Photoionization Of Atoms Research Articles

Laser stabilization to neutral Yb in a discharge with polarization-enhanced frequency modulation spectroscopy

Isotope selective optical excitation of atoms is important for experiments with neutral atoms, metrology, and work with trapped ions, including quantum information processing. Polarization-enhanced absorption spectroscopy is used to frequency stabilize a tunable external cavity laser diode system at 398.9 nm for isotope selective photoionization of neutral Yb atoms. This spectroscopy technique is used to measure isotope resolved dispersive features from transitions within a see-through configuration ytterbium hollow-cathode discharge lamp. This Doppler-free dichroic polarization spectroscopy is realized by retro-reflecting a laser beam through the discharge and analyzing the polarization dependent absorption with balanced detection. The spectroscopy signal is recovered using lock-in detection of frequency modulation induced by current modulation of the external cavity laser diode. Here, we show an order of magnitude improvement in the long-term stability using polarization-enhanced absorption spectroscopy of Yb compared to polarization spectroscopy.

Carbon monoxide interacting with free-electron-laser pulses

We study the interaction of a heteronuclear diatomic molecule, carbon monoxide, with a free-electron laser (FEL) pulse. We compute the ion yields and the intermediate states by which the ion yields are populated. We do so using rate equations, computing all relevant molecular and atomic photo-ionisation cross-sections and Auger rates. We find that the charge distribution of the carbon and oxygen ion yields differ. By varying the photon energy, we demonstrate how to control higher-charged states being populated mostly by carbon or oxygen. Moreover, we identify the differences in the resulting ion yields and pathways populating these yields between a homonuclear molecule, molecular nitrogen, and a heteronuclear molecule, carbon monoxide, interacting with an FEL pulse. These two molecules have similar electronic structure. We also identify the proportion of each ion yield which accesses a two-site double-core-hole state and tailor pulse parameters to maximise this proportion.

Laser-assisted photoionization: Streaking, sideband, and pulse-train cases

We present a theoretical study of atomic laser-assisted photoionization emission (LAPE). We consider an atom driven by a linearly polarized XUV laser in two different scenarios: i) a single attosecond pulse (in both the streaking and sideband regimes) and ii) an attosecond pulse train. The process takes place assisted by a linearly polarized infrared (IR) laser field. In all these cases the energy and angle-resolved photoelectron spectrum (PES) is determined by a leading contribution, related to the intracycle factor [Gramajo et al., J. Phys. B 51, 055603 (2018)], complemented by other ones, derived from the periodicity and symmetry properties of the dipole transition matrix with respect to the IR field. Each of these terms imprint particular features in the PES that can be straightforwardly understood in terms of generalized energy conservation laws. We investigate in detail these PES structures, in particular, for the case of argon initially in the 3s quantum state. Our theoretical scheme, based on the strong-field approximation (SFA), can be applied, however, to other atomic species and field configurations as well.

Attosecond electron\u2013spin 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 insight into the complex electron-spin dynamics of photo-induced phenomena.

Photoionization of superheavy atoms: correlation and relativistic effects

Calculations of the photoionization cross sections of the ground states of the superheavy atoms No (Z = 102), Cn (Z = 112) and Og (Z = 118) have been performed using fully relativistic methodologies. The photoionization cross sections are dominated by interchannel coupling, in all cases, over a broad energy range including both outer and inner shells.

Transport dynamics in a high-brightness magneto-optical-trap Li ion source

Laser-cooled gases offer an alternative to tip-based methods for generating high-brightness ion beams for focused ion beam applications. These sources produce ions by photoionization of ultracold neutral atoms, where the narrow velocity distribution associated with microkelvin-level temperatures results in a very low emittance, high-brightness ion beam. In a magneto-optical trap-based ion source, the brightness is ultimately limited by the transport of cold neutral atoms, which restricts the current that can be extracted from the ion-generating volume. We explore the dynamics of this transport in a 7Li magneto-optical trap ion source by performing time-dependent measurements of the depletion and refilling of the ionization volume in a pulsed source. An analytic microscopic model for the transport is developed, and this model shows excellent agreement with the measured results.

Glory oscillations in photoionization microscopy: Connection with electron dynamics and Stark spectral structures in the continuum

In classical scattering theory, the term “glory scattering” implies the divergence of the classical differential cross section that occurs as soon as the deflection function goes through zero for a nonzero value of the impact parameter. This critical effect also occurs in slow photoelectron imaging where near-threshold atomic photoionization is performed in the presence of an external static electric field. In this case, glory scattering manifests itself by the appearance of an intense peak at the center of the photoelectron momentum distribution. In the present work we examine the magnitude variation of this central peak as a function of electron energy. We experimentally study near-threshold two-photon ionization of ground state magnesium atoms, below as well as above the field-free ionization limit. It is found that, apart from its behavior of classical origin, the glory signal additionally exhibits strong oscillations and beating effects over the full spectral range of the recordings. Of particular interest are its oscillations above the zero-field limit, many aspects of which are expected to be independent of the atomic target. Our results are analyzed with the help of classical, semiclassical, and quantum mechanical calculations devoted to the hydrogenic Stark effect. It is theoretically found that these continuum glory oscillations are related to the resonantlike Stark structures appearing under certain conditions in the total photoionization cross section and implying energy quantization in the continuum. The striking outcome of the present study, however, is that both theory and experiment clearly support the connection between the energy- and static field-dependent periodicity of glory oscillations with the classical dynamics of electron motion. In particular, it is shown that the Fourier transform of the glory signal provides information on the differences between the origin-to-detector times of flight corresponding to specific pairs of classical electron trajectories.

Photoionization of Astrophysically Relevant Atomic Ions at PIPE

We review recent work on the photoionization of atomic ions of astrophysical interest that has been carried out at the photon-ion merged-beams setup PIPE, a permanently installed end station at the XUV beamline P04 of the PETRA III synchrotron radiation source operated by DESY in Hamburg, Germany. Our results on single and multiple L-shell photoionization of Fe+, Fe2+, and Fe3+ ions, and on single and multiple K-shell photoionization of C−, C+, C4+, Ne+, and Si2+ ions are discussed in astrophysical contexts. Moreover, these experimental results bear witness of the fact that the implementation of the photon-ion merged-beams method at one of the world’s brightest synchrotron light sources has led to a breakthrough for the experimental study of atomic inner-shell photoionization processes with ions.

Angle-resolved studies of XUV–IR two-photon ionization in the RABBITT scheme

Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is an established technique for studying time-delay in photoionization of atoms and molecules. It has been recently extended to angle-resolved studies, accessing diverse fingerprint observables of the attosecond photoemission dynamics within the bound-continuum and continuum–continuum transitions. In this work, we address the general form of the ISB(θ,τ) two-photon photoelectron angular distributions (PADs) associated to the RABBITT sideband signal, as a function of the emission angle θ, and the delay τ between the XUV attosecond pulse train and the infrared (IR) dressing field at play in the RABBITT scheme. Relying on the expansion in Legendre polynomials, the PAD is synthesized in terms of a reduced set of coefficients which fully describe both its static (τ-independent) and dynamic (τ-dependent) components and enables us to retrieve any observable characterizing the PAD. This unified framework streamlines the comparison between different experimental or theoretical data sets and emphasizes how some observables depend on the experimental conditions. Along with the modelled analysis, we report new results of angle-resolved RABBITT direct ionization of the np valence orbital of Ar(3p6) and Ne(2p6), employing electron-ion coincidence momentum spectroscopy at the new Attolab facility. In this case, the nine coefficients synthesizing the PAD are further linked to the magnitude and phase of the transition dipole matrix elements, providing a fundamental test of theoretical predictions. Similarities and differences are found between Ar and Ne in the explored low energy region, up to 20 eV above the ionization threshold, where the electron dynamics is most sensitive to electronic correlation. Further interpretation of these results would benefit from a comparison with advanced many-body theoretical simulations.

Population transfer to high angular momentum states in infrared-assisted XUV photoionization of helium

An extreme-ultraviolet (XUV) laser pulse consisting of harmonics of a fundamental near-infrared (NIR) laser frequency is combined with the NIR pulse to systematically study two-color photoionization of helium atoms. A time-resolved photoelectron spectroscopy experiment is carried out where energy- and angle-resolved photoelectron distributions are obtained as a function of the NIR intensity and wavelength. Time-dependent Schrödinger equation calculations are performed for the conditions corresponding to the experiment and used to extract residual populations of Rydberg states resulting from excitation by the XUV + NIR pulse pair. The residual populations are studied as a function of the NIR intensity (3.5 × 1010 − 8 × 1012 W cm−2) and wavelength (760–820 nm). The evolution of the photoelectron distribution and the residual populations are interpreted using an effective restricted basis model, which includes the minimum set of states relevant to the features observed in the experiments. As a result, a comprehensive and intuitive picture of the laser-induced dynamics in helium atoms exposed to a two-color XUV–NIR light field is obtained.

The Rb + –Rb collision rate in the energy range of 103–104 K

We study both theoretically and experimentally the energy dependence of the low-energy Rb+–Rb total collision rate k ia in the energy range from 103 to 104 K. We calculate the integral elastic cross-section and the resonant charge-transfer cross-section by the quantum mechanical molecular orbital close-coupling method, and then obtain k ia for temperatures by averaging the cross-sections over a Maxwell–Boltzmann velocity distribution. The experiments are conducted in an ion–neutral hybrid trap, where the Rb+ ions are created by photo-ionization of the cold atoms in a magneto-optic trap (MOT) and accumulated in the linear Paul ion trap. The total ion–atom collision rate k ia is measured by monitoring the fluorescence reduction of the steady-state MOT atoms by sequentially introducing photo-ionization and ion–atom collisions. The ion–atom collision energy E col ≈ T i is modified by changing T i due to T i being more than six orders of magnitude larger than the T a of cold atoms. The temperature of ions T i is obtained by comparing the time-of-flight mass spectrometry of Rb+ from experimental results to that obtained by SIMION simulation. The equilibrium steady T i is modified by changing the initial root-mean-squared position of the ion cloud, and the k ia are measured with E col from 8000 to 16 000 K. Both the theoretical and experimental results show that k ia increases with E col. More specifically, the measured k ia increases rapidly with the enlargement of E col near 10 000 K. The theoretical calculation results show that k ia increases slowly with E col. The specific difference may be due to the influence of the ratio of excited states f e on the trend of k ia at different E col.

Super-interference in atomic photoionization: Moiré patterns in momentum maps

SynopsisWe theoretically investigate on the origin of lateral ring structures in the doubly differential momen-tum distribution for atomic ionization by laser pulses in the midinfrared spectral region. We demonstrate that such structures stems from the interplay between intra- and intercycle interference patterns which work as two separate grids in the two-dimensional momentum domain. When the periods of the two grids (intra- and intercycle) are similar, moiré patterns arise as concentric rings at high electron kinetic energy.

Photoionization microscopy: linear polarization rotation effects

SynopsisPhotoionization microscopy (PM) aims at imaging the flux of slow (meV) electrons released by atomic photoionization in the presence of a static electric field. We discuss the rotation of the linear light polari-zation with respect to the electric field direction. Two-photon ionization out of an m=0 initial state allows for the population of |m|=0,1,2 Stark states. The resulting |m|-beating effects in the PM images are demonstrated theoretically (in hydrogen atom) and experimentally (in Mg atom). Implications on the applicability of tomographic techniques for slow electrons are also discussed.

Phase sensitive coherent control excitation schemes applied to photoionization microscopy of the hydrogen atom

SynopsisPhotoionization microscopy (PM) is employed for imaging the flux of slow (meV) electrons ejected via atomic photoionization in the presence of a static electric field. Just above the ionization limit continuum and quasi-disrete states are degenerate. In hydrogen atom resonant excitation dominates over the continuum one, while the reverse holds for more complex atoms. We demonstrate theoretically that by using a bichromatic ω/2ω laser field and by applying phase sensitive coherent control techniques it is possible to unbury and isolate other-wise obscured resonant features in PM images.

XUV+IR photoionization of argon atoms: selection of sideband orders

We present a theoretical study of atomic ionization due to an XUV pulse in the presence of an infrared laser. Within the strong field approximation and considering the periodicity and symmetry of the transition matrix we show that the photoelectron spectrum can be described from the contribution during only one (or half) infrared cycle. These symmetry and periodicity properties impress selection rules which destructively cancel certain sideband orders favoring others. In particular, we analyze the photoionization of Argon in four geometrical arrangements of the polarization vector and the photoelectron momentum direction.

A look into the photoionization of medium-sized molecular systems from an XCHEM perspective

SynopsisIn recent years, the XCHEM methodology has been successfully applied to describe photoionization of many-electron atoms and diatomic molecules. In this communication we present the first application of XCHEM to describe photoionization of medium-sized halomethanes and pyrazine.

NewStock, a time-dependent close-coupling program for atomic ionization

SynopsisWe present NewStock, a time-dependent program to compute the photoionization of polyelectronic atoms by arbitrary light pulses. The program, which expands the capabilities of the Stock B-spline close-coupling structure code to the time-dependent domain, is applied to the pump-probe ionization of the neon atom.

Dynamic interference in photoemission by chirped ultrashort extreme ultraviolett pulses

SynopsisWe investigated dynamical interference (DI) in the photoionization of hydrogen atoms in intense ultrashort chirped extreme ultraviolett (XUV) pulses by numerically solving the time-dependent Schrödinger equation(TDSE) and examined its dependence on pulse intensity, duration, and chirp. We find the pulse chirp to red shift the photoelectron spectrum and weaken the DI effect.

Dynamic photoemission interference of hydrogen atoms in intense ultra-fast elliptically polarized extreme ultraviolett pulses

SynopsisWe investigated dynamic interference (DI) in the photoionization of ground-state hydrogen atoms by intense extreme-ultraviolet (XUV) pulses with elliptical polarization. Numerically solving the time-dependent Schrodinger equation, we demonstrate that DI occurs not only in linearly but also in elliptically polarized pulses.

Multi-electron/ion coincidence spectroscopy in Xe triple ionization

SynopsisThe study of atomic multiple photoionization by a single photon can be performed by detecting in coincidence all the corresponding electrons with a magnetic bottle time of flight spectrometer. To reveal minor triple ionization channels of Xe atom that are hindered by radom coincidences, we have detected three electrons in coincidence with the corresponding Xe3+ ion, thanks to a new permanent magnet design using a drilled soft iron pole.