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http://pos.sis charge effects - Zn, Zn, ISOLTRAP’s 82

resolution separation of - ple experiments have been princi - ShareAlike ShareAlike Licence. ToF MS) is a technique that has - of - -

flight analyzer flight that illustrate its power and usefulness.

- of - NonCommercial explored with respect to space -

Institut für Kernphysik, Kernphysik, für Institut - 1

flight spectra and different distributions of the kinetic - Planck - ToF MS is of - - Ca. In addition, proof lived nuclides with a with a nuclides lived 54 -

Max

:

Ca and Flight Flight Spectrometry (MR

- 53

69117 Heidelberg, 69117Germany Heidelberg, flight mass also succeeded in measuring the previously - of -

line setup MR greifswald.de - - reflection time reflection of - - - limits of the abundances that can be handled. The phenomena observed , Marco Rosenbusch, Frank Wienholtz, Robert N. Wolf N. Robert Wienholtz, Frank Rosenbusch, , Marco of short of 1

OLTRAP at ISOLDE/CERN are given roduced to nuclear physics research. The method is reviewed and several

of R.N. of Wolf tored ion species. Universität

-

in in an off , Str. 6 - multi Arndt -

Reflection Time reflection time - - lschweik@uni Moritz Hausdorff - - in in order to find the include peak coalescence in the time energies theof s allow allow precision , which was demonstrated in the case of multi unknown mass values of performed which demonstrate further applications where fast and high of interest from mixtures with Furthermore high abundances of contamination species is required. Multi recently been int examples from IS Initially built for fast separation of the ions of interest from abundant contaminations in or titute of Physics mail: 6 December 2013 Copyright owned by the author(s) under the terms of the Creative Commons the ofCommons author(s) the terms the Attribution Creative owned by Copyright under Speaker address present Saupfercheckweg 1, D Saupfercheckweg -

-

Isobar separation and precision mass spectrometry spectrometry mass precision and separation Isobar  1 2 X Latin American Symposiumon Nuclear Physics and LASNPA) Applications (X 1 Montevideo, Uruguay

Ernst Ins Felix 17489 Greifswald, Germany E Lutz Lutz Schweikhard

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- ], ], 4 ion ion -

nergy is is nergy

ToF) mass ToF) mass ]. - 2 line setup are - utz Schweikhardutz L lived lived and stable - ]. In addition, this 11 flight (MR which which can exceed the -

s of -

charge ratios. Thecharge e ]. charge charge dependent time ions frequency frequency measurements of - - - ew tens of milliseconds) are trometry trometry related to the multi order order focusing, i.e. minimization over It It allows precision measurements over - - 15,16 - st ]. ring ring based at mass spectrometry high selective, selective, resolving power, which is - 14 - - frequency frequency shift - reflection time ] and thus contamination suppression for 12 - ], a fir down down to a f between between the source (“S”, Fig. 1a) and the 8

lives down to the microsecond range [ ral facilities around the world [ world the around facilities ral - 17

still still flight mass spec ToF mass spectrometry with respect to ion 2 ]. ]. Besides performing mass measurements, the - -

of

- 6,7 to to

]. While storage 3 - s of MR 1 etermination D lived lived species ( nuclides nuclides with half -

trap mass spectrometry. Cyclotron - Mass Mass ath from a source to a detector. If the ions have identical kinetic ] and are now used at seve now used and are ] time distribution, can be achieved for arbitrary detector positions. detector arbitrary for be achieved can distribution, time - and and 5 lives of several 100ms and above. However, as more challenging - charge effects are investigated. are effects charge - half trap mass spectrometry is the “contamination” with long arrival - binding binding energies of its nucleons and thus with the structure of the nuclei. defined defined p

gives gives access to - intensity intensity monitoring at high, i.e. isobar the the - flight mass spectrometry is based on the mass - Flight Mass Spectrometry Mass Flight ] has recently been added to the experimental event sequence [ art studies of longer - of - - 10 of - Isobar Separation the ToF mass analyzer. In addition, recent preliminary results from an off - - Time In In this contribution, the basics of time Due Due to the production and ionization processes of exotic nuclides, a major obstacle in The The mass is one of the most fundamental properties of atomic nuclei as it is directly of - ToF - Introduction Time ] and the required duration of ion separation. In order to speed up and to enhance the

9 detector (“D”) are proportional to the square root of root their mass square to are the proportional (“D”) detector given by starting in an acceleration different section initial with positions a in homogenous the electric acceleration field. sections source of appropriate field strengths [ In lead general, to different flight of width of the times. But by use of two 2. travel on a well energies, start positions and times, their flight times reflection method are shortly reviewed reflection aremethod as shortly well as setup the and ISOLTRAP the of achievements its MR reported, where the properties and limit and space interactions purification, isobaric mass isobaric separation purification, mass useby of a multi analyzer [ device can be used as a mass spectrometer of its own [ as well as ion [ determination mass precision studies beyond for many useful intended intended precision by orders of magnitude [ Penning trap can also be used for mass purification [ ions with typical scenarios are addressed, this method reaches its limits with respect to the ions’ intensity ratios [ exotic exotic ions stored in high magnetic fields were introduced [ experiment ISOLTRAP almost three decades ago by the precision Penning species, as the Coulomb interaction leads isotopes isotopes and the “mass defect” were discovered. Today, precision mass spectrometry reaches out to and more more exotic nuclides [ kinetic energies state mostly performed by Penning 1. connected to the Already a century ago mass spectrometry had significant input in nuclear physics when new MR PoS(X LASNPA)011 PoS(X LASNPA)011

. s n t  /2 t limit

, =

times times by

m

], in which  / 21 m lived lived nuclides -

- beam beam facilities utz Schweikhardutz , - ]. Beyond these L 19 14 leration zone) leration time time consequences of - optical mirror that reflects -

very very long drift sections or by

and at GSI [

related energy distribution. The ] reflection device can not only be via - - 13 ] and spectra of short or similar. or celerating celerating has to be high. 22

” , either and thus the resolving power and thus the resolving

t

Ridge [

3

lives and/or low production yields are obvious. beam trap beam -

- extended etermination the the ion path several tens, hundreds or thousands of ermal ermal distribution, there are ions with initial velocities in the D

zers zers have already been installed at radioactive flight mass spectrometry devices. For details see text. see details For devices. spectrometry mass flight - ] was a major step to minimize the flight pulse width, i.e. the remaining turnaround time and possibly a fold - of energies energies penetrate deeper into an ion electrostatic ion electrostatic Mass Mass -

“ 18 of the total flight time of total flight the time [ to

t ] ] (Fig. 1c). In this arrangement the ions pass the first mirror and and  time 10 , the flight time has to be flight mass spectrometer, but also as an ion storage device [ - ToF mass analy m - of  - / MR m Isobar Separation ToF studies at ISOLTRAP studies ISOLTRAP at ToF - A A few of 1: Sketches Fig. The initial temporal ion

However, However, this width is also affected by the ions’ energy distribution prior to their ToF - MR

(with already known mass values) were taken at RIKEN [ and further setups are currently under orconstruction planned, as the with advantages respect to accessibility of nuclides with very short half Offline experiments have been performed at Oak mirror mirror (“ejection”) towards the ion detector. Thus, this multi used as a time to as referred often isit case 3. the temporal distribution the distribution temporal To increase use of a second ion mirror multiple reflections [ (“injection”), are trapped between the mirrors, and are finally released by passing the second finite finite duration of inion creation the (or source of the theinto injection acce and, again in first order, ions of different initial energy have the same total flight time. total flight the same have energy initial of different ions order, first in and, again limits limits the resolving power. In order to keep it low, the ac But a high field leads to invention of a the reflectron correspondingly high position this effect: Ions with higher them towards the detector (Fig. 1b). The longer ion trajectory compensates the higher energy acceleration. acceleration. In particular, for a th direction towards the detector and others against the electric force, slowed are down, and back accelerated tostopped their initial positio with opposite direction. The latter, which where justcontinue they their like that started counterparts in the “forward right from direction” travel but be compensated cannot “turnaround” with this associated time The difference the beginning. MR PoS(X LASNPA)011 PoS(X LASNPA)011

- - ) at by by

]. It ]. It s

. RFQ ], and 5,25 31 see section see section continuous continuous - (

]. utz Schweikhardutz

L resonance resonance (ToF quasi 34 - [

the the first use of an 9 - g. 2. g. ] as s s also demonstrated lived nuclides lived [ nuclides 28 ToF device Typically, Typically, the ions are - A - . For details see text see details . For

]. 8 × 10

cyclotron

- 12 frequency frequency quadrupole ( - ToF device are summarized. are ToF device - trap measurement of a previously - flight ion - f its own [ of -

4

t ction ction (if necessary) and for preparation [ trapping devices as sketched in Fi sketched as devices trapping - ToF device, the ions were transferred directly from the trap for short spectrometer mass - - ToF component for a first mass selection, then send to a - etermination MR ISOLTRAP and typical mass spectra mass and typical ISOLTRAP D ] with relative uncertainties down to down uncertainties relative ] with 33 , Mass Mass eparation eparation followed by a Penning 32 and and ] as well as the first determination of so far unmeasured mass value mass of unmeasured ]so far as the as determination well first second second Penning trap for time keV keV kinetic energy (for singly charged ions).

ToF component, i.e. without forwarding the ions to the Penning traps. Penning to the ions the forwarding without i.e. component, ToF 23

] for further mass sele a - 30 ], several other research areas can profit from the MR ToF component as a mass spectrometer o - 7,24 ], transferred to the MR 29 ]. Currently it includes four ion four includes it ]. Currently principle principle studies, the ISOLTRAP collaboration recently reported Isobar Separation - ed by the MR ed by with up to 60 xotic ions are delivered from the online mass separator ISOLDE [ ISOLDE the separator online mass from delivered are ions xotic

of Before Before the installation of the of components 2: Major Fig. E

ISOLTRAP was the ISOLTRAP first Penning - s installed installed at ISOLDE/CERN in the 1980s and continuously further developed over time ToF device for mass s of of its MR ToF . In the following the properties of ISOLTRAP and its MR and its ISOLTRAP of properties the the following . In

- Overview of the ISOLTRAP experimen the ISOLTRAP of Overview -

) 24,26,27 Paul trap to the preparation Penning trap. It is still possible to let the ions pass though the MR ToF section without multiple reflections. On the other hand, mass measurements can perform also be beam decelerated, accumulated, bunched, and cooled in a linear radio Paul trap [ first Penning trap [ finally forwarded to [ measurements mass ICR)

3.1 was [ MR [ value mass unknown use ISOLTRAP [ 3.3 MR proof PoS(X LASNPA)011 PoS(X LASNPA)011

- - a n

lift lift ms, ms,

trap trap ToF ].

- - 40 [

] based on ] based on 35 ms ms and 30 utz Schweikhardutz ToF calibratio

- L trap trap potential flight and thus to - - ]. Mass resolving of 39 - , data data is currently under keV. keV. For ion separation

11,38 workers workers at the Weizmann interest samples with half - - ToF ion signal as a function ToF mass spectrometry is - - of whose whose -

monstrated monstrated with the first mass trap stacking technique has been 80 cm and consists of two mirrors -

are are around 2

trap achieve higher mass measurements about about - purified purified ions without increasing the space can can provide an identification of MR

Zajfman Zajfman and co

Nielsen ion gate [ 5 , an ingredient important for calculations of the -

] , the mirror potentials are lowered for injection

ToF values is not sufficient. Thus, both methods -

23 ToF measurements red with typical excitation times of the order of [ trapped trapped - cm cm long center electrode which acts as an “in

rap of - ICR contamination ions become MR ions become contamination ICR - Zn ToF mass analyzer mass ToF m m t - 82

he measurement time for highly contaminated ion beams er of t ea

b etermination ]. It has a length of - . Furthermore, a Penning ToF devices D - 2 is a logarithmic plot of the MR 36 ,

ToF method uses the simultaneously monitored flight times of ICR ICR measurements - Thus, - 19 Mass Mass the numb

s lived lived species ther ther MR - and and star crusts o ToF [ of has the been device built University at Greifswald second or above can be reduced by about an order of magnitude of order about an by be reduced can above or second -

- ToF mass separator was intended to support and facilitate the Penning electrodes electrodes and a 46 ICR ICR method requires a reference measurement for -

- um um in Fig. 2) is measured by scanning the excitation frequency with ISOLTRAP’s MR ISOLTRAP’s electrostatic electrostatic ion increase ToF system. ]. These are short compa - around a around 7,11 that ToF mass analyzer at ISOLTRAP analyzer mass ToF - The ToF

Generally, Generally, in lives

- MR Isobar Separation ]: ]: 37 Initially, Initially, the MR The lower spectrum of Fig. Typical Typical energies of the (singly charged) stored ions ISOLTRAP’s MR ISOLTRAP’s scanning scanning method, where all ions observed contribute fully to the time ToF Applications of of Applications - The The -

with half lives on the order of a measurement of the short second or below. This has been composition de of neutron implemented charge in the MR are complementary and mutually beneficial. and mutually are complementary 3.3 trap mass measurements by supplying isobarically purified ion evaluation. calibration. In contrast, the MR ToF The words: other In species. ionother ions. On the other hand, ToF signals in cases where the accuracy of the MR the mass determination. the On determination. the mass other hand, the Penning accuracies. and mass powers resolving of flight time for an isobaric mixture at mass number 149. It extended was study taken of in the the accuracy context of of the an MR mass mass measurements the reduction of time consumption is even higher resonance because the (top cyclotron spectr durations of typically a second for each frequency point. Thus, a single scan with 41 frequency points (top inset in Fig. 2) lasts about a minute. In contrast, MR non the mass analyzer is followed by powers a (FWHM) of 100,000 and Bradbury 200,000 are achieved at trapping times of 12 respectively [ hundreds of milliseconds for selecting isobars in the preparation Penning trap. With respect to and ejection. However, these potentials should be as stable as possible and, thus, switching of the mirror voltages should be avoided. This can be achieved by use of the in (Fig. 1d) that reduces the ion energy after the injection from above the potential height of the ion mirrors down to the trapping energy. ejection. In analogy, the ion energy is raised back up for the design of the Institute of Science, Rehovot [ each composed of six lift” [ MR 3.2 PoS(X LASNPA)011 PoS(X LASNPA)011

- - –

the the .

]. of

ion ion

source source

12 -

” ] “self intensity intensity - ], i.e. the 48 - es. In short, 45 -

46 measurements charge charge effects, determinations utz Schweikhardutz - 43 are described are L contaminants Ca, Ca, with an ISOLDE 54

life or decay mode, with ToF mass - - ]. for for target and ion f the nuclear chart [ chart nuclear the f lived lived nuclides, which leads

] for the advanced physics o - lived nuclides. lived

49 - 42 the gap between high

chromium “ chromium the the mass was determined with a , region ]. In fact, this application is closely ] ecent measurements measurements ecent line for the first mass ication ication by use of decay stations, the - 41 n interactions and space 15,24 io ICR) ICR) mass spectrometry [ - - very very beneficial Ca. Ca. In particular for identif 54

Thus, Thus, it closed = 32 in this this in = 32 6 signals signals monitored as a function of the

bunching” bunching” has been observed [ N + ]. ]. In contrast to the other methods available, i.e. - 2

employed employed on 24

, Ca Ca and 53 was and and N life of 86(3) ms [ agnitude. agnitude. 7,16 o “self -

intensity beams of very short of very beams intensity ToF mass analyzer of ISOLTRAP. analyzer ToF mass + - . In this case, the isobaric - etermination recently recently built at Greifswald [ of r results preliminary

beams beams or beam , D - was was ion neutron number number neutron ToF mass spectrometry [

- Mass Mass ToF device - MR and and MR

below one below ppm spite of their repulsing Coulomb interaction the ions do not spread out but out but spread ions interaction not the do Coulomb repulsing of their spite rich calcium isotopes n the following - ToF device I picoampere coalescence coalescence of CO - form form rather short pulses. Similar to the “peak coalescence” effect observed in in in - the the ISOLDE facility [

– ToF device has also shown to be lived nuclides and low and nuclides lived - - ransform ransform Ion Cyclotron Resonance (FT Isobar Separation T ToF studies at Greifswald studies Greifswald at ToF - -

Already Already more than a decade ag Another Another MR Finding efficient excitation schemes for resonance ionization at ISOLDE’s laser source laser ion ISOLDE’s at ionization resonance for schemes excitation efficient Finding The The MR Furthermore, Furthermore, the

intensity. The ToF spectra (right) correspond to the cases marked by the arrows (left). the arrows by marked the cases to correspond (right) spectra ToF The intensity. Fig. 3: Peak ToF mass analyzer opened the possibility to acquire qualitative and quantitative ToF - -

the very neutron MR

on the contrary Fourier [ ion species different of of signals a merging to lead can bunching” laboratory laboratory course. In addition, it is used to study ion which become important at high ion densities, for example when highly contaminated beams handled. toare be that phenomenon there is more than masses for the MR the for masses than more is there 4. a dynamic range of several orders of m of long beams can also be supported by related to studies of isotope shifts and hyperfine structures of short directly back to the investigation of the properties fundamental of these exotic speci developments developments at Faraday cups for MR information from highly resolved isobaric spectra, independent of half of ion yield of only 10 ions/s and a half statistical uncertainty MR The successful masses. ionwere as reference used ISOLDE beam the of the magicity underlined MR PoS(X LASNPA)011 PoS(X LASNPA)011

the the

impact impact doublet doublet 800 for - their ,

while ≈ 2

utz Schweikhardutz L

FWHM R due due to different channel plate (MCP) - ToF setup for several

ectra ectra in Fig. 4 (left) for - could still be separated in the

+ amplitude amplitude of the guiding field. 2 those of Fig. 3.) Fig. of those -

trap lift technique and stored for - investigated investigated by monitoring the ion

e in and N e case of the molecular isobar

+ e ions are produced by were a different mean kinetic energy ( the same as same the

equal equal for both species as they are created

7 e area of the ToF signals for each species as a

from from the Greifswald MR

by by change of the rf

g. p to bottom): For a few hundred ions (case a), the peaks e. (right) (right) are well separated. With increasing number of ions etermination + evice, evice, the ions are detected by a micro 2 D integrated and normalized areas of the ToF peaks and ToF peaks the ofareas and normalized integrated

ToF spectra ion source). Th -

the the evolution of ToF spectra with increasing number of ions is Mass Mass ToF d probed probed experimentally for th =28, which requires a mass resolving power of

- trap - A the signal heights are not are heights the signal and and can can be assumed to be was

(left) (left) and N Paul

+ of of the Paul trap, charge charge effects were already present. The ToF sp - as as a function of the blocking voltage (right). (Note that

s

an example of a kinetic energy of 1 keV. The number of ions can be adjusted by modifying the at mass number

usand usand ions in the trap (case c). As the MCP detection signals are not necessarily linear , Isobar Separation at + 2 Fig. 4: Experimental MR and (left) voltages blocking derivative conditions detector

In In addition, the ions’ kinetic energy distributions In In Fig. 3 This phenomenon ToF device. There, they are captured by means of th /N ToF - these dense ion bunches, the ion numbers are only rough estimates. estimates. rough only are ion numbers the ion bunches, dense these + -

ensity ensity as a function of a blocking voltage applied to deceleration grids in front of the MCP function of the blocking voltage and their first derivative is shown in Fig. 4 (right). 4 (right). in Fig. shown is derivative first their and voltage blocking the of function detector. detector. The ion intensity was chosen in a way that CO spectra, but space different values of the blocking voltage indicate initial kinetic energies simultaneously in the corresponding corresponding to CO their ToF distance decreases (case b) until the peaks are no longer separated, corresponding to some tho for int trapping trapping conditions After ejection from the MR acquisition. data for an oscilloscope to fed is signal Its detector. shown (contour plot on the left, from to CO equal ion intensities. For the present measurements, th ionization in a linear Paul trap and forwarded with a mean kinetic energy of 2 keV towards the MR 1.6 ms MR PoS(X LASNPA)011 PoS(X LASNPA)011

- -

to to ToF ToF - lived lived - proton - also with also with to

line mass

- - –

. dependent dependent ion utz Schweikhardutz

- in in the MR L intensities intensities and ToF device indicate - flight shifts tensity tensity - of absolute absolute beam beam gates. However, the - -

cation cation and Research (BMBF)

.

(2013).

(2005). (2013) , 151

, Elsevier, Amsterdam,, 2006.

3) for for ion separation by energy - 349

123

, 457 ,

principle experiments for several applications 8 (1987). -

).

11 of 350

- (2003). - accurate determination mass and related topics,

ToF settings. If the ion in nuclear nuclear structure at extreme neutron - - , 793 1992 without without switching of ion (

w, w, there are further aspects to be studied in detail. As

, 349 (1991). 38

of of interest MR proof , Vol. 251 (2 for for Ultra lyzer lyzer has demonstrated for the first time on due to the corresponding time due to the corresponding , 1021

ss Spectrom. Spectrom. ss

. , and in case of only a few ions it could not be measured. – 75 , 247, ue to an energy transfer during the ion storage in the MR etermination es , R2140 D 158 46 (2006)

Int. J. Ma particular , 1 Mass Mass Rev. C Eur. J.Spectrom.Mass . In addition, 425 and and , ToF mass ana n n stars and - will be necessary to understand and make use of these effects use of these and make to understand be necessary will Rev. Mod. Phys. Int. Int. J. Spectrom. Mass

Phys. Lett. Phys. A Hyperfine InteractionsHyperfine Phys. et al. , ,

, , ., the effect decreas

et al. et al. Phys. Rep.

et al. et al et al. Yu. Yu. Litvinov, A.

,

olf olf , respectively different ion different species and

charge charge effects have to be considered as they may limit the performance with respect - ToF MS. This feature could be systems, i.e. electrostatic devices Savard Isobar Separation

-

separation is restricted to specific conditions with respect to - G. Bollen K. Blaum, L. SchweikhardL. R.N. W G. D. Lunney F. Bosch G. Bollen This work was supported by the German Ministry for Edu Since the ismethod still relatively ne ISOLTRAP’s ISOLTRAP’s MR Apparently, Apparently, the difference is d

Special issue of Int. Spectrom.Mass J. SchweikhardL. and G. Bollen (Eds.),

ToF - Conclusion Outlook and

[9] [6] [7] [8] [3] [4] [5] [1] [2] References References Acknowledgments under the contracts 05P09HGFNE, 05P12HGCI1, 06GF9101I, and 05P12HGFNE. We thank assistance. their for technical group ISOLDE the as as well Collaboration the ISOLDE an example, preliminary results of recent investigations in a second MR that space to resolving investigation. further under are currently These effects accuracy. mass achievable the to respect separation separation of isobaric nuclides as well as species precision mass with measurements of low very ion short yields, composition which of resulted in neutro valuable asymmetries input for studies of performed. been have determination mass precision the beyond crustal device device is reduced investigations Further 5. ToF. ToF. The separation energy corresponds to ten of percent the total initial mean in kinetic energy the MR transfer energy abundance ratios as well as MR PoS(X LASNPA)011 PoS(X LASNPA)011 utz Schweikhardutz L

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ToF - [36] [37] [38] [39] [33] [34] [35] [29] [30] [31] [32] [25] [26] [27] [28] [22] [23] [24] [18] [19] [20] [21] [15] [16] [17] [11] [12] [13] [14] [10] MR PoS(X LASNPA)011 PoS(X LASNPA)011 utz Schweikhardutz L

(2009).

, 3213 23

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42

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Appl. Appl. BPhys. Proc.AIP Conf. Phys. Phys. and and , J. Am. Soc.J. Am. Spectrom.Mass

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, J. Soc. Spectrom. Mass Jpn. , , Phys. Phys.

et al. , et al. et al.

et al. et al. et al. Chinese Phys.Chinese C , et al. et al.

enbusch enbusch Isobar Separation B.Pedersen, A. Boldin,A. E. N Nikolaev, P.A. Bolotskikh I. G. Audi G. Vladimirov D. Strasser Y. Naito, M. Inoue, M. Ros H. H.B.Pedersen M. Rosenbusch

ToF - [48] [49] [45] [46] [47] [41] [42] [43] [44] [40] MR