Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles...Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles of different forms of atomically-dispersed metals(i.e.,single-atoms and atomic clusters)in photocatalytic reactions remain ambiguous.Herein,we developed an ethylenediamine(EDA)-assisted reduction method to controllably synthesize atomically dispersed Au in the forms of Au single atoms(Au_(SA)),Au clusters(Au_(C)),and a mixed-phase of Au_(SA)and Au_(C)(Au_(SA+C))on CdS.In addition,we elucidate the synergistic effect of Au_(SA)and Au_(C)in enhancing the photocatalytic performance of CdS substrates for simultaneous CO_(2)reduction and aryl alcohol oxidation.Specifically,Au_(SA)can effectively lower the energy barrier for the CO_(2)→*COOH conversion,while Au_(C)can enhance the adsorption of alcohols and reduce the energy barrier for dehydrogenation.As a result,the Au_(SA)and Au_(C)co-loaded CdS show impressive overall photocatalytic CO_(2)conversion performance,achieving remarkable CO and BAD production rates of 4.43 and 4.71 mmol g^(−1)h^(−1),with the selectivities of 93%and 99%,respectively.More importantly,the solar-to-chemical conversion efficiency of Au_(SA+C)/CdS reaches 0.57%,which is over fivefold higher than the typical solar-to-biomass conversion efficiency found in nature(ca.0.1%).This study comprehensively describes the roles of different forms of atomically-dispersed metals and their synergistic effects in photocatalytic reactions,which is anticipated to pave a new avenue in energy and environmental applications.展开更多
Various migration methods have been proposed to image high-angle geological structures and media with strong lateral velocity variations; however, the problems of low precision and high computational cost remain unres...Various migration methods have been proposed to image high-angle geological structures and media with strong lateral velocity variations; however, the problems of low precision and high computational cost remain unresolved. To describe the seismic wave propagation in media with lateral velocity variations and to image high-angle structures, we propose the generalized screen propagator based on particle swarm optimization (PSO-GSP), for the precise fitting of the single-square-root operator. We use the 2D SEG/EAGE salt model to test the proposed PSO-GSP migration method to image the faults beneath the salt dome and compare the results to those of the conventional high-order generalized screen propagator (GSP) migration and split-step Fourier (SSF) migration. Moreover, we use 2D marine data from the South China Sea to show that the PSO-GSP migration can better image strong reflectors than conventional imaging methods.展开更多
Herein, we report self-assembly of tadpole-like single chain polymeric nanoparticles (TPPs) and the ultrasonic response of the resultant superparticles. The TPPs are with an intramolecularly crosslinked poly(2-(me...Herein, we report self-assembly of tadpole-like single chain polymeric nanoparticles (TPPs) and the ultrasonic response of the resultant superparticles. The TPPs are with an intramolecularly crosslinked poly(2-(methacryloyloxy)ethyl pent-4-ynoate)-rpoly(hydroxyethyl methacrylate) (PMAEP-r-PHEMA) chain as the "head" and a poly(2- (dimethylamino)ethyl methacrylate (PDMAEMA) linear chain as the "tail", and are pre- pared simply and emciently by Glaser-coupling of the pendant alkynes in the PMAEP-r- PHEMA block in the common solvent methanol. The formation of the TPPs was confirmed by gel permeation chromatograph, nuclear magnetic resonance spectroscopy, dynamic light scattering, static dynamic scattering, and transmission electron microscopy. In aqueous solution, the amphiphilic TPPs could self-assemble into regular superparticles, driven by aggregation of the hydrophobic "heads". Since in the structure there is no chain entanglement and the embedding of PDMAEMA chains disturb close-packing of the "heads", the superpartieles are responsive to a low-energy ultrasonic vibration, as evidenced by greatly enhanced release of the functional molecules from the superparticles by treatment of a low-energy ultrasound. Therefore, the superparticles should be very promising in the use as the drug carriers that can be manipulated from a long distance, considering that ultrasonic energy can be focused at a small area in a relatively long distance from the ultrasound-radiating source.展开更多
Heterogeneous catalysts with ultra-small clusters and atomically dispersed(USCAD)active sites have gained increasing attention in recent years.However,developing USCAD catalysts with high-density metal sites anchored ...Heterogeneous catalysts with ultra-small clusters and atomically dispersed(USCAD)active sites have gained increasing attention in recent years.However,developing USCAD catalysts with high-density metal sites anchored in porous nanomaterials is still challenging.Here,through the template-free S-assisted pyrolysis of low-cost Fe-salts with melamine(MA),porous alveolate Fe/g-C3N4 catalysts with high-density(Fe loading up to 17.7 wt%)and increased USCAD Fe sites were synthesized.The presence of a certain amount of S species in the Fe-salts/MA system plays an important role in the formation of USCAD S-Fe-salt/CN catalysts;the S species act as a"sacrificial carrier"to increase the dispersion of Fe species through Fe-S coordination and generate porous alveolate structure by escaping in the form of SO2 during pyrolysis.The S-Fe-salt/CN catalysts exhibit greatly promoted activity and reusability for degrading various organic pollutants in advanced oxidation processes compared to the corresponding Fe-salt/CN catalysts,due to the promoted accessibility of USCAD Fe sites by the porous alveolate structure.This S-assisted method exhibits good feasibility in a large variety of S species(thiourea,S powder,and NH4SCN)and Fe salts,providing a new avenue for the low-cost and large-scale synthesis of high-density USCAD metal/g-C3N4 catalysts.展开更多
The interaction of a single three-level trapped ion with two laser beams has been studied theoretically. With application of two successive unitary transformations, an analytical solution to this quantum system has be...The interaction of a single three-level trapped ion with two laser beams has been studied theoretically. With application of two successive unitary transformations, an analytical solution to this quantum system has been obtained.展开更多
The cavity field spectrum of a cascade three-level atom interacting with single-mode field with Kerr-like medium in the cavity is investigated. The numerical results for the initial field in pure number state, coheren...The cavity field spectrum of a cascade three-level atom interacting with single-mode field with Kerr-like medium in the cavity is investigated. The numerical results for the initial field in pure number state, coherent state and squeezed vacuum state are calculated, respectively. It is found that the Kerr-like medium affects the spectral structure even though the initial field is in vacuum when the atom is in upper level. In the case of strong input field, the number state spectrum shows two peaks with different heights; and the superposition state spectrum shows a multipeak structure with an equal distance of two neighboring peaks. The spectral "central frequency" shifts away from the resonant frequency with the increasing of average photon number.展开更多
Non-contact atomic force microscopy(nc-AFM) atomic-scale imaging process of monocrystalline silicon surface using capped single-wall carbon nanotube tip is simulated by molecular dynamic method. The simulation resuh...Non-contact atomic force microscopy(nc-AFM) atomic-scale imaging process of monocrystalline silicon surface using capped single-wall carbon nanotube tip is simulated by molecular dynamic method. The simulation resuhs show that the nc-AFM imaging force mainly comes from the C-Si and C-C chemical covalent bonding forces, especially the former, the nonbonding Van der Waals force change is small during the range of stable imaging height. When the tip-surface distance is smaller than the stable imaging height, several neighboring carbon atoms at the tip apex are attracted, and some of them jump onto the sample surface. Finally the tip apex configuration is destroyed with the tip indenting further.展开更多
A very simpJe theoretical scheme is proposed to implement two-and three-qubit controlled-phase gates firstly only using a single resonant interaction between ladder-type three-level atoms and the single-mode cavity. I...A very simpJe theoretical scheme is proposed to implement two-and three-qubit controlled-phase gates firstly only using a single resonant interaction between ladder-type three-level atoms and the single-mode cavity. In the presented protocol, the quantum information is encoded on the stable ground states of the atoms (as the controlling qubits) and the zero- and one-photon Fock states of cavity-field (as the target qubit). Under the influence of the atomic spontaneous emission, the decay of the cavity-mode, and deviation of the coupling strength, the three-qubit controlled- phase gate may have a comparatively high fidelity. The experimental feasibility of controlled-phase gate and the ease that is extended to realize N-qubit controlled-phase gate are also discussed.展开更多
Using multipohton Tavis-Cummings model,the entanglement evolution of two coupling two-level atoms in Bell states interacting with a single-mode vacuum field is investigated by using negativity.The influences of coupli...Using multipohton Tavis-Cummings model,the entanglement evolution of two coupling two-level atoms in Bell states interacting with a single-mode vacuum field is investigated by using negativity.The influences of coupling constants between atoms,the atomic initial states and the photon number of transition on the entanglement evolution of two coupling two-level atoms are discussed.The results obtained using the numerical method show that the entanglement of two atoms is related with coupling constants between atoms,the atomic initial states and the photon number of transition.The two-atom entanglement state will forever stay in the maximum entanglement state when the initial state is β11〉.When the initial state of two atoms is β01〉,the entanglement of two atoms displays periodic oscillation behavior.And its oscillation period decreases with increasing of coupling constant between atoms or the photon number of transition.On the other hand,when the initial state is β00〉 or β10〉,the entanglement of two atoms displays quasiperiodic oscillation behavior and its oscillation period decreases with increasing of coupling constant between atoms or the photon number of transition.展开更多
Proton exchange membrane fuel cells(PEMFCs)suffer extreme CO poisoning even at PPM level(<10 ppm),owning to the preferential CO adsorption and the consequential blockage of the catalyst surface.Herein,however,we re...Proton exchange membrane fuel cells(PEMFCs)suffer extreme CO poisoning even at PPM level(<10 ppm),owning to the preferential CO adsorption and the consequential blockage of the catalyst surface.Herein,however,we report that CO itself can become an easily convertible fuel in PEMFC using atomically dispersed Rh catalysts(Rh-N-C).With CO to CO_(2) conversion initiates at 0 V,pure CO powered fuel cell attains unprecedented power density at 236 mW cm^(-2),with maximum CO turnover frequency(64.65 s^(-1),363 K)far exceeding any chemical or electrochemical catalysts reported.Moreover,this feature enables efficient CO selective removal from H_(2) gas stream through the PEMFC technique,with CO concentration reduced by one order of magnitude through running only one single cell,while simultaneously harvesting electricity.We attribute such catalytic behavior to the weak CO adsorption and the co-activation of H_(2)O due to the interplay between two adjacent Rh sites.展开更多
The echo-enabled harmonic generation (EEHG) scheme holds promising prospects for efficiently generat- ing intense coherent radiation at very high harmonics of the initial seed laser. In this paper, we study the feas...The echo-enabled harmonic generation (EEHG) scheme holds promising prospects for efficiently generat- ing intense coherent radiation at very high harmonics of the initial seed laser. In this paper, we study the feasibility of operating the Shanghai X-ray free-electron laser test facility with a single stage EEHG setup. With a combina- tion of existing numerical codes, start-to-end simulations considering various three-dimensional effects have been carried out to show the possible performance of the EEHG FEL. Simulation results demonstrate that a single stage EEHG can generate high power soft X-ray radiation pulses with narrow bandwidth directly from UV seed lasers. With the help of the harmonic lasing technique or upgraded linac, we also show the possibility of generating coherent soft X-ray radiation in the "water window" with a single stage EEHG.展开更多
As a continuation of previous work, in this paper, we mainly study the finite simple groups which have abelian Sylow subgroups in term of p-local rank, especially a group theoretic characterization will be given.
文摘Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles of different forms of atomically-dispersed metals(i.e.,single-atoms and atomic clusters)in photocatalytic reactions remain ambiguous.Herein,we developed an ethylenediamine(EDA)-assisted reduction method to controllably synthesize atomically dispersed Au in the forms of Au single atoms(Au_(SA)),Au clusters(Au_(C)),and a mixed-phase of Au_(SA)and Au_(C)(Au_(SA+C))on CdS.In addition,we elucidate the synergistic effect of Au_(SA)and Au_(C)in enhancing the photocatalytic performance of CdS substrates for simultaneous CO_(2)reduction and aryl alcohol oxidation.Specifically,Au_(SA)can effectively lower the energy barrier for the CO_(2)→*COOH conversion,while Au_(C)can enhance the adsorption of alcohols and reduce the energy barrier for dehydrogenation.As a result,the Au_(SA)and Au_(C)co-loaded CdS show impressive overall photocatalytic CO_(2)conversion performance,achieving remarkable CO and BAD production rates of 4.43 and 4.71 mmol g^(−1)h^(−1),with the selectivities of 93%and 99%,respectively.More importantly,the solar-to-chemical conversion efficiency of Au_(SA+C)/CdS reaches 0.57%,which is over fivefold higher than the typical solar-to-biomass conversion efficiency found in nature(ca.0.1%).This study comprehensively describes the roles of different forms of atomically-dispersed metals and their synergistic effects in photocatalytic reactions,which is anticipated to pave a new avenue in energy and environmental applications.
基金supported by the 863 Program of China(No.2013AA064201)National Science and Technology Major Project(No.2016ZX05003-003)
文摘Various migration methods have been proposed to image high-angle geological structures and media with strong lateral velocity variations; however, the problems of low precision and high computational cost remain unresolved. To describe the seismic wave propagation in media with lateral velocity variations and to image high-angle structures, we propose the generalized screen propagator based on particle swarm optimization (PSO-GSP), for the precise fitting of the single-square-root operator. We use the 2D SEG/EAGE salt model to test the proposed PSO-GSP migration method to image the faults beneath the salt dome and compare the results to those of the conventional high-order generalized screen propagator (GSP) migration and split-step Fourier (SSF) migration. Moreover, we use 2D marine data from the South China Sea to show that the PSO-GSP migration can better image strong reflectors than conventional imaging methods.
基金This work was supported by the National Natural Science Foundation of China (No.21334001 and No.91127030).
文摘Herein, we report self-assembly of tadpole-like single chain polymeric nanoparticles (TPPs) and the ultrasonic response of the resultant superparticles. The TPPs are with an intramolecularly crosslinked poly(2-(methacryloyloxy)ethyl pent-4-ynoate)-rpoly(hydroxyethyl methacrylate) (PMAEP-r-PHEMA) chain as the "head" and a poly(2- (dimethylamino)ethyl methacrylate (PDMAEMA) linear chain as the "tail", and are pre- pared simply and emciently by Glaser-coupling of the pendant alkynes in the PMAEP-r- PHEMA block in the common solvent methanol. The formation of the TPPs was confirmed by gel permeation chromatograph, nuclear magnetic resonance spectroscopy, dynamic light scattering, static dynamic scattering, and transmission electron microscopy. In aqueous solution, the amphiphilic TPPs could self-assemble into regular superparticles, driven by aggregation of the hydrophobic "heads". Since in the structure there is no chain entanglement and the embedding of PDMAEMA chains disturb close-packing of the "heads", the superpartieles are responsive to a low-energy ultrasonic vibration, as evidenced by greatly enhanced release of the functional molecules from the superparticles by treatment of a low-energy ultrasound. Therefore, the superparticles should be very promising in the use as the drug carriers that can be manipulated from a long distance, considering that ultrasonic energy can be focused at a small area in a relatively long distance from the ultrasound-radiating source.
文摘Heterogeneous catalysts with ultra-small clusters and atomically dispersed(USCAD)active sites have gained increasing attention in recent years.However,developing USCAD catalysts with high-density metal sites anchored in porous nanomaterials is still challenging.Here,through the template-free S-assisted pyrolysis of low-cost Fe-salts with melamine(MA),porous alveolate Fe/g-C3N4 catalysts with high-density(Fe loading up to 17.7 wt%)and increased USCAD Fe sites were synthesized.The presence of a certain amount of S species in the Fe-salts/MA system plays an important role in the formation of USCAD S-Fe-salt/CN catalysts;the S species act as a"sacrificial carrier"to increase the dispersion of Fe species through Fe-S coordination and generate porous alveolate structure by escaping in the form of SO2 during pyrolysis.The S-Fe-salt/CN catalysts exhibit greatly promoted activity and reusability for degrading various organic pollutants in advanced oxidation processes compared to the corresponding Fe-salt/CN catalysts,due to the promoted accessibility of USCAD Fe sites by the porous alveolate structure.This S-assisted method exhibits good feasibility in a large variety of S species(thiourea,S powder,and NH4SCN)and Fe salts,providing a new avenue for the low-cost and large-scale synthesis of high-density USCAD metal/g-C3N4 catalysts.
基金The project supported by the Natural Science Foundation of Education Committee of Anhui Province of China under Grant No. 2004kj186
文摘The interaction of a single three-level trapped ion with two laser beams has been studied theoretically. With application of two successive unitary transformations, an analytical solution to this quantum system has been obtained.
基金The project supported by the Natural Science Foundation of Shandong Province under Grant No. Y2004A09
文摘The cavity field spectrum of a cascade three-level atom interacting with single-mode field with Kerr-like medium in the cavity is investigated. The numerical results for the initial field in pure number state, coherent state and squeezed vacuum state are calculated, respectively. It is found that the Kerr-like medium affects the spectral structure even though the initial field is in vacuum when the atom is in upper level. In the case of strong input field, the number state spectrum shows two peaks with different heights; and the superposition state spectrum shows a multipeak structure with an equal distance of two neighboring peaks. The spectral "central frequency" shifts away from the resonant frequency with the increasing of average photon number.
文摘Non-contact atomic force microscopy(nc-AFM) atomic-scale imaging process of monocrystalline silicon surface using capped single-wall carbon nanotube tip is simulated by molecular dynamic method. The simulation resuhs show that the nc-AFM imaging force mainly comes from the C-Si and C-C chemical covalent bonding forces, especially the former, the nonbonding Van der Waals force change is small during the range of stable imaging height. When the tip-surface distance is smaller than the stable imaging height, several neighboring carbon atoms at the tip apex are attracted, and some of them jump onto the sample surface. Finally the tip apex configuration is destroyed with the tip indenting further.
基金Supported by Key Scientific Research Fund of Hunan Provincial Education Department of China under Grant No. 09A013Natural Science Foundation of Hunan Province of China under Grant No. 08J J3001Normal and Science Foundation of Hengyang Normal University of China under Grant No. 09A28
文摘A very simpJe theoretical scheme is proposed to implement two-and three-qubit controlled-phase gates firstly only using a single resonant interaction between ladder-type three-level atoms and the single-mode cavity. In the presented protocol, the quantum information is encoded on the stable ground states of the atoms (as the controlling qubits) and the zero- and one-photon Fock states of cavity-field (as the target qubit). Under the influence of the atomic spontaneous emission, the decay of the cavity-mode, and deviation of the coupling strength, the three-qubit controlled- phase gate may have a comparatively high fidelity. The experimental feasibility of controlled-phase gate and the ease that is extended to realize N-qubit controlled-phase gate are also discussed.
基金Supported by the Natural Science Foundation of Fujian Province under Grant (No.2008J0217)
文摘Using multipohton Tavis-Cummings model,the entanglement evolution of two coupling two-level atoms in Bell states interacting with a single-mode vacuum field is investigated by using negativity.The influences of coupling constants between atoms,the atomic initial states and the photon number of transition on the entanglement evolution of two coupling two-level atoms are discussed.The results obtained using the numerical method show that the entanglement of two atoms is related with coupling constants between atoms,the atomic initial states and the photon number of transition.The two-atom entanglement state will forever stay in the maximum entanglement state when the initial state is β11〉.When the initial state of two atoms is β01〉,the entanglement of two atoms displays periodic oscillation behavior.And its oscillation period decreases with increasing of coupling constant between atoms or the photon number of transition.On the other hand,when the initial state is β00〉 or β10〉,the entanglement of two atoms displays quasiperiodic oscillation behavior and its oscillation period decreases with increasing of coupling constant between atoms or the photon number of transition.
基金supported by the National Key Research and Development Program of China (2017YFB0102900)the National Natural Science Foundation of China (21875243, 21633008, 21673221, and U1601211)+3 种基金Jilin Provincial Science and Technology Development Program (20200201001JC, 20190201270JC, and 20180101030JC)supported by the High Performance Computing Center of Jilin University and Jilin ProvinceNetwork and Computing Center of Changchun Institute of Applied Chemistry, Chinese Academy of Sciencessupported by Linglu Instruments (Shanghai) Co., Ltd.
文摘Proton exchange membrane fuel cells(PEMFCs)suffer extreme CO poisoning even at PPM level(<10 ppm),owning to the preferential CO adsorption and the consequential blockage of the catalyst surface.Herein,however,we report that CO itself can become an easily convertible fuel in PEMFC using atomically dispersed Rh catalysts(Rh-N-C).With CO to CO_(2) conversion initiates at 0 V,pure CO powered fuel cell attains unprecedented power density at 236 mW cm^(-2),with maximum CO turnover frequency(64.65 s^(-1),363 K)far exceeding any chemical or electrochemical catalysts reported.Moreover,this feature enables efficient CO selective removal from H_(2) gas stream through the PEMFC technique,with CO concentration reduced by one order of magnitude through running only one single cell,while simultaneously harvesting electricity.We attribute such catalytic behavior to the weak CO adsorption and the co-activation of H_(2)O due to the interplay between two adjacent Rh sites.
基金This work was partially supported by the National Development and Reform Commission ([201312347), the National Natural Science Foundation of China (11475250, 11175240, 11275253 and 11322550) and the National Basic Research Program of China (2015CB859700).
文摘The echo-enabled harmonic generation (EEHG) scheme holds promising prospects for efficiently generat- ing intense coherent radiation at very high harmonics of the initial seed laser. In this paper, we study the feasibility of operating the Shanghai X-ray free-electron laser test facility with a single stage EEHG setup. With a combina- tion of existing numerical codes, start-to-end simulations considering various three-dimensional effects have been carried out to show the possible performance of the EEHG FEL. Simulation results demonstrate that a single stage EEHG can generate high power soft X-ray radiation pulses with narrow bandwidth directly from UV seed lasers. With the help of the harmonic lasing technique or upgraded linac, we also show the possibility of generating coherent soft X-ray radiation in the "water window" with a single stage EEHG.
基金supported by National Natural Science Foundation of China (Grant No. 10701006)
文摘As a continuation of previous work, in this paper, we mainly study the finite simple groups which have abelian Sylow subgroups in term of p-local rank, especially a group theoretic characterization will be given.