A multifaceted agreement between ab initio theoretical predictions and experimental measurements, including branching ratios, channel-specific kinetic energy release, three-body momentum correlation spectra, leads to the identification of new mechanisms in Coulomb-explosion (CE) induced two- breakup processes methanol. These identified include direct nonadiabatic Coulomb explosion responsible for CO bond-breaking, a long-range " inverse harpooning" dominating production H2+ + HCOH+,...

The time scales and formation mechanisms of tri-hydrogen cation products in organic molecule ionization processes are poorly understood, despite their cardinal role the chemistry interstellar medium other chemical systems. Using an ultrafast extreme-ultraviolet pump time-resolved near-IR probe, combined with high-level ab initio molecular dynamics calculations, here we report unambiguously that H3+ double-ionization methanol occurs on a sub 100 fs scale, settling previous conflicting...

Two- and three-body Coulomb explosion dynamics of isolated ethanol dications are studied via single-photon double-ionization with ultrafast extreme-ultraviolet pulses. The measured 3-body momentum correlations obtained 3D coincidence imaging the ionic products provide evidence for several concerted sequential mechanisms: (1) a breakup mechanism, dominating channels such as CH3+ + COH+ H2; (2) dissociation in which ejection low-kinetic-energy neutral OH precedes C2H52+ → CH2+; (3) mechanism...

Electron-transfer reactions are ubiquitous in chemistry and biology. The electrons' quantum nature allows their transfer across long distances. For example, the well-known harpoon mechanism, electron results Coulombic attraction between initially neutral reactants, leading to a marked increase reaction rate. Here, we present different mechanism which from reactant multiply charged cation strong repulsion that encodes electron-transfer distance kinetic energy release. Three-dimensional...

We study the competing mechanisms involved in Coulomb explosion of 2-propanol CH32CHOH2+ dication, formed by an ultrafast extreme ultraviolet pulse. Over 20 product channels are identified and characterized using 3D coincidence imaging ionic fragments. The momentum correlations three-body fragmentation provide evidence for a dominant sequential mechanism, starting with cleavage C-C bond, ejecting CH3+ CH3CHOH+ cations, followed secondary hydroxyethyl cation that can be delayed up to...

Photoionization can initiate structural reorganization of molecular matter and drive formation new chemical bonds. Here, we used time-resolved extreme ultraviolet (EUV) pump – EUV probe Coulomb explosion imaging carbon dioxide dimer ion $${\left({{{\rm{C}}}}{{{{\rm{O}}}}}_{2}\right)}_{2}^{+}$$ dynamics, that combined with ab initio dynamics simulations, revealed unexpected asymmetric rearrangement. We show ionization by the pulse induces rearrangement from slipped-parallel (C2h) geometry...

Despite the abundance of data concerning single-photon double ionization methanol, spin state emitted electron pair has never been determined. Here we present first evidence that identifies as overwhelmingly singlet when dication forms in low-energy configurations. The experimental show while yield CH

Abstract The trihydrogen ion has a central role in creating complex molecules the interstellar medium. Therefore, its formation and destruction mechanisms high photon energy environments involving organic are drawing significant experimental theoretical attention. Here, we employ combination of time‐resolved ultrafast extreme‐ultraviolet pump near‐infrared probe spectroscopy applied to deuterated CH 3 OD methanol molecule. Similar other double‐ionization studies, isotopic labeling reveals...

Triatomic Coulomb explosion dynamics are initiated by single-photon double ionization of N2O with an ultrafast EUV pulse and probed delayed near-IR pulses. The triatomic benchmark system exhibits competing two- three-body dissociation that reflected in the time resolved branching ratios co-linear momentum correlation spectra. Both N-NO NN-O bond channels result vibrationally excited molecular products. Channel kinetic energy release (KER) spectra exhibit shifts emerging at long probe delays...

CO2 single-photon double photoionization, Coulomb explosion, and dissociative ionization are studied with ultrafast extreme-ultraviolet pump time-delayed near-infrared probe pulses. Kinetic energy release momentum correlations for the two-body CO+ + O+ three-body C+ O fragmentation products determined by 3D coincidence fragment imaging. The transient enhancement of ratio vs explosion events time dependence low high kinetic dissociation discussed in terms dynamics.

Dissociative electron attachment (DEA) to acetone is studied in terms of the absolute cross section for various fragment channels energy range 0–20 eV. H− found be most dominant followed by O− and OH− with only one resonance peak between 8 9 The DEA dynamics measuring angular distribution kinetic anions using Velocity Slice Imaging technique. fragments suggest a many body break-up lone observed. ab initio calculations show that captured multi-centered anti-bonding molecular orbital which...

We report the molecular dynamics of dissociative electron attachment to sulfur dioxide (SO2) by measuring momentum distribution fragment anions using velocity slice imaging technique in energy range 2-10 eV. The S- channel results from symmetric dissociation which exhibits competition between stretch mode and bending vibration excited parent anion. asymmetric leads production O- SO- channels where corresponding neutral fragments are formed their ground as well electronic states. also...

The negative ion resonances in molecular chlorine are probed using velocity slice imaging of the Cl− fragment produced dissociative electron attachment (DEA). capability to cover entire 360° allows us obtain clear evidence for presence resonance 2.5 eV DEA peak along with is expected be contributor only 0 peak. Its calls a relook at theoretical calculations which have not identified any We also identify and 5.6 momentum images indicate no signature resonant contribution dipolar dissociation...

A nanocluster ionized by a femtosecond pulse of wavelength larger than the cluster size is known to set up an electron cloud that oscillates with respect ion cloud. Most theoretical frameworks on understanding ionization are built this dipole oscillation model. Here, we probe pump-probe absorption spectroscopy. linearly polarized pump sets and polarization comes after prescribed time varied, differential changes in measured. The dependence gives direct measure asymmetry ellipticity...

The velocity Slice Imaging technique has revolutionised electron molecule interaction studies. Multiple electrostatic lens assemblies are often used in spectrometers for resolving low kinetic energy fragments. However, a crossed-beam experiment with an effusive molecular beam, the extended source of ion generation due to presence background gas creates artefacts on momentum images as we try magnify them beyond certain size. Here, present systematic study this effect imaging and solutions...

We report, for the first time, detailed dynamics of dissociative electron attachment to atmospherically important chlorine dioxide (OClO) molecule exploring all product anion channels. Below 2 eV, production vibrationally excited OCl- dominates DEA process whereas at energies greater than three-body dissociation is found result in O- and Cl- production. find that internal energy kinetic are large enough them be relevant ozone-depleting catalytic cycle more investigations on reaction these...

Synopsis Dissociative electron attachment (DEA) is the most efficient way to explore structure and dynam-ics of excited states molecular negative ions. More importantly, DEA has been shown be a tool for chemical control. One crucial aspect control using functional group dependence present in this process. Here we cases on effect delocalized electrons patterns observed simple aromatic compounds.

We report the study of dissociative electron attachment to molecular chlorine in energy range 1 20 eV using velocity slice imaging technique. Based on angular distributions at various energies, we identify partial waves involved resonance formation that lead DEA.

We report the study of dissociative electron attachment to ozone (O3) in energy range 1 10 eV using velocity slice imaging technique. Based on momentum images that we obtained for O− and O2− channels at various energies unravel molecular dynamics leading DEA.

We report the study of dissociative electron attachment (DEA) to chlorine dioxide (OClO) in energy range 1 10 eV using velocity slice imaging technique. DEA OClO shows Cl−, O−, O2−, and OCl− as fragment channels at various energies. Based on momentum images these ions we unravel molecular dynamics leading DEA.

The Velocity Slice Imaging technique has revolutionized electron molecule interaction studies. Multiple electrostatic lens assemblies are often used in spectrometers for resolving low kinetic energy fragments. In a crossed-beam experiment with an effusive molecular beam, the background gas forms strong extended source of ions where charged particle projectile beam is without focusing. This creates artefacts on momentum images as we try to magnify them beyond certain size. Here, present...

We have investigated the dynamics of dissociative electron attachment to sulfur dioxide (SO2) using velocity slice imaging (VSI) technique. The symmetric dissociation transient parent anion results in S− formation whereas its asymmetric O− and SO− channels. clearly see competition between bending stretch mode vibrations anions modes dominate other two ions production.