Attosecond transient absorption of a bound wave packet coupled to a smooth continuum

We investigate the possibility to use transient absorption of a coherent bound electron wave packet in hydrogen as an attosecond pulse characterization technique. In recent work we have shown that photoionization of such a coherent bound electron wave packet opens up for pulse characterization with unprecedented temporal accuracy --- independent of the atomic structure --- with maximal photoemission at all kinetic energies given a wave packet with zero relative phase [Pabst and Dahlstr\"om, Phys. Rev. A, 94, 13411 (2016)]. Here, we perform numerical propagation of the time-dependent Schr\"odinger equation and analytical calculations based on perturbation theory to show that the energy-resolved maximal absorption of photons from the attosecond pulse does not uniquely occur at zero relative phase of the initial wave packet. Instead, maximal absorption occurs at different relative wave packet phases, distributed as a non-monotonous function with a smooth $-\pi/2$ shift across the central photon energy (given a Fourier-limited Gaussian pulse). Similar results are found also in helium. Our finding is surprising because it implies that the energy-resolved photoelectrons are not mapped one-to-one with the energy-resolved absorbed photons of the attosecond pulse.Comment: 10 pages, 8 figues, submitted as part of a Special Issue on Emerging Attosecond Technologies in Journal of Optic

Attosecond dynamics of light-induced resonant hole transfer in high-order-harmonic generation

We present a study of high-order-harmonic generation (HHG) assisted by extreme ultraviolet (XUV) attosecond pulses, which can lead to the excitation of inner-shell electrons and the generation of a second HHG plateau. With the treatment of a one-dimensional model of krypton, based on time-dependent configuration interaction singles (TDCIS) of an effective two-electron system, we show that the XUV-assisted HHG spectrum reveals the duration of the semiclassical electron trajectories. The results are interpreted by the strong-field approximation (SFA) and the importance of the hole transfer during the tunneling process is emphasized. Finally, coherent population transfer between the inner and outer holes with attosecond pulse trains is discussed.Comment: 13 pages, 8 figure

Attosecond photoionization dynamics with stimulated core-valence transitions

We investigate ionization of neon atoms by an isolated attosecond pump pulse in the presence of two coherent extreme ultraviolet or x-ray probe fields. The probe fields are tuned to a core-valence transition in the residual ion and induce spectral shearing of the photoelectron distributions. We show that the photoelectron-ion coincidence signal contains an interference pattern that depends on the temporal structure of the attosecond pump pulse and the stimulated core-valence transition. Many-body perturbation theory is used to compute "atomic response times" for the processes and we find strikingly different behavior for stimulation to the outer-core hole (2p - 2s) and stimulation to the inner-core hole (2p - 1s). The response time of the inner-core transition is found to be comparable to that of state-of-the-art laser-based characterization techniques for attosecond pulses.Comment: 12 pages, 5 figure

Multiphoton interaction phase shifts in attosecond science

Ab initio simulations of a range of interferometric experiments are used to identify a strong dependence on multiphoton phase shifts in above-threshold ionization. A simple rule of thumb for interaction phase shifts is derived to explain both the conservation of photoelectron yield and its absolute CEP-dependence. For instance, it is found that interferometric above-threshold ionization experiments are shifted by $\pi/4$ relative to RABBIT experiments, and that there is no RABBIT-term in a laser-assisted photoionization experiment with odd and even harmonics. Thus, our work helps to resolve the issues of interpretation of quantum dynamics in attosecond and free-electron laser sciences

Photoelectron signature of dressed-atom stabilization in intense XUV field

Non-perturbative resonant multiphoton ionization $(1+1)$ is studied using the resolvent operator technique. Scaling parameters for effective two-level Hamiltonians are computed for hydrogen and helium atoms to provide a quantitative description of Rabi oscillations at XUV wavelengths, which were recently observed using a seeded Free-Electron Laser [S. Nandi et al., Nature 608, 488-493 (2022)]. The resulting photoelectron spectra exhibit a range of Autler-Townes doublets, which are studied for different intensities, detunings and interaction times. We identify a photoelectron signature that originates from stabilization against ionization of helium atoms interacting with intense circularly polarized XUV light. Thus, our work shows how it is possible to test the prediction of dressed-atom stabilization by Beers and Armstrong [B. L. Beers and L. Armstrong, Phys. Rev. A 12, 2447 (1975)], without the demanding requirement of atomic saturation in the time domain.Comment: 14 pages, 6 figures, 3 tables; accepted versio

Gauge-invariant absorption of light from a coherent superposition of states

Absorption and emission of light is studied theoretically for excited atoms in coherent superposition of states subjected to isolated attosecond pulses in the extreme ultraviolet range. A gauge invariant formulation of transient absorption theory is motivated using the energy operator from Yang's gauge theory. The interaction, which simultaneously couples both bound and continuum states, is simulated by solving the time dependent Schr\"odinger equation for hydrogen and neon atoms. A strong dependence on the angular momentum and the relative phase of the states in the superposition is observed. Perturbation theory is used to disentangle the fundamental absorption processes and a rule is established to interpret the complex absorption behaviour. It is found that non-resonant transitions are the source of asymmetry in energy and phase, while resonant transitions to the continuum contribute symmetrically to absorption of light from coherent superpositions of states

Pulse analysis by delayed absorption from a coherently excited atom

In this tutorial we provide a short review of attosecond pulse characterization techniques and a pedagogical account of a recently proposed method called Pulse Analysis by Delayed Absorption (PANDA) [Pabst and Dahlstr\"om, Phys. Rev. A, 94, 13411 (2016)]. We discuss possible implementations of PANDA in alkali atoms using either principal quantum number wave packets or spin-orbit wave packets. The main merit of the PANDA method is that it can be used as a pulse characterization method that is free from atomic latency effects, such as scattering phase shifts and long-lived atomic resonances. Finally, we propose that combining the PANDA method with angle-resolved photoelectron detection should allow for experimental measurements of attosecond delays in photoionization from bound wave packets on the order of tens of attoseconds.Comment: 12 pages, 7 figure

Frustrated tunneling dynamics in ultrashort laser pulses

We study a model for frustrated tunneling ionization using ultrashort laser pulses. The model is based on the strong field approximation and it employs the saddle point approximation to predict quasiclassical trajectories that are captured on Rydberg states. We present a classification of the saddle-point solutions and explore their behavior as functions of angular momentum of the final state, as well as the carrier--envelope phase (CEP) of the laser pulse. We compare the final state population computed by the model to results obtained by numerical propagation of the time-dependent Schr\"odinger equation (TDSE) for the hydrogen atom. While we find qualitative agreement in the CEP dependence of the populations in principal quantum numbers, $n$, the populations to individual angular momentum channels, $\ell$, are found to be inconsistent between model and TDSE. Thus, our results show that improvements of the quasiclassical trajectories are in order for a quantitative model of frustrated tunneling ionizaiton