Molecular frame photoemission is a very sensitive probe of the photoionization （PI） dynamics of molecules. This paper reports a comparative study of non-resonant and resonant photoionization of D2 induced by VUV cir...Molecular frame photoemission is a very sensitive probe of the photoionization （PI） dynamics of molecules. This paper reports a comparative study of non-resonant and resonant photoionization of D2 induced by VUV circularly polarized synchrotron radiation at SOLEIL at the level of the molecular frame photoelectron angular distributions （MFPADs）. We use the vector correlation method which combines imaging and time-of-flight resolved electron-ion coincidence techniques, and a generalized formalism for the expression of the Ⅰ（χ, θe, Фe） MFPADs, where χ is the orientation of the molecular axis with respect to the light quantization axis and （θe, Фe） the electron emission direction in the molecular frame. Selected MFPADs for a molecule aligned parallel or perpendicular to linearly polarized light, or perpendicular to the propagation axis of circularly polarized light, are presented for dissociative photoionization （DPI） of D2 at two photon excitation energies, hv=19 eV, where direct PI is the only channel opened, and hv=32.5 eV, i.e. in the region involving resonant excitation of Q1 and Q2 doubly excited state series. We discuss in particular the properties of the circular dichroism characterizing photoemission in the molecular frame for direct and resonant PI. In the latter case, a remarkable behavior is observed which may be attributed to the interference occurring between undistinguishable autoionization decay channels.展开更多
A new type of dispenser cathode with dual-layer (Os-W/Re) is developed. The cathode coated with Os-W/Re shows better emission performance than the cathode coated with Os-W alloy. X-ray Photoelectron Spectroscopy (XPS)...A new type of dispenser cathode with dual-layer (Os-W/Re) is developed. The cathode coated with Os-W/Re shows better emission performance than the cathode coated with Os-W alloy. X-ray Photoelectron Spectroscopy (XPS) spectra demonstrate that ternary alloy coating (Os-W-Re) formed on the surface of the cathode with dual-layer (Os-W/Re) after full activation is the major reason why it has better emission than the cathode with Os-W alloy. The surface of each variety of the cathode is characterized with Scanning Electron Microscope (SEM) before and after activation: the emitting surface of the cathode with Os-W alloy after ageing appeared non-adherence (flaking) in localized areas, which is one of the reasons for non-uniform emission. However, the surface of the cathode with dual-layer (Os-W/Re) does not present film peeling under the same conditions. Thus it ensures better emission uniformity and functional reliability for the dispenser cathode.展开更多
The product channels and mechanisms of the C2HC12＋O2 reaction are investigated by step-scan time-resolved Fourier transform infrared emission spectroscopy and the G3MP2// B3LYP/6-311G（d,p） level of electronic struc...The product channels and mechanisms of the C2HC12＋O2 reaction are investigated by step-scan time-resolved Fourier transform infrared emission spectroscopy and the G3MP2// B3LYP/6-311G（d,p） level of electronic structure calculations. Vibrationally excited products of HCI, CO, and CO2 are observed in the IR emission spectra and the product vibrational state distribution are determined which shows that HCI and CO are vibrationally excited with the nascent average vibrational energy estimated to be 59.8 and 51.8 kJ/mol respectively. In combination with the G3MP2//B3LYP/6-311G（d,p） calculations, the reaction mechanisms have been characterized and the energetically favorable reaction pathways have been suggested.展开更多
ZnO:Cu/ZnO core/shell nanocrystals are synthesized by a two-step solution-phase process. The morphology, structure and optical properties of the samples are detected by scanning electron microscopy, Raman, absorption ...ZnO:Cu/ZnO core/shell nanocrystals are synthesized by a two-step solution-phase process. The morphology, structure and optical properties of the samples are detected by scanning electron microscopy, Raman, absorption and luminescence spectroscopy. The increase of particle size confirms the growth of ZnO shell. The segregation of CuO phase observed in ZnO: Cu core is not detected in ZnO:Cu/ZnO core/shell nanocrystals from Raman spectra. It is suggested that some Cu ions can be segregated from ZnO nanocrystals, and the separated Cu ions can be incorporated inside ZnO shell after the growth of ZnO shell. The visible emission mechanism is discussed in detail, and the photoluminescence analysis indicates that the core/shell structure helps to eliminate the surface-related emission.展开更多
文摘Molecular frame photoemission is a very sensitive probe of the photoionization （PI） dynamics of molecules. This paper reports a comparative study of non-resonant and resonant photoionization of D2 induced by VUV circularly polarized synchrotron radiation at SOLEIL at the level of the molecular frame photoelectron angular distributions （MFPADs）. We use the vector correlation method which combines imaging and time-of-flight resolved electron-ion coincidence techniques, and a generalized formalism for the expression of the Ⅰ（χ, θe, Фe） MFPADs, where χ is the orientation of the molecular axis with respect to the light quantization axis and （θe, Фe） the electron emission direction in the molecular frame. Selected MFPADs for a molecule aligned parallel or perpendicular to linearly polarized light, or perpendicular to the propagation axis of circularly polarized light, are presented for dissociative photoionization （DPI） of D2 at two photon excitation energies, hv=19 eV, where direct PI is the only channel opened, and hv=32.5 eV, i.e. in the region involving resonant excitation of Q1 and Q2 doubly excited state series. We discuss in particular the properties of the circular dichroism characterizing photoemission in the molecular frame for direct and resonant PI. In the latter case, a remarkable behavior is observed which may be attributed to the interference occurring between undistinguishable autoionization decay channels.
基金Supported by the National Science Fund for Distinguished Young Scholars of China (No.60125104).
文摘A new type of dispenser cathode with dual-layer (Os-W/Re) is developed. The cathode coated with Os-W/Re shows better emission performance than the cathode coated with Os-W alloy. X-ray Photoelectron Spectroscopy (XPS) spectra demonstrate that ternary alloy coating (Os-W-Re) formed on the surface of the cathode with dual-layer (Os-W/Re) after full activation is the major reason why it has better emission than the cathode with Os-W alloy. The surface of each variety of the cathode is characterized with Scanning Electron Microscope (SEM) before and after activation: the emitting surface of the cathode with Os-W alloy after ageing appeared non-adherence (flaking) in localized areas, which is one of the reasons for non-uniform emission. However, the surface of the cathode with dual-layer (Os-W/Re) does not present film peeling under the same conditions. Thus it ensures better emission uniformity and functional reliability for the dispenser cathode.
基金V. ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.20733005, No.20673126, and No.20973179）, the National Basic Research Program of China （No.2007CB815200 and No.2007AA02Z116）, and the Chinese Academy of Sciences.
文摘The product channels and mechanisms of the C2HC12＋O2 reaction are investigated by step-scan time-resolved Fourier transform infrared emission spectroscopy and the G3MP2// B3LYP/6-311G（d,p） level of electronic structure calculations. Vibrationally excited products of HCI, CO, and CO2 are observed in the IR emission spectra and the product vibrational state distribution are determined which shows that HCI and CO are vibrationally excited with the nascent average vibrational energy estimated to be 59.8 and 51.8 kJ/mol respectively. In combination with the G3MP2//B3LYP/6-311G（d,p） calculations, the reaction mechanisms have been characterized and the energetically favorable reaction pathways have been suggested.
基金supported by the National Natural Science Foundation of China (Nos.60877029,10904109,60977035 and 60907021)the Natural Science Foundation of Tianjin (No.09JCYBJC01400)the Tianjin Key Subject for Materials Physics and Chemistry
文摘ZnO:Cu/ZnO core/shell nanocrystals are synthesized by a two-step solution-phase process. The morphology, structure and optical properties of the samples are detected by scanning electron microscopy, Raman, absorption and luminescence spectroscopy. The increase of particle size confirms the growth of ZnO shell. The segregation of CuO phase observed in ZnO: Cu core is not detected in ZnO:Cu/ZnO core/shell nanocrystals from Raman spectra. It is suggested that some Cu ions can be segregated from ZnO nanocrystals, and the separated Cu ions can be incorporated inside ZnO shell after the growth of ZnO shell. The visible emission mechanism is discussed in detail, and the photoluminescence analysis indicates that the core/shell structure helps to eliminate the surface-related emission.
