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EPJ Web of Conferences 63 , 03002 (2013) / / DOI: 10.1051 epjconf 20136303002 C Owned by the authors, published by EDP Sciences, 2013

Stellar capture rates – key data for the s process

F. Käppeler1,a 1Karlsruhe Institute of Technology, Campus North, IKP,76021 Karlsruhe, Germany

Abstract. Neutron reactions are responsible for the formation of the elements heavier than iron. The corre- sponding scenarios relate to the He- and C- burning phases of stellar evolution (s process) and to supernova explosions (r and p processes). The s process, which is characterized by low neutron densities, operates in or near the valley of stability and has produced about half of the elemental abundances between Fe and Bi in the solar system and in the Universe. Because the s abundances are essentially determined by the (n,) cross sections along the reaction path, accurate neutron data constitute the key input for s process studies. Important constraints for the physical conditions at the stellar sites can be inferred by comparison of the abundance pat- terns from current s-process models with solar system material or presolar grains. The experimental methods for the determination of stellar (n,) rates are outlined at the example of recent cross section measurements and remaining quests will be discussed with respect to existing laboratory neutron sources and new developments.

1 Introduction eration occurs by alternate episodes of radiative H burn- ing and convective He burning in a comparably thin shell The concept of as the ori- around the inert C/O core. Along with H burning, gin of the heavy elements beyond the Fe group has been are liberated by the 13C(↵, n)16O reaction at temperatures 8 formulated half a century ago in the pioneering work of of T8 1(T8 means T in units of 10 K), yielding neu- 2 ⇡ 7 3 Burbidge, Burbidge, Fowler and Hoyle (B FH) [1] and of tron densities of about 10 cm . Because there are only Cameron [2]. Accordingly, the elements heavier than iron few seed nuclei in this thin shell, the neutron/seed ratio are predominantly produced either by the slow (s) or the is high and the s process operates very eciently over a rapid (r) neutron capture process, which are characterized long period of time. During the subsequent convective He by their typical neutron capture times with respect to the flashes, the freshly synthesized material is mixed and di- average -decay half lives. Both processes are contribut- luted with the He intershell and is again exposed to neu- ing about half of the observed solar abundances between trons liberated by the 22Ne(↵, n)25Mg reaction at temper- Fe and U. A third process, the so-called p (photodissocia- atures T 2.5. The second neutron exposure is rather 8 ⇡ tion) process, is responsible for the origin of about 30 rare, weak and not sucient to produce s on a grand -rich nuclei, but does not contribute significantly to scale but strong enough to determine the ratios the synthesis of the elements in general (<1%). of s-process branchings. After the He flash, where peak 10 3 Since the formulation of these concepts, considerable neutron densities of 10 cm are reached, part of the progress has been achieved in the quantitative description freshly synthesized material is mixed with the envelope of the s process, which meanwhile provides rather detailed and brought to the surface of the star, where it is detectable information of the s component in the solar system abun- by optical spectroscopy. A famous example is the early dances as well as of the role the s process plays in galactic discovery of Tc lines by Merrill [4], which confirmed that chemical evolution. Two s components have been identi- heavy elements are produced during the red giant phase of fied, the main and the weak s process, which are connected stellar evolution. with the specific burning phases in stars of di↵erent mass. The weak s component, which is responsible for the Initially, a third component, the strong s process, had been production of nuclei between iron and (56 < A < invoked for explaining part of the observed 208Pb abun- 90), takes place during convective core-He burning in mas- dance, but was eventually ascribed to the main s process sive stars (M 8M ), where temperatures reach (2.2 - in low-metallicity stars [3]. 3.5) 108 K, thus marginally activating the 22Ne(↵, n)25Mg The main s process, by far the most studied pro- ⇥ . Because the resulting neutron exposure cess, occurs in the He-rich intershell of thermally pulsing is rather limited, the s-process reaction flow cannot over- asymptotic giant branch (AGB) stars with M 3M (M  come the bottleneck caused by the small cross sections denotes the mass of the ) and produces predominantly of the isotopes with closed neutron shells at N = 50. nuclei between 90Zr and 209Bi. At this stage, energy gen- However, most of the material in the core is reprocessed ae-mail: [email protected] by the following burning stages and only a part survives

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in the outer layers and is ejected during the final su- complex reaction paths far from stability, which must be pernova explosion. A second neutron exposure occurs described by huge networks including several thousand during convective carbon shell burning in massive stars reactions. By far most of these reaction rates have to be [5, 6], where neutrons are produced mostly by the re- obtained by statistical model calculations [10, 11]. Never- maining 22Ne(↵, n)25Mg, but also via 17O(↵, n)20Ne and theless, experimental data for stable and as many unstable 13C(↵, n)16O. The high temperatures during carbon burn- isotopes as possible are required for testing the necessary ing of T9 1 cause high neutron densities, which start at extrapolation to the region of unstable nuclei. 11⇡ 12 3 about 10 10 cm and then decrease exponentially. To cover the range of s-process temperatures between The nucleosynthesis yields of the weak component in T8 = 1 to 9, experimental neutron capture cross sections massive stars are also important for the r process, since are needed over an energy range from about 300 eV to they determine the composition of a star before the super- several hundred keV, which then have to be folded with nova explosion. In contrast to the s process, where neu- the fully thermalized neutron energy distribution in the tron capture times of the order of days to years confine the stellar plasma. These Maxwellian averaged cross sections reaction path to or close to the valley of stability, ex- (MACS) are defined as 22 3 tremely high neutron densities of 10 cm are reached 1 En/kT in the r process, giving rise to capture times of the order of v 2 0 (En) En e dEn kT = h i = , (1) milliseconds. These parameters are clearly indicating an E /kT h i vT p⇡ R 1 En e n dEn explosive scenario for the r process either related to super- 0 novae or neutron star mergers. In either case, the extreme lab R where En = En (A/(A+1) denotes the total kinetic energy neutron densities imply that (n,) reactions are becoming in the center-of-mass system, Elab the laboratory neutron much more rapid than decays, thus driving the reaction n energy, vT = p2kT/m the mean thermal velocity, and m path to the region of very neutron-rich nuclei at the limits the reduced mass for the neutron-target system. of stability. The initial reaction products of the explosive MACS values are required for all nuclei and all tem- r process, which lasts for about a second, are highly - peratures involved in a particular scenario, essentially unstable and decay after the explosion back to the valley from 12C up to the Pb/Bi region. It is important to note of stability, where they mix with the s abundances. that the high s-process temperatures imply that excited nu- The reaction paths of the s and r process are sketched clear states are in thermal equilibrium by the intense and in Fig. 1. The neutron-rich isotopes outside the s path can energetic thermal photon bath, resulting in a significant be ascribed to the r process. Apart from these r-only iso- population of low-lying states. The e↵ect of neutron cap- topes the r process contributes also to most of the other tures in these excited states has to be determined by theory isotopes, provided that they are not shielded by stable iso- and may require significant corrections to the experimental bars. The corresponding ensemble of the r-shielded, s- data [12]. only isotopes is important for the separation of the respec- The thermal environment can have also a considerable tive abundance distributions and, more importantly, to set impact on the weak decays of the unstable branch point constraints for the overall s-process eciency and for the isotopes along the reaction chain: The rate for -decays parameters governing the abundance pattern in s-process may be dramatically enhanced if the excited states have branchings. The subset of r-only nuclei can be used for much shorter half-lives than the ground state. The rates calibration of the abundance contributions from the r pro- for EC-decay are a↵ected by the high degree of ionization cess. About 32 stable isotopes on the proton-rich side, in two ways: a reduction due to the loss of K-shell elec- which cannot be produced by stellar neutron reactions, are trons is partly compensated by capture of free electrons. attributed to the p process, which is likely to occur also in Bound , where electrons are emitted in unoccu- supernova explosions [7]. With very few exceptions, these pied atomic orbits, can result in a dramatic enhancement p abundances are much smaller than the s and r compo- as well. For a full discussion of s-process beta decays see nents. Refs. [13, 14].

2 Stellar neutron capture cross sections 3 Experimental methods Presently, experimental techniques for (n,) measure- ments have reached a stage, where the 1-2% accuracy level 3.1 Time-of-flight experiments required for suciently detailed analyses of the s-process abundance patterns can be met [8, 9]. While this level has Time-of-flight (TOF) measurements are essential for ob- been achieved so far only for a minority of the relevant iso- taining energy-di↵erential neutron capture cross sections topes, a large number of cross sections with uncertainties over a suciently large energy range so that MACS values in excess of 10% await improvement, still including many can be determined from these data for any stellar temper- remaining key nuclei. With a few exceptions, experimen- ature of interest. Recent developments and improvements tal data for the important unstable branch point isotopes in pulsed neutron sources and detection techniques have are still completely missing. led to (n,) cross section measurements with improved ac- In contrast to the favorable situation of the s process, curacy, in many cases with uncertainties of 2 - 4%. where mostly stable isotopes are involved, explosive nu- As far as the laboratory neutron sources are concerned, cleosynthesis scenarios of the r and p processes imply reactions induced by energetic particle beams

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Figure 1. Illustration of the main neutron-capture processes responsible for the formation of the nuclei between iron and the actinides. The reaction path of the s process follows the stability valley because the neutron capture times are much slower than decay on average. The abundance contributions from the r process (dashed arrows) are mixing with the s component, except where the s- only isotopes are shielded by stable isobars. Note also the occurrence of branchings in the s-process path at suciently long-lived unstable nuclei. The branching points give rise to a local abundance pattern that carries important information on neutron density and temperature at the s-process site. The small cross sections at magic neutron numbers introduce another important constraint for the s process because they act as bottle necks for the reaction flow.

constitute the most prolific pulsed sources of fast neutrons ergy represents the best signature of a capture event, 4⇡ for TOF measurements. Presently, spallation sources in detector arrays with an eciency close to 100% are the routine operation are LANSCE at Los Alamos [15], the most direct way to unambiguously identify (n,) reactions n_TOF facility at CERN [16, 17], and ANNRI at J-PARC and to determine capture cross sections with good accu- [18]. The main advantage of these facilities is the out- racy. Such calorimeters are designed either in spherical standing eciency for neutron production due to the high geometry, using BaF2 crystals arranged in a fullerene-type primary proton beam energies, reaching 300 neutrons per configuration with each module covering the same solid incident proton at n_TOF, for example. Spallation sources angle with respect to the central sample [21–23], or in a are providing a wide neutron energy range and are oper- barrel-type geometry, where the sample is surrounded by ated at rather low repetition rates, typically between 0.4 layers of hexagonal crystals [24, 25]. and 50 Hz, while still maintaining high average intensi- The main problem in using calorimeter type detectors ties. Rather high intensities can also be achieved via (, n) arises from their response to neutrons scattered in the sam- reactions at electron linear accelerators, such as GELINA ple. Although the BaF scintillator is selected to consist at Geel, Belgium, by bombarding heavy targets with 2 of nuclei with small (n,) cross sections, about 10% of electron beams of typically 50 MeV. All these facilities the scattered neutrons are still captured in the scintillator. provide very good resolution in neutron energy and have While the related background can be handled in most mea- been extensively used to study the resolved resonance re- surements, it may complicate the analysis of resonances gion. with very small capture-to-scattering ratios. The spectrum of keV neutron facilities includes also The problem of neutron sensitivity is largely avoided small accelerators, where neutrons are produced by nu- by using comparably small, hydrogen-free liquid scintilla- clear reactions, such as the 7Li(p, n)7Be reaction, which tors in combination with the pulse-height weighting tech- o↵er the possibility of tailoring the neutron spectrum ex- nique (PHWT) [26], in particular since the second gener- actly to the stellar energy range. Limitations in source ation of detectors, which are based on deuterated benzene strength can be compensated by low backgrounds and the (C D ), has been designed to minimize backgrounds due use of comparably short neutron flight paths [19, 20]. 6 6 to scattered neutrons to a practically negligible level [27]. Current TOF measurements of (n,) cross sections With advanced Monte Carlo codes, realistic descriptions are based on two types of detectors. Total absorption of the detector response and of the weighting functions calorimeters are designed to detect the full energy sum of (WF) could be obtained on the basis of detailed computer the -ray cascade emitted in the decay of the compound models of the experimental setup [28–31]. Such refined nucleus, which corresponds essentially to the neutron sep- simulations have been shown to reduce the systematic un- aration energy of the captured neutron. Because this en- certainty of the PHWT to about 2% [30]. Although the

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Figure 2. Left: Schematic sketch of the activation setup. Right: The quasi-stellar neutron spectrum obtained with the 7Li(n,)7Be reaction (histogram and symbols) compared to a true Maxwell-Boltzmann distribution for a thermal energy of = Figure 3. The s-process reaction flow in the mass region 140 kT 25 keV [32].  A 150 including the crucial s-only isotope 142Nd and the  branchings at A = 147, 148. eciency of C6D6 detectors is only about 20%, they are clearly of advantage in studies of resonance-dominated cross sections with very small capture-to-scattering ratios. testing the validity of stellar s-process models related to He shell burning in thermally pulsing AGB stars. In addi- tion, the measurement of the small cross sections of abun- 3.2 Activation with quasi-stellar neutrons dant light isotopes and their role as neutron poisons are discussed at the example of 13C. The activation method represents a well established and accurate approach for MACS measurements at a ther- 142 mal energy of kT = 25 keV by irradiating samples in a 4.1 Nd: confirming the stellar model for the quasi-stellar neutron spectrum that can be produced via main s process the 7Li(p, n)7Be reaction [32, 33]. Such a spectrum is ob- The s-only isotope 142Nd belongs to the stable neutron- tained by using a proton beam energy of E = 1912 keV, p magic nuclei with N=82, which act as bottle necks for the 30 keV above the reaction threshold. With this choice of reaction flow. The small MACS values of these isotopes E , neutrons are kinematically collimated into a forward p prevent that flow equilibrium is locally achieved in the cone of 120 deg opening angle. The e↵ect of fluctuations mass range A = 138 142. Because the s-abundance dis- in beam intensity during the irradiations can be corrected tribution below and above that critical region is well con- by continuously monitoring the neutron yield by means of strained by the important s-only isotopes 124Te and 150Sm, a 6Li-glass detector. the N=82 region provides a crucial test for the mean neu- With typical beam intensities of 100 µA, neutron inten- tron exposure of the main s-process component, ⌧ [36]. sities of 3 109 s 1 can be reached, orders of magnitude 0 ⇥ In particular, the resulting 142Nd abundance is sensitively higher than in TOF experiments. Accordingly, the activa- probing the way an s-process model is treating the reaction tion method o↵ers unique sensitivity. Further advantages flow across the bottle-neck region. are (i) that isotopically enriched samples are not required, The classical steady s-process model [36, 37] has long because the reaction products are identified by their char- been considered a useful tool for describing the s-process acteristic radiation, and (ii) that contributions from the abundances and for estimating the physical conditions dur- direct radiative capture (DRC) channel are automatically ing the s process via the abundance pattern of the various considered. A sketch of the experimental setup and the branchings. The left panels of Fig. 4 illustrate the abun- comparison of the resulting quasi-stellar neutron spectrum dances of the s-only isotopes between 130Xe and 160Dy as with a true Maxwell-Boltzmann distribution are shown in obtained with the classical model before and after an ac- Fig. 2. Note that the experimental spectrum in the right curate cross section of 142Nd became available. The new panel of Fig. 2 falls below the Maxwell-Boltzmann distri- MACS of 142Nd [38], which was 25% lower than the value bution above 80 keV and is truncated at a neutron energy used before, gave rise to a significant 12% excess of 142Nd of 106 keV. Meanwhile, it has been found that the high- compared to the solar abundance. In view of the 2% un- energy part of the spectrum can be better approximated by certainty of the quoted value, this discrepancy revealed using an energy-broadened proton beam with a spread of the first convincing inherent inconsistency of the classical about 20 keV [34, 35]. model, indicating that the simplifying assumptions of this approach are not adequate for describing the true stellar 4 The role of key cross sections scenario. Although necessarily more complex, realistic prescrip- The key isotopes 142Nd and 147Pm, which are included in tions on the basis stellar s-process scenarios have been de- the s-process reaction flow shown in Fig. 3, are used to veloped as sketched in Sec. 1. For the main component illustrate the crucial role of stellar (n,) cross sections for (including the mass region of Fig. 4) the He shell burning

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So far, most branching analyses are based on solar iso- tope patterns [8, 39], but it should be noted that important information on the s-process neutron density can be de- rived directly from spectroscopic data of individual AGB stars via the branchings at 85Kr and 93Zr [40] or from anal- yses of presolar grains preserved in primitive meteorites [41]. The branching at 147Pm (Fig. 3) is part of a series of important branchings in the lanthanide region. Apart from the "normal" branch point isotopes 147Nd, 147,148Pm, which are only sensitive to the stellar neutron density, the half-lives of 151Sm, 152,154Eu exhibit a temperature depen- dence [13], which makes these branchings potential ther- Figure 4. The overproduction factors of the s-only isotopes rel- mometers for the s-process environment [42, 43]. ative to solar material (normalized at 150Sm) in the mass region The measurement of neutron capture cross sections on 130 A 160. While a perfect model would always yield   unstable isotopes is complicated by the radioactivity of the factors of unity, the upper panels ("a" for the classical and "b" sample. For many of the branch point isotopes, this results 142 for the stellar model) indicate an underproduction of Nd when in an immense background that can hardly be handled the previous cross section was used for this key isotope, regard- by the detectors and hampers the safe identification of cap- less of the s-process model. The lower panels illustrate the e↵ect ture events in the sample. Also, the required samples are of the improved, accurate cross section of 142Nd [38], which is clearly favoring the physical stellar model (d) over the purely most often not available in amounts needed for TOF exper- phenomenological, classical approach (c). iments. Therefore, measurements have resorted to the ac- tivation technique. The excellent sensitivity of this method permitted the use of samples in the µg range, thus reducing the radiation hazards by several orders of magnitude. episodes in low mass AGB stars have been shown to repro- The example of 147Pm is quite illustrative in this re- duce the s abundances to better than 10% [39]. Contrary spect, because the activation was performed with only 28 to the classical picture, this rather complex model is char- ng of material, the smallest sample used in (n,) studies acterized by two neutron sources operating with very dif- at keV energies so far. To compensate for the low induced ferent strength and at di↵erent neutron densities and tem- activities that can be obtained with such a small sample, peratures. an optimized setup for counting had to be used by plac- The success of the stellar model compared to the clas- ing the irradiated sample between two large Clover-type sical approach is illustrated in the right panels of Fig. 4, HPGe detectors in very close geometry. For suppression showing that the new 142Nd cross section [38] resulted in of the still dominant background from the decay of 147Pm a perfect reproduction of the solar value (panel d). More- (t / = 2.62 yr), one had to go a step further, using the over, there is clearly an improved overall agreement for 1 2 eight-fold geometry of the two Clover detectors for the co- the other s-only isotopes as well. incident detection of the (915+550) keV cascade in the decay of 148Pm. In this way, the dominant 40K background 147 4.2 Branchings as diagnostic tools: Pm could be suciently reduced to determine the stellar cross 147 Branchings in the reaction path are the result of the com- section of Pm with an uncertainty of 14%, leading to a mean neutron density of n = 4.9 0.6 cm 3 [44]. petition between neutron capture and -decay whenever n ± an isotope with a half-life comparable to the neutron cap- ture time is encountered. This competition is expressed 4.3 13C: a potential by a branching factor f = that depends formally on +n the -decay rate = ln2/t1/2 and on the neutron capture Limits of MACS measurements with the activation method rate = n v with n being the neutron density, v the refer to cases where the induced activity is very low, un- n n T h i n T mean thermal velocity, and the MACS for the radioac- certain, or dicult to detect. For such reactions, accelera- h i tive branch point nucleus. tor mass spectrometry (AMS) o↵ers a powerful alternative The s-process branchings are producing a local abun- with the important advantage compared to decay counting dance pattern that includes an s-only nucleus, which is par- that it is independent of the half-lives and decay properties tially bypassed by the reaction flow. Accordingly, these of the reaction products. The main feature of AMS is the nuclei exhibit a smaller N value than what is charac- unsurpassed sensitivity for specific , much higher h i teristic of the full reaction flow and thus provide a mea- than can be obtained with conventional mass spectrome- sure for the strength of the branching. The di↵erent ratios try, disadvantages are often elaborate sample preparation of neutron capture and -decay in the various branchings and the destruction of the sample by the measurement. along the s-process path from Fe to Bi represent viable AMS has first been applied to neutron capture reac- and stringent tests of s-process prescriptions and, hence, tions in s-process environments for 62Ni by Nassar et al. for models of the He and C burning phases of stellar evo- [45] and subsequently to a number of target nuclei includ- lution. ing 40Ca, 58Ni, 62Ni, and 78Se [46–48]. The 13C(n,)14C

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the b regime: 13C(n, ) an example for activation + AMS

148Pm

40 K - 1461 keV

Wallner et al., Pub. Astron. Soc. Australia 29 (2012) 115

Figure 5. Discrimination of the induced 148Pm activity against Figure 6. Experimental cross sections for the 13C(n,)14C re- the 1461 keV background from 40K by coincident detection the actions in the keV neutron energy region together with calcu- (915+550) keV cascade in the decay of 148Pm (from Ref. [44]). lated values [50] and recent evaluations from the JEFF-3.1 data library. The width of the experimental neutron energy distribu- tions are indicated by horizontal bars. The shaded areas corre- spond to spectrum-averaged cross sections derived from the cal- culated data of Ref. [50]. reaction was studied as part of a recently completed series of measurements [49] and represents a typical example for combining activation at keV neutron energies with subse- quent AMS detection of the long-lived reaction product of that resonance is much less significant than previously 14C. assumed. An interesting feature of this reaction is the strength of the resonance at En = 143 keV (Fig. 6), which interferes 5 Status and Outlook with the p-wave contribution of the direct capture compo- nent. At temperatures above T8 = 3 the reaction rate is The current MACS status is collected in the KADoNiS dominated by the 143 keV resonance, at lower tempera- database [54], which contains an almost complete set of tures by the p-wave and s-wave contributions. The calcu- experimental MACS values for the 279 stable isotopes on lations [50] are in reasonable agreement with two previ- the s-process path. KADoNiS also includes data for 77 ous experiments [51, 52], but exhibit a significant discrep- radioactive nuclei, albeit this subset still has to rely on ancy compared to the most recent evaluation of JEFF-3.1, theoretical calculations with the HF statistical model (e.g. which is consistently higher than the calculation, culmi- [10]). An important aspect of the MACS data refers to the nating in a 25 times higher peak value for the 143 keV accuracy needed for meaningful abundance predictions. resonance. On average, cross sections should be available with an ac- 13 curacy of 5% or better, but uncertainties as low as 1-2% This discrepancy, which is important for the role of C are mandatory for a number of key isotopes, e.g., for the as an s-process neutron poison, was studied using the acti- 33 s-only nuclei on the s-process path. Examples for this vation technique [53]. The samples were irradiated at the species are 148,150Pm in Fig. 3. Karlsruhe Institute of Technology in the quasi-stellar neu- Similarly accurate data are needed for the interpre- tron spectrum for the direct determination of the MACS tation of the s-process signatures of presolar grains [41] = at kT 25 keV, and also using neutron spectra with 123 that concern about 70 isotopes. The discovery of preso- ↵ and 178 keV mean energy to investigate the e ect of the lar grains in primitive meteorites opened a new window 143 keV resonance. After the irradiations the produced 14 to and galactic chemical evolu- amount of C was quantitatively determined by AMS. In tion, because they represent material from individual stars, this experiment, the cross sections could be obtained with which survived the high temperature phase during the for- uncertainties of 7 to 12%. mation of the solar system. Accordingly, analyses of such Fig. 6 shows that the results of the AMS measure- grains provide insight into the sensitivity of the s process ment at 25 keV are in fair agreement with the previous to stellar mass and metallicity. experimental [51, 52] and theoretical [50] data, but about Although experimental data exist for most stable iso- two times higher than the JEFF-3.1 evaluation. For the topes of interest for the s process, the criteria of complete- two higher neutron energies a striking discrepancy was ness and accuracy are met only in a minority of cases. found with respect to the strength of the 143 keV reso- From the standpoint of accuracy, this aspect is illustrated nance, which turned out to be a factor of 10 lower than in Fig. 7, where the respective uncertainties are plot- the calculation of Herndl et al.[50] (indicated by the hor- ted versus . Though the requested uncer- izontal bars in Fig. 6). Accordingly, the poisoning e↵ect tainties have been locally achieved, further improvements

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mass spectrometry were used to illustrate the direct impact of neutron capture studies on the s-process contribution to galactic chemical evolution as well as the unbiased infor- mation on the physical properties of the stellar s-process sites that can be derived from s-process branchings.

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