Clustering and photochemistry of freon CF2Cl2 on argon and ice nanoparticles.

Clustering and photochemistry of freon CF2Cl2 on argon and ice nanoparticles.
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氟利昂 CF2Cl2 在氩和冰纳米颗粒上的聚类和光化学。

DOI:
10.1021/jp503983x
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发表时间:
2014
期刊:
The journal of physical chemistry. A
影响因子:
--
通讯作者:
M. Farnik
M. Farnik
中科院分区:
--
文献类型:
--
作者:
V. Poterya;J. Kočišek;J. Lengyel;P. Svrčková;A. Pysanenko;D. Hollas;P. Slavíček;M. Farnik

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研究了沉积在氩和冰纳米颗粒上的CF2 Cl 2分子的光化学。团簇的特征在于通过电子电离质谱,和光化学反应揭示的Cl碎片的速度图成像后,CF2 Cl 2在193 nm的光解。复杂分子束实验的补充从头计算。(CF_2Cl_2)_n团簇是在Ar缓冲气体的共膨胀中产生的。(CF2 Cl 2)n团簇中分子的光解主要产生具有零动能的Cl片段:笼化。在拾取实验中,沉积在大的氩团簇上的CF2 Cl 2分子是高度移动的,并且在ArN上凝聚形成(CF2 Cl 2)n团簇。CF_2Cl_2分子和团簇在ArN上的光解离导致Cl碎片的笼化。另一方面,吸附在(H2O)N冰纳米颗粒上的CF2 Cl 2分子不形成簇,并且从它们的光解离中没有观察到Cl碎片。由于CF2 Cl 2分子明显吸附在(H2O)N上,因此缺失的Cl信号可以解释为表面取向,可能是通过所谓的卤键和/或CF2 Cl 2分子嵌入在冰纳米颗粒的无序表面上。
The photochemistry of CF2Cl2 molecules deposited on argon and ice nanoparticles was investigated. The clusters were characterized via electron ionization mass spectrometry, and the photochemistry was revealed by the Cl fragment velocity map imaging after the CF2Cl2 photodissociation at 193 nm. The complex molecular beam experiment was complemented by ab initio calculations. The (CF2Cl2)n clusters were generated in a coexpansion with Ar buffer gas. The photodissociation of molecules in the (CF2Cl2)n clusters yields predominantly Cl fragments with zero kinetic energy: caging. The CF2Cl2 molecules deposited on large argon clusters in a pickup experiment are highly mobile and coagulate to form the (CF2Cl2)n clusters on ArN. The photodissociation of the CF2Cl2 molecules and clusters on ArN leads to the caging of the Cl fragment. On the other hand, the CF2Cl2 molecules adsorbed on the (H2O)N ice nanoparticles do not form clusters, and no Cl fragments are observed from their photodissociation. Since the CF2Cl2 molecule was clearly adsorbed on (H2O)N, the missing Cl signal is interpreted in terms of surface orientation, possibly via the so-called halogen bond and/or embedding of the CF2Cl2 molecule on the disordered surface of the ice nanoparticles.
DOI: 10.1126/science.1225468
发表时间: 2012-09-21
期刊: SCIENCE
影响因子: 56.9
作者:
Pradzynski, Christoph C.;Forck, Richard M.;Buck, Udo
通讯作者: Buck, Udo