The Astrophysical Journal, 594:605–616, 2003 September 1 # 2003. The American Astronomical Society. All rights reserved. Printed in U.S.A. THE PREDICTABLE COLLATERAL CONSEQUENCES OF NUCLEOSYNTHESIS BY SPALLATION REACTIONS IN THE EARLY SOLAR SYSTEM I. Leya, A. N. Halliday, and R. Wieler Institute for Isotope Geochemistry and Mineral Resources, ETH Zürich, NO C60.6, CH-8092 Zürich, Switzerland; [email protected] Received 2003 April 2; accepted 2003 May 8 ABSTRACT Ever since their first discovery in 1960, the origin of the relatively short-lived radionuclides, now extinct but alive in the early solar system, has been under debate. Possible scenarios are either nucleosynthetic production in stellar sources, e.g., asymptotic giant branch stars, Wolf-Rayet stars, novae, and supernovae, with subsequent injection into the solar nebula, or the production by spallation reactions in the early solar system. Here we present model calculations for the second scenario, the production of the relatively short-lived radionuclides by solar energetic particle events at the start of the solar system. The model is based on our current best knowledge of the nuclear reaction probabilities. In addition, the modeling depends on the relative fluence contribution of protons, 3He, and 4He in the solar particle events as well as on their energy distribution. The relative fluence contribution is the only free parameter in the system. Finally, the modeling depends on the chemical composition assumed for the irradiated target. The model simultaneously describes the observed solar system initial ratios 7Be/9Be, 10Be/9Be, 26Al/27Al, 41Ca/40Ca, 53Mn/55Mn, and 92Nb/93Nb. In the framework of the local production scenario, the concordance of measured and modeled data for nuclides with half-lives ranging from 53 days up to 36 Myr enables us to put some stringent constraints on possible calcium-aluminum–rich refractory inclusion (CAI) production and its timing. One important requirement in such a scenario is that the material forming most of the CAIs must have experienced a surprisingly homogenous particle fluence. CAIs showing evidence for live 10Be, 26Al, 41Ca, 53Mn, and 92Nb close to the inferred solar system initial ratios would have to have been irradiated within 1 Myr. Much more stringent would be the time constraint for the one CAI for which formerly live 7Be has been reported. Such CAIs would have to have been irradiated for less than about 1 yr. Such a short timescale requires flux densities as high as 1016 cm2 s1. To allow further tests of the local production scenario, we also predict solar system initial ratios for 14C/12C, 22Na/23Na, 36Cl/35Cl, 44Ti/48Ti, 54Mn/55Mn, 63Ni/60Ni, and 91Nb/93Nb, whose correlated shifts in the daughter isotopes would help to further test the local production scenario. Subject headings: nuclear reactions, nucleosynthesis, abundances — solar system: formation abundances in the early solar system is not straightforward, since three different stellar events are needed, and their timing is crucial (Meyer & Clayton 2000). Another difficulty is that this scenario requires that only the outermost layers of a supernova, about 1 Myr prior to solar system formation, were injected into the collapsing molecular cloud core. However, such a scenario is so far not widely accepted. In addition, recent experimental data yield evidence for the existence of two short-lived radionuclides in the early solar system that are difficult to explain within a stellar production scenario. In recent years 10B excesses resulting from the in situ decay of 10Be in the early solar system have been reported by various authors (e.g., McKeegan, Chaussidon, & Robert 2000; MacPherson & Huss 2001; Sugiura, Shuzou, & Ulyanov 2001). The existence of live 10Be is difficult to explain by nucleosynthetic production because in most stellar events Be is destroyed rather than produced. 10Be production in bursts emitted from a rapidly rotating neutron star has been proposed as an explanation for this (Cameron 2001). More recently, a 7Li excess thought to be from the in situ decay of 7Be has been reported for one CAI (Chaussidon et al. 2001; Chaussidon, Robert, & McKeegan 2002). The easiest explanation for this finding in the context of stellar production would be that stellar explosions carried the nuclide into the solar system in so-called presolar grains, which are believed to be direct condensates in late-stage stellar outflows. However, Chaussidon and coworkers 1. INTRODUCTION Numerous studies have unambiguously proved the existence of relatively short-lived radionuclides in early solar system objects. Their former presence is indicated by excesses of their daughter isotopes. The most promising objects for such studies are refractory condensates found in some types of meteorites, the so-called calcium-aluminum– rich refractory inclusions (CAIs). Because of analytical improvements, the number of relatively short-lived radionuclides that were known to be alive in the early solar system has shown a dramatic increase since the first detection of 129I and 26Al (Reynolds 1960; Lee, Papanastassiou, & Wasserburg 1977). The relatively short-lived radionuclides offer great potential for chronological studies of early solar system events with a high time resolution. However, before they can be used for dating, the origin of the radionuclides has to be known, and the question of whether they were homogeneously distributed throughout the early solar system has to be answered. For many years the most promising hypothesis was that these radionuclides were produced by stellar nucleosynthesis, e.g., asymptotic giant branch stars, WolfRayet stars, novae, or supernovae. Connected to this stellar production scenario is the hypothesis that the source of the nuclides may also have triggered the collapse of the molecular cloud core, from which the solar system formed. However, a self-consistent description of the radionuclide 605 606 LEYA, HALLIDAY, & WIELER conclude from systematic mineralogical studies of the respective CAI that it once contained live 7Be, and one therefore has to consider the consequences if this nuclide really was extant in the early solar system and related to the formation of the other short-lived nuclides. If 7Be was really alive in the early solar system (so far, 7Li excesses have been found in only one CAI), the half-life of only 53.25 days excludes scenarios of 7Be production by stellar nucleosynthesis with subsequent injection of live 7Be into the solar system. Therefore, the report of live 7,10Be in the early solar system does reinforce the arguments based on 10Be that at least some of the relatively short-lived radionuclides were produced within the early solar system by spallation reactions. The projectiles may have been accelerated to high energies by various mechanisms in young stellar objects (YSOs). For example, regions of projectile acceleration near the surface of the YSO (as for the recent Sun), in the X-region as well as close to the accretion disk, are discussed by Feigelson, Garmire, & Pravdo (2002). In the framework of the X-wind model, flare generation and acceleration are in the X-region (e.g., Russell, Gounelle, & Hutchison 2001). Throughout this paper we refer to this as the ‘‘ local production scenario.’’ The local production scenario is further supported by astronomical observations. Systematic studies of X-ray emissions from YSOs indicate that most of them eject significant amounts of their material as solar energetic particles (SEPs) and/or bipolar outflows. In a recent systematic study, Feigelson et al. (2002) show that the so-called T Tauri phases are common for stellar objects with 0.8–1.4 M and that the particle flux in the YSO phase is up to 105 times higher than for recent solar SEP events. The energy of the emitted particles, i.e., mostly protons, 3He, and 4He, is as high as some tens of MeV nucleon1 in present-day SEP events. Particles in this energy range induce nuclear reactions in the irradiated material. If SEP production is either near the accretion disk or in the X-region, various kinds of nuclear reactions within the disk material are induced. If the SEP production is on the surface of the YSO, a magnetic connection of the protostar with the accretion disk is required for any local production scenario. In such nuclear interactions, among others, short-lived radioactive isotopes are produced. Depending on the mechanism for SEP production, the projectiles might be focused on small regions, leading to high nuclide production rates. Therefore, nuclear spallation reactions may well have contributed to the nucleosynthesis of some of the relatively short-lived radionuclides, e.g., 7,10Be, 26Al, 36Cl, 41Ca, and 53Mn. In recent years various groups tested the local production scenario by comparing the modeled nuclear spallation yields with the inferred solar system initial ratios (e.g., Lee et al. 1998; Gounelle et al. 2001; Goswami, Marhas, & Sahijpal 2001). However, they all failed to simultaneously describe the initial solar system radionuclide abundances for targets having a common chemical composition (solar or CAI). If the projectile spectrum was adjusted so that the modeled 26Al/27Al was in agreement with the initial ratio inferred from meteorite data, the modeled initial 41Ca/40Ca was about 2 orders of magnitude larger than the experimental ratio (e.g., Lee et al. 1998). This problem was circumvented in a later study by assuming a Ca-poor rim around the irradiated material (Gounelle et al. 2001). However, such a layering is not supported by mineralogical observations. Another independent approach to solve this Vol. 594 problem was made by Goswami et al. (2001). These authors studied whether the introduction of shielding effects in the target could result in concordancy between measured and modeled 26Al/27Al and 41Ca/40Ca ratios. However, as expected from nuclear reaction analyses, shielding mostly changes the total particle fluxes but only slightly affects relative proportions of the various nuclides, e.g., the 26Al/41Ca ratio. Here we present new model calculations for the production of 7,10Be, 14C, 22Na, 26Al, 36Cl, 41Ca, 44Ti, 53,54Mn, 60Fe, 63Ni, and 91,92Nb by spallation reactions in the early solar system. In contrast to the earlier studies, our approach is based on the particle spectra for protons, 3He, and 4He in current SEP events; i.e., all three projectile types are included. A further advantage of this approach is that both types of SEP events (gradual and impulsive; see below) are included, with their relative fluence as a free parameter. All excitation functions used are based on our current best knowledge of the relevant nuclear reactions. Assuming a chemical composition of the irradiated material and adjusting the modeled production rate for 10Be to the inferred solar system initial 10Be/9Be ratio of 103 (for a discussion, see below) enables one to estimate the particle fluence needed to produce sufficient 10Be in the irradiated object (the ‘‘ proto-CAI ’’ material). Using this fluence, the collateral production rates for the other short-lived radionuclides are then determined. Assuming spectral parameters (energy distribution, chemical composition) of the SEP events similar to those values for the recent Sun and assuming further solar chemical composition for the target material enables one to simultaneously describe most of the inferred solar system initial abundances of the relatively short-lived radionuclides. Based on the agreement between measured and inferred solar system initial ratios, stringent constraints are placed on the CAI production scenario and its timing in the framework of the local production scenario. 2. MODEL CALCULATIONS The calculations of production rates for the relatively short-lived radionuclides in the early solar system are based on a model originally developed over many years to describe solar and galactic cosmic-ray induced production of cosmogenic nuclides in meteorites and lunar rocks (e.g., Michel & Neumann 1998; Leya et al. 2000, 2001). For these samples the model calculations are now able to predict measured production rates to within 12%. The model is based on the differential projectile spectra, the excitation functions of the relevant nuclear reactions, and the chemical composition of the irradiated target. The production rates (g1 s1) for the product nuclide, Pj(), are calculated using X XZ 1 ci A1 j;i;k ðE ÞJk ðE; ÞdE ; ð1Þ Pj ðÞ ¼ NA i i k 0 where NA is Avogadro’s number, Ai is the mass number of the target element i, and ci is the concentration of i (g g1). The excitation function is j,i,k(E), and Jk(E, ) is the differential flux density of the projectile type k. In the present Sun the particles emitted from the solar surface and accelerated via magnetic fields to energies up to a few hundred MeV nucleon1 originate in either gradual (G-SEP) or impulsive (I-SEP) solar particle events. The G-SEP events typically have He/H and 3He/4He ratios similar to solar values and No. 1, 2003 COLLATERAL CONSEQUENCES OF NUCLEOSYNTHESIS are characterized by relatively high flux densities and moderately steep particle spectra. The I-SEP events are enriched in He and 3He relative to solar H and 4He, respectively. Besides these enrichments, the I-SEP events are characterized by relatively low flux densities and steep particle spectra. Today the G-SEP events contribute considerably more to the total fluence than I-SEP events. For modeling we assume that the SEP events from the early Sun were similar in their spectral shapes and their chemical compositions to those from the recent Sun. This means that we assume the projectiles to be a mixture of recent I-SEP and G-SEP events, both described by a power law in energy per nucleon, E, with ¼ 2:7 for impulsive and ¼ 4:0 for gradual events. However, to check the calculations for robustness we varied between 2.5 and 3.0 for I-SEP events and between 3.5 and 4.5 for G-SEP events. Since detailed information about the activity of the early Sun is lacking, we consider the relative contributions of G-SEP and I-SEP events to the total fluence as an adjustable parameter. The total fluence, however, is adjusted in a way that the modeled 10Be/9Be ratio fits the experimental data of 1 103 (see also discussion below). Note that our knowledge on the early Sun is so limited that we do not even know the origin of the SEP events in the YSO. For example, while in the present Sun G-SEP and I-SEP events originate at the solar surface, the X-wind model assumes particle acceleration within the so-called X-region, i.e., 0.06 AU away from the surface of the YSO (e.g., Shu, Shang, & Lee 1996; Lee et al. 1998; Ostriker & Shu 1995). In addition, an origin of SEP events near the accretion disk has been discussed (e.g., Feigelson et al. 2002). Therefore, the spectral shapes of the SEP events of the YSO might have been different from present-day I-SEP and G-SEP events. Since we have no information about the energy distribution of the particles accelerated in the various possible regions in the early solar system, we assume that the shapes of recent solar I-SEP and G-SEP events are reasonable approximations. The particle spectra are shown in Figure 1, and their parameters are compiled in Table 1. Fig. 1.—SEP spectra used for modeling. For the gradual solar particle events [solid line; JðEÞ / E 2:7 ] the spectral shapes were varied between E 2:5 and E 3:0 (shaded area). For the impulsive events [solid line; JðEÞ / E 4:0 ] spectral shapes were varied between E 3:5 and E 4:5 (shaded area). 607 TABLE 1 Parameters of the SEP Spectra Used for Modeling Parameter Impulsive Events Gradual Events Shape ..................... H/He ..................... He-3/He-4 ............. Weight ................... Fluence (cm2) ....... E2.7 10 1 1 9.95 1022 E4.0 300 4 104 1000 9.95 1022 The production rates calculated with equation (1) require for each product nuclide detailed excitation functions for all relevant target elements and all relevant projectile types. The model calculations are restricted to proton-, 3He-, and 4He-induced reactions. From meteorite studies it is known that SEPs produce few secondary neutrons within the target (e.g., Bodemann 1993; Neumann 1999; Rao et al. 1994). We therefore do not include neutron-induced reactions. Note that at the very beginning of the solar system (before deuterium is burned to 3He) 2H-induced reactions might also have been important. However, as long as information about possible deuterium flux densities and their temporal variations is lacking, adding 2H to the list of projectiles would mainly add another free parameter to the system. Therefore, 2H-induced reactions are not included here. Concerning the required cross section data, the situation is best for proton-induced reactions because of many years of effort modeling cosmogenic production rates in meteorites and the Moon (see, e.g., Leya et al. 2000, 2001). The proton excitation functions adopted here are the same as those used by Leya et al. (2000, 2001), Neumann (1999), and Michel & Neumann (1998). For some product nuclides, e.g., 92,91Nb, no measured proton-induced cross sections exist. For these target product combinations we have to rely on excitation functions determined using nuclear model codes. Here we use a Hauser-Feshbach approach in the programmed version GNASH-FKK (Young, Arthur, & Chadwick 1998). For 3He- and 4He-induced reactions, essentially no measured cross sections exist, and we have to rely exclusively on excitation functions determined using nuclear model codes. Again the cross section data are calculated on the basis of a Hauser-Feshbach model using the program GNASH-FKK. However, the predictive power of nuclear model codes is limited to within a factor of 2 at best (Michel & Nagel 1997). We therefore assume the calculated excitation functions for 3He- and 4He-induced reactions to be rather uncertain. In addition, the Hauser-Feshbach model is a statistical approach, and an accurate description of nuclear interactions in light target elements cannot be expected. In order to overcome some of these problems, the production rates by 3He- and 4He-induced reactions are not directly modeled. We instead calculate the excitation functions for proton-, 3He-, and 4He-induced reactions using the GNASHFKK code. From these data and using equation (1), the production rates Pp,GNASH, PHe3,GNASH, and PHe4,GNASH are modeled. From this the ratios PHe3,GNASH/Pp,GNASH and PHe4,GNASH/Pp,GNASH are calculated. We expect that the Hauser-Feshbach approach describes production rate ratios more accurately than absolute production rates. The final production rates used for further discussion, Pp,final, PHe3,final, and PHe4,final, are then determined by multiplying the modeled GNASH-FKK production rate ratios with the 608 LEYA, HALLIDAY, & WIELER TABLE 2 Target Elements Considered for Modeling the Production Rates of the Relatively Short-lived Radionuclides Isotope Target Elements Isotope Target Elements Be-7, 10 ............... C-14 .................... Na-22.................. Al-26................... Cl-36 ................... Ca-41 .................. Be, B, C, O O Na, Mg, Al, Si Mg, Al, Si K, Cl Ca Ti-44 ............ Mn-53, 54 .... Fe-60 ........... Ni-63............ Nb-91, 92 ..... Ca, Ti, Fe Mn, Fe, Ni Fe, Ni Ni, Cu Zr, Nb, Mo production rates due to protons, Pp,exp, determined using the best available proton cross sections (usually experimental values): Pp;final ¼ Pp;exp ; PHe3;GNASH PHe3;final ¼ Pp;exp ; Pp;GNASH PHe4;GNASH Pp;exp : PHe4;final ¼ Pp;GNASH ð2Þ However, for some reactions, e.g., 44Ti from Ca, production is possible by 3He- and 4He-induced reactions but not by protons. In those cases we have to assume PHe3;final ¼ PHe3;GNASH and PHe4;final ¼ PHe4;GNASH . The applied method reduces the uncertainties of the model calculations due to the limited knowledge of the excitation functions as far as possible. However, as long as experimental cross sections for 3He- and 4He-induced reactions are missing, we expect the uncertainties in the model calculations from the cross section data alone to be about a factor of 2. Table 2 summarizes the nuclear reactions and target elements considered in our study. Figure 2 shows as an example the cross sections for the production of 53Mn from iron. The symbols indicate experimental data for the proton-induced reaction (for references see Leya et al. 2000, 2001). The excitation functions given by lines are calculated Vol. 594 using the GNASH-FKK code with five different input parameter sets, i.e., different sets for the transmission coefficients (the variations of the five cross section data sets are smaller than the line thickness in Fig. 2). The production rates Pp,GNASH, PHe3,GNASH, and PHe4,GNASH are calculated using the average of the five results. 3. MODELED ISOTOPIC RATIOS In order to allow for a comparison of modeled and experimental data, we summarize in Table 3 the adopted solar system initial ratios that have been inferred from meteorites. Note that the value for the solar system initial 92Nb/93Nb has been a matter of some debate, being either 1 105 as given by Schönbächler et al. (2002) or 1 103 as measured by Münker et al. (2000). The finding of 7Li anomalies from live 7Be in the early solar system suggests, in the context of the local production scenario, very short timescales between nuclide production and crystallization of the early condensates. If true, we would expect isotopic anomalies from other relatively short-lived radionuclides as well. We therefore modeled also the collateral production rates for 14C, 22Na, 36Cl, 54Mn, 63Ni, and 91Nb. The nuclide 14C is included in our study because the radioactive decay (T1=2 ¼ 5730 yr) might lead to the production of excess 14N in carbon-rich early solar system condensates. Assuming that the irradiated material either had been degassed prior to or during the irradiation or that the refractory CAIs crystallized essentially noble gas free, the production of 22Na (T1=2 ¼ 2:603 yr) and 36Cl (T1=2 ¼ 0:3 Myr) would lead to the buildup of pure 22Ne (Ne-E) and 36Ar in early objects. Excess 44Ca and 54Cr in early solar system condensates correlated with Ti/Ca and Mn/Cr ratios would be expected if 44Ti (T1=2 ¼ 60:4 yr) and 54Mn (T 1=2 ¼ 312:2 yr) were alive in the early solar system. Excesses in 54Cr, which seem to be correlated to the excesses in 53Cr, have already been observed in meteorites (Shukolyukov & Lugmair 2001). In a recent study 63Cu excesses, which are suggested to be from the in situ decay of 63Ni (T 1=2 ¼ 100 yr), have been observed in carbonaceous and ordinary chondrites (Luck et al. 2003). Finally, if 92Nb were produced by spallation reactions in the early solar system, there would also be some collateral production of 91Nb (T1=2 ¼ 680 yr). Consequently, the isotopic excesses in 91Zr and 92Zr should be correlated. Since the relative production rates of 91Nb and 92Nb are independent of the chemical composition of the target, this radionuclide pair would be very useful to further test the local production scenario and would help to set time constraints on the formation of early solar system objects. 3.1. Uncertainties Fig. 2.—Excitation functions for the production of 53Mn from Fe. The open symbols are experimental data from thin target experiments. The results from theoretical model calculations for protons, 3He, and 4He are obtained using a Hauser-Feshbach approach in the programmed version GNASH-FKK. The uncertainties of the model calculations are difficult to estimate because of the large number of input data. A significant contribution to the overall uncertainty is from the cross section data, i.e., the missing of experimental cross sections for 3He- and 4He-induced reactions. As discussed in detail by Michel & Nagel (1997), the predictive power of cross section data derived from theoretical nuclear model codes is at best a factor of 2. However, using a statistical model like the Hauser-Feshbach approach makes the resulting uncertainties strongly dependent on the target mass number. For example, production rates of both 7Be and No. 1, 2003 COLLATERAL CONSEQUENCES OF NUCLEOSYNTHESIS 609 TABLE 3 Short-lived Radionuclides, Their Half-Lives, and Their Inferred Abundances in the Early Solar System Radioactive Isotope Half-Life Reference Isotope Solar System Initial Ratio Be-7 .............................. Be-10 ............................ C-14 .............................. Na-22............................ Al-26............................. Cl-36 ............................. Ca-41 ............................ Ti-44 ............................. Mn-53........................... Mn-54........................... Fe-60 ............................ 53.29 days 1.6 Myr 5730 yr 2.6 yr 0.716 Myr 0.3 Myr 0.1043 Myr 60.4 yr 3.7 Myr 312.2 days 1.5 Myr Be-9 Be-9 C-12 Na-23 Al-27 Cl-35 ... Ti-48 Mn-55 Mn-55 Fe-56 Ni-63............................. Nb-91............................ Nb-92............................ 100 yr 680 yr 36 Myr Ni-58 Nb-93 Nb-93 0.22 1 103 ... ... 5 105 106 1.5 108 ... 2 105 ... 4 109 >8 108 (1.1–3.5) 107 4 106 ... 105 103 Reference 1, 2 3, 4, 5, 6 7 8 9 10 11 12 13 14 15 16 References.—(1) Chaussidon et al. 2001; (2) Chaussidon et al. 2002; (3) McKeegan et al. 2000; (4) MacPherson & Huss 2001; (5) Sugiura et al. 2001; (6) Srinivasan 2002; (7) MacPherson et al. 1995; (8) Murty et al. 1997; (9) Srinivasan, Ulyanov, & Goswami 1994; (10) Lugmair & Shukolyukov 1998; (11) Shukolyukov & Lugmair 1993; (12) Mostefaoui et al. 2003; (13) Tachibana & Huss 2003; (14) Luck et al. 2003; (15) Schönbächler et al. 2002; (16) Münker et al. 2000. 10Be from oxygen by proton-induced reactions calculated using either experimental cross sections or GNASH-FKK results differ by about an order of magnitude. Fortunately, at higher masses the predictive power of the GNASH-FKK code is considerably higher. For example, the production rates for 22Na and 26Al from Al and Si derived from GNASH-FKK results differ by about a factor of 2 from the data calculated using experimental cross sections. For 53Mn and 55Mn the calculated excitation functions give production rates in reasonable agreement, i.e., to within 50%, with those derived from measured cross sections. However, despite the significant uncertainties in the excitation functions for 3He- and 4He-induced reactions, we estimate that the contribution of the cross sections to the total uncertainty should not be higher than about a factor of 2. This is because the procedure used to calculate the total production rates considerably reduces the uncertainties introduced by the GNASH-FKK cross section data. Additional uncertainties might arise from the fact that our approach neglects shielding effects and production of secondary particles in the target region. Assuming that the region where the magnetic field lines from the YSO were connected with the accretion disk was narrow and that the material now forming most of the CAIs and chondrules originated in this region, self-shielding of the material might have been significant. However, introducing shielding into the system will have two effects. First, shielding will lower the total flux densities of the SEP events. Since the total fluence is estimated by adjusting the modeled 10Be/9Be to the inferred solar system initial ratio of 103, shielding mostly changes the particle fluence but only slightly affects the modeled relative proportions of the various nuclides, e.g., the 26Al/41Ca ratio. Second, shielding effects change the shapes of the projectile spectra; i.e., the spectra become harder. This in turn affects the calculated production rates. However, the effect is similar for reactions with similar threshold energies, and the relative proportions of the production rates are only slightly changed. To summarize, shielding effects are neglected in the present version of the model calculations because we expect them to be only of minor importance and because their consideration would add another free parameter to the system. One of the major uncertainties arises from the fact that the starting chemical composition of the irradiated material (we assume that in the very beginning of the solar system everything started with solar chemical composition) and its possible chemical evolution with time are not well constrained. Throughout this paper we assume that the irradiated target material (the proto-CAI material) initially had solar chemical composition. During the irradiation the composition might eventually change to the refractory composition of the present-day CAIs, but it is unclear if and when this change happened. We have taken this uncertainty into account by modeling the solar system initial ratios of the relatively short-lived radionuclide also for present-day CAI composition. We expect that the values inferred from meteorites should lie somewhere between both hypothetical end-members. Unfortunately, the abundances of some crucial elements in the refractory end-member are not well constrained since few data exist for bulk CAI chemistry. We adopt values from the following sources: Be (Chaussidon et al. 2001, 2002; Phinney, Whitehead, & Anderson 1979), B (Chaussidon et al. 2001, 2002; McKeegan et al. 2000), Mg, Al, Si, Ca, and Ti (Simon et al. 2002), Na, K, and Cr (Srinivasan, Huss, & Wasserburg 2000), Mn (Shukolyukov & Lugmair 2001), and Fe (Bischoff 1976; Grossmann & Ganaphaty 1976). Since no data for Ni and Cu were found, we assume that the Ni/Fe and Cu/Fe ratios are unaffected by the chemical alteration, an assumption that is not critical for 53,55Mn because their production from Ni is only minor. 610 LEYA, HALLIDAY, & WIELER Vol. 594 TABLE 4 Chemical Composition (g g1) Assumed for Modeling Element Solar CAI Element Solar CAI Be ............... B ................. C................. N ................ O................. Na............... Mg .............. Al................ Si ................ Cl................ K ................ 2.64 108 8.70 107 3.45 102 3.18 106 5.21 101 5.00 103 9.89 102 8.86 103 1.06 101 7.04 104 5.58 104 2.37 107 9.93 107 3.45 102 1.00 106 3.00 101 1.03 103 7.12 102 1.75 101 1.26 101 ... 1.12 104 Ca ............... Ti ................ Mn.............. Cr ............... Fe ............... Ni ............... Cu............... Zr................ Nb .............. Mo.............. 9.28 103 4.36 104 1.99 103 2.66 103 1.90 101 1.90 102 1.26 104 3.94 106 2.46 107 9.28 107 1.87 101 1.19 102 2.08 104 3.50 104 8.48 102 8.48 103 1.26 105 5.80 105 3.76 106 1.39 105 For 63Ni, however, this assumption significantly increases the uncertainty of the modeled solar system initial 63Ni/58Ni. The C concentration is assumed to be unaffected by the chemical evolution of the target, which is a critical assumption for calculating the solar system initial 14C/12C and the expected isotopic shifts in N; the (14N/15N) values given for present-day CAI composition are only rough estimates. The concentrations for Zr and Nb are given by Kornacki & Fegley (1986). Since we found no data for Mo, we simply assume Mo to be enriched relative to solar by the same factor as Zr and Nb. Again, this assumption is not crucial, since Mo contributes only very little to the production of 91,92Nb. The chemical compositions used for modeling are compiled in Table 4. To summarize, a major part of the total uncertainties is attributable to the excitation functions and the chemical composition of the refractory end-member. Considering all possible contributions to the overall uncertainties, we estimate the total uncertainty of the modeled solar system initial ratios to be about a factor of 10. The relative production rates for similar target product combinations, e.g., 7Be/9Be relative to 10Be/9B and 53Mn/55Mn relative to 54Mn/55Mn, should be more accurate, i.e., about a factor of 2. However, since the experimental data inferred from meteorites often vary substantially, the uncertainties of 1 order of magnitude and a factor of 2 for the modeled absolute and relative production rates, respectively, do not restrict the major statements given below. ferent in the YSO compared to the recent Sun, by treating the ratio G-SEP/I-SEP as a free parameter. The results are compiled in Table 5, where we distinguish between two irradiation scenarios. In the first scenario (second and third columns), we assume an irradiation time short enough to neglect saturation effects for the production of any radionuclide considered. In the second (fourth and fifth columns), an irradiation time of about 1 Myr is assumed, and saturation of the isotopes is taken into account. For further discussion see x 4. Some of the modeled results for the first scenario (no saturation) are plotted in Figure 3. Figure 3a depicts the ratio of modeled to inferred solar system initial ratios for 10Be/9Be (1, because of the normalization), 26Al/27Al, 41Ca/40Ca, and 53Mn/55Mn as a function of the ratio G-SEP/I-SEP assuming solar composition for the target. In such a plot an ordinate value of 1 indicates perfect agreement of experimental and modeled solar system initial ratios. Figure 3b depicts the results for targets having CAI composition throughout the irradiation. To adjust the fluence ratios G-SEP/I-SEP, we consider only 10Be, 26Al, 41Ca, and 53Mn because the inferred solar system initial for TABLE 5 Modeled Solar System Initial Ratios for the Relatively Short-lived Radionuclides for Targets Having Solar or Present-Day CAI Composition Without Saturation 3.2. Modeling the Solar System Initial Ratios 7 Be=9 Be, 10 Be=9 Be, 26 Al=27 Al, 41 Ca=40 Ca, 53 Mn=55 Mn, and 60 Fe=56 Fe For modeling the solar system initial ratios, the shape of the particle spectra and their chemical composition, as well as the fluence ratio of G-SEP to I-SEP events, have to be assumed. The spectral shapes and the 3He/4He and H/He ratios of G-SEP and I-SEP are summarized in Table 1. The data are compiled from the results given by Gosling (1993), Miller (1998), Mason, Mazur, & Dwyler (1999), Mason, Dwyler, & Mazur (2000), and Reames et al. (1997). Note that adopting these data from recent SEP events implies that we assume that the energy distribution of the emitted particles as well as the chemical composition of the SEP events did not change during the evolution of the Sun. However, we do allow for the possibility that the relative fluence contributions of G-SEP and I-SEP events were significantly dif- Ratio 10Be/9Be .......... .......... 14C/12C ............ 22Na/23Na........ 26Al/27Al.......... 36Cl/35Cl .......... 41Ca/40Ca ........ 44Ti/48Ti .......... 53Mn/55Mn ...... 54Mn/53Mn ...... 60Fe/56Fe ......... 63Ni/58Ni ......... 92Nb/93Nb ....... 91Nb/92Nb ....... 7Be/10Be Tirr ¼ 1 Myr Solar CAI Solar CAI 1.0 103 ! 70 2.0 108 1.4 105 1.2 105 1.3 104 1.5 107 1.5 108 6.5 105 0.20 3.0 1012 2.5 109 1.3 104 0.70 1 103 ! 70 1.5 107 6.4 104 1.7 105 ... 1.9 106 1.5 107 3.7 103 0.16 4.0 1011 6.3 1010 1.7 103 0.70 1.0 103 ! 1.8 105 1.0 1010 6.3 1011 1.0 105 4.8 105 2.6 108 1.2 1013 7.0 105 1.9 107 2.8 1012 2.9 1012 1.6 104 1.1 107 1.0 103 ! 1.8 105 7.5 109 2.9 109 1.4 105 ... 3.3 107 1.2 1012 4.0 103 1.5 107 3.7 1011 7.4 1013 2.1 103 1.1 107 Note.—Two irradiation scenarios, a short-term irradiation without any saturation effects and an irradiation lasting about 1 Myr, are distinguished. No. 1, 2003 COLLATERAL CONSEQUENCES OF NUCLEOSYNTHESIS Fig. 3.—Ratio of modeled and measured solar system initial ratios for and 53Mn/55Mn as a function of the ratio gradual/ impulsive solar particle events for the YSO. The shaded area ranging from 0.1 to 10 indicates the uncertainties expected for the model calculations. (a) Results for targets with solar chemical composition. Assuming a ratio of gradual to impulsive solar particle events of >1000 enables us to simultaneously describe the solar system abundances of 10Be, 26Al, 41Ca, and 53Mn. (b) Results for targets with present-day CAI composition. It can be seen that a simultaneous description of the solar system initial abundances is not possible. 26Al/27Al, 41Ca/40Ca, 92Nb/93Nb is still under debate and 60Fe cannot be explained by local production only (see below). Figure 3a demonstrates that the model simultaneously describes the inferred solar system initial abundances for 10Be, 26Al, 41Ca, and 53Mn within a factor of 10, i.e., within the uncertainties expected for the model calculations, if the ratio G-SEP/I-SEP is assumed to be greater than 1000 and if the chemical composition of the irradiated material is assumed to be solar during the entire irradiation. In contrast, if one assumes present-day CAI compositions for the irradiated target, the model fails to simultaneously describe the solar system initial abundances of 10Be, 26Al, 41Ca, and 53Mn (Fig. 3b). Assuming again G-SEP/I-SEP ¼ 1000 would bring 10Be/9Be and 26Al/27Al in concordance, i.e., within a factor of 3, but 41Ca and 53Mn would be overproduced by the model by factors of 130 and 190, respectively. The differences can entirely be explained by the differences between solar and present-day CAI chemistry. For example, Be in CAIs is enriched relative to solar by a factor of 10. Since the concentration of oxygen, which is the main target element for 7,10Be production, is very similar for solar and 611 present-day CAI chemistry, the total fluence needed to produce 10Be/9Be ¼ 103 is also 10 times higher for material with present-day CAI chemistry than for material having solar composition. The 10 times higher fluence then again brings measured and modeled 26Al/27Al in concordance. The concentration of Si, which is the main target element for 26Al production, does not vary substantially between solar and CAI chemistry. Therefore, the 10 times higher fluence leads to a corresponding increase in the 26Al production rate by about a factor of 10. Since Al is enriched in CAIs relative to solar by about 1 order of magnitude, the modeled 26Al/27Al still is close to the inferred solar system initial ratio. In contrast, since the Fe/Mn ratio in CAIs is about 4 times higher than solar and 53Mn production is dominated by reactions on Fe, the 10 times higher fluence leads to a 53Mn/55Mn ratio in CAIs about 40 times higher than those modeled for solar chemical composition. The production of 41Ca is dominated by reactions on Ca, and increasing the fluence by a factor of 10 directly increases the modeled solar system initial 41Ca/40Ca by the same factor of 10. To summarize, assuming solar chemical composition for the irradiated target, a fluence ratio G-SEP/I-SEP of 1000, and energy spectra as well as the relative proportions of protons, 3He, and 4He in the SEPs that are identical to those in present-day SEP events permits for the first time a simultaneous description of the solar system initial abundances of 10Be, 26Al, 41Ca, and 53Mn in the framework of local production. In addition, the model gives a solar system initial 7Be/10Be of 70, in reasonable agreement with the experimental result of 230 130 given by Chaussidon et al. (2002). The 7Be/10Be ratio is of great importance because it is nearly independent of the chemical composition of the target and can therefore be used to test the projectile spectra used for modeling. In contrast, if one assumes present-day CAI compositions for the irradiated material, the result is an overproduction of 41Ca and 53Mn relative to 10Be and 26Al by more than 2 orders of magnitude. Therefore, in the framework of the local production scenario all radionuclides considered so far must have been mostly produced while the irradiated proto-CAI material maintained a solar composition or, more exactly, had solar O/Be and Si/Al ratios. The change to the more refractory CAI composition had to occur after irradiation ended. The broad range of half-lives of the radionuclides, from 53 days for 7Be up to 36 Myr for 92Nb, permits stringent constraints on the CAI production scenario and its timing. A discussion of a possible CAI formation scenario is given in x 4. An important result therefore is that the target material must have had solar chemical composition throughout the irradiation, and we have to answer the question of how the target material becomes refractory. This is discussed in x 4. If one assumes a solar composition for the irradiated material, the calculated solar system initial 92Nb/93Nb is 1:3 104 . This is an order of magnitude higher than the ratio given by Schönbächler et al. (2002) and an order of magnitude lower than the value presented by Münker et al. (2000). Hence, the modeled ratio agrees with both estimates to within a factor of 10, which is within the uncertainties expected for the model calculations. Note that the 92Nb production rates are exclusively based on theoretically derived input data; i.e., there are no experimental cross sections available for the production of 92Nb. For this reason and because the calculated ratio lies in between both 612 LEYA, HALLIDAY, & WIELER experimental data sets, the model does not provide a constraint on which of the initial ratios inferred by Schönbächler et al. (2002) and Münker et al. (2000) is correct. However, we can conclude that the existence of 92Nb in the early solar system is not necessarily proof for p-process nucleosynthesis shortly before the formation of the solar system. The 92Nb data can be explained by spallation reactions on Nb (with small contributions from Zr and Mo). Whether the internal production scenario can also explain some of the other neutron-poor nuclides needs further study. There are discrepancies between modeled and inferred values of the solar system initial 60Fe/56Fe, a feature already observed in earlier studies (Lee et al. 1998; Gounelle et al. 2001). The model underestimates the initial 60Fe abundance inferred by Shukolyukov & Lugmair (1993) from achondrites by more than 3 and 2 orders of magnitude, respectively, assuming either solar or present-day CAI composition. In general, the production of neutron-rich isotopes by spallation reactions is very inefficient. Therefore, the occurrence of the neutron-rich isotopes 60Fe and 182Hf requires another production mechanism. The existence of 60Fe may therefore indicate r-process nucleosynthesis with subsequent injection of material into the collapsing solar nebula. However, Wasserburg, Gallino, & Busso (1998) concluded that if a supernova is the source of the 26Al in the solar system, then the initial 60Fe/56Fe would be in the range of 3 107 to 1 105 , at least 2 orders of magnitude above the achondrite value (4 109 ; Shukolyukov & Lugmair 1993). However, from analyses of chondrites two groups recently reported evidence for a much higher solar system initial 60Fe/56Fe ratio (Tachibana & Huss 2003; Mostefaoui et al. 2003). The new values of ð1 7Þ 107 are at the lower end of the range proposed by Wasserburg et al. (1998). If confirmed, the new 60Fe data would also provide support for a nucleosynthetic origin of 26Al and hence would require the reassessment of the spallogenic origin of some of the isotopes explained here. 3.3. Early Solar System Production of 14 C, 22 Na, 36 Cl, 44 Ti, 54 Mn, 63 Ni, and 91 Nb In the previous section it was demonstrated that our model calculations allow for a consistent description of the abundances of most of the relatively short-lived radionuclides whose presence in the early solar system is established. In the framework of the local production scenario, production by spallation is also expected for other radioactive and stable nuclides. Here we discuss the radioactive isotopes 14C, 22Na, 36Cl, 44Ti, 54Mn, 63Ni, and 91Nb. Our interest in these radionuclides is motivated by the recent hint of live 7Be in the early solar system in one CAI (Chaussidon et al. 2001, 2002). If the timescale for nuclide production and CAI crystallization was short enough to allow for measurable isotopic anomalies due to the radioactive decay of 7Be, we might expect to see effects from other very short-lived radionuclides as well. Here we discuss the expected abundances of 14C, 22Na, 36Cl, 44Ti, 54Mn, 63Ni, and 91Nb for particle fluences leading to 10Be/9Be ¼ 103 . Note that saturation effects are neglected for all isotopes discussed in this section. If saturation effects were added, the radionuclide abundances would decrease. Therefore, the values given below are upper limits. The modeled 14C/12C in the early solar system is 2 108 . Note that 14C production is entirely by spalla- Vol. 594 tion reactions on oxygen. With a solar O/C ratio of 15, this results in a total of 3:4 1013 g1 14C atoms at the end of the irradiation. If one assumes that the crystallization of the material occurred fast, i.e., that the decay of 14C to 14N occurred entirely in already crystallized material, it would result in ð14N/15NÞ 0:27G for samples with a solar nitrogen concentration of 3 ppm, an effect too low to be detected. To make the discussion more realistic, we assume that the CAIs crystallized essentially free of nitrogen, but we consider typical present-day nitrogen blanks. If we assume a blank level similar to that obtained in a recent study of N2 in single lunar grains, about 1 pmol (Hashizume, Marty, & Wieler 2002), a radiogenic signal of 100G would require 3 1013 isotopes of 14C, which can be translated into 1:5 1021 isotopes of the stable 12C using the modeled solar system initial 12C/14C. Therefore, only 30 mg carbon is needed to produce an isotopic shift of ð14N/15NÞ 100G in material originally free of nitrogen (except for the blank contribution). Note that 7,10Be and 14C are produced by spallation reactions on oxygen. Hence, the isotopic effects produced by the radioactive decay of 7,10Be and 14C should correlate. Therefore, it might be of interest to search in early solar system condensates for 7Li and 10Be enrichments correlated with high 14N/15N. For the solar system initial 22Na/23Na, the model yields 1:5 105 . With a solar Na concentration of 5000 ppm (Table 4), this would lead to a 22Ne concentration of 3 107 cm3 STP g1. This is very much larger than the concentrations found in early solar system condensates. However, whether CAIs contain any trapped Ne is unclear. Whereas Shukolyukov et al. (2001) and Russell et al. (1998) interpret 21Ne/22Ne ratios in an Efremofka and Vigarano CAI, respectively, as possible evidence for the presence of Ne-E, Vogel et al. (2003) showed that Ne in several CAIs can entirely be explained by cosmogenic contributions from Na- and Al-rich minerals. However, the absence of Ne-E does not necessarily allow rejecting a local production scenario, because the absence of formerly present Ne-E can be explained either by Na losses during the irradiation (together with thermally induced losses of other volatile elements) or by noble gas losses during or after irradiation. The latter possibility is indicated by the fact that CAIs are also completely devoid of trapped Ne-HL or Ne-Q (Vogel et al. 2003). Note that Na in CAIs typically is of secondary origin and therefore cannot be used to estimate the expected amount of Ne-E. Note also that Ne-E in meteorites known to be from presolar grains is thought to be nucleosynthetic (e.g., Nichols et al. 2002). The solar system initial 36Cl/35Cl is modeled as 1:3 104 , about 2 orders of magnitude higher than the value of 1 106 reported by Murty, Goswami, & Shukolyukov (1997). As in the case of the ‘‘ missing ’’ Ne-E in early solar system condensates, this discrepancy might also be explained by volatile losses during or after the irradiation. For the solar system initial 44Ti/48Ti, the model gives 1:5 108 . Taking into account the large overabundance of Ca relative to Ti in samples having a solar composition as well as in refractory inclusions, any expected anomalies in 44Ca from the radioactive decay of 44Ti are below presentday analytical precision. For example, assuming solar composition of the target, the expected anomaly in 44Ca/40Ca is less than 30 ppb. This is too low to be detected. If we turn this argument around, to end up with No. 1, 2003 COLLATERAL CONSEQUENCES OF NUCLEOSYNTHESIS ð44Ca/40CaÞ ¼ 2 (where 1 is the isotopic shift of the sample relative to a standard in units of 104), which can be detected with present-day analytical techniques, the sample must have a Ti/Ca ratio 104 times higher than solar. The modeled solar system initial 54Mn/55Mn is 1:3 105 , i.e., about 5 times lower than the modeled initial 53Mn/55Mn. Considering the isotopic abundances of the daughter isotopes 53Cr and 54Cr of 9.5% and 2.36%, respectively, the expected (54Cr) should therefore be about the same as (53Cr). In contrast, the experimental data from carbonaceous chondrites suggest (54Cr) values about 4 times higher than (53Cr) (Shukolyukov & Lugmair 2001). Note that the model calculations predict the relative proportions of the 53Mn and 54Mn production rates to within a factor of about 2, because a large part of the uncertainty cancels out when production rate ratios of products from the same target element are considered. Therefore, the observed difference of a factor of 4 is not expected to be only an artifact of the model calculations. In a recent study on carbonaceous and ordinary chondrites, Luck et al. (2003) found excess 63Cu, which they suggested to be from the in situ decay of refractory 63Ni. From their Figure 6 the solar system initial 63Ni/58Ni can be estimated to be 4 106 , about 3 orders of magnitude higher than our modeled results of 2 109 . Despite the fact that the cross sections for the production of 63Ni from Ni and Cu are entirely based on theoretical model calculations, the observed discrepancy of a factor of 1000 cannot be explained as an artifact of the model calculations. Further, the half-life of 63Ni (T1=2 ¼ 100 yr) makes stellar production scenarios with subsequent injection into the forming solar system highly unlikely. A possibility to explain the existence of live 63Ni is CAI production in a supernova envelope, as recently proposed by Cameron (2003). However, this scenario has difficulties explaining the rather ‘‘ normal ’’ isotopic composition of CAIs relative to accepted presolar grain values. For the solar system initial 91Nb/93Nb, the model gives 9 105 , i.e., 40% lower than the modeled 92Nb/93Nb ratio. Considering the isotopic abundances of 91Zr and 92Zr, the expected (91Zr) should be close to the reported (92Zr). Unfortunately, the present data (Schönbächler et al. 2002) are too uncertain to show any trend. Therefore, further tests of the internal production scenario require more precise isotopic data for 91Zr and 92Zr in early solar system condensates. To summarize, besides the established radionuclides discussed in the previous section, we also modeled the expected solar system initial ratios 14C/12C, 22Na/23Na, 36Cl/35Cl, 54Mn/55Mn, 63Ni/58Ni, and 91Nb/93Nb. The main motivation for this additional modeling was the search for expected collateral isotopic shifts, which might help to further test the local production scenario and possibly to gain new information about the time constraints on the CAI production scenario. Unfortunately, some of the predicted isotopic anomalies might have been eradicated, e.g., 22Ne and 36Ar, whereas others are too low to be detected, e.g., 44Ti and 91Nb. Only 14C, 54Mn, and 63Ni might be useful candidates to test the local production scenario. However, for 54Mn and 63Ni, the model results fall short by about a factor of 4 and 1000, respectively. Whether these differences indicate that most of the relatively short-lived radionuclides were not produced within the early solar system deserves further study. 613 4. A SCENARIO FOR CAI PRODUCTION IN THE FRAMEWORK OF THE X-WIND MODEL Here we discuss the consequences for CAI production if some of the short-lived radionuclides were produced by energetic particles from the young Sun according to the results derived in the previous section. In the following, CAI production is considered in the framework of the X-wind model only (e.g., Ostriker & Shu 1995; Shu et al. 1996; Lee et al. 1998). One of the major challenges for a local production scenario is the experimental finding that the solar system initial ratios in different samples show only modest variations. For example, the initial 10Be/9Be measured so far in 16 CAIs varies by less than a factor of 4 (McKeegan et al. 2000; Chaussidon et al. 2001; MacPherson & Huss 2001; Sugiura et al. 2001; Srinivasan 2002), and the initial 26Al/27Al in many CAIs falls close to the so-called canonical value of 5 105 (MacPherson, Davis, & Zinner 1995). This requires that the material now forming a large part of the CAIs has seen a surprisingly homogeneous projectile fluence, despite a probably variable solar particle flux and variable irradiation times and shielding conditions. In addition, the concordance of measured and modeled ratios for nuclides with different half-lives can only be explained in scenarios in which the time gap between the end of the irradiation and the crystallization is comparable with the half-life of the shortest lived radionuclide considered. Based on the results here, a CAI production scenario in the framework of the X-wind model must fulfill the following requirements: (1) the irradiated material must have had solar composition throughout the irradiation, (2) the irradiation of the material must have been very homogeneous, and (3) the refractory CAIs must have crystallized out of this homogeneously irradiated material on timescales comparable to the shortest half-life of the radionuclides considered. A possible straightforward explanation is to assume that the irradiation occurred on a gas with solar composition and that the refractory CAIs crystallized out of this gas directly after the irradiation. Such a scenario is sketched in Figure 4. A gaseous target naturally results in a homogeneous irradiation because convection and/or turbulent mixing of a gas near a YSO and/or in the X-region should be very common. A further advantage of a gaseous target might be that the chemical composition of the total gas is not expected to change during the irradiation and/or heating events as long as the gas is considered as a closed system. After the irradiation, the gas was either shielded from the young Sun or ejected from the X-region by the X-winds and subsequently injected into the accretion disk at planetary distances. The CAIs crystallized out of this homogeneously irradiated gas on timescales shorter than or at least comparable to the half-life of the shortest lived radionuclide considered. In this scenario, the irradiation time is a crucial parameter because radioactive saturation of the isotopes affects the relative proportions of the modeled solar system initial ratios. Figure 5 shows the ratio of modeled to inferred solar system initial abundances as a function of the irradiation time. The calculations are adjusted such that the modeled 10Be/9Be equals 1 103 (1 in the figure). Figure 5 demonstrates that the concordance of measured and modeled solar system initial abundances for 10Be, 26Al, 41Ca, 53Mn, and 92Nb holds for irradiation times of up to about 1 Myr. Longer irradiation times lead to lower relative proportions of the radionuclides with shorter half-lives. For 614 LEYA, HALLIDAY, & WIELER Vol. 594 Fig. 4.—Production scenario explaining the concordance of spallogenic 7,10Be, 26Al, 41Ca, 53Mn, and 92Nb. A gaseous target with solar chemical composition is homogeneously irradiated in the X-region. After up to 1 Myr of irradiation, the material is ejected from the X-region and/or shielded from the SEPs. Finally, the material is ejected by the X-wind and transported to planetary distances. The refractory CAIs crystallized out of this homogeneously irradiated material. example, 41Ca reaches 87.5% saturation after about 300 kyr, whereas the level of 87.5% saturation for 10Be and 53Mn is reached after 4.8 and 11.1 Myr, respectively. Consequently, the 41Ca abundance monotonically decreases relative to those of 10Be and 53Mn. Concerning the latter two nuclides, the amount of 53Mn relative to 10Be increases for irradiation times larger than 1 Myr, when 10Be is near its saturation level but the amount of 53Mn still increases. However, the time constraints become much more stringent if 7Be is added to the list of radionuclides alive in the early solar system. For CAIs that crystallized with 7Be/10Be 100, the irradiation time must have been shorter than about 1 yr to avoid radioactive saturation of 7Be relative to 10Be. From Figure 5 we conclude that, in the framework of the local production scenario, most of the material now forming the CAIs was homogeneously irradiated over timescales not considerably Fig. 5.—Ratio of modeled to measured solar system initial values for and 92Nb/93Nb as a function of the irradiation time. Because of their different half-lives, ranging from 53 days for 7Be up to 36 Myr for 92Nb, the relative proportions of the nuclide abundances significantly depend on the length of the irradiation. From this picture we conclude that irradiation times of up to 1 Myr are possible for most of the CAIs but that in some rare occasions a high flux density lasting no longer than about 1 yr leads to the formation of 7Be/10Be 100. 10Be/9Be, 26Al/27Al, 41Ca/40Ca, 53Mn/55Mn, more than about 1 Myr. Some material, that from which CAIs with evidence for 7Be crystallized, received flux densities about a factor of 106 times higher than the average, during short times of less than 1 yr, however. Note that in this hypothetical scenario a homogeneous irradiation is accomplished because of two factors. First, a gaseous target is assumed, which enables efficient mixing by convection and/or turbulent mixing during the irradiation. This should result in a homogeneous irradiation even if the projectile spectra have varied during the irradiation. Second, the X-wind model assumes that the SEP events leading to nuclide production have been produced within the X-region itself, i.e., that the projectiles were accelerated in the same region where the irradiation occurred (e.g., Russell et al. 2001), which again should naturally result in a homogeneous irradiation of the material within the X-region. To summarize, we conclude that for the local production scenario to be correct, the irradiated material that formed most of the CAIs was gaseous, with solar composition throughout the irradiation. The irradiation would need to have lasted not considerably more than about 1 Myr. Such CAIs could have crystallized with live 10Be, 26Al, 41Ca, 53Mn, and 92Nb at levels now inferred from meteorite studies. The modeled 7Be/10Be of about 105 would not allow a detection of any 7Li anomalies correlated to the beryllium concentration. However, if some of the material was irradiated by high-flux SEP events, which lasted no longer than about 1 yr, the CAIs would crystallize with 7Be/10Be of about 100 and 10Be, 26Al, 41Ca, 53Mn, and 92Nb concentrations close to their inferred solar system initial ratios. In both cases the irradiation would need to have been very homogeneous, possibly because on one hand the irradiated material was gaseous, which allows efficient mixing during the irradiation, and on the other hand the SEP events originated at the same place where the irradiation occurred, i.e., in the X-region. After the irradiation the material would need to have been ejected from the irradiation area and/or shielded from the SEPs. The irradiated material would have rapidly condensed, and the solar system initial abundances would have been frozen into the earliest refractory condensates. No. 1, 2003 COLLATERAL CONSEQUENCES OF NUCLEOSYNTHESIS 5. CONSEQUENCES FOR THE PROPOSED CAI PRODUCTION SCENARIO In the following we distinguish between two widely different irradiation lengths. First, we assume a short-term irradiation with a high flux density, which lasts less than about 1 yr. As pointed out above, such a short irradiation time is required to produce not only 10Be, 26Al, 41Ca, 53Mn, and 92Nb but also 7Be/10Be in their inferred solar system initial proportions. Second, we assume an irradiation time of 1 Myr, which explains 10Be, 26Al, 41Ca, 53Mn, and 92Nb but neglects the evidence of live 7Be in one Allende CAI, since the modeled initial 7Be/10Be will be too low by about 7 orders of magnitude. Comparing the flux densities needed to produce the short-lived radionuclides with flux densities of SEPs from the present Sun is a further test of the local production scenario. The total flux density, J(E), for the 1 yr and 1 Myr scenarios is 1016 and 1010 cm2 s1, respectively. In the literature, solar particle flux densities are usually given only for particles with energies above 10 MeV, J(E > 10 MeV). The values needed for successful modeling are then JðE > 10 MeVÞ 2 1012 and 2 106 cm2 s1 for the 1 yr and 1 Myr scenarios, respectively [assuming JðEÞ / E 2:7 and JðEÞ / E 4:0 for gradual and impulsive events, respectively]. The long-term average flux density for the present Sun is 102 cm2 s1 (Reedy 1977, 2002). With the 105-fold enhanced flux densities in YSOs compared to the present Sun (Feigelson et al. 2002), this results in JðE > 10 MeVÞ 107 cm2 s1 for the young Sun, in concordance with our modeled estimate for the 1 Myr scenario. Therefore, assuming an X-wind scenario and flux densities 105 times higher than for the present Sun according to observations naturally results in 10Be/9Be, 26Al/27Al, 41Ca/40Ca, 53Mn/55Mn, and 92Nb/93Nb ratios close to the values inferred from meteorites for the early solar system. However, assuming on the other hand an irradiation time of only 1 yr requires flux densities about 10 orders of magnitude above the average present-day value or about 5 orders of magnitude above the values for YSOs reported by Feigelson et al. (2002). Therefore, for proper modeling of the solar system initial 7Be/10Be, a further short-term increase of the flux of about 5 orders of magnitude is needed. Individual solar flares in the present Sun may have flux densities about 3 orders of magnitude higher than the long-term average. Possibly, the material from which the Allende CAI with hints for live 7Be crystallized has been irradiated in such a hypothetical early ultra–high-flux SEP event. Further, the flux given for the present Sun is for 4. In the X-wind scenario the region of SEP production and particle acceleration is not yet clear, but the SEP events in the early Sun need not necessarily have been isotropic. Magnetic focusing of SEP events to small emission angles also increases the flux densities and might enable simultaneous modeling of the production of 10Be, 26Al, 41Ca, 53Mn, 92Nb, and 7Be close to the inferred solar system initial values. To conclude, if we assume in the framework of the local production scenario that most of the material now forming the CAIs has been irradiated not substantially longer than about 1 Myr by low flux density events, CAIs could crystallize with 10Be, 26Al, 41Ca, 53Mn, and 92Nb abundances close to the values inferred from meteorites for the early solar system. However, the 7Be/10Be in those CAIs would be too low to produce detectable shifts in 7Li/6Li. This argument also 615 holds for 14C, 22Na, 44Ti, 54Mn, 63Ni, and 91Nb. Therefore, if the evidence for 7Be is substantiated, there must also have been some short-term SEP events with 105 times higher flux densities by which 7Be at levels 7Be/10Be 100 could have been produced. 6. CONCLUSIONS AND OUTLOOK We present new model calculations for the production of the relatively short-lived radionuclides 7Be, 10Be, 14C, 22Na, 36Cl, 44Ti, 41Ca, 53Mn, 60Fe, 63Ni, 92Nb, and 93Nb by spallation reactions in the early solar system. By assuming that the particle spectra produced by YSOs were similar to those emitted from the present Sun, we can for the first time simultaneously model the solar system initial ratios 10Be/9Be, 26Al/27Al, 41Ca/40Ca, 53Mn/55Mn, and 92Nb/93Nb. The concordance of measured and modeled solar system initial ratios provides stringent constraints on possible CAI production mechanisms in the framework of a local production scenario. A major challenge for any such scenario is to explain the quite similar 26Al/27Al and 10Be/9Be ratios in many different CAIs. This experimental finding requires that the material now forming most of the CAIs has experienced surprisingly homogeneous particle fluences, despite probable variable flux densities, irradiation times, and shielding conditions. By combining the requirement for a homogeneous irradiation with a major result obtained by our model calculations, that the target must have solar composition throughout the irradiation, we present a possible CAI production scenario. In this model a gaseous target with solar chemical composition is irradiated. Convection and/or turbulent mixing in the target results in a homogeneous irradiation of the material. After an exposure time of up to 1 Myr for most of the material, the CAIs crystallized with 10Be, 26Al, 41Ca, 53Mn, and 92Nb abundances close to the values inferred for the early solar system. However, the 7Be/10Be ratios in those CAIs would be too low by about 7 orders of magnitude compared to meteorite data. Therefore, we have to assume that some material must have been irradiated with flux densities about 105 times higher than the early solar system average on timescales of less than about 1 yr. Finally, the flux densities needed for modeling are in both cases within the physically reasonable ranges of YSOs. Besides the established short-lived radionuclides 10Be, 26Al, 41Ca, 53Mn, and 92Nb, we also present initial abundances for 14C, 22Na, 44Ti, 36Cl, 54Mn, 63Ni, and 91Nb. While the modeled solar system initial 14C/12C would lead to permil effects in nitrogen in early solar system carbon-rich condensates, the isotopic anomalies resulting from the decay of 44Ti are much smaller than present-day analytical precision. The modeled solar system initial 22Na/23Na and 36Cl/35Cl would result in easily measurable 22Ne and 36Ar concentrations. Since so far such large amounts of pure 22Ne and 36Ar have not been observed in CAIs, most of the gas produced by early spallation must have been lost by diffusion, if ever present. Unfortunately, the modeled solar system initial 91Nb/93Nb is too low to produce detectable isotopic anomalies in 91Zr. The modeled 60Fe/56Fe falls short by at least 3 orders of magnitude and, according to very recent data, by even about 6 orders of magnitude. From this one can conclude that an external source, e.g., a supernova, is necessary for some of the neutron-rich short-lived radionuclides, e.g., 60Fe and 182Hf. Even more importantly, if a supernova is the 616 LEYA, HALLIDAY, & WIELER source for the 60Fe, the injected material would have a 26Al/60Fe ratio close to the range now inferred for the early solar system (Tachibana & Huss 2003; Mostefaoui et al. 2003). Therefore, if the new value for the solar system initial 60Fe/56Fe is correct, this supports a triggered supernova source for both isotopes. Consequently, a reevaluation of the origin of the other relatively short-lived radionuclides, in particular 26Al, would then be necessary. Some major discrepancies exist for 54Mn and 63Ni. For 54Mn the model predicts (54Cr)/(53Cr) ratios of about unity, which is 4 times lower than some published values. Furthermore, for 63Ni the model gives a solar system initial abundance about 103 times lower than recently inferred from Cu isotope data. It is not clear if these discrepancies indicate that the local production scenario is not an appropriate and/or sole scenario for the origin of the relatively short-lived radionuclides in the early solar system. This deserves further study. This work was supported by the Swiss National Science Foundation. Numerous discussions with M. Chaussidon and G. Lugmair are appreciated. REFERENCES Bischoff, A. 1976, Ph.D. thesis, Univ. Münster Miller, J. M. 1998, Space Sci. Rev., 86, 79 Bodemann, R. 1993, Ph.D. thesis, Univ. Hannover Mostefaoui, S., et al. 2003, Lunar Planet. Sci. Conf., 34, 1585 Cameron, A. G. W. 2001, Lunar Planet. Sci. Conf., 32, 1035 Münker, C., et al. 2000, Science, 289, 1538 Murty, S. V. S., Goswami, J. N., & Shukolyukov, Yu. A. 1997, ApJ, 475, ———. 2003, Lunar Planet. Sci. Conf., 34, 1083 L65 Chaussidon, M., Robert, F., & McKeegan, K. D. 2002, Lunar Planet. Sci. Neumann, S. 1999, Ph.D. thesis, Univ. Hannover Conf., 33, 1563 Nichols, R. H., Jr., et al. 2002, Geochim. Cosmochim. Acta, submitted Chaussidon, M., Robert, F., McKeegan, K. D., & Krot, A. N. 2001, Lunar Ostriker, E. C., & Shu, F. A. 1995, ApJ, 447, 813 Planet. Sci. Conf., 32, 1862 Feigelson, E. D., Garmier, G. P., & Pravdo, S. H. 2002, ApJ, 572, 335 Phinney, D., Whitehead, B., & Anderson, D. 1979, Lunar Planet. Sci. Gosling, J. T. 1993, J. Geophys. Res., 98, 18937 Conf., 10, 885 Goswami, A. N., Marhas, K. K., & Sahijpal, S. 2001, ApJ, 549, 1151 Rao, M. N., et al. 1994, Geochim. Cosmochim. Acta, 58, 4231 Gounelle, M., et al. 2001, ApJ, 548, 1051 Reames, D. V., et al. 1997, ApJ, 483, 515 Grossmann, L., & Ganaphaty, R. 1976, Geochim. Cosmochim. Acta, 40, Reedy, R. C. 1977, Lunar Planet. Sci. Conf., 8, 825 967 ———. 2002, Lunar Planet. Sci. Conf., 33, 1938 Hashizume, K., Marty, B., & Wieler, R. 2002, Earth Planet. Sci. Lett., 202, Reynolds, J. H. 1960, Phys. Rev. Lett., 4, 8 201 Russell, S. S., Gounelle, M., & Hutchison, R. 2001, Philos. Trans. R. Soc. Kornacki, A. S., & Fegley, B., Jr. 1986, Earth Planet. Sci. Lett., 79, 217 London, A359, 1991 Lee, T., Papanastassiou, D. A., & Wasserburg, G. J. 1977, ApJ, 211, L107 Russell, S. S., et al. 1998, Meteoritics Planet. Sci., 32, A132 Lee, T., et al. 1998, ApJ, 506, 898 Schönbächler, M., et al. 2002, Science, 295, 1705 Leya, I., et al. 2000, Meteoritics Planet. Sci., 35, 259 Shu, F. H., Shang, H., & Lee, T. 1996, Science, 271, 1545 ———. 2001, Meteoritics Planet. Sci., 36, 1547 Shukolyukov, A., & Lugmair, G. W. 1993, Science, 259, 1138 Luck, J. M., et al. 2003, Geochim. Cosmochim. Acta, 67, 143 ———. 2001, Meteoritics Planet. Sci., 36, A188 Lugmair, G., & Shukolyukov, A. 1998, Geochim. Cosmochim. Acta, 62, Shukolyukov, Yu. A., et al. 2001, Geochim. Int. 39 (Suppl. 1), 110 2863 Simon, S. B., et al. 2002, Meteoritics Planet. Sci., 37, 533 MacPherson, G. J., Davis, A. M., & Zinner, E. K. 1995, Meteoritics Planet. Srinivasan, G. 2002, Meteoritics Planet. Sci., 37, A135 Sci., 30, 365 Srinivasan, G., Huss, G. R., & Wasserburg, G. J. 2000, Meteoritics Planet. MacPherson, G. J., & Huss, G. R. 2001, Lunar Planet. Sci. Conf., 32, 1882 Sci., 35, 1333 Mason, G. M., Dwyler, J. R., & Mazur, J. E. 2000, ApJ, 545, L157 Srinivasan, G., Ulyanov, A. A., & Goswami, J. N. 1994, ApJ, 431, L67 Mason, G. M., Mazur, J. E., & Dwyler, J. R. 1999, ApJ, 525, L133 Sugiura, N., Shuzou, Y., & Ulyanov, A. 2001, Meteoritics Planet. Sci., 36, McKeegan, K. D., Chaussidon, M., & Robert, F. 2000, Science, 289, 1334 1397 Meyer, B. S., & Clayton, D. D. 2000, Space Sci. Rev., 92, 133 Tachibana, S., & Huss, G. R. 2003, Lunar Planet. Sci. Conf., 34, 1737 Michel, R., & Nagel, P. 1997, International Codes and Model Comparison Vogel, N., et al. 2003, Lunar Planet. Sci. Conf., 34, 1873 Wasserburg, G. J., Gallino, R., & Busso, M. 1998, ApJ, 500, L189 for Intermediate Energy Activation Yields (NSC/DOC[97]-1; Paris: Young, P. G., Arthur, E. D., & Chadwick, M. B. 1998, GNASH-FKK NEA) (computer code system) (PSR-0125/07; Paris: NEA) Michel, R., & Neumann, S. 1998, in Int. Conf. Isotopes in the Solar System, ed. J. N. Goswami & S. Krishnaswami (Proc. Indian Acad. Sci. 107; Bangalore: Indian Acad. Sci.), 441
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