Multiple-reflection Time-of-flight Mass Spectrometer Research Articles

A compact ion source combining electron-impact and thermal ionization for multiple-reflection time-of-flight mass spectrometry.

A compact ion source combining electron impact and thermal ionization has been developed and commissioned in two Multiple-Reflection Time-Of-Flight Mass Spectrometer (MR-TOF-MS) setups at the Fragment Separator Ion Catcher at the GSI Helmholtz Centre for Heavy Ion Research, Darmstadt, Germany, and at TRIUMF's Ion Trap for Atomic and Nuclear science at TRIUMF Canada's particle accelerator center, Vancouver, Canada. The ion source is notable for its compact dimensions of 50mm in height and 68mm in diameter. The ion source is currently in daily operation at both facilities. Design, simulations, and results of combining ions from thermal and electron-impact ionization of different gases (perfluoropropane and sulfur hexafluoride) are presented in this work. The systematic effects of heating power on the thermal source were studied in detail. The source has demonstrated stable and long-term production of reference ions over a wide mass range for the MR-TOF-MS. This versatile ion source has also been used to optimize and investigate the transport of ions with different chemical reactivity and ionization potentials.

Optimizing Ion Optical Design for Laser Ablation Source in Mass Spectrometry

The study focuses on optimizing a Laser Ablation Source (LAS) for use in mass spectrometry, particularly aiming to enhance transmission of ions and and determination of isotopic compositions in diverse matrices at TRIUMF’s Ion Trap for Atomic and Nuclear Science (TITAN). Critical variables affecting mass spectrometer resolution, such as ion kinetic energy distribution and ion transport are optimized through LAS. The paper explores the importance of consistent initial conditions, ion transport efficiency, and ion capture for accurate and reproducible measurements. Using SIMION software, we optimized ion optical design to tackle challenges like collimating ions travelling off-axis and mass filtering. A significant part of the study is dedicated to ion optic design to enable low abundance measurement of ions of interest (e.g., 10 ions of interest out of 1014 total ions). Techniques like high voltage switching and beam shaping were explored, and the final design aims for high transport efficiency and a 4 mm effective target scan area with maximum transport efficiency. The integration of LAS with a Multiple-Reflection Time-Of-Flight Mass Spectrometer (MR-TOF-MS) is expected to yield an analytical tool with high spatial resolution and transport efficiency for isotope abundance measurement.

A laser ablation carbon cluster ion source for the FRS Ion Catcher

A Laser Ablation Carbon Cluster Ion source (LACCI) has been developed and commissioned at the FRS Ion Catcher at GSI. It is the first laser ablation ion source for long-term measurements with a multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). This is enabled by two key developments: (i) a two-dimensional movable target platform that ensures the long-term stable production of ions and (ii) a mass filter for the isolation of the ions of interest. LACCI is capable of providing closely-spaced reference ions in the mass range up to ∼300 u for accurate mass measurements of exotic nuclei (relative mass uncertainty ∼10−8) and systematic studies of the mass uncertainties with the multiple-reflection time-of-flight mass spectrometer. Investigations of the laser energy and repetition rate and long-term measurements have been carried out with carbon targets (Sigradur®, Fullerene) and metallic targets (silver, gold, copper, tungsten, and erbium). In a test experiment, LACCI has delivered a stable ion current for more than 20 h at a laser repetition rate of 100 Hz, corresponding to an operation for one week at 10 Hz. It thus fully satisfies the requirements for long-term accurate mass measurements of exotic nuclei with an MR-TOF-MS. This enables the access of exotic ions, detected with rates as low as 0.1 per hour at the FRS Ion Catcher.

Independent isotopic fission yields of 252Cf spontaneous fission via mass measurements at the FRS Ion Catcher

We present first preliminary results of a novel method for measuring independent isotopic fission yields (IIFYs) of spontaneous fission (SF) via direct mass measurements, at the FRS Ion Catcher (FRS-IC) at GSI. Fission products were generated from a 252Cf source installed in a cryogenic stopping cell, and were identified and counted with the multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS) of the FRS-IC, utilizing well-established measurement and data analysis methods. The MR-TOF-MS resolves isobars unambiguously, even with limited statistics, and its non-scanning nature ensures minimal relative systematic uncertainties amongst fission products. The analysis for extracting IIFYs includes isotope-dependent efficiency corrections for all components of the FRS-IC. In particular, we applied a self-consistent technique that takes into account the element-dependent survival efficiencies in the CSC, due to chemical reactions with the buffer gas. Our IIFY results, which cover several tens of fission products in the less-accessible high-mass peak (Z = 56 to 63) down to fission yields at the level of 10−5, are generally similar to those of the nuclear database ENDF/B-VII.0. Nevertheless, they reveal some structures that are not observed in the database smooth trends. These are the first results of a planned campaign to investigate IIFY distributions of spontaneous fission at the FRS-IC. Upcoming experiments will extend our results to wider Z and N ranges, lower fission yields, and other spontaneously-fissioning actinides.

Investigating nuclear structure near N=32 and N=34: Precision mass measurements of neutron-rich Ca, Ti, and V isotopes

Nuclear mass measurements of isotopes are key to improving our understanding of nuclear structure across the chart of nuclides, in particular for the determination of the appearance or disappearance of nuclear shell closures. We present high-precision mass measurements of neutron-rich Ca, Ti and V isotopes performed at the TITAN and LEBIT facilities. These measurements were made using the TITAN multiple-reflection time-of-flight mass spectrometer (MR-ToF-MS) and the LEBIT 9.4T Penning trap mass spectrometer. In total, 13 masses were measured, eight of which represent increases in precision over previous measurements. These measurements refine trends in the mass surface around $N = 32$ and $N = 34$, and support the disappearance of the $N = 32$ shell closure with increasing proton number. Additionally, our data does not support the presence of a shell closure at $N = 34$.

Summit of the N=40 island of inversion: Precision mass measurements and ab initio calculations of neutron-rich chromium isotopes

Mass measurements continue to provide invaluable information for elucidating nuclear structure and scenarios of astrophysical interest. The transition region between the Z=20 and 28 proton shell closures is particularly interesting due to the onset and evolution of nuclear deformation as nuclei become more neutron-rich. This provides a critical testing ground for emerging ab-initio nuclear structure models. Here, we present high-precision mass measurements of neutron-rich chromium isotopes using the sensitive electrostatic Multiple-Reflection Time-Of-Flight Mass Spectrometer (MR-TOF-MS) at TRIUMF's Ion Trap for Atomic and Nuclear Science (TITAN) facility. Our high-precision mass measurements of 59,61−63Cr confirm previous results, and the improved precision in measurements of 64−65Cr refine the mass surface beyond N=40. With the ab initio in-medium similarity renormalization group, we examine the trends in collectivity in chromium isotopes and give a complete picture of the N=40 island of inversion from calcium to nickel.

First coupling of the FRS particle identification and the FRS-Ion Catcher data acquisition systems: The case of 109In

For the first time, the FRagment Separator (FRS) and the Multiple-Reflection Time-Of-Flight Mass-Spectrometer (MR-TOF-MS) particle identification (PID) systems at GSI have been coupled. This new approach adds to the standard FRS PID an additional unambiguous identification of the fragments and the possibility to identify and count long-lived isomeric states (>ms). For this purpose, single-event timestamp information given by a common clock was used to correlate both systems. Two methods were implemented to improve the signal-to-background ratio by more than a factor 2 in the high resolution mass spectrum obtained with the MR-TOF-MS for the 109In isotope. Moreover, the coupling of the systems allows an improvement in the on-line monitoring of the FRS-Ion Catcher (IC) efficiency and extraction time. In addition, range calculations were implemented in the on-line monitoring; a powerful tool for real-time optimization of stopped beam experiments.

Mapping the N=40 island of inversion: Precision mass measurements of neutron-rich Fe isotopes

Nuclear properties across the chart of nuclides are key to improving and validating our understanding of the strong interaction in nuclear physics. We present high-precision mass measurements of neutron-rich Fe isotopes performed at the TITAN facility. The multiple-reflection time-of-flight mass spectrometer (MR-ToF-MS), achieving a resolving power greater than 600000 for the first time, enabled the measurement of Fe63–70, including first-time high-precision direct measurements (δm/m≈10−7) of Fe68–70, as well as the discovery of a long-lived isomeric state in Fe69. These measurements are accompanied by both mean-field and ab initio calculations using the most recent realizations which enable theoretical assignment of the spin-parities of the Fe69 ground and isomeric states. Together with mean-field calculations of quadrupole deformation parameters for the Fe isotope chain, these results benchmark a maximum of deformation in the N=40 island of inversion in Fe and shed light on trends in level densities indicated in the newly refined mass surface.Received 19 July 2021Revised 24 December 2021Accepted 16 March 2022DOI:https://doi.org/10.1103/PhysRevC.105.L041301©2022 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasBinding energy & massesNuclear structure & decaysRare & new isotopesProperties59 ≤ A ≤ 89TechniquesAb initio calculationsMean field theoryTime-of-flight mass spectrometryNuclear Physics

Commissioning and performance of TITAN’s Multiple-Reflection Time-of-Flight Mass-Spectrometer and isobar separator

TRIUMF’s Ion Trap for Atomic and Nuclear science (TITAN) has specialized in fast Penning Trap mass spectrometry of very short-lived radioactive isotopes. The facility has been upgraded with a Multiple-Reflection Time-of-Flight Mass Spectrometer (MR-TOF-MS) to continue its quest towards more exotic nuclides, which are critical for our understanding of nuclear structure effects far from the valley of beta stability and for the nucleosynthesis of heavy elements in explosive astrophysical environments. In this publication, we discuss the implementation, operation and performance of TITAN’s MR-TOF-MS as a stand-alone high-precision mass spectrometer and as an isobar separator. By using the novel mass-selective re-trapping technique for the isobar separation, the MR-TOF-MS can consecutively perform separation and mass measurement of the same ion population, acting as its own isobar separator. The device boosts the dynamic range and reach of the TITAN facility by several orders of magnitude. The MR-TOF-MS reaches a high mass resolving power (m/Δm∼400000), high precision and mass accuracy (δm/m<10−7), is fast (common cycle time 20ms), shows high sensitivity and very large dynamic range (ion of interest to contaminant ratios of up to 1 to 106).

Mass Measurements of Neutron-Deficient Yb Isotopes and Nuclear Structure at the Extreme Proton-Rich Side of the N=82 Shell.

High-accuracy mass measurements of neutron-deficient Yb isotopes have been performed at TRIUMF using TITAN's multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). For the first time, an MR-TOF-MS was used on line simultaneously as an isobar separator and as a mass spectrometer, extending the measurements to two isotopes further away from stability than otherwise possible. The ground state masses of ^{150,153}Yb and the excitation energy of ^{151}Yb^{m} were measured for the first time. As a result, the persistence of the N=82 shell with almost unmodified shell gap energies is established up to the proton drip line. Furthermore, the puzzling systematics of the h_{11/2}-excited isomeric states of the N=81 isotones are unraveled using state-of-the-art mean field calculations.

Mass measurements of As, Se, and Br nuclei, and their implication on the proton-neutron interaction strength toward the N=Z line

Mass measurements of the $^{69}$As, $^{70,71}$Se and $^{71}$Br isotopes, produced via fragmentation of a $^{124}$Xe primary beam at the FRS at GSI, have been performed with the multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS) of the FRS Ion Catcher with an unprecedented mass resolving power of almost 1,000,000. For the $^{69}$As isotope, this is the first direct mass measurement. A mass uncertainty of 22 keV was achieved with only 10 events. For the $^{70}$Se isotope, a mass uncertainty of 2.6 keV was obtained, corresponding to a relative accuracy of $\delta$m/m = 4.0$\times 10^{-8}$, with less than 500 events. The masses of the $^{71}$Se and $^{71}$Br isotopes were measured with an uncertainty of 23 and 16 keV, respectively. Our results for the $^{70,71}$Se and $^{71}$Br isotopes agree with the 2016 Atomic Mass Evaluation, and our result for the $^{69}$As isotope resolves the discrepancy between previous indirect measurements. We measured also the mass of $^{14}$N$^{15}$N$^{40}$Ar (A=69) with a relative accuracy of $\delta$m/m = 1.7$\times 10^{-8}$, the highest yet achieved with a MR-TOF-MS. Our results show that the measured restrengthening of the proton-neutron interaction ($\delta$V$_{pn}$) for odd-odd nuclei at the N=Z line above Z=29 (recently extended to Z=37) is hardly evident at N-Z=2, and not evident at N-Z=4. Nevertheless, detailed structure of $\delta$V$_{pn}$ along the N-Z=2 and N-Z=4 lines, confirmed by our mass measurements, may provide a hint regarding the ongoing $\approx$500 keV discrepancy in the mass value of the $^{70}$Br isotope, which prevents including it in the world average of ${Ft}$-value for superallowed 0$^+\rightarrow$ 0$^+$ $\beta$ decays. The reported work sets the stage for mass measurements with the FRS Ion Catcher of nuclei at and beyond the N=Z line in the same region of the nuclear chart, including the $^{70}$Br isotope.

Mass measurements of neutron-rich indium isotopes for r -process studies

A new series of neutron-rich indium mass measurements is reported from the TITAN multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). These mass measurements cover In125−134 (N=76–85) and include ground states as well as isomeric states. The masses of nuclei in this region are known to be of great importance for accurately modeling r-process nucleosynthesis, and the significance of the reported neutron-rich indium masses is discussed in this context. Results are compared with earlier experimental data where available as well as theoretical mass models. The measurements reported here include the first mass measurements of In133,134, as well as the first direct mass measurement of In132. The masses of In125−131 ground states and several isomers were previously measured to higher precision by Penning trap mass spectrometry, which also resolved some low-lying isomers that could not be resolved in this work. The earlier Penning trap measurements serve as excellent cross-checks for the MR-TOF-MS measurements, and in some cases the MR-TOF-MS measurements improve the literature uncertainties of higher-lying isomer masses and excitation energies. A new isomeric state for In128, recently reported for the first time by the JYFLTRAP group, is also confirmed by the TITAN MR-TOF-MS, with a measured excitation energy of 1813(17) keV.Received 24 November 2020Accepted 8 February 2021DOI:https://doi.org/10.1103/PhysRevC.103.025811©2021 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasBinding energy & massesNuclear astrophysicsr processProperties90 ≤ A ≤ 149TechniquesSpectrometers & spectroscopic techniquesNuclear Physics

High-precision mass measurement of neutron-rich 96Kr

While the nuclear deformation in the region around Z = 40 and N = 60 has been studied in great detail, the possible onset of nuclear deformation in the isotopic chain of krypton (Z = 36) is still a subject of controversy. Here, we present a high-precision mass measurement of the neutron-rich nuclide 96Kr, as measured by the Multiple-Reflection Time-of-Flight Mass Spectrometer (MR-TOF-MS) at TRIUMF’s Ion Trap for Atomic and Nuclear Science (TITAN). A statistical method, based on a hyper-exponentially modified Gaussian, has been employed to model the data. As such, the uncertainty introduced by overlapping peaks from beam contaminants was reduced and the mass excess of 96Kr determined to be -53097(57)keV. The capability of the method has been confirmed with measurements of the stable isotopic pair 40Ar/40Ca, in which a relative accuracy Δm/m of 3.5 ⋅ 10− 8 and a mass resolving power of more than 400000 were achieved.

Mass and half-life measurements of neutron-deficient iodine isotopes

Neutron-deficient iodine isotopes, ^{116}I and ^{114}I, were produced at relativistic energies by in-flight fragmentation at the Fragment Separator (FRS) at GSI. The FRS Ion Catcher was used to thermalize the ions and to perform highly accurate mass measurements with a Multiple-Reflection Time-of-Flight Mass-Spectrometer (MR-TOF-MS). The masses of both isotopes were measured directly for the first time. The half-life of the ^{114}I was measured by storing the ions in an RF quadrupole for different storage times and counting the remaining nuclei with the MR-TOF-MS. The measured half-life was used to assign the ground state to the measured ^{114}I ions. Predictions on the possible alpha -decay branch for ^{114}I are presented based on the reduced uncertainties obtained for the Q_{alpha }-value. Systematic studies of the mass surface were performed with the newly obtained masses, showing better agreement with the expected trend in this mass region.

Determining spontaneous fission properties by direct mass measurements with the FRS Ion Catcher

We present a direct method to measure fission product yield distributions (FPY) and isomeric yield ratios (IYR) for spontaneous fission (SF) fragments. These physical properties are of utmost importance to the understanding of basic nuclear physics, the astrophysical rapid neutron capture process ('r process') of nucleosynthesis, neutron star composition, and nuclear reactor safety. With this method, fission fragments are produced by spontaneous fission from a source that is mounted in a cryogenic stopping cell (CSC), thermalized and stopped within it, and then extracted and transported to a multiple-reflection time-of-flight mass-spectrometer (MR-TOF-MS). We will implement the method at the FRS Ion Catcher (FRS-IC) at GSI (Germany), whose MR-TOF-MS relative mass accuracy (~ 10-7) and resolving power (~ 600,000 FWHM) are sufficient to separate all isobars and numerous isomers in the fission fragment realm. The system's essential element independence and its fast simultaneous mass measurement provide a new direct way to measure isotopic FPY distributions, which is complementary to existing methods. It will enable nuclide FPY measurements in the high fission peak, which is hardly accessible by current techniques. The extraction time of the CSC, tens of milliseconds, enables a direct measurement of independent fission yields, and a first study of the temporal dependence of FPY distributions in this duration range. The ability to resolve isomers will further enable direct extraction of numerous IYRs while performing the FPY measurements. The method has been recently demonstrated at the FRS-ICr for SF with a 37 kBq 252Cf fission source, where about 70 different fission fragments have been identified and counted. In the near future, it will be used for systematic studies of SF with a higher-activity 252Cf source and a 248Cm source. The method can be implemented also for neutron induced fission at appropriate facilities.

A novel method for the measurement of half-lives and decay branching ratios of exotic nuclei

.A novel method for simultaneous measurement of masses, Q-values, isomer excitation energies, half-lives and decay branching ratios of exotic nuclei has been demonstrated. The method includes first use of a stopping cell as an ion trap, combining storage of mother and daughter nuclides for variable durations in a cryogenic stopping cell (CSC), and afterwards the identification and counting of them by a multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). We utilized our method to record the decay and growth of the 216Po and 212Pb isotopes (alpha decay) and of the 119m2Sb isomer (t_{1/2} = 850pm 90 ms) and 119gSb isotope (isomer transition), obtaining half-lives consistent with literature values. The amount of non-nuclear-decay losses in the CSC up to sim 10 s is negligible, which exhibits its extraordinary cleanliness. For 119Sb isotopes, we present the first direct measurements of the mass of its ground state, and the excitation energy and decay branching ratios of its second isomeric state (119m2Sb). This resolves discrepancies in previous excitation energy data, and is the first direct evidence that the 119m2Sb isomer decays dominantly via gamma emission. These results pave the way for the measurement of branching ratios of exotic nuclei.

The science case of the FRS Ion Catcher for FAIR Phase-0

The FRS Ion Catcher at GSI enables precision experiments with thermalized projectile and fission fragments. At the same time it serves as a test facility for the Low-Energy Branch of the Super-FRS at FAIR. The FRS Ion Catcher has been commissioned and its performance has been characterized in five experiments with 238U and 124Xe projectile and fission fragments produced at energies in the range from 300 to 1000 MeV/u. High and almost element-independent efficiencies for the thermalization of short-lived nuclides produced at relativistic energies have been obtained. High-accuracy mass measurements of more than 30 projectile and fission fragments have been performed with a multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS) at mass resolving powers of up to 410,000, with production cross sections down to the microbarn-level, and at rates down to a few ions per hour. The versatility of the MR-TOF-MS for isomer research has been demonstrated by the measurement of various isomers, determination of excitation energies and the production of a pure isomeric beam. Recently, several instrumental upgrades have been implemented at the FRS Ion Catcher. New experiments will be carried out during FAIR Phase-0 at GSI, including direct mass measurements of neutron-deficient nuclides below 100Sn and neutron-rich nuclides below 208Pb, measurement of β-delayed neutron emission probabilities and reaction studies with multi-nucleon transfer.

Recent upgrades of the multiple-reflection time-of-flight mass spectrometer at TITAN, TRIUMF

A multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS) has been installed and integrated into the TITAN experiment at TRIUMF. The MR-TOF-MS extends the capabilities and improves the performance of the TITAN experiment, for instance it provides fast isobar separation, short measurement cycles, yield measurements and broad-band beam diagnosis, and enhanced rate capabilities and dynamic range. Thereby, even more exotic nuclides become accessible at TITAN for experiments. Such improved capabilities of TITAN have been used in first experiments to investigate the sub-shell closure of neutron-rich nuclides at N = 32 and the r-process nucleo-synthesis for masses at A ∼ 85. The vacuum system, electronics and data-acquisition hardware and software have been recently upgraded. For the first time an isomeric state has been measured with TITAN′s MR-TOF-MS, 84mRb (excitation energy: 464 keV). The accurate measurement of excitation energies of low-lying isomeric states is possible due to the high mass resolving power of TITAN′s MR-TOF-MS and a specialized data-analysis procedure.

High-resolution, accurate multiple-reflection time-of-flight mass spectrometry for short-lived, exotic nuclei of a few events in their ground and low-lying isomeric states

Mass measurements of fission and projectile fragments, produced via $^{238}$U and $^{124}$Xe primary beams, have been performed with the multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS) of the FRS Ion Catcher with a mass resolving powers (FWHM) up to 410,000 and an uncertainty of $6\cdot 10^{-8}$. The nuclides were produced and separated in-flight with the fragment separator FRS at 300 to 1000 MeV/u and thermalized in a cryogenic stopping cell. The data-analysis procedure was developed to determine with highest accuracy the mass values and the corresponding uncertainties for the most challenging conditions: down to a few events in a spectrum and overlapping distributions, characterized only by a broader common peak shape. With this procedure, the resolution of low-lying isomers is increased by a factor of up to three compared to standard data analysis. The ground-state masses of 31 short-lived nuclides of 15 different elements with half-lives down to 17.9~ms and count rates as low as 11 events per nuclide were determined. This is the first direct mass measurement for seven nuclides. The excitation energies and the isomer-to-ground state ratios of six isomeric states with excitation energies down to about 280~keV were measured. For nuclides with known mass values, the average relative deviation from the literature values is $(2.9 \pm 6.2) \cdot 10^{-8}$. The measured two-neutron separation energies and their slopes near and at the N=126 and Z=82 shell closures indicate a strong element-dependent binding energy of the first neutron above the closed proton shell Z=82. The experimental results deviate strongly from the theoretical predictions, especially for N=126 and N=127.

Dawning of the N=32 Shell Closure Seen through Precision Mass Measurements of Neutron-Rich Titanium Isotopes.

A precision mass investigation of the neutron-rich titanium isotopes ^{51-55}Ti was performed at TRIUMF's Ion Trap for Atomic and Nuclear science (TITAN). The range of the measurements covers the N=32 shell closure, and the overall uncertainties of the ^{52-55}Ti mass values were significantly reduced. Our results conclusively establish the existence of the weak shell effect at N=32, narrowing down the abrupt onset of this shell closure. Our data were compared with state-of-the-art abinitio shell model calculations which, despite very successfully describing where the N=32 shell gap is strong, overpredict its strength and extent in titanium and heavier isotones. These measurements also represent the first scientific results of TITAN using the newly commissioned multiple-reflection time-of-flight mass spectrometer, substantiated by independent measurements from TITAN's Penning trap mass spectrometer.