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arXiv:1805.08116

Sub-cycle attosecond control in frustrated double ionization of molecules with orthogonally polarized two-color laser fields

Vilà, A., G. P. Katsoulis, Agapi Emmanouilidou

Published May 21, 2018• 0 citations
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Abstract

We demonstrate sub-cycle control of frustrated double ionization (FDI) in 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 control FDI triggered by a strong near-infrared laser field with a weak mid-infrared laser field. This control as a function of the time delay between the two pulses is demonstrated when the FDI probability and the distribution of the momentum of the escaping electron along the mid-infrared laser field are considered in conjunction. We find that the momentum distribution of the escaping electron has a hive-shape with features that can accurately be mapped to the time one of the two electrons tunnel-ionizes at the start of the break-up process. This mapping distinguishes consecutive tunnel-ionization times within a cycle of the mid-infrared laser field.

DOI
10.48550/arxiv.1805.08116

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We demonstrate sub-cycle control of frustrated double ionization (FDI) in the two-electron triatomic molecule D3+_3^+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 control FDI triggered by a strong near-infrared laser field with a weak mid-infrared laser field. This control as a function of the time delay between the two pulses is demonstrated when the FDI probability and the distribution of the momentum of the escaping electron along the mid-infrared laser field are considered in conjunction. We find that the momentum distribution of the escaping electron has a hive-shape with features that can accurately be mapped to the time one of the two electrons tunnel-ionizes at the start of the break-up process. This mapping distinguishes consecutive tunnel-ionization times within a cycle of the mid-infrared laser field.
We demonstrate a significant enhancement of frustrated double ionization (FDI) in the two-electron triatomic molecule D3+{\mathrm{D}}_{3}{}^{+}D3​+ 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.
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We theoretically investigate strong-field ionization of hydrogen atoms by orthogonally polarized two-color (OTC) laser pulses consisting of a fundamental field that is resonant with the 1s - 2p transition and its second harmonic. Numerical simulations are performed by solving the two-dimensional time-dependent Schrödinger equation and recording the photoelectron momentum distribution. In this strong-field resonant ionization, the atom undergoes many Rabi cycles and the electron can be emitted within a completed Rabi-cycle leading to the splitting of the localized momentum distribution. Here, the splitting is attributed to dynamic Rabi-splitting as a result of the dynamic Stark effect. The employed OTC scheme is shown to be efficient for controlling the dynamic Rabi-splitting through the control of quantum-path interferences involved in one-photon and two-photon absorption processes. The control scheme is accomplished by varying the relative ratio intensity and optical phase between the two pulses, and its footprint is mapped in the momentum distribution. This is shown to lead to an asymmetric distribution and suppression of the ionization process. The obtained results suggest the OTC scheme as a tool for coherent control of dynamic Rabi-oscillations via the controlled quantum-path interferences, thus opening new directions towards designing quantum states via the control OTC scheme.
We study the control of ionization dynamics of aligned N2{\mathrm{N}}_{2}N2​ and O2{\mathrm{O}}_{2}O2​ molecules in orthogonally polarized two-color (OTC) fields and calculate the photoelectron momentum distributions of molecules by solving the time-dependent Schr\"odinger equation and with a semiclassical model. In contrast with that of atoms in the OTC field, we show that the photoelectron momentum distribution is essentially dependent on the molecular outmost orbital, the alignment angle, and the phase of the OTC field. We illustrate the controlling of the molecular frame photoelectron angular distributions and the temporal and spatial double-slit interference effect for strong-field ionization of N2{\mathrm{N}}_{2}N2​ molecules. For O2{\mathrm{O}}_{2}O2​ molecules, it is shown that the ionization wave packets are splitting. The temporal and spatial double-slit interference effect is always present for O2{\mathrm{O}}_{2}O2​, which is not able to be turned off using the OTC field. This work would have implications for probing molecular structures with a two-color synthesized laser field.
Orthogonally polarized two-color sequential laser pulses are used to control the electron localization in the dissociation of H2+{}_{2}{}^{+}2​+. The first single attosecond pulse, whose polarization axis is perpendicular to the molecular axis, excites H2+{}_{2}{}^{+}2​+ from $1s{\ensuremath{\sigma}}_{g}$ to $2p{\ensuremath{\pi}}_{u}$, and the time-delayed infrared pulse, whose polarization axis is parallel to the molecular axis, steers the electron between two nuclei. The simulation of the time-dependent Schr\"odinger equation predicts the control degree of the electron localization can be up to 90% with the current laser technology. In this article, we reveal that the mechanism for this asymmetric localization is due to the mixture of $2p{\ensuremath{\pi}}_{g}$ and $2p{\ensuremath{\pi}}_{u}$, instead of $1s{\ensuremath{\sigma}}_{g}$and $2p{\ensuremath{\sigma}}_{u}$ in the previous studies.
A model which describes the time evolution of strong-field photoionization of atoms is presented. Based on the numerical solution of the non-stationary Schrodinger equation, the model allows one to predict and to interpret the results of experiments on double photoionization of atoms by a combined action of a very short (attosecond) XUV pulse and a few-cycle IR pulse of a powerful laser at various delay times between the two pulses. Depending on the binding energy of the ionized electron, two types of processes are considered. If the electron is tightly bound (Ne case), the XUV pulse ionizes the atom and shakes up another (outer) electron to an excited state, which is subsequently ionized by the strong IR field. For an atom with a weakly bound outer electron (Li case), the IR field ionizes the latter, while the XUV pulse, ionizing the inner shell, terminates (or suppresses) the strong-field ionization. In both cases the yield of doubly ionized ions strongly depends on the delay time between the two pulses, revealing 'steps', oscillations and other features which characterize the time evolution of the ionization process. The presented model describes qualitatively the results of recent experiments on Ne.