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Journal of Physics B Atomic Molecular and Optical Physics

Analysis of absorption time delays in streaking of resonant and non-resonant two-photon ionization

Cory Goldsmith, Jing Su, Agnieszka Jaroń-Becker, Andreas Becker

Published Jun 12, 2018• 6 citations
Publisher

Abstract

Abstract We theoretically study the determination of the time delay between the subsequent absorption of photons in two-photon ionization with the attosecond streaking technique. An analytical model for the absorption time delay based on analysis of the process using perturbation theory is obtained. Model predictions at central frequencies that are resonant and non-resonant with an intermediate bound state agree well with results of numerical streaking simulations, if the intermediate state is well-isolated from other states and the effect of the streaking field on the intermediate state is negligible.

DOI
10.1088/1361-6455/aacc1b

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Abstract We theoretically study the determination of the time delay between the subsequent absorption of photons in two-photon ionization with the attosecond streaking technique. An analytical model for the absorption time delay based on analysis of the process using perturbation theory is obtained. Model predictions at central frequencies that are resonant and non-resonant with an intermediate bound state agree well with results of numerical streaking simulations, if the intermediate state is well-isolated from other states and the effect of the streaking field on the intermediate state is negligible.
We theoretically study time-resolved photoemission in atoms as probed by attosecond streaking. We review recent advances in the study of the photoelectric efect in the time domain and show that the experimentally accessible time shifts can be decomposed into distinct contributions that stem from the feld-free photoionization process itself and from probe-field induced corrections. We perform accurate quantum-mechanical as well as classical simulations of attosecond streaking for efective one-electron systems and determine all relevant contributions to the time delay with attosecond precision. In particular, we investigate the properties and limitations of attosecond streaking for the transition from short-ranged potentials (photodetachment) to long-ranged Coulomb potentials (photoionization). As an example for a more complex system, we study time-resolved photoionization for endohedral fullerenes A @C 60 and discuss how streaking time shifts are modifed due to the interaction of the C 60 cage with the probing infrared streaking field.
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.
By the numerical solution to the time-dependent Schr\"odinger equation, we observe a remarkable asymmetry in the photoelectron streaking spectra when the He+{\mathrm{He}}^{+}He+ ion is ionized by an attosecond pulse from the 2s2s2s state in the presence of a weak infrared pulse. An analytical theory based on the modified perturbation theory is developed to quantitatively account for the underlying mechanism. We find that a transition occurs between the degenerate 2s2s2s and 2p2p2p states under the influence of the infrared electric field before the arrival of the attosecond pulse. The observed asymmetry in the attosecond streaking is formed by the interference of photoelectrons ionized from the 2s2s2s and 2p2p2p states. Using the sensitivity of the asymmetry to the infrared (IR) electric field at the moment of attosecond photoionization, we show that the present finding provides a highly reliable way to fully characterize the IR waveform in the streaking experiment.
Abstract We predict quantitatively that it is possible to use few-femtosecond positive or negative time delays , Δ t , between two XUV Gaussian few-femtosecond pulses of moderate intensities and central frequencies ω 1 and ω 2 , in order to control the probability of ionization at clearly defined exit energies corresponding to the sums of photon frequencies ( ω 1 + ω 1 ), ( ω 2 + ω 2 ), and ( ω 1 + ω 2 , or ω 2 + ω 1 ). The phenomenon is demonstrated quantitatively by obtaining and using nonperturbative solutions of the time-dependent Schrödinger equation for a time-dependent scheme involving the process of two-photon resonant ionization of Helium via the 1 s 2 p P o 1 (58.4 nm) and 1 s 4 p P o 1 (52.22 nm) excited states. The calculations used wavefunctions which are state-specific for the discrete spectrum, (up to the 1 s 7 g
Attosecond chronoscopy enables the exploration of correlated electron dynamics in real time. One key observable of attosecond physics is the determination of "time zero" of photoionization, the time delay with which the wave packet of the ionized electron departs from the ionic core. This observable has become accessible by experimental advances in attosecond streaking and reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) techniques. In this Letter, we explore photoionization time delays by strong extreme ultraviolet fields beyond the linear-response limit. We identify novel signatures in time delays signifying strong coupling between atoms and light fields and the light-field dressing of the ion. As a prototypical case, we study the interelectronic coherence and entanglement in helium driven by a strong extreme ultraviolet field. By the numerical solution of the time-dependent Schrödinger equation in its full dimensionality, we show that the time delay of the photoionized electron allows one to monitor the ultrafast variations of coherence dynamics and entanglement in real time.