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Journal of Petrology Volume 41 Number 12 Pages 1805-1820 2000
© Oxford University Press 2000
Resolving Crustal and Mantle Contributions to Continental Flood Volcanism, Yemen; Constraints from Mineral Oxygen Isotope Data
1DEPARTMENT OF GEOLOGY, ROYAL HOLLOWAY UNIVERSITY OF LONDON, EGHAM HILL, EGHAM TW20 0EX, UK
2DEPARTMENT OF GEOLOGY, UNIVERSITY OF SANAA, SANAA, YEMEN
Received January 28, 1999; Revised typescript accepted May 2, 2000
| ABSTRACT |
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Oxygen isotope ratios determined by laser fluorination analysis on olivine, clinopyroxene and plagioclase separated from 31 Oligocene flood basalts and rhyolites from Yemen display small but significant variations (5·16·2
for olivine; 5·56·9
for clinopyroxene; 5·96·9
for plagioclase). The range in
18O values exceeds: (1) the analytical reproducibility of the technique (±0·15
; 2 SD); (2) the range expected for minerals that would have crystallized from uncontaminated oceanic basalts or primary magmas in equilibrium with mantle peridotite; (3) the range in melt values and equilibrium phenocryst compositions that could be produced by fractional crystallization of these magmas. Samples with the highest
18O values exhibit increases in 87Sr/86Sr ratio, decreases in 143Nd/144Nd ratio, and increasing Pb isotopic heterogeneity. Samples with the lowest
18O values have radiogenic isotope ratios that approach those inferred for the Afar plume. The oxygen isotope data provide unequivocal evidence that assimilation of heterogeneous lower and upper Pan-African crust was the primary control on isotopic variation in this continental flood basalt province. Moreover, new radiogenic and oxygen isotope data for Pan-African crustal samples from Yemen have appropriate crustal isotopic compositions to generate the observed isotopic variations in the volcanic rocks. A near-primary high-MgO basalt with low
Nd and extreme Pb isotope ratios contains strongly zoned clinopyroxene crystals that range from green cores through to greenish brown, brownish green and dark brown or black rims. Handpicked crystals of each colour type display the following correlated range in isotope ratios: 87Sr/86Sr = 0·70360·7049; 143Nd/144Nd = 0·51290·5127; 206Pb/204Pb = 18·617·9;
18O = 5·676·86
. The SrNdPbO isotope variations are attributed to rapid assimilation of
25% Pan-African continental crust by hot mafic magma during clinopyroxene crystallization. Contamination in this flood basalt province varied from combined assimilation and fractional crystallization to rapid assimilation of crust by hot mafic magmas with little fractionation. Laser fluorination oxygen isotope analysis of mineral separates allows small differences in
18O to be correlated with radiogenic isotope data and is a powerful tool for evaluating the relative roles of enriched lithospheric mantle and continental crust in suites of continental flood basalts. KEY WORDS: oxygen isotopes; phenocrysts; flood volcanism; crustal contamination; Yemen
| INTRODUCTION |
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Continental flood volcanism has in the past produced massive (>1 x 106 km3) outpourings of largely basaltic magmas in only a few millions of years (Coffin & Eldholm, 1993
Continental flood basalts exhibit a wide range in trace element and isotopic compositions and, whereas some flood basalts clearly have chemical and isotopic signatures akin to oceanic basalts, many flood basalts have signatures that are more typical of continental crust (e.g. Ferrar; Hergt et al., 1989
). Even examples of flood volcanism that have isotope ratios that fall entirely within the range of oceanic basalts display substantial isotopic variability that must represent multiple contributions to volcanism [e.g. Yemen; Fig. 1 (Baker et al., 1996b
)]. There is general agreement that the enriched isotope ratios (e.g. low
Nd) and lithospheric trace element signatures (e.g. high Rb, K, Ba, Pb and La) of many flood basalts, which distinguishes them from oceanic basalts, must reflect a contribution from the continental lithosphere traversed by these magmas. To date, those who study flood basalt provinces have failed to reach any consensus on the general origin of this lithospheric signature, although it needs to be stressed that the source of this lithospheric signature need not be the same in each province. However, recent studies have reached directly conflicting conclusions on the major control on isotopic variability in many individual examples of continental flood volcanism, e.g. Columbia River Basalt Group (Carlson et al., 1981
; Carlson, 1984
; Brandon et al., 1993
; Hooper & Hawkesworth, 1993
), EthiopianYemeni Traps (Chazot & Bertrand, 1993
; Deniel et al., 1994
; Baker et al., 1996b
; Pik et al., 1999
); Deccan Traps (Lightfoot et al., 1990a
; Peng et al., 1994
); Siberian Traps (Lightfoot et al., 1990b
, 1993
; Arndt et al., 1993
; Wooden et al., 1993
; Horan et al., 1995
).
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Proponents of crustal contamination models argue that crustal contamination is inevitable during the storage and transfer of mantle-derived melts through the lithosphere and, moreover, that the lithospheric mantle (LM) is too cold and refractory and does not have the appropriate composition to generate large volumes of flood basalt (Arndt & Christensen, 1992
; Menzies, 1992
). However, others have argued that addition of small amounts of volatiles to the LM can depress solidus temperatures, allowing large amounts of melting in the presence of a thermal anomaly when coupled with lithospheric extension (Gallagher & Hawkesworth, 1992
). Presumably, hydration and introduction of subducted sediment into the LM by ancient subduction zone processes produces a crustal-like signature in the LM. Recent studies have also suggested that plume-derived carbonatitic metasomatism of the LM could impart a similar signature (Hauri et al., 1993
; Baker et al., 1998
).
What remains beyond question is that only when the primary chemical and isotopic signature of flood volcanism has been identified is it possible to test rigorously and develop models for flood basalt petrogenesis. Using primary magma compositions to identify and temporal and spatial variability in mantle source composition(s) and the degree(s) and depth(s) of partial melting is a powerful tool for testing and developing geochemical and geodynamic models for flood basalt genesis (e.g. White & McKenzie, 1989
, 1995
; Ellam, 1992
; Gallagher & Hawkesworth, 1992
).
Identification of crustal contamination typically relies on identification of correlations between indices of fractionation and chemical or isotopic data. For example, correlations between MgO (negative) or SiO2 (positive) contents with 87Sr/86Sr ratios are taken as evidence for progressive contamination of magmas while fractionation was taking place in lithospheric magma chambers. In principle, however, this approach has a number of limitations: (1) such correlations are not always observed when reconnaissance suites of samples are considered that do not represent a coherent magmatic system (e.g. Baker et al., 1996b
); (2) similar correlations can be produced during fractionation of magmas within the LM, accompanied by a progressive addition of melts from enriched LM (Ellam & Cox, 1991
); (3) contamination processes are thought to vary considerably from combined assimilation and fractional crystallization (AFC; DePaolo, 1981
) through to assimilation of crust by hot mafic magmas with little or no concomitant fractionation (Thirlwall & Jones, 1983
; Cox & Hawkesworth, 1985
; Huppert & Sparks, 1985
; Devey & Cox, 1987
; Kerr et al., 1995
); (4) MgO and SiO2 are not always useful indicators of fractionation, e.g. only small changes in MgO are generated by fractionation of a plagioclase-dominated gabbroic assemblage.
The now well-defined and generally restricted oxygen isotope ratios of crustally uncontaminated oceanic basalts, and mantle peridotites (Ito et al., 1987
; Mattey et al., 1994
; Eiler et al., 1997
), provide a powerful and unequivocal method to test the relative roles of crust and LM in the petrogenesis of continental flood basalts. Assimilation of crustal materials that typically, but not always, have elevated
18O relative to mantle-derived magmas should generate 18O enrichment in the contaminated basalts with predictable correlated changes in radiogenic isotope ratios. To date, oxygen isotope study of continental flood basalts has been hampered by the often altered nature of these rocks and, in some cases, their sparsely porphyritic nature. Susceptibility of the oxygen isotope system to post-eruptive alteration largely precludes the use of whole-rock oxygen isotope data in evaluating the relative roles of crust and mantle in flood basalts (e.g. Hergt et al., 1989
) and perhaps volcanic rocks in general (e.g. Eiler et al., 1995
, 1997
).
Herein, we present laser fluorination oxygen isotope data on milligram-sized phenocrysts separated from flood basalts and rhyolites that were erupted between 31 and 26 Ma in Yemen, which form part of the Oligocene Ethiopian flood basalt province (Baker et al., 1996a
). These rocks have radiogenic isotope ratios that extend out of the fields defined by local LM, mantle plume (Afar plume) and depleted upper mantle [DMM or mid-ocean ridge basalt (MORB) mantle] compositions, although the isotopic variation is less than that exhibited by oceanic basalts (Fig. 1). Baker et al. (1996b)
concluded that correlations between MgO and SiO2 and isotope data, the probable availability of appropriate crustal components, and unavailability of appropriate enriched LM components required much of the chemical and isotopic variability in the Yemen flood basalts to result from contamination of plume-derived magmas with regionally heterogeneous crustal components. Whereas the evidence presented by Baker et al. (1996b)
supporting crustal contamination is largely circumstantial and equivocal, the mineral oxygen isotope data presented herein show substantial variability that exceeds, and extends to higher values than, that observed in oceanic basalts and mantle peridotites. Thus, the oxygen isotope data provide unequivocal evidence for crustal contamination in this flood basalt province and also confirm that contamination mechanisms were variable. We also present new radiogenic and oxygen isotope data for crustal basement samples from Yemen that, in some cases, have precisely the compositions required to generate some of the mixing arrays exhibited by the volcanic rocks in SrNdPbO isotopic space.
| SAMPLES |
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The samples that form the basis of this study are flood volcanic rocks that were erupted from 31 to 29 Ma in Yemen (Baker et al., 1996a
The volcanic rocks can be divided into two suites on the basis of field relationships, chemistry and isotope data. Rocks erupted through the western part of the province display limited and distinct isotopic variations compared with those erupted through the eastern part of the province (Baker, 1996
; Baker et al., 1996b
; see the Origin of isotopic variations section, below) and, as such, this is used to separate the samples into two groups in this paper. Rhyolitic pyroclastic rocks were also erupted from the western part of the province at sites now marked by the presence of granite plutons, which are unroofed caldera centres exhumed in the last 25 my.
| ANALYTICAL TECHNIQUES |
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Oxygen isotope analyses
Approximately 12 mg of clean olivine, clinopyroxene, feldspar (where no mafic silicates were available for analysis) or FeTi oxide phenocrysts were handpicked from coarsely crushed whole-rock volcanic samples to avoid inclusion-rich and altered material. One mafic flood basalt (JB172) contains strongly colour-zoned clinopyroxene crystals that vary from apple-green cores, through slightly brownish green, greenish brown and pale brown zones to black or dark brown crystal rims. The large size of these crystals (13 mm) allowed the OSrNd isotope ratios of the differently coloured zones in this sample to be determined, along with the Pb isotope ratios of the core material. Bulk separates of each colour fraction of the clinopyroxene from JB172 were prepared and homogenized, and these were then split into portions for radiogenic isotope analysis and replicate oxygen isotope analyses. A number of mineral phases (amphibole, biotite, quartz, garnet) were separated from two Pan-African crustal samples for oxygen isotope analysis and, in one case, a fine-grained chip of a whole-rock sample (plagioclase + amphibole) was also analysed.
Oxygen isotope analyses were carried out using the laser fluorination technique of Mattey & Macpherson (1993)
at Royal Holloway University of London. Mineral separates were heated with a NdYAG laser in the presence of ClF3. To optimize oxygen yield, laser power and the quantity of ClF3 used during the fluorination were varied according to the phase being analysed. Feldspar, which is transparent to the NdYAG laser, was mixed with a mafic silicate phase of known oxygen isotope composition (San Carlos mantle olivine; SCOL) to assist fluorination reactions. Using a simple mixing equation involving the relative weight proportions of feldspar to olivine in the reaction mixture, their respective oxygen concentrations, the oxygen isotope ratio of the olivine and the oxygen isotope ratio of the mixture, the isotopic composition of the feldspar could be devolved. After clean-up with KBr, the liberated O2 was converted to CO2 by reaction with hot graphite. CO2 was analysed on a VG PRISM mass spectrometer. Oxygen isotope ratios are reported as the per mil deviation from Vienna Standard Mean Ocean Water in the standard
notation.
Analytical precision can be judged from the mean values for in-house olivine (SCOL) and garnet (Beni Bousera peridotite massif; GP143) standards during the period of analysis: SCOL = 4·90 ± 0·15
(n = 8; 2 SD); GP143 = 7·23 ± 0·20 (n = 19; 2 SD). During the period of analysis, and in the 2 years before this, the following values were determined on these two in-house standards: SCOL = 4·86 ± 0·16
(n = 245; 2 SD); GP143 = 7·21 ± 0·20 (n = 106; 2 SD). Replicate analyses of standards or unknowns on the same day typically show enhanced reproducibility (<±0·1
; 2 SD) compared with these long-term averages. As such, reproducibility of
18O values for analysed mafic silicates with fluorination yields >95% can be taken to be better than ±0·15
(2 SD). Yields for all unknowns and standards were 100 ± 2%.
Feldspar oxygen isotope analyses are inherently less precise than those of mafic phases because of the need to mix samples with a mafic silicate to induce fluorination reactions. However, the reliability of the feldspar analyses can be tested by replicate analyses of NBS28 quartz samples by the same technique, fluxing with the SCOL standard, which yielded a mean value of 9·57 ± 0·36
(n = 17; 2 SD; D. Lowry, unpublished data, 1996); this compares favourably with the recommended value for this NBS standard, i.e. 9.66
. NBS-30 biotite standard analysed in this laboratory gives
18O = 5·03 ± 0·16
(2 SD; n = 80) compared with the recommended value of 5·1
.
SrNdPb isotope analyses
Details of the analytical techniques used to obtain SrNdPb isotope ratios for host basaltic samples (MgO > 3 wt %), from which minerals were separated for oxygen isotope analyses, have been presented by Baker et al. (1996b)
. SrNdPb isotope ratios were determined on whole-rock powders and are reported here as initial ratios; these isotopic data, along with measured isotope ratios and chemical data for the same samples, were presented by Baker et al. (1996b)
. SrNdPb isotope ratios for the rhyolitic samples were obtained on acid-leached mineral separates [anorthoclasesanidine (SrPb), clinopyroxene (SrNd) and amphibole (SrNd)]. The feldspar Pb isotope data can be considered to be initial data given the low U/Pb and Th/Pb ratio of feldspar. However, all the remaining radiogenic isotope data presented herein for volcanic samples have been age-corrected using 40Ar/39Ar ages (3126 Ma) from Baker et al. (1996a)
and trace element data from Baker (1996)
and Baker et al. (1996b)
, including RbSr isotope dilution data determined on the rhyolitic mineral separates.
SrNdPb isotope data on the zoned clinopyroxene phenocrysts from mafic flood basalt JB172 were determined on bulk separates (0·020·1 g) on splits of similarly coloured parts of the zoned phenocrysts as used for oxygen isotope analysis. Clinopyroxene was leached in hot HCl and repeatedly rinsed in deionized water before dissolution, conventional chemical separation and subsequent mass spectrometric analysis as described by Baker et al. (1996b)
. Only sufficient material from the cores was available to perform Pb isotope analyses. To assess isotopic homogeneity between the same-coloured splits used for oxygen and radiogenic isotope analyses, the fluoride residues of two differently coloured parts of the zoned clinopyroxene crystal were recovered after oxygen isotope analysis and analysed for SrNd isotopes. The measured SrNd isotope ratios were within analytical uncertainty of those determined on the bulk separates of the similarly coloured parts of the zoned clinopyroxene phenocrysts, implying that the colour fractions used for radiogenic and oxygen isotope analysis are isotopically homogeneous on the scale of the analytical procedures used in this study.
New SrNdPb isotope ratios have also been determined on five crustal basement samples (whole-rock powders) that were collected from the eastern (two samples) and western (three samples) parts of Yemen.
External precision and reproducibility of SrNd isotope ratios are better than ±0·000018 and ±0·000013 (n > 50; 2 SD), and ratios are reported relative to values of 0·710250 for SRM987 and 0·511424 for an in-house laboratory Nd standard. This 143Nd/144Nd ratio corresponds to 0·511860 and 0·512638 for the international standards La Jolla and BCR-1, respectively. External precision or reproducibility of SRM981 shows that the reproducibility of sample Pb isotope ratios is
±0·010, ±0·012 and ±0·030 (2 SD) for 206Pb/204Pb, 207Pb/204Pb and 208Pb/204Pb, respectively.
| RESULTS |
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Oxygen isotope analyses of 66 mineral separates from 31 volcanic samples are presented in Tables 1 and 2. Table 1 lists mineral oxygen isotope data, host volcanic rock MgO contents and initial SrNdPb isotope ratios, along with five radiogenic and limited mineral oxygen isotope analyses of Pan-African crustal basement samples from Yemen. Table 2 lists OSrNdPb isotope data for differently coloured parts of the strongly zoned clinopyroxene phenocrysts from mafic flood basalt (JB172), along with oxygen isotope data for olivine phenocrysts from the same rock.
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Oxygen isotope data
Olivine
18O values vary from 5·1 to 6·2
and a number of samples have values (5·15·3
) that overlap the range defined by olivine separated from (1) a wide variety of mantle peridotite xenoliths, largely from the subcontinental LM (5·18 ± 0·28
; n = 76; Mattey et al., 1994
), and (2) MORB and ocean island basalts (OIB) (for MORB, 5·16 ± 0·18
, n = 6; for OIB, 5·17 ± 0·49
, n = 62; Eiler et al., 1997
) (Fig. 2).
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Clinopyroxene
18O values also vary widely (5·56·9
) and, again, a number of samples from the lower end of this range have
18O values that closely overlap the range defined by clinopyroxenes from mantle peridotites (5·57 ± 0·32
; n = 57; Mattey et al., 1994
18O values of 5·96·1
, which are actually lower than those observed in some of the basaltic samples. The differently coloured parts of the zoned clinopyroxene crystals separated from mafic flood basalt JB172 have highly variable
18O values (5·676·86
) and this sample is discussed in more detail in the next section.
Plagioclase
18O values range from 5·9 to 6·9
. As a result of the scarcity of plagioclase-facies mantle rocks, no mantle feldspar
18O values are available. However, it is notable, given the relatively small oxygen isotopic fractionation between melt and plagioclase at magmatic temperatures (
melt-plag = -0·1 to -0·3
; Kalamarides, 1986
; Kyser, 1986
, 1990
), that the lower feldspar
18O values (6·0 ± 0·1
) would be in equilibrium with melts that have
18O
5·75·8
(Table 1). Such melt
18O values are characteristic of fresh MORB glasses (5·71 ± 0·34
, Ito et al., 1987
; 5·81 ± 0·10
, Macpherson, 1995
).
Oxygen isotope fractionations observed between different mineral phases separated from the same rock are:
ol-cpx = -0·20 to -0·35
;
ol-plag = -0·86
;
mt-plag = -1·86
. These mineralmineral fractionations are consistent with those measured in studies of phenocrysts from other volcanic rocks (Anderson et al., 1971
; Singer et al., 1992
; Macpherson, 1995
; Eiler et al., 1997
; Thirlwall et al., 1997
; Macpherson et al., 1998
). These fractionations are also broadly consistent with the mineral phases being in equilibrium at magmatic temperatures (12001000°C; Chiba et al., 1989
; Zheng, 1993
).
Figure 2 shows raw mineral
18O values plotted vs host rock MgO contents. A very general trend to higher mineral
18O values, of each mineral type, with decreasing host rock MgO may be evident. However, more importantly, there is much scatter in these possible trends and samples with any MgO contents may have elevated mineral
18O values; for example, olivine and clinopyroxene from JB172, clinopyroxene from JB82 and olivine from JB282.
In summary, ranges in
18O values for each phase (1) exceed the maximum analytical reproducibility of the technique (±0·15
) and (2) extend to higher values than those recorded in either minerals (olivine and clinopyroxene) separated from crustally uncontaminated mantle-derived oceanic basalts (Eiler et al., 1997
) and mantle peridotites (Mattey et al., 1994
) or mineral compositions (plagioclase) that can be calculated to have been in equilibrium with MORB melts. The lowest
18O values obtained for each mineral phase overlap values for these phases in oceanic basalts, mantle peridotite xenoliths, or values that would characterize minerals that crystallized at basaltic temperatures from melts in equilibrium with mantle peridotites. These observations are independent of corrections to the raw mineral
18O values described below (in Correlations between mineral oxygen and host rock radiogenic data) to convert them to values equivalent to clinopyroxene or melt compositions so that all the data can be collectively compared with whole-rock SrNdPb isotope ratios.
Oxygen and radiogenic isotope variations in a mafic flood basalt (JB172)
Sample JB172 is a magnesian basalt containing 10·95 wt % MgO (mg-number 0·68). Its whole-rock powder is characterized by high 87Sr/86Sr (0·70467) and low 143Nd/144Nd (0·51272) ratios, and the lowest 206Pb/204Pb ratio (17·9) and almost the highest
7/4 (+14·3) and
8/4 (+101·9) values of the flood volcanic samples from Yemen [
notation from Hart (1984)
].
From core to rim the
18O values of the clinopyroxene increase systematically from 5·7 to 6·9
(Table 2; Fig. 3), and
18O correlates with changes in 87Sr/86Sr and 143Nd/144Nd ratios (Fig. 3). The cores of the crystals have low 87Sr/86Sr (0·70356) and high 143Nd/144Nd (0·51290) ratios, which are amongst the most depleted compositions measured for the western Yemen flood basalts, and similar to those inferred for the Afar plume (Vidal et al., 1991
; Schilling et al., 1992
; Baker et al., 1996b
, 1997
). The rims have high 87Sr/86Sr (0·70487) and low 143Nd/144Nd (0·51273) ratios that are similar to values measured on the whole-rock powder, where the analysed Sr and Nd would largely have been derived from the groundmass, which is evidently in equilibrium with the clinopyroxene rims. Pb isotope ratios of the green clinopyroxene cores are completely different from the measured whole-rock ratios (Table 2, footnote), falling close to the inferred Afar plume composition (Figs 4 and 5), and are similar to other whole-rock samples with low 87Sr/86Sr and high 143Nd/144Nd ratios.
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Olivine phenocrysts, which on petrographic grounds crystallized after the green clinopyroxene cores but before the clinopyroxene rims, have
18O
6·1
. With our technique it is impossible to assess if there is any zonal heterogeneity with respect to SrNdPbO isotope ratios in the olivine crystals, but olivine
18O values of 6·1
would be in equilibrium with clinopyroxenes with
18O
6·46·5
. This is intermediate between the values determined for the end-member core and rim zones of the clinopyroxene and in agreement with the petrographic evidence for the order of crystallization of these phases.
The correlated changes in SrNdO isotope ratios from core to rim in clinopyroxene crystals from JB172 suggest that a magnesian, near-primary magma with depleted SrNd isotope ratios and Pb isotope ratios approaching those of the Afar plume, and with mantle-like
18O values, progressively, and rapidly, acquired more enriched Sr Nd isotope ratios and higher
18O during clinopyroxene crystallization.
Interestingly, two mafic flows intercalated with the flow from which JB172 was sampled are offset to slightly higher 87Sr/86Sr and lower 143Nd/144Nd ratios than the SrO and NdO mixing arrays defined by the JB172 analyses (Fig. 3). In these rocks (JB166 and JB171) the radiogenic isotope ratios were determined on whole-rock powders and the oxygen isotope ratios were measured on large clinopyroxene phenocrysts. It is therefore possible that these two samples, like JB172, also record some isotopic disequilibrium between phenocryst phases and groundmass, i.e. the clinopyroxenes are isotopically zoned. Unfortunately, the smaller size of the clinopyroxene phenocrysts and lack of colour zoning compared with the JB172 clinopyroxenes precluded further investigation of this hypothesis, in the absence of in situ analytical techniques.
Correlations between mineral oxygen and host rock radiogenic data
The different phenocryst phases present in the volcanic rocks precluded analysis of a common mineral phase in every sample. To compare the oxygen isotope ratios from samples with different analysed phases we have chosen to correct our mineral data to values that are equivalent to clinopyroxene values. We have taken this approach as: (1) clinopyroxene is the phase we have the most data for; (2) conversion to melt
18O values is precluded by a lack of knowledge of mineralmelt fractionation factors and adequate thermometric data for the Yemen flood basalts; (3) although melt
18O values are likely to increase during fractionation of olivine + clinopyroxene ± plagioclase ± FeTi oxides, this is offset by increasing
melt-cpx fractionation at lower melt temperatures (e.g. Kalamarides, 1986
; Fig. 2; Table 3).
The following mineral fractionation factors were used to convert the raw olivine, plagioclase and FeTi oxide oxygen isotope data into equilibrium clinopyroxene isotope data:
cpx-ol = +0·4
;
cpx-plag = -0·35
;
cpx-mt = +1·6
. These fractionation factors are consistent with those measured in basaltic and andesitic rocks (Anderson et al., 1971
; Singer et al., 1992
; Macpherson, 1995
; Thirlwall et al., 1997
; Macpherson et al., 1998
) and also the fractionations predicted from experimental work and theoretical considerations between these phases at magmatic temperatures (10001200°C; Chiba et al., 1989
; Zheng, 1993
).
Actual or calculated equilibrium clinopyroxene
18O values, with JB172 represented by the analysis of crystal rims, are plotted vs host rock SrNdPb isotope ratios (Fig. 4). Although there is considerable scatter in these plots,
18O values increase with: (1) increasing 87Sr/86Sr ratios and also with little change in 87Sr/86Sr; (2) decreasing 143Nd/144Nd ratios; (3) high
8/4 values (such as JB172), and also with little change in
8/4 (such as JB282), and possibly at low
8/4 values (such as JB259) (i.e. increasing Pb isotopic heterogeneity). When the higher
18O samples are considered, it is notable that the samples erupted through the western part of the volcanic province display more limited Nd isotopic variations and trend towards different Pb isotopic compositions compared with those erupted through the eastern part of the volcanic province.
Samples with the lowest
18O values tend to approach isotope ratios of 87Sr/86Sr = 0·7035, 143Nd/144Nd = 0·5129, 206Pb/204Pb = 19·0 and
8/4
40, which are similar to those inferred for the Afar plume (Fig. 4).
Clinopyroxene separates from the rhyolite samples fall on the same trends as the basaltic samples erupted through the western part of the volcanic province, but are displaced to higher 87Sr/86Sr ratios at the same
18O values compared with most of these samples. Like all the basaltic samples erupted through the western part of the volcanic province, the rhyolites exhibit rather limited radiogenic isotope variations compared with basalts erupted through the eastern part of the volcanic province.
Crustal SrNdPbO isotope data
SrNdPb isotope ratios for five crustal basement samples display substantial variations (Table 1; Fig. 5): 87Sr/86Sr = 0·7040·710; 143Nd/144Nd = 0·512860·5119; 206Pb/204Pb = 17·319·9. There is a clear distinction between the basement underlying the western and eastern parts of the volcanic province. Samples from the west have limited isotopic variability and are akin to juvenile, Late Proterozoic, Pan-African basement from elsewhere in the Arabian shield (e.g. Duyvermann et al., 1982
; McGuire & Stern, 1993
; Brueckner et al., 1995
). Samples from basement underlying the eastern part of the volcanic province display more extreme isotope ratios and are examples of the Late Archaean crust that has been recently identified in this part of Yemen (Windley et al., 1996
).
Oxygen isotope data for two crustal samples from these two crustal provinces also exhibit marked differences. A sample from the western part of the volcanic province has relatively low
18O, comparable with values of the flood basalts. However, an Archaean(?) gneiss from the eastern part of the province has much higher
18O (9·613·3
) for all its mineral phases compared with the flood basalts. These values are almost identical to whole-rock
18O values reported by Davidson & Wilson (1989)
for similar Archaean gneisses from Sudan.
| DISCUSSION |
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Origin of isotopic variations
Effects of magma fractionation
Few of the Yemen flood basalts and clearly none of the rhyolites are primary magmas. Petrographic observations along with qualitative and quantitative modelling of fractional crystallization processes (Baker, 1996
Modelling the effects of fractional crystallization on melt and equilibrium mineral oxygen isotope compositions is non-trivial, given the relatively poor constraints on mineralmelt fractionation factors and melt temperatures, and the fact that mineralmelt fractionation factors are temperature dependent and so will change in an evolving magma. However, in Table 3 we crudely illustrate the effects of fractional crystallization for three crystallization steps with changing crystallizing assemblages and mineralmelt fractionation factors in each step (MgO = 13·58·5, 8·54·0, 4·00·5 wt %). The modelling uses a starting magma with
18O = 5·70
and calculates an average mineralmelt fractionation factor over the crystallization interval using the relative proportions of fractionating phases obtained from least-squares mixing modelling of major and trace element variations (Chazot & Bertrand, 1993
; Baker, 1996
). Mineralmelt fractionation factors are calculated from the equations of Kalamarides (1986)
assuming temperature varies as shown in Table 3. It is then finally necessary to recalculate equilibrium clinopyroxene compositions that would have been in equilibrium with the evolving melts as
melt-cpx increases with decreasing MgO (i.e. temperature).
These simple calculations show that fractionation of olivine + clinopyroxene and subsequent minor amounts of plagioclase + FeTi oxides within the basaltic spectrum of rock types (MgO = 13·54·0 wt %) produces only small increases in melt
18O (<0·3
) and that the increasing
melt-cpx fractionation factor with decreasing temperature (or MgO) means that an increase of only 0·1
in clinopyroxene
18O values is likely to result from fractional crystallization (Table 3; Fig. 2). Production of the rhyolitic rocks from basaltic parents requires extensive fractional crystallization (
85%) and the significant amounts of fractionating FeTi oxides result in a modest increase in melt
18O values (0·40·6
). Clinopyroxene in equilibrium with such rhyolitic melts produced by protracted differentiation of basaltic parents would have
18O
5·9
, similar to the lowest values measured in rhyolites in this study.
These calculations show that fractionation of the observed mineral phases in the Yemen flood basalts cannot generate the range in mineral
18O values observed in these rocks (>1
). However, the marginally elevated
18O values measured on clinopyroxenes from the rhyolitic rocks can be largely accounted for by extensive fractional crystallization from basaltic parents. It is vital to note that relatively large
18O variations observed in individual mineral phases from samples with a limited range in MgO contents preclude fractional crystallization control on much of the oxygen isotopic variability in this dataset.
Mantle heterogeneity or crustal contamination?
Volcanic rocks from Yemen have radiogenic isotope ratios that exhibit considerable variation, but still fall within the field of oceanic basalts (Figs 1 and 5), and these correlations correlate with mineral oxygen isotope data (Figs 3 and 4). However, oxygen isotope variations (1·5
) in minerals separated from the flood basalts exceed that observed in mantle peridotites (or minerals that would have crystallized from melts in equilibrium with mantle peridotites), including a large number of peridotites from the continental LM (Mattey et al., 1994
). Oceanic basalts with a wide range in radiogenic isotope ratios exhibit limited oxygen isotope variations when analyses of mineral phases from these rocks are considered (Eiler et al., 1997
). The previous discussion has shown that the mineral oxygen isotope variations are too large to be the product of fractional crystallization. We conclude that assimilation of continental crust, with elevated
18O relative to mantle-derived magmas, rather than a contribution from enriched LM or subcontinental mantle is responsible for the isotopic and also much of the incompatible trace element heterogeneity of the flood volcanic rocks from Yemen.
The oxygen isotope data confirm previous assertions that crustal contamination was an important process in this flood volcanic province (Baker et al., 1996b)
and cast further doubt on the frequently inferred role of an enriched LM contribution to flood volcanism at the Afro-Arabian triple junction (Hart et al., 1989
; Vidal et al., 1991
; Chazot & Bertrand, 1993
; Deniel et al., 1994
).
Crustal provinciality from isotopic data
SrNdPbO isotope variations require the involvement of at least three crustal components (C1, C2 and C3) in the petrogenesis of the Yemen flood basalts and rhyolites (Figs 4 and 5).
Basalts erupted through the eastern part of the volcanic province are contaminated by a component with unradiogenic Pb isotope ratios and elevated
7/4 and
8/4 values, and high 87Sr/86Sr and low 143Nd/144Nd ratios (C1) (Fig. 5). This component has an isotopic composition remarkably similar to analyses of Late Archaean crustal gneisses from eastern Yemen presented herein (Fig. 5).
Basalts and rhyolites erupted through the western part of the volcanic province have been contaminated by at least two components. One component (C2) is difficult to identify on the basis of radiogenic isotopes as it has an isotopic composition relatively close to that of the uncontaminated basalts compared, for example, with C1. This component (C2) has Pb isotope ratios that fall close to the Northern Hemisphere Reference Line and the MORBAfar plume array, with slightly unradiogenic Pb and slightly higher 87Sr/86Sr and lower 143Nd/144Nd ratios compared with the uncontaminated basalts. This composition is inferred to be Late Proterozoic Pan-African lower crust which is not old enough (or particularly chemically evolved enough) to have developed exotic isotope ratios compared with mantle-derived basalts. Analyses of lower-crustal granulite-facies gneisses from the Zabargad Island massif (Brueckner et al., 1995
) and also such xenoliths entrained in Late Cenozoic volcanism throughout Saudi Arabia and Yemen (McGuire & Stern, 1993
; G. Chazot & J. A. Baker, unpublished data, 1998) have precisely the required radiogenic isotope compositions to generate the observed mixing arrays in SrNdPb isotopic space (Fig. 5). The second crustal component (C3) contaminating the basalts (and rhyolites) erupted through the western part of the volcanic province has higher 87Sr/86Sr ratios than, but similar 143Nd/144Nd ratios to, C2 and a distinctive Pb isotope signature marked by radiogenic 206Pb/204Pb isotope ratios with negative
8/4 values. This component is clearly distinct from the MORBAfar plume mixing array in Pb isotope space and analyses of crustal basement from the western part of the volcanic province are a suitable crustal end-member.
Figure 6 illustrates the multi-element patterns of two relatively uncontaminated basalts with low
18O erupted through the western (JB281) and eastern (JB231II) parts of the volcanic province in Yemen. These samples are marked by relatively smooth multi-element patterns with a marked negative K anomaly. Figure 6 also illustrates examples of basalts contaminated by each of the inferred crustal contaminants. Samples contaminated by C1 and C2 show smaller K anomalies and enrichments in Ba and Pb relative to Rb, Th and U, which is consistent with these samples having assimilated RbThU-depleted, granulite-facies, lower crust. Samples contaminated by C3 show enrichments in all the large ion lithophile elements (LILERb, Ba, K and Pb), Th and U relative to Nb. These features are consistent with C3 being an upper-crustal component.
|
Scattered arrays of data in Figs 1, 4 and 5 are a natural consequence of crustal contamination with isotopically heterogeneous crustal components, variable distribution coefficients for Sr during assimilation and fractional crystallization, and differences in primary magma incompatible trace element abundances rendering different samples isotopic systems to have had different susceptibilities to a finite amount of contamination. Semi-quantitative modelling of contamination processes has already been presented by Baker et al. (1996b)
and in Fig. 3. These calculations show that the Yemen flood basalts and rhyolites have variably assimilated 025% crustal material.
Mechanisms of contamination
Mafic magmas erupted through the eastern part of the volcanic province have, in some cases, assimilated large amounts (
2025%) of a Late Archaean silicic lower-crustal component (C1) with little concomitant fractionation, e.g. JB172 and JB129. Although assimilation clearly involved little accompanying fractionation, the occurrence of this lower-crustal component at the surface today (crustal samples F25 and F27) means it is equivocal as to whether or not this assimilation took place at lower-crustal levels.
Mafic magmas erupted through the western part of the volcanic province have also commonly assimilated large amounts of lower-crustal material (C2), e.g. JB282. More evolved samples either show evidence for no further contamination or have a signature of contamination by upper continental crust (C3). The relatively limited isotopic contrast between the primary isotopic composition of the flood basalts and the young, Late Proterozoic, crustal components (C2 and C3) in the western part of the volcanic province means that the radiogenic and oxygen isotope effects of contamination are less obvious in this suite of samples than in the samples erupted through the eastern part of the volcanic province. It also makes it more difficult to model the amounts of contamination. However, given the ubiquitous lithospheric trace element signature of continental crust, regardless of its age, the trace element effects of contamination are similar in both suites of basalts (Fig. 6).
Thus, contamination processes in Yemen varied from early lower-crustal contamination of hot mafic magmas with little or no concomitant fractionation (r > 1) through to combined assimilation and fractional crystallization typically within upper-crustal magma chambers. The most extreme result of the decline in the rate of assimilation to fractional crystallization is probably represented by the rhyolites, which require extensive fractionation with only limited amounts of contamination. The switch from lower- to upper-crustal contamination reflects establishment of magmatic plumbing systems; early intrusion of magmas into the lower crust resulted in hot mafic magmas removing the fusible parts of the lower crust and subsequent establishment of upper-crustal magma chambers produced more evolved magmas with a variable upper-crustal overprint. Plagioclase fractionation in the most evolved and upper crustally contaminated samples is consistent with a switch in the depth of fractionation and assimilation from deep to shallow crustal levels.
Identification of crustal contamination taking place in the lower crust when hot mafic magmas are introduced into the lithosphere has long been postulated as being important in flood basalt provinces (Thirlwall & Jones, 1983
; Cox & Hawkesworth, 1985
; Huppert & Sparks, 1985
; Devey & Cox, 1987
; Kerr et al., 1995
; Martinez et al., 1996
). This has now been verified by oxygen isotope studies of flood basalts from both the Deccan Traps and Yemen (Peng et al., 1994
; herein). Presumably, assimilation is facilitated by the limited heat input required to melt already hot lower crust. What is also important to note is that magmas contaminated at this stage also have near-primary (i.e. low) incompatible trace element contents rendering them highly susceptible to small amounts of contamination and acquisition of lithospheric-like trace element and isotopic signatures.
Origin of rhyolitic volcanism
Clinopyroxene separated from four rhyolitic rocks has
18O = 5·96·1
. These values are lower than those observed in some of the more contaminated flood basalts, including samples contaminated by crustal rocks in the western part of the volcanic province through which the rhyolites were erupted. Moreover, as discussed above, the slightly elevated
18O values of the rhyolite clinopyroxenes may largely be accounted for by extensive crystal fractionation.
Oxygen isotope data for the rhyolite samples might seem to preclude an origin for the rhyolites by extensive crustal melting in this province, and be more consistent with a model for rhyolite petrogenesis involving protracted fractionation with relatively limited assimilation from flood basalt parent magmas (Chazot & Bertrand, 1995
). However, some Pan-African crust clearly has low
18O, which requires examination of other chemical and isotopic data to determine the petrogenesis of the rhyolites. Moreover, currently available chemical and isotope data are not sufficient to test an alternative hypothesis that the rhyolites might have been generated by melting of underplated basaltic material related to the flood volcanic episode (e.g. Harris & Erlank, 1991
). Either of the latter two hypotheses has important implications for melt generation in this volcanic provincelarge amounts of unerupted mafic material equivalent to several times the volume of erupted rhyolite must be present in the lithosphere. Given that the basalt:rhyolite ratio is
1:1 in Yemen and Ethiopia, the volume of (basaltic) melt produced and the rate at which it was produced is at least three times greater than that currently inferred from study of the preserved volcanic volumes.
The primary oxygen isotope signature
Baker et al. (1996b)
noted that the primary trace element and isotopic signature of the Yemen flood basalts is characterized by LILE depletion relative to the high field strength elements and a depleted SrNd isotopic signature that approaches that of HIMU or PREMA mantle (Figs 5 and 6). However, Pb isotope ratios are not as radiogenic as HIMU mantle proper. These features are similar to those exhibited by magmas produced by the Iceland plume and have been explained in terms of recent recycling of oceanic lithosphere, i.e. the Afar and Iceland mantle plumes are immature HIMU mantle plumes (Thirlwall et al., 1994
; Baker et al., 1996b)
.
It is noteworthy that, to date, the least crustally contaminated flood basalt samples from Yemen do not share the particularly low
18O values that have been observed in some rocks from Hawaii, Iceland and some other HIMU ocean islands (Eiler et al., 1997
). Low K/Nb and Ba/Nb ratios (<150 and <5, respectively) in Yemen flood basalts with the lowest
18O values preclude these rocks being substantially crustally contaminated (<<5%) and having primary
18O values significantly lower than their measured values. Moreover, LM xenoliths metasomatized by the Afar plume (Baker et al., 1998
) also do not have low
18O values (Chazot et al., 1997
).
The final point concerning the oxygen isotope signature of the least contaminated Yemen flood basalts is that basanites and basalts sensu stricto have similar oxygen (and radiogenic) isotope ratios. Major and trace element differences between the basanite and basalt rocks are readily explained in terms of depth and degree of partial melting, with the basanites being the product of smaller average degrees of partial melting generated at greater depths than the basalts within the Afar plume. As such, there is apparently no partial melting control on oxygen isotope ratios in the Yemen flood basalt suiteat least within the resolution of the laser fluorination technique.
| CONCLUSIONS |
|---|
|
|
|---|
Oxygen isotope heterogeneity of minerals separated from Oligocene flood volcanic rocks from Yemen exceeds analytical reproducibility and also that observed in oceanic basalts and mantle peridotites. High
18O values are correlated with changes in radiogenic isotope ratios, such as increasing 87Sr/86Sr. Samples with high
18O values include primitive and evolved compositions. The oxygen isotope data place the following constraints on magma genesis during flood volcanism in Yemen:
- assimilation of heterogeneous Pan-African crust is unequivocally confirmed to have been the major control on isotopic and much trace element variability in this flood volcanic province.
- The assimilated crustal components include both upper and lower crust of variable age. Assimilation of lower crust was a particularly important process in the Yemen flood volcanic province.
- Crustal contamination processes can be demonstrated to have varied from combined assimilation and fractional crystallization through to rapid assimilation of crust by hot mafic magmas with little or no concomitant fractionation.
- Rhyolitic magmas are not characterized by excessively high
18O values and/or crustal radiogenic isotope ratios, which seems to preclude their origin by wholesale crustal anatexis. The
18O data suggest they are probably either the product of extensive assimilation with small amounts of crustal contamination from basaltic parents or the result of melting underplated flood basalt material.
- Least contaminated samples with low
18O have radiogenic isotope ratios that approach those inferred for the Afar plume, and these samples have
18O values within the range of other crustally uncontaminated plume-related magmas, i.e. ocean island basalts.
Laser fluorination oxygen isotope analysis of mineral separates is a powerful tool for examining the relative roles of crust and mantle in suites of continental volcanic rocks. Future combined oxygen and osmium isotope studies, along with in situ mineral multi-collectorinductively coupled plasma mass spectrometry studies, should finally resolve the debate regarding the relative contributions of crust and LM to flood basalt magmas.
| ACKNOWLEDGEMENTS |
|---|
Abdulkarim Al-Subbary is thanked for assistance with fieldwork in Yemen. Gerry Ingram helped with radiogenic isotope analyses. The British Council, Royal Society and the Industrial Association at RHUL supported this research. The radiogenic and stable isotope laboratories at RHUL are University of London Intercollegiate facilities. Constructive reviews by John Eiler, Richard Carlson and Chris Harris, which improved this manuscript, are gratefully acknowledged.
| FOOTNOTES |
|---|
*Corresponding author. Present address: Danish Lithosphere Centre, Øster Voldgade 10, L, 1350 Copenhagen K, Denmark. Telephone: +45 38 14 26 42. Fax: +45 33 11 08 78. e-mail: jab{at}dlc.ku.dk
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, Yemen flood basalts erupted through the western part of the volcanic province;
, rhyolites erupted through the western part of the volcanic province;
, flood basalts erupted through the eastern part of the volcanic province. 






