The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields

Jochim, Bethany; Zohrabi, M.; Voznyuk, O.; Mahowald, J.B.; Schmitz, Dominik; Betsch, K. J.; Berry, Ben; Severt, T.; Kling, Nora G.; Burwitz, T.G.; Carnes, K. D.; Kling, Matthias F.; Ben‐Itzhak, I.; Wells, E.; Vivie‐Riedle, Regina de

doi:10.1038/s41598-017-04638-0

Cited by 14 publications

(10 citation statements)

References 97 publications

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“…allows us to conclude transformation of the LUMO results from a large stabilization of one of the Rydberg orbitals upon application of large E-fields. Such E-field-induced stabilization of Rydberg orbitals is in line with the results recently found for ethylene in intense laser fields 54. In broader terms, the strong decrease of the HOMO-LUMO gap found for biphenyl derivatives under large fields is also in line with the results reported in Ref 55.…”

supporting

confidence: 91%

Twistable dipolar aryl rings as electric field actuated conformational molecular switches

Lozano

Santiago

Ribas‐Ariño

et al. 2021

Phys. Chem. Chem. Phys.

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supporting

confidence: 91%

Twistable dipolar aryl rings as electric field actuated conformational molecular switches

Lozano

Santiago

Ribas‐Ariño

et al. 2021

Phys. Chem. Chem. Phys.

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“…with those of FigureS4allows us to conclude transformation of the LUMO results from a large stabilization of one of the Rydberg orbitals upon application of large E-fields. Such E-field-induced stabilization of Rydberg orbitals is in line with the results recently found for ethylene in intense laser fields 54. In broader terms, the strong decrease of the HOMO-LUMO gap found for biphenyl derivatives under large fields is also in line with the results reported in Ref 55.…”

supporting

confidence: 91%

Twistable Dipolar Aryl Rings as Electric Field Actuated Conformational Molecular Switches

Lozano¹,

Santiago²,

Ribas‐Ariño³

et al. 2020

Preprint

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The ability to control the chemical conformation of a system via external stimuli is a promsing route for developing molecular switches. For eventual deployment as viable sub-nanoscale components that are compatible with current electronic device technology, conformational switching should controllable by a local electric field (i.e. E-field gateable) and accompanied by a rapid change in conduction. In organic chemical systems the degree of π-conjugation is linked to the degree of electronic delocalisation, and thus largely determines the conductivity. Here, by means of accurate first principles calculations, we study the prototypical biphenyl based molecular system in which the dihedral angle between the two rings determines the degree of conjugation. In order to make this a gateable system we create a net dipole by asymmetrically functionalising one ring with electronegative substituents (F, Br and CN) with different polarisabilities. In this way, the application of an E-field interacts with the dipolar system to influence the dihedral angle, thus controlling the conjugation. For all three considered substituents we consider a range of E-fields, and in each case extract conformational energy profiles. Using this data we obtain the minimum E-field required to induce a barrierless switching event for each system. We further extract the estimated switching speeds, the conformational probabliities at finite temperatures, and the effect of applied E-field on electronic structure. Consideration of these data allow us to assess which factors are most important in the design of efficient gateable electrical molecular switches.

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“…Moreover, this method can be directly applied to experiments on electron trapping in laser-induced molecular ionization and dissociation processes using multi-particle coincidence detection. This may trigger new research on the impact of Rydberg elec-trons on laser-induced molecular reactions and the interaction between Rydberg atoms and/or molecules [38][39][40].…”

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confidence: 99%

Frustrated double ionization of argon atoms in strong laser fields

Larimian

Erattupuzha

Baltuška

et al. 2020

Phys. Rev. Research

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We demonstrate kinematically complete measurements on frustrated double ionization of argon atoms in strong laser fields with a reaction microscope. We found that the electron trapping probability after strong field double ionization is much higher than that after strong field single ionization, especially in case of high laser intensity. The retrieved electron momentum distributions of frustrated double ionization show a clear transition from the nonsequential to the sequential regime, similar to those of strong field double ionization. The dependence of electron momentum width on the laser intensity further indicates that the second released electron has a dominant contribution to frustrated double ionization in the sequential regime. PACS numbers: 33.80.Rv, 42.50.Hz, 82.50.Nd When an atom or a molecule is exposed to a strong laser field it may become singly or multiply ionized [1,2]. After the strong field interaction, a fraction of the ionized electron wave packets with near-zero kinetic energies can be trapped into high-lying Rydberg states, a process also known as frustrated field ionization [3][4][5][6][7][8][9][10][11]. Frustrated double ionization (electron trapping after double ionization) has been experimentally studied for small molecules, including H 2 and argon dimers, using Coulomb explosion imaging [4][5][6][12][13][14] and theoretically using the classical trajectory Monte Carlo method [15,16]. In these experiments the trapping process is identified by the kinetic energy released (KER) during the Coulomb explosion of the molecules. Since an electron trapped in high-lying Rydberg states does not fully shield the nuclear charge, the KER for a molecule with an electron in Rydberg states is higher than that for a nonexcited molecule. Since this method is based on the measurement of KER from molecules undergoing Coulomb explosion, it is applicable to neither atomic targets nor molecules that do not fragment.In this paper, using an alternative method developed in our previous work [10], we report on kinematically complete experiments of electron trapping processes during strong field double ionization of argon atoms. Strong field double ionization may happen sequentially, where the two electrons are removed one after another by the laser field, or non-sequentially, where the second electron is released during the recollision of the first electron with the parent ion [17][18][19]. We show that the trapping probability is strongly enhanced in the sequential ionization regime. Based on our experimental data we explain the electron dynamics underlying these observations.In our experiments we employed a reaction microscope [20,21] for three-body coincidence detection of two electrons and their parent ion created during the interaction of argon atoms with strong laser pulses ( Fig. 1(a)). Laser pulses linearly polarized along the spectrometer axis (z-direction) were provided by a home-built Titanium:sapphire laser amplifier system. The pulses had a center wavelength of 790 nm, a pulse duration of 25 fs an...

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The importance of Rydberg orbitals in dissociative ionization of small hydrocarbon molecules in intense laser fields

Cited by 14 publications

References 97 publications

Twistable dipolar aryl rings as electric field actuated conformational molecular switches

Twistable dipolar aryl rings as electric field actuated conformational molecular switches

Twistable Dipolar Aryl Rings as Electric Field Actuated Conformational Molecular Switches

Frustrated double ionization of argon atoms in strong laser fields

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