GEOSCIENCE FRONTIERS 3(6) (2012) 801e811

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China University of Geosciences (Beijing)

GEOSCIENCE FRONTIERS
journal homepage: www.elsevier.com/locate/gsf

RESEARCH PAPER

Phase equilibrium modeling of incipient charnockite

formation in NCKFMASHTO and MnNCKFMASHTO
systems: A case study from Rajapalaiyam, Madurai
Block, southern India
Takahiro Endo a, Toshiaki Tsunogae a,b,*, M. Santosh c,d, E. Shaji e

a
Graduate School of Life and Environmental Sciences, University of Tsukuba, Ibaraki 305-8572, Japan
b
Department of Geology, University of Johannesburg, Auckland Park 2006, South Africa
c
Division of Interdisciplinary Science, Faculty of Science, Kochi University, Kochi 780-8520, Japan
d
China University of Geosciences (Beijing), 29 Xueyuan Road, Beijing 100083, China
e
Department of Geology, University of Kerala, Kariyavattom, Trivandrum 695 581, India

Received 26 March 2012; received in revised form 2 May 2012; accepted 17 May 2012
Available online 26 May 2012

KEYWORDS Abstract Incipient charnockites represent granulite formation on a mesoscopic scale and have received
Incipient charnockite; considerable attention in understanding fluid processes in the deep crust. Here we report new petrological
Granulite; data from an incipient charnockite locality at Rajapalaiyam in the Madurai Block, southern India, and
Pseudosection; discuss the petrogenesis based on mineral phase equilibrium modeling and pseudosection analysis.
Reduced fluid; Rajapalaiyam is a key locality in southern India from where diagnostic mineral assemblages for
Petrology; ultrahigh-temperature (UHT) metamorphism have been reported. Proximal to the UHT rocks are patches
Southern India and lenses of charnockite (Kfs þ Qtz þ Pl þ Bt þ Opx þ Grt þ Ilm) occurring within Opx-free Grt-Bt
gneiss (Kfs þ Pl þ Qtz þ Bt þ Grt þ Ilm þ Mt) which we report in this study. The application of mineral
equilibrium modeling on the charnockitic assemblage in NCKFMASHTO system yields a p-T range of
w820  C and w9 kbar. Modeling of the charnockite assemblage in the MnNCKFMASHTO system
* Corresponding author. Graduate School of Life and Environmental
Sciences, University of Tsukuba, Tennoudai 1-1-1, Ibaraki 305-8572,
Japan.
E-mail address: tsunogae@geol.tsukuba.ac.jp (T. Tsunogae).
1674-9871 ª 2012, China University of Geosciences (Beijing) and Peking
University. Production and hosting by Elsevier B.V. All rights reserved.

Peer-review under responsibility of China University of Geosciences

(Beijing).
doi:10.1016/j.gsf.2012.05.005

Production and hosting by Elsevier

802 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811

indicates a slight shift of the equilibrium condition toward lower p and T (w760  C and w7.5 kbar),
which is consistent with the results obtained from geothermobarometry (710e760  C, 6.7e7.5 kbar),
but significantly lower than the peak temperatures (>1000  C) recorded from the UHT rocks in this
locality, suggesting that charnockitization is a post-peak event. The modeling of T versus molar H2O
content in the rock (M(H2O)) demonstrates that the Opx-bearing assemblage in charnockite and Opx-
free assemblage in Grt-Bt gneiss are both stable at M(H2O) Z 0.3 mol%e0.6 mol%, and there is no
significant difference in water activity between the two domains. Our finding is in contrast to the previous
petrogenetic model of incipient charnockite formation which envisages lowering of water activity and
stabilization of orthopyroxene through breakdown of biotite by dehydration caused by the infiltration
of CO2-rich fluid. T-XFe3þ (ZFe2O3/(FeO þ Fe2O3) in mole) pseudosections suggest that the oxidation
condition of the rocks played a major role on the stability of orthopyroxene; Opx is stable at XFe3þ
<0.03 in charnockite, while Opx-free assemblage in Grt-Bt gneiss is stabilized at XFe3þ >0.12. Such
low oxygen fugacity conditions of XFe3þ <0.03 in the charnockite compared to Grt-Bt gneiss might be
related to the infiltration of a reduced fluid (e.g., H2O þ CH4) during the retrograde stage.
ª 2012, China University of Geosciences (Beijing) and Peking University. Production and hosting by
Elsevier B.V. All rights reserved.

1. Introduction The Rajapalaiyam area in the southern margin of the Madurai

The Southern Granulite Terrane (SGT) in India is known as one of
the classic examples of regionally metamorphosed granulite-facies
complexes formed during late Neoproterozoic to early Cambrian
(w0.55 Ga, e.g., Braun et al., 1998; Santosh et al., 2003, 2006a,b,
2009; Collins et al., 2007a,b) collisional orogeny related to the
amalgamation of Gondwana supercontinent. The SGT is composed
of several granulite blocks (e.g., Trivandrum Block, Madurai
Block, Nilgiri Block) and shear/suture zones that dissect these
blocks (Fig. 1a). The SGT has also been in focus with regard to
granulite formation on a mesoscopic scale where orthopyroxene-
bearing patches, veins and lenses termed as “incipient charnock-
ites” have developed within garnet-biotite gneisses representing
dehydration induced by fluids (e.g., Santosh et al., 1990; Raith and
Srikantappa, 1993; Tsunogae and Santosh, 2003; Endo et al., 2012).
Block is a key locality in the SGT, where sapphirine þ quartz
assemblage was first reported from southern India by Tateishi
et al. (2004), suggesting peak metamorphism at ultrahigh-
temperature conditions of w1000  C. In this study, we report
the occurrence of incipient charnockites in a gneissic quarry
close to the sapphirine þ quartz locality (Fig. 1b). We present
new mineralogical and petrological data on the incipient char-
nockite and surrounding orthopyroxene-free gneiss and apply
mineral equilibrium modeling to evaluate the petrogenesis of the
charnockite formation. For the phase analysis, we adopted the
complex system, including TiO2, Fe2O3, and MnO for the
application to natural rocks. Particularly, this is the first attempt
to apply MnNCKFMASHTO system on charnockites, and our
results challenge the existing models on incipient charnockite
genesis.

Figure 1 (a) Geological map of southern India showing various granulite blocks and major shear/suture zones (modified after GSI, 1995;
Santosh and Sajeev, 2006) and the locality of incipient charnockite (star) discussed in this study. ACSZ: Achankovil Shear Zone, PCSZ: Palghat-
Cauvery Suture Zone, CSZ: Cauvery Shear Zone. (b) Geological map of the area and sample location.
 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811
2. Geological setting
The Madurai Block in the SGT is composed dominantly of
massive charnockites, hornblende-biotite orthogneiss, metasedi-
ments, marble/calc-silicate associations, mafic/ultramafic rocks,
Mg-Al-rich rocks, and late alkali-feldspar granites. The pelitic
and Mg-Al-rich units preserve the evidence for peak UHT
metamorphism as confirmed by the occurrence of some key
minerals or mineral assemblages such as sapphirine þ quartz,
orthopyroxene þ sillimanite þ quartz, spinel þ quartz, Al-rich
orthopyroxene, and mesoperthite (e.g., Sajeev et al., 2004;
Tamashiro et al., 2004; Tateishi et al., 2004; Tsunogae and
Santosh, 2006, 2010, 2011; Santosh and Sajeev, 2006; Braun
et al., 2007; Tsunogae et al., 2008; Kondou et al., 2009). The
timing of UHT metamorphism in this region has been constrained
as 550e520 Ma, associated with the final assembly of the Indian
fragment within the Gondwana supercontinent (Santosh et al.,
2006b). At Rajapalaiyam, the dominant rock types are garnet-
bearing granulites (dominantly quartzo-feldspathic and pelitic
gneisses) intruded by pink alkali-feldspar granite (Fig. 1b).
The granulites show NNW-SSE trending foliation with steep dips
(85 ) toward NE with well-defined alternation of garnet-
orthopyroxene-rich and quartzo-feldspathic layers. Sriramguru
et al. (2002) first reported sapphirine in this locality from pelitic
xenoliths (garnet þ orthopyroxene þ cordierite þ spinel þ
plagioclase þ perthite) in the alkali-feldspar granite, and deter-
mined peak temperatures of 860  C from garnet-orthopyroxene
geothermometer and 950  C from feldspar thermometer on mes-
operthite. Tateishi et al. (2004) reported fine-grained intergrowth
of sapphirine þ quartz within porphyroblastic garnet in pelitic and
quartzo-feldspathic granulites from the locality and inferred peak
metamorphism at >1000  C, which is consistent with their
temperature estimates using ternary feldspar and sapphirine-spinel
geothermometers (950e1000  C). Tsunogae and Santosh (2006,
2010) performed detailed investigation on various reaction
textures in sapphirine þ quartz bearing granulites and estimated
peak p-T condition of 1050e1070  C and 8.5e9.5 kbar, which
was followed by isobaric cooling from sapphirine þ quartz field to
orthopyroxene þ sillimanite þ quartz field and subsequent
decompression to form various corona textures.
The gneiss-incipient charnockite pairs analyzed in this study
were collected from a previously unreported quarry located about
200 m east-southeast of the UHT locality from where Tateishi et al.
(2004) first reported sapphirine þ quartz assemblage. Both expo-
sures are along quarried hillocks about 4 km east-southeast of the
Rajapalaiyam town (Fig. 1). The locality exposes charnockites
occurring within foliated orthopyroxene-free garnet-biotite (Grt-Bt)
gneiss (Fig. 2a). The Grt-Bt gneiss is the dominant lithology in the
quarry. Foliation defined by alternation of pink K-feldspar-rich
layers and quartz þ biotite - rich gray layers can be seen in weathered
surface (Fig. 2b). Irregular patches or lenses of dark grayish to
brownish charnockite are present throughout the quarry. The size of
the patches varies from 50 cm to up to 3 m. Although foliation is
obvious in the Grt-Bt gneiss, it disappears while passing into the
charnockite patches (Fig. 2b). The lack of foliation observed in the
present case is closely comparable with a similar feature displayed
by gneiss-incipient charnockite locations elsewhere in southern
India (e.g., Pichamuthu, 1960; Santosh et al., 1990; Raith and
Srikantappa, 1993). The charnockite patches in the Rajapalaiyam
quarry do not show any systematic distribution pattern, although
a prominent structural control in incipient charnockite patches has
803
been described in previous studies from other localities (e.g., Santosh
et al., 1990; Raith and Srikantappa, 1993). Two representative
samples (charnockite (sample MD31-3A) and Grt-Bt gneiss (sample
MD31-3B)) collected from this quarry were examined in detail.
3. Petrography
The Grt-Bt gneiss (sample MD31-3B) is composed mainly of K-
feldspar (30%e40%), plagioclase (20%e30%), quartz (20%e30%),
biotite (3%e5%), and garnet (1%e3%), with accessory apatite,
zircon, and Fe-Ti and Fe oxides (Fig. 2c, d). Coarse-grained (up to
3.4 mm) K-feldspar is the most dominant mineral in the sample and
occurs as subidioblastic porphyroblast showing perthitic texture.
Quartz (0.3e4.2 mm) and plagioclase (0.6e2.5 mm) are also coarse
grained and scattered in the matrix. Garnet (0.8e1.3 mm) is sub-
idioblastic and contains minor inclusions of quartz. Brownish biotite
(0.3e1.6 mm) occurs along grain boundaries of quartz and feldspars,
and is often aligned along the rock foliation.
The charnockite sample (MD31-3A) is composed of plagioclase
(25%e35%), K-feldspar (25%e35%), quartz (20%e30%), ortho-
pyroxene (3%e5%), biotite (2%e3%), and Fe-Ti oxide (2%e3%)
(Fig. 2e, f). Accessory minerals are apatite and zircon. The
measured grain size of plagioclase (0.5e2.1 mm), quartz
(0.4e4.0 mm), K-feldspar (0.5e2.9 mm), and biotite (0.3e1.2 mm)
are nearly consistent with those in Grt-Bt gneiss, although a coars-
ening of grain size in charnockite as compared to the surrounding
orthopyroxene-free gneiss is reported from many incipient char-
nockite localities (e.g., Santosh et al., 1990). Plagioclase shows
antiperthitic texture with thick (w30 mm) exsolution lamellae of
K-feldspar. Orthopyroxene (0.4e2.2 mm) is subidioblastic to
xenoblastic, and occurs along grain boundaries of quartz and feld-
spars. Biotite occurs in the matrix and is not associated with
orthopyroxene, due to which we regard the mineral as a prograde/
peak phase, although biotite is often regarded as a retrograde
mineral in charnockite. Garnet is rare but its presence was identified
during mineral separation. The opaque mineral is dominantly
ilmenite and no magnetite was found in the rock. We therefore
regard K-feldspar þ quartz þ plagioclase þ biotite þ garnet þ
orthopyroxene þ ilmenite as the stable mineral assemblage during
high-grade metamorphism.
4. Mineral chemistry
Chemical analyses of all minerals were carried out using an electron
microprobe analyzer (JEOL JXA8530F) at the Chemical Analysis
Division of the Research Facility Center for Science and Tech-
nology, the University of Tsukuba. The analyses were performed
under conditions of 15 kV accelerating voltage and 10 nA sample
current, and the data were regressed using an oxide-ZAF correction
program supplied by JEOL. Below we summarize the salient results
from mineral chemistry data from the analyzed rocks. Represen-
tative compositions of minerals are given in Table 1.
4.1. Garnet
Garnet in the Grt-Bt gneiss (sample MD31-3B) is essentially a solid
solution of pyrope and almandine (XMg Z Mg/(Fe þ Mg) Z 0.22). It
shows low grossular (4 mol%e6 mol%) and spessartine (7 mol%e
8 mol%) contents (Table 1). The mineral displays a slight rimward
increase of almandine content and decrease of grossular content such
804 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811

Figure 2 Field and thin-section photographs of charnockite and Grt-Bt gneiss discussed in this study. (a) Dark brownish patches of charnockite
(CH) in Grt-Bt gneiss (GBG) from Rajapalaiyam in the Madurai Block. (b) Enlarged photograph of charnockite patch in Grt-Bt gneiss. Foliation
of the Grt-Bt gneiss is defined by alternation of quartzo-feldspathic and Grt-Bt-rich layers, which disappears in charnockite. (c) and (d)
Photomicrographs of Grt-Bt gneiss (sample MD31-3B). (e) and (f) Photomicrograph of charnockite (sample MD31-3A). (c) and (e) are polarized
light, while (d) and (f) are crossed polars.

as Alm66-67 Prp19-20 Grs5-6 Sps8 (core) to Alm67-69 Prp19-20 Grs4-5
Sps8 (rim), which is a common compositional zoning pattern of
garnet in granulites. Garnet in charnockite (sample MD31-3A) has
higher almandine, grossular, and spessartine contents (Alm70-71
Prp12-13 Grs6-7 Sps10-11) than that of Grt-Bt gneiss.
which the orthopyroxene in sample MD31-3A of present study is
classified as metamorphic in origin. The mineral contains w(MnO)
up to 2.1%.
4.3. Biotite

4.2. Orthopyroxene Matrix biotite in sample MD31-3B (Grt-Bt gneiss) is character-

Orthopyroxene in the charnockite (sample MD31-3A) is Fe-rich
as XMg Z 0.38. Al content in the mineral is low as 0.05e0.06 pfu
(w(Al2O3) Z 1.2%e1.4%), which is a common feature of the
charnockites in southern India (e.g., Rajesh et al., 2011). Rajesh
et al. (2011) distinguished magmatic and metamorphic orthopyr-
oxenes on the basis of XMg and XAl ratios of the mineral, based on
ized by high w(TiO2) content (4.3%e4.7%, Ti Z 0.49e0.53 pfu)
and XMg (0.47e0.48). Biotite included in garnet shows signifi-
cantly higher XMg of 0.64, although its w(TiO2) content is similar
to the matrix phase (4.4%, Ti Z 0.50 pfu). The biotite in
sample MD31-3A (charnockite) is slightly TiO2-poor
(w(TiO2) Z 3.9%e4.0%, Ti Z 0.44e0.46 pfu) and less magne-
sian (XMg Z 0.46).
 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811 805

Table 1 Representative electron microprobe analyses of minerals in charnockite (CH, sample MD31-3A) and Grt-Bt gneiss (GBG, sample
MD31-3B) from Rajapalaiyam.
Lithology CH CH GBG GBG CH GBG CH GBG CH GBG GBG
Mineral name Opx Grt Grt Grt Pl Pl Kfs Kfs Bt Bt Bt
a
O 6 12 12 12 8 8 8 8 22 22 22
Remarks Core Rim Matrix In Grt Matrix
SiO2 49.89 37.29 38.90 38.73 63.13 62.67 64.97 65.58 36.67 37.78 36.76
Al2O3 1.60 20.81 21.24 20.97 22.51 23.15 18.39 18.42 13.91 14.38 14.75
TiO2 0.07 0.02 0.02 0.10 0.01 0.00 0.00 0.00 3.75 4.43 4.57
Cr2O3 0.00 0.13 0.00 0.01 0.02 0.03 0.02 0.00 0.01 0.05 0.00
FeOb 34.90 31.61 30.21 30.34 0.03 0.04 0.04 0.02 20.92 14.42 20.74
MnO 2.07 4.79 3.59 3.66 0.01 0.03 0.03 0.06 0.25 0.03 0.12
MgO 12.12 3.08 4.84 4.73 0.00 0.00 0.00 0.00 10.22 14.26 10.16
CaO 0.26 2.17 2.08 1.72 4.30 4.94 0.17 0.14 0.05 0.00 0.00
Na2O 0.02 0.02 0.03 0.08 9.14 8.75 1.95 2.12 0.10 0.22 0.15
K2O 0.00 0.00 0.02 0.02 0.42 0.16 14.05 13.69 9.52 9.81 9.71
Total 100.93 99.96 100.93 100.35 99.57 99.77 99.62 100.04 95.41 95.37 96.96
Si 1.969 3.004 3.048 3.055 2.808 2.782 2.995 3.003 5.653 5.636 5.563
Al 0.074 1.976 1.961 1.949 1.180 1.211 0.999 0.994 2.527 2.528 2.630
Ti 0.002 0.001 0.001 0.006 0.000 0.000 0.000 0.000 0.434 0.497 0.520
Cr 0.000 0.008 0.000 0.001 0.001 0.001 0.001 0.000 0.002 0.006 0.000
Fe2þ 1.152 2.129 1.979 2.001 0.001 0.001 0.001 0.001 2.695 1.798 2.624
Mn 0.069 0.326 0.238 0.245 0.000 0.001 0.001 0.002 0.032 0.003 0.015
Mg 0.713 0.369 0.564 0.555 0.000 0.000 0.000 0.000 2.346 3.169 2.290
Ca 0.011 0.187 0.174 0.145 0.205 0.235 0.008 0.007 0.009 0.000 0.000
Na 0.002 0.004 0.005 0.012 0.788 0.752 0.174 0.188 0.031 0.063 0.043
K 0.000 0.000 0.002 0.002 0.024 0.009 0.826 0.799 1.872 1.866 1.873
Total 3.992 8.005 7.973 7.971 5.007 4.993 5.005 4.994 15.601 15.565 15.560
Mg/(Fe þ Mg) 0.38 0.15 0.22 0.22 0.47 0.64 0.47
Alm(%) 70.7 67.0 67.9 An(%) 20.1 23.6 0.8 0.7
Prp(%) 12.3 19.1 18.8 Ab(%) 77.5 75.5 17.3 18.9
Grs(%) 6.2 5.9 4.9 Or(%) 2.4 0.9 81.9 80.4
Sps(%) 10.8 8.0 8.3
a
Number of oxygens.
b
Total Fe as FeO.

4.4. Feldspars geothermobarometer to the sample in order to obtain pressure and

Plagioclase occurs as a medium-grained phase in the matrix of
both the charnockite and Grt-Bt gneiss. It shows consistent albite-
rich composition of An19-20 (charnockite) and An21-22 (Grt-Bt
gneiss). K-feldspar in the charnockite (Or81-82) is slightly rich in
potassium than that in Grt-Bt gneiss (Or79-80).
5. Pressure-temperature conditions
5.1. Geothermobarometry
Sample MD31-3A contains dominant orthopyroxene þ plagioclase
þ quartz assemblage. Garnet occurs only rarely, and was identi-
fied through mineral separation, and therefore the textural
relationship of garnet with the other minerals could not be studied
in detail. We consider that garnet could have been in equilibrium
with orthopyroxene þ plagioclase þ quartz because of fast
volume diffusion of Fe, Mg, and Ca in garnet compared
to other minerals and its very low modal abundance. We
therefore attempted to apply conventional Grt-Opx-Pl-Qtz
temperature values, the results from which are summarized below.
5.1.1. Grt-Opx geothermometer
The Grt-Opx geothermometer was applied to garnet-
orthopyroxene pairs in charnockite. The estimated temperature
ranges for the mineral pairs using the methods of Bhattacharya
et al. (1991) are in the order of 710e760  C. The temperature
was calculated at 7 kbar, a reference pressure based on the peak
pressure condition estimated by Grt-Opx-Pl-Qtz geobarometer of
Moecher et al. (1988) (see below). Application of the method of
Lee and Ganguly (1988) also gave consistent but slightly higher
temperatures of 730e820  C.
5.1.2. Grt-Opx-Pl-Qtz geobarometer
Metamorphic pressure was estimated for the assemblage in the
same sample based on the experimental calibration of Perkins
and Newton (1981). The calculated results are 5.0e6.2 kbar at
750  C. Application of the revised geobarometer of Moecher
et al. (1988) yielded a pressure range of 6.7e7.5 kbar, which
is slightly higher than the method of Perkins and Newton
(1981).
806 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811
5.2. Mineral equilibrium modeling
Metamorphic p-T conditions of the stability of mineral assemblages
in the charnockite and Grt-Bt gneiss from Rajapalaiyam were
constrained using THERMOCALC 3.33 (Powell and Holland,
1988; updated October 2009) with an updated version of the inter-
nally consistent data set of Holland and Powell (1998; data set
tcds55s, file created November 2003). The computations using this
software are based on the stable mineral assemblage and phase
compositions from Gibbs Free Energy minimization for a given bulk
composition at specified p-T conditions, and the results are used to
construct rock - specific equilibrium assemblage diagrams
(also called pseudosections). Calculations were undertaken in the
system Na2O-CaO-K2O-FeO-MgO-Al2O3-SiO2-H2O-TiO2-Fe2O3
(NCKFMASHTO) (White et al., 2003, 2007), which provides
a realistic approximation to model the examined rocks. In this study,
Mn-bearing MnNCKFMASHTO system was also adopted for
charnockite as garnet in the rock contains w(MnO) up to 4.8%
(w11 mol% spessartine component), which is likely to have
affected the stability of the mineral assemblage in the rock. The
phases are considered in the modeling and the corresponding a-x
models used are garnet, biotite, and melt (White et al., 2007),
plagioclase and K-feldspar (Holland and Powell, 2003), clinopyr-
oxene (Green et al., 2007), amphibole (Diener et al., 2007),
muscovite (Coggon and Holland, 2002), spinel and magnetite
(White et al., 2002), and ilmenite-hematite (White et al., 2000).
Quartz and H2O are treated as pure end-member phases. For the
analysis, slabs of relatively homogeneous part of the examined
granulites were used for thin-section preparation, and the counter-
part of the same slabs was used for chemical analysis. Bulk
rock compositions for the rocks were determined by X-ray fluo-
rescence spectroscopy at Activation Laboratories, Canada. The
chemical composition of sample MD31-3A (charnockite) is
w(SiO2) Z 70.73%, w(Al2O3) Z 13.92%, w(Fe2O3) Z 0.05%,
w(FeO) Z 3.50%, w(MgO) Z 0.41%, w(MnO) Z 0.049%,
w(CaO) Z 1.75%, w(Na2O) Z 3.83%, w(K2O) Z 4.02%,
w(TiO2) Z 0.30%. Fe2O3 is taken into account for the calculations
because magnetite is present in the Grt-Bt gneiss. The charnockite
sample contains w(P2O5) up to 0.14%, which is reflected in the ca.
0.5 modal percent of apatite. As we neglect P2O5 from the system,
the CaO content equivalent to apatite should be extracted from the
calculation. The corrected w(CaO) content (1.57%) is adopted for
the pseudosection calculation. The Grt-Bt gneiss (sample MD31-
3B) shows similar composition of w(SiO2) Z 70.65%,
w(Al2O3) Z 14.31%, w(Fe2O3) Z 1.13%, w(FeO) Z 2.17%,
w(MgO) Z 0.33%, w(CaO) Z 1.95%, w(Na2O) Z 3.72%,
w(K2O) Z 4.22%, w(TiO2) Z 0.37%. MnO is neglected in the
modeling because the w(MnO) content of this sample is low
(0.028%). The rock is slightly enriched in Fe2O3 as compared to the
charnockite, which is consistent with the occurrence of magnetite in
Grt-Bt gneiss. The corrected w(CaO) content is 1.81% calculated
based on the bulk w(P2O5) content (0.11%).
Sample MD31-3A (charnockite) contains K-feldspar þ
quartz þ plagioclase þ biotite þ orthopyroxene þ garnet
þ ilmenite  inferred melt, representing the probable high-grade
assemblage. Fig. 3a shows a p-T pseudosection for sample MD31-3A
calculated using the compositional factors listed in Fig. 3 and at
molar H2O content in the rock (M(H2O)) of 0.2 mol%. The stability
field of the peak mineral assemblage of the rock plotted in the
pseudosection suggests a wide p-T range of 2e6 kbar at 600  C to
w9 kbar at 800  C (hatched area in Fig. 3a) for the assemblage. The
upper temperature stability limit of the assemblage is defined by the
absence of biotite, whereas the lower limit is set by the absence of
rutile. Orthopyroxene has a wide stability field of w8 kbar at 600  C,
w10 kbar at 800  C, and w12 kbar at 1000  C (Fig. 3a). Even if we
adopted higher M(H2O) values such as 1.0 mol% (Fig. 3b), there is no
significant difference in the stability field of the assemblage except
for the increase of its lower stability limit (>5 kbar at 750  C). We
subsequently constructed T-M(H2O) pseudosection at 7 kbar for
evaluating the approximate water content of the rock (Fig. 4a). The
result suggests that the assemblage is stable at M(H2O) less than
1.0 mol% at ca. 750  C as orthopyroxene disappears at
M(H2O) > 1.0 mol%. We therefore adopted this value as the
maximum H2O content of the rock during the stage of charnockite
formation. We subsequently constructed MnNCKFMASHTO pseu-
dosections of the charnockite at M(H2O) Z 0.2 mol% (Fig. 5a) and
1.0 mol% (Fig. 5b) to evaluate the effect of Mn on the stability. If Mn
is taken into account, the stability field of garnet expands to lower
pressure, and the stability of the mineral assemblage shifts toward
lower p-T in about 50e70  C and 1e1.5 kbar as w760  C and
w7.5 kbar (Fig. 5).
Fig. 3 also shows pseudosections for K-feldspar þ quartz þ
plagioclase þ biotite þ garnet þ ilmenite þ magnetite  inferred
melt assemblage in sample MD31-3B (Grt-Bt gneiss) at
M(H2O) Z 0.2 mol% (Fig. 3c) and 1.0 mol% (Fig. 3d). Mole Fe2O3/
(FeO þ Fe2O3) ratio of 0.190 was considered for the calculation
based on the result of bulk chemical analysis. The stability field of the
mineral assemblage is 10e12.5 kbar at 750  C and w820  C at
10.5 kbar if we adopt M(H2O) Z 0.2 mol% (hatched area in Fig. 3c),
whereas the field shifts toward higher T at 1.0 mol% (850  C at
10 kbar; Fig. 3d). The upper temperature and pressure stability limit
of the assemblage is defined by the disappearance of biotite and
magnetite, respectively. Fig. 4b (T-M(H2O) pseudosection) suggests
that the assemblage is stable at H2O Z 0.3 mol%e0.6 mol% at 7 kbar
and 700e750  C. At higher M(H2O), garnet will disappear, whereas
at lower M(H2O) orthopyroxene should occur as a stable mineral.
6. Discussion
6.1. Petrology and p-T conditions
Incipient charnockite patches in Rajapalaiyam within the Madurai
Block of southern India are characterized by the assemblage K-
feldspar þ quartz þ plagioclase þ biotite þ orthopyroxene þ
garnet þ ilmenite  inferred melt, probably formed during high-
grade metamorphism, whereas the host Grt-Bt gneiss lacks
orthopyroxene. Although charnockite and Grt-Bt gneiss discussed
in this study were collected from the same locality, within
a distance of few centimeters, the absence of foliation in char-
nockite patches suggests that the charnockite was probably formed
later than host Grt-Bt gneiss. Higher Mn content of minerals in
charnockite could also support lower-T origin of the rock. Fig. 6
shows the stability fields of the mineral assemblages in the two
rock types at M(H2O) Z 0.2 mol% and 1.0 mol% in
NCKFMASHTO system. Fig. 6a suggests that, at
M(H2O) Z 0.2 mol%, Grt-Bt gneiss and charnockite assemblages
were formed at 9e12 kbar and <8.5 kbar, respectively, at
700e800  C. Such high-pressure conditions of Grt-Bt gneiss
within the stability field of kyanite are, however, contrasting to the
evidence that sillimanite is the only aluminosilicate mineral
present in the pelitic granulites collected from the adjacent pelitic
 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811 807

Figure 3 p-T diagrams showing calculated pseudosections of mineral assemblages in charnockite (sample MD31-3A) and Grt-Bt gneiss
(sample MD31-3B) from Rajapalaiyam in NCKFMASHTO system. Hatched areas show the peak mineral assemblage. q: quartz, pl: plagioclase,
ksp: K-feldspar, g: garnet, opx: orthopyroxene, di: diopside, bi: biotite, mu: muscovite, cu: cummingtonite, mt: magnetite, ilm: ilmenite, ru: rutile,
liq: inferred melt. (a) p-T pseudosection of charnockite at M(H2O) Z 0.2; (b) p-T pseudosection of charnockite at M(H2O) Z 1.0; (c) p-T
pseudosection of Grt-Bt gneiss at M(H2O) Z 0.2; (d) p-T pseudosection of Grt-Bt gneiss at M(H2O) Z 1.0.
808 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811

Figure 4 T-M(H2O) diagrams showing calculated pseudosections of mineral assemblages in charnockite (sample MD31-3A) and Grt-Bt gneiss
(sample MD31-3B) from Rajapalaiyam in NCKFMASHTO system. Hatched areas show the peak mineral assemblage. (a) T-M(H2O) pseudo-
section of charnockite at p Z 7 kbar; (b) T-M(H2O) pseudosection of Grt-Bt gneiss at p Z 7 kbar.

granulite locality in Rajapalaiyam (e.g., Tsunogae and Santosh, Grt-Bt gneiss (750e850  C and 4e11 kbar in the stability field of
2010). Therefore the water content of M(H2O) Z 0.2 mol% sillimanite) than charnockite (<830  C, <9 kbar), but such lower
might be too low for the Grt-Bt gneiss. The p-T conditions p-T condition from charnockite is consistent with the field and
calculated at M(H2O) Z 1.0 mol% (Fig. 6b) are also higher for petrological data discussed above, as well as the p-T data

Figure 5 p-T diagrams showing calculated pseudosections of mineral assemblages in charnockite (sample MD31-3A) from Rajapalaiyam in
MnNCKFMASHTO system. (a) p-T pseudosection of charnockite at M(H2O) Z 0.2; (b) p-T pseudosection of charnockite at M(H2O) Z 1.0. See
Fig. 3 for abbreviations.
 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811 809

Figure 6 p-T diagrams showing the stability fields of high-grade mineral assemblages in charnockite and Grt-Bt gneiss at M(H2O) Z 0.2 (a)
and M(H2O) Z 1.0 (b). Phase relations of aluminosilicates are based on thermodynamic data of Holland and Powell (1998).

estimated by geothermobarometry of charnockite (710e760  C,
6.7e7.5 kbar). Our results also suggest that the mineral assem-
blage of Grt-Bt gneiss was stable at higher M(H2O) of 1.0 mol%,
whereas that of charnockite could be stable both at 0.2 mol% and
1.0 mol%.
Application of MnNCKFMASHTO system yielded slightly
lower p-T condition of w760  C and w7.5 kbar for charnockite,
but almost equivalent to the results obtained from conventional
geothermobarometry. The results of this study therefore indicate
that MnNCKFMASHTO system is probably more realistic for
application to natural Mn-bearing charnockite than the
NCKFMASHTO system. The metamorphic condition is also
nearly consistent with the p-T ranges estimated from other char-
nockites from southern India (e.g., Chacko et al., 1987; Santosh
et al., 1992), but significantly lower than that of the adjacent
sapphirine granulites that yielded peak UHT conditions of
w1000  C (e.g., Tateishi et al., 2004; Tsunogae and Santosh,
2006, 2010, 2011; Braun et al., 2007). As the UHT locality is
only 200 m apart from the charnockite locality and there is no
obvious tectonic boundary between them, it is inferred that the
charnockitization took place during a retrograde stage possibly
related to post-peak thermal overprint and/or fluid infiltration.
6.2. Origin of incipient charnockite in Rajapalaiyam
Endo et al. (2012) performed phase equilibrium modeling of peak
mineral assemblages in incipient charnockite and adjacent Grt-Bt
gneiss from Mavadi in the Trivandrum Block in NCKFMASHTO
system. They concluded that orthopyroxene-bearing mineral
assemblage in the charnockite is stable at lower M(H2O)
(<0.3 mol%) than that of the host Grt-Bt gneiss (0.3 mol%e
1.5 mol%), which is consistent with the previous studies of

Figure 7 T-XFe3þ (ZFe2O3/(FeO þ Fe2O3) in mole) diagrams showing calculated pseudosections of mineral assemblages in charnockite and
Grt-Bt gneiss from Rajapalaiyam at p Z 7 kbar and M(H2O) Z 0.5 in NCKFMASHTO system. Hatched areas show the peak mineral assemblage.
(a) T-XFe3þ pseudosection of charnockite (sample MD31-3A); (b) T-XFe3þ pseudosection of Grt-Bt gneiss (sample MD31-3B).
810 T. Endo et al. / Geoscience Frontiers 3(6) (2012) 801e811
incipient charnockite formation in the SGT that considered the
infiltration of CO2-rich anhydrous fluids along structural pathways
within upper amphibolite-facies gneisses, resulting in the lowering
of water activity and stabilization of orthopyroxene through
breakdown of biotite (e.g., Janardhan et al., 1979; Newton et al.,
1980; Hansen et al., 1987; Santosh et al., 1990; Newton, 1992;
among others), as well as for the general of anhydrous granulites
in the lower crust in general (e.g., Touret and Huizenga, 2012; and
references therein). However, phase equilibrium modeling in the
present study shows that CO2 infiltration and lowering of water
activity are not essential mechanisms for charnockite formation,
because the mineral assemblages in both charnockite and Grt-Bt
gneiss from Rajapalaiyam are found to be stable at similar
M(H2O) (0.3 mol%e0.6 mol% at 7 kbar, see Fig. 4).
As mentioned previously, the charnockite and Grt-Bt gneiss
have similar bulk compositions except for the high molar Fe2O3/
(FeO þ Fe2O3) ratio of Grt-Bt gneiss (0.190) than that of the
charnockite (0.006). We therefore evaluated the effect of Fe3þ on
the stability of orthopyroxene. Fig. 7 shows T-XFe3þ (ZFe2O3/
(FeO þ Fe2O3) in mole) diagrams for charnockite and Grt-Bt
gneiss at 7 kbar and M(H2O) Z 0.5 mol%, an M(H2O) value of
high-grade metamorphism inferred from Fig. 4. Fig. 7a suggest
that the charnockite assemblage is stable at low (0e0.03) XFe3þ
condition, whereas the Grt-Bt assemblage is stable at higher XFe3þ
(>0.12 at 700e750  C, 7 kbar, and M(H2O) Z 0.5 mol%; Fig. 7),
which implies that charnockitization in Rajapalaiyam might have
been controlled by oxygen fugacity rather than water activity. The
oxidized condition of Grt-Bt gneiss is supported by the occurrence
of magnetite in the rock, whereas magnetite is absent in the
charnockite. Although the process to decrease oxygen fugacity to
form charnockite is not known, infiltration of a reduced fluid (such
as H2O þ CH4 bearing fluid; e.g., Huizenga and Touret, 2012)
could be a possible mechanism to lower the oxidation state.
Infiltration of such reduced fluid during retrograde metamorphism
(ca. 700  C) and buffering of oxygen fugacity to low level, might
have dehydrated biotite and stabilized orthopyroxene, and could
have served as a possible mechanism to form incipient charnockite
in Rajapalaiyam. Detailed microthermometric and Raman spec-
troscopic studies of fluid inclusion in charnockite might be a key
to fully understand the charnockitization process of these rocks.
7. Conclusion
Phase equilibrium modeling of incipient charnockite
(Kfs þ Qtz þ Pl þ Bt þ Opx þ Grt þ Ilm) and adjacent Opx-free
Grt-Bt gneiss (Kfs þ Pl þ Qtz þ Bt þ Grt þ Ilm þ Mt) from
Rajapalaiyam in NCKFMASHTO system demonstrates that the
mineral assemblage in charnockite formed at w820  C and
w9 kbar. Application of MnNCKFMASHTO system on the
charnockite indicates a slight shift of the equilibrium condition of
the assemblage toward lower p and T (w760  C and w7.5 kbar),
which is consistent with the results of geothermobarometry
(710e760  C, 6.7e7.5 kbar), but significantly lower than the peak
temperatures (>1000  C) recorded from the UHT rocks in this
locality, suggesting that charnockitization is a post-peak event.
The results from T-M(H2O) modeling demonstrate that the
assemblages in charnockite and Grt-Bt gneiss are both stable at
M(H2O) Z 0.3 mol%e0.6 mol%, and there is no significant
difference in water activity between the two domains. Our finding
is in contrast to the previous petrogenetic model of incipient
charnockite formation which envisages lowering of water activity
and stabilization of orthopyroxene through breakdown of biotite
by dehydration caused by infiltration of CO2-rich fluid. T-XFe3þ
pseudosections suggest that the oxidation condition of the rocks
probably played a major role on the stability of orthopyroxene;
Opx is stable at XFe3þ <0.03 in charnockite, while Opx-free
assemblage in Grt-Bt gneiss is stabilized at XFe3þ >0.12. Such
low oxygen fugacity conditions of XFe3þ <0.03 in the charnockite
compared to Grt-Bt gneiss might be related to the infiltration of
reduced fluid (e.g., H2O þ CH4) during the retrograde stage.
Acknowledgments
We thank Ms. Preetha Warrier and the staff at Gondwana Research
Office in Trivandrum for their valuable field support. Special
thanks are due to Dr. N. Nishida and Ms. Hisako Shimizu for their
assistance on microprobe and pseudosection analyses. We also
thank Guest Editor Prof. H.M. Rajesh and two reviewers (Prof.
Oleg Safonov and Dr. Shoujie Liu) for constructive and helpful
comments. Partial funding for this project was produced by
a Grant-in-Aid for Scientific Research (B) from Japan Society for
the Promotion of Science (JSPS) to Tsunogae (Nos. 20340148,
22403017).
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