D. C. Haynes, M. Wurzer, A. Schletter, A. Al-Haddad, C. Blaga, C. Bostedt, J. Bozek, M. Bucher, A. Camper, S. Carron, R. Coffee, J. T. Costello, L. F. DiMauro, … 展开作者
D. C. Haynes, M. Wurzer, A. Schletter, A. Al-Haddad, C. Blaga, C. Bostedt, J. Bozek, M. Bucher, A. Camper, S. Carron, R. Coffee, J. T. Costello, L. F. DiMauro, Y. Ding, K. Ferguson, I. Grguraš, W. Helml, M. C. Hoffmann, M. Ilchen, S. Jalas, N. M. Kabachnik, A. K. Kazansky, R. Kienberger, A. R. Maier, T. Maxwell, T. Mazza, M. Meyer, H. Park, J. S. Robinson, C. Roedig, H. Schlarb, R. Singla, F. Tellkamp, K. Zhang, G. Doumy, C. Behrens, A. L. Cavalieri
Intense X-ray free-electron lasers (XFELs) can rapidly excite matter, leaving it in inherently unstable states that decay on femtosecond timescales. As the relaxation occurs primarily via Auger emission, excited state observations are constrained by Auger decay. In situ measurement of this process is therefore crucial, yet it has thus far remained elusive at XFELs due to inherent timing and phase jitter, which can be orders of magnitude larger than the timescale of Auger decay. Here, we develop a new approach termed self-referenced attosecond streaking, based upon simultaneous measurements of streaked photo- and Auger electrons. Our technique enables sub-femtosecond resolution in spite of jitter. We exploit this method to make the first XFEL time-domain measurement of the Auger decay lifetime in atomic neon, and, by using a fully quantum-mechanical description, retrieve a lifetime of $2.2^{ + 0.2}_{ - 0.3}$ fs for the KLL decay channel. Importantly, our technique can be generalised to permit the extension of attosecond time-resolved experiments to all current and future FEL facilities.
A tenet of time-resolved spectroscopy is -faster laser pulses for shorter timescales- . Here we suggest turning this paradigm around, and slow down the system dynamics via repeated measurements, to do spectroscopy on longer timescales. This is the principle of the quantum Zeno effect. We exemplify our approach with the Auger process, and find that repeated measurements increase the core-hole lifetime, redistribute the kinetic energy of Auger electrons, and alter entanglement formation. We further provide an explicit experimental protocol for atomic Li, to make our proposal concrete.
We examine the archetype of an interference experiment for Auger electrons: two electron wave packets are launched by inner-shell ionizing a krypton atom using two attosecond light pulses with a variable time delay. This setting is an attosecond realization of the Ramsey method of separated oscillatory fields. Interference of the two ejected Auger-electron wave packets is predicted, indicating that the coherence between the two pulses is passed to the Auger electrons. For the detection of the interference pattern an accurate coincidence measurement of photo- and Auger electrons is necessary. T…
The mechanism leading to an Auger transition is based on the residual Coulomb interaction between the valence electron and the core electrons. On the assumption that the wave field is switched on adiabatically, the probability of the Auger effect of the inner electrons of the atom is determined.
We predict that attosecond spectroscopy could be used to observe time delay for electron emission {in the C$^{1+}$ ion} from a few step processes {that include electron impact excitation}. The results reveal that the photon energy corresponding to the excitation to the $1s 2s^{2} 2p^{2} \, ^{2}D_{1.5}$ level from the ground one has to be used to study the emission of the electrons produced with the largest probability from a few step processes. Double and triple Auger processes are investigated in the C$^{1+}$ ion as a sequence of single Auger transition with subsequent ionization by the Auger…
Using attoscience, we study the electron correlations responsible for Auger decay in krypton atoms. The Auger decay is induced by a pulse train or a twin pulse composed of subpulses of attosecond duration. During the Auger decay an optical dressing laser may be present. Interference effects between the ejected Auger electron wave packets are predicted.
Multiple ionization and charge equilibration in slow, multiply charged $\mathrm{Ar^{q+} + Ar}$ collision studied via L-MM Auger-Meitner electron spectroscopy
Indian Institute of Technology Kanpur（坎普尔印度理工学院）；Tata Institute of Fundamental Research（塔塔基础研究所）
Multiple electron processes occur widely in atoms, molecules, clusters, and condensed matters when they are interacting with energetic particles or intense laser fields. In this work, a unified and accurate theoretical formalism is proposed on the direct multielectron processes of atoms including the multiple Auger decay and multiple ionization by an impact of an energetic electron or a photon based on the atomic collision theory described by a correlated many-body Green's function. Such a practical treatment is made possible due to different coherence features of the particles (matter waves) …
Results of the most sophisticated measurements in coincidence of the angular resolved K-shell photo- and Auger-electrons, and of two atomic ions produced by dissociation of N2 molecule, are analyzed. Detection of photoelectrons at certain angles allows separating the Auger decay processes of the 1σg and 1σu core hole states. The Auger electron angular distributions for each of these hole states are measured as a function of the kinetic energy release of two atomic ions and are compared with the corresponding theoretical angular distributions. From that comparison one can disentangle the contri…
Aims. In the context of black-hole accretion disks, the main goal of the present study is to estimate the plasma environment effects on the atomic structure and radiative parameters associated with the K-vacancy states in ions of the oxygen isonuclear sequence. Methods. We use a time-averaged Debye-Huckel potential for both the electron-nucleus and the electron-electron interactions implemented in the fully relativistic multiconfiguration Dirac-Fock (MCDF) method. Results. Modified ionization potentials, K thresholds, Auger widths and radiative transition wavelengths and rates are reported for…
We devise an ab initio formalism for the quantum dynamics of Auger decay by laser-dressed atoms which are inner-shell ionized by extreme ultraviolet (XUV) light. The optical dressing laser is assumed to be sufficiently weak such that ground-state electrons are neither excited nor ionized by it. However, the laser has a strong effect on continuum electrons which we describe in strong-field approximation with Volkov waves. The XUV light pulse has a low peak intensity and its interaction is treated as a one-photon process. The quantum dynamics of the inner-shell hole creation with subsequent Auge…
Single photon laser enabled Auger decay (spLEAD) has been redicted theoretically [Phys. Rev. Lett. 111, 083004 (2013)] and here we report its first experimental observation in neon. Using coherent, bichromatic free-electron laser pulses, we have detected the process and coherently controlled the angular distribution of the emitted electrons by varying the phase difference between the two laser fields. Since spLEAD is highly sensitive to electron correlation, this is a promising method for probing both correlation and ultrafast hole migration in more complex systems.
The KLM+KLN Auger electron spectrum of rubidium (Z=37) emitted in the electron capture decay of radioactive $^{83}$Sr in a polycrystalline platinum matrix and also $^{85}$Sr in polycrystalline platinum and carbon matrices as well as in an evaporated layer onto a carbon backing was experimentally studied in detail for the first time using a combined electrostatic electron spectrometer. Energies, relative intensities, and natural widths of fifteen basic spectrum components were determined and compared with both theoretical predictions and experimental data for krypton (Z=36). Relative spectrum l…
We discuss the possibility of non-exponential Auger decay of atoms irradiated by X-ray photons. This effect can occur at times, which are greater than the lifetime of a system under consideration. The mechanism for non-exponential depletion of an initial quasi-stationary state is the cutting of the electron energy spectrum of final continuous states at small energies. Then the Auger decay amplitude obeys power-law dependence on long observation times.
Auger-Meitner processes are electronic decay processes of energetically low-lying vacancies. In these processes, the vacancy is filled by an electron of an energetically higher lying orbital, while another electron is simultaneously emitted to the continuum. In low-lying orbitals relativistic effects can not even be neglected for light elements. At the same time lifetime calculations are computationally expensive. In this context, we investigate which effect spin-orbit coupling has on Auger-Meitner decay widths and aim for a rule of thumb for the relative decay widths of initial states split b…
Aims. In the context of accretion disks around black holes, we estimate plasma-environment effects on the atomic parameters associated with the decay of K-vacancy states in highly charged iron ions, namely Fe xvii - Fe xxv. Methods. Within the relativistic multiconfiguration Dirac-Fock (MCDF) framework, the electron-nucleus and electron-electron plasma screenings are approximated with a time-averaged Debye-Huckel potential. Results. Modified ionization potentials, K thresholds, wavelengths, radiative emission rates and Auger widths are reported for astrophysical plasmas characterized by electr…
Positron annihilation induced Auger electron spectroscopy was used to obtain Cu and Au Auger spectra that are free of primary beam induced background by impinging the positrons at energy below the secondary electron emission threshold. The removal of the core electron via annihilation in the PAES process resulted in the elimination of post-collision affects. The spectrum indicates that there is an intense low energy tail (LET) associated with the Auger peak that extends all the way to 0 eV. The LET has been interpreted as being due to processes in which the filling of the core by a valence ele…
When an electron is emitted from a sub-valence shell, a vacancy is created and there is a not-null probability for different post collisional ionization (PCI) processes giving rise to a higher target charge state. It is reasonable to consider that PCI is a time-delayed electron emission and, therefore, independent of the projectile. We include the tables of the branching ratios of $0-6$ post-collisionally emitted electrons after single ionization of Ne, Ar, Kr and Xe in different inner shells. These values have already been employed with good results in previous calculations of multiple ioniza…
We explore the possibility of retrieving Auger spectra with FEL radiation. Using a laser pulse of 260 eV photon energy, we study the interplay of photo-ionization and Auger processes following the initial formation of a 2p inner-shell hole in Ar. Accounting for the fine structure of the ion states we demonstrate how to retrieve the Auger spectrum of $\mathrm{Ar^{+}\rightarrow Ar^{2+}}$. Moreover, considering two electrons in coincidence we also demonstrate how to retrieve the Auger spectrum of $\mathrm{Ar^{2+}\rightarrow Ar^{3+}}$.
The KLL Auger spectrum of rubidium following the electron capture decay of $^{83}$Sr and $^{85}$Sr isotopes was experimentally studied in detail for the first time using one $^{83}$Sr source and three $^{85}$Sr sources in different host matrices. Energies, relative intensities, and natural widths of all the nine well-resolved basic spectrum components were determined and compared with both predictions and experimental data for krypton. Results of our multiconfiguration Dirac-Fock calculations demonstrated an influence of the "atomic structure effect" on absolute energies of the KLL transitions…
An elaborate least-squares variational technique is proposed for obtaining improved continuum wavefunctions of Auger electrons emitted from arbitrary systems the electronic structures of which are determined via one of the computer codes available. A computer program is developed on the basis of this technique for calculating the Auger transition rates using the angular momentum average scheme. The program is employed for investigating the emission of Auger electrons as a consequence of K- shell ionizations of two configurations of copper atoms. A comparison is presented between the improved A…
The emission of Auger electrons from the K-, L- and M-sheels of two configurations of copper atoms is investigated in detail within the frame work of the momentum average technique. Ab initio calculations for the bound state wavefunctions of the ionized atoms are performed using a Gaussian computer code. The continuum wavefunctions of the emitted electrons are determined by employing an effective potential variational approach. Slight differences have been noticed between the results of both configurations. The transition rates, energies and widths of all possible Auger electrons are listed in…
With an eye on plasma walls we investigate, within an effective model for the two active electrons involved in the process, secondary electron emission due to Auger de-excitation of metastable nitrogen $N_2(^3σ^+_u)$ molecules at metallic surfaces. Modelling bound and unbound molecular states by a LCAO approach and a two-center Coulomb wave, respectively, and the metallic states by the eigenfunctions of a step potential we employ Keldysh Green's functions to calculate the secondary electron emission coefficient $γ_e$ retaining for the Auger self-energy the non-locality in time and the dependen…
Development of a cylindrical mirror analyzer electron spectrometer and associated data acquisition system to study inner shell electron emission following ion-atom collision
The low-energy electron spectra emitted in the radioactive decay of the $^{83}$Rb and $^{83}$Sr isotopes were measured with a combined electrostatic electron spectrometer. Radioactive sources used were prepared by ion implantation of $^{83}$Sr into a high purity polycrystalline platinum foil at 30 keV and by vacuum-evaporation deposition of $^{83}$ Rb on the same type of foil. From the measured conversion electron spectra, the electron binding energies (referenced to the Fermi level) for the K, L$_1$ , L$_2$ , L$_3$ , M$_1$ , M$_2$, and M$_3$ shell/subshells of krypton in the platinum host wer…
In a recent publication [B. Schuette, S. Bauch et al., accepted for publication in Phys. Rev. Lett. 2012] it was demonstrated both, experimentally and theoretically, that Auger electrons are subject to an energetic chirp if a three-body-interaction dubbed post-collision interaction (PCI) is involved. Here, we extend previous theoretical work and give a detailed analysis of field-assisted PCI based on numerical solutions of the time-dependent Schrödinger equation, extensive Monte-Carlo averaged molecular dynamics simulations and analytical theory. The dependence on various streaking and excitat…
The theory of resonant Auger decay of atoms in a high intensity coherent X-ray pulse is presented. The theory includes the coupling between the ground state and the resonance due to an intense X-ray pulse, taking into account the decay of the resonance and the direct photoionization of the ground state, both populating the final ionic states coherently. The theory also considers the impact of the direct photoionization of the resonance state itself which typically populates highly-excited ionic states. The combined action of the resonant decay and of the direct ionization of the ground state i…
We report on theoretical Auger electron kinetic energy distribution originated from sequential two-step Auger decays of molecular double core-hole (DCH) state, using CH4, NH3 and H2CO molecules as representative examples. For CH4 and NH3 molecules, the DCH state has an empty 1s inner-shell orbital and its Auger spectrum has two well separated components. One is originated from the 1st Auger transition from the DCH state to the triply ionized states with one core hole and two valence holes (CVV states) and the other is originated from the 2nd Auger transition from the CVV states to quadruply va…
Modern x-ray sources enable the production of coherent x-ray pulses with a pulse duration in the same order as the characteristic lifetimes of core-hole states of atoms and molecules. These pulses enable the manipulation of the core-hole population during Auger decay processes, modifying the lineshape of the electron spectra. In this work, we present a theoretical model to study those effects in Neon. We identify effects in the Auger-photoelectron coincidence spectrum due to the duration and intensity of the pulses. The normal Auger line-shape is recovered in Auger electron spectrum integrated…
We have unveiled coherent multiphoton interferences originating from different quantum paths taken by the Auger electron induced by a high-intensity x-ray/XUV pulse under the presence of a strong optical field. These interferences give rise to a clear signature in the angle-resolved Auger electron spectrum: an asymmetry with respect to the energy of the Auger decay channel. In order to illustrate this effect we have considered the resonant Auger decay of the transition $2p^{5} \!\leftrightarrow\! 1s^{-1}2p^{6}$ in Ne$^{+}$. The simulations show that these interferences are very sensitive to th…
To benchmark a Monte Carlo model of the Auger cascade that has been developed at the Australian National University (ANU) against the literature data. The model is applicable to any Auger-electron emitting radionuclide with nuclear structure data in the format of the Evaluated Nuclear Structure Data File (ENSDF). Schönfeld's algorithms and the BrIcc code were incorporated to obtain initial vacancy distributions due to electron capture (EC) and internal conversion (IC), respectively. Atomic transition probabilities were adopted from the Evaluated Atomic Data Library (EADL) for elements with ato…
We investigate K-shell ionization of N$_2$ at 40 keV photon energy. Using a COLTRIMS reaction microscope we determine the vector momenta of the photoelectron, the Auger electron and both N$^+$ fragments. These fully differential data show that the dissociation process of the N$_2^{2+}$ ion is significantly modified not only by the recoil momentum of the photoelectron, but also by the photon momentum and the momentum of the emitted Auger electron. We find that the recoil energy introduced by the photon and the photoelectron momentum is partitioned with a ratio of approximately 30/70 between the…
Aims. In the context of black-hole accretion disks, we aim to compute the plasma-environment effects on the atomic parameters used to model the decay of K-vacancy states in moderately charged iron ions, namely Fe ix - Fe xvi. Methods. We used the fully relativistic multiconfiguration Dirac-Fock (MCDF) method approximating the plasma electron-nucleus and electron-electron screenings with a time-averaged Debye-Huckel potential. Results. We report modified ionization potentials, K-threshold energies, wavelengths, radiative emission rates, and Auger widths for plasmas characterized by electron tem…
We study the effects of field fluctuations on the total yields of Auger electrons, obtained in the excitation of neutral atoms to a core-excited state by means of short-wavelength free-electron-laser pulses. Beginning with a self-contained analysis of the statistical properties of fluctuating free-electron-laser pulses, we analyse separately and in detail the cases of single and double Auger resonances, focusing on fundamental phenomena such as power broadening and ac Stark (Autler-Townes) splitting. In certain cases, field fluctuations are shown to influence dramatically the frequency respons…
The excitation energy dependence of the three-hole satellites in the L3-M4,5M4,5 and L2-M4,5M4,5 Auger spectra of nickel metal has been measured using synchrotron radiation. The satellite behavior in the non-radiative emission spectra at the L3 and L2 thresholds is compared and the influence of the Coster-Kronig channel explored. The three-hole satellite intensity at the L3 Auger emission line reveals a peak structure at 5 eV above the L3 threshold attributed to resonant processes at the 2p53d9 shake-up threshold. This is discussed in connection with the 6-eV feature in the x-ray absorption sp…
We present quantum mechanical calculations of Auger decay rates for two Rubidium Rydberg atoms with weakly overlapping electron clouds. We neglect exchange effects and consider tensor products of independent atom states forming an approximate basis of the two-electron state space. We consider large sets of two-atom states with randomly chosen quantum numbers and find that the charge overlap between the two Rydberg electrons allows one to characterise the magnitude of the Auger decay rates. If the electron clouds overlap by more than one percent, the Auger decay rates increase approximately exp…
We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a timescale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron laser. The production and decay of these states is characterized by photoelectron spectroscopy and Auger electron spectroscopy. In molecules, two types of double core holes are expected, the first with two core holes on the same N atom, and the second with one core hole on each N atom. We report the first direct observations of the former type of core hole …
The Auger decay is a relevant recombination channel during the first few femtoseconds of molecular targets impinged by attosecond XUV or soft X-ray pulses. Including this mechanism in time--dependent simulations of charge--migration processes is a difficult task, and Auger scatterings are often ignored altogether. In this work we present an advance of the current state-of-the-art by putting forward a real--time approach based on nonequilibrium Green's functions suitable for first-principles calculations of molecules with tens of active electrons. To demonstrate the accuracy of the method we re…
