Photofragment Imaging of Carbon Cluster Cations: Explosive Ring Rupture

Photofragment Imaging of Carbon Cluster Cations: Explosive Ring Rupture
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碳簇阳离子的光碎片成像:爆炸环破裂

DOI:
10.1021/acs.jpclett.2c00950
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发表时间:
2022
期刊:
The Journal of Physical Chemistry Letters
影响因子:
--
通讯作者:
Duncan, Michael A.
Duncan, Michael A.
中科院分区:
--
文献类型:
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作者:
Dynak, Nathan J.;Rittgers, Brandon M.;Colley, Jason E.;Kellar, Douglas J.;Duncan, Michael A.

文献摘要

相似文献

激光蒸发产生的碳团簇阳离子(Cn+)在355 nm处被质量选择和光解离。较小离子的多光子解离导致中性C3的消除,如在以前的工作中,而较大的集群表现出更多样的碎裂通道。光碎片速度图成像检测到显着的动能释放(KER)在variousn- 3阳离子片段。具有线性结构的小阳离子(n= 6或7)产生中等KER,而具有单环结构的较大阳离子(n= 10、11、12、15或20)产生高得多的KER值。如此高的KER值是预料不到的,因为光激发应该产生广泛的内能分布。这些碳团簇具有惊人的能力,可以吸收紫外线辐射的多个光子,在解离之前达到极端激发的状态。能量的显着非统计分布显然是由显着的环应变,可以在光解离释放的影响。
Carbon cluster cations (Cn+) produced by laser vaporization are mass selected and photodissociated at 355 nm. Multiphoton dissociation of smaller ions leads to the elimination of neutral C3, as in previous work, whereas larger clusters exhibit more varied fragmentation channels. Photofragment velocity-map imaging detects significant kinetic energy release (KER) in the variousn– 3 cation fragments. Small cations (n= 6 or 7) with linear structures produce moderate KER, whereas larger cations (n= 10, 11, 12, 15, or 20) having monocyclic ring structures produce much higher KER values. Such high KER values are unanticipated, as optical excitation should produce a wide distribution of internal energies. These carbon clusters have a surprising ability to absorb multiple photons of ultraviolet radiation, achieving a state of extreme excitation prior to dissociation. The remarkable nonstatistical distribution of energy is apparently influenced by the significant ring strain that can be released upon photodissociation.