The electronic structure of methanol/TiO2(ll0) interface has been studied by photoemis- sion spectroscopy. The pronounced resonance which appears at 5.5 eV above the Fermi level in two-photon photoemission spectrosc...The electronic structure of methanol/TiO2(ll0) interface has been studied by photoemis- sion spectroscopy. The pronounced resonance which appears at 5.5 eV above the Fermi level in two-photon photoemission spectroscopy (2PPE) is associated with the photocatalyzed dissociation of methanol at fivefold coordinated Ti sites (Ti5c) on TiO2 (110) surface [Chem- ical Science 1, 575 (2010)]. To check whether this resonance signal arises from initial or intermediate states, photon energy dependent 2PPE and comparison between one-photon photoemission spectroscopy and 2PPE have been performed. Both results consistently sug- gest the resonance signal originates from the initially unoccupied intermediate states, i.e., excited states. Dispersion measurements suggest the excited state is localized. Time-resolved studies show the lifetime of the excited state is 24 fs. This work presents comprehensive char- acterization of the excited states on methanol/TiO2(110) interface, and provides elaborate experimental data for the development of theoretical methods in reproducing the excited states on TiO2 surfaces and interfaces.展开更多
The crystal phase, morphology and facet significantly influence the catalytic and photocat- alytic activity of TiO2. In view of optimizing the performance of catalysts, extensive efforts have been devoted to designing...The crystal phase, morphology and facet significantly influence the catalytic and photocat- alytic activity of TiO2. In view of optimizing the performance of catalysts, extensive efforts have been devoted to designing new sophisticate TiO2 structures with desired facet exposure, necessitating the understanding of chemical properties of individual surface. In this work, we have examined the photooxidation of methanol on TiO 2 (011)- ( 2 × 1 ) and TiO 2 (110) - (1 ×1) by two-photon photoemission spectroscopy (2PPE). An excited state at 2.5 eV above the Fermi level (EF) on methanol covered (011) and (110) interface has been detected. The excited state is an indicator of reduction of TiO2 interface. Irradiation dependence of the excited resonance signal during the photochemistry of methanol on TiO2(011)-(2×1) and TiO2(110)-(1× 1) is ascribed to the interface reduction by producing surface hydroxyls. The reaction rate of photooxidation of methanol on TiO2(110)-(1× 1) is about 11.4 times faster than that on TiO2(011)-(2×1), which is tentatively explained by the difference in the surface atomic configuration. This work not only provides a detailed characterization of the electronic structure of methanol/TiO2 interface by 2PPE, but also shows the importance of the surface structure in the photoreactivity on TiO2.展开更多
In this paper, collective excitations in the boson-fermion model are investigated by means of functional integration method. The equations of energy gap and excitation spectrum are derived. Moreover, the Bose energy s...In this paper, collective excitations in the boson-fermion model are investigated by means of functional integration method. The equations of energy gap and excitation spectrum are derived. Moreover, the Bose energy spectrum of zero wave vector Fermi fields is also calculated.展开更多
The laser-induced fluorescence excitation spectrum of jet-cooled NiS molecule has been recorded in the energy range of 15500 17200 cm-1. Fifteen bands have been assigned as three transition progressions:[15.65]^3Ⅱ1...The laser-induced fluorescence excitation spectrum of jet-cooled NiS molecule has been recorded in the energy range of 15500 17200 cm-1. Fifteen bands have been assigned as three transition progressions:[15.65]^3Ⅱ1(v′=0-4)-X^3∑0^-(v″=0),[15.69]^3∑0^-(v′=0-4)-X^3∑0^-(v″=0),and [15.81]^3Ⅱ1(v′=0-4)-X^3∑0^-(v″=0).Spectroscopic constants for the three newly identified electronically excited states have been determined for the first time. In addition,the lifetimes for most observed vibronic bands have also been measured.展开更多
In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important f...In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.展开更多
文摘The electronic structure of methanol/TiO2(ll0) interface has been studied by photoemis- sion spectroscopy. The pronounced resonance which appears at 5.5 eV above the Fermi level in two-photon photoemission spectroscopy (2PPE) is associated with the photocatalyzed dissociation of methanol at fivefold coordinated Ti sites (Ti5c) on TiO2 (110) surface [Chem- ical Science 1, 575 (2010)]. To check whether this resonance signal arises from initial or intermediate states, photon energy dependent 2PPE and comparison between one-photon photoemission spectroscopy and 2PPE have been performed. Both results consistently sug- gest the resonance signal originates from the initially unoccupied intermediate states, i.e., excited states. Dispersion measurements suggest the excited state is localized. Time-resolved studies show the lifetime of the excited state is 24 fs. This work presents comprehensive char- acterization of the excited states on methanol/TiO2(110) interface, and provides elaborate experimental data for the development of theoretical methods in reproducing the excited states on TiO2 surfaces and interfaces.
基金This work was supported the Natural Science Foundation of Liaoning Province (No.2015020242), the National Natural Science Foundation of China (No.21203189 and No.21573225), and the State Key Laboratory of Molecular Reaction Dynamics (No.ZZ- 2014-02).
文摘The crystal phase, morphology and facet significantly influence the catalytic and photocat- alytic activity of TiO2. In view of optimizing the performance of catalysts, extensive efforts have been devoted to designing new sophisticate TiO2 structures with desired facet exposure, necessitating the understanding of chemical properties of individual surface. In this work, we have examined the photooxidation of methanol on TiO 2 (011)- ( 2 × 1 ) and TiO 2 (110) - (1 ×1) by two-photon photoemission spectroscopy (2PPE). An excited state at 2.5 eV above the Fermi level (EF) on methanol covered (011) and (110) interface has been detected. The excited state is an indicator of reduction of TiO2 interface. Irradiation dependence of the excited resonance signal during the photochemistry of methanol on TiO2(011)-(2×1) and TiO2(110)-(1× 1) is ascribed to the interface reduction by producing surface hydroxyls. The reaction rate of photooxidation of methanol on TiO2(110)-(1× 1) is about 11.4 times faster than that on TiO2(011)-(2×1), which is tentatively explained by the difference in the surface atomic configuration. This work not only provides a detailed characterization of the electronic structure of methanol/TiO2 interface by 2PPE, but also shows the importance of the surface structure in the photoreactivity on TiO2.
基金The project supported by the Science Foundation of Sichuan Normal University
文摘In this paper, collective excitations in the boson-fermion model are investigated by means of functional integration method. The equations of energy gap and excitation spectrum are derived. Moreover, the Bose energy spectrum of zero wave vector Fermi fields is also calculated.
基金V. ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China (No.20673107), the National Key Basic Research Special Foundation of China (No.G2007CB815203), and the Chinese Academy of Sciences (No.KJCX2-YW-N24).
文摘The laser-induced fluorescence excitation spectrum of jet-cooled NiS molecule has been recorded in the energy range of 15500 17200 cm-1. Fifteen bands have been assigned as three transition progressions:[15.65]^3Ⅱ1(v′=0-4)-X^3∑0^-(v″=0),[15.69]^3∑0^-(v′=0-4)-X^3∑0^-(v″=0),and [15.81]^3Ⅱ1(v′=0-4)-X^3∑0^-(v″=0).Spectroscopic constants for the three newly identified electronically excited states have been determined for the first time. In addition,the lifetimes for most observed vibronic bands have also been measured.
基金The project supported by National Natural Science Foundation of China under Grant No. 10475021 and the Natured Science Foundation of Guangdong Province of China under Grant No. 04009519
文摘In this paper, a negatively charged exciton trapped by a spherical parabolic quantum dot has been investigated. The energy spectra of low-lying states are calculated by means of matrix diagonalization. The important feature of the low-lying states of the negatively charged excitons in a spherical quantum dot is obtained via an analysis of the energy spectra.