Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from...Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.展开更多
Molecular recognition of bioreceptors and enzymes relies on orthogonal interactions with small molecules within their cavity. To date, Chinese scientists have developed three types of strategies for introducing active...Molecular recognition of bioreceptors and enzymes relies on orthogonal interactions with small molecules within their cavity. To date, Chinese scientists have developed three types of strategies for introducing active sites inside the cavity of macrocyclic arenes to better mimic molecular recognition of bioreceptors and enzymes.The editorial aims to enlighten scientists in this field when they develop novel macrocycles for molecular recognition, supramolecular assembly, and applications.展开更多
Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic hav...Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH.Based on this scheme,significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions.However,we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes.Using time-dependent density functional theory,we simulated the dynamics of HHG from NH2COOH and NH2COSH interacting with linearly polarized lasers.We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region.Our analysis indicates that this is due to the complex molecular configuration of NH_(2)COOH and NH_(2)COSH:while the NH_(2) group has C_(2v) symmetry,both COOH and COSH groups lack this symmetry.This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups,but not to NH_(2) group.Additionally,our results reveal a multi-plateau structure in HHG signal along laser polarization direction,a phenomenon arising from multi-electron and multiorbital effects during interaction between complex molecule and strong laser field.展开更多
Biology is governed by macromolecular interactions,perturbation of which often lies at the heart of disease.Most therapeutic drugs,whether they are small molecules or biologics,exert their effects through impeding suc...Biology is governed by macromolecular interactions,perturbation of which often lies at the heart of disease.Most therapeutic drugs,whether they are small molecules or biologics,exert their effects through impeding such interactions,whether they are of an enzyme with its substrate or a ligand with its receptor.Conversely,a handful of approved drugs and a larger number of candidates in development have the opposite effect:They either activate or inhibit a biological output by stabilizing a preexisting complex through reducing the rate at which its components dissociate(koff).展开更多
The ring has been a romantic fascination throughout the ages,embodying not only beauty and order but also harboring numerous undisclosed properties awaiting discovery.In the realm of supramolecular chemistry,macrocycl...The ring has been a romantic fascination throughout the ages,embodying not only beauty and order but also harboring numerous undisclosed properties awaiting discovery.In the realm of supramolecular chemistry,macrocycles,with a cyclic structure and a central cavity like a doughnut,captivate the attention of scientists[1].In 1967,Pedersen's groundbreaking revelation that alkali metal ions could"fall into"the cavities of a cyclic ether named crown ether,even in organic solvents,unveiled a novel universe of macrocycle chemistry.Since then,numerous macrocyclic structures in nature have been discovered,isolated,and scrutinized.Drawing inspiration from nature,chemists endeavor to explore the vast potential of macrocyclic compounds by designing and synthesizing artificial macrocycles with diverse structural features and recognition properties.展开更多
Circularly polarized luminescence(CPL)-active materials have a wide range of technological applications.Traditionally,creating CPL-active materials relies on the use of chiral luminophores.In contrast,supramolecular a...Circularly polarized luminescence(CPL)-active materials have a wide range of technological applications.Traditionally,creating CPL-active materials relies on the use of chiral luminophores.In contrast,supramolecular assembly introduces an innovative and promising strategy for developing CPL-active materials not only from chiral luminophores but also from achiral species.This approach significantly enriches the diversity of CPL-active materials.It also offers an effective means to optimize the performance of CPL-active materials,such as enhancing the asymmetry factor|glum|.Compared to polymers,the assembly of small molecules is generally easier to control.This review systematically summarizes the recent progress and developments in CPL from small-molecule assemblies,particularly focusing on differences,merits,and demerits of three typical assembly modes.The aim is to provide valuable insights for the future development of chiroptical materials.展开更多
CRISPR-based tran-scription regulators(CRISPR-TRs)have revolutionized the field of synthetic biol-ogy by enabling tar-geted activation or repression of any de-sired gene.However,the majority of exist-ing inducible CRI...CRISPR-based tran-scription regulators(CRISPR-TRs)have revolutionized the field of synthetic biol-ogy by enabling tar-geted activation or repression of any de-sired gene.However,the majority of exist-ing inducible CRISPR-TRs are limited by their dependence on specific sequences,which restricts their flex-ibility and controllability in genetic engineering applications.In this study,we proposed a novel strategy to construct sequence-independent inducible CRISPR-TRs,which is achieved by the design of stem loop 2 in the single guide RNA(sgRNA).Under this strategy,by utiliz-ing toehold-mediated strand displacement(TMSD)reactions between small endogenous molecules(miR-20a and TK1 mRNA)and bridge RNA(bRNA)to link bRNA with sgRNA,we achieved synergistic transcriptional activation of VP64 and p65-HSF1 in response to en-dogenous molecules.To enable response to exogenous molecules,we added response se-quences and bRNA sequences to the 5'end of sgRNA to block sgRNA activity,and achieved activation of sgRNA by shearing the response sequence,called sequential unlimited interlock-ing(SUI).Compared with conventional sequence-restricted interlocking(spacer-blocking hairpin(SBH)),the transcriptional activation ratio between response and non-response to the Cas6A protein using our approach was increased by 2.28-fold.Our work presents a modular and versatile framework for endogenous and exogenous molecule-responsive CRISPR-TRs in mammalian cells,without limitations imposed by sequence dependence.展开更多
Natural molecular machines have inspired the development of artificial molecular machines,which have the potential to revolutionize several areas of technology.Artificial molecular machines commonly employ molecular s...Natural molecular machines have inspired the development of artificial molecular machines,which have the potential to revolutionize several areas of technology.Artificial molecular machines commonly employ molecular switches,molecular motors,and molecular shuttles as fundamental building blocks.The observation of artificial molecular machines constructed by these building blocks can be highly challenging due to their small sizes and intricate behaviors.The use of modern instrumentation and advanced observational techniques plays a crucial role in the observation and characterization of molecular machines.Furthermore,a well-designed molecular structure is also a critical factor in making molecular ma-chines more observable.This review summarizes the common methods from diverse perspectives used to observe molecular machines and emphasizes the significance of comprehending their behaviors in the design of superior artificial molecular machines.展开更多
Single-molecule junctions are building blocks for constructing molecular devices.However,intermolecular interactions like winding bring additional interference among the surrounding molecules,which inhibits the intrin...Single-molecule junctions are building blocks for constructing molecular devices.However,intermolecular interactions like winding bring additional interference among the surrounding molecules,which inhibits the intrinsic coherent transport through single-molecule junctions.Here,we employed a nanocavity(dimethoxypillar[5]arene,DMP[5]),which is analogous to electric cables,to confine the conformation of flexible chains(1,8-diaminooctane,DAO)via host-vip interaction.Single-molecule conductance measurements indicate that the conductance of DAO encapsulated with DMP[5]is as high as that of pure DAO,as reproduced by theoretical simulations.Intriguingly,the molecular lengths of the DAO encapsulated with DMP[5]increase from 1.13 nm to 1.46 nm compared with the pure DAO,indicating that DMP[5]keeps DAO upright-standing via the confinement effect.This work provides a new strategy to decouple the intermolecular interaction by employing an insulating sheath,enabling the high-density integration of single-molecule devices.展开更多
Colloidal molecules exhibit unique electronic,optical,and magnetic properties owing to their molecular-like configurations and coupling effects,making them promising building blocks for multifunctional materials.Howev...Colloidal molecules exhibit unique electronic,optical,and magnetic properties owing to their molecular-like configurations and coupling effects,making them promising building blocks for multifunctional materials.However,achieving precise and controllable assembly of isotropic nanoparticles with high yields remains a great challenge.In this study,we present a synergistic strategy that integrates molecular dynamics simulations with interpretable machine learning to develop a programmable assembly system based on block copolymers and DNA-functionalized nanoparticles.Our simulation results reveal that block copolymer modification facilitates stepwise control over surface phase separation and nanoparticle coassembly,thereby enhancing structural stability and efficiently suppressing disordered aggregation of atom-like nanoparticles.Furthermore,we demonstrated that precise,controllable,and programmable assembly of colloidal molecules can be achieved through rational DNA sequence design.SHapley Additive exPlanations(SHAP)analysis identified key structural descriptors that govern assembly outcomes and elucidated their underlying mechanistic roles.This work not only deepens the understanding of colloidal molecule assembly mechanisms but also lays a theoretical foundation for the rational design of functional colloidal architectures in nanomaterial science.展开更多
Despite the exceptional efficiency of hole-selective self-assembled molecular layer(SAML),challenges persist due to SAML agglomeration and the incomplete passivation of buried perovskite defects,which hinder efficient...Despite the exceptional efficiency of hole-selective self-assembled molecular layer(SAML),challenges persist due to SAML agglomeration and the incomplete passivation of buried perovskite defects,which hinder efficient hole transfer and compromise device stability.In this study,we introduce a novel V-shaped molecule,4,4′-(perfluorocyclopent-1-ene-1,2-diyl)bis(N,N-bis(4-methoxyphenyl)aniline)(DPTAE),comprising a perfluorocyclopentene core flanked by two triphenylamine units,designed for incorporation at the perovskite buried interface.Owing to its sterically hindered,nonplanar structure,DPTAE functions as a“wedge”within the SAML,disrupting molecular aggregation and yielding an amorphous hole-selective layer.This redefined interfacial architecture facilitates enhanced charge extraction and minimizes interfacial defect states.As a result,the optimized wide-bandgap perovskite solar cells(PSCs)with a bandgap of 1.68 eV achieved an impressive power conversion efficiency(PCE)of 22.33%and a fill factor(FF)of 86.24%.Notably,the encapsulated devices exhibited superior stability under damp-heat conditions(ISOS-D-3,85%RH,85℃)with a T_(88)of 1000 h,and maintained stable maximum power point tracking(ISOS-L-2,40%RH)with a T_(92)of 500 h.Furthermore,DPTAE-based monolithic perovskite/silicon tandem solar cells attained a remarkable efficiency of 30.50%.This innovative approach not only deepens our understanding of interfacial dynamics but also opens new avenues for engineering advanced solar cell architectures,thereby advancing perovskite-based photovoltaic technologies.展开更多
All-small-molecule organic solar cells(ASM-OSCs)have garnered widespread attention in recent years.However,their power conversion efficiencies(PCEs)still fall behind those of polymer donor-based devices,primarily due ...All-small-molecule organic solar cells(ASM-OSCs)have garnered widespread attention in recent years.However,their power conversion efficiencies(PCEs)still fall behind those of polymer donor-based devices,primarily due to the challenge of realizing optimized morphology in ASM-OSCs.Here,a highly crystalline small molecule donor(SMD)named ZW2 is synthesized and incorporated into the Zn PTSEH:6TIC system.The addition of ZW2 synergistically regulates the morphology,molecular crystallinity,and molecular packing of blends,facilitating efficient charge transport and suppressing charge recombination.Consequently,an impressive PCE of 16.30%was delivered in the ternary device.This work highlights the significance of employing a highly crystalline SMD as the third component in tuning the crystallinity and morphology of blends,providing feasibility for achieving high-efficiency ASM-OSCs.展开更多
We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equatio...We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equations based on a direct numerical solution for the time-dependent density matrix.We analyze the relationship between the frequency chirping rate and the number of Mg F molecules and Rb atoms.In addition,we study the dynamical process of molecular deceleration and the effect of transverse diffusion.Monte–Carlo simulations show that buffer-gas-cooled Mg F and Rb beams,with initial velocities of 200 m/s and 130 m/s respectively,can be decelerated to less than 10 m/s.This is achieved with laser powers of as low as 357 m W for Mg F and 10 m W for Rb per traveling wave.The rapid deceleration minimizes molecular loss due to transverse diffusion during the deceleration process.The estimated number of molecules that can be trapped in a magneto-optical trap(MOT)is about 9.0×10^(6),which is an order of magnitude larger than the number of Mg F molecules decelerated by the spontaneous radiation force.The results offer a promising starting point for further studies of sympathetic cooling.展开更多
Structural optimization of lead compounds is a crucial step in drug discovery.One optimization strategy is to modify the molecular structure of a scaffold to improve both its biological activities and absorption,distr...Structural optimization of lead compounds is a crucial step in drug discovery.One optimization strategy is to modify the molecular structure of a scaffold to improve both its biological activities and absorption,distribution,metabolism,excretion,and toxicity(ADMET)properties.One of the deep molecular generative model approaches preserves the scaffold while generating drug-like molecules,thereby accelerating the molecular optimization process.Deep molecular diffusion generative models simulate a gradual process that creates novel,chemically feasible molecules from noise.However,the existing models lack direct interatomic constraint features and struggle with capturing long-range dependencies in macromolecules,leading to challenges in modifying the scaffold-based molecular structures,and creates limitations in the stability and diversity of the generated molecules.To address these challenges,we propose a deep molecular diffusion generative model,the three-dimensional(3D)equivariant diffusion-driven molecular generation(3D-EDiffMG)model.The dual strong and weak atomic interaction force-based long-range dependency capturing equivariant encoder(dual-SWLEE)is introduced to encode both the bonding and non-bonding information based on strong and weak atomic interactions.Addi-tionally,a gate multilayer perceptron(gMLP)block with tiny attention is incorporated to explicitly model complex long-sequence feature interactions and long-range dependencies.The experimental results show that 3D-EDiffMG effectively generates unique,novel,stable,and diverse drug-like molecules,highlighting its potential for lead optimization and accelerating drug discovery.展开更多
A singlet diatomic molecule naturally carries doubly degenerate ±Λ states when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contri...A singlet diatomic molecule naturally carries doubly degenerate ±Λ states when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contribute equally in conventional measurements and are thus treated the same in corresponding simulations. In this study, we demonstrate that in resonant excitation by intense laser pulses, the doubly degenerate ±Λ states must be clearly identified. This is exemplified in the X^(1)Σ → A^(1)Π transition of CO molecules. This distinction becomes especially important in the case of circularly polarized radiation. We attribute this phenomenon to the interference of electron-rotational pathways in the strong-field coupled transition with the ±Λ-state of the excited Π state. This research sheds light on the fundamental aspects of intense laser-molecule interactions when extending conventional theories.展开更多
Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and e...Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.展开更多
Atomically precise coordination nanoclusters(NCs)constitute a pivotal and rapidly advancing domain in the realms of materials science and chemistry owing to their distinctive crystal structures and exceptional attribu...Atomically precise coordination nanoclusters(NCs)constitute a pivotal and rapidly advancing domain in the realms of materials science and chemistry owing to their distinctive crystal structures and exceptional attributes encompassing molecular magnetism[1],photoluminescence[2],and catalysis[3].Organic ligands play a crucial role in effectively shielding these NCs,serving two primary functions:firstly,vital in preventing NC aggregation,particularly for the formation of robust single-crystal structures;secondly,acting as either bridging or peripheral structural components of NCs[4].This characterization of organic-inorganic hybridization offers unique advantages for unraveling the intricate relationships between structure and properties[5].展开更多
Stroke is the second leading cause of disability and mortality worldwide,imposing a substantial socioeconomic burden on individuals and healthcare systems.Annually,approximately 14 million people experience stroke,wit...Stroke is the second leading cause of disability and mortality worldwide,imposing a substantial socioeconomic burden on individuals and healthcare systems.Annually,approximately 14 million people experience stroke,with ischemic stroke comprising nearly 85%of cases,of which 10%to 20%involve large vessel occlusions.Currently,recombinant tissue plasminogen activator(tPA)remains the only approved pharmacological intervention.However,its utility is limited due to a narrow therapeutic window and low recanalization rates,making it applicable to only a minority of patients.Therefore,there is an urgent need for novel therapeutic strategies,including pharmacological advancements and combinatory treatments.Small-molecule natural medicines,particularly those derived from traditional Chinese herbs,have demonstrated significant therapeutic potential in ischemic stroke management.These compounds exert multiple neuroprotective effects,such as antioxidation,anti-inflammatory action,and inhibition of apoptosis,all of which are critical in mitigating stroke-induced cerebral damage.This review comprehensively examines the pathophysiology of acute ischemic stroke(AIS)and highlights the recent progress in the development of small-molecule natural medicines as promising therapeutic agents for cerebral ischemic stroke.展开更多
OBJECTIVE:To explore if Hewei Jiangni granule(和胃降逆颗粒,HWJNG)could regulate esophageal hypersensitivity via stromal interaction molecule 1(STIM1)/transient receptor potential vanilloid subfamily member 1(TRPV1)pat...OBJECTIVE:To explore if Hewei Jiangni granule(和胃降逆颗粒,HWJNG)could regulate esophageal hypersensitivity via stromal interaction molecule 1(STIM1)/transient receptor potential vanilloid subfamily member 1(TRPV1)pathway.METHODS:Qualitative analysis of HWJNG was analysis by high performance of liquid and gas chromatography.In vivo,animal model of non-erosive reflux disease(NERD)was established by fructose intake and restraint stress.HWJNG and Omeprazole were administered by gavage to the drug intervention group.Reflux and visceral hypersensitivity were analyzed by pathological changes,PH value test,mechanical paw withdrawal threshold,thermal withdrawal latency and mast cells(MCs)degranulation.In vitro,substance P(SP)-induced P815 cells and dorsal root ganglion(DRG)cells were cocultured.Expression in both mice and cells of STIM1,TRPV1,and esophageal visceral hypersensitivity-related gastrointestinal neurochemicals were validated by enzyme linked immunosorbent assays,quantitative realtime polymerase chain reaction(qRT-PCR)and Western blot.Moreover,overexpression and small interfering RNA against STIM1 were utilized to verify of the role of HWJNG in DRG cells.RESULTS:HWJNG significantly suppressed intercellular space widening,injury of mitochondrial,MCs degranulation,mechanical allodynia and heat neuropathic sensory and increased pH value of esophageal mucosa in NERD mice.HWJNG inhibited expression of visceral hypersensitivityrelated gastrointestinal neurochemicals in esophageal mucosa and activated P815 cells,and expression of the STIM1,TRPV1 and related neurotransmitters in DRG and DRG cells.STIM1 siRNA and HWJNG both reduced P815 cells adhesion to DRGs cells and Ca2+flow into the cytoplasmic space of DRG cells.Furthermore,HWJNG could reversed STIM1 overexpression induced upregulation of TRPV1.CONCLUSION:HWJNG suppressed intercellular space widening in NERD mice,stabilized MCs and restored neuronal hyperexcitability by regulating visceral hypersensitivity via STIM1/TRPV1 pathway.展开更多
The process of neurite outgrowth and branching is a crucial aspect of neuronal development and regeneration.Axons and dendrites,sometimes referred to as neurites,are extensions of a neuron's cellular body that are...The process of neurite outgrowth and branching is a crucial aspect of neuronal development and regeneration.Axons and dendrites,sometimes referred to as neurites,are extensions of a neuron's cellular body that are used to start networks.Here we explored the effects of diethyl(3,4-dihydroxyphenethylamino)(quinolin-4-yl)methylphosphonate(DDQ)on neurite developmental features in HT22 neuronal cells.In this work,we examined the protective effects of DDQ on neuronal processes and synaptic outgrowth in differentiated HT22cells expressing mutant Tau(mTau)cDNA.To investigate DDQ chara cteristics,cell viability,biochemical,molecular,western blotting,and immunocytochemistry were used.Neurite outgrowth is evaluated through the segmentation and measurement of neural processes.These neural processes can be seen and measured with a fluorescence microscope by manually tracing and measuring the length of the neurite growth.These neuronal processes can be observed and quantified with a fluorescent microscope by manually tracing and measuring the length of the neuronal HT22.DDQ-treated mTau-HT22 cells(HT22 cells transfected with cDNA mutant Tau)were seen to display increased levels of synaptophysin,MAP-2,andβ-tubulin.Additionally,we confirmed and noted reduced levels of both total and p-Tau,as well as elevated levels of microtubule-associated protein 2,β-tubulin,synaptophysin,vesicular acetylcholine transporter,and the mitochondrial biogenesis protein-pe roxisome prolife rator-activated receptor-gamma coactivator-1α.In mTa u-expressed HT22 neurons,we observed DDQ enhanced the neurite characteristics and improved neurite development through increased synaptic outgrowth.Our findings conclude that mTa u-HT22(Alzheimer's disease)cells treated with DDQ have functional neurite developmental chara cteristics.The key finding is that,in mTa u-HT22 cells,DDQ preserves neuronal structure and may even enhance nerve development function with mTa u inhibition.展开更多
基金supported by the financial support from the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Aqueous Zn-iodine batteries(ZIBs)face the formidable challenges towards practical implementation,including metal corrosion and rampant dendrite growth on the Zn anode side,and shuttle effect of polyiodide species from the cathode side.These challenges lead to poor cycle stability and severe self-discharge.From the fabrication and cost point of view,it is technologically more viable to deploy electrolyte engineering than electrode protection strategies.More importantly,a synchronous method for modulation of both cathode and anode is pivotal,which has been often neglected in prior studies.In this work,cationic poly(allylamine hydrochloride)(Pah^(+))is adopted as a low-cost dual-function electrolyte additive for ZIBs.We elaborate the synchronous effect by Pah^(+)in stabilizing Zn anode and immobilizing polyiodide anions.The fabricated Zn-iodine coin cell with Pah^(+)(ZnI_(2) loading:25 mg cm^(−2))stably cycles 1000 times at 1 C,and a single-layered 3.4 cm^(2) pouch cell(N/P ratio~1.5)with the same mass loading cycles over 300 times with insignificant capacity decay.
文摘Molecular recognition of bioreceptors and enzymes relies on orthogonal interactions with small molecules within their cavity. To date, Chinese scientists have developed three types of strategies for introducing active sites inside the cavity of macrocyclic arenes to better mimic molecular recognition of bioreceptors and enzymes.The editorial aims to enlighten scientists in this field when they develop novel macrocycles for molecular recognition, supramolecular assembly, and applications.
基金supported by the Fundamental Research Funds for the Central Universities(Grant Nos.GK202207012 and QCYRCXM-2022-241).
文摘Permanent dipole moments induced high-order harmonic generation(HHG)signals offer a potential approach to producing elliptically or even circularly polarized X-ray attosecond sources.Previous studies on this topic have mainly focused on diatomic molecules such as CO and HeH.Based on this scheme,significant HHG signals in the direction perpendicular to the molecular axis can be observed in both the high-energy and low-energy regions.However,we found that the high-order harmonics induced by the permanent dipole moments of polyatomic complex molecules involve more intricate physical processes.Using time-dependent density functional theory,we simulated the dynamics of HHG from NH2COOH and NH2COSH interacting with linearly polarized lasers.We found that the harmonic signals in the direction perpendicular to the N-C bond were significantly enhanced in the high-energy photon region.Our analysis indicates that this is due to the complex molecular configuration of NH_(2)COOH and NH_(2)COSH:while the NH_(2) group has C_(2v) symmetry,both COOH and COSH groups lack this symmetry.This structural characteristic results in permanent dipole moments being felt only when electrons return to either COSH or COOH groups,but not to NH_(2) group.Additionally,our results reveal a multi-plateau structure in HHG signal along laser polarization direction,a phenomenon arising from multi-electron and multiorbital effects during interaction between complex molecule and strong laser field.
文摘Biology is governed by macromolecular interactions,perturbation of which often lies at the heart of disease.Most therapeutic drugs,whether they are small molecules or biologics,exert their effects through impeding such interactions,whether they are of an enzyme with its substrate or a ligand with its receptor.Conversely,a handful of approved drugs and a larger number of candidates in development have the opposite effect:They either activate or inhibit a biological output by stabilizing a preexisting complex through reducing the rate at which its components dissociate(koff).
文摘The ring has been a romantic fascination throughout the ages,embodying not only beauty and order but also harboring numerous undisclosed properties awaiting discovery.In the realm of supramolecular chemistry,macrocycles,with a cyclic structure and a central cavity like a doughnut,captivate the attention of scientists[1].In 1967,Pedersen's groundbreaking revelation that alkali metal ions could"fall into"the cavities of a cyclic ether named crown ether,even in organic solvents,unveiled a novel universe of macrocycle chemistry.Since then,numerous macrocyclic structures in nature have been discovered,isolated,and scrutinized.Drawing inspiration from nature,chemists endeavor to explore the vast potential of macrocyclic compounds by designing and synthesizing artificial macrocycles with diverse structural features and recognition properties.
基金support from the National Natural Science Foundation of China(52473192)。
文摘Circularly polarized luminescence(CPL)-active materials have a wide range of technological applications.Traditionally,creating CPL-active materials relies on the use of chiral luminophores.In contrast,supramolecular assembly introduces an innovative and promising strategy for developing CPL-active materials not only from chiral luminophores but also from achiral species.This approach significantly enriches the diversity of CPL-active materials.It also offers an effective means to optimize the performance of CPL-active materials,such as enhancing the asymmetry factor|glum|.Compared to polymers,the assembly of small molecules is generally easier to control.This review systematically summarizes the recent progress and developments in CPL from small-molecule assemblies,particularly focusing on differences,merits,and demerits of three typical assembly modes.The aim is to provide valuable insights for the future development of chiroptical materials.
基金supported by the National Natural Science Foundation of China(No.22073090,No.21991132,No.52021002)the National Key R&D Program of China(No.2020YFA0710700)the Funds of Youth Innovation Promotion Association,and the Fundamental Research Funds for the Central Universities(WK3450000009).
文摘CRISPR-based tran-scription regulators(CRISPR-TRs)have revolutionized the field of synthetic biol-ogy by enabling tar-geted activation or repression of any de-sired gene.However,the majority of exist-ing inducible CRISPR-TRs are limited by their dependence on specific sequences,which restricts their flex-ibility and controllability in genetic engineering applications.In this study,we proposed a novel strategy to construct sequence-independent inducible CRISPR-TRs,which is achieved by the design of stem loop 2 in the single guide RNA(sgRNA).Under this strategy,by utiliz-ing toehold-mediated strand displacement(TMSD)reactions between small endogenous molecules(miR-20a and TK1 mRNA)and bridge RNA(bRNA)to link bRNA with sgRNA,we achieved synergistic transcriptional activation of VP64 and p65-HSF1 in response to en-dogenous molecules.To enable response to exogenous molecules,we added response se-quences and bRNA sequences to the 5'end of sgRNA to block sgRNA activity,and achieved activation of sgRNA by shearing the response sequence,called sequential unlimited interlock-ing(SUI).Compared with conventional sequence-restricted interlocking(spacer-blocking hairpin(SBH)),the transcriptional activation ratio between response and non-response to the Cas6A protein using our approach was increased by 2.28-fold.Our work presents a modular and versatile framework for endogenous and exogenous molecule-responsive CRISPR-TRs in mammalian cells,without limitations imposed by sequence dependence.
基金supported by“Zhishan”Scholars Programs of Southeast University,Jiangsu Innovation Team Program,and the Fundamental Research Funds for the Central Universities.
文摘Natural molecular machines have inspired the development of artificial molecular machines,which have the potential to revolutionize several areas of technology.Artificial molecular machines commonly employ molecular switches,molecular motors,and molecular shuttles as fundamental building blocks.The observation of artificial molecular machines constructed by these building blocks can be highly challenging due to their small sizes and intricate behaviors.The use of modern instrumentation and advanced observational techniques plays a crucial role in the observation and characterization of molecular machines.Furthermore,a well-designed molecular structure is also a critical factor in making molecular ma-chines more observable.This review summarizes the common methods from diverse perspectives used to observe molecular machines and emphasizes the significance of comprehending their behaviors in the design of superior artificial molecular machines.
基金supported by the National Natural Science Foundation of China(Nos.22205084,42307566,22325303,22250003,T2222002,21991130,22032004)Fujian Provincial Natural Science Foundation of China(No.2022H6014)+4 种基金the China Postdoctoral Science Foundation(Nos.2023M741039,2023M742199)Project funded by National&Local Joint Engineering Research Center for Mineral Salt Deep Utilization(No.SF202303)State Key Laboratory of Efficient Utilization for Low Grade Phosphate Rock and Its Associated Resources WFKF(2023)013the Fundamental Research Funds for the Central Universities(Xiamen University,No.20720240053)State Key Laboratory of Vaccines for Infectious Diseases,Xiang An Biomedicine Laboratory(No.2023XAKJ0103074)。
文摘Single-molecule junctions are building blocks for constructing molecular devices.However,intermolecular interactions like winding bring additional interference among the surrounding molecules,which inhibits the intrinsic coherent transport through single-molecule junctions.Here,we employed a nanocavity(dimethoxypillar[5]arene,DMP[5]),which is analogous to electric cables,to confine the conformation of flexible chains(1,8-diaminooctane,DAO)via host-vip interaction.Single-molecule conductance measurements indicate that the conductance of DAO encapsulated with DMP[5]is as high as that of pure DAO,as reproduced by theoretical simulations.Intriguingly,the molecular lengths of the DAO encapsulated with DMP[5]increase from 1.13 nm to 1.46 nm compared with the pure DAO,indicating that DMP[5]keeps DAO upright-standing via the confinement effect.This work provides a new strategy to decouple the intermolecular interaction by employing an insulating sheath,enabling the high-density integration of single-molecule devices.
基金financially supported by the National Natural Science Foundation of China(Nos.92477118 and 22173045)the Postgraduate Research and Practice Innovation Program of Jiangsu Province(No.KYCX25_0188)。
文摘Colloidal molecules exhibit unique electronic,optical,and magnetic properties owing to their molecular-like configurations and coupling effects,making them promising building blocks for multifunctional materials.However,achieving precise and controllable assembly of isotropic nanoparticles with high yields remains a great challenge.In this study,we present a synergistic strategy that integrates molecular dynamics simulations with interpretable machine learning to develop a programmable assembly system based on block copolymers and DNA-functionalized nanoparticles.Our simulation results reveal that block copolymer modification facilitates stepwise control over surface phase separation and nanoparticle coassembly,thereby enhancing structural stability and efficiently suppressing disordered aggregation of atom-like nanoparticles.Furthermore,we demonstrated that precise,controllable,and programmable assembly of colloidal molecules can be achieved through rational DNA sequence design.SHapley Additive exPlanations(SHAP)analysis identified key structural descriptors that govern assembly outcomes and elucidated their underlying mechanistic roles.This work not only deepens the understanding of colloidal molecule assembly mechanisms but also lays a theoretical foundation for the rational design of functional colloidal architectures in nanomaterial science.
基金the financial support from the Natural Science Foundation of Xiamen,China(No.3502Z202373075)the Natural Science Foundation of Fujian Province(No.2024J01189)+1 种基金the financial support from the National Natural Science Foundation of China(Grant nos.22175180,52311530673)Universiti Teknologi Malaysia AJ090000.6700.09453-Tabung Pembayaran Lantikan Skim Prominent Visiting Researcher Scheme JTNCPI。
文摘Despite the exceptional efficiency of hole-selective self-assembled molecular layer(SAML),challenges persist due to SAML agglomeration and the incomplete passivation of buried perovskite defects,which hinder efficient hole transfer and compromise device stability.In this study,we introduce a novel V-shaped molecule,4,4′-(perfluorocyclopent-1-ene-1,2-diyl)bis(N,N-bis(4-methoxyphenyl)aniline)(DPTAE),comprising a perfluorocyclopentene core flanked by two triphenylamine units,designed for incorporation at the perovskite buried interface.Owing to its sterically hindered,nonplanar structure,DPTAE functions as a“wedge”within the SAML,disrupting molecular aggregation and yielding an amorphous hole-selective layer.This redefined interfacial architecture facilitates enhanced charge extraction and minimizes interfacial defect states.As a result,the optimized wide-bandgap perovskite solar cells(PSCs)with a bandgap of 1.68 eV achieved an impressive power conversion efficiency(PCE)of 22.33%and a fill factor(FF)of 86.24%.Notably,the encapsulated devices exhibited superior stability under damp-heat conditions(ISOS-D-3,85%RH,85℃)with a T_(88)of 1000 h,and maintained stable maximum power point tracking(ISOS-L-2,40%RH)with a T_(92)of 500 h.Furthermore,DPTAE-based monolithic perovskite/silicon tandem solar cells attained a remarkable efficiency of 30.50%.This innovative approach not only deepens our understanding of interfacial dynamics but also opens new avenues for engineering advanced solar cell architectures,thereby advancing perovskite-based photovoltaic technologies.
基金the National Key Research and Development Program of China(2022YFB4200400)funded by the Ministry of Science and Technology of China,the National Natural Science Foundation of China(52172048,52103221,22205130)+7 种基金the Shandong Provincial Natural Science Foundation(ZR2021ZD06,2023HWYQ026)the Guangdong Basic and Applied Basic Research Foundation(2023A1515012323,2023A1515010943,2022A1515110643,2024A1515010023)the Qingdao New Energy Shandong Laboratory Open Project(QNESL OP 202309)the Open Foundation of State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures(MMCS2023OF04)the Jiangxi Provincial Key Laboratory of Functional Crystalline Materials Chemistry(20212BCD42018)the Fundamental Research Funds of Shandong University,the China Postdoctoral Science Foundation(2023M742063)the Shandong Postdoctoral Science Foundation(SDCX-ZG-202400256)the Guangxi Science and Technology Major Project(AA23073018)。
文摘All-small-molecule organic solar cells(ASM-OSCs)have garnered widespread attention in recent years.However,their power conversion efficiencies(PCEs)still fall behind those of polymer donor-based devices,primarily due to the challenge of realizing optimized morphology in ASM-OSCs.Here,a highly crystalline small molecule donor(SMD)named ZW2 is synthesized and incorporated into the Zn PTSEH:6TIC system.The addition of ZW2 synergistically regulates the morphology,molecular crystallinity,and molecular packing of blends,facilitating efficient charge transport and suppressing charge recombination.Consequently,an impressive PCE of 16.30%was delivered in the ternary device.This work highlights the significance of employing a highly crystalline SMD as the third component in tuning the crystallinity and morphology of blends,providing feasibility for achieving high-efficiency ASM-OSCs.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12174115 and 91836103)。
文摘We propose a scheme for dual-species deceleration and trapping of a cold atom–molecule mixture by a frequency chirping stimulated force.We study the stimulated force exerted on Mg F and Rb using optical Bloch equations based on a direct numerical solution for the time-dependent density matrix.We analyze the relationship between the frequency chirping rate and the number of Mg F molecules and Rb atoms.In addition,we study the dynamical process of molecular deceleration and the effect of transverse diffusion.Monte–Carlo simulations show that buffer-gas-cooled Mg F and Rb beams,with initial velocities of 200 m/s and 130 m/s respectively,can be decelerated to less than 10 m/s.This is achieved with laser powers of as low as 357 m W for Mg F and 10 m W for Rb per traveling wave.The rapid deceleration minimizes molecular loss due to transverse diffusion during the deceleration process.The estimated number of molecules that can be trapped in a magneto-optical trap(MOT)is about 9.0×10^(6),which is an order of magnitude larger than the number of Mg F molecules decelerated by the spontaneous radiation force.The results offer a promising starting point for further studies of sympathetic cooling.
基金supported by the National Key R&D Program of China(Grant No.:2023YFF1205102)the National Natural Science Foundation of China(Grant Nos.:82273856,22077143,and 21977127)the Science Foundation of Guangzhou,China(No.:2Grant024A04J2172).
文摘Structural optimization of lead compounds is a crucial step in drug discovery.One optimization strategy is to modify the molecular structure of a scaffold to improve both its biological activities and absorption,distribution,metabolism,excretion,and toxicity(ADMET)properties.One of the deep molecular generative model approaches preserves the scaffold while generating drug-like molecules,thereby accelerating the molecular optimization process.Deep molecular diffusion generative models simulate a gradual process that creates novel,chemically feasible molecules from noise.However,the existing models lack direct interatomic constraint features and struggle with capturing long-range dependencies in macromolecules,leading to challenges in modifying the scaffold-based molecular structures,and creates limitations in the stability and diversity of the generated molecules.To address these challenges,we propose a deep molecular diffusion generative model,the three-dimensional(3D)equivariant diffusion-driven molecular generation(3D-EDiffMG)model.The dual strong and weak atomic interaction force-based long-range dependency capturing equivariant encoder(dual-SWLEE)is introduced to encode both the bonding and non-bonding information based on strong and weak atomic interactions.Addi-tionally,a gate multilayer perceptron(gMLP)block with tiny attention is incorporated to explicitly model complex long-sequence feature interactions and long-range dependencies.The experimental results show that 3D-EDiffMG effectively generates unique,novel,stable,and diverse drug-like molecules,highlighting its potential for lead optimization and accelerating drug discovery.
基金supported by the National Natural Science Foundation of China(Grant No.12374238)the Postdoctoral Science Foundation of Shaanxi Province (Grant No.2024BSHSDZZ148)Ministry of Science and Higher Education of Russian Federation (Grant No.FSRZ 2023-0006)。
文摘A singlet diatomic molecule naturally carries doubly degenerate ±Λ states when the projection of the total electronic angular momentum onto the internuclear axis is nonzero. These doubly degenerate states contribute equally in conventional measurements and are thus treated the same in corresponding simulations. In this study, we demonstrate that in resonant excitation by intense laser pulses, the doubly degenerate ±Λ states must be clearly identified. This is exemplified in the X^(1)Σ → A^(1)Π transition of CO molecules. This distinction becomes especially important in the case of circularly polarized radiation. We attribute this phenomenon to the interference of electron-rotational pathways in the strong-field coupled transition with the ±Λ-state of the excited Π state. This research sheds light on the fundamental aspects of intense laser-molecule interactions when extending conventional theories.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFE0134200)the National Natural Science Foundation of China(Grant No.12204214)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.GK202207012)QCYRCXM-2022-241。
文摘Multi-electron and multi-orbital effects play a crucial role in the interaction of strong laser fields with complex molecules.Here,multi-electron effects encompass not only electron-electron Coulomb interactions and exchangecorrelation effects but also the interference between the dynamics of different electron wave packets.
基金financial support from the National Natural Science Foundation of China(Nos.22171094,21925104,92261204,and 22431005)Hubei Provincial Science and Technology Innovation Team Project[2022]The National Key R&D Program of China(No.2022YFB3807700)。
文摘Atomically precise coordination nanoclusters(NCs)constitute a pivotal and rapidly advancing domain in the realms of materials science and chemistry owing to their distinctive crystal structures and exceptional attributes encompassing molecular magnetism[1],photoluminescence[2],and catalysis[3].Organic ligands play a crucial role in effectively shielding these NCs,serving two primary functions:firstly,vital in preventing NC aggregation,particularly for the formation of robust single-crystal structures;secondly,acting as either bridging or peripheral structural components of NCs[4].This characterization of organic-inorganic hybridization offers unique advantages for unraveling the intricate relationships between structure and properties[5].
基金supported by the National Natural Science Foundation of China(Nos.82174010 and 81973512)。
文摘Stroke is the second leading cause of disability and mortality worldwide,imposing a substantial socioeconomic burden on individuals and healthcare systems.Annually,approximately 14 million people experience stroke,with ischemic stroke comprising nearly 85%of cases,of which 10%to 20%involve large vessel occlusions.Currently,recombinant tissue plasminogen activator(tPA)remains the only approved pharmacological intervention.However,its utility is limited due to a narrow therapeutic window and low recanalization rates,making it applicable to only a minority of patients.Therefore,there is an urgent need for novel therapeutic strategies,including pharmacological advancements and combinatory treatments.Small-molecule natural medicines,particularly those derived from traditional Chinese herbs,have demonstrated significant therapeutic potential in ischemic stroke management.These compounds exert multiple neuroprotective effects,such as antioxidation,anti-inflammatory action,and inhibition of apoptosis,all of which are critical in mitigating stroke-induced cerebral damage.This review comprehensively examines the pathophysiology of acute ischemic stroke(AIS)and highlights the recent progress in the development of small-molecule natural medicines as promising therapeutic agents for cerebral ischemic stroke.
基金National Natural Science Foundation of China:Study on the Molecular Mechanism of the Regulation of Crypt Goblet Cell Pyroptosis and Exocytosis to Repair Ulcerative Colitis Mucus Barrier by the Method of Clearing and Opening the Xuanfu from the Perspective of"Xuanfu-Crypt"(No.82305143),and National Natural Science Foundation of China:Exploring the Molecular Mechanism of"Hewei Jiangni Fang"Intervention in Non-erosive Reflux Disease Esophageal Hypersensitivity from the Perspective of Mas-related Gene X2/Stromal Interaction Molecule 1/Cell Adhesion Molecule 1 Pathway Regulation of Mast Cell/Dorsal Root Ganglion Communication based on the"Xinkai-Kujiang"Method(No.82374401)。
文摘OBJECTIVE:To explore if Hewei Jiangni granule(和胃降逆颗粒,HWJNG)could regulate esophageal hypersensitivity via stromal interaction molecule 1(STIM1)/transient receptor potential vanilloid subfamily member 1(TRPV1)pathway.METHODS:Qualitative analysis of HWJNG was analysis by high performance of liquid and gas chromatography.In vivo,animal model of non-erosive reflux disease(NERD)was established by fructose intake and restraint stress.HWJNG and Omeprazole were administered by gavage to the drug intervention group.Reflux and visceral hypersensitivity were analyzed by pathological changes,PH value test,mechanical paw withdrawal threshold,thermal withdrawal latency and mast cells(MCs)degranulation.In vitro,substance P(SP)-induced P815 cells and dorsal root ganglion(DRG)cells were cocultured.Expression in both mice and cells of STIM1,TRPV1,and esophageal visceral hypersensitivity-related gastrointestinal neurochemicals were validated by enzyme linked immunosorbent assays,quantitative realtime polymerase chain reaction(qRT-PCR)and Western blot.Moreover,overexpression and small interfering RNA against STIM1 were utilized to verify of the role of HWJNG in DRG cells.RESULTS:HWJNG significantly suppressed intercellular space widening,injury of mitochondrial,MCs degranulation,mechanical allodynia and heat neuropathic sensory and increased pH value of esophageal mucosa in NERD mice.HWJNG inhibited expression of visceral hypersensitivityrelated gastrointestinal neurochemicals in esophageal mucosa and activated P815 cells,and expression of the STIM1,TRPV1 and related neurotransmitters in DRG and DRG cells.STIM1 siRNA and HWJNG both reduced P815 cells adhesion to DRGs cells and Ca2+flow into the cytoplasmic space of DRG cells.Furthermore,HWJNG could reversed STIM1 overexpression induced upregulation of TRPV1.CONCLUSION:HWJNG suppressed intercellular space widening in NERD mice,stabilized MCs and restored neuronal hyperexcitability by regulating visceral hypersensitivity via STIM1/TRPV1 pathway.
基金supported by NIH grants AG079264(to PHR)and AG071560(to APR)。
文摘The process of neurite outgrowth and branching is a crucial aspect of neuronal development and regeneration.Axons and dendrites,sometimes referred to as neurites,are extensions of a neuron's cellular body that are used to start networks.Here we explored the effects of diethyl(3,4-dihydroxyphenethylamino)(quinolin-4-yl)methylphosphonate(DDQ)on neurite developmental features in HT22 neuronal cells.In this work,we examined the protective effects of DDQ on neuronal processes and synaptic outgrowth in differentiated HT22cells expressing mutant Tau(mTau)cDNA.To investigate DDQ chara cteristics,cell viability,biochemical,molecular,western blotting,and immunocytochemistry were used.Neurite outgrowth is evaluated through the segmentation and measurement of neural processes.These neural processes can be seen and measured with a fluorescence microscope by manually tracing and measuring the length of the neurite growth.These neuronal processes can be observed and quantified with a fluorescent microscope by manually tracing and measuring the length of the neuronal HT22.DDQ-treated mTau-HT22 cells(HT22 cells transfected with cDNA mutant Tau)were seen to display increased levels of synaptophysin,MAP-2,andβ-tubulin.Additionally,we confirmed and noted reduced levels of both total and p-Tau,as well as elevated levels of microtubule-associated protein 2,β-tubulin,synaptophysin,vesicular acetylcholine transporter,and the mitochondrial biogenesis protein-pe roxisome prolife rator-activated receptor-gamma coactivator-1α.In mTa u-expressed HT22 neurons,we observed DDQ enhanced the neurite characteristics and improved neurite development through increased synaptic outgrowth.Our findings conclude that mTa u-HT22(Alzheimer's disease)cells treated with DDQ have functional neurite developmental chara cteristics.The key finding is that,in mTa u-HT22 cells,DDQ preserves neuronal structure and may even enhance nerve development function with mTa u inhibition.
