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时间和角度分辨的光电离实验能够跟踪原子分子的几何构型和电子态演化，这需要在自由电子激光中测量电子离子全空间角分布。本文报道在上海软X射线自由电子激光装置上的复合速度成像谱仪的首次实验结果。在263.8 eV下，用自由电子激光电离Kr和CCl4样品，通过Andor和TPX3CAM两台相机分别获得电子动量图像与离子质谱。Kr的3p、3d、4p光电子及俄歇电子峰的强度与前人实验符合，角分布参数β与前人计算符合。同样，CCl4分子Cl的2p光电子、2p俄歇电子及价壳层电子的角分布也与已有计算结果符合良好。用TPX3CAM相机测量了碎片离子的动量分布，揭示了CCl4的光解离路径。结果表明，复合速度成像谱仪在实验中兼具全立体角收集与高分辨率优势，为自由电子激光光诱导动力学研究提供了可靠的实验平台。Temporal- and angular-resolved photoionization experiments are essential for probing the geometric and electronic structural dynamics of atoms and molecules. Such studies require the measurement of full angular distributions of electrons and ions in free electron laser (FEL) experiments. Here, we present the first experimental results from the composite velocity imaging spectrometer (CpVMI) at the Shanghai Soft X-ray Free Electron Laser Facility (SXFEL). The study demonstrates its ability to capture energy and angular information for electrons and ions with high resolution and full solid-angle collection.
Krypton (Kr) atoms and carbon tetrachloride (CCl4) molecules are ionized using FEL pulses at 263.8 eV. Electron momentum images were recorded with an Andor Zyla 4.2 PLUS camera, while ion time-of-flight mass spectra and momentum distributions were acquired using a TPX3CAM. For Kr, the electron spectrum contains peaks from 3p, 3d, and 4p photoionization, as well as the Auger electrons from 3d and 3p levels. The measured anisotropy parameters (β) of these electrons show good agreement with previous theoretical Hartree-Fock calculations. Ion abundance in the time-of-flight mass spectra of Kr was consistent with the ratio derived from the intensities of the corresponding photoelectron peaks.
For CCl4, the electron spectrum contains Cl 2p photoelectrons, 2p Auger electrons, and valence-shell photoelectrons, with their angular distribution parameters also aligning with theoretical predictions. The TPX3CAM enabled direct measurement of the momenta of fragment ions without the need for inverse Abel transformation. By integrating the high-resolution flight time mass spectrometry and momentum imaging data obtained from TPX3CAM, we successfully visualized and analyzed the key photodissociation pathways of CCl4 molecules under the action of soft X-ray FEL. In particular, it distinguished between direct two-body dissociation and multi-step dissociation processes, and observed the unique angular distributions and kinetic energy release characteristics of different dissociation channels.
In conclusion, the experimental results clearly demonstrate that the CpVMI fully meets the technical requirements for FEL user experiments in terms of energy, angular distribution, and momentum measurement, offering a platform for FEL light-induced dynamics research. Future enhancements, including improved light focusing and the use of supersonic molecular beams, are expected to further advance the instrument's performance.-
Keywords:
- X-ray free electron laser /
- velocity imaging spectrometer /
- angular distribution of charged particles
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