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在千兆瓦强度激光辐照下,团簇展开对铁五羰基掺杂惰性气体团簇光致电离的影响。

Effect of cluster expansion on photoionization of iron pentacarbonyl doped inert gas clusters under gigawatt intensity laser irradiation.

机构信息

Chemistry Division, Bhabha Atomic Research Centre, Mumbai 400 085, India.

出版信息

Rapid Commun Mass Spectrom. 2012 Oct 15;26(19):2204-10. doi: 10.1002/rcm.6341.

Abstract

RATIONALE

The aim of the investigation was to understand the variation in ionization dynamics of inert gas clusters upon doping with species with lower ionization energy than the inert gas constituent. It was postulated that the use of dopant species having lower ionization energy would lead to facile ionization of doped inert gas clusters, resulting in enhancement of the charge state of atomic ions compared with those obtained for pure inert gas clusters.

METHODS

Inert gas clusters (Ar(n), Kr(n) or Xe(n)) doped with iron pentacarbonyl were generated by supersonic expansion and subjected to gigawatt intensity laser pulses (266, 355, 532 and 1064 nm wavelengths) obtained from a nanosecond Nd:YAG laser. The ions generated upon laser-cluster interaction were characterized using a time-of-flight mass spectrometer.

RESULTS

Upon interaction of the laser with the doped inert gas clusters, the charge states of the atomic ions were found to increase with the laser wavelength. However, the highest observed charge states were found to be lower for doped inert gas clusters than for pure inert gas clusters, at all laser wavelengths.

CONCLUSIONS

Wavelength-dependent generation of multiply charged atomic ions has been explained based on the three stage model, i.e. multiphoton ionization ignited-inverse bremsstrahlung heating, and electron ionization. This model explains enhancement in the charge state of atomic ions with increasing wavelength based on inverse bremsstrahlung heating of the inner ionized electron, which is a more efficient process at longer wavelengths. Inefficient coupling of laser energy in the case of doped inert gas clusters compared with pure inert gas clusters has been rationalized on the basis of accelerated disintegration of the cluster due to facile initial ionization of dopant molecules having low ionization energy. The results suggest that a longer laser wavelength and a slower rate of cluster expansion facilitate the efficient transfer of optical energy into cluster systems.

摘要

原理

本研究旨在探究惰性气体团簇掺杂电离能低于惰性气体组分的物种后,其离化动力学的变化。假设使用具有较低电离能的掺杂物种将导致掺杂惰性气体团簇的易离化,从而导致与纯惰性气体团簇相比,原子离子的电荷态增强。

方法

通过超声速膨胀产生掺杂有五羰基铁的惰性气体团簇(Ar(n)、Kr(n)或 Xe(n)),并使用纳秒 Nd:YAG 激光获得的千兆瓦强度激光脉冲(266、355、532 和 1064nm 波长)对其进行照射。利用飞行时间质谱仪对激光-团簇相互作用产生的离子进行了表征。

结果

当激光与掺杂惰性气体团簇相互作用时,原子离子的电荷态随着激光波长的增加而增加。然而,在所有激光波长下,掺杂惰性气体团簇的最高观察到的电荷态都比纯惰性气体团簇低。

结论

基于三阶段模型,即多光子电离引发-逆韧致辐射加热和电子电离,解释了多电荷原子离子的波长依赖性产生。该模型基于内电离电子的逆韧致辐射加热来解释原子离子电荷态随波长增加的增强,这在较长波长下是一个更有效的过程。与纯惰性气体团簇相比,掺杂惰性气体团簇中激光能量的耦合效率较低,这是由于具有低电离能的掺杂分子的初始离化导致团簇的快速分解。结果表明,较长的激光波长和较慢的团簇膨胀速率有利于将光能量有效地传递到团簇系统中。

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