Ultrafast Laser-Induced Isomerization Dynamics in Acetonitrile

McDonnell, Matteo; LaForge, Aaron; Reino-González, Juan; Disla, Martin; Kling, Nora G.; Mishra, Debadarshini; Obaid, Razib; Sundberg, Margaret; Svoboda, Vít; Díaz‐Tendero, Sergio; Martín, Fernando; Berrah, N.

doi:10.1021/acs.jpclett.0c01344

Cited by 26 publications

(33 citation statements)

References 25 publications

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“…In particular, for the ionic organic molecules, numerous studies have been conducted to elucidate the formation and evolution of ultrafast hydrogen migration through the sophisticated momentum imaging techniques [5][6][7][8][9][10][11][12][13][14][15][16][17] . It has been found that the hydrogen-migration channel can dominate over direct fragmentation in molecular cations 5 . In addition to the well-known single hydrogen migration, another more complicated process, that is, the double hydrogen migration has been proven to play a more important role than generally assumed in molecular fragmentation 6 .…”

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confidence: 99%

Formation of H3+ from ethane dication induced by electron impact

et al. 2020

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Hydrogen migration plays an important role in the chemistry of hydrocarbons which considerably influences their chemical functions. The migration of one or more hydrogen atoms occurring in hydrocarbon cations has an opportunity to produce the simplest polyatomic molecule, i.e. H3+. Here we present a combined experimental and theoretical study of H3+ formation dynamics from ethane dication. The experiment is performed by 300 eV electron impact ionization of ethane and a pronounced yield of H3+ + C2H3+ coincidence channel is observed. The quantum chemistry calculations show that the H3+ formation channel can be opened on the ground-state potential energy surface of ethane dication via transition state and roaming mechanisms. The ab initio molecular dynamics simulation shows that the H3+ can be generated in a wide time range from 70 to 500 fs. Qualitatively, the trajectories of the fast dissociation follow the intrinsic reaction coordinate predicted by the conventional transition state theory. The roaming mechanism, compared to the transition state, occurs within a much longer timescale accompanied by nuclear motion of larger amplitude.

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Formation of H3+ from ethane dication induced by electron impact

et al. 2020

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“…In each trajectory, E exc was randomly redistributed among the nuclear degrees of freedom. This method has been used with success in the past to study the fragmentation dynamics of ionized molecules and clusters of different nature [26][27][28][29][30][31][32][33].…”

Section: Computational Detailsmentioning

confidence: 99%

Total Electron Detachment and Induced Cationic Fragmentation Cross Sections for Superoxide Anion (O2−) Collisions with Benzene (C6H6) Molecules

Guerra

Kumar

Aguilar-Galindo

et al. 2022

IJMS

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In this study, novel experimental total electron detachment cross sections for O2− collisions with benzene molecules are reported for the impact energy range (10–1000 eV), as measured with a transmission beam apparatus. By analysing the positively charged species produced during the collision events, relative total ionisation cross sections were derived in the incident energy range of 160–900 eV. Relative partial ionisation cross sections for fragments with m/z ≤ 78 u were also given in this energy range. We also confirmed that heavier compounds (m/z > 78 u) formed for impact energies between 550 and 800 eV. In order to further our knowledge about the collision dynamics governing the fragmentation of such heavier molecular compounds, we performed molecular dynamics calculations within the framework of the Density Functional Theory (DFT). These results demonstrated that the fragmentation of these heavier compounds strongly supports the experimental evidence of m/z = 39–42, 50, 60 (u) cations formation, which contributed to the broad local maximum in the total ionisation observed from 550 to 800 eV. This work reveals the reactivity induced by molecular anions colliding with hydrocarbons at high energies, processes that can take place in the interstellar medium under various local conditions.

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“…The Coulomb explosion imaging method provides instantaneous 3D imaging of nuclear positions [54], such as the structure of hydrogen dimers [55], laser-induced isomerization in acetonitrile (CH 3 CN) [56] and photodissociation dynamics of chlorocarbonylsulfenyl chloride [27] and CH 2 BrI [57]. In CEI experiments, the bonding electrons of molecules are stripped away by ultrashort lasers in a time scale shorter than nuclear motion, leaving positive ions in the positions of molecular nuclei.…”

Section: Coulomb Explosion Imagingmentioning

confidence: 99%

Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

Zhang¹,

Guo²,

Mi³

et al. 2022

Preprint

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The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, x-ray and electron sources have enabled the direct imaging of evolving molecular structures in chemical processes.And recent experimental advances in preparing ultrafast laser and electron pulses equipped molecular imaging with femtosecond time resolution. This Perspectives present an overview of versatile imaging methods of molecular dynamics. High-order harmonic generation imaging maps the harmonic order of photons to the time delay for nuclear motion and can reach attosecond time resolution. Coulomb explosion imaging retrieves molecular structural information by detecting the momentum vectors of fragmented ions. Diffraction imaging encodes molecular structural and electronic information in reciprocal space, achieving high spatial resolution by using x-ray or electrons with short wavelengths. The enhancement of x-ray and electron source brightness pushes diffraction into single molecular limit without the restriction of crystalline materials. Laser-induced electron diffraction is a self-imaging method based on coherent electron scattering. We also present various applications of these ultrafast imaging methods in resolving laser-induced nuclear and electronic dynamics, as well as dynamic symmetry evolution of molecules.

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Ultrafast Laser-Induced Isomerization Dynamics in Acetonitrile

Cited by 26 publications

References 25 publications

Formation of H3+ from ethane dication induced by electron impact

Formation of H3+ from ethane dication induced by electron impact

Total Electron Detachment and Induced Cationic Fragmentation Cross Sections for Superoxide Anion (O2−) Collisions with Benzene (C6H6) Molecules

Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

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