The structure-property relationship of Fe-doped SrCoO3-δ was studied. With increase of Fe content in SrCol-xFexO3-δ from x=0 to x=0.2, the phase composition changed pro- gressively in the order of hexagonal→brownmi...The structure-property relationship of Fe-doped SrCoO3-δ was studied. With increase of Fe content in SrCol-xFexO3-δ from x=0 to x=0.2, the phase composition changed pro- gressively in the order of hexagonal→brownmillerite （main）＋hexagonal→cubic （main）＋ brownmillerite→single cubic phase. Transition between the hexagonal/brownmillerite phase and the cubic phase took place with variation of the operating conditions, and was associated with remarkable changes in the electrical conductivity and oxygen permeation flux.展开更多
Doping with various impurities is an effective approach to improve the photoelectrochemical properties of TiO2. Here, we explore the effect of oxygen vacancy on geometric and elec- tronic properties of compensated （i...Doping with various impurities is an effective approach to improve the photoelectrochemical properties of TiO2. Here, we explore the effect of oxygen vacancy on geometric and elec- tronic properties of compensated （i.e. V-N and Cr-C） and non-compensated （i.e. V-C and Cr-N） codoped anatase TiO2 by performing extensive density functional theory calculations. Theoretical results show that oxygen vacancy prefers to the neighboring site of metal dopant （i.e. V or Cr atom）. After introduction of oxygen vacancy, the unoccupied impurity bands located within band gap of these codoped TiO2 will be filled with electrons, and the posi- tion of conduction band offset does not change obviously, which result in the reduction of photoinduced carrier recombination and the good performance for hydrogen production via water splitting. Moreover, we find that oxygen vacancy is easily introduced in V-N codoped TiO2 under O-poor condition. These theoretical insights are helpful for designing codoped TiO2 with high photoelectrochemical performance.展开更多
We explore the electronic and transport properties of zigzag graphene nanoribbons （GNRs） with nitrogen-vacancy defects by performing fully self-consistent spin-polarized density functional theory calculations combin...We explore the electronic and transport properties of zigzag graphene nanoribbons （GNRs） with nitrogen-vacancy defects by performing fully self-consistent spin-polarized density functional theory calculations combined with non-equilibrium Green＇s function technique. We observe robust negative di erential resistance （NDR） effect in all examined molecular junctions. Through analyzing the calculated electronic structures and the bias-dependent transmission coefficients, we find that the narrow density of states of electrodes and the bias-dependent effective coupling between the central molecular orbitals and the electrode subbands are responsible for the observed NDR phenomenon. In addition, the obvious di erence of the transmission spectra of two spin channels is observed in some bias ranges, which leads to the near perfect spin-filtering effect. These theoretical findings imply that GNRs with nitrogenvacancy defects hold great potential for building molecular devices.展开更多
Spin-crossover （SCO） magnets can act as one of the most possible building blocks in molec- ular spintronics due to their magnetic bistability between the high-spin （HS） and low-spin （LS） states. Here, the electr...Spin-crossover （SCO） magnets can act as one of the most possible building blocks in molec- ular spintronics due to their magnetic bistability between the high-spin （HS） and low-spin （LS） states. Here, the electronic structures and transport properties through SCO magnet Fe（II）-N4S2 complexes sandwiched between gold electrodes are explored by performing exten- sive density functional theory calculations combined with non-equilibrium Green＇s function formalism. The optimized Fe-N and Fe-S distances and predicted magnetic moment of the SCO magnet Fe（II）-N4S2 complexes agree well with the experimental results. The reversed spin transition between the HS and LS states can be realized by visible light irradiation according to the estimated SCO energy barriers. Based on the obtained transport results, we observe nearly perfect spin-filtering effect in this SCO magnet Fe（II）-N4S2 junction with the HS state, and the corresponding current under small bias voltage is mainly contributed by the spin-down electrons, which is obviously larger than that of the LS case. Clearly, these theoretical findings suggest that SCO magnet Fe（II）-N4S2 complexes hold potential applications in molecular spintronies.展开更多
As a clean and renewable future energy source, hydrogen fuel can be produced via solar water splitting. Two-dimensional (2D) black phosphorene (black-P) can harvest visible light due to the desirable band gap, which p...As a clean and renewable future energy source, hydrogen fuel can be produced via solar water splitting. Two-dimensional (2D) black phosphorene (black-P) can harvest visible light due to the desirable band gap, which promises it as a metal-free photocatalyst. However, black-P can be only used to produce hydrogen since the oxidation potential of water locates lower than the position of the valence band maximum. To improve the photocatalytic performance of black-P, here, using black-P and blue phosphorene (blue-P) monolayers, we propose a 2D van der Waals (vdW) heterojunction. Theoretical results, including the band structures, density of states, Bader charge population, charge density di erence, and optical absorption spectra, clearly reveal that the visible light absorption ability is obviously improved, and the band edge alignment of the proposed vdW heterojunction displays a typical type-II feature to effectively separate the photogenerated carriers. At the same time, the built-in interfacial electric field prevents the electron-hole recombination. These predictions suggest that the examined phosphorene-based vdW heterojunction is an efficient photocatalyst for solar water splitting.展开更多
Among various photocatalytic materials,Z-scheme photocatalysts have drawn tremendous research interest due to high photocatalytic performance in solar water splitting.Here,we perform extensive hybrid density functiona...Among various photocatalytic materials,Z-scheme photocatalysts have drawn tremendous research interest due to high photocatalytic performance in solar water splitting.Here,we perform extensive hybrid density functional theory calculations to explore electronic structures,interfacial charge transfer,electrostatic potential profile,optical absorption properties,and photocatalytic properties of a proposed two-dimensional(2D)small-lattice-mismatched GaTe/Bi2Se3 heterostructure.Theoretical results clearly reveal that the examined heterostructure with a small direct band gap can effectively harvest the broad spectrum of the incoming sunlight.Due to the relative strong interfacial built-in electric field in the heterostructure and the small band gap between the valence band maximum of Ga Te monolayer and the conduction band minimum of Bi2Se3 nanosheet with slight band edge bending,these photogenerated carriers transfer via Z-scheme pathway,which results in the photogenerated electrons and holes effectively separating into the Ga Te monolayer and the Bi2Se3 nanosheet for the hydrogen and oxygen evolution reactions,respectively.Our results imply that the artificial 2D GaTe/Bi2Se3 is a promising Z-scheme photocatalyst for overall solar water splitting.展开更多
Magnetic tunnel junction with a large tunneling magnetoresistance has attracted great attention due to its importance in the spintronics applications.By performing extensive density functional theory calculations comb...Magnetic tunnel junction with a large tunneling magnetoresistance has attracted great attention due to its importance in the spintronics applications.By performing extensive density functional theory calculations combined with the nonequilibrium Green’s function method,we explore the spin-dependent transport properties of a magnetic tunnel junction,in which a non-polar SrTiO_(3) barrier layer is sandwiched between two Heusler alloy Co_(2)MnSi electrodes.Theoretical results clearly reveal that the near perfect spin-filtering effect appears in the parallel magnetization configuration.The transmission coefficient in the parallel magnetization configuration at the Fermi level is several orders of magnitude larger than that in the antiparallel magnetization configuration,resulting in a huge tunneling magnetoresistance(i.e.>10^(6)),which originates from the coherent spin-polarized tunneling,due to the half-metallic nature of Co_(2)MnSi electrodes and the significant spin-polarization of the interfacial Ti_(3)d orbital.展开更多
Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS)has been widely adopted as hole transport material(HTM)in inverted perovskite solar cells(PSCs),due to high optical transparency,good mechanical flexib...Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS)has been widely adopted as hole transport material(HTM)in inverted perovskite solar cells(PSCs),due to high optical transparency,good mechanical flexibility,and high thermal stability;however,its acidity and hygroscopicity inevitably hamper the long-term stability of the PSCs and its energy level does not match well with perovskite materials with a relatively low open-circuit voltage.In this work,p-type delafossite CuCrO_(2)nanoparticles synthesized through hydrothermal method was employed as an alternative HTM for triple cation perovskite[(FAPbI_(3))_(0.87)(MAPbBr_(3))_(0.13)]_(0.92)(CsPbI_(3))_(0.08)(possessing better photovoltaic performance and stability than conventional CH3NH3PbI3)based inverted PSCs.The average open-circuit voltage of PSCs increases from 908 mV of the devices with PEDOT:PSS HTM to 1020 m V of the devices with CuCrO_(2)HTM.Ultraviolet photoemission spectroscopy demonstrates the energy band alignment between CuCrO_(2)and perovskite is better than that between PEDOT:PSS and perovskite,the electrochemical impedance spectroscopy indicates CuCrO_(2)-based PSCs exhibit larger recombination resistance and longer charge carrier lifetime than PEDOT:PSS-based PSCs,which contributes to the high VOCof CuCrO_(2)HTM-based PSCs.展开更多
文摘The structure-property relationship of Fe-doped SrCoO3-δ was studied. With increase of Fe content in SrCol-xFexO3-δ from x=0 to x=0.2, the phase composition changed pro- gressively in the order of hexagonal→brownmillerite （main）＋hexagonal→cubic （main）＋ brownmillerite→single cubic phase. Transition between the hexagonal/brownmillerite phase and the cubic phase took place with variation of the operating conditions, and was associated with remarkable changes in the electrical conductivity and oxygen permeation flux.
基金This work was supported by the National Natural Sci- ence Foundation of China （No.11034006, No.21273208, and No.21473168）, the Anhui Provincial Natural Sci- ence Foundation （No.1408085QB26）, the hmdamental Research Funds for the Central Universities, the China Postdoctoral Science Foundation （No.2012M511409）, and the Supercomputing Center of Chinese Academy of Sciences, Shanghai and USTC Supercomputer Cen- ters.
文摘Doping with various impurities is an effective approach to improve the photoelectrochemical properties of TiO2. Here, we explore the effect of oxygen vacancy on geometric and elec- tronic properties of compensated （i.e. V-N and Cr-C） and non-compensated （i.e. V-C and Cr-N） codoped anatase TiO2 by performing extensive density functional theory calculations. Theoretical results show that oxygen vacancy prefers to the neighboring site of metal dopant （i.e. V or Cr atom）. After introduction of oxygen vacancy, the unoccupied impurity bands located within band gap of these codoped TiO2 will be filled with electrons, and the posi- tion of conduction band offset does not change obviously, which result in the reduction of photoinduced carrier recombination and the good performance for hydrogen production via water splitting. Moreover, we find that oxygen vacancy is easily introduced in V-N codoped TiO2 under O-poor condition. These theoretical insights are helpful for designing codoped TiO2 with high photoelectrochemical performance.
基金This work was partially supported by the National Natural Science Foundation of China （No.20903003 and No.21273208）, the Anhui Provincial Natural Science Foundation （No.1408085QB26）, the China Postdoctoral Science Foundation （No.2012M511409）, the Supercomputer Center of Chinese Academy of Sciences, and University of Science and Technology of China and Shanghai Supercomputer Centers.
文摘We explore the electronic and transport properties of zigzag graphene nanoribbons （GNRs） with nitrogen-vacancy defects by performing fully self-consistent spin-polarized density functional theory calculations combined with non-equilibrium Green＇s function technique. We observe robust negative di erential resistance （NDR） effect in all examined molecular junctions. Through analyzing the calculated electronic structures and the bias-dependent transmission coefficients, we find that the narrow density of states of electrodes and the bias-dependent effective coupling between the central molecular orbitals and the electrode subbands are responsible for the observed NDR phenomenon. In addition, the obvious di erence of the transmission spectra of two spin channels is observed in some bias ranges, which leads to the near perfect spin-filtering effect. These theoretical findings imply that GNRs with nitrogenvacancy defects hold great potential for building molecular devices.
基金supported by the National Natural Science Foundation of China(No.21473168 and No.11634011)the Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology
文摘Spin-crossover （SCO） magnets can act as one of the most possible building blocks in molec- ular spintronics due to their magnetic bistability between the high-spin （HS） and low-spin （LS） states. Here, the electronic structures and transport properties through SCO magnet Fe（II）-N4S2 complexes sandwiched between gold electrodes are explored by performing exten- sive density functional theory calculations combined with non-equilibrium Green＇s function formalism. The optimized Fe-N and Fe-S distances and predicted magnetic moment of the SCO magnet Fe（II）-N4S2 complexes agree well with the experimental results. The reversed spin transition between the HS and LS states can be realized by visible light irradiation according to the estimated SCO energy barriers. Based on the obtained transport results, we observe nearly perfect spin-filtering effect in this SCO magnet Fe（II）-N4S2 junction with the HS state, and the corresponding current under small bias voltage is mainly contributed by the spin-down electrons, which is obviously larger than that of the LS case. Clearly, these theoretical findings suggest that SCO magnet Fe（II）-N4S2 complexes hold potential applications in molecular spintronies.
基金supported by the National Natural Science Foundation of China (No.21473168 and No.21873088)the Natural Science Foundation of the Anhui Higher Education Institutions (No.KJ2016A144)
文摘As a clean and renewable future energy source, hydrogen fuel can be produced via solar water splitting. Two-dimensional (2D) black phosphorene (black-P) can harvest visible light due to the desirable band gap, which promises it as a metal-free photocatalyst. However, black-P can be only used to produce hydrogen since the oxidation potential of water locates lower than the position of the valence band maximum. To improve the photocatalytic performance of black-P, here, using black-P and blue phosphorene (blue-P) monolayers, we propose a 2D van der Waals (vdW) heterojunction. Theoretical results, including the band structures, density of states, Bader charge population, charge density di erence, and optical absorption spectra, clearly reveal that the visible light absorption ability is obviously improved, and the band edge alignment of the proposed vdW heterojunction displays a typical type-II feature to effectively separate the photogenerated carriers. At the same time, the built-in interfacial electric field prevents the electron-hole recombination. These predictions suggest that the examined phosphorene-based vdW heterojunction is an efficient photocatalyst for solar water splitting.
基金the National Natural Science Foundation of China(No.21873088 and NO.11634011)。
文摘Among various photocatalytic materials,Z-scheme photocatalysts have drawn tremendous research interest due to high photocatalytic performance in solar water splitting.Here,we perform extensive hybrid density functional theory calculations to explore electronic structures,interfacial charge transfer,electrostatic potential profile,optical absorption properties,and photocatalytic properties of a proposed two-dimensional(2D)small-lattice-mismatched GaTe/Bi2Se3 heterostructure.Theoretical results clearly reveal that the examined heterostructure with a small direct band gap can effectively harvest the broad spectrum of the incoming sunlight.Due to the relative strong interfacial built-in electric field in the heterostructure and the small band gap between the valence band maximum of Ga Te monolayer and the conduction band minimum of Bi2Se3 nanosheet with slight band edge bending,these photogenerated carriers transfer via Z-scheme pathway,which results in the photogenerated electrons and holes effectively separating into the Ga Te monolayer and the Bi2Se3 nanosheet for the hydrogen and oxygen evolution reactions,respectively.Our results imply that the artificial 2D GaTe/Bi2Se3 is a promising Z-scheme photocatalyst for overall solar water splitting.
基金partially supported by the National Natural Science Foundation of China(No.21873088 and No.11634011)the Natural Science Foundation of the Anhui Higher Education Institutions(No.KJ2010A061 and No.KJ2016A144)。
文摘Magnetic tunnel junction with a large tunneling magnetoresistance has attracted great attention due to its importance in the spintronics applications.By performing extensive density functional theory calculations combined with the nonequilibrium Green’s function method,we explore the spin-dependent transport properties of a magnetic tunnel junction,in which a non-polar SrTiO_(3) barrier layer is sandwiched between two Heusler alloy Co_(2)MnSi electrodes.Theoretical results clearly reveal that the near perfect spin-filtering effect appears in the parallel magnetization configuration.The transmission coefficient in the parallel magnetization configuration at the Fermi level is several orders of magnitude larger than that in the antiparallel magnetization configuration,resulting in a huge tunneling magnetoresistance(i.e.>10^(6)),which originates from the coherent spin-polarized tunneling,due to the half-metallic nature of Co_(2)MnSi electrodes and the significant spin-polarization of the interfacial Ti_(3)d orbital.
基金jointly supported by the National Natural Science Foundation of China(No.62075223 and No.11674324)CAS Pioneer Hundred Talents Program of Chinese Academy of Sciences+5 种基金CAS-JSPS Joint Research Projects(GJHZ1891)Director Fund of Advanced Laser Technology Laboratory of Anhui Province(AHL2020ZR02)Key Lab of Photovoltaic and Energy Conservation Materials of Chinese Academy of Sciences(PECL2019QN005 and PECL2018QN001)the Natural Science Foundation of Top Talent of Shenzhen Technology University(No.2020101)Natural Science Research Project of Higher School of Anhui Province(KJ2020A0477)Initial Scientific Research Fund of Anhui Jianzhu University(No.2018QD60)。
文摘Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS)has been widely adopted as hole transport material(HTM)in inverted perovskite solar cells(PSCs),due to high optical transparency,good mechanical flexibility,and high thermal stability;however,its acidity and hygroscopicity inevitably hamper the long-term stability of the PSCs and its energy level does not match well with perovskite materials with a relatively low open-circuit voltage.In this work,p-type delafossite CuCrO_(2)nanoparticles synthesized through hydrothermal method was employed as an alternative HTM for triple cation perovskite[(FAPbI_(3))_(0.87)(MAPbBr_(3))_(0.13)]_(0.92)(CsPbI_(3))_(0.08)(possessing better photovoltaic performance and stability than conventional CH3NH3PbI3)based inverted PSCs.The average open-circuit voltage of PSCs increases from 908 mV of the devices with PEDOT:PSS HTM to 1020 m V of the devices with CuCrO_(2)HTM.Ultraviolet photoemission spectroscopy demonstrates the energy band alignment between CuCrO_(2)and perovskite is better than that between PEDOT:PSS and perovskite,the electrochemical impedance spectroscopy indicates CuCrO_(2)-based PSCs exhibit larger recombination resistance and longer charge carrier lifetime than PEDOT:PSS-based PSCs,which contributes to the high VOCof CuCrO_(2)HTM-based PSCs.
