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Register a new userDissecting strong-field excitation dynamics with atomic-momentum spectroscopy
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Added by
Serguei Patchkovskii
Publication date
2020
fields
Physics
and research's language is
English
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Observation of internal quantum dynamics relies on correlations between the system being observed and the measurement apparatus. We propose using the center-of-mass (c.m.) degrees of freedom of atoms and molecules as a built-in monitoring device for observing their internal dynamics in non-perturbative laser fields. We illustrate the idea on the simplest model system - the hydrogen atom in an intense, tightly-focused infrared laser beam. To this end, we develop a numerically-tractable, quantum-mechanical treatment of correlations between internal and c.m. dynamics. We show that the transverse momentum records the time excited states experience the field, allowing femtosecond reconstruction of the strong-field excitation process. The ground state becomes weak-field seeking, an unambiguous and long sought-for signature of the Kramers-Henneberger regime.
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We report on the experimental observation of strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of $mu$J. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, reveals a direct link between strong-field-induced energy and phase shifts of the doubly excited state and the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of few meV, induced by strong XUV fields. These results open up a new way of performing non-perturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.
Neutral atoms have been observed to survive intense laser pulses in high Rydberg states with surprisingly large probability. Only with this Rydberg-state excitation (RSE) included is the picture of intense-laser-atom interaction complete. Various mechanisms have been proposed to explain the underlying physics. However, neither one can explain all the features observed in experiments and in time-dependent Schr{o}dinger equation (TDSE) simulations. Here we propose a fully quantum-mechanical model based on the strong-field approximation (SFA). It well reproduces the intensity dependence of RSE obtained by the TDSE, which exhibits a series of modulated peaks. They are due to recapture of the liberated electron and the fact that the pertinent probability strongly depends on the position and the parity of the Rydberg state. We also present measurements of RSE in xenon at 800 nm, which display the peak structure consistent with the calculations.
Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (both H$_2$O and D$_2$O) in 10-fs and 40-fs 800-nm laser pulses. We find that 10-fs pulses turn off before substantial internuclear motion occurs, whereas rapid internuclear motion can take place during the double ionization process for 40-fs pulses. The short-pulse measurements are consistent with a simple tunnel ionization picture, whose predictions help interpret the motion observed in the long-pulse measurements.
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.
Imaging structures at the molecular level is a fast developing interdisciplinary research field that spans across the boundaries of physics and chemistry. High spatial resolution images of molecules can be obtained with photons or ultrafast electrons. In addition, images of valence molecular orbitals can be extracted via tomographic techniques based on the coherent XUV radiation emitted by a molecular gas exposed to an intense ultra-short infrared laser pulse. In this paper, we demonstrate that similar information can be obtained by inverting energy resolved photoelectron spectra using a simplified analytical model.
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