Toolkit for semiclassical computations for strongly driven molecules: Frustrated ionization of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>driven by elliptical laser fields

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

doi:10.1103/physreva.90.053419

Cited by 30 publications

(73 citation statements)

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“…This model has provided significant insights into FDI for strongly-driven H 2 [2] and D [28,31]. We initialize the nuclei at rest for all vibrational levels, since an initial pre-dissociation does not significantly modify the ionization dynamics [32].The combined strength of the two laser fields is within the below-the-barrier ionization regime. To formulate the initial state of the two electrons, we assume that one electron (electron 1) tunnel-ionizes at time t 0 in the field-lowered Coulomb potential.…”

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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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“…The time propagation is classical, starting from time t 0 . We solve the classical equations of motion for the Hamiltonian of the stronglydriven five-body system, while fully accounting for the Coulomb singularities [32].…”

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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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“…In our simulations, we take the three nuclei A, B and C to be on the x-z plane. In addition, we simplify our model by considering the nuclei initially at rest since an initial pre-dissociation does not significantly modify the ionization dynamics [9]. We note that for I p 1 = 1.208 a.u.…”

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“…We have done so in the context of strongly-driven H 2 [8,9]. Our 3D method has several assets, namely, it treats the motion of the electrons and the nuclei at the same time and fully addresses the Coulomb singularity [8,9].…”

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

Chen

Lazarou

Price

et al. 2016

J. Phys. B: At. Mol. Opt. Phys.

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Abstract. Using a semi-classical model, we study the formation of highly excited neutral fragments during the fragmentation of H + 3 , a two-electron triatomic molecule, driven by an intense near-IR laser field. To do so, we first formulate a microcanonical distribution for arbitrary one-electron triatomic molecules. We then study frustrated double and single ionization in strongly-driven H + 3 and compute the kinetic energy release of the nuclei for these two processes. Moreover, we investigate the dependence of frustrated ionization on the strength of the laser field as well as on the geometry of the initial molecular state.

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“…If the second (first) ionization step is "frustrated", we label the FDI pathway as FSIS (FFIS), previously referred to as pathway A (B) [12]. Electron-electron correlation, underlying pathway FFIS [12,15], can be controlled with orthogonally polarised two-color linear (OTC) laser fields [14].Here, we show that counter-rotating two-color circular (CRTC) laser fields are a powerful tool for controlling FDI in strongly-driven molecules. CRTC fields have attracted a lot of interest due to their applicability to the production, via high harmonic generation, of circular pulses with extreme-ultraviolet to soft-x-ray wavelengths [16][17][18][19][20].…”

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Enhancing frustrated double ionization with no electronic correlation in triatomic molecules using counter-rotating two-color circular laser fields

2020

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We demonstrate significant enhancement of frustrated double ionization (FDI) in the two-electron triatomic molecule D + 3 when driven by counter-rotating two-color circular (CRTC) laser fields. We employ a three-dimensional semiclassical model that fully accounts for electron and nuclear motion in strong fields. For different pairs of wavelengths, we compute the probabilities of the FDI pathways as a function of the ratio of the two field-strengths. We identify a pathway of FDI that is not present in strongly-driven molecules with linear fields. In this pathway the first ionization step is "frustrated" and electronic correlation is essentially absent. This pathway is responsible for enhancing FDI with CRTC fields. We also employ a simple model that predicts many of the main features of the probabilities of the FDI pathways as a function of the ratio of the two field-strengths. PACS numbers: 33.80.Rv, 34.80.Gs, 42.50.Hz Formation of highly excited Rydberg states, during the interaction of atoms and molecules with laser fields, is a fundamental problem with a wide range of applications. Rydberg states underlie, for instance, acceleration of neutral particles [1], spectral features of photoelectrons [2], formation of molecules via long-range interactions [3], and inversion of N 2 in free-space air lasing [4]. Recently, the formation of Rydberg states in weakly-driven H 2 was accounted for by electron-nuclear correlated multiphoton resonant excitation [5]. For H 2 driven by intense infrared laser fields (strongly-driven), this latter process was shown to merge with frustrated double ionization (FDI) [5]. FDI accounts for the formation of Rydberg fragments in strongly-driven two-electron molecules. In frustrated ionization an electron first tunnel ionizes in the driving laser field. Then, due to the electric field, this electron is recaptured by the parent ion in a Rydberg state [6]. In FDI an electron escapes while another one occupies a Rydberg state at the end of the laser pulse.For linear laser fields, FDI is a major process during the breakup of strongly-driven molecules, accounting for roughly 10% of all ionization events. Hence, FDI has been the focus of intense experimental studies in the context of H 2 [7], D 2 [8] and of the two-electron triatomic molecules D + 3 and H + 3 [9-11]. For strongly-driven twoelectron diatomic and triatomic molecules, FDI proceeds via two pathways [12][13][14]. One electron tunnel ionizes early on (first step), while the remaining bound electron does so later in time (second step). If the second (first) ionization step is "frustrated", we label the FDI pathway as FSIS (FFIS), previously referred to as pathway A (B) [12]. Electron-electron correlation, underlying pathway FFIS [12,15], can be controlled with orthogonally polarised two-color linear (OTC) laser fields [14].Here, we show that counter-rotating two-color circular (CRTC) laser fields are a powerful tool for controlling FDI in strongly-driven molecules. CRTC fields have attracted a lot of interest due to their applicabi...

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Toolkit for semiclassical computations for strongly driven molecules: Frustrated ionization ofH2driven by elliptical laser fields

Cited by 30 publications

References 62 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

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

Enhancing frustrated double ionization with no electronic correlation in triatomic molecules using counter-rotating two-color circular laser fields

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Toolkit for semiclassical computations for strongly driven molecules: Frustrated ionization ofH2driven by elliptical laser fields

Cited by 30 publications

References 62 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

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

Enhancing frustrated double ionization with no electronic correlation in triatomic molecules using counter-rotating two-color circular laser fields

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