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Register a new userFrustrated double ionization in two-electron triatomic molecules
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Using a semi-classical model, we investigate frustrated double ionization (FDI) in $mathrm{D_3^+}$, a two-electron triatomic molecule, when driven by an intense, linearly polarized, near-infrared (800 nm) laser field. We compute the kinetic energy release of the nuclei and find a good agreement between experiment and our model. We explore the two pathways of FDI and show that, with increasing field strength, over-the-barrier ionization overtakes tunnel ionization as the underlying mechanism of FDI. Moreover, we compute the angular distribution of the ion fragments for FDI and identify a feature that can potentially be observed experimentally and is a signature of only one of the two pathways of FDI.
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Using a semi-classical model, we study the formation of highly excited neutral fragments during the fragmentation of $mathrm{H_3^+}$, 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 $mathrm{H_3^+}$ 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.
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 frustrated double ionization 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 frustrated double ionization 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.
We formulate a microcanonical distribution for an arbitrary one-electron triatomic molecule. This distribution can be used to describe the initial state in strongly-driven two-electron triatomic molecules. Namely, in many semiclassical models that describe ionization of two-electron molecules driven by intense infrared laser fields in the tunneling regime initially one electron tunnels while the other electron is bound. The microcanonical distribution presented in this work can be used to describe the initial state of this bound electron.
We study frustrated double ionization in a strongly-driven heteronuclear molecule HeH$^{+}$ and compare with H$_2$. We compute the probability distribution of the sum of the final kinetic energies of the nuclei for strongly-driven HeH$^{+}$. We find that this distribution has more than one peak for strongly-driven HeH$^{+}$, a feature we do not find to be present for strongly-driven H$_{2}$. Moreover, we compute the probability distribution of the n quantum number of frustrated double ionization. We find that this distribution has several peaks for strongly-driven HeH$^{+}$, while the respective distribution has one main peak and a shoulder at lower n quantum numbers for strongly-driven H$_{2}$. Surprisingly, we find this feature to be a clear signature of the intertwined electron-nuclear motion.
Electron-impact direct double ionization (DDI) process is studied as a sequence of two and three step processes. Contribution from ionization-ionization, ionization-excitation-ionization, and excitation-ionization-ionization processes is taken into account. The present results help to resolve the long-standing discrepancies; in particular, a good agreement with experimental measurements is obtained for double ionization cross-sections of $O^{1+}$, $O^{2+}$, $O^{3+}$, $C^{1+}$, and $Ar^{2+}$ ions. We show that distribution of the energy of scattered and ejected electrons, which participate in the next step of ionization, strongly affects DDI cross-sections.
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