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Physical Review A

Ionization enhancement and suppression by phase-locked ultrafast pulse pairs

David B. Foote, Y.-J. Lin, Liang-Wen Pi, J. M. Ngoko Djiokap, Anthony F. Starace, W. T. Hill

Published Aug 29, 2017• 3 citations
Publisher

Abstract

We present the results of a study of ionization of Xe atoms by a pair of phase-locked pulses, which is characterized by interference produced by the twin peaks. Two types of interference are considered: ordinary optical interference, which changes the intensity of the composite pulse and thus the ion yield, and a quantum interference, in which the excited electron wave packets interfere. We use the measured ${\mathrm{Xe}}^{+}$ yield as a function of the temporal delay and/or relative phase between the peaks to monitor the interferences and compare their relative strengths. We model the interference with a pulse intensity function and by calculating the ionization yield with the time-dependent Schr\"odinger equation. Our results provide insight into optimal control pulses generated with learning algorithms. The results also show that the relative phase between peaks of a control pulse, along with small features such as distortions and imperfections in the wings of an ideal shape, play a significant role in the control process.

DOI
10.1103/physreva.96.023425

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Molecular or atomic coherence generated with the irradiation of ultrashort optical pulses should make a significant role for realizing the control of quantum states in a matter. By virtue of the advancement of the ultrashort light sources towards the short wavelength region, the energy range of the quantum states that could be coherently generated reached much more than 15 eV at the present [1] . In particular, Ramsey-type interference fringes observed by scanning the delay between a pair of phase-locked XUV femtosecond pulses unveiled spectral information of the atomic states [2] - [4] . The time ranges of the delay scans in such preceding studies were long enough to finely resolve the spectral features, while the XUV pulse pairs could not temporally overlap because the light sources were split into two before generating the XUV pulses. The near 0 delay control of the XUV pulse pair is important for investigating the dynamics of a cationic system entangled with an ionized continuum electron [5] . In this paper, we performed the delay scan of the XUV pulse pair starting from the complete temporal overlap to show that the optical interference seamlessly continued to the Ramsey-type atomic interference as a prototype of such study.
The quantum interference of two molecular wave packets has been precisely controlled in the B electronic state of the I2 molecule by using a pair of fs laser pulses whose relative phase is locked within the attosecond time scale and its real-time evolution has been observed by another fs laser pulse. It is clearly observed that the temporal evolution changes drastically as a function of the relative phase between the locked pulses, allowing us to read both amplitude and phase information stored in the wave functions of the molecular ensemble.
Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.
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The effect of temporal coherent control on the two-photon-resonant third-harmonic generation and multiphoton ionization into the continuum states of an atomic system is experimentally and theoretically investigated by means of a pair of partially incoherent, identical laser pulses. The evidence of quantum interference as a function of the delay between the pulses is reported. The transition from the resonant to the nonresonant case is also shown. The obtained results agree with the prediction of a theoretical model showing that the onset of quantum interference appears to be related to the coherence time of the laser radiation, which is much shorter than the pulse duration.
We study the photoelectron spectra of hydrogen and helium ionized by intense ultrafast two-color XUV laser pulses by numerically solving the time-dependent Schrödinger equation.The photon energy of the pump pulse is tuned to the 1s-2p excitation energy, inducing Rabi oscillations between these bound states and forming an Autler-Townes (AT) doublet of dressed states.When ionized by a time-delayed ultrafast XUV pulse with duration shorter than the Rabi oscillation period, we find novel and drastically enhanced AT splittings in the photoionization spectrum.We identify their origin in terms of the temporal interference of two attosecond wave packets whose spectral distribution is controlled by the interplay between Rabi frequency and bandwidth of the probe pulse.These time-dependent features in the spectra can be much larger than the standard AT spacing induced by the pump pulse alone and can be controlled by the time delay and the duration of the probe pulse.