Ferromagnetism is induced in pure TiO2 single crystals by oxygen ion irradiation. The ferro- magnetism is observed up to room temperature and is with weak temperature dependence. By combining X-ray diffraction, Ruther...Ferromagnetism is induced in pure TiO2 single crystals by oxygen ion irradiation. The ferro- magnetism is observed up to room temperature and is with weak temperature dependence. By combining X-ray diffraction, Rutherford backseattering/channelling, Raman scattering, and electron-spin resonance spectroscopy, supperconducting quantum interference device, displacement per atom, we measured tile lattice damage accumulation with increasing flu- ences. A defect complex, i.e., Ti3＋ on the substitutional accoiflpanied by oxygen vacancies, has been identified in the irradiated Ti02. This kind of defect complex results in a local （TiO6-x） stretching Raman mode. We elucidate that Ti3＋ with one unpaired 3d electron provide the local magnetic moments.展开更多
Single atom catalysts have recently attracted interest due to their maximization of the utilization of expensive noble metals as well as their unique catalytic properties. Based on its surface atomic properties, CeO2 ...Single atom catalysts have recently attracted interest due to their maximization of the utilization of expensive noble metals as well as their unique catalytic properties. Based on its surface atomic properties, CeO2 is one of the most common supports for stabilizing single metal atoms. Many single atom catalysts are limited in their metal contents by the formation of metal nanoparticles once the catalyst support capacity for single atoms has been exceeded. Currently, there are no direct measurements to determine the capacity of a support to stabilize single atoms. In this work we develop a nanoparticle-based technique that allows for quantification of that capacity by redispersing Ru nanoparticles into single atoms and taking advantage of the different catalytic properties of Ru single atoms and nanoparticles in the CO2 hydrogenation reaction. This method avoids complications in metal loading caused by counterions in incipient wetness impregnation and can eventually be applied to a variety of different metals. Results using this technique follow trends in oxygen vacancy concentration and surface oxygen content and show promise as a new method for quantifying support single atom stabilization capacity.展开更多
Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion.Herein,oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues were su...Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion.Herein,oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues were successfully fabricated via a facile solvothermal strategy by the multifunctional regulatory mechanism of introduced chloridion.Both DFT calculations and speciation determination revealed that chloridion displayed a more pronounced effect in the controllable synthesis of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues:ultrathinning and defect-engineering.This built-in multi-cooperative interface endowed Bi_(2)WO_(6)with intriguing photoelectrochemical properties,O_(2) activation ability,and ultrahigh activity in visible-light powered deep oxidation of NO.A reasonable photocatalytic mechanism was proposed based on in situ infrared spectroscopy analysis and theoretical calculations.We believe that this multi-cooperative interface engineering of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues could provide new insights into the design of two-dimensional(2D)layered materials with efficient active sites and pave the way for efficient NO photooxidation systems.展开更多
An in situ heating system was built for the Auger electron spectroscopy to investigate the thermal effect of Auger lines. A GaN sample was studied in this system. The kinetic energy of Ga LMM and MVV Auger lines were ...An in situ heating system was built for the Auger electron spectroscopy to investigate the thermal effect of Auger lines. A GaN sample was studied in this system. The kinetic energy of Ga LMM and MVV Auger lines were observed to shift negatively with temperature increasing. By using ab initio calculation, the theoretical Ga MVV Auger line shape was fit, which well reflects the inner property of the line. The Auger shift with heating is related with the valence electron rearrangement in the thermal expansion of the local bonds.展开更多
The combination effect of cation vacancies and O2 adsorption on ferromagnetism of Na0.5Bi0.5TiO3（100） surface is studied by using density functional theory. An ideal Na0.5Bi0.5TiO3（100） surface is non-magnetic and...The combination effect of cation vacancies and O2 adsorption on ferromagnetism of Na0.5Bi0.5TiO3（100） surface is studied by using density functional theory. An ideal Na0.5Bi0.5TiO3（100） surface is non-magnetic and the cation vacancy could induce the magnetism. By comparing the formation energies for Na, Bi and Ti vacancy, the Na vacancy is more stable than the others. Therefore, we focus on the configuration and electric structure for the system of O2 molecule adsorption on the Na0.5Bi0.5TiO3（100） surface with a Na vacancy. Among the five physisorption configurations we considered, the most likely adsorption position is Na vacancy. The O2 adsorption enhances the magnetism of the system. The contribution of spin polarization is mainly from the O 2p orbitals. The characteristics of exchange coupling are also calculated, which show that the ferromagnetic coupling is favorable. Compared with the previous calculation results, our calculations could explain the room-temperature ferromagnetism of Na0.5Bi0.5TiO3 nanocrytalline powders more reasonably, because of taking into account adsorbed oxygen and cation vacancies. Moreover, our results also show that adsorption of O2 molecule as well as introduction of cation vacancies may be a promising approach to improve multiferroic materials.展开更多
Rational engineering of oxygen vacancy(VO) at atomic precision is the key to comprehensively understanding the oxygen chemistry of oxide materials for catalytic oxidations. Here, we demonstrate that VO can be spatiall...Rational engineering of oxygen vacancy(VO) at atomic precision is the key to comprehensively understanding the oxygen chemistry of oxide materials for catalytic oxidations. Here, we demonstrate that VO can be spatially confined on the surface through a sophisticated surface hydrogen bond(HB) network.The HB network is constructed between a hydroxyl-rich Bi OCl surface and polyprotic phosphoric acid,which remarkably decreases the formation energy of surface VO by selectively weakening the metal–oxygen bonds in a short range. Thus, surface-confined VO enables us to unambiguously distinguish the intrafacial and suprafacial oxygen species associated with NO oxidation in two classical catalytic systems.Unlike randomly distributed bulk VO that benefits the thermocatalytic NO oxidation and lattice O diffusion by the dominant intrafacial mechanism, surface VOis demonstrated to favor the photocatalytic NO oxidation through a suprafacial scheme by energetically activating surface O2, which should be attributed to the spatial confinement nature of surface VO.展开更多
We propose a scheme for implementation of a universal set of quantum logic gates in decoherence-free subspace with atoms trapped in distant cavities connected by optical fibers.The selective dispersive couplings betwe...We propose a scheme for implementation of a universal set of quantum logic gates in decoherence-free subspace with atoms trapped in distant cavities connected by optical fibers.The selective dispersive couplings between the ground states and the first-excited states of the atom-cavity-fiber system produce a state-dependent Stark shift,which can be used to implement nonlocal phase gates between two logic qubits.The single-logic-qubit quantum gates are achieved by the local two-atom collision and the Stark shift of a single atom.During all the logic operations,the logic qubits remain in decoherence-free subspace and thus the operation is immune to collective dephasing.展开更多
The charge-trapping process, with HfO2 film as the charge-capturing layer, has been investigated by using in situ electron energy-loss spectroscopy and in situ energy-filter image under positive external bias. The res...The charge-trapping process, with HfO2 film as the charge-capturing layer, has been investigated by using in situ electron energy-loss spectroscopy and in situ energy-filter image under positive external bias. The results show that oxygen vacancies are non-uniformly distributed throughout the HfO2 trapping layer during the programming process. The distribution of the oxygen vacancies is not the same as that of the reported locations of the trapped electrons, implying that the trapping process is more complex. These bias-induced oxygen defects may affect the device performance characteristics such as the device lifetime. This phenomenon should be considered in the models of trapping processes.展开更多
The spontaneous emission of an excited atom embedded in photonic crystals with two atomic position-dependent bands is investigated.The distribution of the density of states between two bands depends on the atomic posi...The spontaneous emission of an excited atom embedded in photonic crystals with two atomic position-dependent bands is investigated.The distribution of the density of states between two bands depends on the atomic position in a unit cell of the photonic crystal and is described with an atomic position-dependent parameter.The result shows that the emitted field and the time evolution of the upper-level population are affected by the atomic position and the gap width.The spontaneous emission spectrum in free space can be shifted and narrowed with the photonic reservoir and the gap width.展开更多
In this paper we have studied the dynamical evolution of Shannon information entropies in position and momentum spaces for two classes of（nonstationary） atom-field entangled states,which are obtained via the JaynesC...In this paper we have studied the dynamical evolution of Shannon information entropies in position and momentum spaces for two classes of（nonstationary） atom-field entangled states,which are obtained via the JaynesCummings model and its generalization.We have focused on the interaction between two- and（1）-type three-level atoms with the single-mode quantized field.The three-dimensional plots of entropy densities in position and momentum spaces are presented versus corresponding coordinates and time,numerically.It is observed that for particular values of the parameters of the systems,the entropy squeezing in position space occurs.Finally,we have shown that the well-known BBM（Beckner,Bialynicki-Birola and Mycielsky） inequality,which is a stronger statement of the Heisenberg uncertainty relation,is properly satisfied.展开更多
Particulate pollution has raised serious concerns regarding its potential impacts on human health in developing countries. However, much less attention has been paid to the threat of haze particles to machinery and in...Particulate pollution has raised serious concerns regarding its potential impacts on human health in developing countries. However, much less attention has been paid to the threat of haze particles to machinery and industry. By employing a state-of-the-art in situ scanning electron microscope compression testing technique, we demonstrate that iron-rich and fly ash haze particles, which account for nearly 70% of the total micron-sized spherical haze particles, are strong enough to generate abrasive damage to most engineering alloys, and therefore can generate significant scratch damage to moving contacting surfaces in high precision machineries. Our finding calls for preventive measures to protect against haze related threat.展开更多
文摘Ferromagnetism is induced in pure TiO2 single crystals by oxygen ion irradiation. The ferro- magnetism is observed up to room temperature and is with weak temperature dependence. By combining X-ray diffraction, Rutherford backseattering/channelling, Raman scattering, and electron-spin resonance spectroscopy, supperconducting quantum interference device, displacement per atom, we measured tile lattice damage accumulation with increasing flu- ences. A defect complex, i.e., Ti3＋ on the substitutional accoiflpanied by oxygen vacancies, has been identified in the irradiated Ti02. This kind of defect complex results in a local （TiO6-x） stretching Raman mode. We elucidate that Ti3＋ with one unpaired 3d electron provide the local magnetic moments.
基金support from the Stanford Precourt Institute for Energysupport from the School of Engineering at Stanford University+3 种基金a Terman Faculty Fellowshipsupport from a Stanford Graduate Fellowship(SGF)an EDGE fellowshipsupported by the National Science Foundation under award ECCS-1542152。
文摘Single atom catalysts have recently attracted interest due to their maximization of the utilization of expensive noble metals as well as their unique catalytic properties. Based on its surface atomic properties, CeO2 is one of the most common supports for stabilizing single metal atoms. Many single atom catalysts are limited in their metal contents by the formation of metal nanoparticles once the catalyst support capacity for single atoms has been exceeded. Currently, there are no direct measurements to determine the capacity of a support to stabilize single atoms. In this work we develop a nanoparticle-based technique that allows for quantification of that capacity by redispersing Ru nanoparticles into single atoms and taking advantage of the different catalytic properties of Ru single atoms and nanoparticles in the CO2 hydrogenation reaction. This method avoids complications in metal loading caused by counterions in incipient wetness impregnation and can eventually be applied to a variety of different metals. Results using this technique follow trends in oxygen vacancy concentration and surface oxygen content and show promise as a new method for quantifying support single atom stabilization capacity.
文摘Engineering an efficient interface is a trustworthy strategy for designing advanced photocatalytic systems for solar energy conversion.Herein,oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues were successfully fabricated via a facile solvothermal strategy by the multifunctional regulatory mechanism of introduced chloridion.Both DFT calculations and speciation determination revealed that chloridion displayed a more pronounced effect in the controllable synthesis of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues:ultrathinning and defect-engineering.This built-in multi-cooperative interface endowed Bi_(2)WO_(6)with intriguing photoelectrochemical properties,O_(2) activation ability,and ultrahigh activity in visible-light powered deep oxidation of NO.A reasonable photocatalytic mechanism was proposed based on in situ infrared spectroscopy analysis and theoretical calculations.We believe that this multi-cooperative interface engineering of oxygen-deficient Bi_(2)WO_(6)atomic layers without organic residues could provide new insights into the design of two-dimensional(2D)layered materials with efficient active sites and pave the way for efficient NO photooxidation systems.
基金The author would like to express thanks to Professor Jun-yong Kang and Dr. Duan-jun Cai for their valuable discussions. This work was partly supported by the National Nature Science Foundation of China （No.60206030, No.10134030 and No.69976023） and the Natural Science Found of Xiamen University （No.B200337）.
文摘An in situ heating system was built for the Auger electron spectroscopy to investigate the thermal effect of Auger lines. A GaN sample was studied in this system. The kinetic energy of Ga LMM and MVV Auger lines were observed to shift negatively with temperature increasing. By using ab initio calculation, the theoretical Ga MVV Auger line shape was fit, which well reflects the inner property of the line. The Auger shift with heating is related with the valence electron rearrangement in the thermal expansion of the local bonds.
基金supported by the National Natural Science Foundation of China (No.11547176, No.11704006)Henan College Key Research Project (No.15A140017)
文摘The combination effect of cation vacancies and O2 adsorption on ferromagnetism of Na0.5Bi0.5TiO3（100） surface is studied by using density functional theory. An ideal Na0.5Bi0.5TiO3（100） surface is non-magnetic and the cation vacancy could induce the magnetism. By comparing the formation energies for Na, Bi and Ti vacancy, the Na vacancy is more stable than the others. Therefore, we focus on the configuration and electric structure for the system of O2 molecule adsorption on the Na0.5Bi0.5TiO3（100） surface with a Na vacancy. Among the five physisorption configurations we considered, the most likely adsorption position is Na vacancy. The O2 adsorption enhances the magnetism of the system. The contribution of spin polarization is mainly from the O 2p orbitals. The characteristics of exchange coupling are also calculated, which show that the ferromagnetic coupling is favorable. Compared with the previous calculation results, our calculations could explain the room-temperature ferromagnetism of Na0.5Bi0.5TiO3 nanocrytalline powders more reasonably, because of taking into account adsorbed oxygen and cation vacancies. Moreover, our results also show that adsorption of O2 molecule as well as introduction of cation vacancies may be a promising approach to improve multiferroic materials.
基金the National Key Research and Development Program of China (2016YFA0203000)National Natural Science Funds for Distinguished Young Scholars (21425728)+2 种基金the National Natural Science Foundation of China (21872061)111 Project (B17019)Self-Determined Research Funds of CCNU from the Colleges’ Basic Research and Operation of MOE (CCNU16A02029)。
文摘Rational engineering of oxygen vacancy(VO) at atomic precision is the key to comprehensively understanding the oxygen chemistry of oxide materials for catalytic oxidations. Here, we demonstrate that VO can be spatially confined on the surface through a sophisticated surface hydrogen bond(HB) network.The HB network is constructed between a hydroxyl-rich Bi OCl surface and polyprotic phosphoric acid,which remarkably decreases the formation energy of surface VO by selectively weakening the metal–oxygen bonds in a short range. Thus, surface-confined VO enables us to unambiguously distinguish the intrafacial and suprafacial oxygen species associated with NO oxidation in two classical catalytic systems.Unlike randomly distributed bulk VO that benefits the thermocatalytic NO oxidation and lattice O diffusion by the dominant intrafacial mechanism, surface VOis demonstrated to favor the photocatalytic NO oxidation through a suprafacial scheme by energetically activating surface O2, which should be attributed to the spatial confinement nature of surface VO.
基金supported by the Major State Basic Research Development Program of China (Grant No. 2012CB921601)the National Natural Science Foundation of China (Grant No. 10974028)+1 种基金the Doctoral Foundation of the Ministry of Education of China (Grant No. 20093514110009)the Natural Science Foundation of Fujian Province (Grant No. 2009J06002)
文摘We propose a scheme for implementation of a universal set of quantum logic gates in decoherence-free subspace with atoms trapped in distant cavities connected by optical fibers.The selective dispersive couplings between the ground states and the first-excited states of the atom-cavity-fiber system produce a state-dependent Stark shift,which can be used to implement nonlocal phase gates between two logic qubits.The single-logic-qubit quantum gates are achieved by the local two-atom collision and the Stark shift of a single atom.During all the logic operations,the logic qubits remain in decoherence-free subspace and thus the operation is immune to collective dephasing.
基金Acknowledgements This work was supported by the National Basic Research Program of China （Nos. 2012CB932302, 2010CB934202 and 2013CB932904）, the National Natural Science Foundation of China （No. 10974235）.
文摘The charge-trapping process, with HfO2 film as the charge-capturing layer, has been investigated by using in situ electron energy-loss spectroscopy and in situ energy-filter image under positive external bias. The results show that oxygen vacancies are non-uniformly distributed throughout the HfO2 trapping layer during the programming process. The distribution of the oxygen vacancies is not the same as that of the reported locations of the trapped electrons, implying that the trapping process is more complex. These bias-induced oxygen defects may affect the device performance characteristics such as the device lifetime. This phenomenon should be considered in the models of trapping processes.
基金supported by the Natural Science College Key Projects of Anhui Province (Grant Nos. KJ2010A335 and KJ2012Z023)the National Natural Science Foundation of China (Grant Nos. 41075027 and 61205115)the Key Project of Chinese Ministry of Education (Grant No. 212076)
文摘The spontaneous emission of an excited atom embedded in photonic crystals with two atomic position-dependent bands is investigated.The distribution of the density of states between two bands depends on the atomic position in a unit cell of the photonic crystal and is described with an atomic position-dependent parameter.The result shows that the emitted field and the time evolution of the upper-level population are affected by the atomic position and the gap width.The spontaneous emission spectrum in free space can be shifted and narrowed with the photonic reservoir and the gap width.
文摘In this paper we have studied the dynamical evolution of Shannon information entropies in position and momentum spaces for two classes of（nonstationary） atom-field entangled states,which are obtained via the JaynesCummings model and its generalization.We have focused on the interaction between two- and（1）-type three-level atoms with the single-mode quantized field.The three-dimensional plots of entropy densities in position and momentum spaces are presented versus corresponding coordinates and time,numerically.It is observed that for particular values of the parameters of the systems,the entropy squeezing in position space occurs.Finally,we have shown that the well-known BBM（Beckner,Bialynicki-Birola and Mycielsky） inequality,which is a stronger statement of the Heisenberg uncertainty relation,is properly satisfied.
基金supported by the National Natural Science Foundation of China(Grant Nos.5123100551471128 and 51321003)+3 种基金the National Basic Research Program of China("973"Project)(Grant No.2012CB619402)the"111"Project of China(Grant No.B06025)W.Z.Han was supported by the Youth Thousand Talents Plan and the Young Talent Support Plan of XJTU.J.L.support by the NSF DMR-1120901 and DMR-1410636
文摘Particulate pollution has raised serious concerns regarding its potential impacts on human health in developing countries. However, much less attention has been paid to the threat of haze particles to machinery and industry. By employing a state-of-the-art in situ scanning electron microscope compression testing technique, we demonstrate that iron-rich and fly ash haze particles, which account for nearly 70% of the total micron-sized spherical haze particles, are strong enough to generate abrasive damage to most engineering alloys, and therefore can generate significant scratch damage to moving contacting surfaces in high precision machineries. Our finding calls for preventive measures to protect against haze related threat.
