Wu Chengyin, Wu Cong, Song Di, Su Hongmei, Xie Xiguo, Li Min, Deng Yongkai, Liu Yunquan, Gong Qihuang
State Key Laboratory for Mesoscopic Physics, Department of Physics, Peking University, Beijing 100871, People's Republic of China.
State Key Laboratory of Molecular Reaction Dynamics, Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, People's Republic of China.
J Chem Phys. 2014 Apr 14;140(14):141101. doi: 10.1063/1.4871205.
We experimentally reconstructed the structure of the N2Ar van der Waals complex with the technique of laser-based channel-selected Coulomb explosion imaging. The internuclear distance between the N2 center of mass and the Ar atom, i.e., the length of the van der Waals bond, was determined to be 3.88 Å from the two-body explosion channels. The angle between the van der Waals bond and the N2 principal axis was determined to be 90° from the three-body explosion channels. The reconstructed structure was contrasted with our high level ab initio calculations. The agreement demonstrated the potential application of laser-based Coulomb explosion in imaging transient molecular structure, particularly for floppy van der Waals complexes, whose structures remain difficult to be determined by conventional spectroscopic methods.
我们利用基于激光的通道选择库仑爆炸成像技术，通过实验重建了N₂Ar范德华复合物的结构。从双体爆炸通道确定，N₂质心与Ar原子之间的核间距，即范德华键的长度为3.88 Å。从三体爆炸通道确定，范德华键与N₂主轴之间的夹角为90°。将重建的结构与我们的高精度从头算计算结果进行了对比。这种一致性证明了基于激光的库仑爆炸在成像瞬态分子结构方面的潜在应用，特别是对于结构难以用传统光谱方法确定的松散范德华复合物。
