We propose a novel analytical model to describe the drain-source current as well as gate-source of single-electron transistors (SETs) at high temperature. Our model consists on summing the tunnel current and thermioni...We propose a novel analytical model to describe the drain-source current as well as gate-source of single-electron transistors (SETs) at high temperature. Our model consists on summing the tunnel current and thermionic contribution. This model will be compared with another model.展开更多
The characteristics and structures of single-electron halogen bond complexes H3C…Br-Y(Y = H,CCH,CN,NC,C2H3) have been investigated by theoretical calculation methods.The geometries were optimized and frequencies calc...The characteristics and structures of single-electron halogen bond complexes H3C…Br-Y(Y = H,CCH,CN,NC,C2H3) have been investigated by theoretical calculation methods.The geometries were optimized and frequencies calculated at the B3LYP/6-311++G level.The interaction energies were corrected for basis set superposition error(BSSE) and the wavefunctions obtained by the natural bond orbital(NBO) and atom in molecule(AIM) analyses at the MP2/6-311++G level.For each H3C…Br-Y complex,a single-electron Br bond is formed between the unpaired electron of the CH3(electron donor) radical and the Br atom of Br-Y(electron acceptor);this kind of single-electron bromine bond also possesses the character of a"three-electron bond".Due to the formation of the single-electron Br bond,the C-H bonds of the CH3 radical bend away from the Br-Y moiety and the Br-Y bond elongates,giving red-shifted single-electron Br bond complexes.The effects of substituents,hybridization of the carbon atom,and solvent on the properties of the complexes have been investigated.The strengths of single-electron hydrogen bonds,single-electron halogen bonds and single-electron lithium bonds have been compared.In addition,the single-electron halogen bond system is discussed in the light of the first three criteria for hydrogen bonding proposed by Popelier.展开更多
Alloying is an important strategy in tailoring the functionality of materials.In metal nanoclusters(NCs),the introduction of a heterometal leads to alloy nanoclusters that often outperform the homometal ones in terms ...Alloying is an important strategy in tailoring the functionality of materials.In metal nanoclusters(NCs),the introduction of a heterometal leads to alloy nanoclusters that often outperform the homometal ones in terms of the physical and chemical properties.In this work,a series of four M_(144)(PET)60 alloy NCs(where,M=Au/Ag,PET=–SCH_(2)CH_(2)Ph)are synthesized and characterized.The silver doping into the homogold template(Au_(144))leads to more prominent optical absorption features in the steady-state spectrum in the visible range.Femtosecond transient absorption spectroscopy reveals the effect of Ag doping on the electronic relaxation dynamics compared to Au_(144)and the pump fluence independent dynamics.Electrochemical results reflect a narrowing of HOMO–LUMO gap(E_(g))induced by Ag doping.A temperature dependence of the single-electron charging is also observed for the series of alloy NCs,in which the E_(g)values of the alloy NCs enlarge as the temperature decreases,which is characteristic of semiconducting behavior.展开更多
The efficient Cu(0) wire-catalyzed single-electron transfer-living radical polymerization (SET-LRP) in organic solvents and mixtures of the organic solvents with water has been thoroughly investigated. 01igo(ethylene ...The efficient Cu(0) wire-catalyzed single-electron transfer-living radical polymerization (SET-LRP) in organic solvents and mixtures of the organic solvents with water has been thoroughly investigated. 01igo(ethylene oxide) methyl ether acrylate was used as an exemplar oligomer monomer to determine the optimum polymerization conditions for rapid, controlled, and quantitative production of well-defined polymers. The effects of Cu(0)-wire length (12.5 or 4.5 cm), ligand type (tris(dimethylaminoethyl)amine, Me6-TREN, or tris(2-aminoethyl)amine, TREN), and solvent type (dipolar aprotic solvents, cyclic ethers, alcohol, or acetone) on the polymerization have been evaluated. Kinetic experiments were performed for all polymerizations to assess the "living" behavior of each system employed. Importantly, TREN could be used as a replacement for Me6-TREN in Cu(0) wire-catalyzed SET-LRP of oligomer monomer, which probably provides the most economical and efficient methodology since TREN is 80 times less expensive than Me6-TREN. The high chain-end fidelity of resulting polymer was experimentally verified by thiol-Michael addition reaction at the a-Br chain end and subsequent chain extension with methyl acrylate.展开更多
Single-electron oxidation of a diiron-sulfur complex [Cpπ*Fe(μ-bdt)FeCp^*] (1, Cp^*=η^5-C5Me5; bdt = benzene-1,2-dithiolate) to [Cp^*Fe(μ-bdt)FeCp^*]]^+ (2) has been experimentally conducted. The bdt...Single-electron oxidation of a diiron-sulfur complex [Cpπ*Fe(μ-bdt)FeCp^*] (1, Cp^*=η^5-C5Me5; bdt = benzene-1,2-dithiolate) to [Cp^*Fe(μ-bdt)FeCp^*]]^+ (2) has been experimentally conducted. The bdt ligand with redoxactive character has been computationally proposed to be a dianion (bdt62-) rather than previously proposed monoanion (bdt^-) radical in 1 though it has un-equidistant aromatic C-C bond lengths. The ground state of 1 is predicted to be two low-spin ferrous ions (SFe= 0) and 2 has a medium-spin ferric ion (SFe= 1/2) and a low-spin ferrous center (SFe=0), and the oxidation of 1 to 2 is calculated to be a single-metal-based process. Both complexes have no significant antiferromagnetic coupling character.展开更多
Diluted magnetic semiconductors(DMSs)have traditionally been employed to implement spin-based quantum computing and quantum information processing.However,their low Curie temperature is a major hurdle in their use in ...Diluted magnetic semiconductors(DMSs)have traditionally been employed to implement spin-based quantum computing and quantum information processing.However,their low Curie temperature is a major hurdle in their use in this field,which creates the necessity for wide bandgap DMSs operating at room temperature.In view of this,a single-electron transistor(SET)with a global back-gate was built using a wide bandgap ZnO nanobelt(NB).Clear Coulomb oscillations were observed at 4.2 K.The periodicity of the Coulomb diamonds indicates that the Coulomb oscillations arise from single quantum dots of uniform size,whereas quasi-periodic Coulomb diamonds correspond to the contribution of multi-dots present in the ZnO NB.By applying an AC signal to the global back-gate across a Coulomb peak with varying frequencies,single-electron pumping was observed;the increase in current was equal to the production of electron charge and frequency.The current accuracy of about 1%for both single-and double-electron pumping was achieved at a high frequency of 25 MHz.This accurate single-electron pumping makes the ZnO NB SET suitable for single-spin injection and detection,which has great potential for applications in quantum information technology.展开更多
The single electron local kinetic energy is rigorously defined and explained based on Schrdinger equation for an electronic system. Its uniqueness and asymptotic behavior are demonstrated through two theorems, there...The single electron local kinetic energy is rigorously defined and explained based on Schrdinger equation for an electronic system. Its uniqueness and asymptotic behavior are demonstrated through two theorems, thereby clarifying the problem of arbitrary choice of the kinetic energy functional in density functional theory. The adequate models of the kinetic energy functional that satisfy the condition are suggested.展开更多
Using the Keldysh nonequilibrium Green function and equation-of-motion technique, we have qualitatively studied the spin-dependent transport of a triple-QD system in the Kondo regime. It is shown that the Kondo resona...Using the Keldysh nonequilibrium Green function and equation-of-motion technique, we have qualitatively studied the spin-dependent transport of a triple-QD system in the Kondo regime. It is shown that the Kondo resonance and Fang interference coexist, and in this system the Fang Kondo effect shows dip behaviours richer than that in the T-shaped QDs. The interdot coupling, the energy level of the side coupled QDs and the spin polarization strength greatly influence the DOS of the central quantum dot QDo. Either the increase of the coupling strength between the two QDs or that of the energy levels of the side coupled QDs enhances the Kondo resonance. Especially, the Kondo resonance is strengthened greatly when the side dot energy is fixed at the Fermi energy. Meanwhile, the Kondo resonance splits for the spin-up and spin-down configurations due to the polarization: the down-spin resonance is enhanced, and the up-spin resonance is suppressed.展开更多
Taking account of the electron--electron (hole) and electron--hole interactions, the tunneling processes of the main quantum dot (QD) Coulomb-coupled with a second quantum dot embedded in n--n junction have been i...Taking account of the electron--electron (hole) and electron--hole interactions, the tunneling processes of the main quantum dot (QD) Coulomb-coupled with a second quantum dot embedded in n--n junction have been investigated. The eighteen resonance mechanisms involved in the tunneling processes of the system have been identified. It is found that the tunneling current depends sensitively on the electron occupation number in the second quantum dot. When the electron occupation number in the second dot is tiny, both the tunneling current peaks and the occupation number plateaus in the main QD are determined by the intra-resonance mechanism. The increase of the electron occupation number in the second dot makes the inter-resonance mechanism participate in the transport processes. The competition between the inter and intra resonance mechanisms persists until the electron occupation number in the second dot reaches around unity, leading to the consequence that the inter-resonance mechanisms completely dominate the tunneling processes.展开更多
A single-molecule magnet (SMM) coupled to two normal metallic electrodes can both switch spin-up and spin- down electronic currents within two different windows of SMM gate voltage. Such spin current switching in th...A single-molecule magnet (SMM) coupled to two normal metallic electrodes can both switch spin-up and spin- down electronic currents within two different windows of SMM gate voltage. Such spin current switching in the SMM tunnel junction arises from spin-selected single electron resonant tunneling via the lowest unoccupied molecular orbit of the SMM. Since it is not magnetically controlled but all-electrically controlled, the proposed spin current switching effect may have potential applications in future spintronics.展开更多
We theoretically investigate properties of the ground state of a closed dot-ring system with a magnetic flux in the Kondo regime by means of a tight-banding Anderson Hamiltonian, using the Slave-Boson mean-field appro...We theoretically investigate properties of the ground state of a closed dot-ring system with a magnetic flux in the Kondo regime by means of a tight-banding Anderson Hamiltonian, using the Slave-Boson mean-field approach. The persistent current shows interesting dependences on the parity and on the size of the system. The signature of Kondo resonance at ζk/L = 0.15 is expected to be observed experimentally in the future. With the intensity of the coupling tD changes from weak to strong, the properties of the system changes largely, which are different from the in-line one because of the attached dot.展开更多
This paper presents a basic block for building large-scale single-electron neural networks. This macro block is completely composed of SET inverter circuits. We present and discuss the basic parts of this device. The ...This paper presents a basic block for building large-scale single-electron neural networks. This macro block is completely composed of SET inverter circuits. We present and discuss the basic parts of this device. The full design and simulation results were done using MATLAB and SIMON, which are a single-electron tunnel device and circuit simulator based on a Monte Carlo method. Special measures had to be taken in order to simulate this circuit correctly in SIMON and compare results with those of SPICE simulation done before. Moreover, we study part of the network as a memory cell with the idea of combining the extremely low-power properties of the SET and the compact design.展开更多
The quantum harmonic oscillator(QHO),one of the most important and ubiquitous model systems in quantum mechanics,features equally spaced energy levels or eigenstates.Here we present a new class of nearly ideal QHOs fo...The quantum harmonic oscillator(QHO),one of the most important and ubiquitous model systems in quantum mechanics,features equally spaced energy levels or eigenstates.Here we present a new class of nearly ideal QHOs formed by hydrogenic substitutional dopants in an AlGaAs/GaAs heterostructure.On the basis of model calculations,we demonstrate that,when aδ-doping Si donor substitutes the Ga/Al lattice site close to AlGaAs/GaAs heterointerface,a hydrogenic Si QHO,characterized by a restoring Coulomb force producing square law harmonic potential,is formed.This gives rise to QHO states with energy spacing of~8–9 meV.We experimentally confirm this proposal by utilizing gate tuning and measuring QHO states using an aluminum single-electron transistor(SET).A sharp and fast oscillation with period of~7–8 mV appears in addition to the regular Coulomb blockade(CB)oscillation with much larger period,for positive gate biases above 0.5 V.The observation of fast oscillation and its behavior is quantitatively consistent with our theoretical result,manifesting the harmonic motion of electrons from the QHO.Our results might establish a general principle to design,construct and manipulate QHOs in semiconductor heterostructures,opening future possibilities for their quantum applications.展开更多
An example of iron-catalyzed cross-electrophile couplingof inert C-O bonds with alkyl bromides via aniron/B_(2)pin_(2) catalytic system has been developed.Aryl and heteroaryl carbamates can smoothly undergothis transf...An example of iron-catalyzed cross-electrophile couplingof inert C-O bonds with alkyl bromides via aniron/B_(2)pin_(2) catalytic system has been developed.Aryl and heteroaryl carbamates can smoothly undergothis transformation under mild conditions, deliveringthe alkylated products with good efficiency.This protocol exhibits good functional group compatibilityand enables the late-stage functionalizationof biorelevant compounds, thus providingexcellent opportunities for applications in medicinalchemistry. Control experiments and computationalstudies reveal that a high spin Fe(I/II/III) catalyticmechanism might be involved in this reactionthrough single electron transfer to activate alkylbromides, oxidative addition of aryl carbamates, andreductive elimination to form Csp^(2)-Csp^(3) bonds.展开更多
Metal-free anti-Markovnikov hydroalkylation of unactivated alkenes with cyanoacetate has been developed,featuring the use of a dual-component initiator containing an organic photocatalyst and a radical precursor.When ...Metal-free anti-Markovnikov hydroalkylation of unactivated alkenes with cyanoacetate has been developed,featuring the use of a dual-component initiator containing an organic photocatalyst and a radical precursor.When combined,the two components can undergo visible light-induced singleelectron transfer,and serve as a versatile and effective alkyl radical generator.展开更多
Water radical cations,the crucial intermediates in many aqueous reactions and biochemical processes,are difficult to investigate experimentally due to their short lifetime andlowabundance.Herein,ahomemade device based...Water radical cations,the crucial intermediates in many aqueous reactions and biochemical processes,are difficult to investigate experimentally due to their short lifetime andlowabundance.Herein,ahomemade device based on energy-tunable discharge was employed to deposit suitable amounts of energy to atmospheric pressure pure water vapor for abundant production of water radical cations,stabilized as(H_(2)O)n^(+·)(n=2-5)with a maximal abundance of≥8.3×10^(6) cps for(H_(2)O)_(2)^(+·),characterized by mass spectrometry(MS).The abundance of water radical cations was optimized by adjusting the experimental parameters such as the discharge voltage(2.5 kV),temperature of the MS inlet(140℃),carrier gas flow(20mL/min),and the distance between the discharge tip and MS inlet(12 mm).The ambient formation of water radical cationswas further confirmedby thehigh reactivity of as-prepared water radical cations,which reacted with benzene,ethyl acetate,and dimethyl disulfide instantly,showing rich chemistry with ionic and radical characteristics.Moreover,the computations usingCCSD(T)//MP2 method and density functional theory confirmed that the O-O single-electron bound dimer(B),as well as the hydronium hydroxyl radical complex(A),accounted for the unusual chemistry of the water radical cations,providing a facile approach to access the high reactivity ofwater radical cations under the ambient conditions.展开更多
Higher-order topological phase in 2-dimensional(2D)systems is characterized by in-gap corner states,which are hard to detect and utilize.We numerically investigate transport properties of topological corner states in ...Higher-order topological phase in 2-dimensional(2D)systems is characterized by in-gap corner states,which are hard to detect and utilize.We numerically investigate transport properties of topological corner states in 2D honeycomb lattice,where the second-order topological phase is induced by an in-plane Zeeman field in the conventional Kane–Mele model.Through engineering multihollow structures with appropriate boundaries in honeycomb lattice,multiple corner states emerge,which greatly increases the probability to observe them.A typical two-probe setup is built to study the transport features of a diamond-shaped system with multihollow structures.Numerical results reveal the existence of global resonant states in bulk insulator,which corresponds to the resonant tunneling of multiple corner states and occupies the entire scattering region.Furthermore,based on the well separated energy levels of multiple corner states,a single-electron source is constructed.展开更多
Dispersity(D)of polymers has a great effect on the properties of polymeric materials,and therefore how to control θ is very important but still a huge challenge in polymer synthesis,especially for reversible-deactiva...Dispersity(D)of polymers has a great effect on the properties of polymeric materials,and therefore how to control θ is very important but still a huge challenge in polymer synthesis,especially for reversible-deactivation radical polymerization(RDRP)strategy.Herein,we successfully developed a novel strategy to adjust D of polymers by visible light-controlled reversible complexation mediated living radical polymerizatio n(RCMP)and combi nation of single-electron transfer-degenerative chain tran sfer living radical polymerization(SET-DTLRP)at room temperature.In RCMP system,2-iodo-2-methylpropionitrile(CP-I)and ethyl 2-iodo-2-phenylacetate(EIPA)were used as alkyl iodide initiators,by using methyl methacrylate(MMA)as the model monomer and n-butylacrylate(BA)as the end-capping reagent to regulate D of polymers.Subsequently,we successfully prepared the block copolymer PMMA-b-PBA with adjustable D by reactivating the polymer end-chains via SET-DTLRP in the presence of copper wire,fully dem on strati ng that it is a promising strategy that can keep the"living"feature of polymers while regulating their molar mass dispersities easily.展开更多
文摘We propose a novel analytical model to describe the drain-source current as well as gate-source of single-electron transistors (SETs) at high temperature. Our model consists on summing the tunnel current and thermionic contribution. This model will be compared with another model.
基金supported by the Foundation of the Education Committee of Gansu Province (Grant No. 0708-11)"Qinglan" Talent Engineering Funds of Tianshui Normal University
文摘The characteristics and structures of single-electron halogen bond complexes H3C…Br-Y(Y = H,CCH,CN,NC,C2H3) have been investigated by theoretical calculation methods.The geometries were optimized and frequencies calculated at the B3LYP/6-311++G level.The interaction energies were corrected for basis set superposition error(BSSE) and the wavefunctions obtained by the natural bond orbital(NBO) and atom in molecule(AIM) analyses at the MP2/6-311++G level.For each H3C…Br-Y complex,a single-electron Br bond is formed between the unpaired electron of the CH3(electron donor) radical and the Br atom of Br-Y(electron acceptor);this kind of single-electron bromine bond also possesses the character of a"three-electron bond".Due to the formation of the single-electron Br bond,the C-H bonds of the CH3 radical bend away from the Br-Y moiety and the Br-Y bond elongates,giving red-shifted single-electron Br bond complexes.The effects of substituents,hybridization of the carbon atom,and solvent on the properties of the complexes have been investigated.The strengths of single-electron hydrogen bonds,single-electron halogen bonds and single-electron lithium bonds have been compared.In addition,the single-electron halogen bond system is discussed in the light of the first three criteria for hydrogen bonding proposed by Popelier.
基金R.J.thanks the financial support from the National Science Foundation(No.DMR-1808675)G.W.acknowledges the funding support from National Science Foundation PAPID CHE(No.2034498)H.W.thanks the financial support from,the Air Force Office of Scientific Research(AFOSR)Nos.(FA9550-17-1-0099 and sFA9550-21-1-0192).
文摘Alloying is an important strategy in tailoring the functionality of materials.In metal nanoclusters(NCs),the introduction of a heterometal leads to alloy nanoclusters that often outperform the homometal ones in terms of the physical and chemical properties.In this work,a series of four M_(144)(PET)60 alloy NCs(where,M=Au/Ag,PET=–SCH_(2)CH_(2)Ph)are synthesized and characterized.The silver doping into the homogold template(Au_(144))leads to more prominent optical absorption features in the steady-state spectrum in the visible range.Femtosecond transient absorption spectroscopy reveals the effect of Ag doping on the electronic relaxation dynamics compared to Au_(144)and the pump fluence independent dynamics.Electrochemical results reflect a narrowing of HOMO–LUMO gap(E_(g))induced by Ag doping.A temperature dependence of the single-electron charging is also observed for the series of alloy NCs,in which the E_(g)values of the alloy NCs enlarge as the temperature decreases,which is characteristic of semiconducting behavior.
基金financially supported by the National Natural Science Foundation of China (Nos. 21774107, 21774029, and 21801217)the Natural Science Foundation of Jiangsu ProvinceGeneral Program (No. BK20171273)+2 种基金"Six Talent Peak" High-level Talent Project (JNHB-068)Qing Lan Project of Jiangsu Provincethe Initial Scientific Research Foundation of Yancheng Institute of Technology (No. KJC2014002)
文摘The efficient Cu(0) wire-catalyzed single-electron transfer-living radical polymerization (SET-LRP) in organic solvents and mixtures of the organic solvents with water has been thoroughly investigated. 01igo(ethylene oxide) methyl ether acrylate was used as an exemplar oligomer monomer to determine the optimum polymerization conditions for rapid, controlled, and quantitative production of well-defined polymers. The effects of Cu(0)-wire length (12.5 or 4.5 cm), ligand type (tris(dimethylaminoethyl)amine, Me6-TREN, or tris(2-aminoethyl)amine, TREN), and solvent type (dipolar aprotic solvents, cyclic ethers, alcohol, or acetone) on the polymerization have been evaluated. Kinetic experiments were performed for all polymerizations to assess the "living" behavior of each system employed. Importantly, TREN could be used as a replacement for Me6-TREN in Cu(0) wire-catalyzed SET-LRP of oligomer monomer, which probably provides the most economical and efficient methodology since TREN is 80 times less expensive than Me6-TREN. The high chain-end fidelity of resulting polymer was experimentally verified by thiol-Michael addition reaction at the a-Br chain end and subsequent chain extension with methyl acrylate.
基金This work was partly supported by the National Natural Science Foundation of China (Nos. 21429201, 21231003, 21571026). The authors also thank the Network and Information Center of the Dalian University of Technology for part of the computational resources.
文摘Single-electron oxidation of a diiron-sulfur complex [Cpπ*Fe(μ-bdt)FeCp^*] (1, Cp^*=η^5-C5Me5; bdt = benzene-1,2-dithiolate) to [Cp^*Fe(μ-bdt)FeCp^*]]^+ (2) has been experimentally conducted. The bdt ligand with redoxactive character has been computationally proposed to be a dianion (bdt62-) rather than previously proposed monoanion (bdt^-) radical in 1 though it has un-equidistant aromatic C-C bond lengths. The ground state of 1 is predicted to be two low-spin ferrous ions (SFe= 0) and 2 has a medium-spin ferric ion (SFe= 1/2) and a low-spin ferrous center (SFe=0), and the oxidation of 1 to 2 is calculated to be a single-metal-based process. Both complexes have no significant antiferromagnetic coupling character.
基金supported by the National Natural Science Foundation of China(Grant Nos.51761145104,11934019,61675228,11721404,and 11874419)the Strategic Priority Research Program,the Instrument Developing Project and the Interdisciplinary Innovation Team of the Chinese Academy of Sciences(Grant Nos.XDB28000000,and YJKYYQ20180036)the Key R&D Program of Guangdong Province(Grant No.2018B030329001).
文摘Diluted magnetic semiconductors(DMSs)have traditionally been employed to implement spin-based quantum computing and quantum information processing.However,their low Curie temperature is a major hurdle in their use in this field,which creates the necessity for wide bandgap DMSs operating at room temperature.In view of this,a single-electron transistor(SET)with a global back-gate was built using a wide bandgap ZnO nanobelt(NB).Clear Coulomb oscillations were observed at 4.2 K.The periodicity of the Coulomb diamonds indicates that the Coulomb oscillations arise from single quantum dots of uniform size,whereas quasi-periodic Coulomb diamonds correspond to the contribution of multi-dots present in the ZnO NB.By applying an AC signal to the global back-gate across a Coulomb peak with varying frequencies,single-electron pumping was observed;the increase in current was equal to the production of electron charge and frequency.The current accuracy of about 1%for both single-and double-electron pumping was achieved at a high frequency of 25 MHz.This accurate single-electron pumping makes the ZnO NB SET suitable for single-spin injection and detection,which has great potential for applications in quantum information technology.
文摘The single electron local kinetic energy is rigorously defined and explained based on Schrdinger equation for an electronic system. Its uniqueness and asymptotic behavior are demonstrated through two theorems, thereby clarifying the problem of arbitrary choice of the kinetic energy functional in density functional theory. The adequate models of the kinetic energy functional that satisfy the condition are suggested.
文摘Using the Keldysh nonequilibrium Green function and equation-of-motion technique, we have qualitatively studied the spin-dependent transport of a triple-QD system in the Kondo regime. It is shown that the Kondo resonance and Fang interference coexist, and in this system the Fang Kondo effect shows dip behaviours richer than that in the T-shaped QDs. The interdot coupling, the energy level of the side coupled QDs and the spin polarization strength greatly influence the DOS of the central quantum dot QDo. Either the increase of the coupling strength between the two QDs or that of the energy levels of the side coupled QDs enhances the Kondo resonance. Especially, the Kondo resonance is strengthened greatly when the side dot energy is fixed at the Fermi energy. Meanwhile, the Kondo resonance splits for the spin-up and spin-down configurations due to the polarization: the down-spin resonance is enhanced, and the up-spin resonance is suppressed.
基金supported by the National Natural Science Foundation of China (Grant No. 60776062)the National Fundamental Fund of Personnel Training (Grant No. J0730317)the Natural Science Foundation of Shanxi Province, China (Grant Nos.2008011001-1 and 2008011001-2)
文摘Taking account of the electron--electron (hole) and electron--hole interactions, the tunneling processes of the main quantum dot (QD) Coulomb-coupled with a second quantum dot embedded in n--n junction have been investigated. The eighteen resonance mechanisms involved in the tunneling processes of the system have been identified. It is found that the tunneling current depends sensitively on the electron occupation number in the second quantum dot. When the electron occupation number in the second dot is tiny, both the tunneling current peaks and the occupation number plateaus in the main QD are determined by the intra-resonance mechanism. The increase of the electron occupation number in the second dot makes the inter-resonance mechanism participate in the transport processes. The competition between the inter and intra resonance mechanisms persists until the electron occupation number in the second dot reaches around unity, leading to the consequence that the inter-resonance mechanisms completely dominate the tunneling processes.
基金supported by the National Natural Science Foundation of China (Grant Nos. 60825402,60421003,11074111 and 10974058)the State Key Program for Basic Research of China (Grant Nos. 2011CB922103,2009CB929504 and 2011CBA00205)
文摘A single-molecule magnet (SMM) coupled to two normal metallic electrodes can both switch spin-up and spin- down electronic currents within two different windows of SMM gate voltage. Such spin current switching in the SMM tunnel junction arises from spin-selected single electron resonant tunneling via the lowest unoccupied molecular orbit of the SMM. Since it is not magnetically controlled but all-electrically controlled, the proposed spin current switching effect may have potential applications in future spintronics.
文摘We theoretically investigate properties of the ground state of a closed dot-ring system with a magnetic flux in the Kondo regime by means of a tight-banding Anderson Hamiltonian, using the Slave-Boson mean-field approach. The persistent current shows interesting dependences on the parity and on the size of the system. The signature of Kondo resonance at ζk/L = 0.15 is expected to be observed experimentally in the future. With the intensity of the coupling tD changes from weak to strong, the properties of the system changes largely, which are different from the in-line one because of the attached dot.
文摘This paper presents a basic block for building large-scale single-electron neural networks. This macro block is completely composed of SET inverter circuits. We present and discuss the basic parts of this device. The full design and simulation results were done using MATLAB and SIMON, which are a single-electron tunnel device and circuit simulator based on a Monte Carlo method. Special measures had to be taken in order to simulate this circuit correctly in SIMON and compare results with those of SPICE simulation done before. Moreover, we study part of the network as a memory cell with the idea of combining the extremely low-power properties of the SET and the compact design.
基金Profs.Y.Zhang,J.Chen,J.Zhao,and C.Lin are greatly appreciated.M.Feng thanks financial support from the National Key R&D Program of China(Grant No.2018YFA0305802)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XD30000000)+1 种基金the National Natural Science Foundation of China(Grant Nos.11574364 and 11774267)L.Mao thanks financial support from the National Key R&D Program of China by the Ministry of Science and Technology of China(Grant No.2015C8932400).
文摘The quantum harmonic oscillator(QHO),one of the most important and ubiquitous model systems in quantum mechanics,features equally spaced energy levels or eigenstates.Here we present a new class of nearly ideal QHOs formed by hydrogenic substitutional dopants in an AlGaAs/GaAs heterostructure.On the basis of model calculations,we demonstrate that,when aδ-doping Si donor substitutes the Ga/Al lattice site close to AlGaAs/GaAs heterointerface,a hydrogenic Si QHO,characterized by a restoring Coulomb force producing square law harmonic potential,is formed.This gives rise to QHO states with energy spacing of~8–9 meV.We experimentally confirm this proposal by utilizing gate tuning and measuring QHO states using an aluminum single-electron transistor(SET).A sharp and fast oscillation with period of~7–8 mV appears in addition to the regular Coulomb blockade(CB)oscillation with much larger period,for positive gate biases above 0.5 V.The observation of fast oscillation and its behavior is quantitatively consistent with our theoretical result,manifesting the harmonic motion of electrons from the QHO.Our results might establish a general principle to design,construct and manipulate QHOs in semiconductor heterostructures,opening future possibilities for their quantum applications.
基金We thank the National Key Research and Development Program of China(grant no.2021YFA1500100)National Natural Science Foundation of China(grant nos.92156017 and 21890722)+3 种基金Natural Science Foundation of Sichuan(grant no.2021YJ0413)the Natural Science Foundation of Tianjin Municipality(grant no.19JCJQJC62300)Chongqing Postdoctoral Science Foundation(grant no.cstc2020jcyj-bshX0052)Affiliated Hospital of North Sichuan Medical College(grant no.2022JB001)for financial support.
文摘An example of iron-catalyzed cross-electrophile couplingof inert C-O bonds with alkyl bromides via aniron/B_(2)pin_(2) catalytic system has been developed.Aryl and heteroaryl carbamates can smoothly undergothis transformation under mild conditions, deliveringthe alkylated products with good efficiency.This protocol exhibits good functional group compatibilityand enables the late-stage functionalizationof biorelevant compounds, thus providingexcellent opportunities for applications in medicinalchemistry. Control experiments and computationalstudies reveal that a high spin Fe(I/II/III) catalyticmechanism might be involved in this reactionthrough single electron transfer to activate alkylbromides, oxidative addition of aryl carbamates, andreductive elimination to form Csp^(2)-Csp^(3) bonds.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDB17000000)the National Natural Science Foundation of China (Nos.21672227, 21922113)+3 种基金the National Key Research and Development Program of China (No.2017YFA0206903)Beijing Natural Science Foundation (No.L182020)Fundamental Research Funds for the Central Universities (No.FRF-TP-19-013B1)K.C.Wong Education Foundation,and the TIPC Director’s Fund。
文摘Metal-free anti-Markovnikov hydroalkylation of unactivated alkenes with cyanoacetate has been developed,featuring the use of a dual-component initiator containing an organic photocatalyst and a radical precursor.When combined,the two components can undergo visible light-induced singleelectron transfer,and serve as a versatile and effective alkyl radical generator.
基金supported by a grant from the National Natural Science Foundation of China(grant no.215201-02007)the US National Science Foundation(grant no.1905087).
文摘Water radical cations,the crucial intermediates in many aqueous reactions and biochemical processes,are difficult to investigate experimentally due to their short lifetime andlowabundance.Herein,ahomemade device based on energy-tunable discharge was employed to deposit suitable amounts of energy to atmospheric pressure pure water vapor for abundant production of water radical cations,stabilized as(H_(2)O)n^(+·)(n=2-5)with a maximal abundance of≥8.3×10^(6) cps for(H_(2)O)_(2)^(+·),characterized by mass spectrometry(MS).The abundance of water radical cations was optimized by adjusting the experimental parameters such as the discharge voltage(2.5 kV),temperature of the MS inlet(140℃),carrier gas flow(20mL/min),and the distance between the discharge tip and MS inlet(12 mm).The ambient formation of water radical cationswas further confirmedby thehigh reactivity of as-prepared water radical cations,which reacted with benzene,ethyl acetate,and dimethyl disulfide instantly,showing rich chemistry with ionic and radical characteristics.Moreover,the computations usingCCSD(T)//MP2 method and density functional theory confirmed that the O-O single-electron bound dimer(B),as well as the hydronium hydroxyl radical complex(A),accounted for the unusual chemistry of the water radical cations,providing a facile approach to access the high reactivity ofwater radical cations under the ambient conditions.
基金supported by the National Natural Science Foundation of China(Grant Nos.12174262 and 11774238)the Natural Science Foundation of Guangdong(Grant No.2020A1515011418)the Natural Science Foundation of Shenzhen(Grant Nos.20200812092737002,JCYJ20190808150409413,JCYJ20190808115415679,and JCYJ20190808152801642).
文摘Higher-order topological phase in 2-dimensional(2D)systems is characterized by in-gap corner states,which are hard to detect and utilize.We numerically investigate transport properties of topological corner states in 2D honeycomb lattice,where the second-order topological phase is induced by an in-plane Zeeman field in the conventional Kane–Mele model.Through engineering multihollow structures with appropriate boundaries in honeycomb lattice,multiple corner states emerge,which greatly increases the probability to observe them.A typical two-probe setup is built to study the transport features of a diamond-shaped system with multihollow structures.Numerical results reveal the existence of global resonant states in bulk insulator,which corresponds to the resonant tunneling of multiple corner states and occupies the entire scattering region.Furthermore,based on the well separated energy levels of multiple corner states,a single-electron source is constructed.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22071168 and 21774082)the Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Dispersity(D)of polymers has a great effect on the properties of polymeric materials,and therefore how to control θ is very important but still a huge challenge in polymer synthesis,especially for reversible-deactivation radical polymerization(RDRP)strategy.Herein,we successfully developed a novel strategy to adjust D of polymers by visible light-controlled reversible complexation mediated living radical polymerizatio n(RCMP)and combi nation of single-electron transfer-degenerative chain tran sfer living radical polymerization(SET-DTLRP)at room temperature.In RCMP system,2-iodo-2-methylpropionitrile(CP-I)and ethyl 2-iodo-2-phenylacetate(EIPA)were used as alkyl iodide initiators,by using methyl methacrylate(MMA)as the model monomer and n-butylacrylate(BA)as the end-capping reagent to regulate D of polymers.Subsequently,we successfully prepared the block copolymer PMMA-b-PBA with adjustable D by reactivating the polymer end-chains via SET-DTLRP in the presence of copper wire,fully dem on strati ng that it is a promising strategy that can keep the"living"feature of polymers while regulating their molar mass dispersities easily.