Photoelectron angular distributions from resonant two-photon ionisation of adiabatically aligned naphthalene and aniline molecules

Photoelectron angular distributions from resonant two-photon ionisation of adiabatically aligned naphthalene and aniline molecules
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DOI:
10.1080/00268976.2020.1836411
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发表时间:
2020-10
期刊:
影响因子:
1.7
通讯作者:
Jacqueline Arlt;Dhirendra P. Singh;James O. F. Thompson;A. Chatterley;P. Hockett;H. Stapelfeldt;K. L. Reid
Jacqueline Arlt;Dhirendra P. Singh;James O. F. Thompson;A. Chatterley;P. Hockett;H. Stapelfeldt;K. L. Reid
中科院分区:
化学4区
文献类型:
--
作者:
Jacqueline Arlt;Dhirendra P. Singh;James O. F. Thompson;A. Chatterley;P. Hockett;H. Stapelfeldt;K. L. Reid

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本文测量了气相萘和苯胺分子排列分布电离后的光电子像。通过与100 ps红外激光脉冲的相互作用实现了绝热状态下的对准,并使用持续时间为0.6ps的低强度紫外脉冲在双光子共振方案中实现了电离。所得到的图像被发现表现出各向异性,增加时的对齐脉冲存在,与苯胺PAD峰值沿着的电离光和萘PAD的偏振矢量开发一个特性的四叶结构。使用ePolyScat从头算套件计算由分子的未对准和完全对准分布的电离产生的光电子角分布(PAD),并将其转换为二维光电子图像。在萘的情况下,观察到实验和模拟之间的完全对齐的分布,显示出的对齐步骤,使我们能够探测分子框架,但在苯胺的情况下,很明显,额外的过程发生后的单光子共振步骤。图形摘要
ABSTRACT Photoelectron images have been measured following the ionisation of aligned distributions of gas phase naphthalene and aniline molecules. Alignment in the adiabatic regime was achieved by interaction with a 100 ps infrared laser pulse, with ionisation achieved in a two-photon resonant scheme using a low intensity UV pulse of ∼6 ps duration. The resulting images are found to exhibit anisotropy that increases when the alignment pulse is present, with the aniline PADs peaking along the polarisation vector of the ionising light and the naphthalene PADs developing a characteristic four-lobed structure. Photoelectron angular distributions (PADs) that result from the ionisation of unaligned and fully aligned distributions of molecules are calculated using the ePolyScat ab initio suite and converted into two-dimensional photoelectron images. In the case of naphthalene excellent agreement is observed between experiment and the simulation for the fully aligned distribution, showing that the alignment step allows us to probe the molecular frame, but in the case of aniline it is clear that additional processes occur following the one-photon resonant step. GRAPHICAL ABSTRACT