首页|(H2O)n+(n=2~5)团簇离子在308 nm处的光解动力学

(H2O)n+(n=2~5)团簇离子在308 nm处的光解动力学

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本文利用一套高分辨圆柱形低温离子阱速度成像谱仪装置研究了小团簇离子(H2O)n+(n=2~5)在308 nm处的光解动力学.通过记录光解产物碎片质谱和速度影像,发现二聚体水团簇(H2O)2+解离生成H3O+和H2O+光碎片,表明其同时存在质子转移(H3O+-OH)和半束缚(H2O-OH2)+两种构型.水团簇离子(H2O)n+(n=3~5)普遍通过同时丢失OH和H2O部分解离得到H+(H2O)n-2,…,1光碎片,并且(H2O)5+团簇离子有一个仅通过丢失OH的额外通道得到H+(H2O)4.前者表明(H2O)n+(n=3~5)的构型是(H2O)n-2H3O+OH,后者表明在(H2O)5+团簇离子中核H3O+和OH被H2O分开.基于实验影像得到的光碎片各向异性参数为负值并且值较小,表明(H2O)n+(n=2~5)团簇离子在光子吸收后经历垂直电子跃迁,随后缓慢解离,并导致光碎片的高内部激发.
Photodissociation Studies on(H2O)n+(n=2-5)Clusters at 308 nm
The photodissociation dynamics of small(H2O)n+(n=2-5)clusters have been studied at 308 nm using a high resolution cryogenic cylin-drical ion trap velocity map imaging spectrome-ter.Time-of-flight mass spectra and images of ionic photofragments are recorded.(H2O)2+clusters dissociate to yield H3O+and H2O+photofragments,indicating the presence of both proton-transferred(H3O+-OH)and hemibond-ed(H2O-OH2)+structures for the dimer clus-ter.(H2O)n+(n=3-5)clusters prevailingly dis-sociate to the H+(H2O)n-2,…,1 photofragments by losing both of OH and H2O components,and the(H2O)5+cluster shows an additional channel to produce H+(H2O)4 by only losing OH.The former suggests the(H2O)n-2H3O+OH structures for the(H2O)n+(n=3-5)clus-ters,while the latter suggests in(H2O)5+that,the H3O+core and OH are separated by H2O.The results elucidate the structure progresses of small(H2O)n+clusters.The experi-mental images yield negative and small values for the anisotropy parameters of photofrag-ments,indicating that(H2O)n+(n=2-5)clusters undergo vertical electronic transitions up-on photon absorption followed by slow dissociation,and lead to highly internally excited photofragments.

(H2O)n+clustersPhotodissociation dynamicsTime-of-flightVelocity map imaging

赵云肖、胡高明、李佑卿、陈旸、赵东锋

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中国科学技术大学化学物理系,合肥微尺度物质科学国家研究中心,合肥 230026

(H2O)n+团簇 光解动力学 飞行时间质谱 速度成像

国家自然科学基金国家自然科学基金国家自然科学基金国家重点研发计划国家重点研发计划

2210307521827804221730892021YFA07168012017YFA0303502

2024

化学物理学报(英文版)
中国物理学会

化学物理学报(英文版)

CSTPCDEI
影响因子:0.162
ISSN:1674-0068
年,卷(期):2024.37(2)
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