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Register a new userStrong-field extreme-ultraviolet dressing of atomic double excitation
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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.
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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.
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.
We present a joint experimental-theoretical study on the effect of the carrier-envelope phase (CEP) of a few-cycle pulse on the atomic excitation process. We focus on the excitation rates of argon as a function of CEP in the intensity range from 50-300 TW/cm$^2$, which covers the transition between the multiphoton and tunneling regimes. Through numerical simulations based on solving the time-dependent Schr{o}dinger equation (TDSE), we show that the resulting bound-state population is highly sensitive to both the intensity and the CEP. Because the intensity varies over the interaction region, the CEP effect is considerably reduced in the experiment. Nevertheless, the data clearly agree with the theoretical prediction, and the results encourage the use of precisely tailored laser fields to coherently control the strong-field excitation process. We find a markedly different behavior for the CEP-dependent bound-state population at low and high intensities with a clear boundary, which we attribute to the transition from the multiphoton to the tunneling regime.
We investigate AC Stark-shifted resonances in argon with ultrashort near-infrared pulses. Using 30 fs pulses we observe periodic enhancements of the excitation yield in the intensity regions corresponding to the absorption of 13 and 14 photons. By reducing the pulse duration to 6 fs with only a few optical cycles, we also demonstrate that the enhancements are significantly reduced beyond what is measurable in the experiment. Comparing these to numerical predictions, which are in quantitative agreement with experimental results, we find that even though the quantum-state distribution can be broad, the enhancements are largely due to efficient population of a select few AC Stark-shifted resonant states rather than the closing of an ionization channel. Because these resonances are dependent on the frequency and intensity of the laser field, the broad bandwidth of the 6 fs pulses means that the resonance condition is fulfilled across a large range of intensities. This is further exaggerated by volume-averaging effects, resulting in excitation of the $5g$ state at almost all intensities and reducing the apparent magnitude of the enhancements. For 30 fs pulses, volume averaging also broadens the quantum state distribution but the enhancements are still large enough to survive. In this case, selectivity of excitation to a single state is reduced below 25% of the relative population. However, an analysis of TDSE simulations indicates that excitation of up to 60% into a single state is possible if volume averaging can be eliminated and the intensity can be precisely controlled.
We present experimental data on the non-adiabatic strong field ionization of atomic hydrogen using elliptically polarized femtosecond laser pulses at a central wavelength of 390 nm. Our measured results are in very good agreement with a numerical solution of the time-dependent Schrodinger equation (TDSE). Experiment and TDSE show four above-threshold ionization (ATI) peaks in the electrons energy spectrum. The most probable emission angle (also known as attoclock-offset angle or streaking angle) is found to increase with energy, a trend that is opposite to standard predictions based on Coulomb interaction with the ion. We show that this increase of deflection-angle can be explained by a model that includes non-adiabatic corrections of the initial momentum distribution at the tunnel exit and non-adiabatic corrections of the tunnel exit position itself.
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