, scalable materials whose spins can be coherently manipulated at room temperature is thus highly attractive for a sustainable future of quantum information science. Here we report ambient-condition all-optical initialization, manipulation and readout of hole spins in an ensemble of solution-grown CsPbBr 3 perovskite quantum dots with a single hole in each dot. The hole spins are initialized by sub-picosecond electron scavenging following circularly polarized femtosecond-pulse excitation. A transverse magnetic field induces spin precession, and a second off-resonance femtosecond-pulse coherently rotates hole spins via strong light-matter interaction. These operations accomplish near-complete quantum-state control, with a coherent rotation angle close to the π radian, of hole spins at room temperature., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

As an analogue to thermally activated delayed fluorescence (TADF) of organic molecules, thermally activated delayed photoluminescence (TADPL) observed in molecule-functionalized semiconductor nanocrystals represents an exotic mechanism to harvest energy from dark molecular triplets and to obtain controllable, long-lived PL from nanocrystals. The reported TADPL systems have successfully covered the visible spectrum. However, TADF molecules already emit very efficiently in the visible, diminishing the technological impact of the less-efficient nanocrystal-molecule TADPL. Here we report bright, near-infrared TADPL in lead-free CuInSe 2 nanocrystals functionalized with carboxylated tetracene ligands, which results from efficient triplet energy transfer from photoexcited nanocrystals to ligands, followed with thermally activated reverse energy transfer from ligand triplets back to nanocrystals. This strategy prolonged the nanocrystal exciton lifetime from 100 ns to 60 μs at room temperature., (© 2022 Wiley-VCH GmbH.)

Purpose: Carbapenem-resistant Klebsiella pneumoniae (CRKP) has seriously threatened public health worldwide. This study aimed to investigate the antimicrobial resistance patterns, sequence types (STs), virulence and carbapenemase genes of CRKP isolates from patients in Zunyi, China., Methods: CRKP isolates were collected from the First People's Hospital of Zunyi between January 2018 and December 2020. Antimicrobial susceptibility was determined using a VITEK ® 2 analyzer and confirmed using either the broth dilution method, Kirby-Bauer method, or E-test assays. Carbapenemase production was examined using a modified carbapenem inactivation method. STs of the studied isolates were determined by multilocus sequence typing, and the presence of carbapenemase and virulence genes was examined using polymerase chain reaction assays., Results: In total, 94 CRKP isolates were collected. All studied isolates produced carbapenemase, and the most common carbapenemase gene was New Delhi metallo-β-lactamase (NDM; 72.3%), followed by Klebsiella pneumoniae carbapenemase (KPC; 24.5%), and Verona integron-encoded metallo-β-lactamase (VIM; 3.2%). Of the studied isolates, 74.3% exhibited multidrug-resistant (MDR) phenotype, and 25.7% were either pandrug-resistant (PDR) or extensively drug-resistant (XDR) phenotypes. The most prevalent sequence type was ST2407 (37.2%), followed by ST76 (21.3%) and ST11 (11.7%). The NDM gene was present in 97.1% of ST2407 isolates and 90.0% of ST76 isolates, whereas the KPC gene was present in 90.9% of ST11 isolates. The majority of the isolates carried wabG, uge , and fimH virulence genes, with prevalence rates of 94.7%, 92.6%, and 94.7%, respectively., Conclusion: This study describes NDM-producing ST2407 and ST76, as well as KPC-producing ST11, as the major clonal types of CRKP isolates in Zunyi, China. All CRKP isolates were resistant to multiple types of antibiotics, and the majority of isolates carried carbapenemase and virulence genes. Clonal spread of NDM-producing CRKP ST2407 and ST76, and KPC-producing CRKP ST11 should be strictly monitored., Competing Interests: The authors report no conflicts of interest in this work., (© 2023 Shen et al.)

Synthetic fluorescent protein chromophores have been reported for their singlet state fluorescence properties and applications in bioimaging, but rarely for the triplet state chemistries. Herein, we enabled their photo-sensitizing and photo-crosslinking properties through rational modulations. Extension of molecular conjugation and introduction of heavy atoms promoted the generation of reactive oxygen species. Unlike other photosensitizers, these chromophores selectively photo-crosslinked aggregated proteins and uncovered the interactome profiles. We also exemplified their general applications in chromophore-assisted light inactivation, photodynamic therapy and photo induced polymerization. Theoretical calculation, pathway analysis and transient absorption spectroscopy provided mechanistic insights for this triplet state chemistry. Overall, this work expands the function and application of synthetic fluorescent protein chromophores by enabling their triplet excited state properties., (© 2022 Wiley-VCH GmbH.)

Orbital mixing is paramount to chemistry as it plays a central role in bond formation. It is also important for technologies such as molecular doping of polymers, where the concept of fractional charge transfer is essentially orbital mixing between dopants and hosts. Likewise, it would be both fundamentally interesting and technologically relevant to investigate orbital mixing in emerging hybrid materials containing both inorganic and organic moieties. Here we report experimental observation of orbital mixing between valence band levels of strongly confined PbS quantum dots (QDs) and lowest unoccupied molecular levels of surface-bound high-electron affinity molecules (F4TCNQ), manifested as both an absorption blue-shift of PbS and the emergence of visible and infrared signatures of the fractional charge-transfer species of F4TCNQ. The degree of mixing can be controlled by varying the QD size or by varying the molecule/QD ratio for a specific QD size and can be quantitatively reproduced by a nondegenerate, two-level perturbation model.

It is well known that charge separation is crucial for efficient photocatalytic solar conversion. Although some covalent-organic frameworks (COFs) exhibit visible-light harvest, the large exciton binding energies reduce their photocatalytic efficiencies. Herein, we developed a novel method to post-treat the olefin-linked COFs with end-capping polycyclic aromatic hydrocarbons (PAHs) for spontaneous charge separation. Interestingly, a type-II heterostructure is constructed in our perylene-modified COFs which displays drastically enhanced performance for photocatalytic CO 2 reduction, with an efficiency of 8-fold higher than that of unmodified COF. A combination of electrochemical, steady-state, and time-resolved spectroscopic measurements indicates that such drastically enhanced performance should be attributed to photoinduced spontaneous charge separation in the heterostructure. These results illustrate the feasibility of engineering the charge-separation properties of crystalline porous frameworks at a molecular level for artificial photosynthesis., (© 2022 Wiley-VCH GmbH.)

Colloidal quantum dots (QDs) can photocatalyze diverse organic reactions. However, reported QD-photocatalysts often contain highly-toxic elements Cd or Pb, and have not surpassed prototypical transition-metal complexes in terms of their photoredox power or excited-state energy. Here we report low-toxicity ZnSe/ZnS core/shell QDs as potent visible photocatalysts to drive challenging organic transformations. To overcome the limitation of short excited-state lifetime of the QDs, we functionalize their surfaces with benzophenone ligands which can rapidly extract electrons from photoexcited QDs and sustain long-lived charge-separated states. The benzophenone anions function as potent electron relay to drive dehalogenation of aryl chlorides and additive-free polymerization of acrylates. Alternatively, the QDs are functionalized with biphenyl ligands to store energy in long-lived, energetic triplets, enabling [2+2] homo-cycloaddition of styrene and cycloaddition of carbonyls with alkenes., (© 2022 Wiley-VCH GmbH.)

Anisotropic exchange splitting in semiconductor quantum dots results in bright-exciton fine-structure splitting important for quantum information processing. Direct measurement of fine-structure splitting usually requires single/few quantum dots at liquid-helium temperature because of its sensitivity to quantum dot size and shape, whereas measuring and controlling fine-structure splitting at an ensemble level seem to be impossible unless all the dots are made to be nearly identical. Here we report strong bright-exciton fine-structure splitting up to 1.6 meV in solution-processed CsPbI 3 perovskite quantum dots, manifested as quantum beats in ensemble-level transient absorption at liquid-nitrogen to room temperature. The splitting is robust to quantum dot size and shape heterogeneity, and increases with decreasing temperature, pointing towards a mechanism associated with orthorhombic distortion of the perovskite lattice. Effective-mass-approximation calculations reveal an intrinsic 'fine-structure gap' that agrees well with the observed fine-structure splitting. This gap stems from an avoided crossing of bright excitons confined in orthorhombically distorted quantum dots that are bounded by the pseudocubic {100} family of planes., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

Luminescent solar concentrators (LSCs) have emerged as a disruptive technology that can potentially enable carbon-neutral buildings. The issues with current LSCs, however, are low optical efficiencies and limited long-term outdoor stability. Here we simultaneously address them by developing an LSC with aggregation-induced-emission (AIE) molecules embedded in a polydimethylsiloxane (PDMS) matrix. The AIE-emitter displayed a near unity emission quantum yield when embedded in the PDMS and the apparent absorption-emission Stokes shift reached 0.59 eV, effectively suppressing the reabsorption loss of waveguided photons inside an LSC. Moreover, the surface texture of the PDMS matrix was engineered using a bioinspired nanolithography method with a natural lotus leaf as the template. This allowed the fabricated AIE-PDMS LSC to inherit the superhydrophobic, self-cleaning properties of the leaf and meanwhile to possess a light-trapping capability. Our 100 cm 2 LSC, when coupled with commercial Si PVs, delivered efficient solar power conversion, high visible transmittance, and high working stability.

Copper matrix composites have a wide application as magnetic conductive materials, electromagnetic materials, electrical discharge machining materials, etc. Such materials are expected to have a good combination of excellent electrical conductivity and good mechanical strength. In this work, micro/nano hybrid reinforcements with Fe microspheres and reduced graphene oxide (rGO) nanosheets were developed for copper matrix composites. The rGO/Fe/Cu powders were firstly wet-mixed and then densified by the vacuum hot-pressing sintering to obtain the bulk compacts. Microstructure, electrical conductivity and mechanical properties of such compacts were investigated. Microstructural result of as-sintered compacts shows that the Fe microspheres could distribute in the matrix uniformly, and rGO nanosheets exhibit both agglomerated and dispersed states. The grain size of Cu matrix decreased with the increase of the rGO content. Hardness, compression and tensile 0.2% yield strength of the as-sintered compacts were improved evidently by the addition of the hybrid Fe/rGO, comparing with pure Cu and single Fe-added composites. However, a lower electrical conductivity appeared in the more rGO-added composites, but still reached more than 33.0% international annealing copper standard (IACS). These performance change could be sought in the spatially geometrical distribution and characteristics of such micro/nano Fe/rGO hybrid addition, and the relevant mechanisms were discussed.

Coherent interaction between matter and light field induces both optical Stark effect and Bloch-Siegert shift. Observing the latter has been historically challenging, because it is weak and is often accompanied by a much stronger Stark shift. Herein, by controlling the light helicity, we can largely restrict these two effects to different spin-transitions in CsPbI 3 perovskite quantum dots, achieving room-temperature Bloch-Siegert shift as strong as 4 meV with near-infrared pulses. The ratio between the Bloch-Siegert and optical Stark shifts is however systematically higher than the prediction by the non-interacting, quasi-particle model. With a model that explicitly accounts for excitonic effects, we quantitatively reproduce the experimental observations. This model depicts a unified physical picture of the optical Stark effect, biexcitonic optical Stark effect and Bloch-Siegert shift in low-dimensional materials displaying strong many-body interactions, forming the basis for the implementation of these effects to information processing, optical modulation and Floquet engineering., (© 2022. The Author(s).)

A relatively new addition to the application portfolio of lead halide perovskites is to photosensitize molecular triplets for a variety of photochemical applications. Here we report visible-light-driven isomerization and cycloaddition of organic molecules sensitized by spectrally-tunable perovskite nanocrystals. We first demonstrate with stilbene as the substrate molecule that photoisomerization can proceed efficiently and rapidly by either directly grafting carboxylated stilbene onto nanocrystal surfaces or using triplet-acceptor ligands as the energy relay. The relay approach is more generally applicable as it does not require anchoring-group functionalization of substrate molecules, allowing us to facilely extend it to isomerization of a series of substituted stilbene molecules and ring-closing isomerization of diarylethene, as well as intermolecular [2+2] cycloaddition of acenaphthylene. This study opens an avenue of energy-transfer photocatalysis using perovskite nanocrystals., (© 2022 Wiley-VCH GmbH.)