Experimental Investigation of left-right Asymmetry in Photon-Atom Interaction

Single ionization of noble-gas atoms by linearly polarized synchrotron radiation has been studied by employingangle- and energy-resolved photoelectron spectroscopy. The measurements were carried out in the plane definedby the momentum and polarization vectors of the photon. Parameters describing the left-right asymmetry(LRA; relative to the photon propagation direction) of the photoelectron angular distribution were determinedexperimentally for the s shells of He, Ne, Ar, Kr, and Xe atoms and H2 molecules and for the p shells of Ne, Ar,Kr, and Xe atoms. The values of the left-right asymmetry differ significantly from zero for both subshells. Thephoton and photoelectron energy dependence of the LRA parameters is presented also. Possible experimentaland instrumental sources that could generate asymmetry are discussed and excluded as well

Near K-edge Photoionization and Photoabsorption of Singly, Doubly, and Triply Charged Silicon Ions

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 lifetime of K-shell ionized neutral silicon is inferred. In addition, theoretical cross sections for photoabsorption and multiple photoionization were obtained from large-scale Multi-Configuration Dirac-Hartree-Fock (MCDHF) calculations. The present calculations agree with the experiment much better than previously published theoretical results. The importance of an accurate energy calibration of laboratory data is pointed out. The present benchmark results are particularly useful for discriminating between silicon absorption in the gaseous and in the solid component (dust grains) of the interstellar medium

Isomer-specific photofragmentation of C3_3H3_3+^+ at the carbon K-edge

Individual fingerprints of different isomers of C$_3$H$_3$$^+$ cations have been identified by studying photoionization, photoexcitation, and photofragmentation of C$_3$H$_3$$^+$ near the carbon K-edge. The experiment was performed employing the photon-ion merged-beams technique at the photon-ion spectrometer at PETRA III (PIPE). This technique is a variant of near-edge X-ray absorption fine-structure spectroscopy, which is particularly sensitive to the 1s → π* excitation. The C$_3$H$_3$$^+$ primary ions were generated by an electron cyclotron resonance ion source. C$_3$H$_n^{2+}$ product ions with n = 0, 1, 2, and 3 were observed for photon energies in the range of 279.0 eV to 295.2 eV. The experimental spectra are interpreted with the aid of theoretical calculations within the framework of time-dependent density functional theory. To this end, absorption spectra have been calculated for three different constitutional isomers of C$_3$H$_3$$^+$. We find that our experimental approach offers a new possibility to study at the same time details of the electronic structure and of the geometry of molecular ions such as C$_3$H$_3$$^+$

Near K-edge Photoionization and Photoabsorption of Singly, Doubly, and Triply Charged Silicon Ions

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 lifetime of K-shell ionized neutral silicon is inferred. In addition, theoretical cross sections for photoabsorption and multiple photoionization were obtained from large-scale Multi-Configuration Dirac-Hartree-Fock (MCDHF) calculations. The present calculations agree with the experiment much better than previously published theoretical results. The importance of an accurate energy calibration of laboratory data is pointed out. The present benchmark results are particularly useful for discriminating between silicon absorption in the gaseous and in the solid component (dust grains) of the interstellar medium

Cover Feature: Vibrationally Resolved Inner‐Shell Photoexcitation of the Molecular Anion C2−C_{2}^− (ChemPhysChem 11/2023)

The cover illustrates the application of the photon-ion merged-beams method to vibrationally-resolved inner-shell excitation of carbon dimer anions by synchrotron radiation. Cover design by Elisa Monte. More information can be found in the Research Article by Stefan Schippers, Pierre-Michel Hillenbrand, Alexander Perry-Sassmannshausen and coworkers (https://doi.org/10.1002/cphc.202300061)

Double differential cross sections for proton induced electron emission from molecular analogues of DNA constituents for energies in the Bragg peak region

International audienceFor track structure simulations in the Bragg peak region, measured electron emission cross sections of DNA constituents are required as input for developing parameterized model functions representing the scattering probabilities. In the present work, double differential cross sections were measured for the electron emission from vapor-phase pyrimidine, tetrahydrofuran, and trimethyl phosphate that are structural analogues to the base, the sugar, and the phosphate residue of the DNA, respectively. The range of proton energies was from 75 keV to 135 keV, the angles ranged from 15° to 135°, and the electron energies were measured from 10 eV to 200 eV. Single differential and total electron emission cross sections are derived by integration over angle and electron energy and compared to the semi-empirical Hansen-Kocbach-Stolterfoht (HKS) model and a quantum mechanical calculation employing the first Born approximation with corrected boundary conditions (CB1). The CB1 provides the best prediction of double and single differential cross section, while total cross sections can be fitted with semi-empirical models. The cross sections of the three samples are proportional to their total number of valence electrons.</jats:p

Multiple Photodetachment of Carbon Anions via Single and Double Core-Hole Creation

We report on new measurements of m-fold photodetachment (m = 2 − 5) of carbon anions via K-shellexcitation and ionization. The experiments were carried out employing the photon-ion merged-beamstechnique at a synchrotron light source. While previous measurements were restricted to doubledetachment (m = 2) and to just the lowest-energy K-shell resonance at about 282 eV, our absoluteexperimental m-fold detachment cross sections at photon energies of up to 1000 eV exhibit a wealth of newthresholds and resonances. We tentatively identify these features with the aid of detailed atomic-structurecalculations. In particular, we find unambiguous evidence for fivefold detachment via double K-holeproduction

Role of L -shell single and double core-hole production and decay in m -fold ( 1 ⩽\leqslant m ⩽\leqslant 6 ) photoionization of the Ar+^+ ion

Multiple ionization of the Ar$^{+}(3s^2 3p^5)$ ion by a single photon has been investigated in the photon-energy range 250-1800~eV employing the photon-ion merged-beams technique. Absolute partial cross sections were measured for all Ar$^{(1+m)+}$ product-ion channels with 1 $\leqslant$ m $\leqslant$ 6 covering a size range from several tens of Mb down to a few b. Narrow $2p$-subshell excitation resonances were observed in all channels up to quadruple ionization at a photon-energy bandwidth of 52~meV. Double excitations involving a $2p$ and a $3s$ or $3p$ electron were also studied at high resolution and the measurements of the broad $2s$ excitation resonances directly showed their natural widths. Contributions of direct photo double ionization (PDI) to the production of the highest final Ar ion charge states are revealed, with PDI of the $2s$ subshell being mainly responsible for the production of Ar$^{7+}$. The experiment made use of the PIPE setup installed at beamline P04 of the PETRA III synchrotron light source of DESY in Hamburg. The measurements were supported by theoretical calculations to identify the main contributions to the observed cross sections. Comparisons of theory and experiment show remarkable agreement but also hint to additional ionization mechanisms that are not considered in the theoretical models such as core ionization accompanied by excitations with subsequent Auger decays leading to net $m$-fold ionization with m $\leqslant$ 4

Soft X-Ray-induced Dimerization of Methane

Carbon 1s excitation of methane, CH4, has been studied in the gas phase using the ion trap integrated with the photon–ion instrument at PETRA III/DESY and soft X-rays from the beamline P04. The created photoions are stored within the ion trap so that in further steps the photoions can undergo reactions with neutral methane molecules. The ionic photoproducts as well as reaction products created thereby are mass-over-charge analyzed by an ion time-of-flight spectrometer. Besides the photoions, product ions with up to three carbon atoms are found. In contrast to experiments using vacuum ultraviolet radiation, especially highly reactive product ions with a small number of hydrogen atoms such as ${{\rm{C}}}_{2}{{\rm{H}}}_{2}^{+}$ and ${{\rm{C}}}_{2}{{\rm{H}}}_{3}^{+}$ are found, which are important precursors for larger hydrocarbons such as C6H6. Possible production routes of the product ions are analyzed on the basis of a model that considers the probabilities for photofragmentation and the first subsequent chemical reaction step. The model indicates that the high degree of fragmentation by photons with energies around 280 eV is favoring these products. The results of the measurements show that the products like ${{\rm{C}}}_{2}{{\rm{H}}}_{2}^{+}$ and ${{\rm{C}}}_{2}{{\rm{H}}}_{3}^{+}$ can be generated by a single collision of the ionization product with neutral methane. The results suggest that soft X-rays might be important for chemical reactions in planetary atmospheres, which has usually not been taken into account. However, due to the high degree of fragmentation and large cross sections involved, they can have a large influence even when the corresponding photon flux is rather small

Near-K -edge single, double, and triple photoionization of C+C^{+} ions

Single, double, and triple ionization of the $C^{+}$ ion by a single photon have been investigated in the energy range 286 to 326 eV around the K-shell single-ionization threshold at an unprecedented level of detail. At energy resolutions as low as 12 meV, corresponding to a resolving power of 24 000, natural linewidths of the most prominent resonances could be determined. From the measurement of absolute cross sections, oscillator strengths, Einstein coefficients, multielectron Auger decay rates, and other transition parameters of the mainK-shell excitation and decay processes are derived. The cross sections are compared to results of previous theoretical calculations. Mixed levels of agreement are found despite the relatively simple atomic structure of the $C^{+}$ ion with only five electrons. This paper is a followup to a previous Letter [A. Müller et al., Phys. Rev. Lett. 114, 013002 (2015)]