Thermo-Hydro-Mechanical (THM) coupling pro- cesses in unsaturated soils are very important in both theoretical researches and engineering applications. A coupled formulation based on hybrid mixture theory is derived...Thermo-Hydro-Mechanical (THM) coupling pro- cesses in unsaturated soils are very important in both theoretical researches and engineering applications. A coupled formulation based on hybrid mixture theory is derived to model the THM coupling behavior of unsaturated soils. The free-energy and dissipative functions for different phases are derived from Taylor's series expansions. Constitutive relations for THM coupled behaviors of unsaturated soils, which include deformation, entropy change, fluid flow, heat conduction, and dynamic compatibility conditions on the interfaces, are then established. The number of field equations is shown to be equal to the number of unknown variables; thus, a closure of this coupling problem is established. In addition to modifications of the physical conservation equations with coupling effect terms, the constitutive equations, which consider the coupling between elastoplastic deformation of the soil skeleton, fluid flow, and heat transfer, are also derived.展开更多
A mixture theory is developed for multi-component micropolar porous media with a combination of the hybrid mixture theory and the micropolar continuum theory. The system is modeled as multi-component micropolar elasti...A mixture theory is developed for multi-component micropolar porous media with a combination of the hybrid mixture theory and the micropolar continuum theory. The system is modeled as multi-component micropolar elastic solids saturated with multi- component micropolar viscous fluids. Balance equations are given through the mixture theory. Constitutive equations are developed based on the second law of thermodynamics and constitutive assumptions. Taking account of compressibility of solid phases, the volume fraction of fluid as an independent state variable is introduced in the free energy function, and the dynamic compatibility condition is obtained to restrict the change of pressure difference on the solid-fluid interface. The constructed constitutive equations are used to close the field equations. The linear field equations are obtained using a linearization procedure, and the micropolar thermo-hydro-mechanical component transport model is established. This model can be applied to practical problems, such as contaminant, drug, and pesticide transport. When the proposed model is supposed to be porous media, and both fluid and solid are single-component, it will almost agree with Eringen's model.展开更多
Conventional overconstrained parallel manipulators have been widely studied both in industry and academia,however the structural synthesis of hybrid mechanisms with additional constraints is seldom studied,especially ...Conventional overconstrained parallel manipulators have been widely studied both in industry and academia,however the structural synthesis of hybrid mechanisms with additional constraints is seldom studied,especially for the four degrees of freedom(DOF) hybrid mechanisms.In order to develop a manipulator with additional constraints,a class of important spatial mechanisms with coupling chains(CCs) whose motion type is two rotations and two translations(2R2T) is presented.Based on screw theory,the combination of different types of limbs which are used to construct parallel mechanisms and coupling chains is proposed.The basic types of the general parallel mechanisms and geometric conditions of the kinematic chains are given using constraint synthesis method.Moreover,the 2R2T motion pattern hybrid mechanisms which are derived by adding coupling chains between different serial kinematic chains(SKCs) of the corresponding parallel mechanisms are presented.According to the constraint analysis of the mechanisms,the movement relationship of the moving platform and the kinematic chains is derived by disassembling the coupling chains.At last,fourteen novel hybrid mechanisms with two or three serial kinematic chains are presented.The proposed novel hybrid mechanisms and construction method enrich the family of the spatial mechanisms and provide an instruction to design more complex hybrid mechanisms.展开更多
A single intersection of two phases is selected as a model to put forward a new optimal time-planning scheme for traffic light based on the model of hybrid automata for single intersection. A method of optimization is...A single intersection of two phases is selected as a model to put forward a new optimal time-planning scheme for traffic light based on the model of hybrid automata for single intersection. A method of optimization is proposed for hybrid systems, and the average queue length over all queues is used as an objective function to find an optimal switching scheme for traffic light. It is illustrated that traffic light control for single intersection is a typical hybrid system, and the optimal planning-time scheme can be obtained using the optimal hybrid systems control based on the two stages method.展开更多
A theoretical study on the reaction of aluminum with water in the gas phase was performed using the hybrid density functional B3LYP and QCISD(T) methods with the 6-311+G(d,p) and the 6-311++G(d,p) basis sets....A theoretical study on the reaction of aluminum with water in the gas phase was performed using the hybrid density functional B3LYP and QCISD(T) methods with the 6-311+G(d,p) and the 6-311++G(d,p) basis sets. The results show that there are three possible reaction pathways that involve four isomers, seven transition structures, and two possible products for the reaction of aluminum with water. The two most favorable reaction pathways were found, whose intermediates and products agreed quite well with experimental results. The enthalpy and Gibbs free energy change of the reaction between A1 and H2O at 298 and 2000 K were calculated. Some results are also in good agreement with the previous calculations or experimental results.展开更多
In this article, we present a new type of unified dynamic scaling property for synchronizability, which can describe the scaling relationship between dynamic synehronizability and four hybrid ratios under the unified ...In this article, we present a new type of unified dynamic scaling property for synchronizability, which can describe the scaling relationship between dynamic synehronizability and four hybrid ratios under the unified hybrid network theory framework (UHNTF). Our theory results can not only be applied to judge and analyze dynamic synehronizability for most of complex networks associated with the UHNTF, but also we can flexibly adjust and design different hybrid ratios and sealing exponent to meet actual requirement for the dynanfic characteristics of the UHNTF.展开更多
The effects of inner nanowire radius,shell thickness,the dielectric functions of middle layer and surrounding medium on localized surface plasmon resonance(LSPR)of gold-dielectric-silver nanotube are studied based on ...The effects of inner nanowire radius,shell thickness,the dielectric functions of middle layer and surrounding medium on localized surface plasmon resonance(LSPR)of gold-dielectric-silver nanotube are studied based on the quasi-static approximation.Theoretical calculation results show that LSPR of gold-dielectric-silver nanotube and LSPR numbers can be well optimized by adjusting its geometrical parameters.The longer wavelength of |ω--> mode takes place a distinct red-shift with increasing the inner nanowire radius and the thickness of middle dielectric layer,while a blue-shift with increasing outer nanotube thickness.The physical mechanisms are explained based on the plasmon hybridization theory,induced charges and phase retardation.In addition,the effects of middle dielectric function and surrounding medium on LSPR,and the local electric field factor are also reported.Our study provides the potential applications of gold-dielectricsilver nanotube in biological tissues,sensor and related regions.展开更多
The demands of a rapidly advancing technology for faster and more accurate controllers have always had a strong influence on the progress of automatic control theory. In recent years control problems have been arising...The demands of a rapidly advancing technology for faster and more accurate controllers have always had a strong influence on the progress of automatic control theory. In recent years control problems have been arising with increasing frequency in widely different areas, which cannot be addressed using conventional control techniques. The principal reason for this is the fact that a highly competitive economy is forcing systems to operate in regimes where presence of large uncertainties as well as nonlinearities plays a major role. For instance, the design of unmanned aircraft, unmanned underwater vehicles, and automatic driving systems for automobiles are all typical examples of such difficult control problems. The large uncertainties concerning the plant may arise due to large external disturbances, large parameter variations because of faults in the system, or failure of some of the subsystems. In such cases, the controller has to determine the specific situation that exists at any instant, and take the appropriate control action. Accomplishing this rapidly, accurately, and in a stable fashion is the objective of control design.展开更多
To evaluate transmission rate of highly dynamic space networks,a new method for studying space network capacity is proposed in this paper. Using graph theory,network capacity is defined as the maximum amount of flows ...To evaluate transmission rate of highly dynamic space networks,a new method for studying space network capacity is proposed in this paper. Using graph theory,network capacity is defined as the maximum amount of flows ground stations can receive per unit time. Combined with a hybrid constellation model,network capacity is calculated and further analyzed for practical cases. Simulation results show that network capacity will increase to different extents as link capacity,minimum ground elevation constraint and satellite onboard processing capability change. Considering the efficiency and reliability of communication networks,how to scientifically design satellite networks is also discussed.展开更多
The electronic properties of zinc-blende BxGal-xN alloys are comparatively investigated by employ- ing both the Perdewe-Burkee-Ernzerhof generalized-gradient approximation (PBE-GGA) and the Heyd-Scuseria- Ernzerhof ...The electronic properties of zinc-blende BxGal-xN alloys are comparatively investigated by employ- ing both the Perdewe-Burkee-Ernzerhof generalized-gradient approximation (PBE-GGA) and the Heyd-Scuseria- Ernzerhof screened hybrid functional methods (HSE06). HSE06 reproduced much closer ground-state properties to experiments. Large and composition-dependent bowing parameters br for the direct band gaps were obtained from both PBE and HSE06. The crossover composition where alloy switches from direct to indirect was predicted to occur at very similar x from PBE and HSE06. We can obtain direct gap BxGal-xN with a gap value much larger than that of GaN by alloying x 〈 0.557 boron into GaN.展开更多
Deoxyribonucleic acid(DNA) carries the genetic information in all living organisms. It consists of two interwound single-stranded(ss) strands, forming a double-stranded(ds) DNA with a right-handed double-helical confo...Deoxyribonucleic acid(DNA) carries the genetic information in all living organisms. It consists of two interwound single-stranded(ss) strands, forming a double-stranded(ds) DNA with a right-handed double-helical conformation. The two strands are held together by highly specific basepairing interactions and are further stabilized by stacking between adjacent basepairs. A transition from a dsDNA to two separated ssDNA is called melting and the reverse transition is called hybridization. Applying a tensile force to a dsDNA can result in a particular type of DNA melting, during which one ssDNA strand is peeled away from the other. In this work, we studied the kinetics of strand-peeling and hybridization of short DNA under tensile forces. Our results show that the force-dependent strand-peeling and hybridization can be described with a simple two-state model. Importantly, detailed analysis of the force-dependent transition rates revealed that the transition state consists of several basepairs dsDNA.展开更多
A nonlinear multi-field coupled model for multi-constituent three-phase soils is derived by using the hybrid mixture theory. The balance equations with three levels (constituents, phases and the whole mixture soil) ar...A nonlinear multi-field coupled model for multi-constituent three-phase soils is derived by using the hybrid mixture theory. The balance equations with three levels (constituents, phases and the whole mixture soil) are set up under the assumption that soil is composed of multi-constituent elastic-plastic solid skeleton (which is different from the linearization method) and viscous liquid and ideal gas. With reasonable constitutive assumptions in such restrictive conditions as the principles of determinism, equipresence, material frame-indifference and the compatible principle in continuum mechanics, a theoretical framework of constitutive relations modeling three-phase soil in both non-equilibrium and equilibrium states is established, thus the closed field equations are formed. In the theoretical framework, the concept of effective generalized thermodynamic forces is introduced, and the nonlinear coupling constitutive relations between generalized dissipation forces and generalized flows within the system at nonequilibrium state are also presented. On such a basis, four special coupling relations, i.e., solid thermal elastic-plastic constitutive relation, liquid visco-elastic-plastic constitutive relation, the generalized Fourier’s law, and the generalized Darcy’s law are put forward. The generalized or nonlinear results mentioned above can degenerate into the linear coupling results given by Bennethum and Singh. Based on a specific dissipation function, the concrete form of generalized Darcy’s law is deduced, which may degenerate into the traditional form of Darcy’s law by neglecting the influence of skeleton deformation and temperature. Without considering temperature and other coupling effects, the nonlinear coupled model in this paper can degenerate into a soil elastic-plastic constitutive model.展开更多
It has been demonstrated that intermolecular interaction,crucial in a plenty of chemical and physical processes,may vary in the presence of metal surface.However,such modification is yet to be quantitatively revealed....It has been demonstrated that intermolecular interaction,crucial in a plenty of chemical and physical processes,may vary in the presence of metal surface.However,such modification is yet to be quantitatively revealed.Here,we present a systematical density functional theory study on adsorbed bis(para-pyridyl)acetylene(BPPA) tetramer on Au(111) surface.We observed unusually high electron density between two head-to-head N atoms,an intermolecular "non-bonded" region,in adsorbed BPPA tetramer.This exceptional electron density originates from the wavefunction hybridization of the two compressed N lone-electron-pair states of two BPPA,as squeezed by a newly revealed N-Au-N threecenter bonding.This bond,together with the minor contribution from N...H-C intermolecular hydrogen bonding,shortens the N-N distance from over 4 A to 3.30 A and offers an attractive lateral interacting energy of 0.60 eV,effectively to a surface-confined in-plane pressure.The overlapped non-bonding vvavefunction hybridization arising from the effective pressure induced by the N-Au-N three-center bonding,as not been fully recognized in earlier studies,was manifested in non-contact Atomic Force Microscopy.展开更多
The formation, structural and electronic properties of silicene oxides(SOs) that result from the oxidation of silicene on Ag(111) surface have been investigated in the framework of density functional theory(DFT)...The formation, structural and electronic properties of silicene oxides(SOs) that result from the oxidation of silicene on Ag(111) surface have been investigated in the framework of density functional theory(DFT).It is found that the honeycomb lattice of silicene on the Ag(111) surface changes after the oxidation. SOs are strongly hybridized with the Ag(111) surface so that they possess metallic band structures. Charge accumulation between SOs and the Ag(111) surface indicates strong chemical bonding, which dramatically affects the electronic properties of SOs. When SOs are peeled off the Ag(111) surface, however, they may become semiconductors.展开更多
基金supported by the National Natural Science Foundation of China(51208031 and 51278047)the National Basic Research Program of China(2010CB732100)
文摘Thermo-Hydro-Mechanical (THM) coupling pro- cesses in unsaturated soils are very important in both theoretical researches and engineering applications. A coupled formulation based on hybrid mixture theory is derived to model the THM coupling behavior of unsaturated soils. The free-energy and dissipative functions for different phases are derived from Taylor's series expansions. Constitutive relations for THM coupled behaviors of unsaturated soils, which include deformation, entropy change, fluid flow, heat conduction, and dynamic compatibility conditions on the interfaces, are then established. The number of field equations is shown to be equal to the number of unknown variables; thus, a closure of this coupling problem is established. In addition to modifications of the physical conservation equations with coupling effect terms, the constitutive equations, which consider the coupling between elastoplastic deformation of the soil skeleton, fluid flow, and heat transfer, are also derived.
基金supported by the National Natural Science Foundation of China (No.50778013)the Natural Science Foundation of Beijing (No.8082020)
文摘A mixture theory is developed for multi-component micropolar porous media with a combination of the hybrid mixture theory and the micropolar continuum theory. The system is modeled as multi-component micropolar elastic solids saturated with multi- component micropolar viscous fluids. Balance equations are given through the mixture theory. Constitutive equations are developed based on the second law of thermodynamics and constitutive assumptions. Taking account of compressibility of solid phases, the volume fraction of fluid as an independent state variable is introduced in the free energy function, and the dynamic compatibility condition is obtained to restrict the change of pressure difference on the solid-fluid interface. The constructed constitutive equations are used to close the field equations. The linear field equations are obtained using a linearization procedure, and the micropolar thermo-hydro-mechanical component transport model is established. This model can be applied to practical problems, such as contaminant, drug, and pesticide transport. When the proposed model is supposed to be porous media, and both fluid and solid are single-component, it will almost agree with Eringen's model.
基金Supported by National Natural Science Foundation of China(Grant Nos.51175029,51475035)
文摘Conventional overconstrained parallel manipulators have been widely studied both in industry and academia,however the structural synthesis of hybrid mechanisms with additional constraints is seldom studied,especially for the four degrees of freedom(DOF) hybrid mechanisms.In order to develop a manipulator with additional constraints,a class of important spatial mechanisms with coupling chains(CCs) whose motion type is two rotations and two translations(2R2T) is presented.Based on screw theory,the combination of different types of limbs which are used to construct parallel mechanisms and coupling chains is proposed.The basic types of the general parallel mechanisms and geometric conditions of the kinematic chains are given using constraint synthesis method.Moreover,the 2R2T motion pattern hybrid mechanisms which are derived by adding coupling chains between different serial kinematic chains(SKCs) of the corresponding parallel mechanisms are presented.According to the constraint analysis of the mechanisms,the movement relationship of the moving platform and the kinematic chains is derived by disassembling the coupling chains.At last,fourteen novel hybrid mechanisms with two or three serial kinematic chains are presented.The proposed novel hybrid mechanisms and construction method enrich the family of the spatial mechanisms and provide an instruction to design more complex hybrid mechanisms.
文摘A single intersection of two phases is selected as a model to put forward a new optimal time-planning scheme for traffic light based on the model of hybrid automata for single intersection. A method of optimization is proposed for hybrid systems, and the average queue length over all queues is used as an objective function to find an optimal switching scheme for traffic light. It is illustrated that traffic light control for single intersection is a typical hybrid system, and the optimal planning-time scheme can be obtained using the optimal hybrid systems control based on the two stages method.
基金This work was supported by the National Natural Science Foundation of China (No.50476025).
文摘A theoretical study on the reaction of aluminum with water in the gas phase was performed using the hybrid density functional B3LYP and QCISD(T) methods with the 6-311+G(d,p) and the 6-311++G(d,p) basis sets. The results show that there are three possible reaction pathways that involve four isomers, seven transition structures, and two possible products for the reaction of aluminum with water. The two most favorable reaction pathways were found, whose intermediates and products agreed quite well with experimental results. The enthalpy and Gibbs free energy change of the reaction between A1 and H2O at 298 and 2000 K were calculated. Some results are also in good agreement with the previous calculations or experimental results.
基金The work was supported by the National Natural Science Foundation of China (Grant Nos. 60874087 and 61174151).
文摘In this article, we present a new type of unified dynamic scaling property for synchronizability, which can describe the scaling relationship between dynamic synehronizability and four hybrid ratios under the unified hybrid network theory framework (UHNTF). Our theory results can not only be applied to judge and analyze dynamic synehronizability for most of complex networks associated with the UHNTF, but also we can flexibly adjust and design different hybrid ratios and sealing exponent to meet actual requirement for the dynanfic characteristics of the UHNTF.
基金Project supported by the Programs for Anhui Provincial Natural Science Foundation,China(Grant Nos.1808085MA20 and 1808085MA05)Excellent Young Talents in University of Anhui Province,China(Grant No.gxyq2017027)+2 种基金the Key Scientific Research Foundation of Anhui Provincial Education Department,China(Grant Nos.KJ2019A0564 and KJ2018A0366)the Key Research and Development Projects of Anhui Province,China(Grant No.202004f06020021)Higher Educational Quality Engineering Projects of Anhui Province,China(Grant Nos.2020szsfkc0540,2020szsfkc0548,2020jyxm1080,and aqnu2019jyzc066).
文摘The effects of inner nanowire radius,shell thickness,the dielectric functions of middle layer and surrounding medium on localized surface plasmon resonance(LSPR)of gold-dielectric-silver nanotube are studied based on the quasi-static approximation.Theoretical calculation results show that LSPR of gold-dielectric-silver nanotube and LSPR numbers can be well optimized by adjusting its geometrical parameters.The longer wavelength of |ω--> mode takes place a distinct red-shift with increasing the inner nanowire radius and the thickness of middle dielectric layer,while a blue-shift with increasing outer nanotube thickness.The physical mechanisms are explained based on the plasmon hybridization theory,induced charges and phase retardation.In addition,the effects of middle dielectric function and surrounding medium on LSPR,and the local electric field factor are also reported.Our study provides the potential applications of gold-dielectricsilver nanotube in biological tissues,sensor and related regions.
文摘The demands of a rapidly advancing technology for faster and more accurate controllers have always had a strong influence on the progress of automatic control theory. In recent years control problems have been arising with increasing frequency in widely different areas, which cannot be addressed using conventional control techniques. The principal reason for this is the fact that a highly competitive economy is forcing systems to operate in regimes where presence of large uncertainties as well as nonlinearities plays a major role. For instance, the design of unmanned aircraft, unmanned underwater vehicles, and automatic driving systems for automobiles are all typical examples of such difficult control problems. The large uncertainties concerning the plant may arise due to large external disturbances, large parameter variations because of faults in the system, or failure of some of the subsystems. In such cases, the controller has to determine the specific situation that exists at any instant, and take the appropriate control action. Accomplishing this rapidly, accurately, and in a stable fashion is the objective of control design.
基金Sponsored by the National Natural Science Foundation of China(Grant No.6137110061001093+6 种基金61401118)the Natural Science Foundation of Shandong Province(Grant No.ZR2014FP016)the Natural Scientific Research Innovation Foundation in Harbin Institute of Technology(Grant No.HIT.NSRIF.2011114HIT.NSRIF.2013136HIT.NSRIF.2016100)the Scientific Research Foundation of Harbin Institute of Technology at Weihai(Grant No.HIT(WH)201409HIT(WH)201410)
文摘To evaluate transmission rate of highly dynamic space networks,a new method for studying space network capacity is proposed in this paper. Using graph theory,network capacity is defined as the maximum amount of flows ground stations can receive per unit time. Combined with a hybrid constellation model,network capacity is calculated and further analyzed for practical cases. Simulation results show that network capacity will increase to different extents as link capacity,minimum ground elevation constraint and satellite onboard processing capability change. Considering the efficiency and reliability of communication networks,how to scientifically design satellite networks is also discussed.
基金supported by the Fundamental Research Funds for the Central Universities(No.2010LKWL03)the Special Fund for Theoretical Physics(No.11047130)the National Natural Science Foundation of China(No.11104345)
文摘The electronic properties of zinc-blende BxGal-xN alloys are comparatively investigated by employ- ing both the Perdewe-Burkee-Ernzerhof generalized-gradient approximation (PBE-GGA) and the Heyd-Scuseria- Ernzerhof screened hybrid functional methods (HSE06). HSE06 reproduced much closer ground-state properties to experiments. Large and composition-dependent bowing parameters br for the direct band gaps were obtained from both PBE and HSE06. The crossover composition where alloy switches from direct to indirect was predicted to occur at very similar x from PBE and HSE06. We can obtain direct gap BxGal-xN with a gap value much larger than that of GaN by alloying x 〈 0.557 boron into GaN.
基金supported by the Fundamental Research Funds for the Central Universities(Grant No.2013121005)the National Natural Science Foundation of China(Grant Nos.11474237 and 11574310)+1 种基金the 111 Project (Grant No.B16029)the National Research Foundation of Singapore through the NRF Investigatorship and the Mechanobiology Institute
文摘Deoxyribonucleic acid(DNA) carries the genetic information in all living organisms. It consists of two interwound single-stranded(ss) strands, forming a double-stranded(ds) DNA with a right-handed double-helical conformation. The two strands are held together by highly specific basepairing interactions and are further stabilized by stacking between adjacent basepairs. A transition from a dsDNA to two separated ssDNA is called melting and the reverse transition is called hybridization. Applying a tensile force to a dsDNA can result in a particular type of DNA melting, during which one ssDNA strand is peeled away from the other. In this work, we studied the kinetics of strand-peeling and hybridization of short DNA under tensile forces. Our results show that the force-dependent strand-peeling and hybridization can be described with a simple two-state model. Importantly, detailed analysis of the force-dependent transition rates revealed that the transition state consists of several basepairs dsDNA.
基金supported by the National Natural Science Foundation of China (Grant No. 51078019)the National Basic Research Program of China ("973" Program) (Grant No. 2010CB732100)Beijing Munici-pal Natural Science Foundation (Grant No. 8112024)
文摘A nonlinear multi-field coupled model for multi-constituent three-phase soils is derived by using the hybrid mixture theory. The balance equations with three levels (constituents, phases and the whole mixture soil) are set up under the assumption that soil is composed of multi-constituent elastic-plastic solid skeleton (which is different from the linearization method) and viscous liquid and ideal gas. With reasonable constitutive assumptions in such restrictive conditions as the principles of determinism, equipresence, material frame-indifference and the compatible principle in continuum mechanics, a theoretical framework of constitutive relations modeling three-phase soil in both non-equilibrium and equilibrium states is established, thus the closed field equations are formed. In the theoretical framework, the concept of effective generalized thermodynamic forces is introduced, and the nonlinear coupling constitutive relations between generalized dissipation forces and generalized flows within the system at nonequilibrium state are also presented. On such a basis, four special coupling relations, i.e., solid thermal elastic-plastic constitutive relation, liquid visco-elastic-plastic constitutive relation, the generalized Fourier’s law, and the generalized Darcy’s law are put forward. The generalized or nonlinear results mentioned above can degenerate into the linear coupling results given by Bennethum and Singh. Based on a specific dissipation function, the concrete form of generalized Darcy’s law is deduced, which may degenerate into the traditional form of Darcy’s law by neglecting the influence of skeleton deformation and temperature. Without considering temperature and other coupling effects, the nonlinear coupled model in this paper can degenerate into a soil elastic-plastic constitutive model.
基金supported by the Ministry of Science and Technology(MOST)of China(Nos.2012CB932704,2012CB933001)the National Natural Science Foundation of China(NSFC,Nos.11274380,91433103,21173058,11622437,61674171 and 21203038)supported by the Outstanding Innovative Talents Cultivation Funded Programs 2015 of Renmin University of China
文摘It has been demonstrated that intermolecular interaction,crucial in a plenty of chemical and physical processes,may vary in the presence of metal surface.However,such modification is yet to be quantitatively revealed.Here,we present a systematical density functional theory study on adsorbed bis(para-pyridyl)acetylene(BPPA) tetramer on Au(111) surface.We observed unusually high electron density between two head-to-head N atoms,an intermolecular "non-bonded" region,in adsorbed BPPA tetramer.This exceptional electron density originates from the wavefunction hybridization of the two compressed N lone-electron-pair states of two BPPA,as squeezed by a newly revealed N-Au-N threecenter bonding.This bond,together with the minor contribution from N...H-C intermolecular hydrogen bonding,shortens the N-N distance from over 4 A to 3.30 A and offers an attractive lateral interacting energy of 0.60 eV,effectively to a surface-confined in-plane pressure.The overlapped non-bonding vvavefunction hybridization arising from the effective pressure induced by the N-Au-N three-center bonding,as not been fully recognized in earlier studies,was manifested in non-contact Atomic Force Microscopy.
基金supported by the National Basic Research Program of China (Grant No. 2013CB632101)the National Natural Science Foundation of China (Grant Nos. 61222404 and 61474097)the Program of the Ministry of Education of China for Innovative Research Teams in Universities (Grant No. IRT13R54)
文摘The formation, structural and electronic properties of silicene oxides(SOs) that result from the oxidation of silicene on Ag(111) surface have been investigated in the framework of density functional theory(DFT).It is found that the honeycomb lattice of silicene on the Ag(111) surface changes after the oxidation. SOs are strongly hybridized with the Ag(111) surface so that they possess metallic band structures. Charge accumulation between SOs and the Ag(111) surface indicates strong chemical bonding, which dramatically affects the electronic properties of SOs. When SOs are peeled off the Ag(111) surface, however, they may become semiconductors.