1¾«%^ĀŠŠŃŃŃC:\WORD\KURATA-I\STANDARD.DFVCAN130EBŅ@äZÅŽŠŠŃµ Collection and Microanalysis of Antarctic Micrometeorites M. Maurette and C. Engrand CSNSM, Bat. 104, F-91405 Campus Orsay, France G. Kurat Naturhistorisches Museum, Postfach 417 A-1014 Vienna, Austria 1. Introduction The present day accretionary influx of extraterrestrial matter onto the Earth (about 40.000 t/a) is dominated by meteoroids in the size-range 50-400 ęm with most of the mass being delivered by particles around 220 ęm in diameter (Love & Brownlee 1993). Such large particles cannot survive atmospheric entry unaltered. They should be in general frictionally heated to such an extend that partial to total melting and even partial evaporation will occur (e.g., Kornblum 1969). However, for low entry velocities and almost tangential entry angles there exists a small window which allows large particles to enter without being melted (Brownlee 1981, Love & Brownlee 1991). Unmelted particles were not found in deep sea sediments where they are indistinguishable from terrestrial matter. In contrast, cosmic spherules, the products of melting of sub-mm-sized interplanetary dust particles, can easily be identified and can also be found in sediments throughout geological times (e.g., Taylor & Brownlee 1991). Large unmelted interplanetary dust is also unlikely to be ever captured during U2 stratospheric collection flights for several reasons (e.g., Warren & Zolensky 1994). With the first successful recovery of large unmelted interplanetary dust particles - dubbed micrometeorites - from Greenland ice (Maurette et al. 1986) a new window into interplanetary matter was opened. Subsequent searches in Antarctica were highly successful and provided large amounts of unmelted and almost unaltered samples of the interplanetary dust particles which contribute most to the recent accretion rate on Earth (e.g., Maurette et al. 1991). Only since a few years such samples are available for study and, therefore, our knowledge of this matter is still fragmentary. Here we present a summary of what is known of micrometeorites as of today. 2. Collection The first unmelted micrometeorite (MM) samples were collected in July 1984 by sampling "cryoconite", a dark sediment consisting of dust and cocoons of blue algee and siderobacteria from a melt water lake (Blue Lake I) situated about 20 km from the margin of the Sondestromfjord ice field. This lake contained sediments from melt water formed through about 2000 years (e.g., Maurette et al. 1994). Many more lakes were sampled during subsequent years and as of today a total mass of about 250 kg of wet cryoconite from more than 50 locations is available. The cryoconite typically contains fine-grained sand and dust (~10 g/kg) most of it of terrestrial origin. Extraterrestrial matter is present in minor amounts. On overage ~800 cosmic spherules and ~200 partially melted to unmelted MMs are present in 1 kg of wet cryoconite. It is usually easy to recover cosmic spherules and MMs from cryoconite but some mechanical force has to be applied. This and the metabolism of the siderobacteria leads to an unwanted bias in the collection because only tough particles make it into our instruments. In spite of these shortcomings, the Greenland ice sheet remains to be the most prospective location for the collection of inter-planetary matter of the next largest size-range, particles >500 ęm (minimeteorites). A first search was under way this summer (1995). The samples, however, could not yet been studied. The biases introduced by the cryoconite in Greenland could be avoided by searching for MMs in the Antarctic ice shield which is usually free of melt water and hence cannot support sidero-bacteria. The first attempt to recover micrometeorites from the Antarctic ice by melting pockets of ice was highly successful (season December 1987 - January 1988; see also Maurette et al. 1994 for a summary). Sofar about 500 tons of ice have been melted and cosmic spherules and micrometeorites were collected in the size-range 50 - >400 ęm. The concentration of extraterrestrial matter in the blue ice fields of Antarctica is surprisingly high. About 100 cosmic spherules with diameters >50 ęm were collected per ton of ice. The ratio of spherules to partially melted and unmelted MMs is <0.2 in the size-fraction richest (~10%) in extra-terrestrial matter (50-100 ęm). Thus, the total amount of partially melted and unmelted MMs collected up to date is about 100.000, and the search will continue. Future collecting is designed to extend the range in particle size in both directions in spite of the fact that the small (<50 ęm) dust particles from Antarctic ice are heavily dominated by terrestrial eolian dust. Procedures will have to be worked out to extract the extra-terrestrial component from this dust - an important undertaking, because we have good reasons to expect a different mineralogy and petrography to be present among the smaller particles as compared to MMs. This view is strongly supported by studies of stratospheric interplanetary dust particles (SIDPs) of about 10 ęm average diameter (e.g., Zolensky 1994) which consist of two different lithologies, one of them not present among MMs and meteorites. 3. Methods The small size and mass of MMs allows only the application of microanalytical techniques. The investigation of a specific particle usually begins with a study of its shape and surface by optical microscopy. The mass is determined with an ultramicro-balance (typical masses are 1-20 ęg). It is then analyzed for a variety of major and trace elements (up to 35 elements depending on sample mass and element content) by instrumental neutron activation analysis (INAA). After the sample has cooled, its surface is investigated and analyzed by analytical scanning electron microscopy (ASEM). In the next step either the whole particle or portions thereof are embedded in epoxy and polished. The polished sample is studied by optical microscopy and ASEM and the bulk as well as the individual phases present are analyzed by utilizing an electron microprobe X-ray analyzer. Samples can be taken from the polished mounts as well as from splits of the particle and mounted in epoxy, ultramicrotomed and investigated with the transmission electron microscope. The same polished mount or aliquots ca be analyzed by a variety of non-destructive (optical spectroscopy, cathodoluminescence, proton induced X-ray emission, synchrotron X-ray fluorescence analysis, Raman spectroscopy etc.), partly destructive (e.g., secondary ion mass spectrometry - SIMS, a diversity of laser ablation techniques, etc.), and finally totally destructive methods (e.g., rare gas analysis). In the ideal case, as many as possible analytical techniques should be applied in the study of a particular micrometeorite. However, only in a few cases this goal can be achieved. 4. Results Without going into details we present her a selection of the most important results published sofar on micrometeorites. We will refer to other extraterrestrial matter like meteorites and to the small particle fraction of the interplanetary dust (the stratospheric interplanetary dust particles - SIDPs) only when comparing some micrometeorite properties. A large portion of unmelted micrometeorites has suffered severe alteration by heating. Many of them are partially to almost totally melted, consisting of a foamy melt and variable amounts of unmelted phases. Another portion of MMs has been just thermally altered (metamorphosed) without melting. These and the few not altered MMs provide the basis for the general characterization of MMs. We will also just briefly mention the various alterations some MMs suffered in the terrestrial environment. The summary is mainly based on the reports by Maurette et al. (1991, 1993, 1994) and Kurat et al. (1993, 1994a) and a variety of special investigations which will be cited separately. 4.1 Mineralogy and Mineral Chemistry The mineralogy of micrometeorites is surprisingly simple. Major minerals are olivine [(Mg,Fe)2 SiO4], low-Ca pyroxene [(Mg,Fe) SiO3], magnetite (Fe3O4), and hydrous Mg-Fe silicates (phyllo-silicates) like serpentine and saponite (a clay mineral). Individual MMs are usually dense, low-porosity mixtures of all proportions of anhydrous and hydrous phases (Fig. 1). Minor phases comprise Ca-rich pyroxenes, feldspars, sulfides of Fe and Ni, Fe/Ni metal, Mg-Fe hydroxides, Mg-Al and Fe-Cr spinels, perovskite (CaTiO3), ilmenite (FeTiO3), hibonite [Ca(Al,Ti)12O18], and others. The chemical compositions of the major silicates are highly variable in the Fe, Mg, ratios, also within a given particle (unequilibrated mineral assemblage) and are usually very rich in minor elements as compared to terrestrial counterparts. The hydrous minerals contain some elements in chondritic abundances (e.g., Ti, Al, Cr, Ma, K). The refractory minerals like Mg-Al spinel are strongly enriched in refractory trace elements (e.g., rare earth elements, Sc, Zr, Hf, etc. - Kurat et al. 1994b) compared to chondritic rocks. Mineralogy, mineral chemistry, and the presence of refractory mineral and mineral assemblages are typical features of carbonaceous chondrites, in particular CM-type (Mighei-type) carbonaceous chondrites. However, the match is not perfect. Major differences between MMs and CM chondrites exist in the presence of abundant Ca-poor pyroxene in MMs (most CM chondrites do not contain such pyroxenes), in the lack of almost Fe-free olivines with high Al and Ca contents in MMs (they are common in CM chondrites), and in the high abundance of Fe-rich olivines and pyroxenes in MMs. 4.2. Bulk Chemistry Bulk major and minor element abundances (Fig. 2) in phyllo-silicate-rich MMs are mostly chondritic, except for Ca, Na, Ni, and S, which are depleted with respect to CI (and CM) carbonaceous chondrites. Coarse - grained crystalline, anhydrous MMs deviate usually from the chondritic composition, a feature typical also for anhydrous aggregates and chondrules in carbonaceous chondrites. Lithophile trace element abundances in phyllosilicate-rich MMs (Fig. 3) straddle the abundance pattern of CM chondrites and deviate significantly from that only in the abundance of K. However, the abundances of siderophile elements in MMs are significantly fractionated as compared to CI and CM chondrites. Just the highly refractory elements Os and Ir and the highly volatile Se are present at CI and CM chondrite abundances. The common siderophile elements Ni and Co are depleted compared to chondritic abundances and also fractionated from each other (the Ni/Co ratio is non-chondritic). Enriched over chondritic abundances are Fe (moderately) and Au and As (stongly). The depletion in Ni, Co, and S has been shown (Presper et al. 1993) to be due to terrestrial leaching of Ni-bearing Mg-Fe sulfates from the MMs. Indeed, MMs do not contain sulfates which are very abundant in CM and CI chondrites but instead large voids can be seen which must have been occupied by a mineral before the particle came into the laboratory (Fig. 1). Similarily, the depletion of MMs in Ca as compared to CM chondrites is possibly due to leaching of carbonates, minerals which are common in CM chondrites but absent from MMs. The enrichments of MMs in Au, As, and K over chondritic levels must be due to terrestrial contamination. All three elements are strongly enriched in the terrestrial crust as compared to chondrites. A very special compositional feature of MMs (and also SIDPs) is their richness in C. Perreau et al. (1993) and Engrand et al. (1994) showed that MMs have C/O ratios which are on average higher than that of CI chondrites, the most C-rich chondrites. MMs are up to 5x richer in C than CM chondrites - another distinct difference between these two solar system matters. 4.3. Isotopic Compositions A few attemps have been made to measure stable isotope abundances in MMs. A search for D anomalies was negative (Alexander et al. 1992) and subsequent searches (unpublished) were also not successful. This ist in clear contrast to the results obtained from SIDPs which commonly bear anomalies and in some of which weren found the largest anomalies yet seen in solar system matter (Messenger & Walker, this volume). Also, searches for substantial anomalies in isotopic abundances of C and N were negative (Stadermann & Olinger 1992). Anomalies in O isotope abundances have been found in several refractory spinel-rich objects in MMs (Hoppe et al. 1995). These anomalies in 16O abundances are comparable to those from chondrites and SIDPs. Calcium and Ti isotope anomalies, commonly found in refractory inclusions of carbonaceous chondrites have not yet been seen in MMs. Too few attempts have been directed towards detection of isotopic anomalies in MMs and much remains to be done in this field. 4.4 Rare Gas Analysis So far only the concentrations and isotopic composition of Ne have been measured in MMs and cosmic spherules (Olinger 1990, Maurette et al. 1991). Many of the MMs have - not unexpected (Eberhardt & Eberhardt 1988) - very high Ne contents - in excess of 10-5cm-3g-1 at STP, comparable only to a few very gas-rich chondrites and lunar regolith samples. Neon isotope abundances confirmed the extraterrestrial origin of MMs (and some cosmic spherules) as they are comparable to that of solar energetic particles (SEP) neon. In addition, a small contribution from cosmic ray spallation neon could also be identified. Thus, MMs were exposed to cosmic rays and to the solar wind. For the solar wind exposure the particles must have been of the size as recovered. Thus, MMs (and by anology also the SIDPs - see Nier & Schlutter 1990) were true inter-planetary dust meteoroids and cannot be products of the break-up of a larger meteoroid in the atmosphere. 5. Discussion The collection of data on MMs is - unfortunately - still highly incomplete. However, what is available today already puts tight constraints on the nature of the matter constituting the main mass of the interplanetary dust of the solar system. Although there can be (and probably is) a bias in our sample against highly porous and friable particles. Such particles constitute about half of the SIDPs (Brownlee 1985) and are a matter not known from any other extraterrestrial material available to us. It is likely, that this type of matter is not very abundant among the larger inter-planetary dust particles but some can be expected to be around. Their physical weakness, however, prevented their recovery. New recovery procedures should help to settle that question. As to the available matter constituting the micrometeorites, the mineralogical and bulk chemical characteristics unequivocally point towards carbonaceous chondrite matter, in particular CM carbonaceous chondrites. Such chondrites are rare, representing just about 2% of all recent meteorite falls (e.g., Dodd 1981). The most common meteorites, ordinary chondrites (80% of falls) appear to be represented by <1% of MMs (Walter et al. 1995) and other types seem to be even less abundant. Thus, the main mass of matter accreting on the Earth today is representative of a rare meteorite type. This could either mean that CM chondrite-type planetesimals dominate today's source region of the dust or CM chondrites are rare aggregates of the most common dust in the solar system. Of course, the dust could not have survived as such for 4.6x109 a and therefore, must have been stored somewhere for most of its life time and from where it was released in geologic recent times. The CM chondrite parent bodies must be excluded from the possible storage candidates for several reasons. The composition and abundance of minerals do not fit those of CM chondrites. They could represent a primitive solar system matter which was processed in the solar nebula clearly more extensively than the matter which constitutes the CM chondrites. This is indicated by the presence of Ca-poor pyroxene (a reaction product of olivine with the solar nebula gas) and of abundant Fe-rich olivines and pyroxenes (Fe was introduced into the phases at a late stage by Mg-Fe exchange between the solids and the solar nebula gas - see Kurat 1988). In addition, the high C content of MMs precludes their derivation from a CM chondrite parent body and also points towards prolonged processing in and accumulation (organic compounds) from the solar nebula. Finally, of the >500 particles investigated by us sofar, none shows any evidence for physical force - a feature to be expected for dust produced by shattering large, dense rocks. Because the majority of MMs, hydrous and anhydrous, consists of dense particles, a possible parent must be assumed also to have been a dense rock. We are left with not many possibilities which could provide shelter for small particles for a very long time and gently release them in recent times. The only possible way to accomplish these constraints seems to be a storage in an icy body. This way, the particles will be protected and can be gently released by sublimation of the ice. Only a few types of solar system bodies meet these requirements with clearly the best match provided by comets (e.g., Whipple 1950). The high C content of MMs also points into that direction. 6. Conclusions We have good reason to believe that our sample of MMs is biased in favour of the physically tough particles of the interplanetary dust. Nevertheless, the sample we have reveals a clear picture which by all likelihood will not be fundamentally altered by addition of the possibly missing matter. Thus, it can be firmly stated that the matter accreting onto the Earth today bears some similarities to the rare CM carbonaceous chondrites but differs from them in so many ways that it must be considered a solar system matter of its own. The features making it different from chondrites are likely to be of primordial origin. This includes the mineral abundances, mineral chemistry, and the bulk C content. Some deviations of MM composition from that of chondrites are due to extraction of - water soluble - sulfates and carbonates. We cannot be sure about where this extraction took place. If MMs come mainly from comets, the loss of water soluble phases could already have happened on the comet parent. However, the terrestrial environment clearly offers more efficient possibilities. We do not have any evidence for the source of MMs. However, we have good reasons to favour comets as the source of most of the inter-planetary dust in the solar system - in accordance with conclusions reached by others on the basis of different data sets (e.g., Whipple 1967, Bradley & Brownlee 1986). 7. Outlook Much is left to be done on MMs with many fields not properly explored. In particular, TEM investigations are due to characterize the major phases, very fine-grained phases, the C-bearing phases, and measure solar flare and cosmic ray tracks. The carbonaceous matter which is apparently present in large amounts in MMs, has not been characterized, although investigations are under way. The search for isotope anomalies in H, C, O, N, and others elements needs to be intensified in order to identify presolar grains (some hints were found by Yates et al. 1994) and molecules. Finally, investigations of the abundances and isotopic composition of He, Ar, Kr, and Xe need to be done. In addition we have to continue to search for particles which were deliberately or unintentionally excluded from our collections. These will include highly friable MMs (if they exist), small particles (<50 ęm) as the bridge to SIDPs, possible inter-stellar particles, and samples of particles >500 ęm in diameter, the minimeteorites, which should provide us with a link to meteorites. It is of particular importance to fill the gaps in the fragment size distribution because these transitional ranges apparently hide also transitions in mineral abundances and bulk chemical composition. Furthermore, the potential of MMs to provide the ingredients for the formation of life on Earth - either through direct delivery of amino acids or acting as catalyzers - needs to be investigated. Acknowledgements This work was done with the help of Franz Brandst„tter, Christian Koeberl, Jrgen Walter, Thomas Presper, and Michel Perreau. Support was recieved from IN2P3, CNES, IFRTO and the European Community SCIENCE Program in France and from FWF in Austria. References Alexander, C.M. O'D., Maurette, M., Swan, P., & Walker, R.M. 1992 Lunar Planet. Sci., XXIII, 7 Bradley, J.P. & Brownlee, D.E. 1986, Science, 231, 1542 Brownlee, D.E. 1985 Ann. Rev. Earth Planet. Sci., 13, 147 Dodd, R.T. 1981, Meteorites, Cambridge: Cambr. Univ. Press, 368pp Eberhardt, A. & Eberhardt P. 1988 Lunar Planet. 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Weinberg (ed.), Houston: NASA SP-150, 409 Yates, P.D., Arden, J.W., Wright, I.P., Pillinger, C.T., & Huchison, R. 1992, Meteoritics, 27, 309 Zolensky, M.E. 1994, in Analysis of Interplanetary Dust, M.E. Zolensky, T.L. Wilson, F.J.M. Rietmeijer, & G.J. Flynn (eds.), New York: Amer. Inst. Physics, 1994, ... Figure captions Fig. 1: Phyllosilicate-rich micrometeorite with abundant platy and framboidal magnetites (white) typical of CI and CM chondrites. Note the large voids, probably the sites of water soluble minerals. Scanning electron microscope image of a polished mount. Scale bar is 10 ęm. Fig. 2: Chondrite-normalized major and minor element abundances in phyllosilicate-rich and coarse-grained crystalline micro- meteorites (electron microprobe data from Kurat et al. 1994). Lithophile (left) and siderophile (right) elements are arranged in order of increasing volatility. Fig. 3: Chondrite-normalized abundances of selected trace elements in phyllosilicate-rich micrometeorites (INAA data from Kurat et al. 1994). 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