While discussing the vibrational radiative cooling of isolated cluster molecules, it is common to apply statistical models based on the density of vibrational states and calculated transition strengths. In the current work, we put this assumption to the test by studying the cooling rates of isolated Al-5 ions across very long timescales ranging up to 2000 s. To this end, we stored Al-5 ions in the Cryogenic Storage Ring (CSR) and monitored their internal excitation by laser-induced delayed electron emission. We find that once the internal energy drops below the first electronically excited state, the cooling rates scale linearly with energy. Our results are consistent with the calculated vibrational relaxation rates through the emission of infrared photons, based on the harmonic cascade model, thus validating quantitatively the assumption of a statistical cooling process for the relaxation of small cluster molecules with infrared-active vibrational modes.

The NECTAR (Nuclear rEaCTions At storage Rings) experiment at the ESR heavy-ion storage ring at GSI/FAIR Darmstadt is dedicated to surrogate reaction studies of neutron-induced reactions on heavy nuclei in inverse kinematics. In this work, we report on the implementation and performance of a newly developed fission-fragment detection system integrated into the NECTAR experimental setup. The upgraded detector configuration enables, for the first time in a surrogate experiment, the simultaneous detection ofgamma-decay residues, multi-neutron-emission residues, and fission fragments. The full setup was used for the first time in an experiment where a stored beam of bare 238U92+ ions at 17.24 MeV/u interacted with a gas-jet deuterium target, populating excited 238U and 239U nuclei via the 238U(d,d') and 238U(d,p) reactions. We describe the geometry of the used fission fragment detectors, design constraints, and simulation-based efficiency determination. The target-like particle identification and beam-like residue spectra demonstrating the performance of the complete setup are also shown.

Neutron-induced reaction cross sections of short-lived nuclei are imperative to understand the origin of heavy elements in stellar nucleosynthesis and for societal applications, but their measurement is extremely complicated due to the radioactivity of the targets involved. One way of overcoming this issue is to combine surrogate reactions with the unique possibilities offered by heavy-ion storage rings. In this work, we describe the first surrogate-reaction experiment in inverse kinematics, which we successfully conducted at the Experimental Storage Ring (ESR) of the GSI/FAIR facility, using the ^{208}Pb(p,p^{'}) reaction as a surrogate for neutron capture on ^{207}Pb. Thanks to the outstanding detection efficiencies possible at the ESR, we were able to measure for the first time the neutron-emission probability as a function of the excitation energy of ^{208}Pb. We have used this probability to select different descriptions of the γ-ray strength function and nuclear level density, and provide reliable results for the neutron-induced radiative capture cross section of ^{207}Pb at energies for which no experimental data exist.

The probabilities for gamma-ray and particle emission as a function of the excitation energy of a decaying nucleus are valuable observables for constraining the ingredients of the models that describe the deexcitation of nuclei near the particle emission threshold. These models are essential in nuclear astrophysics and applications. In this paper, we have for the first time simultaneously measured the gamma-ray and neutron emission probabilities of 208Pb. The measurement was performed in inverse kinematics at the Experimental Storage Ring (ESR) of the GSI/FAIR facility, where a 208Pb beam interacted through the 208Pb(p, p') reaction with a hydrogen gas jet target. Instead of detecting the gamma rays and neutrons emitted by 208Pb, we detected the heavy beamlike residues produced after gamma and neutron emission. These heavy residues were fully separated by a dipole magnet of the ESR and were detected with outstanding efficiencies. The comparison of the measured probabilities with model calculations has allowed us to test and select different descriptions of the gamma-ray strength function and the nuclear level density available in the literature.

We have experimentally studied dissociative recombination (DR) of electronically and vibrationally relaxed ArH+ in its lowest rotational levels, using an electron-ion merged-beams setup at the Cryogenic Storage Ring. We report measurements for the merged-beams rate coefficient of ArH+ and compare it to published experimental and theoretical results. In addition, by measuring the kinetic energy released to the DR fragments, we have determined the internal state of the DR products after dissociation. At low collision energies, we find that the atomic products are in their respective ground states, which are only accessible via nonadiabatic couplings to neutral Rydberg states. Published theoretical results for ArH+ have not included this DR pathway. From our measurements, we have also derived a kinetic temperature rate coefficient for use in astrochemical models. Published by the American Physical Society 2024

Highly excited C_2^- ions prominently feature electron detachment at a mean decay time near 3 milliseconds with hitherto unexplained origin. Considering various sources of unimolecular decay, we attribute the signal to the electronic C^4Σ^+_u state. Quartet C_2^- levels are found to be stabilized against autodetachment by high rotation. Time constants of their rotationally assisted autodetachment into levels opening energetically at lower rotation are calculated by a theory based on the non-local resonance model. For some final levels of significantly less rotation the results conclusively explain the puzzling observations.

Ion-neutral reactions are driving the formation of small molecules in the gas phase of interstellar clouds, where hydrogen molecules and their ions are by far the most important collision partners for any species in the astrochemical network. Here we present absolute rate coefficient measurements for the reactions HD++C→CH+/CD++D/H and H3++C→CH+/CH2++H2/H obtained using a recently commissioned ion-neutral collision setup at the Cryogenic Storage Ring. Our measurements with vibrationally cold ions result in significantly higher rate coefficients when compared with previous studies using internally excited ions, bringing them in better agreement with classical capture theories. Moreover, we have performed detailed quasiclassical trajectory (QCT) calculations for the HD++C reaction, using new potential energy surfaces. Our experimental results and the QCT calculations show very good agreement for the absolute cross section of the reactions, as well as for the isotope effect. These results have great potential relevance for the chemistry of the interstellar medium and the onset of organic chemistry in space. Published by the American Physical Society 2024

We show that strong molecular rotation drastically modifies the autodetachment of C-2 ions in the lowest quartet electronic state a4 Sigma & thorn;u . In the strong-rotation regime, levels of this state only decay by a process termed "rotationally assisted" autodetachment, whose theoretical description is worked out based on the nonlocal resonance model. For autodetachment linked with the exchange of six rotational quanta, the results reproduce a prominent, hitherto unexplained electron emission signal with a mean decay time near 3 ms, observed on stored C-2 ions from a hot ion source.

We present a merged-beams study of reactions between HD+ ions, stored in the Cryogenic Storage Ring (CSR), and laser-produced ground-term C atoms. The molecular ions are stored for up to 20 s in the extreme vacuum of the CSR, where they have time to relax radiatively until they reach their vibrational ground state (within 0.5 s of storage) and rotational states with J≤3 (after 5 s). We combine our experimental studies with quasiclassical trajectory calculations based on two reactive potential energy surfaces. In contrast to previous studies with internally excited H2+ and D2+ ions, our results reveal a pronounced isotope effect, favoring the production of CH+ over CD+ across all collision energies, and a significant increase in the absolute rate coefficient of the reaction. Our experimental results agree well with our theoretical calculations for vibrationally relaxed HD+ ions in their lowest rotational states. Published by the American Physical Society 2024

We have measured triple differential momentum distributions for electron detachment in collisions of 30- and 300-keV anions (C− and Si−) with atoms and molecules (He, Ar, and N2). The entire angular range of the ejected electrons was covered. The binary encounter ring, well known from positive ion-atom collisions, was observed in most cases. In a quasifree-electron scattering model this structure represents elastic scattering of the active electron from the target. However, especially for the slowest projectiles, this model fails to reproduce the angular distributions. In this regime it is probably necessary to use quasimolecular models to describe the collision. Indications for a projectile cusp are observed, implying that excitation-induced dipole moments in the ion projectile may be important. Published by the American Physical Society 2024

On the millisecond to second time scale, stored beams of diatomic carbon anions C2-from a sputter ion source feature unimolecular decay of yet unexplained origin by electron emission and fragmentation. To account for the magnitude and time dependence of the experimental rates, levels with high rotational and vibrational excitation are modeled for the lowest electronic states of C2-, also including the lowest quartet potential. Energies, spontaneous radiative decay rates (including spin-forbidden quartet-level decay), and tunneling dissociation rates are determined for a large number of highly excited C2-levels and their population in sputter-type ion sources is considered. For the quartet levels, the stability against autodetachment is addressed and recently calculated rates of rotationally assisted autodetachment are applied. Nonadiabatic vibrational autodetachment rates of high vibrational levels in the doublet C2- ground potential are also calculated. The results are combined to model the experimental unimolecular decay signals. Comparison of the modeled to the experimental rates measured at the cryogenic storage ring facility CSR gives strong evidence that C2- ions in quasistable levels of the quartet electronic states are the so far unidentified source of unimolecular decay.

Determining the cross sections of neutron-induced reactions on short-lived nuclei is imperative to rate calculations in stellar nucleosynthesis and applications of nuclear physics. It is also an immense experimental challenge due to the radioactivity of the targets involved. Our goal is to circumvent this obstacle by using surrogate reactions in inverse kinematics at the heavy-ion storage rings of GSI/FAIR. We present here preliminary results from the first proof of principle experiment, where a beam of 208 Pb impinged on a H 2 gas jet target in the Experimental Storage Ring (ESR).

Observations of OH + are used to infer the interstellar cosmic ray ionization rate in diffuse atomic clouds, thereby constraining the propagation of cosmic rays through and the shielding by interstellar clouds, as well as the low energy cosmic ray spectrum. In regions where the H 2 -to-H number density ratio is low, dissociative recombination (DR) is the dominant destruction process for OH + and the DR rate coefficient is important for predicting the OH + abundance and inferring the cosmic ray ionization rate. We have experimentally studied DR of electronically and vibrationally relaxed OH + in its lowest rotational levels, using an electron–ion merged-beams setup at the Cryogenic Storage Ring. From these measurements, we have derived a kinetic temperature rate coefficient applicable to diffuse cloud chemical models, i.e., for OH + in its electronic, vibrational, and rotational ground level. At typical diffuse cloud temperatures, our kinetic temperature rate coefficient is a factor of ∼5 times larger than the previous experimentally derived value and a factor of ∼33 times larger than the value calculated by theory. Our combined experimental and modeling results point to a significant increase for the cosmic ray ionization rate inferred from observations of OH + and H 2 O + , corresponding to a geometric mean of (6.6 ± 1.0) × 10 −16 s −1 , which is more than a factor of 2 larger than the previously inferred values of the cosmic ray ionization rate in diffuse atomic clouds. Combined with observations of diffuse and dense molecular clouds, these findings indicate a greater degree of cosmic ray shielding in interstellar clouds than has been previously inferred.

While the dissociative recombination (DR) of ground-state molecular ions with low-energy free electrons is generally known to be exothermic, it has been predicted to be endothermic for a class of transition-metal oxide ions. To understand this unusual case, the electron recombination of titanium oxide ions (TiO+) with electrons has been experimentally investigated using the Cryogenic Storage Ring. In its low radiation field, the TiO+ ions relax internally to low rotational excitation (≲100 K). Under controlled collision energies down to ∼2 meV within the merged electron and ion beam configuration, fragment imaging has been applied to determine the kinetic energy released to Ti and O neutral reaction products. Detailed analysis of the fragment imaging data considering the reactant and product excitation channels reveals an endothermicity for the TiO+ dissociative electron recombination of (+4 ± 10) meV. This result improves the accuracy of the energy balance by a factor of 7 compared to that found indirectly from hitherto known molecular properties. Conversely, the present endothermicity yields improved dissociation energy values for D0(TiO) = (6.824 ± 0.010) eV and D0(TiO+) = (6.832 ± 0.010) eV. All thermochemistry values were compared to new coupled-cluster calculations and found to be in good agreement. Moreover, absolute rate coefficients for the electron recombination of rotationally relaxed ions have been measured, yielding an upper limit of 1 × 10-7 cm3 s-1 for typical conditions of cold astrophysical media. Strong variation of the DR rate with the TiO+ internal excitation is predicted. Furthermore, potential energy curves for TiO+ and TiO have been calculated using a multi-reference configuration interaction method to constrain quantum-dynamical paths driving the observed TiO+ electron recombination.

Neutron-induced reaction cross sections of unstable nuclei are essential for understanding the synthesis of heavy elements in stars. However, their measurement is very difficult due to the radioactivity of the targets involved. We propose to circumvent this problem by using for the first time the surrogate reaction method in inverse kinematics at heavy-ion storage rings. In this contribution, we describe the developments we have done to perform surrogate-reaction studies at the storage rings of GSI/FAIR. In particular, we present the first results of the proof of principle experiment, which we conducted recently at the Experimental Storage Ring (ESR).

We describe a merged beams experiment to study ion-neutral collisions at the Cryogenic Storage Ring of the Max Planck Institute for Nuclear Physics in Heidelberg, Germany. We produce fast beams of neutral atoms in their ground term at kinetic energies between 10 and 300 keV by laser photodetachment of negative ions. The neutral atoms are injected along one of the straight sections of the storage ring, where they can react with stored molecular ions. Several dedicated detectors have been installed to detect charged reaction products of various product-to-reactant mass ranges. The relative collision energy can be tuned by changing the kinetic energy of the neutral beam in an independent drift tube. We give a detailed description of the setup and its capabilities, and present proof-of-principle measurements on the reaction of neutral C atoms with D2 + ions.

We present state-selected measurements of rotational cooling and excitation rates of CH^{+} molecular ions by inelastic electron collisions. The experiments are carried out at a cryogenic storage ring, making use of a monoenergetic electron beam at matched velocity in combination with state-sensitive laser dissociation of the CH^{+} ions for simultaneous monitoring of the rotational level populations. Employing storage times of up to 600 s, we create conditions where electron-induced cooling to the J=0 ground state dominates over radiative relaxation, allowing for the experimental determination of inelastic electron collision rates to benchmark state-of-the-art theoretical calculations. On a broader scale, our experiments pave the way to probe inelastic electron collisions for a variety of molecular ions relevant in various plasma environments.

Observations of CH+ are used to trace the physical properties of diffuse clouds, but this requires an accurate understanding of the underlying CH+ chemistry. Until this work, the most uncertain reaction in that chemistry was dissociative recombination (DR) of CH+. Using an electron–ion merged-beams experiment at the Cryogenic Storage Ring, we have determined the DR rate coefficient of the CH+ electronic, vibrational, and rotational ground state applicable for different diffuse cloud conditions. Our results reduce the previously unrecognized order-of-magnitude uncertainty in the CH+ DR rate coefficient to ∼20% and are applicable at all temperatures relevant to diffuse clouds, ranging from quiescent gas to gas locally heated by processes such as shocks and turbulence. Based on a simple chemical network, we find that DR can be an important destruction mechanism at temperatures relevant to quiescent gas. As the temperature increases locally, DR can continue to be important up to temperatures of ∼600 K, if there is also a corresponding increase in the electron fraction of the gas. Our new CH+ DR rate-coefficient data will increase the reliability of future studies of diffuse cloud physical properties via CH+ abundance observations.

For sensitive studies of molecular ions in electrostatic storage rings, the exact knowledge of the isobaric composition of stored beams from a variety of ion sources is essential. Conventional mass-filtering techniques are often inefficient to resolve the beam components. Here, we report the first isochronous mass spectrometry in an electrostatic storage ring, which offers a high mass resolution of Δm/m < 1 × 10-5 even for heavy molecular species with m > 100 u and uncooled ion beams. Mass contaminations can be resolved and identified at relative fractions down to 0.02%.

Surrogate reactions are the most promising alternative method to indirectly infer neutron-induced cross sections. They can constrain key parameters for the theoretical prediction of the neutron-induced cross sections. Several experimental studies have been devoted to this topic and have demonstrated the potential of such approach. Nevertheless, to overcome certain experimental restrains new experiments are being designed to provide new and better-quality data. Here we present the current developments aiming at performing surrogate-reaction studies in inverse kinematics at storage rings.