Observation of Photoion Backward Emission in Photoionization of He and N2
Sven Grundmann, Max Kircher, Isabel Vela-Perez, Giammarco Nalin, Daniel Trabert, Nils Anders, Niklas Melzer, Jonas Rist, Andreas Pier, Nico Strenger, Juliane Si… 展开作者
Sven Grundmann, Max Kircher, Isabel Vela-Perez, Giammarco Nalin, Daniel Trabert, Nils Anders, Niklas Melzer, Jonas Rist, Andreas Pier, Nico Strenger, Juliane Siebert, Philipp V. Demekhin, Lothar Ph. H. Schmidt, Florian Trinter, Markus S. Schoeffler, Till Jahnke, Reinhard Doerner
We experimentally investigate the effects of the linear photon momentum on the momentum distributions of photoions and photoelectrons generated in one-photon ionization in an energy range of 300 eV $\leq~E_γ~\leq$ 40 keV. Our results show that for each ionization event the photon momentum is imparted onto the photoion, which is essentially the system's center of mass. Nevertheless, the mean value of the ion momentum distribution along the light propagation direction is backward-directed by $-3/5$ times the photon momentum. These results experimentally confirm a 90 year old prediction.
Experimental measurements of photoionization rates of $nD_{5/2}$ Rydberg states of Cs ($50 \leq n \leq 75$) in a 1064 nm far off-resonance dipole trap are presented. The photoionization rates are obtained by measuring the lifetimes of Rydberg atoms produced inside of a 1064 nm far off-resonance trap and comparing the lifetimes to corresponding control experiments in a magneto-optical trap. Experimental results for the control experiments agree with recent theoretical predictions for Rydberg state lifetimes and measured photoionization rates are in agreement with transition rates calculated fro…
The relations between photoionization cross sections and photon radius are obtained on basis of quantum mechanics and the particle-like properties of a photon. The photoionization cross sections of H atom and H-like ions, He atom and He like ions, alkali metal atoms, and Rydberg atoms are calculated using the relations. The calculation results are found to be good agreement with the known experimental data. The results show that the photoionization cross section is always smaller than the cross section of the photon to ionize the atom or ion and can be expressed as the product of the cross sec…
Photoionization of an atom in the presence of a neighboring atom of different species is studied. The latter first undergoes resonant photoexcitation, leading to an autoionizing state of the diatomic system. Afterwards, the excitation energy is transferred radiationlessly via a two-center Auger process to the other atom, causing its ionization. Assuming a fixed internuclear distance, it has been predicted theoretically that this indirect ionization pathway can strongly dominate over the direct photoionization. Here, we extend the theory of resonant two-center photoionization by including the n…
A fully relativistic calculation of the double photoionization of helium-like atoms is presented. The approach is based on the partial-wave representation of the Dirac continuum states and accounts for the retardation in the electron-electron interaction as well as the higher-order multipoles of the absorbed photon. The electron-electron interaction is taken into account to the leading order of perturbation theory. The relativistic effects are shown to become prominent already for the medium-Z ions, changing the shape and the asymptotic behaviour of the photon energy dependence of the ratio of…
The photoionization cross-sections of two even-parity excited states, $5d6d ^3D_1$ and $6s7d ^3D_{2}$, of atomic Ba at the ionization-laser wavelength of 556.6 nm were measured. We found that the total cross-section depends on the relative polarization of the atoms and the ionization-laser light. With density-matrix algebra, we show that, in general, there are at most three parameters in the photoionization cross-section. Some of these parameters are determined in this work. We also present the measurement of the radiative lifetime of five even-parity excited states of barium.
We have considered the processes of excitation and ionization of light multicharged ions by impact of high-energy particles, which proceed with participation of the $ns$ electrons. The screening corrections to the energy levels and photoionization cross sections are evaluated analytically within the framework of the non-relativistic perturbation theory with respect to the electron-electron interaction. The universal scalings for the excitation and ionization cross sections are studied for arbitrary principal quantum numbers $n$.
This is a sequel to an earlier article on the theory of angular correlation for double photoionization. Here we consider the two-step double photoionization of a rare gas atom under the influence of a polarized photon beam described by appropriate Stokes parameters. Cylindrical mirror analysers (CMA) are used to detect the outgoing electrons. Theoretical values of the correlation functions are obtained for linearly polarized light. Two different situations is handled. Once, the value of the correlation function is obtained keeping the photo-electron in a fixed direction. The other case the dir…
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 theo…
The photon-ion merged-beams technique for the photoionization of mass/charge selected ionized atoms, molecules and clusters by x-rays from synchrotron radiation sources is introduced. Examples for photoionization of atomic ions are discussed by going from outer-shell ionization of simple few-electron systems to inner-shell ionization of complex many-electron ions. Fundamental ionization mechanisms are elucidated and the importance of the results for applications in astrophysics and plasma physics is pointed out. Finally, the unique capabilities of the photon-ion merged-beams technique for the …
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 compe…
Two-photon ionization of Rubidium atoms in a magneto-optical trap and a Bose-Einstein condensate (BEC) is experimentally investigated. Using 100 ns laser pulses, we detect single ions photoionized from the condenstate with a 35(10)% efficiency. The measurements are performed using a quartz cell with external electrodes, allowing large optical access for BECs and optical lattices.
Photoionization of an atom $A$ by a strong laser field in the presence of a spatially well-separated neighboring atom $B$ is considered. The laser field frequency is assumed to lie below the ionization potential of atom $A$ and be resonant with a dipole-allowed transition in atom $B$. In this situation, the ionization may occur either directly by multiphoton absorption from the laser field at the first atomic center. Or via an indirect pathway involving two-center electron-electron correlations, where the neighbor atom $B$ is first photoexcited and, afterwards, transfers its energy upon deexci…
We offer a theoretical and experimental study of the single-photon photoionization of Ne III. The high photon flux and the high-resolution capabilities of the Advanced Light Source at the LBNL were employed to measure absolute photoionization cross sections. The resulting spectrum has been benchmarked against high accuracy relativistic Breit-Pauli $R$-matrix calculations. A large close-coupling wave function expansion which comprises up to 58 fine-structure levels of the residual ion Ne IV of configurations $2s^22p^3$, $2s2p^4$, $2p^5$, $2s^22p^23s$, $2s^22p^23p$ and $2s^22p^23d$ was included.…
It is demonstrated that recent experiments on ionization of 3p and 3s electrons in Ni film and solid body cannot be described in the frames of Hartree-Fock or the random phase approximation with exchange. The deviation is so big that from the theoretical side it requires inclusion of huge and yet not entirely understood effects. Perhaps, it requires also experimental efforts in order to clarify the prominent difference obtained for films and crystal samples.
We give examples showing that two well-known versions of the S-matrix theory, which describes a nonresonant multiphoton ionization of atoms and ions in intense laser fields, lead to qualitatively different results. The latter refer not only to total ionization rates, but also to energy distributions of photoelectrons, for instance in a polarization plane of the laser field. It should be possible to make an experiment testing predictions of both theories in the near future.
It is discovered theoretically that significant confinement resonances in an $nl$ photoionization of a \textit{multielectron} atom $A$ encaged in carbon fullerenes, A@C$_{60}$, may re-appear and be strong at photon energies far exceeding the $nl$ ionization threshold, as a general phenomenon. The reasons for this phenomenon are unraveled. The Ne $2p$ photoionization of the endohedral anion Ne@C$_{60}^{5-}$ in the photon energy region of about a thousand eV above the $2p$ threshold is chosen as case study.
Absolute cross-section measurements for valence-shell photoionization of Ar$^{+}$ ions are reported for photon energies ranging from 27.4 eV to 60.0 eV. The data, taken by merging beams of ions and synchrotron radiation at a photon energy resolution of 10 meV, indicate that the primary ion beam was a statistically weighted mixture of the $^2P^o_{3/2}$ ground state and the $^2P^o_{1/2}$ metastable state of Ar$^{+}$. Photoionization of this C$\ell$-like ion is characterized by multiple Rydberg series of autoionizing resonances superimposed on a direct photoionization continuum. Observed resonanc…
Time-delays in the photoionization of molecules are investigated. As compared to atomic ionization, the time-delays expected from molecular ionization present a much richer phenomenon, with a strong spatial dependence due to the anisotropic nature of the molecular scattering potential. We investigate this from a scattering theory perspective, and make use of molecular photoionization calculations to examine this effect in representative homonuclear and hetronuclear diatomic molecules, nitrogen and carbon monoxide. We present energy and angle-resolved maps of the Wigner delay time for single-ph…
Double photoionization by a single photon is often discussed in terms of two contributing mechanisms, {\it knock-out} (two-step-one) and {\it shake-off} with the latter being a pure quantum effect. It is shown that a quasi-classical description of knock-out and a simple quantum calculation of shake-off provides a clear separation of the mechanisms and facilitates their calculation considerably. The relevance of each mechanism at different photon energies is quantified for helium. Photoionization ratios, integral and singly differential cross sections obtained by us are in excellent agreement w…
We experimentally demonstrate a detection scheme suitable for state analysis of single optically trapped atoms in less than 1 μs with an overall detection efficiency η exceeding 98%. The method is based on hyperfine-state-selective photoionization and subsequent registration of the correlated photoion-electron pairs by coincidence counting via two opposing channel electron multipliers. The scheme enables the calibration of absolute detection efficiencies and might be a key ingredient for future quantum information applications or precision spectroscopy of ultracold atoms.
Theoretically self-consistent calculations for photoionization and (e + ion) recombination are described. An identical eigenfunction expansion for the ion is employed in coupled channel calculations for both processes, thus ensuring consistently accurate cross sections and rates in an ab initio manner. The theoretical treatment of (e + ion) recombination subsumes both the non-resonant recombination ('radiative recombination'), and the resonant recombination ('di-electronic recombination') processes in a unified scheme. In addition to the total, unified recombination rates, level-specific recom…
A methodology is developed to compute photoionization cross-sections beyond the electric dipole (BED) approximation from response theory, using Gaussian type orbitals and plane waves for the initial and final states, respectively. The methodology is applied to compute photoionization cross-sections of atoms and ions from the first four rows of the Periodic Table. Analysing the error due to the plane wave description of the photoelectron, we find kinetic energy and concomitant photon energy thresholds above which the plane wave approximation becomes applicable. The correction introduced by goin…
Experimental and theoretical results are presented for double, triple, and quadruple photoionization of Si$^+$ and Si$^{2+}$ ions and for double photoionization of Si$^{3+}$ ions by a single photon. The experiments employed the photon-ion merged-beams technique at a synchrotron light source. The experimental photon-energy range 1835--1900 eV comprises resonances associated with the excitation of a $1s$ electron to higher subshells and subsequent autoionization. Energies, widths, and strengths of these resonances are extracted from high-resolution photoionization measurements, and the core-hole…
We report measurements of energy-dependent attosecond photoionization delays between the two outer-most valence shells of N$_2$O and H$_2$O. The combination of single-shot signal referencing with the use of different metal foils to filter the attosecond pulse train enables us to extract delays from congested spectra. Remarkably large delays up to 160 as are observed in N$_2$O, whereas the delays in H$_2$O are all smaller than 50 as in the photon-energy range of 20-40 eV. These results are interpreted by developing a theory of molecular photoionization delays. The long delays measured in N$_2$O…
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 PETRAIII 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 o…
It is shown in the framework of the fully relativistic Dirac-Fock treatment of photoionization and radiative recombination processes that taking into account all significant multipoles of the radiative field is of considerable importance at electron energy higher than several keV. For the first time, we show that the relativistic Maxwell-Bolzmann distribution of continuum electrons should be used in hot thermal plasmas. This decreases the radiative recombination rate coefficient up to several multipoles compared to the non-relativistic distribution commonly used.
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 phot…
Two efficient and isotope-selective resonant two-photon ionization techniques for loading barium ions into radio-frequency (RF)-traps are demonstrated. The scheme of using a strong dipole-allowed transition at λ=553 nm as a first step towards ionization is compared to the established technique of using a weak intercombination line (λ=413 nm). An increase of two orders of magnitude in the ionization efficiency is found favoring the transition at 553 nm. This technique can be implemented using commercial all-solid-state laser systems and is expected to be advantageous compared to other narrowban…
Absolute photoionization cross-section measurements are reported for Se+ in the photon energy range 18.0-31.0 eV, which spans the ionization thresholds of the 4S_{3/2} ground state and the low-lying 2P_{3/2,1/2} and 2D_{5/2,3/2} metastable states. The measurements were performed using the Advanced Light Source synchrotron radiation facility. Strong photoexcitation-autoionization resonances due to 4p-->nd transitions are seen in the cross-section spectrum and identified with a quantum-defect analysis.
Intense laser ionization expands Einstein's photoelectric effect rules giving a wealth of phenomena widely studied over the last decades. In all cases, so far, photons were assumed to carry one unit of angular momentum. However it is now clear that photons can possess extra angular momentum, the orbital angular momentum (OAM), related to their spatial profile. We show a complete description of photoionization by OAM photons, including new selection rules involving more than one unit of angular momentum. We explore theoretically the interaction of a single electron atom located at the center of…
