Lithos 85 (2005) 1 14 www.elsevier.

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Extrusive carbonatites: A brief review

A.R. Woolleya,*, A.A. Churchb
a

Department of Mineralogy, Natural History Museum, Cromwell Road, London SW7 5BD, UK b Le Grand Crolier, Rue de la Trigale, Torteval, Guernsey, GY8 0PX, Channel Islands, UK Received 27 February 2004; accepted 11 March 2005 Available online 14 June 2005

Abstract 49 known extrusive carbonatite occurrences are listed with brief details of their tectonic setting, structure, lithologies, associated silicate rocks, chemistry and presence or absence of included mantle materials. Half the occurrences appear to be related to tephra cones, tuff rings, diatremes and maars and the rest occur within strato-volcanoes. Pyroclastic carbonatitic rocks are present at all the localities, with carbonatite lava flows occurring at only 14 of them. The pyroclastic rocks, which include fallout tephra and deposits from pyroclastic surges and flows and products of phreatomagmatic eruptions, vary from rocks composed principally of carbonate to varieties with as little as 20% igneous carbonate. The most abundant silicate rocks associated with extrusive carbonatites are melilite-bearing rocks, nephelinite and/or ijolite, and phonolite and/or nepheline syenite; seven occurrences have no associated silicate rocks. 16 occurrences, most of them associated with small extrusive centres, contain mantle xenoliths or megacrysts, details of which are tabulated, with spinel lherzolite the most abundant rock type, but amphibole, phlogopite and garnet are also recorded. The lack of such materials in intrusive carbonatites may reflect their less energetic environment of emplacement. It is proposed that carbonatites are essentially of two types: (a) those rising energetically and rapidly from the mantle, which form small explosion craters, ash or tuff cones, or diatremes, have only lowvolume associated silicate rocks, and entrain mantle debris, and (b) those which occur in strato-volcanoes, are associated with large volumes of silicate rocks and follow a more complex genesis, probably involving ponding and differentiation (separation from carbonate-bearing silicate magma) at higher levels in the mantle and/or crust. Most of the classic intrusive carbonatite complexes probably fall into the second category. D 2005 Elsevier B.V. All rights reserved.
Keywords: Carbonatite review; Extrusive carbonatite; Pyroclastic; Lava

1. Introduction It has long been appreciated that most chemical analyses of carbonatite do not represent the composi* Corresponding author. E-mail address: a.woolley@nhm.ac.uk (A.R. Woolley). 0024-4937/$ - see front matter D 2005 Elsevier B.V. All rights reserved. doi:10.1016/j.lithos.2005.03.018

tions of the primary liquids from which they are derived. For instance, most intrusive carbonatites have fenite aureoles that indicate loss of alkalis (e.g., Woolley, 1969), and probably other elements, while it is probable that the carbonate textures displayed by most large intrusive bodies of carbonatite are the result of extensive re-crystallization (Barker,

2 Table 1 World occurrences of extrusive carbonatite with brief details of tectonic setting, structure, nature of extrusive carbonatite, associated silicate rocks and presence or absence of mantle debris Locality Tectonic Structure Nature of setting extrusive carbonatite C T R? ? F R R nR R R T nR C C R ? ? R nR O? O? T R R R R SVE ? SVE V V V SVE SVE SVE SVE SVE SVE V SVE V V V V SVE? V V SVE SVE SVE SVE V Nature of carbonate Extrusive silicate rocks Me A,M,N N,Te,P M N,M,T M,P M M Lc B,P M,N,Lc,B P TB,D Lc M,N ? B N,TB,A M M,N M,Lc,K M,N,P,Ba,T Intrusive silicate rocks Me NS Px,M P,A M,E,T P,M M Lc,P Px,Mlt,NS,Sy Sy Px,NS Intrusive Mantle Selected references carbonatite debris C C C D,Ank? C,Al C C C C,Ank C C,Al X X X X X X X X X X X Dimroth, 1970 Hoy and Pell, 1986 Stewart, 1970 Gaspar and Danni, 1981 Fletcher et al., 1981 Keller, 1989 Keller et al., 1990 Riley et al., 1996 Stoppa and Woolley, 1997 Stoppa and Woolley, 1997 Stoppa and Woolley, 1997 Stoppa et al., pers. comm., 2003 Chazot et al., 2003 Bailey et al., 2003 Vikhter et al., 1976 Vikhter et al., 1976 Yu et al., 2003 Pyatenko and Saprykina, 1976 Yarmolyuk et al., 1997 Woolley et al., 1991 Nasir and Klemd, 1998 Mourtada et al., 1997 Nixon and Hornung, 1973 von Knorring, 1967 Stoppa et al., 2003 Deans and Roberts, 1984 A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26

Castignon Lake, Canada Mount Grace, Canada Qagssiarsuk, Greenland Santo Antonio da Barra, Brazil Cerro Manomo, Bolivia Kaiserstuhl, Germany Hegau, Germany Auf Dickel, Germany San Venanzo, Italy Cupaello, Italy Monticchio, Italy Oricola, Italy Chabrieres, France ` Calatrava, Spain Khan Neshin, Afghanistan Dasht-I-Nawar, Afghanistan Lixian, China Kontozero, Russia Khaluta and Arschan, Russia Uyaynah, U.A.E. Hatta Zone, U.A.E. Tamazert, Morocco Fort Portal, Uganda Katwe-Kikorongo, Uganda Bunyaraguru, Uganda Tinderet, Kenya

P cc,ank P cc P,L cc,(dol) L cc P,L dol,ank? P(Lp, Ash) cc P cc P(Lp, Ash) cc P cc P cc P cc P cc P dol P cc? P,L cc,ank P cc? P,L cc P,L P cc P cc P cc Lp Dol,ank (cc) P,L cc P cc P cc P cc

27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 A B C D

Homa Mountain, Kenya Nyamaji, Kenya Ruri, Kenya Rangwa, Kenya Shombole, Kenya Oldoinyo Lengai, Tanzania Kerimasi, Tanzania Sadiman, Tanzania Arusha-Monduli, Tanzania Hanang, Tanzania Kwahera, Tanzania Basotu tuff cones, Tanzania Kaluwe, Zambia Mwambuto, Zambia Chasweta, Zambia Gross Brukkaros, Namibia Goudini, South Africa Kruidfontein, South Africa Melkfontein, South Africa Catanda, Angola Santiago, Cape Verde Islands Brava, Cape Verde Islands Mont Auber de la Rue, Kerguelen Chagatai, Uzbekistan Polino, Italy Natron-Engaruka, Tanzania Laacher See, Germany

R R R R R R R R R R R R R R R C C C C C? O O O nR nR R nR

V V V V V V V V SVE V V SVE ? SVE,V SVE,V SVE V V SVE V V V V SVE SVE SVE V

P P P P Ash P,L P,L P P P,L P,L P P,L P P P P P P P,L P L P P P P P

cc cc cc,ank cc cc Alk cc (dol) cc cc cc cc cc,dol cc,(dol) dol,ank dol,ank dol,cc cc cc cc cc? dol cc dol cc cc cc cc

N,P,M N,P P,N N,M N,P,F N,P N,P,M M,N,P M,B N N,M N P,T,R N P,N H N,M P

I I NS,P I,NS,M I,Mlt,M,Px, M,I L Px,NS Sy Ti,P N I,Sy,NS T

C,Al,F C C,Al,F C,Al,F C C,Al,D C C D,Ank C D(C ) C C D C C C

X X X X X X X X

Clarke and Roberts, 1986 Le Bas, 1977 Le Bas, 1977 Le Bas, 1977 Peterson, 1989 Bell and Keller, 1995 Church, 1996 Hay, 1978 Rudnick et al., 1993 Thomas et al., 1966 Mudd and Orridge, 1966 Downie and Wilkinson, 1962 Turner and Rex, 1991 Bailey, 1989 Bailey, 1989 Stachel et al., 1995 Verwoerd, 1993 Verwoerd, 1993 Boctor et al., 1984. Silva, 1973 Silva et al., 1984 Hoernle et al., 2002 B.N. Moine, pers. comm., 2003 Djuraev and Divaev, 1999 Stoppa and Lupini, 1993 Dawson and Powell, 1970 Taylor et al., 1967

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114 3

For significance of bottom four localities (AD) see text. Tectonic setting column: R rift; nR near rift; O oceanic; C cratonic; T thrust belt; F fold mountains. ? Not clear. Nature of extrusive carbonatite column: P pyroclastics; L lava; Lp lapilli tuff; Ash ash. Extrusive silicate rocks column: M melilitite or melilite nephelinite; N nephelinite; Te tephrite; P phonolite; T trachyte; B basalt; Ba basanite; TB trachybasalt; Me meimechite; A analcimitite; Lc leucitite; D dacite; H hawaiite; R rhyolite. Intrusive silicate rocks column: Px pyroxenite; Mlt melteigite; I ijolite; E essexite; Sy syenite; M melilitolite; L lamprophyre; P phonolite; NS nepheline syenite; Ti tinguaite; T trachyte; A analcime-bearing phonolite. Intrusive carbonatite column: C calciocarbonatite; Al alvikite; Ank ankerite carbonatite; D dolomite carbonatite; F ferrocarbonatite. Mantle debris column: X mantle debris identified.

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

1989). Many carbonatite intrusions appear to have undergone some degree of alteration resulting in the development of, amongst others, secondary minerals of the RE and other rare elements, while dolomitizationT can be seen at, for instance, Jacupiranga. Because carbonate glasses are unknown in nature, an approach to primary compositions via quenched melt products is difficult, although some dykes may possibly be close to primary in composition. We believe, however, that considerable information can be gleaned about primary carbonatite magma compositions from a study of the extrusive products, a point already stressed by Bailey (1993) who noted that bEvidence from effusive carbonatite is essential for understanding the wider aspects of carbonatite magmatism, and for identifying the most relevant applications of the results from experimental petrologyQ. We find that considerable petrogenetic information is indeed provided by the extrusives that is not revealed by a study of intrusive carbonatites. Although the Oldoinyo Lengai volcano and its pristine natrocarbonatite lavas is well known, few other occurrences of extrusive carbonatite have been investigated in such detail, and it does not seem to be widely appreciated how many such occurrences have in fact been recognised. Of the N500 carbonatites that have been described (Woolley and Kjarsgaard, in press.) only some 10% are solely extrusive or include an extrusive component. It is probable that some of the carbonatites considered at present to consist only of intrusive rocks will prove, on further work, to include some extrusive components. Further, the nature of the carbonate mineral phases in some alkaline volcanic rocks, particularly tuffs, will prove to be of a primary carbonatitic nature. We are aware of 49 localities (Table 1) that include extrusive carbonatite and feel confident that this number will increase substantially once it is more widely appreciated that the carbonate in some pyroclastic sequences is of primary magmatic origin. Outside the Russian literature modern investigations of extrusive carbonatites can be considered to begin with papers by Keller (1981) and Deans and Roberts (1984). The work of the latter does not seem to have been fully appreciated partly, we suggest, because of the general disagreement with their identification of certain rectangular crystals or crystal aggregates of calcite as being after nyerereite, a ubiq-

uitous phase in the recent Oldoinyo Lengai natrocarbonatite lavas. This calcite is now generally considered to be primary (e.g., Bailey, 1993), but the disagreement seems to have precluded the widespread appreciation of the fact that Deans and Roberts had correctly recognised several carbonatitic tuff sequences in East Africa. A most useful and well illustrated review of extrusive carbonatites is that of Keller (1989) who pointed out that carbonatitic lavas, ashes, tuffs, tuff breccias and phreatomagmatic deposits occur and that teardrop lapilli, juvenile carbonatite bombs, agglutinated lapilli tuffs, welded spatter and agglomerates are common and characteristic of carbonatite volcanic activity. He also noted that quenched juvenile fragments in carbonatite pyroclastic deposits are important in constraining the physical properties and original chemical composition of carbonatite melts. Keller (1989) refers to some of the principal occurrences of extrusive carbonatite then known and is thus a source of many references on these occurrences. Bailey (1990), in discussing the extrusive carbonatites of southeast Zambia, noted the importance of considering those carbonatites that are apparently generated directly in the mantle and in that paper, and a later review (Bailey, 1993), discussed at some length the importance of the extrusive carbonatites when considering a whole range of carbonatite petrogenetic problems. Many of Baileys conclusions, such as the importance of the distinction of dprimaryT and dderivedT (high level) carbonatites, possible relationships to kimberlites, and the role of rapid eruption are, we feel, substantiated by consideration of the extrusive carbonatites as a whole. The present paper lists 49 occurrences of extrusive carbonatite (Table 1), all that we have been able to trace from the literature. The principal objective is to categorise these occurrences, with a view to trying to discern patterns that might promote a further understanding of their nature and genesis, while also investigating any differences from intrusive carbonatites that might also have genetic significance. Special mention must be made of four occurrences, which are given at the foot of Table 1, the classification of which is not certain. The Chagatai (Uzbekistan) and Polino (Italy) occurrences are certainly carbonatites but essentially intrusive. However, the fascinating Chagatai centre (it contains diamonds

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

and melilite) comprises a series of dykes and two ddiatremesT which Djuraev and Divaev (1999) indicate are sub-volcanic, while the Polino occurrence consists of a dvery shallow-level diatremeT, according to Stoppa and Lupini (1993). Although there is no evidence at present for a truly extrusive carbonatitic facies at either of these localities, it appears very likely that there was an extrusive component, that has not been preserved, which probably had a composition close to, if not identical with, that of the diatreme rock. (F. Stoppa, pers. comm., 2004). The Natron-Engaruka explosion craters in Tanzania include a suite of tuff rings, tuff cones and maars (Dawson and Powell, 1970) and in some cones there are extensive carbonate-rich tuffs. It is probable that these tuffs will prove to be carbonatitic, but at present a definitive description is lacking. Carbonatite has been described from the pyroclastic rocks of the Laacher See volcano in Germany (Taylor et al., 1967) but this comprises xenoliths of sovite, so there is no direct evidence that a carbonatitic melt reached the surface (J. Keller, pers. comm., 2004). For these various reasons these four localities have not been included in the main list of extrusive carbonatite occurrences, but they are shown at the bottom of Tables 1 and 4. It should also be noted that the Igwisi Hills in Tanzania have been omitted. This locality has been described as including carbonatite but it is now generally thought to be kimberlitic (Dawson, 1994). The Jabal El Arab locality in Syria has been identified as including extrusive carbonatite (Mahfoud and Beck, 1995), but we consider that it is probably not so; it has, therefore, also been omitted.

2. Distribution, form and lithology The setting and distribution of extrusive carbonatite occurrences does not appear to differ significantly from those of intrusive carbonatites. They are almost invariably intra-plate and on the African continent, where 35% of all known carbonatite occurrences are located, appear to be concentrated in zones marginal to the ancient craton cores. There is a very clear relationship to continental rifts, about two thirds lying within or closely adjacent to them. Carbonatites are found in the Cape Verdes, Canary Islands and

Kerguelen, but these are the only occurrences known in an oceanic setting. For the purposes of this paper, occurrences of extrusive carbonatite have been divided into two types: those associated with large volcanoes, generally strato-volcanoes, and those forming, or associated with, smaller volcanic edifices such as tephra cones, tuff rings, diatremes and maars. There appears to be no general volcanic term for the latter so these are referred to in Table 1 simply as bSVEQ - smaller volcanic edifices. Extrusive carbonatites generally form only a small part of the volcanic succession in either large volcanoes or SVEs. An exception is the Fort Portal occurrence which comprises numerous carbonatitic tuff cones and volcanic craters, a single carbonatite lava flow, and 142 km2 of carbonatitic tuffs, apparently with no contemporaneous silicate lavas or tuffs. In the large volcanoes (30 are listed in Table 1) the carbonatitic facies is predominantly pyroclastic, with lava flows present in only 11 occurrences, although the identification of some of the carbonatite as lava is not always conclusive. Even in Oldoinyo Lengai, which is well known for its recent carbonatite lavas, carbonatitic tuffs and breccias are probably the more voluminous. The Kontozero complex in Russia is instructive in so far as it consists of a 55 km2 caldera containing a 2 km thick succession of which some 10% comprises carbonatite tuffs and lavas. In carbonatite-bearing SVEs also pyroclastic rocks are predominant, with carbonatite flows being found at only two of the 18 such localities listed in Table 1. Thus the field evidence for the SVEs, in particular, is for a generally explosive regime, which is supported by the widespread occurrence of debris of mantle origin. The identification of some of the Fort Portal carbonatitic tuffs as ignimbrites (Barker and Nixon, 1989) also points to a high energy, gas-charged extrusive environment. The observed carbonatitic ashes and tuffs vary from varieties in which the carbonate is minor to types, almost invariably lapilli tuffs, consisting of a high proportion of carbonate. Primary carbonates in the ashes is commonly in the form of broken crystals and fragments as well as lapilli and fragments of carbonatite rock. There is generally also a secondary carbonate cement. The rest of the rock tends to consist of a wide range of crystal and lithic fragments of

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114 Table 3 Comparison of abundances of silicate rock types present in occurrences of extrusive and intrusive carbonatites Combined number of intrusive and extrusive silicate rock types associated with the 49 occurrences that include extrusive carbonatite Melilitite and melilitolite Nephelinite and ijolite/melteigite Phonolite, tinguaite, tephrite and nepheline syenite Trachyte and syenite No associated silicate rocks 21 21 21 43% 43% 43% Number of occurrences of silicate rocks associated with 337 intrusive carbonatites* 28 116 147 8% 34% 44%

primary igneous origin, as well as abundant accidental material, presumably from the walls of the feeder conduit. Some detailed petrographic descriptions are given by Deans and Roberts (1984) and there are descriptions and some excellent photomicrographs in Keller (1989). A feature of many of the lavas is the presence of euhedral to subhedral calcite phenocrysts which appear to be of undoubted primary origin, and not pseudomorphs after nyerereite, as originally suggested by Deans and Roberts (1984). The presence of nyerereite and gregoryite phenocrysts in the recent lavas of Oldoinyo Lengai appear to be unique to that volcano, whilst the Fort Portal lava and lava bombs are apparently also unique their mineral assemblages including primary spurrite and periclase.

6 7

12% 14%

109 68

32% 20%

*Data taken from Woolley (2003, Table 4), which based on 337 carbonatite occurrences lacking extrusive carbonatite (see Woolley, 2003, Table 1).

3. Associated silicate rocks Table 2 indicates the nature and abundance of the extrusive and intrusive silicate rocks found in association with the 49 extrusive carbonatite occurrences. The relative abundances of the silicate rocks associated with the extrusive carbonatite occurrences appear to differ little, at least statistically, from the silicate rocks associated with intrusive carbonatites (i.e., carbonatite occurrences with no extrusive carbonatite component). In Table 3 the data for both the extrusive and intrusive silicate rocks associated with the extruTable 2 Nature of silicate rocks associated with occurrences of extrusive carbonatite Associated extrusive silicate rocks Melilite-bearing rocks Nephelinite Phonolite and tephrite Trachyte Basalt, basanite and trachybasalt Meimechite Analcimitite Leucitite Other rock types No silicate rocks 18 21 14 3 7 1 1 4 3 11 Associated intrusive silicate rocks Melilite-bearing rocks Ijolite and melteigite Phonolite/tinguaite/ nepheline syenite Trachyte and syenite Essexite Meimechite Analcime-bearing phonolite Lamprophyre Pyroxenite No silicate rocks 7 6 11 4 1 1 1 1 4 27

Numbers indicate number of occurrences at which rock type occurs.

sive carbonatites (Tables 1 and 2) have been combined and are shown in columns 2 and 3 in terms of number of localities and percentages of the total number of localities. Table 3 indicates that 21 extrusuve carbonatite occurrences, representing 43% of the total, include melilite-bearing rocks (melilitite, melilite nephelinite and melilitolite). In contrast, only 8% of occurrences of intrusive carbonatite are associated with melilite-bearing rocks. Of the 18 centres categorised as SVEs (Table 1) 10 include melilitite, whilst four lack associated silicate rocks. One third of the carbonatite-bearing centres classified as strato-volcanoes contain melilitite-bearing rocks, although nephelinites are generally the most voluminous rock type. The possible significance of the apparent relative abundances of melilite-bearing rocks in the extrusive and intrusive carbonatite associations will be discussed later, but it is stressed that, in the opinion of the authors, the clear association of extrusive carbonatites with melilite-bearing rocks is of considerable significance when the petrogenesis of the carbonatites comes to be considered. Of the 29 extrusive carbonatite localities which do not include melilite-bearing silicate rocks eight are associated with nephelinites, 14 contain phonolite, generally in combination with nephelinite, melilite rocks or both, and eight occurrences include neither extrusive nor intrusive silicate rocks. The relative abundances of nephelinite (ijolite/melteigite) and phonolite, tephrite and tinguaite (nepheline syenite) occurring in the intrusive and extrusive carbonatite

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associations are closely similar (Table 3), as are the proportions of occurrences with which no silicate rocks are associated. In contrast, there is a difference in the abundance of trachyte and syenite in the extrusive and intrusive carbonatite associations, only 12% of the former but 32% of the latter including these rock types, and this is the second noteworthy difference which this examination of the data brings to light.

4. Mantle debris There has not, as far as we aware, been any general investigation of mantle xenoliths and megacrysts in carbonatitic rocks, so that they are not distinguished as a particular category in, for instance, the comprehensive volume on mantle xenoliths edited by Nixon (1987), although there have been de-

tailed studies of mantle assemblages from particular localities e.g., Monticchio, Italy (Jones et al., 2000) . Carbonatites, however, clearly hold considerable potential for mantle petrogenetic studies. We are unaware of any identifiable mantle debris, in the form of xenoliths or xenocrysts, having been described from intrusive carbonatites, with the following exceptions. Some material is found in the small, dtypeT, damkjernite intrusion near the Fen carbonatite complex, Norway and in dykes and intrusions of alnoite near the Alno complex, Sweden (Griffin and Kresten, 1987). The Chagatai and Polino diatremes have already been mentioned, the former remarkable for containing diamonds, and it is considered probable that true extrusive facies were generated at these localities. Sixteen of the extrusive carbonatite occurrences listed in this paper do contain mantle-derived material. Table 4 lists these localities and includes brief mineralogical details.

Table 4 Extrusive carbonatite occurrences with brief details of the mantle materials they contain Locality 7 9 10 11 12 14 20 22 23 24 25 33 35 40 41 46 A B C Hegau, Germany San Venanzo, Italy Cupaello, Italy Monticchio, Italy Oricola, Italy Calatrava, Spain Uyaynah, U.A.E. Tamazert, Morocco Fort Portal, Uganda Katwe-Kikorongo, Uganda Bunyaraguru, Uganda Kerimasi, Tanzania Arusha-Monduli, Tanzania Mwambuto, Zambia Chasweta, Zambia Catanda, Angola Chagatai, Uzbekistan Polino, Italy Natron-Engaruka, Tanzania Structure SVE SVE SVE SVE SVE SVE V SVE SVE SVE SVE V SVE SVE,V SVE,V V SVE SVE SVE Nature of mantle debris Spinel lherzolite xenoliths and cores to lapilli and grains of Cr-spinel, Cr-diopside and orthopyroxene Ultramafic nodules and crystal fragments of olivine (FoN92), Cr-diopside and phlogopite Rare Cr-diopside and Cr-spinel grains Xenoliths of Cr-diopside, orthopyroxene, olivine, Cr-spinel. Also Cr-diopside, olivine and Cr-spinel cores to lapilli Xenocrysts of Cr-diopside Xenoliths of wehrlite and lherzolite; xenocrysts of Cr-spinel Grains of Cr-spinel Grains of Cr-spinel Spinel lherzolite xenoliths Xenoliths of clinopyroxenite with phlogopite and minor apatite, Ti-magnetite and titanite Xenoliths of clinopyroxenite with phlogopite, wehrlite and phlogopite dunite Pargasite and clinopyroxene xenocrysts Xenoliths of harzburgite, lherzolite, wehrlite, olivine orthopyroxenite, clinopyroxene dunite Xenocrysts of Cr-spinel Xenocrysts of Cr-spinel Xenocrysts of Cr-spinel and Cr-diopside Diamond Xenocrysts of olivine and phlogopite Xenoliths of clinopyroxenite with amphibole and phlogopite; amphibole peridotite; dunite

V volcano; SVE small volcanic edifice.

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

Information on the mantle materials found at the Chagatai, Polino and Natron-Engaruka localities (mentioned earlier) have been appended to Table 4. Spinel lherzolite xenoliths, and xenocrysts derived from them, are the most abundant mantle rock type (Table 4), but amphibole and phlogopite have been found in some occurrences. The presence of pyrope in a xenolith from Monticchio, Italy (Jones et al., 2000), suggests sampling of the mantle at greater depths at these localities, as does the occurrence of diamond at Chagatai. Pargasite xenocrysts at Kerimasi and Monticchio all suggest that metasomatised mantle is being sampled, as do the phlogopite-bearing xenoliths at Katwe-Kikorongo and the phlogopite xenocrysts at San Venanzo. The minor apatite, Timagnetite and titanite in the Katwe-Kikorongo xenoliths probably have a similar metasomatic origin (Lloyd et al., 1987). The presence of mantle phases in these carbonatitic rocks is clear evidence of direct eruption from a mantle source and suggests that these carbonatites have not undergone dhigh levelT (crustal?) fractionation processes. It is noteworthy that most of these occurrences take the form of SVEs (Table 4) and hence the entrained mantle debris probably survived because of rapid transport to the surface. The occurrences with mantle inclusions are also characterised by an association with melilite-bearing silicate rocks, 11 of the 16 listed in Tables 1 and 4 revealing such an association. The apparent lack of mantle xenoliths and xenocrysts in intrusive carbonatites is probably a reflection of the physical processes of magma transport and emplacement. Intrusive carbonatite complexes are likely to have been emplaced relatively passively, in comparison with SVEs, and probably involve one or more stages of ponding and differentiation of the magma within the mantle or crust, or both, before final emplacement. Any solid mantle fragments would thus almost invariably be altered or, if not, such high density material would rapidly settle gravitationally in low density and allegedly ultra-low viscosity carbonatite magma. If differentiation of a carbonated silicate magma is involved, whether by crystal fractionation or a process of liquid immiscibility, then the mantle materials would probably remain in the silicate fractionation and so be efficiently separated from the carbonate portion.

5. Chemistry Chemical analyses of 64 extrusive carbonatite lavas and fragmental rocks (tuffs, ashes, breccias) have been found in the literature, of which 26 are from Fort Portal (Nixon and Hornung, 1973). We also have access to a further 29 analyses of Fort Portal lavas and tuffs (collected by N. Eby, F.E. Lloyd, F. Stoppa and A.R. Woolley) which are as yet unpublished. Because tuffs, in particular, generally contain a proportion of entrained debris, they probably do not represent liquid compositions and it is clearly difficult to manipulate the data in a meaningful way. An idea of the range of compositions represented is illustrated by a plot of SiO2 against CaO (Fig. 1). The plot demonstrates the variation from relatively dpureT carbonatites with N 50 wt.% CaO, and hence N 90%

Fig. 1. Plot of SiO2 against CaO (wt.%) for published analyses of extrusive carbonatites. Carbonatite lavas and pyroclastic rocks are distinguished and the abundant data from Fort Portal (Nixon and Hornung, 1973 and unpublished data) are also differentiated. A clear trend is apparent but the analysis of Oldoinyo Lengai natrocarbonatite lava and four other analyses, which are named individually, lie off this trend. Santiago (S), Goudini (G) and Mwambuto (M) are dolomitic carbonatites. The main rock type at Castignon Lake (C) is dmeimechiteT, the categorisation of which is problematical. For further discussion see text. References: lava from Castignon Lake, Canada (Dimroth, 1970); dolomitic tuff from Mwambuto (Bailey, 1990); dolomitic tuff from Goudini, South Africa (Verwoerd, 1967); dolomitic carbonatite lava from Santiago, Cape Verde Islands (Kogarko, 1993).

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

calcite, to carbonatitic rocks with only some 20 wt.% of CaO. The former rocks cluster, in terms of Fig. 1, around an average calcite carbonatite composition for intrusive carbonatites (Woolley and Kempe, 1989). It should be noted, however, that Woolley and Kempe (1989) excluded carbonatites with N 10% SiO2 for purposes of calculating their average and it could be that some of the silica-rich carbonatites do in fact represent primary liquids and not simply carbonatite liquids plus entrained silicate debris. The fragmental rocks define a very clear trend from rocks with negligible silica to those with silica values approaching 40%, and it is the data for the Fort Portal tuffs that dominate the values from about 15% to 38% SiO2. The other very high silica tuffs are from San Venanzo and Monticchio in Italy (Stoppa and Woolley, 1997) and Gross Brukkaros, Namibia (Stachel et al., 1995). Although data on these high silica carbonatitic tuffs are scarce, apart from Fort Portal, this scarcity does not reflect the abundance of these rocks, merely the fact that they have been widely ignored, probably because the abundance of entrained debris would seem to preclude any chemical data as being meaningful. The well-defined trend on Fig. 1 from zero SiO2 and about 55% CaO to around 40% SiO2 and about 18% CaO probably reflects mixing of carbonatite liquid and crustal debris and, for Fort Portal rocks, a lesser amount of mantle material. The tuffs from Mwambuto and Goudini that plot on Fig. 1 well below the overall trend are dolomitic, and hence the CaO is partly replaced by MgO. Excluding the data for the Fort Portal lavas, and the lavas from Santiago and Castignon Lake (Fig. 1) which are dolomitic, it is apparent that the analysed lavas do not generally extend to such high values of silica as the tuffs, although the data are scarce. The Fort Portal analyses (Nixon and Hornung, 1973, and unpublished data) also demonstrate that generally the lavas are lower in SiO2 than the tuffs, the Fort Portal lavas having SiO2 values that average 15.54%, whereas the tuffs average 24.9% SiO2. The principal reason for this difference is undoubtedly that the more energetically erupted tuffs contain a significantly higher proportion of entrained crustal and mantle material. Although the lavas are probably closer in composition to primary carbonatitic liquid than the tuffs, it is difficult to decide what proportion of the silica represents secondary material. Intrusive calcite carbonatites

generally have much lower silica values than the Fort Portal extrusives, 116 analyses giving an average of 2.72% SiO2 (Woolley and Kempe, 1989). Although this average was reached after excluding carbonatites with N10% SiO2, in fact there are not very many such analyses in the literature, the majority being represented by dykes associated with the Alno complex (von Eckermann, 1958), so that the average is not increased substantially if such rocks are included. We surmise that the silica value of primary intrusive carbonatite liquids is rather higher than the calculated average carbonatite, but is reduced through gravitational settling of silicate phases while, conversely, the value for the extrusives was enhanced by incorporation of crustal material. On a plot of SiO2 against MgO (wt.%) (Fig. 2) a clear positive correlation is indicated for the low silica extrusive carbonatites, which are essentially calciocarbonatites. This trend extends to the Fortal Portal lavas,

Fig. 2. Plot of SiO2 against MgO (wt.%) for published analyses of extrusive carbonatites. The majority of the data define a positive trend (dot-dash arrow) passing through the carbonatitic lavas of Fort Portal, and this trend corresponds to increasing contamination with debris of mantle origin (olivine, pyroxene etc.). However, the carbonatitic tuffs from Fort Portal form a distinct trend from the lavas towards higher SiO2values, which is explicable in terms of contamination with crustal materials. The carbonatite tuffs at Mwambuto are dolomites and heavily contaminated with K-feldspar, and thus lie on a dolomiteK-feldspar trend (dashed arrow). Localities indicated by letters as on Fig. 1.

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A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

and is explicable in terms of increasing amounts of debris of mantle, and possibly cognate, origin (olivine, pyroxene, phlogopite etc.). The Fort Portal tuffs, however, show a decrease of MgO with increasing silica, probably reflecting an increase in contamination by crustal materials, particularly quartz and feldspar. The only strongly dolomitic carbonatite represented is that from Mwambuto, Zambia (SiO2 17.2%, MgO 12.9%; Bailey, 1990), and this appears to lie on a trend from dolomite to K-feldspar, the two principal phases of this rock. The Fort Portal lavas appear to show evidence of a trend of increasing MgO with increasing SiO2. This trend may reflect the greater importance of mantle debris (high in MgO) in the lava in comparison with the tuffs (low in MgO high in SiO2). Both Figs 1 and 2 make clear the distinct chemistry of the Fort Portal carbonatites and the difference between the lava and tuffs. It is unfortunate that this is the only suite of extrusive carbonatites in the world that have been investigated chemically in any depth. Fig. 1 underlines the uniqueness of the chemistry of the Oldoinyo Lengai natrocarbonatite lavas, this property, or otherwise, having been widely discussed in the literature. We are of the opinion that the Lengai lavas are not unique and that similar lavas have been erupted elsewhere in the past. For instance, the limestones that form a carapace on the adjacent volcano of Kerimasi are considered to have been originally natrocarbonatitic. The ubiquity of fenite aureoles indicates that most intrusive carbonatite magmas contain alkalis, but there is probably a spectrum of abundances from a few percent to values in the 3040 wt.% range as represented by the Lengai natrocarbonatites. Although the mixed nature of many carbonatite and carbonatitic tuffs makes them difficult to interpret, while the fact that most have also been subjected to some degree of weathering exacerbates the difficulties further, the relatively abundant data from Fort Portal suggest that much more information could be gleaned from these rocks. The lavas, in particular, should certainly afford much more insight while Keller (1981) has demonstrated that some idea of melt composition can be obtained by analysis of carbonatite lapilli, which are to be found at a number of localities. Dolomitic carbonatites are relatively rare amongst intrusive carbonatites and, apart from Mwambuto, hardly feature amongst the extrusives. There is clearly

a need for a thorough chemical study of the Zambian extrusive carbonatite occurrences, which appear to be the only extensive dolomitic ones in the world.

6. Discussion This review was undertaken for a number of reasons including the belief that few, if any, intrusive carbonatites represent liquid compositions but that extrusive carbonatites might do so, that the mantle xenoliths and xenocrysts being discovered in extrusive carbonatites were of fundamental importance to understanding the genesis of these rocks and finally, that by considering these rocks as a whole some differences from intrusive carbonatites would come to light which might further the understanding of carbonatite genesis as a whole. It is believed that these objectives were met in so far as it can be demonstrated that there are differences between extrusive and intrusive carbonatites in terms of (a) general geology and mechanism of emplacement, (b) the nature of the associated silicate rocks and (c) the presence or absence of materials derived from the mantle. It is considered that some of the differences of the extrusive carbonatites from the intrusive is caused by the physical differences of their emplacement, but that these differences may also reflect fundamental differences of genesis. For instance, the widespread presence of mantle materials in some extrusives, particularly those around diatremes, is probably the result of their energetic emplacement, the very rapid rise of a turbulent mixture of solid, liquid and gas components enabling dense mantle material to be transported to the surface, while the mere presence of the mantle phases demonstrates that these particular carbonatites are generated at mantle depths and are not high level products of crystal fractionation or separation by immiscibility processes. Conversely, the carbonatites found in large volcanoes may represent ponding at high levels of carbonate-rich melt in the uppermost mantle, or even crust, with subsequent differentiation, and loss of volatiles to the surrounding rocks to produce fenitization. Whether the second type of carbonatite is simply the product of a more quiescent physical environment at high level mantle/ crustal levels working on the same primary precursor

A.R. Woolley, A.A. Church / Lithos 85 (2005) 114

11

is not immediately apparent, but some evidence may be provided by the associated silicate rocks. It was pointed out earlier that a high proportion of all the occurrences of extrusive carbonatite are associated with melilite-bearing rocks, but that the ratio is much lower for the intrusive carbonatites. What does this mean? Although some carbonatite intrusions may represent magmatic activity that was never expressed at the surface, it is thought probable that a high proportion of such intrusions did indeed have a surface manifestation, from which it is concluded that there is unlikely to be any fundamental difference between the magmas represented by the extrusive and the intrusive carbonatites and their associated silicate rocks. It is therefore suggested that the relative paucity of melilite-bearing rocks in the intrusive carbonatite association is a high level effect and both physical and chemical mechanisms suggest themselves. One such mechanism involves the physical replacement of early melilitite-bearing rocks by later melilite-free rocks, notably carbonatite. Many centres are dominated by large carbonatite intrusions which are emplaced at the very end of the igneous events and which probably destroyed and replaced earlier intrusions. Chilwa Island, in the Chilwa Province of Malawi, is an example of a complex consisting overwhelmingly of carbonatite which forms an approximately circular intrusion that probably occupies an earlier vent through which a suite of silicate magmas passed. Another mechanism may involve the instability of melilite in high level intrusions. Wollastonite is a common constituent of ijolite in many carbonatite centres and it seems likely that it, and perhaps garnet, are produced by the breakdown of melilite. That some melilitites are very intimately associated with carbonatite are nicely demonstrated by the accretionary lapilli from Italy in which inner melilitite zones, around cores of mantle minerals, are rimmed by carbonatite (Stoppa and Woolley, 1997), and by the similar, but even more spectacular lapilli from the Deeti tuff cones, Tanzania (Johnson et al., 1997). A mechanism for the generation of the extrusive carbonatites by separation of a carbonate-rich liquid from carbonate-bearing melilitite or nephelinite seems to be supported by both the chemistry and the zoned melilitite-carbonatite lapilli.

It was noted earlier that generally the extrusive carbonatites are higher in silica than the intrusive ones, and that the higher values of many extrusives are undoubtedly in part caused by entrained crystals and fragments of silicate country rocks picked up during the emplacement process, whereas, it is suggested, the more passive conditions pertaining in intrusions would allow settling of silicate phases and particularly any dense mantle xenoliths or xenocrysts that may be present. However, it seems possible that a relatively high silica content may be a primary feature of many carbonatite magmas. An impression has been gained that, apart from the entrained dforeignT materials of high level origin, the extrusive carbonatites contain an abundance of cognate silicate phases and that such relatively silicate-rich carbonate rocks may reflect more closely the primary composition of typical carbonatite magmas than the relatively silicate-free carbonate rocks typical of most carbonatite intrusions. Such a conclusion does, of course, have important implications for genetic modelling and for experimentalists modelling carbonatite systems. In an earlier paper (Woolley, 1969) the role of alkalis in carbonatites was discussed and it was assumed that most carbonatites are endowed with alkalis that are lost to the surrounding rocks to produce fenites, or as brines at the surface. Earlier in this paper it was suggested that the Oldoinyo Lengai natrocarbonatite is probably not unique but that at the adjacent Kerimasi volcano, for instance, alkalis were certainly lost from alkali-rich carbonatites during weathering. The alkali problem may be related to the two general types of carbonatite that have been distinguished here, namely those associated with small volcanic edifices, involving carbonatitic magmas that moved rapidly to the surface directly from their source deep in the mantle, and those in large volcanoes, in which the carbonatite may have been generated by high level fractionation/immiscibility processes. It is proposed that in the latter type high level fractionation of carbonate-bearing peralkaline magmas generates carbonatites with a high alkali content, like those of Oldoinyo Lengai, but that the deeply sourced carbonatites contain rather less alkalis, as a result of which there is little fenitization associated with them. Further, the rapid ascent involved in the SVEs is probably not so conducive to fluid loss to the walls of the

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A.R. Woolley, A.A. Church / Lithos 85 (2005) 114 tuffs from the Massif Central, France. Journal of Petrology 44, 1917 1936. Church, A.A., 1996. The petrology of the Kerimasi carbonatite volcano and the carbonatites of Oldoinyo Lengai with a review of other occurrences of extrusive carbonatites. PhD thesis, University of London. 384 pp. Clarke, M.C.G., Roberts, B., 1986. Carbonated melilitites and calcitized alkali carbonatites from Homa Mountain, Western Kenya: a reinterpretation. Geological Magazine 123, 683 692. Dawson, J.B., 1994. Quaternary kimberlitic volcanism on the Tanzanian Craton. Contributions to Mineralogy and Petrology 116, 473 485. Dawson, J.B., Powell, D.G., 1970. The Natron-Engaruka explosion crater area, northern Tanzania. Bulletin Volcanologique 33, 791 817. Deans, T., Roberts, B., 1984. Carbonatite tuffs and lava clasts of the Tinderet foothills, western Kenya: a study of calcified natrocarbonatites. Journal of the Geological Society (London) 141, 563 580. Dimroth, E., 1970. Meimechites and carbonatites of the Castignon Lake complex, New Quebec. Neues Jahrbuch fur Mineralogie Abhandlungen 112, 239 278. Djuraev, A.D., Divaev, F.K., 1999. Melanocratic carbonatites new type of diamond-bearing rocks, Uzbekistan. In: Stanley, C.J. (Ed.), Mineral Deposits: Processes and Processing, Proceedings of the Fifth Biennial SGA Meeting and Tenth Quadrennial IAGOD Symposium, London, U.K.Balkema, Rotterdam, pp. 639 642. Downie, C., Wilkinson, P., 1962. The explosion craters of Basotu, Tanganyika Territory. Bulletin Volcanologique 24, 389 428. Fletcher, C.J.N., Appleton, J.D., Webb, B.C., Basham, I.R., 1981. Mineralization in the Cerro Manomo carbonatite complex, eastern Bolivia. Transactions of the Institution of Mining and Metallurgy B90, 37 50. Gaspar, J.C., Danni, J.C.M., 1981. Aspectos petrogaficos da provincia alcalino-carbonatitica de Santo Antonio da Barra SW de Goias. Revista Brasileira de Geociencias 11, 74 83. Griffin, W.L., Kresten, P., 1987. In: Nixon, P.H. (Ed.), Mantle Xenoliths. John Wiley, Chichester, pp. 101 106. Hay, R.L., 1978. Melilitite-carbonatite tuffs in the Laetolil beds of Tanzania. Contributions to Mineralogy and Petrology 67, 357 367. Hoernle, K., Tilton, G., Le Bas, M.J., Duggen, S., Garbe-Schon berg, D., 2002. Geochemistry of oceanic carbonatites compared with continental carbonatites: mantle recycling of oceanic crustal carbonate. Contributions to Mineralogy and Petrology 142, 520 542. Hoy, T., Pell, J., 1986. Carbonatites and associated alkalic rocks Perry River and Mount Grace areas Shuswap complex southeastern British Columbia. Paper, British Columbia Ministry of Energy, Mines and Mineral Resources, Geological Fieldwork, 1986-1, 69-87. Johnson, L.H., Jones, A.P., Church, A.A., Taylor, W.R., 1997. Ultramafic xenoliths and megacrysts from a melilitic tuff cone, Deeti, northern Tanzania. Journal of African Earth Sciences 25, 29 42.

conduit. In the case of the high level generation of carbonatite it would be expected that a range of carbonatite magmas containing varying amounts of alkalis (and other incompatible elements) would be produced, depending on the chemistry of the parental magmas, and particularly their degree of peralkalinity. Further, the ratio of Na : K would differ, although at crustal levels this might also be controlled by differential loss of the alkalis during the fenitization process, as discussed earlier (Woolley, 1969).

Acknowledgements We are most grateful to Prof. D.K. Bailey for his interest in this work and for many pertinent comments and useful suggestions for improving the paper. Dr Chris Stanley also kindly commented on the MS. Prof. J. Keller and Dr B.A. Kjarsgaard gave detailed and useful reviews, which are much appreciated. We are grateful to N. Eby, F.E. Lloyd and F. Stoppa for allowing us to use unpublished data of Fort Portal tuffs and lavas.

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