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EXCESS RADIOGENIC.. Hebeda1980
EXCESS RADIOGENIC.. Hebeda1980
[11
E.H. HEBEDA, N.A.I.M. BOELRIJK, H.N.A. PRIEM, E.A.Th. VERDURMEN, R.H. VERSCHURE
z. It/.0. Laboratorium voor Isotopen-Geologie, De Boelelaan 1085, 1081 H V Amsterdam (The Netherlands)
and
O.J. SIMON
Geologisch Instituut, Universiteit van Amsterdam, Nieuwe Prinsengracht 130, 1018 VZ Amsterdam (The Netherlands)
Metamorphosed basic intrusives in the Alpine orogen of southern Spain contain relicts of unmetamorphosed
gabbroic rock. Rb-Sr investigation of one of these relicts indicates that the rock and constituent minerals remained
closed to Rb-Sr during the plurifacial Alpine metamorphism. The Rb-Sr isochron age is 146 -+ 3 Ma with initial
87Sr/86Sr of 0.7028 -+ 0.0001 (h87 Rb = 1.42 × 10 -11 a-l), which is taken as approaching the intrusion age. All
investigated relicts of unmetamorphosed rock are characterized by excess 4 OAr contents between about 6 × 10-6
and 14 × 10 -6 cm 3 NTP/g, whereas the metamorphosed parts of the basic intrusives rarely show this phenomenon.
It is argued that this argon, which is very inhomogeneously distributed, was acquired during the Alpine meta-
morphism. A comparison of the excess 4°Ar contents of the pyroxene and the plagioclase with published data
suggests that in all cases the crystals have acquired the argon under about the same prevailing 4 OAr partial pressure,
even when the geologic conditions were different.
ALICANTE
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CARTAGENA
- - ~ POST-NAPPES SEDIMENTS
MALAGUtDE COMPLEX
~= ,so,area outc,ops
~ ALPUJARRIDE COMPLEX
1~ B A L L A B O N A - C U C H A R O N COMPLEX
NEVADO-FII-ABRIDE COMPLEX
ALMERIA
SAMPLING SITE
J ÷
N
M E 0
I
510kin
Fig. 1. Major tectonic units of the internal (or Betic) zone of the Betic Cordilleras. All investigated basic intrusives are in the
Nevado-FilabrideComplex and the Ballabona-Cuchar6n Complex. The Universal Transverse Mercator coordinates of the sampling
sites are: site 1, 06.80.05/42.18.65; site 2, 05.61.12/41.28.38; site 3, 05.82.55/41.19.47; site 4, 06.70.28/42.14.28; site 5,
06.46.75/41.86.43; site 6, 06.06.23/41.52.18; site 7, 05.70.25/41.24.70; site 8, 05.48.82/41.29.65.
[ 7 - 9 ] . Most rocks o f the Alpujarride Complex dis- graphical methods due to the apparent absence o f
play low-grade metamorphism, but the basal post-Triassic sediments in the lower nappe complexes,
sequences have been affected by higher-grade Alpine but they are thought to have started in the Late
regional metamorphism [ 4 , 1 0 - 1 2 ] . Cretaceous to Paleocene [4]. All overthrusting came
Opinions differ strongly as to the direction(s) and to an end in the Early Miocene [13], in accordance
ages o f the phases of (over)thrusting. The onset of the with a number o f K-Ar and Rb-Sr mica ages between
overthrust movements cannot be dated by biostrati- 19 and 12 Ma [ 1 4 - 1 6 ] .
83
were measured as powders; the mass-absorption cor- and initial 87Sr/86Sr ratio are quoted at the 95% con-
rections for both sample and external standard are fidence level as computed from the scatter o f the data
based upon the Compton scattering of the Mo-Ka about the regression line.
primary beam [22]. The Rb and Sr contents of the The age calculations are based upon the following
whole-rock and the other minerals were determined constants (lUGS recommended values): ~.87Rb =
by mass-spectrometric isotope dilution. Sr isotopic 1.42 × 10 -11 a-1;X4°K~ = 4.962 × 10 -1° a - l ;
compositions were measured directly on unspiked Sr Xa°K e = 0.581 X 10 -1° a - l ; isotopic abundance
and also calculated from the isotope dilution runs. 4°K = 0.01167 atom % total K.
The Rb samples were prepared by a double cation
exchange procedure. Blanks for the total procedure
were 0 . 2 - 0 . 3 ng; as the nominal amounts of Rb 4. Rb-Sr age of the basic intrusive near Lubrin
separated from the olivine and plagioclase were
about 50 ng, the error in the Rb content due to con- The Rb-Sr systematics o f one spheroid o f unmeta-
tamination is less than 1% relative. The isotope mea- morphosed gabbro from an intrusive near the village
surements were made on a computer-controlled of Lubrin (ALM 104, site 3 ) w e r e investigated in
Varian CH5 mass-spectrometer with Faraday cage detail. Measurements were made on the whole-rock
collector and digital output (value of normalised and on the separated minerals clinopyroxene, olivine,
87Sr/a6Sr of the NBS 987 8r(CO3)2 standard mea- plagioclase, hornblende and biotite. The results are
sured as 0.71016 -+ 0.00008). For the analytical listed in Table 1 and plotted in the isochron diagram
accuracies, see Table 1. of Fig. 2.
Potassium contents were determined by flame The data-points are very well linearly correlated
photometry with lithium internal standard and a and define an isochron o f 146 -+ 3 Ma with initial
buffer of caesium chloride + aluminium nitrate. 878r/86Sr o f 0.7028 -+ 0.0001. This age is essentially
Argon was extracted in a bakeable glass vacuum appa- determined by the biotite: the pair whole-rock/
ratus and determined by isotope dilution techniques biotite yields an age o f 146 Ma with initial 87Sr/86Sr
on a GD-150 mass spectrometer. For K and Ar the of 0.7027. If the biotite is excluded from the calcula-
relative analytical accuracies are estimated at 1% and tion, the other points define an isochron of 126 Ma,
2%, respectively. but in view of the large error limits this age can be
The Rb-Sr isochron was computed by means of taken to be concordant with the biotite age o f
a least-square regression analysis according to York 146 Ma.
(1966, 1967). Errors in the calculated isochron age We assume that the age o f 146 Ma represents a
TABLE 1
Rb-Sr data of the basic intrusive near Lubrfil (ALM 104, site 3)
* Isotope dilution data, except for the pyroxene and hornblende which were analyzed by X-ray fluorescence spectrometry. (2)
and (4), average of two and four analyses, respectively.
** (3), (4) and (5), average of three, four and five analyses, respectively. Accuracies estimated at 0.03%.
*** Accuracy estimated at 2% for the whole-rock and biotite, and 10% for the olivine, plagioclase and hornblende. The accuracy
for the pyroxene is very poor because of the low Rb content; these data were not used for the isochron calculation.
85
0704 ( 87Sr/86sr)O = 0" 7020 ~ 0.0001 The whole-rock and separated minerals of the un-
metamorphosed gabbro investigated for their Rb-Sr
0.720
relationships (ALM 104) were also analysed for K-At.
0~ OLM
~ cpx From the same intrusive (site 3) two other samples of
0.716
unmetamorphosed gabbro (ALM 20 and 37) were
analysed, along with a sample of the amphibolitic
0702 part (ALM 38). Moreover, K-Ar whole-rock measure-
ments were made on 10 samples from seven other
o, R /8osr o2
basic intrusives, six of unmetamorphosed or weakly
Fig. 2. Rb-Sr isochron plot of whole-rock and separated metamorphosed gabbroic-doleritic rock and four of
minerals from a relict of unmetamorphosed gabbroic rock metabasite. The analytical data and calculated ages
within the metamorphosed basic intrusive near Lubrfn are given in Table 2.
(site 3). BIO = biotite; HBL = hornblende; OLV = olivine; The apparent ages of the analysed samples vary
PLG = plagioclase; CPX = clinopyroxene; WR = whole-rock.
greatly (Fig. 3), without any correlation with their
geologic position. All nine samples of unmetamor-
phosed or weakly metamorphosed gabbroic-doleritic
rock contain varying amounts of excess radiogenic
At, ranging from about 6 × 10 -6 to 14 × 10 -6 cm 3
minimum age for the basic intrusion. The geological NTP/g with respect to the Rb-Sr age of 146 Ma. Of
relationships only indicate that the basaltic magma- the five metabasite samples, however, only one con-
tism took place during or later than the Late Triassic tains some excess radiogenic Ar (ALM 38); all others
and before the Early Miocene. However, basaltic show younger K-At ages, apparently resulting from
flows and intrusions of Late Jurassic and Early Creta- partial or complete Ar loss during the Alpine meta-
ceous age have been reported from sedimentary morphism.
sequences at several places in the Subbetic Zone of The metabasite sample ALM 38 containing excess
southeastern Spain [16,23] and the Haut Atlas of radiogenic Ar comes from the amphibolitic mass in
Morocco [24,25]. The age of 146 Ma (Late Jurassic, the basic intrusive near Lubrfn (site 3), but the con-
approximately Oxfordian [26]) could thus very well
approach the true age of the basic intrusives in the
Nevado-Filabride Complex. This implies that the i i I
parently, the local absence of fluid phases under con- Fig. 3. Histogram of apparent K-Ar ages of basic intrusives in
ditions o f regional metamorphism in a relatively dry the internal (Betic) zone of the Betic Cordilleras. Hatched,
rock prevents not only the occurrence of metamor- samples from metamorphosed rocks; blank, samples from
phic reactions, but also the Rb-Sr isotopic redistribu- unmetamorphosed or weakly metamorphosed rocks; B10 =
tion between the constituent minerals. A similar biotite; CPX = clinopyroxene; OLV = olivine; PLG = plagio-
clase; all others, sieve fractions (-250, +125 t~m) of the
observation has been reported for pre-Alpine biotites whole-rock. The Rb-Sr isochron age of the Lubrfn metabasite
from ultramaflc masses in the Alps [27]. (site 3) is also shown.
86
TABLE 2
K-Ar data of the investigated basic intrusives
* Sieve fractions: whole-rocks, -250, +125/~m; pyroxene and olivine, -100, +80 ~m; plagioclase, hornblende and biotite, -125,
+63 ~m. The numbers between brackets refer to the sites of the intrusives shown on the map of Fig. 1.
** With reference to the Rb-Sr age of 146 Ma.
centration in this sample is much smaller than in the through all components of the rock. However, much
three samples of unmetamorphosed gabbro from the less excess radiogenic Ar occurs in the constituent
same intrusive (0.3 × 10 -6 cm 3 versus about 7 X 10 -6 minerals than in the whole-rock. The highest concen-
to 14 X 10 -6 cm 3 NTP/g). The sample of unmeta- tration in any of the minerals is about 10 X 10 -6 cm 3
morphosed gabbro from which the minerals were NTP/g, some 30% lower than in the whole-rock. This
separated (ALM 104) contains about 13 X 10 -6 cm a discrepancy may partly be attributed to the fact that
NTP/g excess radiogenic Ar. Although the analyses the separated minerals were ground to a finer grain
were made on aliquots of 0.5 to 0.8 g, the reproduci- size than the whole-rock: - 1 2 5 , +63/am for the
bility of the five Ar determinations is extremely poor. plagioclase, hornblende and biotite and - 1 0 0 , + 8 0 / l m
(Table 2), however, in comparison with the analytical for the pyroxene and olivine, versus - 2 5 0 , +I 25/~m
precision usually obtained in our laboratory. This for the whole-rock. It appears that the rock contains
indicates that the excess radiogenic Ar is very inhomo- sites with a very high excess radiogenic Ar content,
geneously distributed through the rock. part of which is set free during the grinding and
Analysis of the constituent minerals shows that mineral separation. Such sites may be, for example,
the excess radiogenic Ar is not confined to a single or interstitial grains of K-feldspar [28], grain boundaries,
a few mineral components, but that it is distributed fluid inclusions, and defects within the crystal lattice
87
such as structural holes, edge dislocations and anion NTP/g. This difference in partial pressure of 4 ° A r
vacancies [29]. between the basic intrusives and the environmental
Cases of basic rocks with whole-rocks containing rocks resulted in an introduction of 4°Ar into the
a higher excess radiogenic Ar content than the con- basic rocks. A similar explanation has been invoked
stituent minerals have also been reported from else- for the excess radiogenic Ar observed in the Precam-
where. For the Early Jurassic diabase dikes in Liberia brian dolerites of Suriname [33].
Dalrymple et al. [30] described two samples (L3 and During the subsequent metamorphic recrystalliza-
L6) with a higher content of excess radiogenic Ar in tions, the 4°At acquired from the degassing environ-
the whole-rock than in the constituent plagioclase mental rocks was expelled again from the basic intru-
and pyroxene. sives. Most of the strongly recrystallized metabasites
therefore now contain none or very little excess
radiogenic Ar. However, in those portions of the basic
6. Origin of the excess radiogenic Ar intrusives that were sufficiently shielded against the
agents of metamorphism to preserve their original
A magmatic origin does not seem to be a plau- mineralogical compostion and to remain closed with
sible explanation for the excess radiogenic Ar in the regard to Rb-Sr, the acquired 4°Ar was not, or only
rocks under discussion. The highest amounts of partially expelled.
excess 4°Ar of undoubtedly magmatic derivation are The release of the accumulated radiogenic Ar from
reported for basaltic lavas erupted at the deep ocean the environmental country rocks may very well have
floor [31,32] and they are at least one order of mag- started before the beginning of the metamorphic
nitude smaller. Also, incorporation of excess radio- reconstitution of the rocks. One might speculate that
genic Ar in the magma at the time of the intrusion the introduction of excess radiogenic Ar took place at
and crystallization [30] does not provide a satis- the onset of the first phase of regional metamor-
factory explanation, as it is difficult to visualize how phism, the synkinematic glaucophane schist facies.
enough heat can have been set free by the relatively Due to the penetrative deformation under the prevail-
small intrusive to release substantial amounts of ing high-pressure conditions, passage ways may have
radiogenic Ar from the wall rock in a cold crustal been opened, allowing the introduction of the 4 ° A r
environment. gas into the basic intrusives with a lower prevailing
We postulate that the excess radiogenic Ar in the 4°Ar partial pressure and incorporation in the mineral
basic intrusives was acquired during Alpine meta- components. During the metamorphic reconstitution
morphism. When the outgassing of the crustal block of the intrusives the original igneous rock has survived
started at the beginning of the metamorphism, say unchanged in relatively small domains, apparently
about 70 Ma ago, the prevailing 4°Ar pressure must because they remained shielded against percolating
have been higher in the environmental country rocks fluids and consequently did not adjust to the meta-
(much of them Triassic pelitic sediments, converted morphic conditions. Possibly, this shielding was
to schists during the metamorphism) than in the rela- brought about by the reconstituted rock mass sur-
tively small basic intrusives. If we assume a K content rounding these domains, which mass may have acted
between 0.5 and 2.5% for the sediments, as much as as a "protective armour". Much or all the newly
between 3 X 10 -6 and 15 × 10 -6 c m 3 NTP/g radio- acquired excess radiogenic Ar remained stored within
genic Ar was generated in situ in the time interval such "armoured relicts" of unmetamorphosed gab-
between deposition and metamorphism (of the order broic-doleritic rock during the later phase of meta-
of 150 Ma); in addition there was an unknown morphism.
amount of inherited radiogenic Ar, already present
in the detrital minerals at the time of deposition.
Much or all of this Ar was set free during the Alpine 7. Excess radiogenic Ar in pyroxene and plagioclase
metamorphism and became available as a gaseous
phase to the basic intrusives with radiogenic Ar con- In the histograms of Fig. 4 the contents of excess
tents of the order of 0.5 × 10 -6 to 1.5 X 10 -6 cm 3 radiogenic Ar in pyroxene and plagioclase from the
88
T T
572 64.1
PYROXENE !i
%
~2o
1 2
re
ILl 10
m
=E I I I
.-3 10 o o
Z o L~27c
• o •1•
L 27 d "~ L 27a
@ PLAGIOCLASE t i
K(%)
Fig. 4. Histograms of excess radiogenic Ar contents in higher in the plagioclase than in the pyroxene; the
pyroxenes and plagioclases from basic intrusives. Open circle, ratios are 5.1 in our sample ALM 104, between 4.9
Great Dyke, Rhodesia [ 36]; open asterisks, diabase dikes,
and 6.7 in the samples from the Liberian dikes [30]
Liberia [ 30] ; triangles, Avanavero Dolerite, Suriname [ 33 ] ;
diamonds, Roraima Dolerites, Guyana [ 37 ] ; closed circles, and 5.0 for one sample from the Precambrian
Freetown Complex, Sierra Leone [38] ; closed asterisks, Avanavero Dolerite in Suriname [33].
Lubrl"n metabasites, this study. For the plagioclase the excess radiogenic Ar con-
tents are plotted against the corresponding K con-
tents in Fig. 5, along with those calculated from the
unmetamorphosed gabbro sample ALM 104 are published data. There appears to be no correlation
plotted, along with the contents published for these between b o t h variables, nor between these variables
minerals from a number of other basic intrusives. For and the nature o f the country rock. For example, the
each mineral the contents appear to be o f the same Early Jurassic basic dikes intrusive into the 550 Ma
magnitude, in spite of the fact that the excess radio- old basement and those intrusive into the 2.7 Ga old
genic Ar has been acquired by different mechanisms basement of Liberia contain both excess radiogenic
and under different pressuretemperature conditions. Ar contents o f the same order of magnitude [30] :
Experimental studies have shown that there is a pro- mean values o f about 7 X 10 -6 and 9 X 10 -6 cm 3
portionality between the amount of incorporated NTP/g, respectively, assuming that the dikes are o f
noble gases and the partial pressure [34], so it may be the same age as the Freetown Complex in Sierra
assumed that the minerals have acquired their excess Leone, i.e. 193 Ma [35]. The only significant differ-
radiogenic Ar under approximately the same environ- ence between b o t h groups may be that the latter
mental partial 4°Ar pressure. In those cases where shows a larger spread in the K contents than the
data are available for the corresponding pyroxene and former. There also appears to be no consistent differ-
plagioclase from the same rock sample, the amount ence in excess radiogenic Ar content between plagio-
of excess radiogenic Ar appears to be about five times clase from the chilled border zone and from the more
89
tion of Morocco and eastern North America: a Triassic- 32 J.G. Funkhouser, D.E. Fisher and E. Bonatti, Excess
Liassic stratigraphic record, Geol. Soc. Am. Bull. 89 argon in deep-sea rocks, Earth Planet. Sci. Lett. 5 (1968)
(1978) 901-920. 95-100.
26 J.E. van Hinte, A Jurassic time scale, Am. Assoc. Pet. 33 E.H. Hebeda, N.A.I.M. Boelrijk, H.N.A. Priem, E.A.Th.
Geol. Bull. 60 (t976) 489-497. Verdurmen and R.H. Verschure, Excess radiogenic argon
27 A. Arnold and E. J~iger, Altersbestimmungen an Glim- in the Precambrian Avanavero Dolerite in western
mern und Grenzbereich zwischen voralpinen Alterswerten Suriname (South America), Earth Planet. Sci. Lett. 20
und alpiner Verjiingung der Biotite. Eclogae Geol. Helv. (1973) 189-200.
58/1 (1965) 369-390. 34 T. Kirsten, Incorporation of rare gases in solidifying
28 E.A. Mankinen and G.B. Dalrymple, Electron microprobe enstatite melts. J. Geophys. Res. 73 (1968) 2807-2810.
evaluation of terrestrial basalts for whole-rock K-Ar 35 R.D. Beckinsale, J.F.W. Bowles, R.J. Pankhurst and M.K.
dating, Earth Planet. Sci. Lett. 17 (1972) 89-94. Wells, Rubidium-strontium age studies and geochemistry
29 M.S. Lancet and E. Anders, Solubilities of noble gases in of acid veins in the Freetown complex, Sierra Leone,
magnetite: implications for planetary gases in meteorites, Mineral. Mag. 41 (1977) 501-511.
Geochim. Cosmochim. Acta 37 (1973) 1371-1388. 36 H.L. Altsopp, Rb-Sr and K-Ar age measurements on the
30 G.B. Dalrymple, C.S. Gromme and R.W. White, Potas- Great Dyke of southern Rhodesia, J. Geophys. Res. 70
sium-argon age and paleomagnetism of diabase dikes in (1965) 977-984.
Liberia: initiation of central Atlantic rifting, Geol. Soc. 37 I. McDougall, Isotopic dating of the Roraima Dolerites,
Am. Bull. 86 (1975) 399-411. Geophys. J.R. Astron. Soc. 16 (1968) 141-145.
31 G.B. Dalrymple and J.G. Moore, Argon-40: excess in sub- 38 N.J. Snelling, Institute of Geological Sciences, London,
marine pillow basalts from Kilauea volcano, Hawaii, private communication (1978).
Science 161 (1968) 1132-1135.