arXiv subjects

Jan Marcus Dahlström

Publications and source records attributed to Jan Marcus Dahlström.

At least 37 records · Page 2Linked to original sources

arXiv2022

General Time-Dependent Configuration-Interaction Singles II: The Atomic Case

We present a specialization of the grid-based implementation of the time-dependent configuration-interaction singles described in the preceding paper (arXiv:2204.09966) to the case of spherical symmetry. We describe the intricate time propagator in detail, and conclude with a few example calculations. Among these, of note are high-resolution photoelectron spectra in the vicinity of the Fano resonances in photoionization of neon, and spin-polarized photoelectrons from xenon, in agreement with recent experiments.

physics.atom-ph↗

arXiv2022

Thomas--Reiche--Kuhn Correction for Truncated Configuration Interaction Spaces: Case of Laser-Assisted Dynamical Interference

The Thomas--Reiche--Kuhn sum rule is used to form an effective potential that is added to the time-dependent configuration interaction singles (TDCIS) equations of motion in velocity gauge. The purpose of the effective potential is to include virtual coupling from singles to doubles, which is required for size-consistent velocity gauge TDCIS results. The proposed method is compared to length gauge TDCIS results for laser-assisted photoionization. Finally, a novel dynamical interference effect controlled by two-color fields is predicted for atomic targets.

physics.atom-ph↗

arXiv2022

Studying ultrafast Rabi dynamics with a short-wavelength seeded free-electron laser

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field. They are ubiquitous in physics with applications in different areas such as photonics, nano-electronics, electron microscopy, and quantum information. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interaction within the rotating wave approximation\cite. Although intense nanometer-wavelength light-sources have been available for more than a decade, Rabi dynamics at such short wavelengths have not been observed directly. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser can drive Rabi oscillations between the ground state and an excited state in helium atoms. The measured photoemission signal revealed an Autler-Townes doublet as well as an avoided crossing, phenomena that are both trademarks of quantum optics. Using theoretical analyses that go beyond the strong-field approximation, we found that the ultrafast build-up of the doublet structure follows from a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond and few-femtosecond extreme-ultraviolet pulses, our results offer opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

quant-ph↗

arXiv2021

Relativistic time-dependent configuration-interaction singles

In this work, a derivation and implementation of the relativistic time-dependent configuration interaction singles (RTDCIS) method is presented. Various observables for krypton and xenon atoms obtained by RTDCIS are compared with experimental data and alternative relativistic calculations. This includes energies of occupied orbitals in the Dirac-Fock ground state, Rydberg state energies, Fano resonances and photoionization cross sections. Diagrammatic many-body perturbation theory, based on the relativistic random phase approximation, is used as a benchmark with excellent agreement between RTDCIS reported at the Tamm-Dancoff level. Results from RTDCIS are computed in the length gauge, here the negative energy states can be omitted with acceptable loss of accuracy. A complex absorbing potential, that is used to remove photoelectrons far from the ion, is implemented as a scalar potential and validated for RTDCIS. The RTDCIS methodology presented here opens for future studies of strong-field processes, such as attosecond transient absorption and high-order harmonic generation, with electron and hole spin dynamics and other relativistic effects described by first principle via the Dirac equation.

physics.atom-ph↗

arXiv2021

Complete characterization of multi-channel single photon ionization

Ionization of atoms and molecules by absorption of a light pulse results in electron wavepackets carrying information on the atomic or molecular structure as well as on the dynamics of the ionization process. These wavepackets can be described as a coherent sum of waves of given angular momentum, called partial waves, each characterized by an amplitude and a phase. The complete characterization of the individual angular momentum components is experimentally challenging, requiring the analysis of the interference between partial waves both in energy and angle. Using a two-photon interferometry technique based on extreme ultraviolet attosecond and infrared femtosecond pulses, we characterize the individual partial wave components in the photoionization of the 2p shell in neon. The study of the phases of the angular momentum channels allows us to unravel the influence of short-range, correlation and centrifugal effects. This approach enables the complete reconstruction of photoionization electron wavepackets in time and space, providing insight into the photoionization dynamics.

physics.atom-ph↗

arXiv2021

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 Schrödinger 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.

quant-ph↗

arXiv2021

Noise Free On-Demand Atomic Frequency Comb Quantum Memory

We present an extension of the atomic frequency comb protocol that utilizes the Stark effect to perform noise-free, on-demand, control. An experimental realization of this protocol was implemented in the Pr$^{3+}$:Y$_2$SiO$_5$ solid-state system, and a recall efficiency of 38\% for a 0.8 $μ$s storage time was achieved. Experiments were performed with both bright pulses as well as weak-coherent states, the latter achieving a signal-to-noise ratio of $570 \pm 120$ using input pulses with an average photon number of $\sim 0.1$. The principal limitation for a longer storage time was found to be the minimum peak width attainable for Pr$^{3+}$:Y$_2$SiO$_5$. We employ an adaptation of an established atomic-frequency comb model to investigate an on-demand, wide-bandwidth, memory based on Eu$^{3+}$:Y$_2$SiO$_5$. From this we determine that a storage time as long as 100 $μ$s may be practical even without recourse to spin-wave storage.

quant-ph↗

arXiv2021

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 $π/4$ 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.

physics.atom-ph↗

arXiv2020

Implementation and validation of the relativistic transient absorption theory within the dipole approximation

A relativistic transient absorption theory is derived, implemented and validated within the dipole approximation based on the time-dependent Dirac equation. Time-dependent simulations have been performed using the Dirac equation and the Schrödinger equation for the Hydrogen atom in two different attosecond transient absorption scenarios. These simulations validate the present relativistic theory. The presented work can be seen as a first step in the development of a more general relativistic attosecond transient absorption spectroscopy method for studying heavy atoms, but it also suggests the possibility of studying relativistic effects, such as Zitterbewegung, in the time domain.

physics.atom-ph↗

arXiv2020

Attosecond electron-spin dynamics in Xe 4d photoionization

The photoionization of xenon atoms in the 70-100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe$^+$ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide new insight into the complex electron-spin dynamics of photo-induced phenomena.

physics.atom-ph↗

arXiv2019

Propensity rules and interference effects in laser-assisted photoionization of helium and neon

We investigate the angle-resolved photoelectron spectra from laser-assisted photoionization for helium and neon atoms using an \textit{ab initio} method based on time-dependent surface flux and configuration interaction singles. We find that the shape of the distributions can be interpreted using a propensity rule, an intrinsic difference in the absorption and emission processes, as well as interference effects between multiple paths to the final angular momentum state. In neon we find that the difference between absorption and emission is hidden in the first sideband due to the multiple competing $m$ channels. Together, this aids the understanding of the formation of minima in the angular distributions, which can be transferred to an improved understanding on photoionization time delays in attosecond science.

physics.atom-ph↗

arXiv2019

Many-body calculations of two-photon, two color matrix elements for attosecond delays

We present calculations for attosecond atomic delays in photoionization of noble gas atoms based on full two-color two-photon Random-Phase Approximation with Exchange in both length and velocity gauge. Gauge invariant atomic delays are demonstrated for the complete set of diagrams. The results are used to investigate the validity of the common assumption that the measured atomic delays can be interpreted as a one-photon Wigner delay and a universal continuum--continuum contribution that depends only on the kinetic energy of the photoelectron, the laser frequency and the charge of the remaining ion, but not on the specific atom or the orbital from which the electron is ionized. Here we find that although effects beyond the universal IR--photoelectron continuum--continuum transitions are rare, they do occur in special cases such as around the $3s$ Cooper minimum in argon. We conclude also that in general the convergence in terms of many-body diagrams is considerably faster in length gauge than in velocity gauge.

physics.atom-ph↗

arXiv2019

Fano's propensity rule in angle-resolved attosecond pump-probe photoionization

In a seminal article, Fano predicts that absorption of light occurs preferably with increase of angular momentum. Here we generalize Fano's propensity rule to laser-assisted photoionization, consisting of absorption of an extreme-ultraviolet photon followed by absorption or emission of an infrared photon. The predicted asymmetry between absorption and emission leads to incomplete quantum interference in attosecond photoelectron interferometry. It explains both the angular-dependence of the photoionization time delays and the delay-dependence of the photoelectron angular distributions. Our theory is verified by experimental results in Ar in the 20-40 eV range.

physics.atom-ph↗

arXiv2018

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 Dahlström, 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.

quant-ph↗

arXiv2017

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.

physics.atom-ph↗

arXiv2017

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 Dahlström, Phys. Rev. A, 94, 13411 (2016)]. Here, we perform numerical propagation of the time-dependent Schrödinger 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 $-π/2$ 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.

physics.optics↗

arXiv2017

Attosecond delays in laser-assisted photodetachment from closed-shell negative ions

We study laser-assisted photodetachment time delays by attosecond pulse trains from the closed-shell negative ions F- and Cl-. We investigate the separability of the delay into two contributions: (i) the Wigner-like delay associated with one-photon ionization by the attosecond pulse train and (ii) the delay associated with exchange of an additional laser photon in the presence of the potential of the remaining target. Based on the asymptotic form of the wave packet, the latter term is expected to be negligible because the ion is neutralized leading to a vanishing laser-ion interaction with increasing electron-atom separation. While this asymptotic behavior is verified at high photoelectron energies, we also quantify sharp deviations at low photoelectron energies. Further, these low-energy delays are clearly different for the two studied anions indicating a breakdown of the universality of laser-ion induced delays. The fact that the short-range potential can induce a delay of as much as 50 as can have implications for the interpretation of delay measurements also in other systems that lack long-range potential.

physics.atom-ph↗

arXiv2017

Characterization of attosecond pulses in the soft x-ray regime

Attosecond x-ray pulses offer unprecedented opportunities for probing and triggering new types of ultrafast motion. At the same time, pulse characterization of x-rays presents new challenges that do not exist in the UV regime. Inner-shell ionization is the dominant ionization mechanism for x-rays and it is followed by secondary processes like fluorescence, Auger decay, and shake-up.In general, we find that inner-shell ionization and secondary processes can create additional delay-dependent modulations that will affect pulse reconstruction schemes. Our recently proposed pulse characterization method [Pabst and Dahlström, PRA 94, 013411 (2016)], where a bound electron wavepacket is sequentially photoionized by the attosecond pulse, can be adapted to mitigate the impact of these effects, thus opening up an avenue for reliable pulse reconstruction in the x-ray regime.

physics.atom-ph↗