The authors combine modern theoretical calculations with evaluated selected experimental data to produce a comprehensive data resource of K- and L-x-ray transition and absorption edge energies for all of the elements from neon to fermium. The theoretical and experimental components of this work are the result of programs of parallel development extending over more than 20 years. At each of several progressively more refined comparisons, it was possible to identify theoretical components whose systematic improvement then led to the next level of refinement in comparisons with an increasingly robust experimental reference data set. We have now reached a certain practical limit in what can be undertaken with reasonable levels of theoretical effort. This limit is not very different from the practical level of accuracy that can be meaningfully associated with the experimental data. For the more prominent diagram lines, experiment and theory are concordant with a zero-centered distribution of residuals whose statistical metrics allow the uncertainties to be estimated. For the light elements and the very heavy elements there are significant difficulties, as is also the case for a few isolated elements and transitions for Overall, the results reported here represent improvements over previously available data compilations not only because of their scope but also because of their attempt to offer internal metrics of the database accuracy. The identified regions of difficulty are areas where further experimental work may be directed to see if there may remain theoretical issues that are still unresolved.
28 September 1986 in Journal of Physics B: Atomic and Molecular Physics
Resetting the clock on photoemission: The ability to produce attosecond pulses of light provides access to some of the fastest electronic processes occurring within atoms. Tracking the temporal dynamics of the photoemission process in which an atom absorbs a high-energy photon and the electron escapes has exposed a discrepancy between the initial experimental findings and subsequent theoretical modeling. Isinger et al. present an ultrafast process that can account for and distinguish the different contributions to the photoemission processes in neon atoms. The findings reveal an “electron shake-up” process that may explain the discrepancy, bringing closure to a 7-year discussion. Science , this issue p. 893
Electron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20–40 eV spectral range, in the vicinity of the 3s−1np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.
Electron dynamics induced by resonant absorption of light is of fundamental importance in nature and has been the subject of countless studies in many scientific areas. Above the ionization threshold of atomic or molecular systems, the presence of discrete states leads to autoionization, which is an interference between two quantum paths: direct ionization and excitation of the discrete state coupled to the continuum. Traditionally studied with synchrotron radiation, the probability for autoionization exhibits a universal Fano intensity profile as a function of excitation energy. However, without additional phase information, the full temporal dynamics cannot be recovered. Here we use tunable attosecond pulses combined with weak infrared radiation in an interferometric setup to measure not only the intensity but also the phase variation of the photoionization amplitude across an autoionization resonance in argon. The phase variation can be used as a fingerprint of the interactions between the discrete state and the ionization continua, indicating a new route towards monitoring electron correlations in time.
Time delays of electrons emitted from an isotropic initial state with the absorption of a single photon and leaving behind an isotropic ion are angle independent. Using an interferometric method involving XUV attosecond pulse trains and an IR-probe field in combination with a detection scheme, which allows for full three-dimensional momentum resolution, we show that measured time delays between electrons liberated from the spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the common linear polarization axis of the ionizing XUV light and the IR-probing field. Such time delay anisotropy, for which we measure values as large as 60 as, is caused by the interplay between final quantum states with different symmetry and arises naturally whenever the photoionization process involves the exchange of more than one photon. With the support of accurate theoretical models, the angular dependence of the time delay is attributed to small phase differences that are induced in the laser-driven continuum transitions to the final states. Since most measurement techniques tracing attosecond electron dynamics involve the exchange of at least two photons, this is a general and significant effect that must be taken into account in all measurements of time delays involving photoionization processes.