Ion Storage Ring Research Articles

The first in-beam reaction measurement at CRYRING@ESR using the CARME array

AbstractIn the last decade nuclear reaction measurements using heavy ion storage rings became an important tool for nuclear astrophysics studies. The new CRYRING Array for Reaction MEasurements (CARME), recently commissioned at the low energy CRYRING@ESR storage ring (GSI/FAIR), is designed to take this novel approach one step further and perform direct nuclear reaction measurements at stellar energies, as well as indirect studies of nuclear properties of interest for nuclear astrophysics. CRYRING is unique worldwide in being able to store high quality, isotopically pure, radioactive beams produced in-flight at the low energies required for nuclear astrophysics. This paper describes the first in-beam reaction measurement with CARME at CRYRING, the first beam on (conventional) target measurement for FAIR Phase-0, and the data analysis approach required by this unprecedented, unique experimental approach.

Operational tests of CRYRING@ESR without electron cooler solenoid compensation

We have tested operation of FAIR’s low-energy ion storage ring CRYRING@ESR with uncompensated electron cooler solenoid. With its standard working point on the lowest-order difference resonance, a second solenoid is normally used to cancel betatron coupling introduced by the cooler’s magnetic field. In operation with a D+ test beam, we found that omission of the compensation solenoid did not lead to a notable deterioration of beam intensity, quality, or cooling time, though the expected coupling of betatron motion is then clearly observed.

Dielectronic recombination experiment of Na-like Kr<sup>25+</sup> at heavy ion storage ring CSRe

The experimental study of precision spectroscopy of dielectronic recombination (DR) of highly charged ions is not only important for astronomical plasma and fusion plasma, but also can be used as a new precision spectroscopy to test the strong-field quantum electrodynamic effect, measure isotope shift, and extract the radius of atomic nuclei. An specially designed electron beam energy detuning system for electron-ion recombination precision spectroscopy experiments has been installed on the heavy ion storage ring CSRe in Lanzhou, China, where the electron-ion collision energy in the center-of-mass system can be detuned to 1 keV, and an independently-developed plastic scintillator detector and multiwire proportional chamber detector have been installed downstream of the electron cooler of the CSRe for detecting recombined ions. The multiwire proportional chamber detector has the ability to non-destructively monitor the profile of the ion beam in real-time while acquiring the recombined ion counts, providing guidance for optimizing the ion beam. On this basis, the first test experiment on dielectronic recombination of Kr<sup>25+</sup> ions is carried out at the CSRe, and the dielectronic recombination rate coefficients in a range of 0–70 eV in the frame of center-of-mass are measured. In order to fully understand the experimental results, we calculate the dielectronic recombination rate coefficient of the Kr<sup>25+</sup> ion by using the flexible atomic code (FAC) and make a detailed comparison with the experimental result, showing that they are in good agreement with each other, and only the resonance energy values of the two resonance peaks at 1.695 eV and 2.573 eV are significantly different. In addition, the DR resonance energy values and intensities are obtained by fitting the experimental results in a range of 0–35 eV, and we find that the transition 3s→4l (∆<i>n</i> = 1) contributes significantly to the experimental spectral lines. Furthermore, we compare the plasma rate coefficients derived from the DR rate coefficients with those derived from the AUTOSTRUCTURE and FAC theories, which differ by 20 percent in a temperature range less than 10<sup>6</sup> K. The experimental results show that the DR experimental platform of the CSRe has very good stability and reproducibility, and can provide support for the future DR experiments of highly charged ion, i.e. for testing strong-field quantum electrodynamics effect and measuring the properties of atomic nuclei.

Hyperfine-induced effects on linear polarization following electron-impact excitation of heliumlike Tl79+ ions with nuclear spin

A most general density-matrix formalism is presented to investigate linear polarization of characteristic lines following electron-impact excitation of atoms or ions with arbitrary nuclear spin, which can account for depolarization of energy levels and multipole mixing of radiation fields. It is then applied to the linear polarization of the line radiated from heliumlike ions with nuclear spin . As an example, detailed calculations are performed for Tl79+ ions using the multi-configurational Dirac-Fock method and relativistic distorted-wave theory. It is found that the effect of the hyperfine interaction on the linear polarization depends dominantly on impact electron energy. For low impact energies close to the excitation threshold, the hyperfine interaction results in an enhancement of the linear polarization, especially for those photons emitted perpendicularly to the impact electron beam. In contrast, such a hyperfine-induced effect diminishes quickly with increasing impact energy and vanishes at medium and high energies, which is very different from the results for the case of radiative electron capture (Surzhykov et al 2013 Phys. Rev. A 87 052507). The present study is experimentally accessible at both electron-beam ion traps and ion storage rings and, thus, accurate polarization measurements at low energies can be utilized to probe the hyperfine interaction in highly charged few-electron ions.

Gas-phase electronic action absorption spectra of protonated oxygen-functionalized polycyclic aromatic hydrocarbons (OPAHs)

Context. Extended red emission (ERE) denotes a broad unassigned feature extending from 540 to 800 nm observed in many regions of the interstellar medium (ISM), and is thought to originate from photoluminescence of cosmic dust. However, definitive assignment of specific carriers remains to be achieved. Aims. Our aim is to investigate the photoabsorption spectra of astrophysically relevant protonated oxygen-functionalized polycyclic aromatic hydrocarbons (OPAHs) to probe their ability to absorb photons in the near-ultraviolet (UV) and visible (vis) spectral region and to search for any low-lying electronic states that may account for the ERE. Methods. Gas-phase electronic action absorption spectra of the protonated OPAHs were recorded in the spectral range of 200–700 nm using the ELISA ion-storage ring. Additional time-dependent density functional theory (TD-DFT) calculations were performed to compute excited state transitions that complement the experimental spectra. Results. A set of five protonated (O)PAHs was considered, namely pentacene and the four oxygen-functionalized PAHs, pentacenequinone, pentacenetetrone, anthraquinone, and phenathrenequinone. All pentacene-related species show a main absorption band between 400 and 500 nm, while the smaller OPAHs, anthraquinone and phenanthrenequinone, generally absorb further to the blue compared to the pentacenes. Interestingly, pentacenequinone and phenanthrenequinone exhibit wide absorption plateaus towards the red side of their main absorption band(s), which places them among the potential candidates to contribute to ERE. Additional photodissociation mass spectra reveal the formation of smaller functionalized PAHs and small oxygen-bearing species. Conclusions. Our results demonstrate the ability of OPAHs to absorb in the UV/vis spectral region. Among the four studied OPAHs, two revealed very broad absorption characteristics at wavelengths up to 700 nm, which makes them suitable candidates to contribute to a part of the ERE spectrum. Moreover, these two OPAHs, pentacenequinone and phenanthrenequinone, could dissociate efficiently into oxygen-bearing molecules and smaller functionalized PAHs in photon-dominated regions (PDRs) of the ISM.

Excitation and probing of low-energy nuclear states at high-energy storage rings

$^{229}\mathrm{Th}$ with a low-lying nuclear isomeric state is an essential candidate for a nuclear clock as well as many other applications. Laser excitation of the isomeric state has been a long-standing goal. With relativistic $^{229}\mathrm{Th}$ ions in storage rings, high-power lasers with wavelengths in the visible range or longer can be used to achieve high excitation rates of $^{229}\mathrm{Th}$ isomers. This can be realized through direct resonant excitation or excitation via an intermediate nuclear or electronic state, facilitated by the tunability of both the laser-beam and ion-bunch parameters. Unique opportunities are offered by highly charged $^{229}\mathrm{Th}$ ions due to the nuclear-state mixing. The significantly reduced isomeric-state lifetime corresponds to a much higher excitation rate for direct resonant excitation. Importantly, we propose electric dipole transitions changing both the electronic and nuclear states that are opened by the nuclear hyperfine mixing. We suggest using them for efficient isomer excitation in Li-like $^{229}\mathrm{Th}$ ions, via stimulated Raman adiabatic passage or single-laser excitation. We also propose schemes for probing the isomers, utilizing nuclear radiative decay or laser spectroscopy on electronic transitions, through which the isomeric-state energy can be determined with an orders-of-magnitude higher precision than the current value. The schemes proposed here for $^{229}\mathrm{Th}$ could also be adapted to low-energy nuclear states in other nuclei, such as $^{229}\mathrm{Pa}$.

Cooling dynamics of energized naphthalene and azulene radical cations.

Naphthalene and azulene are isomeric polycyclic aromatic hydrocarbons (PAHs) and are topical in the context of astrochemistry due to the recent discovery of substituted naphthalenes in the Taurus Molecular Cloud-1 (TMC-1). Here, the thermal- and photo-induced isomerization, dissociation, and radiative cooling dynamics of energized (vibrationally hot) naphthalene (Np+) and azulene (Az+) radical cations, occurring over the microsecond to seconds timescale, are investigated using a cryogenic electrostatic ion storage ring, affording "molecular cloud in a box" conditions. Measurement of the cooling dynamics and kinetic energy release distributions for neutrals formed through dissociation, until several seconds after hot ion formation, are consistent with the establishment of a rapid (sub-microsecond) Np+ ⇌ Az+ quasi-equilibrium. Consequently, dissociation by C2H2-elimination proceeds predominantly through common Az+ decomposition pathways. Simulation of the isomerization, dissociation, recurrent fluorescence, and infrared cooling dynamics using a coupled master equation combined with high-level potential energy surface calculations [CCSD(T)/cc-pVTZ], reproduce the trends in the measurements. The data show that radiative cooling via recurrent fluorescence, predominately through the Np+ D0 ← D2 transition, efficiently quenches dissociation for vibrational energies up to ≈1eV above dissociation thresholds. Our measurements support the suggestion that small cations, such as naphthalene, may be more abundant in space than previously thought. The strategy presented in this work could be extended to fingerprint the cooling dynamics of other PAH ions for which isomerization is predicted to precede dissociation.

Low-energy nuclear reactions with stored ions: a new era of astrophysical experiments at heavy ion storage rings

Heavy ion storage rings are powerful tools to store and observe key nuclear properties of rare radioactive isotopes. Recent developments in ring physics and enhanced beam intensities have now opened up the possibility to carry out low-energy investigations of nuclear reactions at rings. Pure, intense, exotic beams of isotopes that are otherwise challenging to access can be impinged on pure, ultra-thin targets, allowing the study of long-standing nuclear astrophysical puzzles in a variety of stellar sites that have so far resisted traditional approaches. In this review paper, we will describe pioneering studies with decelerated beams at the ESR storage ring at GSI (Germany), as well as future exciting prospects at the ESR and CRYRING at GSI/FAIR.

Implementation of a dipole magnet power supply control system to improve magnetic field stability at the CSRe storage ring facility for precision mass measurement

Stable magnetic field is crucial for the precision experiments conducted at the heavy ion storage rings. Besides the current stability of the power supply, the magnetic field is also influenced by varying ambient factors such as temperatures. This paper proposed a dual-loop hysteresis control method to passively change the output current of the power supply according to the magnetic field monitored by the nuclear magnetic resonance (NMR) probes. As a result, the long-term relative changes of magnetic field were reduced from dB/B≈5.75× 10−5 to 2.3 × 10−5 within three days.

Excited-state dynamics and fluorescence lifetime of cryogenically cooled green fluorescent protein chromophore anions.

Time-resolved action spectroscopy together with a fs-pump probe scheme is used in an electrostatic ion-storage ring to address lifetimes of specific vibrational levels in electronically excited states. Here we specifically consider the excited-state lifetime of cryogenically cooled green fluorescent protein (GFP) chromophore anions which is systematically measured across the S0-S1 spectral region (450-482 nm). A long lifetime of 5.2 ± 0.3 ns is measured at the S0-S1 band origin. When exciting higher vibrational levels in S1, the lifetime changes dramatically. It decreases by more than two orders of magnitude in a narrow energy region ∼250 cm-1 (31 meV) above the 0-0 transition. This is attributed to the opening of internal conversion over an excited-state energy barrier. The applied experimental technique provides a new way to uncover even small energy barriers, which are crucial for excited-state dynamics.

First Experiments with CRYRING@ESR

The low-energy heavy ion storage ring CRYRING was transported from Stockholm to Darmstadt, modernized and reconfigured, and recommissioned as CRYRING@ESR. The machine is now in operation with all installations in service and is available as a user facility for experiments proposed through the SPARC collaboration. During the 2020–2022 period, we brought a number of experimental installations into service and used them to measure first data: the ultra-cold electron cooler for merged-beam electron–ion collisions, the gas jet target for atomic collisions, a next-generation microcalorimeter-based X-ray spectroscopy setup, and others. Ions can be injected either in low charge states from a local ion source through a 300 keV/u RFQ linac, or in high charge states from the GSI accelerator chain through ESR. This allows for very broad access to ions across the entire periodic table. CRYRING@ESR is able to de- or accelerate ions and cool and store beams of isotopically pure species in a desired charge state. While the analysis is still largely ongoing, the first experimental data already show that the machine reached its expected performance level, and our high expectations regarding achievable resolution in spectroscopy experiments have been fulfilled. With access to new classes of ions available through ESR injection and a new generation of experimental instrumentation, CRYRING@ESR is a unique facility for experiments with heavy, highly charged ions. Here, we will review our present setup and machine performance, discuss the data from our first commissioning experiments and briefly preview the upcoming new installations for the coming years.

Modeling space-resolved ion dynamics in ECR plasmas for predicting in-plasma β-decay rates

Lifetimes of radioactive nuclei are known to be affected by the level configurations of their respective atomic shells. Immersing such isotopes in environments composed of energetic charged particles such as stellar plasmas can result in β-decay rates orders of magnitude different from those measured terrestrially. Accurate knowledge of the relation between plasma parameters and nuclear decay rates are essential for reducing uncertainties in present nucleosynthesis models, and this is precisely the aim of the PANDORA experiment. Currently, experimental evidence is available for fully stripped ions in storage rings alone, but the full effect of a charge state distribution (CSD) as exists in plasmas is only modeled theoretically. PANDORA aims to be the first to verify these models by measuring the β-decay rates of select isotopes embedded in electron cyclotron resonance (ECR) plasmas. For this purpose, it is necessary to consider the spatial inhomogeneity and anisotropy of plasma ion properties as well as the non-local thermodynamic equilibrium (NLTE) nature of the system. We present here a 3D ion dynamics model combining a quasi-stationary particle-in-cell (PIC) code to track the motion of macroparticles in a pre-simulated electron cloud while simultaneously using a Monte Carlo (MC) routine to check for relevant reactions describing the ion population kinetics. The simulation scheme is robust, comprehensive, makes few assumptions about the state of the plasma, and can be extended to include more detailed physics. We describe the first results on the 3D variation of CSD of ions both confined and lost from the ECR trap, as obtained from the application of the method to light nuclei. The work culminates in some perspectives and outlooks on code optimization, with a potential to be a powerful tool not only in the application of ECR plasmas but for fundamental studies of the device itself.

Photodetachment Spectroscopy of Highly Excited \(\text{C}_{2}^{ - }\) and Their Temporal Evolution in the Ion Storage Ring RICE

We performed laser-induced electron detachment spectroscopy of \(\text{C}_{2}^{ - }\) ions, produced by a cesium-sputter ion source and stored in the electrostatic ion storage ring RICE, to study highly excited states and their temporal evolution. From the observed peaks originating in the doublet–doublet transition X \(^{2}\Sigma_{g}^{ + }\)–B \(^{2}\Sigma_{u}^{ + }\), we determined the spectroscopic constants for B \(^{2}\Sigma_{u}^{ + }\) v′ = 5–8 by applying the Δv = −1 transition. Moreover, we found that the overall spectra showed a striking difference from previously reported spectroscopic measurements. The majority of the observed peaks could not be ascribed to doublet–doublet transitions. We studied the lifetimes of these unassigned peaks by varying the ion storage time prior to pulsed laser irradiation and discovered shorter- and longer-lived components of 1.5–3 ms and more than 10 ms, respectively. The former lifetime is in good agreement with the autodetachment component observed without laser irradiation, suggesting a possible detachment channel from a metastable quartet state.

Ion and neutral beams merge to measure reactions under cold interstellar medium conditions

Experiment becomes the first to employ the merged beams technique to study ion-neutral collisions at a heavy ion storage ring.

On the temperature of large biomolecules in ion-storage rings

On the temperature of large biomolecules in ion-storage rings

Statistical vibrational autodetachment and radiative cooling rates of para-benzoquinone.

We report measurements of the statistical vibrational autodetachment (VAD, also called thermionic emission) and radiative cooling rates of isolated para-benzoquinone (pBQ, C6H4O2) radical anions using the cryogenic electrostatic ion storage ring facility DESIREE. The results are interpreted using master equation simulations with rate coefficients calculated using statistical detailed balance theory. The VAD rate is determined by measuring the time-dependent yield of neutral pBQ due to spontaneous electron emission from a highly-excited ensemble of anions formed in an electron-attachment ion source. Competition with radiative cooling quenches the VAD rate after a critical time of τc = 11.00(5) ms. Master equation simulations which reproduce the VAD yield provide an estimate of the initial effective vibrational temperature of the ions of 1100(20) K, and provide insight into the anion formation scenario. A second measurement of the radiative cooling rate of pBQ- stored for up to 0.5 s was achieved using time-dependent photodetachment action spectroscopy across the 2Au ← 2B2g and 2B2u ← 2B2g transitions. The rate at which hot-band contributions fade from the action spectrum is quantified by non-negative matrix factorisation. This is found to be commensurate with the average vibrational energy extracted from the simulations, with 1/e lifetimes of 0.16(3) s and 0.1602(7) s, respectively. Implications for astrochemistry are discussed.

Relic neutrinos at accelerator experiments

We present a new technique for observing low energy neutrinos with the aim of detecting the cosmic neutrino background using ion storage rings. Utilising high energy targets exploits the quadratic increase in the neutrino capture cross section with beam energy, and with sufficient beam energy, enables neutrino capture through inverse-beta decay processes from a stable initial state. We also show that there exist ion systems admitting resonant neutrino capture, capable of achieving larger capture cross sections at lower beam energies than their non-resonant counterparts. We calculate the neutrino capture rate and the optimal experimental runtime for a range of different resonant processes and target ions and we demonstrate that the resonant capture experiment can be performed with beam energies as low as $\mathcal{O}(10\,\mathrm{TeV})$ per target nucleon. Unfortunately, none of the ion systems discussed here can provide sufficient statistics to discover the cosmic neutrino background with current technology. We address the challenges associated with realising this experiment in the future, taking into account the uncertainty in the beam and neutrino momentum distributions, synchrotron radiation, as well as the beam stability.

Radiative recombination of twisted electrons with hydrogenlike heavy ions: Linear polarization of emitted photons

We present a theoretical investigation of the radiative recombination of twisted Bessel electrons with initially hydrogen-like (finally helium-like) heavy ions. In our study, we focus especially on the linear polarization of x-ray photons emitted in the electron capture into the ground $1{s}_{1/2}^{2}$ ionic state. Particular emphasis is placed on the question of how this polarization is affected if incident hydrogen-like ions are themselves spin-polarized. To explore such a ``polarization transfer'' we apply the density matrix theory and derive the Stokes parameters of recombination x rays for the realistic case of collisions between macroscopic electron and ion beams. Based on the developed general approach two scenarios are discussed that are of interest for the planned experiments at ion storage rings. First, we demonstrate how the use of twisted electrons can empower the known method for the diagnostics of spin-polarized ion beams, based on the rotation of the linear polarization of recombination light. In the second scenario we show how the internal structure of ions beams with inhomogeneous intensity and spin patterns can be probed by the capture of Bessel electrons, carrying different values of angular momentum.

Experimental and theoretical study of photo-dissociation spectroscopy of pyrene dimer radical cations stored in a compact electrostatic ion storage ring.

In this paper, we present an experimental and theoretical study of the photo-dissociation of free-flying dimer radical cations of pyrene (C16H10)2+. Experimentally, the dimers were produced in the plasma of an electron cyclotron resonance ion source and stored in an electrostatic ion storage ring, the Mini-Ring for times up to 10 ms and the photo-dissociation spectrum was recorded in the 400 to 2000 nm range. Two broad absorption bands were observed at 550 (2.25 eV) and 1560 nm (0.79 eV), respectively. Theoretical simulations of the absorption spectrum as a function of the temperature were performed using the Density Functional based Tight Binding approach within the Extended Configuration Interaction scheme (DFTB-EXCI) to determine the electronic structure. The simulation involved all excited electronic states correlated asymptotically with the five lowest excited states D1-D5 of the monomer cation and a Monte Carlo exploration of the electronic ground state potential energy surface. The simulations exhibit three major bands at 1.0, 2.1 and 2.8 eV respectively. They allow assigning the experimental band at 1560 nm to absorption by the charge resonance (CR) excited state correlated with the ground state of the monomer D0. The band at 550 nm is tentatively attributed to dimer states correlated with excited states D2-D4, in the monomer cation. Simulations also show that the CR band broadens and shifts towards longer wavelength with increasing temperature. It results from the dependence on the geometry of the energy gap between the ground state and the lowest excited state. The comparison of the experimental spectrum with theoretical spectra at various temperatures allows us to estimate the temperature of the stored (C16H10)2+ in the 300-400 K range, which is also in line with the expected temperatures of the ions deduced from the analysis of the natural decay curve.

Photodissociation spectroscopy of N2O+ in the ion storage ring RICE.

The A2Σ+-X2Π electronic transition of the nitrous oxide cation, N2O+, was measured via photodissociation spectroscopy in a cryogenic electrostatic ion storage ring. Rotationally resolved spectra of the N-O stretching vibrational sequence were obtained by detecting neutral N fragments produced via N2O+ → NO+ + N predissociation channels. A new set of molecular constants was determined for the high-lying vibrational levels of the A2Σ+ state.