Meteoritics & Planetary Science 40, Nr 2, 315–327 (2005) Abstract available online at http://meteoritics.org Regolith history of lunar meteorites S. LORENZETTI,† H. BUSEMANN,‡ and O. EUGSTER* †Present Physikalisches Institut, Universität Bern, 3012 Bern, Switzerland address: Laboratorium für Biomechanik, Eidgenössische Technische Hochschule Zürich, 8093 Zürich, Switzerland ‡Present address: Carnegie Institution, Washington, D.C. 20015, USA *Corresponding author. E-mail: [email protected] (Received 1 December 2003; revision accepted 12 December 2004) Abstract–The regolith evolution of the lunar meteorites Dhofar (Dho) 081, Northwest Africa (NWA) 032, NWA 482, NWA 773, Sayh al Uhaymir (SaU) 169, and Yamato (Y-) 981031 was investigated by measuring the light noble gases He, Ne, and Ar. The presence of trapped solar neon in Dho 081, NWA 773, and Y-981031 indicates an exposure at the lunar surface. A neon three-isotope diagram for lunar meteorites yields an average solar 20Ne/22Ne ratio of 12.48 ± 0.07 representing a mixture of solar energetic particles neon at a ratio of 11.2 and solar wind neon at a ratio of 13.8. Based on the production rate ratio of 21Ne and 38Ar, the shielding depth in the lunar regolith of NWA 032, NWA 482, SaU 169, and Y-981031 was obtained. The shielding depth of these samples was between 10.5 g/cm2 and >500 g/cm2. Based on spallogenic Kr and Xe, the shielding depth of Dho 081 was estimated to be most likely between 120 and 180 g/cm2. Assuming a mean density of the lunar regolith of 1.8 g/cm3, 10.5 g/cm2 corresponds to a depth of 5.8 cm and 500 g/cm2 to 280 cm below the lunar surface. The range of regolith residence time observed in this study is 100 Ma up to 2070 Ma. INTRODUCTION Lunar samples collected during the Apollo and Luna missions represent just a small part of the lunar surface. Numerous lunar meteorites have been recovered in cold or hot desert areas in the last two decades. Lunar meteorites were ejected by asteroidal and cometary impacts spread over the entire lunar surface. Hence, the lunar meteorites can be a source of extensive information about the nature of the Moon and, particularly, the lunar crust. The average lunar regolith layer thickness can be estimated with radar and optical data. The thickness is 5 m for maria and 12 m for highlands (Shkuratov and Bondarenko 2001). The transfer time for lunar meteorites from the parent body to Earth is rather short compared to other meteorite classes. Only Calcalong Creek, Yamato (Y-) 82192/3/86032, and Dhofar (Dho) 025 were in space for more than 1.5 Ma. As summarized in this work (Table 1), the range for the MoonEarth transfer time of the lunar meteorites is between 0.01 and 10.8 Ma. The short transfer times imply that most of the cosmogenic noble gases in lunar meteorites were produced during the residence time in the regolith at the lunar surface. The material from which lunar meteorites were formed was exposed to cosmic rays in the lunar regolith. Solar gases are trapped by the material in the top layer of the Moon. The penetration depth of solar wind particles (SW) and solar energetic particles (SEP) is only tens of nanometers and a few micrometers, respectively (Rao et al. 1991). Galactic cosmic ray (GCR) particles and their secondary particles penetrate lunar material down to a depth on the order of a few meters. Thus, lunar rocks may be irradiated by cosmic rays, but do not trap any solar gases. During the regolith residence time TR, the lunar material is exposed in a 2π-irradiation geometry. The ejection age from the Moon is Tej = Ttrans + Tterr, where Ttrans is the Moon-Earth transfer time and Tterr the terrestrial residence time since the meteorites fell on Earth. Tej, Ttrans, and Tterr and are listed in Table 1. During the transfer from the Moon to Earth, the meteorite is exposed in a 4π-irradiation geometry. To determine Ttrans, the cosmic-rayproduced radionuclides such as 10Be, 14C, and 36Cl were used (cf., Nishiizumi et al. 2001a, b, 2004). For many lunar meteorites, Ttrans is sufficiently short that the irradiation in the lunar regolith is clearly visible in the radionuclides, and the radionuclide concentration can in fact be used to determine the ejection depth. An irradiation in the lunar regolith is not visible in the radionuclides if the time since the irradiation is much longer than the half-life of the respective radionuclide. The stable cosmogenic noble gases 3He, 21Ne, and 38Ar in lunar meteorites are, in general, predominantly produced 315 © The Meteoritical Society, 2005. Printed in USA. 316 S. Lorenzetti et al. Fig. 1. Ca/Ti versus lunar ejection time for lunar meteorites. during the first exposure in the lunar regolith and during the second one in free space during the transfer to Earth. Meteorites that were ejected by the same cratering event are called “source crater paired.” These meteorites must have the same Tej. On the other hand, it is possible that meteorites with similar Tej were ejected separately at different ejection events. Thus, the number of ejection events as obtained from Tej is a lower limit. Of course, an impactor can hit a nonuniform region with different material. To count the ejection events on the Moon, we considered both Tej and the ratio Ca/ Ti that characterizes the type of meteorite (Fig. 1). A ratio Ca/ Ti >60 represents the lunar highlands and Ca/Ti <15 lunar mare material. We assume that it is unlikely that material from both regions were ejected by the same event. Consequently, highland breccias and mare basalts are not considered to be crater paired. For the lunar meteorites collected until now, we propose 3–5 ejection events in the highlands and 5–6 events in the mare regions. The aim of this study of lunar meteorites was to determine the residence time of the meteoritic material and its shielding depth in the regolith. Here, we present the noble gas data of six recently recovered lunar meteorites and will discuss their regolith exposure history. Preliminary or incomplete data of the investigated meteorites were published earlier: Dho 081 (Eugster et al. 2001), NWA 032 (Fagan et al. 2002); NWA 773 (Fagan et al. 2003); SaU 169 (Gnos et al. 2004); and Y-981031 in the framework of a consortium study published in an NIPR journal (Lorenzetti et al. 2002). SAMPLES AND EXPERIMENTAL PROCEDURE For each meteorite, we selected samples without fusion crust. Dho 081 was found in 1999 as a single fragment in the desert Dhofar in Oman. It is a shocked feldspatic fragmental highland breccia dominated by anorthosite-rich lithic and mineral clasts embedded into a fine-grained mostly shock melted clastic matrix (Greshake et al. 2001). Cahill et al. (2002, 2004) conclude that Dho 081 may originate from a highland terrain on the far side of the Moon. Dho 081 is similar in composition and weathering to Dho 280 (Demidova et al. 2003). These two meteorites appear to be fall paired (Nazarov et al. 2003). Dho 081 was bought from J. Nauber (Meteorite Laboratory, Zürich). Two samples were analyzed: 5.48 mg (for He, Ne, and Ar) and 4.22 mg (for Kr and Xe). NWA 032 is the third unbrecciated meteorite from the lunar maria (Fagan et al. 2000) and is geochemically and petrographically distinct from the previously identified lunar mare meteorites Y-793169 and Asuka-881757. The trace element concentrations of NWA 032 were measured by Korotev et al. (2001). The sample of NWA 032 was obtained from T. Fagan (University of Hawai’i). The sample was crushed to a grain size <750 µm to obtain average bulk material. We measured two splits of 22.31 mg and 22.80 mg. Daubar et al. (2002) concluded that NWA 482 is a crystalline impact melt breccia from the highlands of the Moon, and furthermore, that its short terrestrial age, combined with the unique lithology, preclude any pairing with other NWA lunar meteorites. The chemical composition was measured by Warren and Kallemeyn (2001). Two samples of NWA 482 (obtained from P. Warren, UCLA) weighing 4.98 mg and 4.87 mg were crushed to <750 µm and measured to determine the He, Ne, and Ar isotope abundances. NWA 773 consists of two lithologies: a green olivine-rich cumulate and a black impact breccia (Fagan et al. 2001). A part of our noble gas data was published in a work on lunar origin, iron-enrichment trend, and brecciation of NWA 773 (Fagan et al. 2003). Nishiizumi et al. (2004b) determined the radionuclides. The proposed models to explain the data will be discussed later. The sample was separated by P. Warren (UCLA) into a cataclastic breccia fraction (cbf, black lithology) and into a peridotite fraction (p, green lithology). For the breccia fraction, we prepared three grain size splits (350–750 µm, 15.84 mg; 35–350 µm, 15.01 mg; <35 µm, 14.65 mg) to obtain a separation of the surface-correlated trapped solar gases from the volume-correlated cosmic-rayproduced gases and radiogenic gases. For the peridotite fraction, we analyzed a sample of 18.40 mg. SaU 169 was found by a group of Swiss scientists in the Omani desert. It consists of an extremely KREEP-rich anorthosite-free impact-melt breccia and adherent KREEP-rich regolith (Gnos et al. 2004). A slice of the impact-melt breccia (imp) without fusion crust was crushed into pieces. Two samples of 5.24 mg and 5.14 mg were used for the He, Ne, and Ar analyses. From the lithologies IIE and IIF (Gnos et al. 2004), both regolith breccia samples (reg), 5.31 mg and 10.20 mg, respectively, were measured. Of the lithology IIH, part of the KREEP clast (Gnos et al. 2004), 11.92 mg was analyzed. Regolith history of lunar meteorites 317 Table 1. Ca/Ti ratios, lunar regolith residence times TR, Moon-Earth transfer times Ttrans, terrestrial ages Tterr, and lunar ejection times Tej, for lunar meteorites. All ages in million years. Meteorite Mass (g) Ca/Ti TR Ttrans Highland breccias ALH A81005 DaG 262 DaG 400 Dhofar 025 Dhofar 301 Dhofar 304 Dhofar 081 Dhofar 280 Dhofar 026 Dhofar 302 Dhofar 303 Dhofar 305 Dhofar 306 Dhofar 307 Dhofar 310 Dhofar 489 MET 01210 MAC 88104 MAC 88105 NWA 482 QUE 93069 QUE 94269 Yamato-791197 Yamato-82192 Yamato-82193 Yamato-86032 31.4 513 1425 751 9 10 174 251 148 3.8 4.2 7 2.6 50 – 34.4 22.8 61.2 662.5 1015 – 24.6 52.4 36.7 27.0 648.4 66.9a 90.5e 112.7h – – 52P ~90c – – – – 119P 123P 230P – – – – 84.4a 68.7F – 94.7k 64.0a 55.8a 99.1a 97.9a 580 ± 180 100−1000f, K <3i – – – 680 ± 140D – – – – – – – – ~20W – – 630 ± 200b 2070 ± 420D – 1000 ± 400k 910l – 11j – <0.05r 0.15e ≤1i >10U – – ≤0.01E – <0.01R – – – – – – – – – 0.04−0.05r 0.9E – 0.02−0.15k, n <<0.1r 10.6 +0.6/−5.6j 10.6 +0.6/−5.6j 10.8 +0.7/−5.8j 19 23.4 8.7 186 290 22.3u 23.4y 24.3o 21.5J 31.5L ~600A 400 ± 60y 700 ± 200w – – 3 ± 1p <0.1z <0.01x – <0.02x 442 154 30.7 paired 53.0 – 252.5 244.1 59.0 156 ~300 633 22.4 206.4 6.1 6.9o – 15.4o 19.3f – – – – – 4.2B ~14G – 5.5N 8.2o <1k – 28.5f – – – – – – 207 ± 43D 100 ± 20H – <200D 50 ± 10k 0.9 ± 0.1p <0.05p – – <0.01s 0.01−0.08s, t – – – – – – – – – – – – 0.042 ± 0.005 <0.01C <0.03d – – – ≤0.34N 0.0097 ± 0.0013N 1.1 ± 0.2p <0.05p paired paired paired paired paired paired Highland/mare rocks Calcalong Creek QUE 94281 Yamato-793274 paired Yamato-981031 Yamato-983885 Mare basalts Asuka-881757 Dhofar 287 EET 87521 EET 96008 LAP 02205 LAP 02224 LAP 02226 LAP 02436 NWA 479 NWA 032 NWA 773 PCA 02007 SaU 169 Yamato-793169 Tterr 0.04−0.10r 0.05−0.06g – 0.5−0.6E – – 0.04 ± 0.02E – – – – – – – – – – – 0.21−0.35j, r 0.06−0.12E – 0.005−0.01n 0.03−0.09r – 0.072−0.083j – <0.03p 0.25 ± 0.10z 0.02−0.035x – 0.045 ± 0.01x Tej 0.040−0.15 0.05−0.075 ≤1 >10U – – 0.04 ± 0.02 – – – – – – – – several kyW – – 0.25−0.40 0.28 – 0.025−0.16 0.03−0.19 – 8±3 – 3±1 0.35 ± 0.10 0.032–0.003x – 0.045 ± 0.01x 0.9 ± 0.1 – 0.02–0.09 – – – – – – 0.05 ± 0.01 0.017 ± 0.001d – ≤0.35N 1.1 ± 0.2 References: a = Warren and Kallemeyn (1991); b = Eugster et al. (1991); c = Nishiizumi et al. (1989); d = Nishiizumi et al. (2004b); e = Bischoff et al. (1998); f = Eugster et al. (2000); g = Nishiizumi et al. (1998); h = Zipfel et al. (1998); i = Scherer et al. (1998); j = Eugster et al. (1989); k = Thalmann et al. (1996); l = Takaoka (1986); n = Nishiizumi et al. (1996b); o = Arai et al. (1996); p = Nishiizumi et al. (1992); r = Nishiizumi et al. (1991a); s = Nishiizumi et al. (1991b); t = Vogt et al. (1993); u = Hill et al. (1991); w = Eugster et al. (1992); x = Nishiizumi et al. (2004a); y = Polnau et al. (1998); z = Nishiizumi et al. (1996a); A = Swindle et al. (1995), adopting P38(2π) = 0.12 × 10−8 cm3 STP/g Ma; B = Fagan et al. (2002); C = Nishiizumi et al. (2001a); D = This work; E = Nishiizumi et al. (2001b); F = Grossman et al. (2001); G = Mittlefehldt (2001), personal communication; H = This work, peridotite fraction; J = Kojima (2000); K = Fernandes et al. (2000); L = Kaiden et al. (2002); N = Gnos et al. (2004); P = Demidova et al. (2003); R = Shukolyukov et al. (2001); U = Nishiizumi (2003); W = Nishiizumi (2004). 318 S. Lorenzetti et al. Fig. 2. Three-isotope plot for Ne containing all available data of lunar meteorites. SW and SEP data from Wieler (2002), noble gas data from Schultz and Franke (2002) and from this work. The mixing line yields a solar ratio Ne/Ne = 12.48 ± 0.07. Y-981031 is the seventh Antarctic lunar meteorite of mare origin (Arai et al. 2002). These authors conclude that the overall texture and the presence and composition of pyroclastic/impact glasses suggest “source-crater pairing” of Y-981031 with Y793274 and QUE 94281, and “source-basalt pairing” with Y793169 and Asuka-881757 because of the similarity of the pyroxene zoning trend, the presence of symplectic pyroxene, and the mineral composition of the mesostases in the mare basalt component. Y-981031 was allocated to us by the Antarctic Meteorite Research Center of the National Institute of Polar Research, Tokyo and the first data were published in an NIPR journal (Lorenzetti et al. 2002). For the analyses, we used a 5.05 mg and a 5.10 mg sample. To desorb terrestrial atmospheric gases, we heated the samples in the storage arm of the extraction system for about a week at 90 °C. The measurements of He, Ne, and Ar were performed using our mass spectrometer system B, described in detail by Eugster et al. (1993). Typical blank corrections are <1% for He and Ne and <2% for Ar. The Kr and Xe measurements of Dhofar 081 were done according to the procedures described by Busemann et al. (2002). Blank corrections amount to 6 and 12% of the measured Kr and Xe concentrations, respectively. RESULTS AND DISCUSSION The analytical results are given in Tables 2–4. Experimental errors are 2σ mean for all analyses. The grainsize splits from NWA 773 show no differences neither in the absolute amounts nor in the ratios. Therefore, we calculated average values for these splits. Neon is a mixture of trapped (tr) and in situ produced cosmogenic (c) Ne. For argon, an additional component is present: the radiogenic (r) component is a product of 40K decay to 40Ar. For the calculation of the Ne and Ar components, we adopted the following ratios: (20Ne/22Ne)c = 0.8; (21Ne/22Ne)tr = 0.033; (36Ar/38Ar)c = 0.65; (36Ar/38Ar)tr = 5.32; and (20Ne/ 22Ne) = 12.48 (as determined below), except for NWA 773, tr SaU 169, and Y-981031. Four fractions of NWA 773 were measured. They contain solar gases and yield a solar ratio of (20Ne/22Ne)tr = 13.09. SaU 169 and Y-981031 contain trapped Ne with a solar ratio of (20Ne/22Ne)tr = 11.21 and 12.84, respectively. The noble gas components are given in Table 5. Isotopic Abundances of Trapped Ne The (20Ne/22Ne)tr ratio in a meteorite can be derived from a Ne three-isotope plot. If no fractionation during the trapping process occurred and the noble gas isotopes were not disturbed by a secondary process, such as differentiation or mixing with another gas source, all extractions form a specific sample plot on a mixing line between the trapped and the cosmogenic components. Possible sources for the trapped component are the SW, SEPs, or planetary sources. Contamination with terrestrial atmospheric light noble gases, as observed in the lunar meteorite Dho 026 (Shukolyukov et al. 2001) and in chondrites (Scherer et al. 1994), was not observed in our samples. Lunar meteorites contain much less 5.48 22.31 22.80 average 4.98 4.87 average 15.84 15.01 14.65 average 18.40 5.24 5.14 average 5.31 10.20 11.92 5.05 5.10 average Sample Dho 081 NWA 032 NWA 032 NWA 032 NWA 482 NWA 482 NWA 482 NWA 773 cbf 340–750 µm NWA 773 cbf 35–340 µm NWA 773 cbf <35 µm NWA 773 cbf NWA 773 p SaU 169 imp SaU 169 imp SaU 169 imp SaU 169 IIE SaU 169 IIF SaU 169 IIH Y-981031.66 Y-981031.66 Y-981031.66 Weight (mg) 4.22 Sample Dho 081 407 ± 13 3676 ± 118 5168 ± 206 4422 ± 119 1148 ± 35 1161 ± 35 1154 ± 25 181071 ± 6922 191541 ± 16030 175248 ± 6972 182620 ± 6267 16516 ± 609 41266 ± 1415 42651 ± 1500 41939 ± 1500 2330 ± 70 5000 ± 155 2590 ± 79 100610 ± 4561 146206 ± 5695 123408 ± 3648 4He 1184 ± 178 (10−12 cm3 STP/g) 86Kr Table 3. Results of Kr measurements. Weight (mg) Table 2. Results of He, Ne, and Ar measurements. cm3 STP/g) 20 ± 0.4 80Kr 7635 ± 167 2345 ± 54 2398 ± 57 2371 ± 39 1141 ± 29 973 ± 24 1057 ± 19 5469 ± 121 5962 ± 129 5048 ± 115 5493 ± 70 1537 ± 34 7303 ± 230 7595 ± 400 7449 ± 25 5806 ± 125 5124 ± 207 10875 ± 335 30526 ± 923 39207 ± 1363 34866 ± 823 40Ar 3.43 ± 0.06 78Kr 426 ± 13 17.61 ± 0.54 19.00 ± 0.62 18.31 ± 0.41 13.69 ± 0.56 13.72 ± 0.52 13.71 ± 0.38 20419 ± 614 22249 ± 670 16909 ± 508 19859 ± 347 8.75 ± 0.33 23.42 ± 0.92 23.36 ± 0.77 23.4 ± 0.9 97.1 ± 3.1 325 ± 10 14.4 ± 0.4 30945 ± 1049 41102 ± 2008 36023 ± 1133 (10−8 20Ne 86Kr = 100 4.485 ± 0.033 0.681 ± 0.005 0.667 ± 0.005 0.674 ± 0.004 0.661 ± 0.006 0.673 ± 0.008 0.667 ± 0.005 5.27 ± 0.04 5.27 ± 0.04 5.28 ± 0.04 5.27 ± 0.02 1.85 ± 0.04 0.960 ± 0.020 1.001 ± 0.026 0.981 ± 0.026 2.24 ± 0.02 3.59 ± 0.04 1.46 ± 0.02 5.17 ± 0.05 5.22 ± 0.05 5.20 ± 0.04 36Ar/ 38Ar 78.1 ± 1.5 83Kr 3.76 ± 0.044 1.138 ± 0.012 1.154 ± 0.015 1.146 ± 0.010 1.230 ± 0.029 1.251 ± 0.030 1.240 ± 0.021 23.68 ± 0.34 23.41 ± 0.24 22.77 ± 0.24 23.29 ± 0.16 1.42 ± 0.23 1.197 ± 0.030 1.197 ± 0.013 1.197 ± 0.030 1.57 ± 0.03 2.29 ± 0.03 1.155 ± 0.016 20.47 ± 0.22 22.08 ± 0.22 21.28 ± 0.16 22Ne/ 21Ne 74.1 ± 1.5 82Kr 8.66 ± 0.09 0.832 ± 0.009 0.806 ± 0.008 0.819 ± 0.006 0.814 ± 0.024 0.800 ± 0.020 0.807 ± 0.016 12.93 ± 0.13 12.89 ± 0.13 12.94 ± 0.13 12.92 ± 0.08 3.53 ± 0.23 0.789 ± 0.022 0.815 ± 0.012 0.802 ± 0.020 3.87 ± 0.06 6.346 ± 0.070 0.825 ± 0.012 12.63 ± 0.15 12.63 ± 0.13 12.63 ± 0.10 20Ne/ 22Ne 0.0002 ± 0.01 81Kr 587 ± 72 177 ± 2 226 ± 2 201 ± 2 40.95 ± 0.71 41.33 ± 0.45 41.14 ± 0.42 2576 ± 66 2472 ± 44 2244 ± 51 2431 ± 31 3413 ± 266 723 ± 21 795.5 ± 8.1 744.5 ± 8.1 277 ± 35 253.3 ± 5.9 474.5 ± 8.4 1941 ± 65 2045 ± 21 1993 ± 34 4He/3He 334 ±7 84Kr 10.76 ± 0.09 176 ± 2.2 179.8 ± 1.4 177.7 ± 1.3 48.44 ± 1.00 48.27 ± 0.94 48.35 ± 0.69 2.21 ± 0.02 2.25 ± 0.02 2.30 ± 0.03 2.25 ± 0.01 1338 ± 48 411 ± 7 439 ± 10 425 ± 15 87.1 ± 1.1 24.3 ± 0.3 389 ± 4 2.36 ± 0.03 2.34 ± 0.05 2.35 ± 0.03 40Ar/ 36Ar Regolith history of lunar meteorites 319 4.22 Sample Dho 081 597 ± 90 (10−12 cm3 STP/g) 132Xe 5.48 average average average 18.40 average 5.31 10.20 11.92 average Sample Dho 081 NWA 032 NWA 482 NWA 773 NWA 773 p SaU 169 imp SaU 169 IIE SaU 169 IIF SaU 169 IIH Y-981031.66 c 12.0 ± 0.5 20 ± 1 13.7 ± 0.6 17 ± 2 1.73 ± 0.31 24.4 ± 1.3 15.7 ± 0.6 21.6 ± 0.7 15.1 ± 0.5 44 ± 2 21Ne SW (lunar soil 71501) SEP (lunar soil 71501) Modern SW Aubrite parent body Lunar meteorites (10−8 13.8 ± 0.1 11.2 ± 0.2 13.8 ± 0.1 12.1 ± 0.2 12.48 ± 0.07 20Ne/22Ne 28.3 ± 1.6 19.7 ± 1.0 32.2 ± 1.2 – 0.46 ± 0.06 16.6 ± 1.0 19.6 ± 0.5 21.7 ± 0.8 15.8 ± 0.4 75 ± 8 c 0.95 ± 0.05 124Xe 38Ar Table 6. Solar Ne in different solar system reservoirs. Weight (mg) Table 5. Noble gas components of Ne and Ar. Weight (mg) Table 4. Results of Xe measurements. cm3 tr tr 132Xe 100.4 ± 3.8 129Xe 691 ± 16 <0.5 <0.1 – 0.85 ± 0.05 6.73 ± 1.2 54.0 ± 1.7 197 ± 7 17.6 ± 0.7 14800 ± 2500 36Ar 9.57 ± 0.32 128Xe 13 ± 13 <0.7 <0.3 19850 ± 1985 7.21 ± 0.35 – 82.0 ± 3.2 306 ± 10 <0.4 36000 ± 6000 STP/g) 20Ne 1.46 ± 0.06 126Xe – – – 13.08 ± 0.19 13.08 ± 0.19 – 11.21 ± 0.30 11.21 ± 0.30 11.21 ± 0.30 12.84 ± 0.60 33.0 ± 1.3 136Xe 0.058 ± 0.016 1.10 ± 0.06 2.05 ± 0.11 – 2.80 ± 0.61 2.27 ± 0.17 0.53 ± 0.10 0.87 ± 0.05 0.349 ± 0.021 0.57 ± 0.15 (3He/21Ne)c 38.7 ± 1.7 134Xe (20Ne/22Ne)tr 86.0 ± 3.2 131Xe Wieler (2002) Wieler (2002) Benkert et al. (1993) Lorenzetti et al. (2003) This work Reference 1.33 ± 0.08 1.14 ± 0.01 1.25 ± 0.03 1.08 ± 0.02 1.08 ± 0.02 1.198 ± 0.060 1.207 ± 0.063 1.110 ± 0.055 1.152 ± 0.058 – (22Ne/21Ne)c 16.5 ± 0.7 = 100 130Xe 320 S. Lorenzetti et al. Regolith history of lunar meteorites Fe than chondrites and are, therefore, less affected by weathering. The cosmogenic component varies with the chemical composition of the meteorite and its shielding depth. Different meteorites lie on the mixing line if they have cosmogenic and trapped components with the same composition of Ne. To compare the average trapped Ne in lunar meteorites with the SW and the trapped Ne of other parent bodies, we estimate the mean solar ratio of Ne for lunar meteorites by plotting all available data from the compilation by Schultz and Franke (2002) in a three-isotope plot (Fig. 2). Using the Least-Squares Fit to calculate the mixing line, we obtain a (20Ne/22Ne)tr ratio of 12.48 ± 0.07 for (21Ne/22Ne)tr = 0.03. The given error is the standard deviation. Ninety percent of the lunar meteorites lie within 10% of this mixing line. In Table 6, the 20Ne/22Ne ratios in various solar system reservoirs are summarized. The value of the lunar meteorites lies between that for the SW and the SEPs. Kr and Xe Components We assume a priori that the composition of the trapped Kr and Xe in Dho 081 is unknown and preliminarily decompose the Xe data (Table 4) using both possible trapped Xe components SW (Pepin et al. 1995) and air (see Busemann et al. 2002). For the spallogenic (sp) Xe composition, we used Xesp spectra (Hohenberg et al. 1981) based on the Ba and REE concentrations in Dho 081 (Warren et al. 2001). The pure trapped Xe isotope ratios for Dho 081, corrected for the expected Xesp, are identical to those of air, except for the ratios 128Xe/132Xe and 131Xe/132Xe. Solar Xe is clearly absent, as is fissiogenic Xe. This is consistent with the low concentrations of U and Th in Dho 081, compared to other lunar meteorites (Warren et al. 2001). Thus, we corrected for trapped Xe assuming that 136Xe is entirely of trapped origin and Xetr = Xeair. The subtraction of air yields (124Xe/126Xe)sp = 0.53 ± 0.06, (128Xe/126Xe)sp = 2.15 ± 0.40, (130Xe/126Xe)sp = 1.2 ± 0.8, (131Xe/126Xe)sp = 6.1 ± 4.0, 126Xe = (6.7 ± 0.4) × 10−12 cm3 STP/g and 131Xe = (41 ± sp sp 27) × 10−12 cm3 STP/g. (128Xe/126Xe)sp and (131Xe/126Xe)sp are high and indicate an origin of Dho 081 from a large depth, in agreement with the absence of SW (this work) and the lack of a “genuine regolith component” in this meteorite (Greshake et al. 2001). Adopting (131Xe/126Xe)sp ratio = 6.1, the Ba and La concentrations from Warren et al. (2001), and the production rate systematics given in Hohenberg et al. (1978), the shielding depth of Dho 081 would be ~80 g/cm2. Taking in account the uncertainty of the (131Xe/126Xe)sp ratio, shielding depths lie within a range of 0 to 175 g/cm2. The transfer time from the Moon to Earth of <10 ka implies that 126Xe was essentially produced during the 2π irradiation of sp Dho 081 on the lunar surface. Thus, here we use the production rates P126 = 0.012 × 10−12 cm3 STP/(g Ma) and P131 = 0.075 × 10−12 cm3 STP/(g Ma), which are given for a 321 shielding depth of 80 g/cm2 (Hohenberg et al. 1978) and the Ba and La concentrations in Dho 081 (Warren et al. 2001). Assuming a simple exposure history for Dho 081, the Xe isotope systematics alone would yield a residence time in the lunar surface of ~550 Ma. Kr in Dho 081 (Table 3) was partitioned assuming Krtr = Krair and 86Kr to be entirely of trapped origin, because Xe in Dho 081 did not indicate the presence of SW. The lack of fissiogenic Xe in Dho 081 also excludes the presence of fissiogenic 86Kr. 81Kr in Dho 081 was below detection limit, precluding the determination of a 81Kr-83Kr cosmic ray exposure age. A small excess of 80Kr due to neutron-induced production on 79Br may be visible, whereas an excess on 82Kr is within the uncertainty absent. The subtraction of trapped Kr yields the Krsp composition of Dho 081 (78Kr: 80Kr: 82Kr: 83Kr: 84Kr: 86Kr = 0.118 ± 0.015, 0.579 ± 0.079, 0.653 ± 0.146, 1, 0.509 ± 0.548, 0). The low value for (78Kr/83Kr)sp of 0.118 implies, similar to a high (131Xe/126Xe)sp, a large shielding depth of Dho 081 on the lunar surface. The depth can be estimated with the production rates given by Regnier et al. (1979) and the target element concentrations for Kr in Dho 081. Only the concentration for Sr (240 ppm), the main target element for Kr, is known (Warren et al. 2001), whereas the concentrations of Rb (0.74 ± 0.15 ppm), Y (8.8 ± 0.7 ppm), and Zr (34.5 ± 0.9 ppm) are adopted mean concentrations from values given for MAC 88104/5 (Eugster et al. 1991; Jolliff et al. 1991; Koeberl et al. 1991; Neal et al. 1991; Palme et al. 1991; Warren and Kallemeyn 1991). We have chosen this lunar highland anorthosite because it might be crater paired with Dho 081 (Greshake et al. 2001). The choice of the lunar highland anorthosite data set for Rb, Y, and Zr is not critical. The shielding depth deduced for Dho 081 is ~180 g/cm2. Considering the uncertainty of the (78Kr/83Kr)sp ratio, we obtain a range from 120 to 260 g/cm2, which overlaps with the depth range obtained for Xe. Both data sets imply a most probable shielding depth for Dho 081 of 120 up to 180 g/cm2. Nishiizumi et al. (2004b) calculated an ejection depth of 200– 230 g/cm2 based on the cosmogenic radionuclides. Adopting the depth of 180 g/cm2 and assuming a simple irradiation in the lunar surface for Dho 081, we obtain the production rates P78 = 0.0266 × 10−12 cm3 STP/(g Ma) and P83 = 0.2256 × 10−12 cm3 STP/(g Ma), respectively. These yield a residence time for Dho 081 of ~640 Ma. The Kr and Xe concentrations in Dho 081 are ~50% higher than those given by Greshake et al. (2001). Nevertheless, based on the Kr and Xe isotopic compositions, we cannot confirm the presence of solar Kr and Xe in this meteorite as found by Greshake et al. (2001). Elemental Ratios of the Trapped Noble Gases A (4He/20Ne)tr versus (20Ne/36Ar)tr is very illustrative (Fig. 3) to compare the trapped solar noble gases in lunar meteorites with those in other, so called “gas-rich” 322 S. Lorenzetti et al. Fig. 3. Trapped noble gas ratios for all available data of lunar meteorites containing >2 × 10−5 cm3 STP/g 4He, of all available data of other meteorites containing >100,000 × 10−8 cm3 STP/g 4He, and of the lunar soils from Apollo 11 and Apollo 12 (Eberhardt et al. 1972). The noble gas data are from Schultz and Franke (2002) and from this work. Table 7. Chemical composition in weight percent. Sample 081a Dho NWA 032b NWA 482c NWA 773 cbf f NWA 773 pf SaU 169 impd SaU 169 regd SaU 169 KREEPd Y-981031e Ti Cr Mn Fe Ni Mg Al Si S Ca K Na 0.060 1.85 0.078 0.5 0.24 1.32 1.5 0.88 0.43 0.052 0.27 0.048 0.29 0.62 0.10 0.13 0.08 0.18 0.039 0.26 – 0.21 0.15 0.11 0.11 0.09 0.16 2.49 17.9 2.72 15.4 15.9 8.29 8.62 6.84 9.66 0.009 0.005 – – – 0.02 0.008 0.006 – 1.448 5.10 2.17 8.54 15.3 6.69 4.79 4.17 5.68 16.9 4.63 15.5 4.32 2.9 8.41 9.28 8.65 9.76 21.0 20.9 20.9 21.4 19.6 21.1 21.9 23.4 21.0 – – – 0.06 – 0.33 – – – 11.4 7.79 12.5 6.37 3.6 7.26 8.38 7.58 9.18 0.050 0.091 0.025 0.091 0.17 0.45 0.38 0.73 0.033 0.52 0.28 0.30 0.16 0.11 0.73 0.58 0.88 0.25 a Greshake et al. (2001). et al. (2002). c Warren and Kallemeyn (2001). d Gnos et al. (2004). e Kojima (2000). fFagan et al. (2003). b Fagan meteorites (trapped 4He >100,000 × 10−8 cm3 STP/g). These are supposed to originate from regoliths of parent bodies. To calculate the trapped component of 4He, we assumed 4Her = 2 × 10−5 cm3 STP/g, which results in a correction of less than 5% in all cases. All lunar meteorites are in the range of (4He/ 20Ne) = 1 to 11 and (20Ne/36Ar) = 1 to 9. The gas-rich nontr tr lunar meteorites clearly differ from the lunar meteorites. They all have ratios (4He/20Ne)tr >50 and, in most cases, (20Ne/36Ar)tr >9. We can deduce, therefore, that a meteorite containing trapped noble gases, with elemental ratios in the range defined above, most likely comes from the Moon. Surprisingly, the lunar soils of Apollo 11 (A11) and Apollo 12 (A12) yield about a factor of 10 higher (4He/20Ne)tr ratios than the lunar meteorites. Compared to the lunar soils A11 and A12, the 4Hetr in lunar meteorites seems to be depleted. Perhaps this depletion is caused by the ejection process from the Moon. Non-lunar meteorites do not show this 4He depletion, as less energy is required to eject meteoroids from asteroidal parent bodies than from the Moon. Alternatively, 4He could have been lost during the compaction process of the regolith into the solid rock material of the meteorite. Regolith history of lunar meteorites 323 Fig. 4. Production rate ratio P21/P38 versus shielding depth. The large open symbols represent the measured 21Ne/38Ar ratios. Table 8. Production rates (10−8cm3STP/[g Ma]), cosmogenic ratios, shielding depths, and regolith residence times TR.a Sample 4π irradiation P21 P38 Measured in the sample (3He/21Ne)c Produced on the Moon (21Ne/38Ar)c (g/cm2)b 2π irradiation P21 P38 TR (Ma) Dho 081 NWA 032 NWA 482 NWA 773 cbf NWA 773 p SaU 169 imp SaU 169 IIE SaU 169 IIF SaU 169 IIH Y-981031 0.2011 0.1869 0.2041 0.2420 0.3354 0.2346 0.2116 0.2116 0.2051 0.2268 0.058 1.1 2.05 – 2.80 2.27 0.53 0.871 0.349 0.57 0.42 ± 0.03 0.99 ± 0.07 0.42 ± 0.02 – 3.8 ± 0.8 1.47 ± 0.12 0.80 ± 0.04 0.99 ± 0.05 0.95 ± 0.04 0.58 ± 0.07 180c 42 >500 – >500 10.5 >500 64.1 129 >500 0.0894 0.0949 0.0150 – 0.0046 0.0776 0.0106 0.1032 0.0787 0.0115 275 ± 40 207 ± 43 2070 ± 420 – 100 ± 20 216 ± 45 1840 ± 370 210 ± 40 200 ± 40 4500 ± 1500 0.2115 0.1702 0.2301 0.1366 0.0895 0.1584 0.1778 0.1778 0.1691 0.1882 0.0514 0.0947 0.0068 – 0.0174 0.1120 0.0086 0.1033 0.0756 0.0093 a The production rates for a 4π irradiation were calculated according to Eugster et al. (1995), those for a 2π irradiation according to Hohenberg et al. (1978). depth. c Based on Kr and Xe systematics. b Shielding Shielding Depth in the Lunar Regolith To calculate the amount of the cosmogenic component produced on the Moon, we subtracted the amount produced in free space as calculated from Ttrans and the 4π production rate according to Eugster et al. (1995). The chemical composition of the investigated meteorites is summarized in Table 7. The production rates in the lunar regolith vary with the target material and the shielding depth. For stable isotopes produced by cosmic rays, the ratio of the production rates is equal to the ratio of the concentrations: 21Nec/38Arc = P21/P38. Model calculations for the production rates of Ne and Ar, based on nuclear systemactics, were performed by Hohenberg et al. (1978) and Leya et al. (2001). Leya et al. (2001) give the production rates for the Ar isotopes from Fe and Ni and Hohenberg et al. (1978) from K, Ca, Ti, and Fe. Because Ca is a significant target element in lunar meteorites for the production of Ar isotopes, we used the production rates of Hohenberg et al. (1978). For an Apollo drill core, Leya et al. (2001) found an up to 60% higher production rate for 21Ne compared to the model of Hohenberg et al. (1978). Neon production rates, based on the chemistry in our samples, are 10–50% lower than those given by Leya et al. (2001). A direct comparison for the ratio P21/P38 between the two different data sets is only possible for Fe. Using the Leya et al. (2001) data set, the ratio of the production rates is a factor of ~3 and 324 S. Lorenzetti et al. a factor 1.1 higher at low shielding and at 500 g/cm2, respectively. Obviously, this is not representative for bulk composition of lunar meteorites. However, a part of the systematic error disappears by using the ratio of P21 and P38 based on the same model. We assumed an error of the production rates of 20%. The ratio of the production rates is very sensitive to the elemental composition of the meteorite. At a shielding depth of 65 g/cm2 the ratio P21/P38 varies from 0.65 in NWA 482 up to 3.83 in the peridotite fraction of NWA 773. The variation of the ratio (21Ne/38Ar)c in duplex samples is smaller than the experimental error of an single measurement. Therefore, we conclude that our crushed sample used for the noble gas analyses represents bulk material. In Fig. 4, the ratio of the production rates versus the shielding depth is plotted. This ratio depends on the chemical composition and the shielding depth of the analyzed sample. To calculate the shielding depth from (21Ne/38Ar)c, we fitted the values for the ratio of production rates with a power function. The calculated shielding depths are given in Table 8. This method is applicable if the meteorite did not suffer any loss of 21Nec and 38Arc due to diffusion, shock, or heat. For these processes, the loss of the light noble gases can be assumed to be larger than the loss of the heavy ones. As an indicator for such a diffusion process, the ratio (3He/21Ne)c can be used. We assume that if (3He/ 21Ne) is >1, the diffusion losses of 21Ne and 38Ar are c c c negligible. This is the case for NWA 032, NWA 482, and the impact melt sample of SaU 169. For samples with diffusion loss, the ratio of the production rates P21/P38 seems to be low. Hence, the calculated shielding depth is too high and the values for the shielding depth and the regolith residence time are upper limits. The adopted error for the production rate is 20%. Dho 081 has suffered a loss of cosmogenic gases. Therefore, the method described above is not suitable for this meteorite. For the shielding depth, we assumed 180 g/cm2 based on the Kr measurements, which appears more precise than the Xe measurement. The TR for the different isotopes are: TR (21Ne) = 233 Ma, TR (38Ar) = 316 Ma, TR (83Kr) = 640 Ma, and TR (Xe) = 830 Ma (based on a shielding depth of 80 g/cm2, as determined with the Xe isotope systematics alone, we would obtain ~550 Ma). The light noble gases 21Nec and 38Arc yield lower ages than the heavy ones, indicating diffusion loss of the light noble gases. The error-weighted “best guess” residence time based on the heavy noble gases, Kr and Xe, for Dho 081 is 680 ± 140 Ma. NWA 032 has a shielding depth of 42 g/cm2 and a TR = 207 ± 43 Ma. Nishiizumi et al. (2001a) measured the radionuclides and calculated exposure at depths of 660– 730 g/cm2 for 10Be, 520–630 g/cm2 for 26Al, and 520–540 g/ cm2 for 36Cl, and an ejection depth of 1100 g/cm2. The authors exclude a production of these radionuclides in the regolith. Therefore, we suggest that the exposure in the regolith occurred 5–10 Ma ago. One or several impacts buried NWA 032 deep enough, so that the radionuclides decayed to the low levels presently observed. The shielding depth of NWA 482 is >500 g/cm2 and the TR = 2070 ± 420 Ma, representing the longest regolith residence time observed in lunar meteorites. The cataclastic breccia fraction of NWA 773 contains solar gases and 17 ± 2 × 10−8 cm3 STP/g 21Nec. This fraction was exposed in the lunar regolith, and most of the cosmogenic Ne was produced at the lunar surface. To the contrary, the peridotite fraction of NWA 773 contains 1.73 ± 0.31 × 10−8 cm3 STP/g 21Nec, and no solar wind noble gases. To produce this amount of cosmogenic Ne, the sample must be irradiated for 5.2 Ma in free space. This is a rather long transfer time for lunar meteorites. Nishiizumi et al. (2004) proposed two models to explain the low levels of 10Be and 41Ca in NWA 773: 1) the meteorite was ejected from a depth of about 800 g/cm2 on the Moon and the transfer time was ~1 ka; and 2) the ejection depth was 1000 g/cm2 and the transfer time was 30 ± 3 ka with and preatmospheric size ≥30 cm. Both models include a short transfer time. Assuming a transfer time of 30 ka, 99% of the cosmogenic noble gases in the peridotite fraction was produced at the lunar surface. The measured ratio (21Ne/38Ar)c can be explained adopting a shielding depth >500 g/cm2 and a corresponding TR of 100 ± 20 Ma. The cataclastic breccia fraction suffered an about 10 times longer exposure to cosmic rays. We propose the following model. The material of the cataclasic breccia fraction trapped solar gases and was exposed to cosmic rays at the very top layer of the Moon. During an impact event, the material was mixed with the peridotite material and deposited at a depth of >500 g/cm2 for 100 Ma. After ejection, the exposure in space was less than 30 ka. The impact melt sample of SaU 169 has no gas loss. The shielding depth of the impact melt sample in the lunar regolith is 10.5 g/cm2 and TR is 216 ± 45 Ma. This sample is the oldest material in SaU 169 with an U-Pb age of 4.24 ± 0.11 Ga (Gnos et al. 2004). The regolith breccia fraction IIE of SaU 169 has suffered more gas loss than the regolith breccia fraction IIF. Therefore, the calculated values for the shielding depth of the fraction IIE of >500 g/cm2 and TR of 1840 ± 370 Ma are too high. The fraction IIF yields a shielding depth of 64.1 g/cm2 and a TR of 210 ± 43 Ma. In the KREEP clast, we also found a low ratio (3He/21Ne)c. This sample has a maximum shielding depth of 129 g/cm2 and an upper limit of the TR of 200 ± 40 Ma. We suggest that the impact melt sample of SaU 169 yields the most reliable value for TR of this meteorite. With the assumption that the 38Arc concentration is reliable and the residence time is 216 Ma, the shielding depth of the regolith breccia is close to the surface. TR of the regolith fraction IIF and the KREEPy sample IIH are within the error bars alike. The ratio (3He/21Ne)c in Y-981031 indicates gas loss. The shielding depth is below 500 g/cm2. Regolith history of lunar meteorites CONCLUSIONS Dho 081, NWA 773, the regolith breccia fraction of SaU 169, and Y-981031 contain trapped solar gases. The other lunar meteorites investigated here do not contain trapped solar wind. Compared to the mean solar ratio (20Ne/22Ne)tr for lunar meteorites of 12.48 ± 0.07, the trapped component in NWA 773 and Y-891031 contains a larger proportion of SW. On the other hand, SaU 169 contains more SEPs. The material of NWA 032, NWA 482, and the peridotite fraction of NWA 773 contains no solar gases and we conclude that this material never resided in the very top layer (few millimeters) of the lunar regolith. Lunar meteorites without any gas loss have a regolith residence time in the range of 207 ± 43 Ma for NWA 032 and up to 2070 ± 420 Ma for NWA 482. The shortest TR of 100 ± 20 Ma was measured for the peridotite fraction of NWA 773. The most reliable residence time obtained for Dho 081 (680 Ma) is based on the heavy noble gases Kr and Xe. NWA 032, NWA 773, and SaU 169 show a complex regolith history. Material of NWA 032 suffered a multistage exposure in different shielding depths. Materials of different depths were also mixed together in NWA 773 and SaU 169. In SaU 169, various impact events were dated (Gnos et al. 2004). Assuming a lunar regolith mean density of 1.8 g/cm3 (Costes et al. 1969), the shielding depths observed for the investigated meteorites correspond to a range of 5.8 cm to >2.8 m. This is consistent with the observed lunar regolith thickness of a few meters (Shkuratov and Bondarenko 2001). Acknowledgments–We thank the National Institute of Polar Research (Tokyo) for providing the Y-981031 sample, Tim Fagan (University of Hawai’i) for the NWA 032 sample and Paul Warren (University of California, Los Angeles) for the NWA 482 and NWA 773 samples. We also thank our colleagues Edwin Gnos, Beda Hofmann and Ali al Khatiri (University of Bern) for collecting the SaU 169 meteorite in Oman. We gratefully acknowledge the technical support by Hans-Erich Jenni, Armin Schaller and Markus Zuber. Helpful reviews by Kees Welten (University of California, Berkeley) and an anonymous reviewer and the editorial handling by Marc Caffee (Purdue University) are greatly appreciated. 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