Smallest Organic Tetracation in the Gas Phase: Stability of Multiply Charged Diiodoacetylene Produced in Intense Femtosecond Laser Fields,The Journal of Physical Chemistry A

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Smallest Organic Tetracation in the Gas Phase: Stability of Multiply Charged Diiodoacetylene Produced in Intense Femtosecond Laser Fields
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2021-09-07 , DOI: 10.1021/acs.jpca.1c06390
Takashi Kawaguchi ₁ , Kosei Kitagawa ₁ , Kazuo Toyota ₁ , Masatoshi Kozaki ₁ , Keiji Okada ₁ , Nobuaki Nakashima ₁ , Tomoyuki Yatsuhashi ₁

Affiliation

Coulomb explosion imaging, which is the reconstruction of a molecular structure by measuring the three-dimensional momenta of atomic ions formed by a Coulomb explosion of multiply charged molecular cations (MMCs), has been utilized widely. In contrast, intact MMCs, whose properties and reactions are interesting from both fundamental and applied scientific perspectives, themselves have been little explored to date. This study demonstrates that the four-atom molecule diiodoacetylene (DIA) can survive as a long-lived species in the gas phase after the removal of four electrons in intense femtosecond laser fields. The electron configurations of the equilibrium structures of the electronic ground states calculated by the complete active space self-consistent field (CASSCF) method reveal the stability of multiply charged DIA. The dissociation energies are estimated to be 3.01, 3.59, 2.57, 1.82, and 1.61 eV for neutral, cation radical, dication, trication radical, and tetracation, respectively. A fairly deep potential well suggests that a DIA tetracation is metastable toward dissociation, whereas the repulsive potential of a pentacation radical confirms its absence in the mass spectrum. With their sufficiently long lifetimes, minimum number of atoms, and simple dissociation paths, DIA MMCs are promising candidates for further experimental and theoretical investigations of multiply charged ion chemistry.

中文翻译：

气相中最小的有机四阳离子：在飞秒强激光场中产生的多电荷二碘乙炔的稳定性

库仑爆炸成像是通过测量多电荷分子阳离子 (MMC) 的库仑爆炸形成的原子离子的三维动量来重建分子结构的方法，已被广泛应用。相比之下，从基础和应用科学的角度来看，其性质和反应都很有趣的完整 MMCs 本身迄今为止很少被探索。这项研究表明，在强飞秒激光场中去除四个电子后，四原子分子二碘乙炔 (DIA) 可以作为长寿命物种在气相中存活。通过完全活性空间自洽场（CASSCF）方法计算的电子基态平衡结构的电子配置揭示了多电荷DIA的稳定性。中性、阳离子自由基、二阳离子、三阳离子自由基和四阳离子的解离能估计分别为 3.01、3.59、2.57、1.82 和 1.61 eV。相当深的势阱表明 DIA 四阳离子对解离是亚稳态的，而五阳离子自由基的排斥势证实了它在质谱中的缺失。DIA MMC 具有足够长的寿命、最少的原子数和简单的解离路径，是多电荷离子化学进一步实验和理论研究的有希望的候选者。而五阳离子自由基的排斥势证实了它在质谱中的缺失。DIA MMC 具有足够长的寿命、最少的原子数和简单的解离路径，是多电荷离子化学进一步实验和理论研究的有希望的候选者。而五阳离子自由基的排斥势证实了它在质谱中的缺失。DIA MMC 具有足够长的寿命、最少的原子数和简单的解离路径，是多电荷离子化学进一步实验和理论研究的有希望的候选者。

更新日期：2021-09-16

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