Recoil Ions Research Articles

CO Dissociation Induced by 1 keV/u Ar2+ Ion

CO is one of the important molecules in dense molecular clouds, and its dissociation induced by cosmic ray heavy ions is a fundamental process for molecular breaking up and rearrangement in astronomical networks. Extensive laboratory simulations are required to understand molecular evolution in astrophysical contexts. Here, we investigate the CO dissociation induced by 1 keV/u Ar2+ using cold target recoil ion momentum spectroscopy. Kinetic energy release for double electron capture Ar2++CO→Ar0+C++O+ and transfer ionization Ar2++CO→Ar++C++O++e− was obtained. The dissociation mechanisms are attributed to different KER distributions. The autoionization process is identified below the CO2+ double ionization threshold.

Impact of Nuclear Motion on Light-Induced Bimolecular Interaction Dynamics

In chemical reactions, the nuclear motion of the molecules plays a crucial role in determining the reaction rates and outcomes. Employing the cold target recoil ion momentum spectroscopy and femtosecond pump-probe techniques, we perform a molecular-level study into the influence of nuclear vibrations on light-induced bimolecular reactions within H2−D2 dimers. The study focuses on the formation dynamics of D2H+ and H2D+ cations, shedding light on the interplay between translational and vibrational motions of the nuclei steering the bimolecular reactions. Our observations reveal a notable yield ratio of 1:1.6 between H2D+ and D2H+ channels, accompanied with a faster formation of D2H+ compared to H2D+. Molecular dynamics simulations unveil that the faster vibrational motion of H2+ than that of D2+ upon single ionization within the dimer accounts for these differences. Our findings provide new insight into the time-resolved kinetic isotope effect on the bimolecular reactions, highlighting the critical relationship between nuclear vibrational motions and reaction dynamics. Published by the American Physical Society 2024

Absolute electron impact ionization cross-sections for CF4: Three dimensional recoil-ion imaging combined with the relative flow technique.

Here we present measurements of dissociative and non-dissociative cross-sections for the electron impact of the CF4 molecule. The present experiments are based on a Recoil Ion Momentum Spectrometer (RIMS), a standard gas mixing setup for CF4, and a reference gas. The measurements were carried out at several electron energies up to 1keV, covering the energy range of previous experiments. We apply the relative flow technique (RFT) to convert the relative cross-sections measured by the RIMS into absolute values. Using the combination of RIMS and RFT, ion collection and calibration errors were minimized. The results were compared with theoretical and experimental studies available in the literature. Previous electron impact experiments present relative cross-sections or use correction terms for the absolute cross-sections due to losses of energetic ions. We elucidate the differences between the new measurement method and the existing ones in the literature and explain why the present method can be considered reliable. Furthermore, we show how reducing correction terms affects the results.

Demonstration of full polarization control of soft X-ray pulses with Apple X undulators at SwissFEL using recoil ion momentum spectroscopy.

The ability to freely control the polarization of X-rays enables measurement techniques relying on circular or linear dichroism, which have become indispensable tools for characterizing the properties of chiral molecules or magnetic structures. Therefore, the demand for polarization control in X-ray free-electron lasers is increasing to enable polarization-sensitive dynamical studies on ultrafast time scales. The soft X-ray branch Athos of SwissFEL was designed with the aim of providing freely adjustable and arbitrary polarization by building its undulator solely from modules of the novel Apple X type. In this paper, the magnetic model of the linear inclined and circular Apple X polarization schemes are studied. The polarization is characterized by measuring the angular electron emission distributions of helium for various polarizations using cold target recoil ion momentum spectroscopy. The generation of fully linear polarized light of arbitrary angle, as well as elliptical polarizations of varying degree, are demonstrated.

Nondipolar photoelectron angular distributions from fixed-in-space N2 molecules

We investigate experimentally and theoretically the N 1s photoionization of fixed-in-space N2 molecules at a photon energy of 880 eV. In our experiment, we employed circularly polarized synchrotron radiation for the photoionization and coincident electron and fragment-ion detection using cold target recoil ion momentum spectroscopy. The accompanying angle-resolved calculations were carried out by the multichannel single-center method and code within the frozen-core Hartree–Fock approximation. The computed emission distributions exhibit two distinct features along the molecular axis, which are the results of a superposition of the direct and nearest-neighbor scattering amplitudes for the photoemission from two nitrogen atoms. In the electric-dipole approximation, these peaks are symmetric with respect to both nitrogen atoms. Including nondipole (retardation) effects in the calculations results in a simultaneous increase and decrease of the scattering peaks towards the nitrogen atoms pointing in the forward and backward directions along the light propagation, respectively. These theoretical findings are in agreement with our experimental findings.

Charge-symmetric and -asymmetric fragmentation dynamics of argon dimers in slow Ar8+–Ar2 collisions

We present an experimental study of multiple-electron capture-induced fragmentation dynamics of Ar2m+ (4 ≤m≤ 7) dimer ions in 4 keV/u Ar8+–Ar2 collisions. The fragment recoil ion pairs and the charge-changing projectiles are coincidentally measured using a double coincidence technique. The branching ratios between the different charge-sharing fragmentation channels show an inherent enhancement of the asymmetric channels. The kinetic energy release (KER) distributions for the associated electron capture process show a shift in the mean KER values toward the higher side with increasing capture stabilization. The interplay between the different projectile autoionization processes sheds light on the energy depositions to the system during collisions. The Coulomb potential energy curves give a physical insight into the role of the projectile final states in the dimer fragmentation dynamics. The dimer-axis orientation-dependent cross sections for the asymmetric fragmentation channels reveal a forward–backward asymmetry that arises from the geometry of the collision system. Our findings thus give insight into the impact parameter-controlled fragmentation dynamics of multiply charged Ar2m+ dimer ions in highly charged ion–dimer slow collisions.

Contribution of different electron-capture mechanisms in the fragmentation of CO23+ upon slow ion-molecule collision

Abstract We present recoil ion - projectile ion coincidence study on the three body fragmentation of CO23+ ion into C+ + O+ + O+ fragments upon impact with
Ar3+, Ar6+ and Ar8+ projectile ions having the same velocity of vp = 0.49 a.u. (atomic units) using recoil ion momentum imaging technique. The kinetic energy
release (KER) distributions are presented and effect of different electron-capture associated processes such as pure capture, electron capture followed by target ionization or projectile auto-ionization is discussed based on the analysis of KER corresponding to different final projectile charge state post collision. As the capture stabilization increased the relative yields in the KER distribution are found to decrease in the high KER side for low charged Ar3+ impact, while an increase is observed for Ar6+ and Ar8+ impacts. We discussed the interplay between electron-capture, projectile auto-ionization and target ionization for the dominance of particular process. We also observed a low-KER feature around 15 eV which was observed for electron
and proton impacts, which was not yet observed for highly charged ion impacts

A high resolution reaction microscope with universal two-region time-focusing method.

This paper presents a novel reaction microscope designed for ion-atom collision investigations, established at the Institute of Modern Physics, Chinese Academy of Sciences, Lanzhou, China. Its time-of-flight (TOF) spectrometer employs an innovative flight-time focusing method consisting of two acceleration regions, providing optimal time focusing conditions for charged fragments with diverse initial velocities. The TOF spectrometer's axis intentionally tilts by 12° relative to the ion beam direction, preventing potential obstructions from the TOF grid electrodes. The introduced focusing method allows for a flexible time-focusing TOF spectrometer design without restricting the length ratio of the two regions. In addition, this configuration in our case significantly suppresses noise on the recoil ion detector produced by residual gas in the ion beam trajectory, which is a considerable challenge in longitudinal spectrometers. In a test experiment on the single electron capture reaction involving 62.5 keV/u He2+ ions and a helium atomic beam, the recoil longitudinal momentum resolution achieved 0.068 atomic units. This novel configuration and successful test run show excellent precision for ion-atom collision studies.

Experimental measurement of state selective double electron capture in 1.4-20 keV/u Ar<sup>8+</sup> collision with He

Electron(s) capture in highly charged ions collision with atoms and molecules is a fundamental process related to the electron transition between bound states belongs to two atomic-centers. The X-ray emission following electron capture is important for X-ray astrophysical modeling, fusion plasma diagnosing, and ion irradiated biophysics. Over past decades, momentum-imaging cold-target recoil ion momentum spectroscopy is one of significantly developed techniques and has been widely applied to measure the quantum state-selective population in electron(s) capture processes. Based on the cold target recoil ion momentum spectroscopy mounted at the 150 kV highly charged ion platform in Fudan University, the state-selectivity of double electron capture in 1.4-20 keV/u Ar<sup>8+</sup> on He collision was measured, and the relative cross sections of the 3<i>l</i>3<i>l</i>’to 3<i>l</i>7<i>l</i>’ double excited states were obtained. It is found that with the increase of collision energy, more quantum state-selectivity channels are open in the double electron capture (DEC) of Ar<sup>8+</sup>-He collision. It is also found that the relative cross section of the quantum state population is strongly dependent on the collision energy of the projectile ion. This present measurement not only enriches the state-selective cross-section repository and collision dynamics for highly charged ion charge exchange processes, but also provides experimental benchmarks for the available theoretical calculations.

Addressing three-body fragmentation of methane dication using "native frames": Evidence of internal excitation in fragments.

The three body fragmentation of methane dication has been studied using the technique of cold target recoil ion momentum spectroscopy. The process is initiated by impact of energetic Ar9+ ions on neutral methane and the data is subsequently collected in coincidence with Ar8+ projectile. By analysing the dissociation channels leading to (H + H+ + CH2+) and (H + H2+ + CH+) fragments, it is concluded that these fragments are formed in a sequential manner via formation of molecular intermediates CH3+ and CH2+ respectively. It is shown that these molecular intermediates carry a few eVs as their internal energies, part of which is released when they emit an H-atom with the open possibility that the final detected fragments may still be internally excited. This was accomplished by analysing the two-steps of the sequential process in their own native frames. For a molecular system having three-dimensional structure, our results prove to be an ideal example to highlight the importance of using native frames for correct interpretation of the obtained results. Our results indicate that the dissociation of methane dication can be a major source of production of H-atoms in addition to H+ fragments with the probability of the two being of similar order.

State-selective charge exchange cross sections in collisions of highly-charged sulfur ions with helium and molecular hydrogen

The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations. In the present work, using the cold target recoil ion momentum spectroscopy, for the first time we investigated the state-selective single electron capture processes for S q+–He and H2 (q = 11–15) collision systems at an impact energy of q × 20 keV and obtained the relative state-selective cross sections. The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process. In particular, the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers. It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model. The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.

Precollision effect on the double ionization of an Ar atom driven by a two-color counter-rotating circularly polarized laser pulse

The double ionization process of an Ar atom driven by a two-color counter-rotating circularly polarized (TCCP) laser pulse is theoretically investigated. Classical trajectory analysis reveals that a significant portion of Nonsequential Double Ionization (NSDI) events occurs through precollision, rather than the well-known recollision mechanism. In the precollision-induced Nonsequential Double Ionization (PCDI) process, the two electrons exhibit a tendency for back-to-back emission, resulting in a lower electronic correlation effect, and the ion recoil momentum concentrated in the zero momentum region. On the other hand, in the recollision-induced Nonsequential Double Ionization (RCDI) process, the two electrons tend to emit in the same direction, leading to a higher electronic correlation effect, and the ion recoil momentum is situated far from the zero momentum region. Moreover, both PCDI and RCDI strongly depend on the parameters of the driving laser pulse. Therefore, the primary mechanism of double ionization can be experimentally probed by observing the corresponding ion recoil momentum.

Detection of recoil ion in the beta decay of laser oriented trapped radioactive isotopes for the MORA Project

The Matter’s Origin from RAdioActivity (mora) project focuses on ion manipulation in traps and laser orientation methods for the searches of New Physics (np) in nuclear beta decay by precisely measuring the D correlation parameter. We predominantly have focussed here on the detection configuration of mora and alongside talked in detail about the Recoil Ion DEtection system (ride) and its characterization focusing mainly on the methods applied to achieve high order position correction.

H2 formation via non-Born-Oppenheimer hydrogen migration in photoionized ethane

Neutral H2 formation via intramolecular hydrogen migration in hydrocarbon molecules plays a vital role in many chemical and biological processes. Here, employing cold target recoil ion momentum spectroscopy (COLTRIMS) and pump-probe technique, we find that the non-adiabatic coupling between the ground and excited ionic states of ethane through conical intersection leads to a significantly high yield of neutral H2 fragment. Based on the analysis of fingerprints that are sensitive to orbital symmetry and electronic state energies in the photoelectron momentum distributions, we tag the initial electronic population of both the ground and excited ionic states and determine the branching ratios of H2 formation channel from those two states. Incorporating theoretical simulation, we established the timescale of the H2 formation to be ~1300 fs. We provide a comprehensive characterization of H2 formation in ionic states of ethane mediated by conical intersection and reveals the significance of non-adiabatic coupling dynamics in the intramolecular hydrogen migration.

Publisher’s Note: “Development of a cold target recoil ion momentum spectrometer and a projectile charge state analyzer setup to study electron transfer processes in highly charged ion–atom/molecule collisions” [Rev. Sci. Instrum. 93, 113313 (2022)

Publisher’s Note: “Development of a cold target recoil ion momentum spectrometer and a projectile charge state analyzer setup to study electron transfer processes in highly charged ion–atom/molecule collisions” [Rev. Sci. Instrum. 93, 113313 (2022)

Fragmentation Dynamics of CO2q+ (q = 2, 3) in Collisions with 1 MeV Proton

The fragmentation dynamics of the CO2q+ (q = 2, 3) molecular ions formed under the impact of 1 MeV protons is studied using a recoil ion momentum spectrometer equipped with a multi-hit time- and position-sensitive detector. Both two-body and three-body fragmentation channels arising from the doubly and triply ionized molecular ions of CO2 are identified and analyzed. Kinetic energy release (KER) distributions have been obtained for various channels. With the help of Dalitz plots and Newton diagrams concerted and sequential processes have been assigned to observed fragmentation channels. In addition, angular correlations are used to determine the molecular geometry of the precursor molecular ion. It is found that the symmetric breakup into C+ + O+ + O+ involves asymmetric stretching of the molecular bonds in CO23+ prior to dissociation via concerted decay implying the fact that collisions with 1 MeV proton induces an asynchronous decay in CO2.

Segmented silicon-based solid-state detector with thin dead layer for superheavy element research

Silicon-based solid-state detectors (SSDs) are crucial for investigating the properties of superheavy elements (SHEs), since they measure the energy of SHEs and charged particles that are emitted as successive decay events of the SHEs. We have developed a segmented SSD for SHE studies using the new gas-filled recoil ion separators (GARIS-II and GARIS-III) at RIKEN. It is based on a back-illuminated Si PIN photodiode in which the irradiation is through the N+ layer. The detector is introduced as a side one for the GARIS focal plane detection system. To investigate the characteristics of the SSD, 241Am α particles were irradiated by automatically moving and rotating the α source for each segmented portion of the SSD. A Monte Carlo simulation was also performed to estimate the dead layer thickness of the segmented SSD.

Cold-target electron-ion-coincidence momentum-spectroscopy study of electron-impact single and double ionization of N2 and O2 molecules

We report experimental studies of electron-impact ionization of nitrogen (${\mathrm{N}}_{2}$) and oxygen (${\mathrm{O}}_{2}$) molecules using a cold target recoil ion momentum spectrometer (COLTRIMS, reaction microscope). The recoil ion is detected in coincidence with one outgoing electron such that the momentum vectors and consequently the kinetic energies for these final-state particles are determined. The ionization cross sections for producing the doubly and singly charged parent ions were measured as a function of the incident electron energy ranging from 50 to 600 eV. For molecular dications, e.g., ${\mathrm{O}}_{2}^{2+}$, the cross sections are obtained by measuring both the ion time of flight and two-dimensional position spectra, which is demonstrated to be an efficient way to suppress the contribution of the dissociation channels with the ${\mathrm{O}}^{+}$ products as both ions have the identical mass-to-charge ratios. The projectile energy-loss spectra correlated to the final-state ions are obtained, which provide direct evidence of the ionization mechanisms of ${\mathrm{N}}_{2}$ and ${\mathrm{O}}_{2}$ molecules. It is found that the ${\mathrm{O}}_{2}^{2+}$ dication is produced mainly by Auger process after single ionization in $2{\ensuremath{\sigma}}_{g}$ inner-valence shell of ${\mathrm{O}}_{2}$ molecule, while the ${\mathrm{N}}_{2}^{2+}$ dication is generated by the direct removal of two electrons from the outermost $3{\ensuremath{\sigma}}_{g}$ orbital of ${\mathrm{N}}_{2}$ molecule.

Low-Energy Collisions of Zeeman-Decelerated NH Radicals with He Atoms.

We report an experimental study of state-to-state inelastic scattering of NH (X 3Σ-, N = 0, j = 1) radicals with He atoms. Using a crossed molecular beam apparatus that combines a Zeeman decelerator and velocity map imaging, we study both integral and differential cross sections in the N = 0, j = 1 → N = 2, j = 3 inelastic channel. We developed various new REMPI schemes to state-selectively detect NH radicals, and tested their performance in terms of sensitivity and ion recoil velocity. We found a 1 + 2' + 1' REMPI scheme using the A 3Π ← X 3Σ- resonant transition, which yields acceptable recoil velocities and is more than an order of magnitude more sensitive than conventional one-color REMPI schemes to detect NH. We used this REMPI scheme to probe state-to-state integral and differential cross sections around the channel opening at 97.7 cm-1, as well as at higher energies where structure in the scattering images could be resolved. The experimental results are in excellent agreement with the predictions from quantum scattering calculations which are based on an ab initio NH-He potential energy surface.

Exploring three-body fragmentation of acetylene trication.

The three-body breakup of [C2H2]3+ formed in collision with Xe9+ moving at 0.5 atomic units of velocity is studied by using recoil ion momentum spectroscopy. Three-body breakup channels leading to (H+, C+, CH+) and (H+, H+, C2 +) fragments are observed in the experiment and their kinetic energy release is measured. The breakup into (H+, C+, CH+) occurs via concerted and sequential modes, whereas the breakup into (H+, H+, C2 +) shows only the concerted mode. By collecting events coming exclusively from the sequential breakup leading to (H+, C+, CH+), we have determined the kinetic energy release for the unimolecular fragmentation of the molecular intermediate, [C2H]2+. By using ab initio calculations, the potential energy surface for the lowest electronic state of [C2H]2+ is generated, which shows the existence of a metastable state with two possible dissociation pathways. A discussion on the agreement between our experimental results and these ab initio calculations is presented.