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Register a new userExperimental Separation of Sub-Cycle Ionization Bursts in Strong-Field Double Ionization of H$_2$
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We report on the unambiguous observation of the sub-cycle ionization bursts in sequential strong-field double ionization of H$_2$ and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase in combination with multi-particle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state specific Coulomb-distortions on emitted electrons in polyatomic molecules.
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We present state-selective measurements on the NH$_2^{+}$ + H$^{+}$ and NH$^{+}$ + H$^{+}$ + H dissociation channels following single-photon double ionization at 61.5 eV of neutral NH$_{3}$, where the two photoelectrons and two cations are measured in coincidence using 3-D momentum imaging. Three dication electronic states are identified to contribute to the NH$_2^{+}$ + H$^{+}$ dissociation channel, where the excitation in one of the three states undergoes intersystem crossing prior to dissociation, producing a cold NH$_2^+$ fragment. In contrast, the other two states directly dissociate, producing a ro-vibrationally excited NH$_2^+$ fragment with roughly 1 eV of internal energy. The NH$^{+}$ + H$^{+}$ + H channel is fed by direct dissociation from three intermediate dication states, one of which is shared with the NH$_2^{+}$ + H$^{+}$ channel. We find evidence of autoionization contributing to each of the double ionization channels. The distributions of the relative emission angle between the two photoelectrons, as well as the relative angle between the recoil axis of the molecular breakup and the polarization vector of the ionizing field, are also presented to provide insight on both the photoionization and photodissociation mechanisms for the different dication states.
We report measurements on the H$^{+}$ + H$^{+}$ fragmentation channel following direct single-photon double ionization of neutral NH$_{3}$ at 61.5 eV, where the two photoelectrons and two protons are measured in coincidence using 3-D momentum imaging. We identify four dication electronic states that contribute to H$^{+}$ + H$^{+}$ dissociation, based on our multireference configuration-interaction calculations of the dication potential energy surfaces. The extracted branching ratios between these four dication electronic states are presented. Of the four dication electronic states, three dissociate in a concerted process, while the fourth undergoes a sequential fragmentation mechanism. We find evidence that the neutral NH fragment or intermediate NH$^+$ ion is markedly ro-vibrationally excited. We also identify differences in the relative emission angle between the two photoelectrons as a function of their energy sharing for the four different dication states, which bare some similarities to previous observations made on atomic targets.
An ionization-induced plasma grating can be formed by spatially selective ionization of gases by the interference of two intersecting ultra-short laser pulses. The density modulation of a plasma grating can approach unity since the plasma is produced only where the two pulses constructively interfere and ionization does not occur in destructive interference regions. Such a large density modulation leads to efficient Thomson scattering of a second ultra-short probe pulse once the Bragg condition is satisfied. By measuring the scattering efficiency, it is possible to determine the absolute electron density in the plasma grating and thereby deduce the ionization degree for a given neutral gas density. In this paper, we demonstrate the usefulness of this concept by showing two applications: ionization degree measurement of strong-field ionization of atoms and molecules and characterization of extremely low-density gas jets. The former application is of particular interest for ionization physics studies in dense gases where the collision of the ionized electron with neighboring neutrals may become important-sometimes referred to as many-body ionization, and the latter is useful for plasma-based acceleration that requires extremely low-density plasmas.
A nonlinear interferometry scheme is described theoretically to induce and resolve electron wave- function beating on time scales shorter than the optical cycle of the time-delayed pump and probe pulses. By employing two moderately intense few-cycle laser fields with a stable carrier-envelope phase, a large range of the entire electronic level structure of a quantum system can be retrieved. In contrast to single-photon excitation schemes, the retrieved electronic states include levels that are both dipole- and non-dipole-accessible from the ground electronic state. The results show that strong-field interferometry can reveal both high-resolution and broad-band spectral information at the same time with important consequences for quantum-beat spectroscopy on attosecond or even shorter time scales.
We investigate the role of nuclear motion and strong-field-induced electronic couplings during the double ionization of deuterated water using momentum-resolved coincidence spectroscopy. By examining the three-body dicationic dissociation channel, D$^{+}$/D$^{+}$/O, for both few- and multi-cycle laser pulses, strong evidence for intra-pulse dynamics is observed. The extracted angle- and energy-resolved double ionization yields are compared to classical trajectory simulations of the dissociation dynamics occurring from different electronic states of the dication. In contrast with measurements of single photon double ionization, pronounced departure from the expectations for vertical ionization is observed, even for pulses as short as 10~fs in duration. We outline numerous mechanisms by which the strong laser field can modify the nuclear wavefunction en-route to final states of the dication where molecular fragmentation occurs. Specifically, we consider the possibility of a coordinate-dependence to the strong-field ionization rate, intermediate nuclear motion in monocation states prior to double ionization, and near-resonant laser-induced dipole couplings in the ion. These results highlight the fact that, for small and light molecules such as D$_2$O, a vertical-transition treatment of the ionization dynamics is not sufficient to reproduce the features seen experimentally in the strong field coincidence double-ionization data.
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