Frustrated double and single ionization in a two-electron triatomic molecule H<sup>+</sup><sub>3</sub>

Chen, Ahai; Lazarou, Constantinos; Price, H. James; Emmanouilidou, A.

doi:10.1088/0953-4075/49/23/235001

Cited by 11 publications

(12 citation statements)

References 38 publications

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“…For electron 1, the velocity component that is transverse to the OTC laser fields is given by a Gaussian [35] and the component that is parallel is set equal to zero. The initial state of the initially bound electron (electron 2) is described by a microcanonical distribution [36].…”

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Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

2017

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We demonstrate the control of electron-electron correlation in frustrated double ionization (FDI) of the two-electron triatomic molecule D + 3 when driven by two orthogonally polarized two-color laser fields. We employ a three-dimensional semi-classical model that fully accounts for the electron and nuclear motion in strong fields. We analyze the FDI probability and the distribution of the momentum of the escaping electron along the polarization direction of the longer wavelength and more intense laser field. These observables when considered in conjunction bear clear signatures of the prevalence or absence of electron-electron correlation in FDI, depending on the time-delay between the two laser pulses. We find that D + 3 is a better candidate compared to H 2 for demonstrating also experimentally that electron-electron correlation indeed underlies FDI.PACS numbers: 33.80. Rv, 34.80.Gs, 42.50.Hz Frustrated double ionization (FDI) is a major process in the nonlinear response of multi-center molecules when driven by intense laser fields, accounting roughly for 10% of all ionization events [1,2]. In frustrated ionization an electron first tunnel-ionizes in the driving laser field. Then, due to the electric field of the laser pulse, it is recaptured by the parent ion in a Rydberg state [3]. This process is a candidate for the inversion of N 2 in free-space air lasing [4]. In FDI an electron escapes and another one occupies a Rydberg state at the end of the laser pulse. In theoretical studies of strongly-driven two-electron diatomic and triatomic molecules, two pathways of FDI have been identified [2,8]. Electron-electron correlation is important, primarily, for one of the two pathways. It is well accepted that electron-electron correlation underlies a significant part of double ionization in strongly-driven molecules-a mechanism known as non-sequential double ionization [9,10]. However, electron-electron correlation in FDI has yet to be accessed experimentally.Here, we propose a road for future experiments to identify the important role of electron-electron correlation in FDI. We identify the parameters of orthogonally polarized two-color (OTC) laser fields that best control the relevant pathway for electron-electron correlation in FDI. We demonstrate traces of attosecond control of electron motion in space and time in two observables of FDI as a function of the time-delay between the fundamental 800 nm and the second harmonic 400 nm laser field. We show that, together, the FDI probability and the momentum of the escaping electron along the fundamental laser field bear clear signatures of the turning on and off of electronelectron correlation.Two-color laser fields are an efficient tool for controlling electron motion [11,12] and for steering the outcome of chemical reactions [13][14][15]. Other applications include the field-free orientation of molecules [16][17][18], the generation of high-harmonic spectra [19][20][21][22] and probing atomic and molecular orbital symmetry [23][24][25]. The strongly-driven dynam...

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Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

2017

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“…The latter arises from standard tunneling theory [32][33][34] and represents the Gaussian-shaped filter with an intensity-dependent width. The initially two bound electrons (electrons 2 and 3), are each represented by a microcanonical distribution for a triatomic molecule [35]. Each electron is assigned an energy equal to 2.21 a.u., which is half the ground-state energy of HeH 2 2+ .…”

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confidence: 99%

Triple ionization and frustrated triple ionization in triatomic molecules driven by intense laser fields

2021

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We formulate a three-dimensional semiclassical model to treat three-electron escape dynamics in a strongly driven linear triatomic molecule, HeH 2 + . Our model includes the Coulomb singularities. Hence, to avoid unphysical autoionization, we employ two criteria to switch off the Coulomb repulsive force between two bound electrons and switch it on when the motion of one electron is mostly determined by the laser field.We investigate triple and so-called frustrated triple ionization. In the latter process, two electrons escape while one electron remains bound in a Rydberg state. We find that two pathways prevail in frustrated triple ionization, as in frustrated double ionization. We also find that the electron that remains in a Rydberg state is more likely to be attached to He 2+ than to H + . Our results indicate that in triple and frustrated triple ionization electronic correlation is weak. Moreover, we compute the sum of the kinetic energies as well as the angular patterns of the final ion fragments in triple and frustrated triple ionization. These patterns suggest that the fragmenting molecule deviates from its initial linear configuration.

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“…The latter arises from standard tunneling theory [31][32][33] and represents the Gaussian-shaped filter with an intensity-dependent width. The initially two bound electrons (electrons 2 and 3), are each represented by a microcanonical distribution for a triatomic molecule [34]. Each electron is assigned an energy equal to 2.21 a.u., which is half the ground state energy of HeH 2+ 2 .…”

Section: Methodsmentioning

confidence: 99%

Triple ionization and "frustrated" triple ionization in triatomic molecules driven by intense laser fields

Peters,

Majety,

Emmanouilidou

2020

Preprint

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We formulate a three-dimensional semi-classical model to treat three-electron escape dynamics in a strongly-driven linear triatomic molecule, HeH + 2 . Our model includes the Coulomb singularities. Hence, to avoid unphysical autoionization, we employ two criteria to switch off the Coulomb repulsive force between two bound electrons and switch it on when the motion of one electron is mostly determined by the laser field. We investigate triple and "frustrated" triple ionization. In the latter process two electrons escape while one electron remains bound in a Rydberg state. We find that two pathways prevail in "frustrated" triple ionization, as in "frustrated" double ionization. We also find that the electron that remains in a Rydberg state is more likely to be attached to He 2+ compared to H + . Our results indicate that in triple and "frustrated" triple ionization electronic correlation is weak. Moreover, we compute the sum of the kinetic energies as well as the angular patterns of the final ion fragments in triple and "frustrated" triple ionization. These patterns suggest that the fragmenting molecule deviates from its initial linear configuration.

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Frustrated double and single ionization in a two-electron triatomic molecule H⁺₃

Cited by 11 publications

References 38 publications

Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

Triple ionization and frustrated triple ionization in triatomic molecules driven by intense laser fields

Triple ionization and "frustrated" triple ionization in triatomic molecules driven by intense laser fields

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Frustrated double and single ionization in a two-electron triatomic molecule H+3

Cited by 11 publications

References 38 publications

Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

Controlling electron-electron correlation in frustrated double ionization of triatomic molecules with orthogonally polarized two-color laser fields

Triple ionization and frustrated triple ionization in triatomic molecules driven by intense laser fields

Triple ionization and "frustrated" triple ionization in triatomic molecules driven by intense laser fields

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Frustrated double and single ionization in a two-electron triatomic molecule H⁺₃