Angle-differential Cross Sections Research Articles

Ion molecule reaction dynamics for disentangling competing reactive pathways

Ion molecule reaction dynamics for disentangling competing reactive pathways

Dynamics of carbene formation in the reaction of methane with the tantalum cation in the gas phase.

The controlled activation of methane has drawn significant attention throughout various disciplines over the last few decades. In gas-phase experiments, the use of model systems with reduced complexity compared to condensed-phase catalytic systems allows us to investigate the intrinsic reactivity of elementary reactions down to the atomic level. Methane is rather inert in chemical reactions, as the weakening or cleavage of a C-H bond is required to make use of methane as C1-building block. The simplest model system for transition-metal-based catalysts is a mono-atomic metal ion. Only a few atomic transition-metal cations activate methane at room temperature. One of the most efficient elements is tantalum, which forms a carbene and releases molecular hydrogen in the reaction with methane: Ta+ + CH4 → TaCH2+ + H2. The reaction takes place at room temperature due to efficient intersystem crossing from the quintet to the triplet surface, i.e., from the electronic ground state of the tantalum cation to the triplet ground state of the tantalum carbene. This multi-state reactivity is often seen for reactions involving transition-metal centres, but leads to their theoretical treatment being a challenge even today. Chemical reactions, or to be precise reactive collisions, are dynamic processes making their description even more of a challenge to experiment and theory alike. Experimental energy- and angle-differential cross sections allow us to probe the rearrangement of atoms during a reactive collision. By interpreting the scattering signatures, we gain insight into the atomistic mechanisms and can move beyond stationary descriptions. Here, we present a study combining collision energy dependent experimentally measured differential cross sections with ab initio calculations of the minimum energy pathway. Product ion velocity distributions were recorded using our crossed-beam velocity map imaging experiment dedicated to studying transition-metal ion molecule reactions. TaCH2+ velocity distributions reveal a significant degree of indirect dynamics. However, the scattering distributions also show signatures of rebound dynamics. We compare the present results to the oxygen transfer reaction between Ta+ and carbon dioxide, which we recently studied.

Dynamics of the Oxygen Atom Transfer Reaction between Carbon Dioxide and the Tantalum Cation.

The understanding of fundamental atomic-level processes often requires well-defined model systems. The oxygen atom transfer from CO2 to a transition metal cation in the gas phase presents such a model system. We investigate the reaction of Ta+ + CO2 for which the formation of TaO+ is highly efficient and attributed to multistate reactivity. Here, we study the atomistic dynamics of the oxygen atom transfer reaction by recording experimental energy and angle differential cross sections by crossed beam velocity map imaging supported by ab initio quantum chemical calculations. Product ion velocity distributions are dominated by signatures for indirect dynamics, despite the reaction being highly exothermic. Product kinetic energy distributions show little dependence on additional collision energy even with only four atoms involved, which hints at dynamical trapping behind a submerged barrier.

Strongly perturbed state-selective charge exchange between slowAr8+and He

We report an experimental and theoretical study of state-selective charge exchange processes in ${\mathrm{Ar}}^{8+}$ on He collisions at 1 and 3 keV/amu, benchmarking the fundamental electron capture dynamics under strong perturbations. The quantum-state selectivity has been experimentally resolved for one $1s$ electron of He capture into $4s$, $4p$, $4d+4f$, and $5s$ states of ${\mathrm{Ar}}^{7+}$ ion along with the corresponding scattering angle differential cross sections. By comparing to theoretical calculations with a two-active-electron semiclassical asymptotic-state close-coupling approach, we are able to verify the important role of electronic correlations during the collisions and that the impact parameter sensitive transition probability significantly mediates the state-selective specifics.

Angle-differential cross sections for Rayleigh scattering of highly linearly polarized hard x rays on Au atoms

We perform a study on Rayleigh scattering of highly linearly polarized hard x rays on a thin Au foil target. In the study the angular distribution of the scattered radiation is analyzed in a relativistic regime both within and out of the plane of polarization of the incident beam. Within this experiment we scatter a synchrotron beam with a photon energy of 175 keV on a high-$Z$ target foil, namely, gold. Our findings correlate well with state-of-the-art calculations of the scattering process performed in the framework of quantum electrodynamics and may have considerable impact on future experiments regarding a polarization-resolved analysis of Delbr\"uck scattering. Furthermore, we show that the angular distribution of Rayleigh scattering can be used for a highly sensitive determination of the degree and orientation of the linear polarization of the incident hard-x-ray beam, if we rely on the theoretical framework.

A new R-matrix module for multi-channel calculations with GECCCOS

A versatile new R-matrix module for multi-channel reaction calculations was introduced into the code GECCCOS (GEneral Coupled-Channel COde System) which has been developed by the nuclear data group at TU-Wien to perform nuclear reaction calculations especially for light nuclear systems. It provides a tool for phenomenological R-matrix analyses of reaction data combined with calculations of a potential-based calculable R-matrix using the Lagrange-mesh technique. In addition it provides a platform for the development of non-standard extensions of R-matrix theory such as Reduced R-matrix analyses and the Hybrid R-matrix. A successful run of the code yields the complete S-matrix (collision matrix) as well as observables for unpolarized beams, angle-differential cross sections, excitation functions and, if existing, angle-integrated cross sections. Recently, extensions to polarization observables for spin-1/2 and spin-1 particles were implemented and tested. For phenomenological R-matrix analyses a separate module assembles calculated and available experimental values, automatically performs transformations with regard to reference frame and matching radii. Furthermore it allows to switch between incident channel and compound nucleus representation and provides the necessary feedback for the chi2 fitting process.

Imaging the Atomistic Dynamics of Single Proton Transfer and Combined Hydrogen/Proton Transfer in the O- + CH3I Reaction.

We report on reactive scattering studies of the proton transfer and combined hydrogen/proton transfer in the O- + CH3I reaction. We combine state-of-the-art crossed-beam velocity map imaging and quantum chemistry calculations to understand the dynamics for the formations of the CH2I- + OH and CHI- + H2O products. The experimental velocity- and angle-differential cross section show for both products and at all collision energies (between 0.3 and 2.0 eV) that the product ions are predominantly forward scattered. For the CHI- + H2O channel, the data show lower product velocities, indicative of higher internal excitation, than in the case of single proton transfer. Furthermore, our results suggest that the combined hydrogen/proton transfer proceeds via a two-step process: In the first step, O- abstracts one H atom to form OH-, and then the transient OH- removes an additional proton from CH2I to form the energetically stable H2O coproduct.

Measurement of differential cross sections of neutron-induced deuteron production reactions on carbon from 25 to 52 MeV * *Supported by the National Natural Science Foundation of China (11775006) and the National Key R&D Program of China (2016YFA0401604)

The angle-differential cross sections of neutron-induced deuteron production from carbon were measured at six neutron energies from 25 to 52 MeV relative to those of n-p elastic scattering at the China Spallation Neutron Source (CSNS) Back-n white neutron source. By employing the Δ E-E telescopes of the Light-charged Particle Detector Array (LPDA) system at 15.1° to 55.0° in the laboratory system, ratios of the angle-differential cross sections of the 12C(n, xd) reactions to those of the n-p scattering were measured, and then, the angle-differential cross sections of the 12C(n, xd) reactions were obtained using the angle-differential cross sections of the n-p elastic scattering from the JENDL-4.0/HE-2015 library as the standard. The obtained results are compared with data from previous measurements, all of which are based on mono-energic neutrons, the evaluated data from the JENDL-4.0/ HE-2015 library and the ENDF-B/VIII.0 library, and those from theoretical calculations based on INCA code and Talys-1.9 code. Being the first white-neutron-source-based systematic measurement of the angle-differential cross sections of neutron-induced deuteron production reactions on carbon in several tens of MeV, the present work can provide a reference to the data library considering the lack of experimental data.

Radiobiological effectiveness of iodouracil and the influence of atomic giant resonance

Hadron therapy combined with nanotechnology has been proposed as an elegant alternative for cancer treatment. Internal amplification of electron emission causing radiobiological effectiveness in nanoinserted biomolecules is of prime importance and has been measured here for the iodouracil molecule. Our experiment involves the measurement of angle and energy resolved double differential cross section (DDCS) of electron emission from iodouraciil and uracil (and also water) in collisions with fast ${\mathrm{C}}^{6+}$ ions. The electron emission from iodouracil is substantially enhanced over that from uracil or water. The enhancement is much larger than the state-of-the-art model for Coulomb ionization based on the continuum distorted wave-eikonal initial state (CDW-EIS) approximation. The electron sensitizing factor ($\ensuremath{\approx}2.4$) is in excellent agreement with the strand-breaking sensitizing factor ($\ensuremath{\approx}2.0$) for metal nanoparticle embedded in a DNA. The enhancement is explained in terms of collective excitation of strongly correlated 4d electrons, known as atomic giant dipole resonance (GDR) in I atoms. The GDR contribution to the enhancement is derived, which is in excellent agreement with recent theoretical prediction, thereby providing conclusive experimental evidence of the crucial role of collective excitation in radio sensitization.

Electron-impact excitation of the ( 5s25p ) P1/22→(5s26s ) S1/22 transition in indium: Theory and experiment

We present angle-integrated and angle-differential cross sections for electron-impact excitation of the (5s25p)P1/22→(5s26s)S1/22 transition in atomic indium. Experimental data for six incident electron energies between 10 and 100 eV are compared with predictions from semirelativistic and fully relativistic B-spline R-matrix calculations, as well as a fully relativistic convergent close-coupling model. Agreement between our measured and calculated data is, with a few exceptions, found to be typically very good. Additionally, the agreement between the present theoretical predictions is generally excellent, with the remaining small deviations being associated with the slightly different, although still very accurate, descriptions of the target structure. Agreement between the present results and an earlier relativistic distorted-wave computation [T. Das, R. Srivastava, and A. D. Stauffer, Phys. Lett. A 375, 568 (2011)PYLAAG0375-960110.1016/j.physleta.2010.12.037] was, however, found to be marginal, particularly at 10 and 20 eV.

First measurement of electron neutrino scattering cross section on argon

We report the first electron neutrino cross section measurements on argon, based on data collected by the ArgoNeuT experiment running in the GeV-scale NuMI beamline at Fermilab. A flux-averaged $\nu_e + \overline{\nu}_e$ total and a lepton angle differential cross section are extracted using 13 $\nu_e$ and $\overline{\nu}_e$ events identified with fully-automated selection and reconstruction. We employ electromagnetic-induced shower characterization and analysis tools developed to identify $\nu_e/\overline{\nu}_e$-like events among complex interaction topologies present in ArgoNeuT data ($\langle E_{\bar{\nu}_e} \rangle = 4.3$ GeV and $\langle E_{\nu_e} \rangle = 10.5$ GeV). The techniques are widely applicable to searches for electron-flavor appearance at short- and long-baseline using liquid argon time projection chamber technology. Notably, the data-driven studies of GeV-scale $\nu_e/\overline{\nu}_e$ interactions presented in this Letter probe an energy regime relevant for future DUNE oscillation physics.

Elastic Photon Scattering on Hydrogenic Atoms near Resonances

Scattering of light on relativistic heavy ion beams is widely used for characterizing and tuning the properties of both the light and the ion beam. Its elastic component—Rayleigh scattering—is investigated in this work for photon energies close to certain electronic transitions because of its potential usage in the Gamma Factory initiative at CERN. The angle-differential cross-section, as well as the degree of polarization of the scattered light are investigated for the cases of 1 s − 2 p 1 / 2 and 1 s − 2 p 3 / 2 resonance transitions in H-like lead ions. In order to gauge the validity and uncertainty of frequently used approximations, we compare different methods. In particular, rigorous quantum electrodynamics calculations are compared with the resonant electric-dipole approximation evaluated within the relativistic and nonrelativistic formalisms. For better understanding of the origin of the approximation, the commonly used theoretical approach is explained here in detail. We find that in most cases, the nonrelativistic resonant electric-dipole approximation fails to describe the properties of the scattered light. At the same time, its relativistic variant agrees with the rigorous treatment within a level of 10% to 20%. These findings are essential for the design of an experimental setup exploiting the scattering process, as well as for the determination of the scattered light properties.

Quantum mechanical potentials and inactive electron effects in charge exchange collisions

Scattering angle differential cross sections for the He+ + He single electron capture process are studied using plane wave Born approximation models for projectile energies between 180 keV and 1.89 MeV. Within this simplistic framework, we study the effects of the frozen core approximation by performing a full 5-Body calculation that explicitly includes all particles in the collision and comparing it with a single bound state model that neglects the bound electron in the projectile and a double bound state model that neglects the inactive electron in the target atom. Results are compared with experiment and we show that inclusion of the inactive electron in the perturbation potential is more important than inclusion in the wave functions. We also introduce a semi-quantum mechanical (SQM) perturbation potential that treats the atomic electrons as a quantum mechanical electron cloud rather than point particles. The SQM perturbation removes the deep, unphysical minimum that exists in cross sections calculated with Born-type models, but also has the effect of greatly reducing the magnitude of the small scattering angle cross sections.

Symmetry-breaking effects on time-dependent dynamics: correct differential cross sections and other properties in H+ + C2H4 at ELab = 30 eV.

We present a computational procedure that introduces low degrees of symmetry breaking into a restricted Hartree-Fock (RHF) state in order to induce higher symmetry breaking during the state's subsequent dynamics. The symmetries herein considered are those of electronic HF states as classified by Fukutome; those symmetries affect bond dissociations and internal rotations among other phenomena. Therefore, this investigation extends a part of Fukutome's time-independent analysis of symmetry breaking to the time-dependent (dynamical) regime. The procedure is formulated in the framework of the simplest-level electron nuclear dynamics, a time-dependent, variational, on-the-fly and non-adiabatic method that employs classical dynamics for the nuclei and a Thouless single-determinantal state for the electrons. We test this procedure on the H+ + C2H4 reaction at 30 eV due to its conspicuous display of symmetry-breaking effects; this reaction is relevant in astrophysics and proton cancer therapy. Fukutome's axial spin density wave (ASDW) HF state is used to represent the symmetry-broken initial states. Through a Thouless parameter, small degrees of symmetry breaking are introduced into the initial ASDW states in a controlled manner. After starting the dynamics from those states, higher degrees of symmetry breaking emerge or not as determined by the direct-dynamics equations without external interventions. Simulations starting from symmetry-conforming states preserve symmetry features during dynamics, whereas simulations starting from symmetry-broken states display an upsurge of symmetry breaking when the reactants collide. Initial symmetry breaking increases the total integral cross sections of collision-induced fragmentations and of target-to-proton 1-electron-transfer reactions and decreases the scattering angle function and primary rainbow angle of the outgoing projectile. Remarkably, symmetry-breaking simulations reproduce the correct relative order and values of the experimental 0- and 1-electron-transfer differential cross sections, whereas symmetry-conforming simulations predict incorrect order and values. Our calculated scattering angle functions and differential cross sections also exhibit expected primary and secondary rainbow angle features that experiments fail to detect. A detailed discussion on the description of symmetry-breaking processes with the ASDW and Thouless states is included to provide a rigorous theoretical basis for this investigation.

Spin–spin correlations and entanglement in elastic electron scattering from hydrogen atoms

In two recent papers, Blum and Lohmann (2016 Phys. Rev. Lett. 116 033201) and Lohmann et al (2016 Phys. Rev. A 94 032331), the possibility of continuously varying the degree of entanglement between an elastically scattered electron and the valence electron of quasi-one electron targets was discussed. Here we present results for elastic electron scattering from atomic hydrogen in the energy regime of 1−10 eV and the full range of scattering angles . We confirm previous calculations at very low energies, which predicted that the hydrogen target is not a promising candidate for Bell correlations through electron collisions. This finding remains unchanged in the near-resonance regime of incident electron energies just below 10 eV. In addition to the spin-correlation parameter P, we present the angle-integrated total cross section, as well as the angle-differential cross section at a few representative collision energies.

Photoelectron distribution of nonresonant two-photon ionization of neutral atoms

Photoelectron angular distributions following the non-resonant two-photon K-shell ionization of neutral atoms are studied theoretically. Using the independent particle approximation and relativistic second-order perturbation theory, the contributions of screening and relativistic effects to the photoelectron angular distribution are evaluated. A simple nonrelativistic expression is presented for the angle-differential cross section in dipole approximation for two-photon ionization by elliptically polarized photons, and its limitations are analyzed numerically. Moreover, we show that screening effects of the inactive electrons can significantly affect the photoelectron distributions and can also lead to a strong elliptical dichroism. Numerical results are resented for the case of two-photon K-shell ionization of neutral Ne, Ge, Xe, and U atoms.

Imaging state-to-state reactive scattering in the Ar+ + H2 charge transfer reaction.

The charge transfer reaction of Ar+ with H2 and D2 has been investigated in an experiment combining crossed beams with three-dimensional velocity map imaging. Angle-differential cross sections for two collision energies have been obtained for both neutral species. We find that the product ions are highly internally excited. In the reaction with H2, the spin-orbit excited Ar+ state's coupling to the "resonant" vibrationally excited product H2+ (υ = 2) dominates for both investigated energies, in line with previous investigations. The observed angular distributions, however, show significantly less back-scattering than was found previously. Furthermore, we discovered that the product ions are highly rotationally excited. In the case of Ar+ reacting with D2, the energetically closest lying vibrational levels are not strictly preferred and higher-lying vibrational levels are also populated. For both species, the backward-scattered products show higher internal excitation.

Magnetic Moments of Excited Baryons

In project A.3, the reaction γ p → π 0 γ ’ p has been studied using the TAPS photon spectrometer in the energy range √s= 1221-1331 MeV. Energy tagged photon beams have been produced with the Glasgow tagging spectrometer from electron beams provided by the MAMI-B accelerator. Angle and energy differential cross sections have been measured and compared to theoretical calculations. This comparison allows the magnetic moment of the Δ + isobar to be extracted for the first time to μ Δ+ = [2.7 +1.3 −1.0 (stat)±1.5(syst)±3(theo)] μ N . In an extension of the A3 project to the meson sector, the time-like transition form factor of the η meson has been measured with the Crystal Ball/TAPS detector system at MAMI-C.

Many-electron effects on x-ray Rayleigh scattering by highly charged He-like ions

The Rayleigh scattering of x-rays by many-electron highly charged ions is studied theoretically. The many-electron perturbation theory, based on a rigorous quantum electrodynamics approach, is developed and implemented for the case of the elastic scattering of (high-energetic) photons by helium-like ion. Using this elaborate approach, we here investigate the many-electron effects beyond the independent-particle approximation (IPA) as conventionally employed for describing the Rayleigh scattering. The total and angle-differential cross sections are evaluated for the x-ray scattering by helium-like Ni$^{26+}$, Xe$^{52+}$, and Au$^{77+}$ ions in their ground state. The obtained results show that, for high-energetic photons, the effects beyond the IPA do not exceed 2% for the scattering by a closed $K$-shell.

Differential Cross Sections and the Impact of Model Defects in Nuclear Data Evaluation

A statistically consistent method for the inclusion of the so-called model defects into Bayesian evaluation methods based on extensive modeling is presented. The method uses Gaussian processes to define a-priori probability distributions for possible model defects. The inclusion is of particular importance for the proper evaluation of differential data, i.e. angle-differential cross sections and spectra of ejectiles. The method is successfully applied to a simple realistic example which clearly shows the impact of model defects in a simultaneous evaluation of angle-differential and angle-integrated cross sections.