The thalamic reticular nucleus(TRN)plays a crucial role in regulating sensory encoding,even at the earliest stages of visual processing,as evidenced by numerous studies.Orientation selectivity,a vital neural response,...The thalamic reticular nucleus(TRN)plays a crucial role in regulating sensory encoding,even at the earliest stages of visual processing,as evidenced by numerous studies.Orientation selectivity,a vital neural response,is essential for detecting objects through edge perception.Here,we demonstrate that somatostatin(SOM)-expressing and parvalbumin(PV)-expressing neurons in the TRN project to the dorsal lateral geniculate nucleus and modulate orientation selectivity and the capacity for visual information processing in the primary visual cortex(V1).These findings show that SOM-positive and PV-positive neurons in the TRN are powerful modulators of visual information encoding in V1,revealing a novel role for this thalamic nucleus in influencing visual processing.展开更多
Fundamental physics often confronts complex symbolic problems with few guiding exemplars or established principles.While artificial intelligence(AI)offers promise,its typical need for vast datasets to learn from hinde...Fundamental physics often confronts complex symbolic problems with few guiding exemplars or established principles.While artificial intelligence(AI)offers promise,its typical need for vast datasets to learn from hinders its use in these information-scarce frontiers.We introduce learning at criticality(LaC),a reinforcement learning scheme that tunes large language models(LLMs)to a sharp learning transition,addressing this information scarcity.At this transition,LLMs achieve peak generalization from minimal data,exemplified by 7-digit base-7 addition-a test of nontrivial arithmetic reasoning.To elucidate this peak,we analyze a minimal concept-network model designed to capture the essence of how LLMs might link tokens.Trained on a single exemplar,this model also undergoes a sharp learning transition.This transition exhibits hallmarks of a second-order phase transition,notably power-law distributed solution path lengths.At this critical point,the system maximizes a“critical thinking pattern”crucial for generalization,enabled by the underlying scale-free exploration.This suggests LLMs reach peak performance by operating at criticality,where such explorative dynamics enable the extraction of underlying operational rules.We demonstrate LaC in quantum field theory:an 8B-parameter LLM,tuned to its critical point by LaC using a few exemplars of symbolic Matsubara sums,solves unseen,higher-order problems,significantly outperforming far larger models.LaC thus leverages critical phenomena,a physical principle,to empower AI for complex,data-sparse challenges in fundamental physics.展开更多
The formation and evolution mechanism of fullerenes in the planetary nebula or in the interstellar medium are still not understood.Here,we present the study on the cluster formation and the relative reactivity of full...The formation and evolution mechanism of fullerenes in the planetary nebula or in the interstellar medium are still not understood.Here,we present the study on the cluster formation and the relative reactivity of fullerene cations(from smaller to larger,C44 to C70) with anthracene molecule(C14H10).The experiment is performed in an apparatus that combines a quadrupole ion trap with a time-of-flight mass spectrometer.By using a 355 nm laser beam to irradiate the trapped fullerenes cations(C60+or C70+),smaller fullerene cations C(60-2 n)+, n=1-8 or C(70-2 m)+,m=1-11 are generated,respectively.Then reacting with anthracene molecules,series of fullerene/anthracene cluster cations are newly formed(e.g.,(C14H10)C(60-2 n)+,n=1-8 and(C14H10)C(70-2 m)+,m=1-11),and slight difference of the reactivity within the smaller fullerene cations are observed.Nevertheless,smaller fullerenes show obviously higher reactivity when comparing to fullerene C60+ and C70+.A successive loss of C2 fragments mechanism is suggested to account for the formation of smaller fullerene cations,which then undergo addition reaction with anthracene molecules to form the fullerene-anthracene cluster cations.It is found that the higher laser energy and longer irradiation time are key factors that affect the formation of smaller fullerene cations.This may indicate that in the strong radiation field environment(such as photon-dominated regions) in space,fullerenes are expected to follow the top-down evolution route,and then form small grain dust(e.g.,clusters) through collision reaction with co-existing molecules,here,smaller PAHs.展开更多
Many photocatalytic reactions such as CO2 reduction and N2 fixation are often limited by the activation of some key molecules. Defects in solid materials can robustly introduce coordinately unsaturated sites to serve ...Many photocatalytic reactions such as CO2 reduction and N2 fixation are often limited by the activation of some key molecules. Defects in solid materials can robustly introduce coordinately unsaturated sites to serve as highly active sites for molecular chemisorption and activation. As a result, rational defect engineering has endowed a versatile approach to further develop photocatalytic applications beyond water splitting. The subtly designed defects in photocatalysts can play critical and decisive roles in molecular activation as proven in recent years. The defects cannot only serve as active sites for molecular chemisorption, but also spatially supply channels for energy and electron transfer. In this review, we aim to summarize the diversiform photocatalytic applications using defects as active sites, including but not limited to CO2 reduction, O2 activation,H2O dissociation, N2 fixation as well as activation of other molecules. In particular, we emphatically outline how the parameters of defects (e.g.,concentration,location,geometric and electronic structures) can serve as the knobs for maneuvering molecular adsorption and activation as well as altering subsequent reaction pathway. Moreover, we underline the remaining challenges at the current stage and the potential development in the future.It is anticipated that this review consolidates the in-depth understanding towards the structure-activity relationship between defects and related reactions.展开更多
BiTe is a potentially attractive candidate for thermoelectric applications because it is the structural analogue of the state-of-the-art thermoelectric material,bismuth telluride(Bi_(2)Te_(3)). However, BiTe has attra...BiTe is a potentially attractive candidate for thermoelectric applications because it is the structural analogue of the state-of-the-art thermoelectric material,bismuth telluride(Bi_(2)Te_(3)). However, BiTe has attracted little attention due to its small band gap and high electron concentration. In this study, remarkable increase in thermoelectric performance in the n-type Bi_(1-x)Sb_(x)Te compounds through tuning the carrier concentration with chemical doping is shown. The Seebeck coefficient of Bi_(1-x)Sb_(x)Te increases remarkably while the electronic thermal conductivity decreases gradually as Sb content is increased, leading to enhanced thermoelectric figure of merit(ZT). Moreover, the simultaneous optimization of the electrical and thermal transport properties leads the peak temperature of the figure of merit to shift toward lower temperature with Sb content increasing in Bi_(1-x)Sb_(x)Te, thus making Bi_(1-x)Sb_(x)Te a potential alternative to bismuth telluride for near-room-temperature thermoelectric applications. In addition, the presence of multiple low-frequency optical phonons and their coupling with the long-wavelength heat carrying acoustic phonons in all the Bi_(1-x)Sb_(x)Te investigated are revealed based on the combined Debye-Einstein model. The present results provide the underlying mechanism connecting thermoelectric performance and lattice dynamics in Bi_(1-x)Sb_(x)Te compounds.展开更多
The effect of the modification of an alumina support with chloride on the structure and the catalytic performance of Ag/Al_(2)O_(3)catalysts(SA)was investigated for the selective catalytic reduction(SCR)of NO using C_...The effect of the modification of an alumina support with chloride on the structure and the catalytic performance of Ag/Al_(2)O_(3)catalysts(SA)was investigated for the selective catalytic reduction(SCR)of NO using C_(3)H_(6)or H_(2)/C_(3)H_(6)as reductants.The Ag/Al_(2)O_(3)catalyst and Cl^(–)-modified Ag/Al_(2)O_(3)catalysts(SA-Cl)were prepared by a conventional impregnation method and characterized by X-ray diffraction,Brunauer-Emmett-Teller isotherm analysis,electron probe microanalysis,transmission electron microscopy,UV-Vis diffuse reflectance spectroscopy,X-ray photoelectron spectroscopy,and hydrogen temperature-programmed reduction.The catalytic activities in the C3H6-SCR and H_(2)/C3H6-SCR reactions were evaluated,and the reaction mechanism was studied using in situ diffuse reflectance infrared Fourier transform spectroscopy and synchrotron vacuum ultraviolet photoionization mass spectroscopy(SVUV-PIMS).We found that Cl^(-)modification of the alumina-supported Ag/Al_(2)O_(3)catalysts facilitated the formation of oxidized silver species(Ag_(n)^(ᵟ+))that catalyze the moderate-temperature oxidation of hydrocarbons into partial oxidation products(mainly acetate species)capable of participating in the SCR reaction.The low-temperature promoting effect of H_(2)on the C3H6-SCR("hydrogen effect")was found to originate from the enhanced decomposition of strongly adsorbed nitrates on the catalyst surface and the conversion of these adsorbed species to–NCO and–CN species.This"H_(2)effect"occurs in the presence of Ag_(n)^(ᵟ+)species rather than the metallic Ag^(0)species.A gaseous intermediate,acrylonitrile(CH_(2)CHCN),was also identified in the H_(2)/C3H6-SCR reaction using SVUV-PIMS.These findings provide novel insights in the structure-activity relationship and reaction mechanisms of the SA-catalyzed HC-SCR reaction of NO.展开更多
Au nanostructures were prepared on uniform Cu2O octahedra and rhombic dodecahedra via the galvanic replacement reaction between HAuCl 4 and Cu2O. The compositions and structures were studied by Scanning Electron Micro...Au nanostructures were prepared on uniform Cu2O octahedra and rhombic dodecahedra via the galvanic replacement reaction between HAuCl 4 and Cu2O. The compositions and structures were studied by Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), High-Resolution Transmission Electron Microscope (HRTEM), X-Ray Diffraction (XRD), X-Ray Absorption Spectroscopy (XAS), X-ray Photoelectron Spectroscopy (XPS) and in-situ DRIFTS spectroscopy of CO adsorption. Different from the formation of Au-Cu alloys on Cu2O cubes by the galvanic replacement reaction (ChemNanoMat 2 (2016) 861-865), metallic Au particles and positively-charged Au clusters form on Cu2O octahedra and rhombic dodecahedra at very small Au loadings and only metallic Au particles form at large Au loadings. Metallic Au particles on Cu2O octahedra and rhombic dodecahedra are more active in catalyzing the liquid phase aerobic oxidation reaction of benzyl alcohol than positively-charged Au clusters. These results demonstrate an obvious morphology effect of Cu2O nanocrystals on the liquid-solid interfacial reactions and prove oxide morphology as an effective strategy to tune the surface reactivity and catalytic performance. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
Understanding of the oxygen reduction reaction(ORR)mechanism for single atom catalysts is pivotal for the rational design of non-precious metal cathode materials and the commercialization of fuel cells.Herein,a series...Understanding of the oxygen reduction reaction(ORR)mechanism for single atom catalysts is pivotal for the rational design of non-precious metal cathode materials and the commercialization of fuel cells.Herein,a series of non-precious metal electrocatalysts based on nitrogen-doped bimetallic(Fe and Co)carbide were modeled by density functional theory calculations to predict the corresponding reaction pathways.The study elucidated prior oxygen adsorption on the Fe atom in the dual site and the modifier role of Co atoms to tune the electronic structures of Fe.The reaction activity was highly correlated with the bimetallic center and the coordination environment of the adjacent nitrogen.Interestingly,the preadsorption of*OH resulted in the apparent change of metal atoms'electronic states with the d-band center shifting toward the Fermi level,thereby boosting reaction activity.The result should help promote the fundamental understanding of active sites in ORR catalysts and provide an effective approach to the design of highly efficient ORR catalysts on an atomic scale.展开更多
Biorefinery is pivotal to the sustainability of modern chemical industry.However,since biomass is oxygen-enriched,new and green chemical strategies are required for expanding the biomass derived chemical space.In this...Biorefinery is pivotal to the sustainability of modern chemical industry.However,since biomass is oxygen-enriched,new and green chemical strategies are required for expanding the biomass derived chemical space.In this work,synthesis of natural products dihydrocapsaicin and dihydrocapsiate was achieved exclusively from lignocellulosic platform chemicals.Natural products dihydrocapsaicin and dihydrocapsiate were synthesized exclusively from lignocellulosic platform chemicals,using furfural(from hemicellulose)and methyl isopropyl ketone(from cellulose)through aldol condensation-hydrolysis-hydrodeoxygenation to synthesize 8-methylnonanoic acid and then combined with vanillin derivates(from lignin).This synthesis demonstrates the feasibility of constructing natural products entirely from renewable biomass platform through green processes.The utilization of inherent functional groups of biomass demonstrates their potential to open up chemical space.展开更多
The undesirable shuttle effect and sluggish redox kinetics of polysulfides seriously result in low sulfur utilization and poor capacity retention.Here,an integrated strategy is proposed by rational designing multifunc...The undesirable shuttle effect and sluggish redox kinetics of polysulfides seriously result in low sulfur utilization and poor capacity retention.Here,an integrated strategy is proposed by rational designing multifunctional architecture to manipulate the redox kinetics of polysulfides,specifically,by employing iron atoms(Fe-As)and iron-species nanoparticles(Fe-NPs)co-embedded nitrogen-doped carbon nanotube(Fe-NCNT)as catalyst and host for sulfur.The synergistic cooperation of Fe-As and Fe-NPs provides efficient active sites to facilitate the diffusion,strengthen the affinities,and promote the conversion reactions for polysulfides.Furthermore,the NCNT not only offers practical Li+transport pathways but also immobilize the polysulfides effectively.Benefiting from these merits,the Fe-NCNT/S electrodes exhibit high initial specific capacity of 1502.6 mAh/g at 0.1 C,outstanding rate performance(830 mAh/g at 2 C),and good cycling performance(597.8 mAh/g after 500 cycles with an ultralow capacity fading rate of 0.069%per cycle).This work features the distinct interaction of iron atom-nanoparticles on facilitating immobilization-diffusion-transformation process of polysulfides,and it also expected to pave the way for the application in practical Li-S batteries.展开更多
By using satellites, ultra-long-distance quantum communication and tests of quantum foundations could be achieved at a global scale. The Quantum Experiment Science Satellite(QUESS) in China, also called Micius, one of...By using satellites, ultra-long-distance quantum communication and tests of quantum foundations could be achieved at a global scale. The Quantum Experiment Science Satellite(QUESS) in China, also called Micius, one of the scientific satellite programs in the Strategic Priority Program on space science, the Chinese Academy of Sciences, was launched on 16 August 2016. There are totally 4 scientific payloads. We give a brief overview of the quantum experiment science satellite project and present most recent science results. The main scientific goal of the quantum experiment science satellite was achieved in 2017. Here, we introduce the latest achievements in satellite-based quantum communication and large-scale tests of quantum foundations obtained by Micius.展开更多
D-peptides are recognized as a new class of synthetic chemical drugs and they possess many interesting advantages such as high enzymatic stability,improved oral bioavailability,as well as high binding affinity and spe...D-peptides are recognized as a new class of synthetic chemical drugs and they possess many interesting advantages such as high enzymatic stability,improved oral bioavailability,as well as high binding affinity and specificity.Recently,D-peptide drugs have been attracting increasing attention in both academic and industrial researches over recent years.One D-peptide etelcalcetide has even entered the market that targets the calcium(Ca2+)-sensing receptor(CaSR) to fight secondary hyperparathyroidism.Effective discovery and optimization of D-peptide ligands that can bind to various disease-related targets with high specificity and potency is of great importance for the development of D-peptide drugs.This review surveys the recent method development in this area especially the chemical protein synthesis-assisted high-throughput screening strategies for D-peptide ligands and their application in drug discovery.展开更多
KSSOLV(Kohn-Sham Solver)is a MATLAB(Matrix Laboratory)toolbox for solving the Kohn-Sham density functional theory(KS-DFT)with the plane-wave basis set.In the KS-DFT calculations,the most expensive part is commonly the...KSSOLV(Kohn-Sham Solver)is a MATLAB(Matrix Laboratory)toolbox for solving the Kohn-Sham density functional theory(KS-DFT)with the plane-wave basis set.In the KS-DFT calculations,the most expensive part is commonly the diagonalization of Kohn-Sham Hamiltonian in the self-consistent field(SCF)scheme.To enable a personal computer to perform medium-sized KS-DFT calculations that contain hundreds of atoms,we present a hybrid CPU-GPU implementation to accelerate the iterative diagonalization algorithms implemented in KSSOLV by using the MATLAB built-in Parallel Computing Toolbox.We compare the performance of KSSOLV-GPU on three types of GPU,including RTX3090,V100,and A100,with conventional CPU implementation of KSSOLV respectively and numerical results demonstrate that hybrid CPU-GPU implementation can achieve a speedup of about 10 times compared with sequential CPU calculations for bulk silicon systems containing up to 128 atoms.展开更多
Zinc phthalocyanines(ZnPc)are widely recognized as efficient triplet photosensitizers in photodynamic therapy and photocatalysis,owing to their intense absorption in the visible range and long triplet-state lifetimes....Zinc phthalocyanines(ZnPc)are widely recognized as efficient triplet photosensitizers in photodynamic therapy and photocatalysis,owing to their intense absorption in the visible range and long triplet-state lifetimes.However,their application in triplet-triplet annihilation(TTA)upconversion is lacking to date.In this study,we synthesized a new ZnPc photosensitizer,4I-ZnPc,and composed a TTA upconversion system using rubrene as the energy acceptor.Upon photoexcitation at 663 nm,yellow fluorescence from rubrene was observed in deoxygenated dichloromethane,demonstrating TTA upconversion with an anti-Stokes shift of 0.331 eV and a quantum yield of 1.82%(out of the 50%maximum).Using nanosecond transient absorption spectroscopy,we determined the triplet lifetime of 4I-ZnPc,the triplet-triplet energy transfer efficiency,and the fluorescence quantum yield.These measurements provide critical insights into the photophysical processes governing the TTA upconversion system.Our results highlight the potential advantages and limitations of ZnPc as a triplet photosensitizer for TTA upconversion.展开更多
ZnO-based catalysts have been widely used in hydrogenation reactions,but less attention has been paid to the electrocatalytic hydrogenation process on ZnO electrodes.In this work,the preparation of hydrogen species an...ZnO-based catalysts have been widely used in hydrogenation reactions,but less attention has been paid to the electrocatalytic hydrogenation process on ZnO electrodes.In this work,the preparation of hydrogen species and the associ-ated reduction properties under electrochemi-cal processes in aqueous solutions have been in-vestigated on ZnO and Au/ZnO electrodes.The measurements of cyclic voltammetry(CV),X-ray diffraction,and electron paramagnetic resonance(EPR)confirm the formation of hydro-gen species on the interstitial sites(Hi)or on the oxygen vacancy sites(H_(O)).The hydrogena-tion reaction of p-nitrophenol(pNP)at 40μmol/L occurs on both ZnO and Au/ZnO elec-trodes,and the hydrogenation reduction performance of Au/ZnO electrode is better than that of ZnO electrode.CVs show H_(O)species is much more reactive with pNP than Hi species.Compared with the ZnO electrode,the presence of Au on ZnO promotes the formation of H_(O)species and improves the electro-reduction performance to pNP.These results help us to un-derstand the reaction processes related to the electrochemical hydrogenation on ZnO and Au/ZnO surfaces and shed new light on the design of new catalytic hydrogenation systems.展开更多
Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO_(2)hydrogenation.Combining density functional theory calculations and microkineti...Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO_(2)hydrogenation.Combining density functional theory calculations and microkinetic analysis,we proposed that graphene-supported isolated Pt atoms(Pt1/graphene)and Pt_(2)dimers(Pt_(2)/graphene)exhibited distinct selectivity in CO_(2)hydrogenation.Pt_(1)/graphene facilitated the conversion of CO_(2)into formic acid,whereas Pt_(2)/graphene favored methanol generation.The variation in product selectivity arose from the synergistic interaction of Pt_(2)dimers,which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from*COOH intermediates to*C(OH)_(2)intermediates,altering the reaction pathways compared to isolated Pt atoms.Additionally,an analysis of the catalytic activities of three Pt_(1)/graphene and three Pt_(2)/graphene structures revealed that the turnover frequencies for formic acid generation on Pt_(1ii)/graphene and methanol generation on Pt_(2i)/graphene were as high as 744.48 h-1and 789.48 h^(-1),respectively.These values rivaled or even surpassed those previously reported in the literature under identical conditions.This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO_(2)hydrogenation.展开更多
Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional th...Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.展开更多
As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit v...As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit voltage deficit de-rived from non-radiative recombination,especial-ly at the buried interface that are often overlooked.Herein,we combined cationic and anion passiva-tion strategies via ammonium tetra-n-butyl tetrafluoroborate(TBABF_(4))pre-treating the buried interface.Theoretical calculation predicts that the tetrabutylammonium(TBA^(+))organic cations and(tetrafluoroborate)BF_(4)^(−)anions can easily interact with charged interfacial defect.Characterizations further confirm the enhance-ment of carrier transport performance and decrease in defect density upon TBABF4 pre-treat-ment.Consequently,a power conversion efficiency of 21.35%with an ultrahigh filling factor of 84.12%is obtained for 1.68 eV-WBG inverted PSCs.In addition,the device with TBABF4 pre-treatment demonstrates excellent shelf,thermal,and operational stability.展开更多
Quantum link models(QLMs)serve as experimentally accessible platforms for studying lattice gauge theories with finite-dimensional Hilbert spaces.In this work,we investigate information scrambling in the partially conf...Quantum link models(QLMs)serve as experimentally accessible platforms for studying lattice gauge theories with finite-dimensional Hilbert spaces.In this work,we investigate information scrambling in the partially confined phase of a spin-1 quantum link model by calculating the dynamics of out-of-time-ordered correlators(OTOCs)and entanglement entropy.We observe that,in the partially confined phase,information scrambling exhibits significant asymmetry,manifested as the unidirectional propagation of both OTOCs and entanglement entropy.This phenomenon stands in stark contrast to the isotropic spreading observed in the deconfined phase and the localization characteristic of the confined phase.Furthermore,the simultaneous occurrence of the unidirectional propagation of both OTOCs and entanglement entropy,together with the q-induced asymmetric excitation propagation,reveals a direct connection between information scrambling and charge confinement.展开更多
On-surface synthesis of semiconducting graphdiyne nanowires usually suffer severe side reactions owing to the high reactivity of the butadiynylene units at noble metal surfaces,limiting the production of isolated nano...On-surface synthesis of semiconducting graphdiyne nanowires usually suffer severe side reactions owing to the high reactivity of the butadiynylene units at noble metal surfaces,limiting the production of isolated nanowires. In this work, we report the high-yield synthesis of branchless graphdiyne nanowires [-C≡C-Ph2-C≡C-]nvia on-surface Ullmann coupling of 1,4-bis（4-bromophenyl）-1,3-butadiyne molecules with chemical vapor deposition method.Non-contact atomic force microscopy with single-bond resolution reveals that single gold adatoms act as effective protecting groups for butadiynylene units by forming Au-π ligand bonds, preventing unwanted branched coupling reactions and enabling the synthesis of ultralong isolated graphdiyne nanowires. This study will stimulate further investigation on the role of various surface adatoms in protecting on-surface reactions.展开更多
基金supported by the Young Scientists Fund of the National Natural Science Foundation of China(32200789)the National Natural Science Foundation of China(32070990).
文摘The thalamic reticular nucleus(TRN)plays a crucial role in regulating sensory encoding,even at the earliest stages of visual processing,as evidenced by numerous studies.Orientation selectivity,a vital neural response,is essential for detecting objects through edge perception.Here,we demonstrate that somatostatin(SOM)-expressing and parvalbumin(PV)-expressing neurons in the TRN project to the dorsal lateral geniculate nucleus and modulate orientation selectivity and the capacity for visual information processing in the primary visual cortex(V1).These findings show that SOM-positive and PV-positive neurons in the TRN are powerful modulators of visual information encoding in V1,revealing a novel role for this thalamic nucleus in influencing visual processing.
基金supported by the National Key Research and Development Program of China(Grant No.2024YFA1408604 for K.C.and X.C.)the National Natural Science Foundation of China(Grant Nos.12047503,12447103 for K.C.and X.C.,12325501 for P.Z.,and 12275263 for Y.D.and S.H.)+1 种基金the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0301900 for Y.D.and S.H.)the Natural Science Foundation of Fujian Province of China(Grant No.2023J02032 for Y.D.and S.H.)。
文摘Fundamental physics often confronts complex symbolic problems with few guiding exemplars or established principles.While artificial intelligence(AI)offers promise,its typical need for vast datasets to learn from hinders its use in these information-scarce frontiers.We introduce learning at criticality(LaC),a reinforcement learning scheme that tunes large language models(LLMs)to a sharp learning transition,addressing this information scarcity.At this transition,LLMs achieve peak generalization from minimal data,exemplified by 7-digit base-7 addition-a test of nontrivial arithmetic reasoning.To elucidate this peak,we analyze a minimal concept-network model designed to capture the essence of how LLMs might link tokens.Trained on a single exemplar,this model also undergoes a sharp learning transition.This transition exhibits hallmarks of a second-order phase transition,notably power-law distributed solution path lengths.At this critical point,the system maximizes a“critical thinking pattern”crucial for generalization,enabled by the underlying scale-free exploration.This suggests LLMs reach peak performance by operating at criticality,where such explorative dynamics enable the extraction of underlying operational rules.We demonstrate LaC in quantum field theory:an 8B-parameter LLM,tuned to its critical point by LaC using a few exemplars of symbolic Matsubara sums,solves unseen,higher-order problems,significantly outperforming far larger models.LaC thus leverages critical phenomena,a physical principle,to empower AI for complex,data-sparse challenges in fundamental physics.
基金supported by the Fundamental Research Funds for the Central Universitiesthe National Natural Science Foundation of China(NSFC,Grant No.11743004)。
文摘The formation and evolution mechanism of fullerenes in the planetary nebula or in the interstellar medium are still not understood.Here,we present the study on the cluster formation and the relative reactivity of fullerene cations(from smaller to larger,C44 to C70) with anthracene molecule(C14H10).The experiment is performed in an apparatus that combines a quadrupole ion trap with a time-of-flight mass spectrometer.By using a 355 nm laser beam to irradiate the trapped fullerenes cations(C60+or C70+),smaller fullerene cations C(60-2 n)+, n=1-8 or C(70-2 m)+,m=1-11 are generated,respectively.Then reacting with anthracene molecules,series of fullerene/anthracene cluster cations are newly formed(e.g.,(C14H10)C(60-2 n)+,n=1-8 and(C14H10)C(70-2 m)+,m=1-11),and slight difference of the reactivity within the smaller fullerene cations are observed.Nevertheless,smaller fullerenes show obviously higher reactivity when comparing to fullerene C60+ and C70+.A successive loss of C2 fragments mechanism is suggested to account for the formation of smaller fullerene cations,which then undergo addition reaction with anthracene molecules to form the fullerene-anthracene cluster cations.It is found that the higher laser energy and longer irradiation time are key factors that affect the formation of smaller fullerene cations.This may indicate that in the strong radiation field environment(such as photon-dominated regions) in space,fullerenes are expected to follow the top-down evolution route,and then form small grain dust(e.g.,clusters) through collision reaction with co-existing molecules,here,smaller PAHs.
基金financially supported in part by the National Key R&D Program of China (2017YFA0207301)NSFC (21725102, 21471141, U1532135, 21703220)+2 种基金CAS Key Research Program of Frontier Sciences (QYZDB-SSW-SLH018)CAS Interdisciplinary Innovation Team, Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology (2016FXCX003)Anhui Provincial Natural Science Foundation (1708085QB26)
文摘Many photocatalytic reactions such as CO2 reduction and N2 fixation are often limited by the activation of some key molecules. Defects in solid materials can robustly introduce coordinately unsaturated sites to serve as highly active sites for molecular chemisorption and activation. As a result, rational defect engineering has endowed a versatile approach to further develop photocatalytic applications beyond water splitting. The subtly designed defects in photocatalysts can play critical and decisive roles in molecular activation as proven in recent years. The defects cannot only serve as active sites for molecular chemisorption, but also spatially supply channels for energy and electron transfer. In this review, we aim to summarize the diversiform photocatalytic applications using defects as active sites, including but not limited to CO2 reduction, O2 activation,H2O dissociation, N2 fixation as well as activation of other molecules. In particular, we emphatically outline how the parameters of defects (e.g.,concentration,location,geometric and electronic structures) can serve as the knobs for maneuvering molecular adsorption and activation as well as altering subsequent reaction pathway. Moreover, we underline the remaining challenges at the current stage and the potential development in the future.It is anticipated that this review consolidates the in-depth understanding towards the structure-activity relationship between defects and related reactions.
基金financially supported by the National Key R&D Program of China(Nos.2018YFB0703602 and 2017YFA0303500)the National Natural Science Foundation of China(Nos.21622107 and U1832142)+2 种基金the Youth Innovation Promotion Association CAS(No.2016392)the Fundamental Research Funds for the Central University(No.WK2340000094)the Key Research Program of Frontier Sciences(No.QYZDY-SSW-SLH011)。
文摘BiTe is a potentially attractive candidate for thermoelectric applications because it is the structural analogue of the state-of-the-art thermoelectric material,bismuth telluride(Bi_(2)Te_(3)). However, BiTe has attracted little attention due to its small band gap and high electron concentration. In this study, remarkable increase in thermoelectric performance in the n-type Bi_(1-x)Sb_(x)Te compounds through tuning the carrier concentration with chemical doping is shown. The Seebeck coefficient of Bi_(1-x)Sb_(x)Te increases remarkably while the electronic thermal conductivity decreases gradually as Sb content is increased, leading to enhanced thermoelectric figure of merit(ZT). Moreover, the simultaneous optimization of the electrical and thermal transport properties leads the peak temperature of the figure of merit to shift toward lower temperature with Sb content increasing in Bi_(1-x)Sb_(x)Te, thus making Bi_(1-x)Sb_(x)Te a potential alternative to bismuth telluride for near-room-temperature thermoelectric applications. In addition, the presence of multiple low-frequency optical phonons and their coupling with the long-wavelength heat carrying acoustic phonons in all the Bi_(1-x)Sb_(x)Te investigated are revealed based on the combined Debye-Einstein model. The present results provide the underlying mechanism connecting thermoelectric performance and lattice dynamics in Bi_(1-x)Sb_(x)Te compounds.
文摘The effect of the modification of an alumina support with chloride on the structure and the catalytic performance of Ag/Al_(2)O_(3)catalysts(SA)was investigated for the selective catalytic reduction(SCR)of NO using C_(3)H_(6)or H_(2)/C_(3)H_(6)as reductants.The Ag/Al_(2)O_(3)catalyst and Cl^(–)-modified Ag/Al_(2)O_(3)catalysts(SA-Cl)were prepared by a conventional impregnation method and characterized by X-ray diffraction,Brunauer-Emmett-Teller isotherm analysis,electron probe microanalysis,transmission electron microscopy,UV-Vis diffuse reflectance spectroscopy,X-ray photoelectron spectroscopy,and hydrogen temperature-programmed reduction.The catalytic activities in the C3H6-SCR and H_(2)/C3H6-SCR reactions were evaluated,and the reaction mechanism was studied using in situ diffuse reflectance infrared Fourier transform spectroscopy and synchrotron vacuum ultraviolet photoionization mass spectroscopy(SVUV-PIMS).We found that Cl^(-)modification of the alumina-supported Ag/Al_(2)O_(3)catalysts facilitated the formation of oxidized silver species(Ag_(n)^(ᵟ+))that catalyze the moderate-temperature oxidation of hydrocarbons into partial oxidation products(mainly acetate species)capable of participating in the SCR reaction.The low-temperature promoting effect of H_(2)on the C3H6-SCR("hydrogen effect")was found to originate from the enhanced decomposition of strongly adsorbed nitrates on the catalyst surface and the conversion of these adsorbed species to–NCO and–CN species.This"H_(2)effect"occurs in the presence of Ag_(n)^(ᵟ+)species rather than the metallic Ag^(0)species.A gaseous intermediate,acrylonitrile(CH_(2)CHCN),was also identified in the H_(2)/C3H6-SCR reaction using SVUV-PIMS.These findings provide novel insights in the structure-activity relationship and reaction mechanisms of the SA-catalyzed HC-SCR reaction of NO.
基金supported by the National Basic Research Program of China(2013CB933104)the National Natural Science Foundation of China(21525313,21173204,21373192,U1332113)+1 种基金MOE Fundamental Research Funds for the Central Universities(WK2060030017)Collaborative Innovation Center of Suzhou Nano Science and Technology
文摘Au nanostructures were prepared on uniform Cu2O octahedra and rhombic dodecahedra via the galvanic replacement reaction between HAuCl 4 and Cu2O. The compositions and structures were studied by Scanning Electron Microscope (SEM), Transmission Electron Microscope (TEM), High-Resolution Transmission Electron Microscope (HRTEM), X-Ray Diffraction (XRD), X-Ray Absorption Spectroscopy (XAS), X-ray Photoelectron Spectroscopy (XPS) and in-situ DRIFTS spectroscopy of CO adsorption. Different from the formation of Au-Cu alloys on Cu2O cubes by the galvanic replacement reaction (ChemNanoMat 2 (2016) 861-865), metallic Au particles and positively-charged Au clusters form on Cu2O octahedra and rhombic dodecahedra at very small Au loadings and only metallic Au particles form at large Au loadings. Metallic Au particles on Cu2O octahedra and rhombic dodecahedra are more active in catalyzing the liquid phase aerobic oxidation reaction of benzyl alcohol than positively-charged Au clusters. These results demonstrate an obvious morphology effect of Cu2O nanocrystals on the liquid-solid interfacial reactions and prove oxide morphology as an effective strategy to tune the surface reactivity and catalytic performance. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金the Joint Fund of the National Natural Science Foundation of China(U1732267).
文摘Understanding of the oxygen reduction reaction(ORR)mechanism for single atom catalysts is pivotal for the rational design of non-precious metal cathode materials and the commercialization of fuel cells.Herein,a series of non-precious metal electrocatalysts based on nitrogen-doped bimetallic(Fe and Co)carbide were modeled by density functional theory calculations to predict the corresponding reaction pathways.The study elucidated prior oxygen adsorption on the Fe atom in the dual site and the modifier role of Co atoms to tune the electronic structures of Fe.The reaction activity was highly correlated with the bimetallic center and the coordination environment of the adjacent nitrogen.Interestingly,the preadsorption of*OH resulted in the apparent change of metal atoms'electronic states with the d-band center shifting toward the Fermi level,thereby boosting reaction activity.The result should help promote the fundamental understanding of active sites in ORR catalysts and provide an effective approach to the design of highly efficient ORR catalysts on an atomic scale.
基金supported by the National Natural Science Foundation of China(21875239)the Fundamental Research Funds for the Central Universities(WK3530000004)。
文摘Biorefinery is pivotal to the sustainability of modern chemical industry.However,since biomass is oxygen-enriched,new and green chemical strategies are required for expanding the biomass derived chemical space.In this work,synthesis of natural products dihydrocapsaicin and dihydrocapsiate was achieved exclusively from lignocellulosic platform chemicals.Natural products dihydrocapsaicin and dihydrocapsiate were synthesized exclusively from lignocellulosic platform chemicals,using furfural(from hemicellulose)and methyl isopropyl ketone(from cellulose)through aldol condensation-hydrolysis-hydrodeoxygenation to synthesize 8-methylnonanoic acid and then combined with vanillin derivates(from lignin).This synthesis demonstrates the feasibility of constructing natural products entirely from renewable biomass platform through green processes.The utilization of inherent functional groups of biomass demonstrates their potential to open up chemical space.
基金supported by the Natural Science Foundation of China(Nos.22125902,U2032202,21975243 and 21825302)the National Program for Support of Topnotch Young Professionals,the Fundamental Research Funds for the Central Universities(No.WK2030020032)+1 种基金the DNL cooperation Fund,CAS(No.DNL202020)the Anhui Science Fund for Distinguished Young Scholars(No.2208085J15).
文摘The undesirable shuttle effect and sluggish redox kinetics of polysulfides seriously result in low sulfur utilization and poor capacity retention.Here,an integrated strategy is proposed by rational designing multifunctional architecture to manipulate the redox kinetics of polysulfides,specifically,by employing iron atoms(Fe-As)and iron-species nanoparticles(Fe-NPs)co-embedded nitrogen-doped carbon nanotube(Fe-NCNT)as catalyst and host for sulfur.The synergistic cooperation of Fe-As and Fe-NPs provides efficient active sites to facilitate the diffusion,strengthen the affinities,and promote the conversion reactions for polysulfides.Furthermore,the NCNT not only offers practical Li+transport pathways but also immobilize the polysulfides effectively.Benefiting from these merits,the Fe-NCNT/S electrodes exhibit high initial specific capacity of 1502.6 mAh/g at 0.1 C,outstanding rate performance(830 mAh/g at 2 C),and good cycling performance(597.8 mAh/g after 500 cycles with an ultralow capacity fading rate of 0.069%per cycle).This work features the distinct interaction of iron atom-nanoparticles on facilitating immobilization-diffusion-transformation process of polysulfides,and it also expected to pave the way for the application in practical Li-S batteries.
文摘By using satellites, ultra-long-distance quantum communication and tests of quantum foundations could be achieved at a global scale. The Quantum Experiment Science Satellite(QUESS) in China, also called Micius, one of the scientific satellite programs in the Strategic Priority Program on space science, the Chinese Academy of Sciences, was launched on 16 August 2016. There are totally 4 scientific payloads. We give a brief overview of the quantum experiment science satellite project and present most recent science results. The main scientific goal of the quantum experiment science satellite was achieved in 2017. Here, we introduce the latest achievements in satellite-based quantum communication and large-scale tests of quantum foundations obtained by Micius.
基金supported by the National Key R&D Program of China(No.2019YFA0706902)National Natural Science Foundation of China(Nos.U1732161 and 91753120)Science and Technological Fund of Anhui Province for Outstanding Youth(No.1808085J04)。
文摘D-peptides are recognized as a new class of synthetic chemical drugs and they possess many interesting advantages such as high enzymatic stability,improved oral bioavailability,as well as high binding affinity and specificity.Recently,D-peptide drugs have been attracting increasing attention in both academic and industrial researches over recent years.One D-peptide etelcalcetide has even entered the market that targets the calcium(Ca2+)-sensing receptor(CaSR) to fight secondary hyperparathyroidism.Effective discovery and optimization of D-peptide ligands that can bind to various disease-related targets with high specificity and potency is of great importance for the development of D-peptide drugs.This review surveys the recent method development in this area especially the chemical protein synthesis-assisted high-throughput screening strategies for D-peptide ligands and their application in drug discovery.
基金supported by the National Natural Science Foundation of China (No.21688102,No.21803066,and No.22003061)the Chinese Academy of Sciences Pioneer Hundred Talents Program (KJ2340000031,KJ2340007002)+7 种基金the National Key Research and Development Program of China(2016YFA0200604)the Anhui Initiative in Quantum Information Technologies (AHY090400)the Strategic Priority Research of Chinese Academy of Sciences(XDC01040100)CAS Project for Young Scientists in Basic Research (YSBR-005)the Fundamental Research Funds for the Central Universities (WK2340000091,WK2060000018)the Hefei National Laboratory for Physical Sciences at the Microscale (SK2340002001)the Research Start-Up Grants (KY2340000094)the Academic Leading Talents Training Program(KY2340000103) from University of Science and Technology of China
文摘KSSOLV(Kohn-Sham Solver)is a MATLAB(Matrix Laboratory)toolbox for solving the Kohn-Sham density functional theory(KS-DFT)with the plane-wave basis set.In the KS-DFT calculations,the most expensive part is commonly the diagonalization of Kohn-Sham Hamiltonian in the self-consistent field(SCF)scheme.To enable a personal computer to perform medium-sized KS-DFT calculations that contain hundreds of atoms,we present a hybrid CPU-GPU implementation to accelerate the iterative diagonalization algorithms implemented in KSSOLV by using the MATLAB built-in Parallel Computing Toolbox.We compare the performance of KSSOLV-GPU on three types of GPU,including RTX3090,V100,and A100,with conventional CPU implementation of KSSOLV respectively and numerical results demonstrate that hybrid CPU-GPU implementation can achieve a speedup of about 10 times compared with sequential CPU calculations for bulk silicon systems containing up to 128 atoms.
基金supported by the National Natural Science Foundation of China(Nos.22473104 and 22403086)support of the China Postdoctoral Science Foundation(No.2023M733378).
文摘Zinc phthalocyanines(ZnPc)are widely recognized as efficient triplet photosensitizers in photodynamic therapy and photocatalysis,owing to their intense absorption in the visible range and long triplet-state lifetimes.However,their application in triplet-triplet annihilation(TTA)upconversion is lacking to date.In this study,we synthesized a new ZnPc photosensitizer,4I-ZnPc,and composed a TTA upconversion system using rubrene as the energy acceptor.Upon photoexcitation at 663 nm,yellow fluorescence from rubrene was observed in deoxygenated dichloromethane,demonstrating TTA upconversion with an anti-Stokes shift of 0.331 eV and a quantum yield of 1.82%(out of the 50%maximum).Using nanosecond transient absorption spectroscopy,we determined the triplet lifetime of 4I-ZnPc,the triplet-triplet energy transfer efficiency,and the fluorescence quantum yield.These measurements provide critical insights into the photophysical processes governing the TTA upconversion system.Our results highlight the potential advantages and limitations of ZnPc as a triplet photosensitizer for TTA upconversion.
基金supported by the National Key Re-search and Development Program of China(No.2021YFA1500403)the National Natural Science Foundation of China(No.21773047 and No.U1832180)partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication.
文摘ZnO-based catalysts have been widely used in hydrogenation reactions,but less attention has been paid to the electrocatalytic hydrogenation process on ZnO electrodes.In this work,the preparation of hydrogen species and the associ-ated reduction properties under electrochemi-cal processes in aqueous solutions have been in-vestigated on ZnO and Au/ZnO electrodes.The measurements of cyclic voltammetry(CV),X-ray diffraction,and electron paramagnetic resonance(EPR)confirm the formation of hydro-gen species on the interstitial sites(Hi)or on the oxygen vacancy sites(H_(O)).The hydrogena-tion reaction of p-nitrophenol(pNP)at 40μmol/L occurs on both ZnO and Au/ZnO elec-trodes,and the hydrogenation reduction performance of Au/ZnO electrode is better than that of ZnO electrode.CVs show H_(O)species is much more reactive with pNP than Hi species.Compared with the ZnO electrode,the presence of Au on ZnO promotes the formation of H_(O)species and improves the electro-reduction performance to pNP.These results help us to un-derstand the reaction processes related to the electrochemical hydrogenation on ZnO and Au/ZnO surfaces and shed new light on the design of new catalytic hydrogenation systems.
基金supported by the National Key Research and Development Program(No.2022YFA1505800)the National Natural Science Foundation of China(No.22373092)+5 种基金CAS Project for Young Scientists in Basic Research(No.YSBR-051)China Association for Science and Technology(No.YESS20200031)the Start-up Funding of Central South University(No.502045005)Industry-University-Research Cooperation Projects with Zhejiang NHU Co.,Ltd.Ningbo Fengcheng Advanced Energy Materials Research Institutesupported by USTC Tang Scholarship。
文摘Manipulating catalyst structures to control product selectivity while maintaining high activity presents a considerable challenge in CO_(2)hydrogenation.Combining density functional theory calculations and microkinetic analysis,we proposed that graphene-supported isolated Pt atoms(Pt1/graphene)and Pt_(2)dimers(Pt_(2)/graphene)exhibited distinct selectivity in CO_(2)hydrogenation.Pt_(1)/graphene facilitated the conversion of CO_(2)into formic acid,whereas Pt_(2)/graphene favored methanol generation.The variation in product selectivity arose from the synergistic interaction of Pt_(2)dimers,which facilitated the migration of H atoms between two Pt atoms and promoted the transformation from*COOH intermediates to*C(OH)_(2)intermediates,altering the reaction pathways compared to isolated Pt atoms.Additionally,an analysis of the catalytic activities of three Pt_(1)/graphene and three Pt_(2)/graphene structures revealed that the turnover frequencies for formic acid generation on Pt_(1ii)/graphene and methanol generation on Pt_(2i)/graphene were as high as 744.48 h-1and 789.48 h^(-1),respectively.These values rivaled or even surpassed those previously reported in the literature under identical conditions.This study provides valuable insights into optimizing catalyst structures to achieve desired products in CO_(2)hydrogenation.
基金supported by the National Natural Science Foundation of China(Nos.22102167 and U21A20317)。
文摘Designing highly active electrocatalysts for the hydrogen evolution reaction(HER)and oxygen evolution and reduction reactions(OER and ORR)is pivotal to renewable energy technology.Herein,based on density functional theory(DFT)calculations,we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks(COF)monolayers with axially coordinated ligands(denotes as Fe N_(4)-X@COF,X refers to axial ligand,X=-SCN,-I,-H,-SH,-NO_(2),-Br,-ClO,-Cl,-HCO_(3),-NO,-ClO_(2),-OH,-CN and-F).The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities.The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center,which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity.Importantly,FeN_(4)-SH@COF and Fe N_(4)-OH@COF are efficient bifunctional catalysts for HER and OER,FeN_(4)-OH@COF and FeN_(4)-I@COF are promising bifunctional catalysts for OER and ORR.These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum ironnitrogen-carbon based catalysts.
文摘As one of the important components of high-effi-ciency perovskite/silicon series devices,wide-bandgap(WBG)perovskite solar cells(PSCs)have been suffering from serious carrier transport barriers and huge open-circuit voltage deficit de-rived from non-radiative recombination,especial-ly at the buried interface that are often overlooked.Herein,we combined cationic and anion passiva-tion strategies via ammonium tetra-n-butyl tetrafluoroborate(TBABF_(4))pre-treating the buried interface.Theoretical calculation predicts that the tetrabutylammonium(TBA^(+))organic cations and(tetrafluoroborate)BF_(4)^(−)anions can easily interact with charged interfacial defect.Characterizations further confirm the enhance-ment of carrier transport performance and decrease in defect density upon TBABF4 pre-treat-ment.Consequently,a power conversion efficiency of 21.35%with an ultrahigh filling factor of 84.12%is obtained for 1.68 eV-WBG inverted PSCs.In addition,the device with TBABF4 pre-treatment demonstrates excellent shelf,thermal,and operational stability.
基金supported by the National Natural Science Foundation of China(Grant Nos.GG2030007011 and GG2030040453)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302004)+1 种基金support from the National Natural Science Foundation of China(Grant No.12174236)the fund for the Shanxi 1331 Project.
文摘Quantum link models(QLMs)serve as experimentally accessible platforms for studying lattice gauge theories with finite-dimensional Hilbert spaces.In this work,we investigate information scrambling in the partially confined phase of a spin-1 quantum link model by calculating the dynamics of out-of-time-ordered correlators(OTOCs)and entanglement entropy.We observe that,in the partially confined phase,information scrambling exhibits significant asymmetry,manifested as the unidirectional propagation of both OTOCs and entanglement entropy.This phenomenon stands in stark contrast to the isotropic spreading observed in the deconfined phase and the localization characteristic of the confined phase.Furthermore,the simultaneous occurrence of the unidirectional propagation of both OTOCs and entanglement entropy,together with the q-induced asymmetric excitation propagation,reveals a direct connection between information scrambling and charge confinement.
基金the National Key R&D Program of China(No.2016YFA0200603 No.2017YFA0205004)the Anhui Initiative in Quantum Information Technologies(AHY090300)+2 种基金the National Natural Science Foundation of China(No.21473174)the Fundamental Research Funds for the Central Universities(No.WK2060190084 and No.WK2340000082)Ai-di Zhao acknowledges a fellow-ship from the Youth Innovation Promotion Association of Chinese Academy of Science(2011322).
文摘On-surface synthesis of semiconducting graphdiyne nanowires usually suffer severe side reactions owing to the high reactivity of the butadiynylene units at noble metal surfaces,limiting the production of isolated nanowires. In this work, we report the high-yield synthesis of branchless graphdiyne nanowires [-C≡C-Ph2-C≡C-]nvia on-surface Ullmann coupling of 1,4-bis（4-bromophenyl）-1,3-butadiyne molecules with chemical vapor deposition method.Non-contact atomic force microscopy with single-bond resolution reveals that single gold adatoms act as effective protecting groups for butadiynylene units by forming Au-π ligand bonds, preventing unwanted branched coupling reactions and enabling the synthesis of ultralong isolated graphdiyne nanowires. This study will stimulate further investigation on the role of various surface adatoms in protecting on-surface reactions.
