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Gondwana Research 9 (2006) 176 – 188 www.elsevier.com/locate/gr Trace element composition and degree of partial melting of pelitic migmatites from the Aoyama area, Ryoke metamorphic belt, SW Japan: Implications for the source region of tourmaline leucogranites Tetsuo Kawakami a,b,*, Tomoyuki Kobayashi c a Institute of Geology and Geoinformation, National Institute of Advanced Industrial Science and Technology (AIST), Central 7, Tsukuba, Ibaraki 305-8567, Japan b Department of Earth and Marine Sciences, The Australian National University, Canberra, ACT 0200, Australia c Department of Geology and Mineralogy, Graduate School of Science, Kyoto University, Kyoto 606-8502, Japan Received 25 October 2004; accepted 24 June 2005 Available online 9 January 2006 Abstract Degree of partial melting of pelitic migmatites from the Aoyama area, Ryoke metamorphic belt, SW Japan is determined utilizing whole-rock trace element compositions. The key samples used in this study were taken from the migmatite front of this area and have interboudin partitions filled with tourmaline-bearing leucosome. These samples are almost perfectly separated into leucosome (melt) and surrounding matrix (solid). This textural feature enables an estimate of the melting degree by a simple mass-balance calculation, giving the result of 5 – 11 wt.% of partial melting. Similar calculations applied to the migmatite samples, which assume average migmatite compositions to be the residue solid fraction, give degree of melt extraction of 12 – 14 wt.% from the migmatite zone. The similarity of the estimated melting degree of 5 – 11 wt.% with that in other tourmaline – leucogranites, such as Harney Peak leucogranite and Himalayan leucogranites, in spite of differences in formation process implies that the production of tourmaline leucogranites is limited to low degrees of partial melting around 10 wt.%, probably controlled by the breakdown of sink minerals for boron such as muscovite and tourmaline at a relatively early stage of partial melting. Because the amount of boron originally available in the pelitic source rock is limited (on average ¨100 ppm), ¨10 wt.% of melting locally requires almost complete breakdown of boron sink mineral(s) in the source rock, in order to provide sufficient boron into the melt to saturate it in tourmaline. This, in turn, means that boron-depleted metapelite regions are important candidates for the source regions of tourmaline leucogranites. D 2005 International Association for Gondwana Research. Published by Elsevier B.V. All rights reserved. Keywords: Degree of partial melting; Leucogranite; Migmatite; Trace element; REE 1. Introduction Estimation of the degree of partial melting in the pelitic migmatite zones is important for understanding how much melt is produced, segregated and extracted from the region to produce leucogranite bodies. Leucosomes in interboudin partitions and shear bands in migmatitic rocks are often interpreted to represent small volumes of felsic magma squeezed out from the deformed matrix and transferred into low-pressure site due to pressure gradients (e.g., Sawyer, 1991; Brown, 1994; Brown et al., 1995; Oliver and Barr, 1997; * Corresponding author. Institute of Geology and Geoinformation, National Institute of Advanced Industrial Science and Technology (AIST), Central 7, Tsukuba, Ibaraki 305-8567, Japan. E-mail address: [email protected] (T. Kawakami). Milord et al., 2001). This type of melt segregation process separates the melt fraction and solid fraction almost perfectly into leucosome and melanosome, respectively (Milord et al., 2001), and the texture preserving this process is useful in estimating the degree of partial melting by simple mass-balance calculation if the compositions of melt and solid fractions are known (Prinzhofer and Allegre, 1985; Sawyer, 1991). Partial melting in the Ryoke metamorphic belt has been recently described in detail and there is a wide occurrence of migmatites (e.g., Hokada, 1996; Morikiyo, 1998; Brown, 1998; Kawakami, 2001a; Kawakami and Ikeda, 2003). The study of partial melting in the Ryoke metamorphic belt, however, still remains qualitative and the degree of partial melting has not been estimated quantitatively. In this paper, the degree of partial melting of migmatites from the Aoyama area, Ryoke metamorphic belt, SW Japan is estimated utilizing samples 1342-937X/$ - see front matter D 2005 International Association for Gondwana Research. Published by Elsevier B.V. All rights reserved. doi:10.1016/j.gr.2005.06.009 T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 collected from the migmatite front that preserves a texture indicative of almost perfect separation of the melt and solid fractions. The estimated degree of partial melting is then compared with that in other tourmaline leucogranite suites, and the similarity of the degree of melting and its importance are discussed. Mineral abbreviations are after Kretz (1983). 2. General geology of the Ryoke metamorphic belt and the Aoyama area The Ryoke metamorphic belt, SW Japan (Fig. 1a) is a highly elongate high-T/low-P type metamorphic belt of approximately 800 km in length (Miyashiro, 1965; Okudaira et al., 1993; Ikeda, 1998a,b; Brown, 1998; Nakajima et al., 1990; Nakajima, 1994; Suzuki and Adachi, 1998). It is mainly composed of pelitic and psammitic metamorphic rocks and metacherts, and the highest grade zones are considered to have reached granulite facies conditions at metamorphic peak (e.g., Ikeda, 2002). The metamorphic belt grades into the unmetamorphosed Jurassic accretionary Mino – Tanba complex to the north (Wakita, 1987). The low-T/high-P type Sanbagawa belt is located to the south of the Ryoke metamorphic belt and the two belts are separated by a major strike-slip fault, the Median Tectonic Line (MTL). Eastward younging of the K –Ar and Rb – Sr ages of the Ryoke granites and metamorphic rocks has been ascribed to an eastward along-arc shift of granitic activity (Nakajima et al., 1990; Nakajima, 1994). The chemical Th – U – total Pb isochron method (CHIME) dating of monazite from gneisses and granitoids, however, gives ages between 102 177 and 98 Ma both in the east and west of the belt, suggesting more or less simultaneous igneous and metamorphic activity along the whole length of the Ryoke belt followed by denudation that was more rapid in the west than the east (Suzuki and Adachi, 1998). The samples used in this study are from the Aoyama area (Fig. 1), one of the well-studied areas of the Ryoke metamorphic belt, where high-grade metasedimentary rocks are widely distributed (Yoshizawa et al., 1966; Hayama et al., 1982; Takahashi and Nishioka, 1994; Kawakami, 2001a). Subordinate amounts of calcareous metasediments, metachert and metabasite are also distributed. The rock facies of the pelitic-psammitic rocks are schists in the northern half of the area (white part of Fig. 1b), and are anatectic migmatites (metatexites to inhomogeneous diatexites; nomenclature after Brown, 1973) in the southern half of the area (gray part of Fig. 1b). There is a tendency that inhomogeneous diatexites are more common in the southwestern part of the migmatite zone (Kawakami, 2001a). The schistosity of pelitic rocks in the northern part of the area generally strikes E –W to WSW– ENE and dips moderately either N or S, due to later upright folds with fold axes trending E – W to WSW – ENE. The migmatitic banding in central and southern parts strikes NW – SE to WNW – ESE and dips, in most cases, NE to NNE. Intrafolial folds with axial planes parallel to the penetrative migmatitic layering are overprinted by upright folds with fold axes trending NW –SE to WNW – ESE (Takahashi and Nishioka, 1994; Kawakami, 2001a). Massive, post-regional metamorphic granodiorite and two-mica granite both intrude discordantly to Fig. 1. (a) Simplified geological map of southwest Japan showing the location of the Aoyama area. (b) Geological map of the Aoyama area, modified from Yoshizawa et al. (1966), Hayama et al. (1982) and Yoshida et al. (1995). Sample localities and metamorphic isograds are also shown. 178 T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 the foliations of metasediments, and granodiorite is accompanied by the contact aureole (Fig. 1b). The evidences of contact metamorphism in the adjacent country rocks are not found around the two-mica granite. The Aoyama area were previously divided into two regional metamorphic zones and one contact metamorphic zone of postregional metamorphic origin, utilizing mineral assemblages in pelitic lithology (Kawakami, 2001a). The regional metamorphic zones in the order of ascending metamorphic grade are (i) sillimanite – K-feldspar zone, where the muscovite + quartz assemblage is unstable and sillimanite + K-feldspar + biotite is stable, and (ii) garnet – cordierite zone, where garnet + cordierite + biotite T sillimanite is stable. The contact metamorphic zone is recognized by the occurrence of randomly oriented andalusite porphyroblasts partly replaced by sillimanite and is defined adjacent to the granodiorite pluton in the sillimanite – K-feldspar zone (Fig. 1b). The granodiorite pluton is discordant with respect to the schistosity of the regional metamorphic rocks and the pluton contains xenoliths of surrounding regional metamorphic rocks (Yoshida et al., 1995). Therefore, the pluton clearly postdates regional metamorphism (Takahashi and Nishioka, 1994, Kawakami, 2001a). The peak P – T conditions estimated using garnet –biotite geothermometers and GASP geobarometers are 3.0– 4.0 kbar, 615 –670 -C for the sillimanite – K-feldspar zone, and 4.5 – 6.0 kbar, 650 – 800 -C for the Grt –Crd zone (Kawakami, 2001a). However, these estimations are affected by the retrograde re-equilibrium of Fe –Mg exchange in between garnet and biotite, and thus are giving low-temperature estimates. It is also probable that introduction of a spessartine content into garnet stabilized the garnet + cordierite assemblage in the low-temperature part of the garnet – cordierite zone, giving low-temperature estimates for the garnet + cordierite assemblage (Kawakami, 2001b). Taking these points and result of pseudosection studies (e.g., White et al., 2001) into account, Kawakami (2001b) considered that P –T paths of low- and high-temperature parts of the garnet– cordierite zone went through the metamorphic peak of ca. 730 -C, 4.5 kbar and ca. 800 -C, 5.5 kbar, respectively. In the garnet – cordierite zone, sillimanite and biotite are included in cordierite that constitutes the melanosome. In addition, euhedral plagioclase that is indicative of the presence of melts is observed in the leucosome. These textures suggest that a dehydration melting reaction that consumed biotite and sillimanite, such as Bt þ Sil þ Qtz ¼ CrdFKfs þ melt ð1Þ and Bt þ Sil þ Qtz ¼ Grt þ CrdFKfsFIlm þ melt ð2Þ took place in the garnet – cordierite zone. At the lowtemperature part of the garnet – cordierite zone, reaction (1) is likely because garnet is not very common. At the hightemperature part of the garnet – cordierite zone, reaction (2) is likely. These reactions are probably responsible for the formation of migmatites in this area (Kawakami, 2001a,b). Besides the garnet – cordierite isograd, a line marking the disappearance of prograde tourmaline with increasing metamorphic grade may be mapped, and is termed the Ftourmalineout isograd_ (Kawakami, 2001a). Near the isograd, textures involving the breakdown of tourmaline to sillimanite + cordierite, and interboudin partitions filled with tourmaline-bearing leucosome, which is the key sample used in this study, are found. The whole-rock composition of the leucosome is suitable for the frozen melt (Kawakami, 2002). Based on these observations, Kawakami (2001a, 2005) considered that the breakdown of tourmaline occurred at the tourmaline-out isograd during regional metamorphism to form sillimanite + cordierite + boron-bearing melt, and that the melt was transferred into low-pressure interboudin partitions to crystallize retrograde tourmaline. The reaction responsible for the tourmaline-out isograd is considered to be: TurFAbFKfs þ Qtz ¼ Sil þ Crd þ boron-bearing melt: ð3Þ Because these pelitic schists with interboudin partitions filled with leucosome are important in this study, description of them is summarized below. 3. Analytical methods and sample description Twenty-six samples including pelitic schists, metatexites and inhomogeneous diatexites (leucocratic and melanocratic diatexites) are taken from the studied area (Fig. 1b) and major and trace element compositions are determined. Nineteen of the 25 samples were previously analyzed for major elements (by XRF) and boron (by PGNAA), and reported by Kawakami (2001b). A 1 : 10 ratio of powdered rock sample (0.4 g) and anhydrous lithium borate flux (4.0 g) was weighed into a Pt crucible and fused at 1200 -C to prepare a glass bead sample. Utilizing these glass bead samples, whole-rock major element compositions of 6 samples are newly determined by Rigaku Simultix system 3550 X-ray fluorescence spectrometer (see details for Goto and Tatsumi, 1994). Trace element compositions including rare earth elements (REE) are determined by LA-ICPMS analyses at the Research School of Earth Sciences, Australian National University (Eggins, 2003). Glass bead samples prepared for XRF analyses as mentioned above are also used in these analyses. Trace element compositions of 2 samples were measured by Rigaku System 3070 (X-ray fluorescence spectrometer) on pressed powder pellets at the Institute for Geothermal Sciences, Kyoto University, Beppu, Japan (Goto and Tatsumi, 1994; 1996). Samples T14, H9, H20, L5, L10, W28 and 85b are pelitic schists, samples U6, U4, 19, 66, 83M, 98, Y32A and Y26 are metatexites, and samples P2, P3 and Y33 are inhomogeneous diatexites (Fig. 1b; Table 1). Appearance of Y26 and P2 is the most melanocratic in metatexites and inhomogeneous diatexites, respectively. Major constituting minerals of these samples are given in Kawakami (2001b). Pelitic schists are considered to be low-grade equivalents of migmatites. Besides these samples, pelitic schists with interboudin partitions filled with leucosome (Fig. 2a) are commonly Table 1 Major and trace element concentrations of pelitic schists and migmatites from the Aoyama area Rock type Pelitic schists Sample no. T14 H20 L5 L10 W28 85b Leucosomes in interboudin partitions SAIT1 SAI991B SAIT2 SAIT3 SAIT1B SAIT2B SAIT3B 59.87 0.89 18.20 5.39 0.04 2.56 1.64 2.25 7.90 0.17 98.93 3 1263.5 36.2 171.4 177.7 15.8 n.a. 256.6 19.2 25.1 n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. – 54.24 1.21 18.59 9.81 0.14 2.04 1.84 2.81 8.29 0.45 99.42 31 558.2 17.1 599.1 174.8 65.2 n.a. 154.5 9.3 42.6 n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. n.a. – 68.55 0.85 15.33 7.03 0.11 2.65 0.28 0.61 4.33 0.10 99.85 79 656.2 18.0 213.5 84.6 16.0 45.7 157.0 17.1 25.1 2.0 1.5 40.6 83.1 33.2 6.2 0.8 8.8 5.3 4.8 0.9 1.1 2.7 0.4 2.7 0.4 10.2 64.49 0.80 18.33 5.82 0.08 2.17 1.47 2.41 4.09 0.21 99.87 77 816.6 22.0 243.8 255.8 13.7 22.7 128.7 15.3 29.4 3.1 1.5 38.7 77.9 35.1 6.7 0.9 8.9 6.0 5.4 1.1 1.2 3.1 0.5 3.2 0.5 8.1 66.25 0.74 17.73 5.45 0.11 1.84 1.51 2.55 3.55 0.14 99.87 19 641.6 21.5 263.0 151.1 12.9 21.3 108.1 14.9 31.3 2.8 1.3 34.1 73.5 31.6 6.1 0.9 8.1 5.7 5.8 1.2 1.1 3.5 0.6 3.5 0.5 6.6 68.49 0.66 15.76 5.45 0.14 2.08 1.70 1.96 3.53 0.18 99.97 64 725.4 16.8 184.2 155.5 10.7 32.4 114.1 13.3 25.6 3.0 1.2 32.8 71.3 29.3 5.5 0.8 7.6 5.2 4.9 1.0 1.3 2.7 0.4 2.6 0.4 8.6 65.04 0.76 17.75 5.72 0.13 2.02 2.06 2.83 3.52 0.18 100.01 2 651.0 21.5 260.0 204.7 13.0 34.2 113.0 12.9 32.6 3.2 1.5 34.1 69.8 31.7 6.3 0.9 8.0 6.3 5.8 1.2 1.4 3.5 0.5 3.3 0.6 7.0 64.28 0.74 19.05 5.59 0.11 1.82 1.90 3.03 3.36 0.16 100.06 n.a. 442.2 18.1 254.5 160.4 12.8 34.7 111.6 12.4 28.8 2.8 1.8 30.7 67.1 28.1 6.0 0.9 7.4 5.7 5.7 1.1 1.1 3.3 0.5 3.5 0.5 6.0 64.41 0.75 18.58 5.79 0.14 1.94 0.99 1.91 5.10 0.14 99.74 n.a. 959.6 26.0 301.8 130.8 13.9 26.4 137.0 17.7 35.1 3.9 1.6 36.5 80.6 33.6 6.7 1.0 8.7 6.2 6.4 1.4 1.0 4.0 0.6 4.3 0.7 5.8 66.12 0.67 18.00 4.98 0.09 1.62 1.72 2.77 4.05 0.12 100.14 n.a. 786.8 22.9 241.5 173.6 9.6 37.5 102.7 11.4 25.1 2.4 1.1 25.2 55.8 24.2 4.9 0.7 6.2 4.7 4.5 0.9 1.0 3.0 0.4 3.0 0.5 5.7 74.98 0.14 14.72 0.93 0.02 0.42 0.66 1.57 5.75 0.24 99.43 745 720.9 37.1 43.4 147.3 3.6 14.6 98.7 3.0 12.0 2.2 1.3 8.1 17.9 7.0 1.6 0.3 1.9 1.9 2.2 0.4 0.7 1.4 0.2 1.6 0.2 3.4 73.96 0.08 15.12 0.47 0.01 0.18 0.64 1.77 7.12 0.21 99.56 283 1080.2 54.6 15.2 154.1 2.7 15.8 139.4 1.3 9.4 6.4 1.5 3.7 8.9 4.0 1.1 0.2 0.9 1.1 1.8 0.4 0.9 1.0 0.2 1.2 0.2 2.1 75.10 0.09 14.29 0.56 0.01 0.25 0.51 1.58 6.89 0.18 99.46 273 1288.4 64.5 28.6 154.8 2.2 17.1 128.9 2.3 10.3 2.0 0.6 5.5 13.1 4.9 1.0 0.2 1.3 1.3 1.7 0.4 1.0 1.1 0.2 1.2 0.2 3.0 72.54 0.16 14.94 1.34 0.03 0.50 0.63 1.35 7.38 0.16 99.03 n.a. 1317.8 50.5 41.6 173.7 4.2 19.1 131.8 2.6 11.1 5.4 2.0 7.0 15.7 6.5 1.6 0.3 1.7 1.6 1.8 0.4 1.0 1.2 0.2 1.6 0.2 2.9 – XRF, Kyoto U. – XRF, Kyoto U. 0.56 LA-ICPMS, ANU 0.57 LA-ICPMS, ANU 0.56 LA-ICPMS, ANU 0.75 LA-ICPMS, ANU 0.66 LA-ICPMS, ANU 0.56 LA-ICPMS, ANU 0.49 LA-ICPMS, ANU 0.61 LA-ICPMS, ANU 1.24 LA-ICPMS, ANU 2.31 LA-ICPMS, ANU 2.47 LA-ICPMS, ANU 1.90 LA-ICPMS, ANU T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5 Total B Ba Pb Zr Sr Nb Ni Rb Th Y U Ta La Ce Nd Sm Tb Pr Gd Dy Ho Eu Er Tm Yb Lu La(N) / Yb(N) Eu / Eu* Trace element analyses H9 Intervening matrix parts of pelitic schists with interboudin partitions filled with leucosome Major element and boron concentrations are from Kawakami (2001b) and this study. wt.% for major elements and ppm for trace elements (B – Lu). Total Fe as Fe2O3. n.a. = not analyzed, < 2 = below 2 ppm. All of the trace element data except for T14, H9, and boron data are the average of three analyses. 179 180 Table 1 (continued) Metatexites Inhomogeneous diatexites Sample no. U6 U4 19 66 83M 98 Y32A Y26 P2 P3 Y33 SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5 Total B Ba Pb Zr Sr Nb Ni Rb Th Y U Ta La Ce Nd Sm Tb Pr Gd Dy Ho Eu Er Tm Yb Lu La(N) / Yb(N) Eu / Eu* Trace element analyses 69.03 0.65 15.83 4.49 0.05 1.73 2.23 3.68 2.31 0.20 100.20 10 193.4 18.0 223.0 265.7 10.6 21.1 94.0 13.1 24.1 2.8 1.4 31.1 64.2 27.5 5.4 0.7 7.0 4.6 4.5 0.9 1.2 2.8 0.4 2.7 0.4 7.7 0.69 LA-ICPMS, ANU 69.26 0.59 16.09 5.23 0.22 1.59 1.41 3.13 2.50 0.10 100.11 <2 246.8 16.9 233.1 147.2 20.6 28.5 139.3 14.5 27.0 3.6 3.0 31.1 71.1 27.4 5.7 0.7 7.1 4.9 4.8 1.0 0.8 3.3 0.5 3.6 0.6 5.8 0.43 LA-ICPMS, ANU 65.18 0.89 16.40 6.44 0.08 2.33 1.92 3.29 3.13 0.18 99.83 <2 276.8 14.6 364.8 172.2 16.2 31.1 174.1 22.5 33.1 2.7 1.2 50.8 99.5 43.0 7.9 1.0 11.3 7.0 6.2 1.3 1.0 3.5 0.5 3.2 0.5 10.7 0.41 LA-ICPMS, ANU 66.04 0.72 17.34 5.22 0.11 2.02 1.77 2.65 4.02 0.17 100.06 2 772.3 23.3 221.6 224.7 14.5 20.7 132.7 15.8 22.7 2.1 1.7 34.8 71.3 30.6 5.7 0.7 7.6 5.0 4.3 0.8 1.2 2.5 0.4 2.8 0.5 8.5 0.67 LA-ICPMS, ANU 61.73 0.88 17.99 7.09 0.19 2.39 2.19 4.06 3.09 0.12 99.75 <2 180.2 17.6 281.8 159.5 15.9 45.5 170.2 16.3 29.2 3.2 1.4 39.4 86.0 34.8 7.2 0.9 9.0 6.0 5.5 1.1 0.9 3.2 0.5 3.7 0.5 7.3 0.41 LA-ICPMS, ANU 66.94 0.58 16.56 5.04 0.19 1.84 2.53 4.33 2.03 0.11 100.15 <2 279.6 17.3 225.9 160.1 9.4 36.3 103.8 12.5 30.0 2.7 1.1 31.3 69.3 29.6 6.1 0.9 7.2 5.6 5.6 1.2 1.3 3.4 0.6 3.8 0.6 5.5 0.67 LA-ICPMS, ANU 63.81 0.96 17.79 7.24 0.09 2.43 1.53 2.54 3.63 0.10 100.12 4 457.4 18.8 289.4 209.5 15.6 36.4 128.8 20.4 29.0 2.0 1.3 47.6 94.9 40.8 7.0 0.9 10.4 6.1 5.8 1.1 1.2 3.3 0.5 3.5 0.5 9.3 0.56 LA-ICPMS, ANU 60.80 1.19 19.26 8.32 0.09 3.22 0.94 1.54 4.19 0.08 99.64 <2 525.5 15.1 333.1 131.8 23.8 56.9 169.5 19.0 31.6 2.1 2.1 43.2 85.4 37.0 6.9 0.9 9.5 5.9 5.6 1.2 0.8 4.0 0.6 4.7 0.7 6.3 0.37 LA-ICPMS, ANU 63.34 1.01 17.15 6.76 0.07 2.35 2.49 3.66 2.70 0.11 99.65 <2 203.2 18.6 279.7 228.2 25.2 33.1 124.9 19.0 16.4 2.6 2.3 41.5 81.6 33.8 5.8 0.6 8.9 4.8 3.5 0.7 1.1 1.6 0.2 1.5 0.2 18.9 0.62 LA-ICPMS, ANU 69.13 0.55 15.96 3.50 0.05 1.12 1.36 2.87 5.30 0.30 100.14 3 883.3 41.8 227.2 197.7 14.8 23.8 155.0 17.2 79.4 4.1 2.0 36.3 77.3 34.1 8.0 1.8 8.5 9.7 13.6 2.8 1.0 8.6 1.1 7.3 1.0 3.4 0.35 LA-ICPMS, ANU 70.14 0.59 16.43 3.99 0.04 1.62 1.47 2.44 3.23 0.10 100.04 5 787.4 18.0 205.7 220.5 13.7 16.9 92.4 13.9 15.5 2.3 1.6 33.1 67.7 27.6 5.5 0.7 7.5 5.0 3.7 0.6 1.1 1.4 0.2 1.2 0.1 19.2 0.65 LA-ICPMS, ANU T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 Rock type T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 181 Fig. 2. (a) A picture of pelitic schist with an interboudin partition filled with leucosome. Black crystals in the midst of the leucosome are tourmaline. (b) CIPW normative Qtz – Ab – Or plot of whole-rock compositions of the leucosomes in interboudin partitions (white circles). Gray shaded area represents the glass compositions obtained by melting two-mica, plagioclase-poor pelites at 800 and 850 -C, 3 kbar (Spicer et al., 2004). Liquidus phase relations in the system Qtz – Ab – Or – H2O at 5 kbar and X(H2O) = 1.0 are taken from Holtz et al. (1992). observed near the tourmaline-out isograd that is defined near the schist/migmatite boundary of the Aoyama area (Fig. 1b; see also Kawakami, 2002). The leucosome is composed of quartz, K-feldspar, plagioclase, tourmaline, biotite, muscovite, T andalusite and apatite. Plagioclase, apatite, andalusite and tourmaline are euhedral. The whole-rock composition of leucosomes is consistent with the leucosome being a frozen melt (Kawakami, 2002). Fig. 2b shows the CIPW normative plot of the compositions of leucosome in interboudin partitions. It is clear from this figure that the leucosomes have similar compositions to melts produced by the melting of pelitic schists of low Na2O / K2O ratio (0.21 – 0.41 in wt.% ratio) at 3 kbar, 800 –850 -C (Spicer et al., 2004). This point will be further discussed below. Tourmaline showing a partial breakdown texture was found in the intervening matrix, which lead Kawakami (2001a) to conclude that the boron in the leucosome was derived from the breakdown of tourmaline in the surrounding country rocks (i.e., closed-system behavior of boron and melt on the sample scale). The interboudin partitions found near the tourmalineout isograd are often connected with each other in the Aoyama area (Kawakami, 2005). However, it is important that all of the leucosome samples used in this study have three-dimensionally closed shapes and not connected to veins or shear zones. Those leucosomes do not contain mafic aggregates and are pure leucosomes. From these lines of evidence, the leucosome was interpreted to be a frozen melt collected from the surroundings (Kawakami, 2001a, 2002) and thus the SAIseries samples are the typical example of partially molten pelites that are almost perfectly separated into the melt fraction (leucosome part; samples SAIT1, SAIT2 and SAIT3) and into the residual solid fraction (intervening matrix parts; SAI991B, SAIT1B, SAIT2B and SAIT3B). Samples SAITn and SAITnB (n = 1, 2 and 3) are separated from the same sample (i.e., SAIT1B is the leucosome in interboudin partitions and SAIT1 is the intervening matrix part of the same sample) and utilized in XRF and LA-ICPMS analyses explained above. Samples L5, L10 and 85b are the pelitic schists collected close to the tourmaline-out isograd, but boudinage structures are not developed. 4. Whole-rock trace element compositions Whole-rock major and trace element compositions of analyzed samples are summarized in Table 1. All of the trace element data listed in Table 1 are the average of three analyses, except for T14, H9, and boron data of all samples. Fig. 3 is the multi-element variation diagrams normalized to primordial mantle of Taylor and McLennan (1985). It is clear from this plot that pelitic schists and migmatites have almost the same trace element composition except for Ba. Leucosomes are enriched in Ba, K and Ta, and depleted in Th, Nb, La, Ce, Nd, Zr, Sm, Ti, Tb and Y than pelitic schists and metatexites. Compositional difference between pelitic schists and the intervening matrix parts of boudinaged rocks (samples SAIT1, SAIT2 and SAIT3) is not observed in this diagram. Inhomogeneous diatexites are different from metatexites in the abundance of Tb and Y. Fig. 4 is the multi-element variation diagrams of pelitic schist compositions normalized to the average trace element abundances of Faverage pelitic schist_, which is the average of samples H20, L5, L10, W28 and 85B (Table 2). Apparently, samples H9 and T14 have extraordinary high concentrations of LIL or HFS elements, such as K, Zr, Ti and Nb for sample H9, and K, Rb and Ba for sample T14, indicative of the effect of Kmetasomatism and/or originally untypical whole-rock chemistry. These samples have very low SiO2 contents compared with other pelitic schist samples. However, these cannot be restites because they are taken from Fschist zone_ where pelitic and psammitic schists dominate and significant partial melting is not observed (Fig. 1). Because samples H9 and T14 are not Ftypical_ pelitic schists and are not appropriate for the aim of 182 T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 matrix part of boudinaged samples, metatexites, and inhomogeneous diatexites. Pelitic schists show negative Eu anomaly (Eu / Eu* = 0.56 – 0.75) with flat HREE pattern, where Eu / Eu* = EuN / (SmN / 2 + GdN / 2). Leucosomes filling the interboudin partitions are depleted in REE relative to pelitic schists and metatexites, and show positive Eu anomaly (Eu / Eu* = 1.24 – 2.47) with flat HREE pattern. Metatexites have almost the same REE patterns with pelitic schists except for the stronger negative Eu anomaly (Eu / Eu* = 0.37– 0.69) than the pelitic schists. Inhomogeneous diatexites show variations in terms of HREE abundance, and no significant difference between metatexites and inhomogeneous diatexites is found in terms of LREE abundances. High concentrations of HREE in sample P3 may be not explained by the high modal abundance of garnet and apatite in P3, because garnet is absent and apatite is very rare in this sample. High modal amount of zircon is excluded because Zr content is not prominently high in P3, relative to other inhomogeneous diatexites. The fact that P3 is also enriched in P (Table 1) and Y (Fig. 3) rather suggests that REE pattern of P3 is strongly reflecting the high modal abundance of xenotime (e.g. Bea, 1996). Intervening matrix parts of boudinaged samples have almost the same pattern as pelitic schists, and the difference between them may be best recognized in the REE-diagram normalized to Faverage pelitic schist_ (Fig. 7). There is a tendency that intervening matrix parts are a little richer in HREE and slightly depleted in LREE, especially Eu, relative to pelitic schists. This may reflect the restitic nature of the intervening matrix parts. Weak negative Eu anomaly observed in the intervening matrix samples may reflect the effect of disequilibrium melting; REE that are mainly contained in accessory minerals went through disequilibrium melting, whereas Eu that is mainly contained in major mineral as feldspars went through equilibrium Fig. 3. Trace element compositions of (a) pelitic schists and intervening matrix parts of boudinaged sample, (b) metatexites and leucosomes in interboudin partitions, and (c) inhomogeneous diatexites from the Aoyama area, normalized to primordial mantle of Taylor and McLennan (1985). this study to estimate the degree of partial melting, they are not used in this study. Excluding these two, the compositional data of pelitic schists show good concentration (Fig. 4). Compositional difference between pelitic schists and other rock types mentioned above may be better recognized by the multielement variation diagrams normalized to Faverage pelitic schist_ (Fig. 5). The trend that metatexites are depleted significantly in Ba and slightly in K than the average pelitic schist is clearly observed in this plot. Fig. 6 is the chondrite-normalized REE-diagram for pelitic schists, leucosomes in interboudin partitions, intervening Fig. 4. Trace element compositions of the pelitic schists from the Aoyama area, normalized to Faverage pelitic schist_. See Table 2 for compositional data of Faverage pelitic schist_. T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 Table 2 Average composition of pelitic schists, leucosomes in interboudin partitions, intervening matrix of boudinaged samples, and metatexites used in calculations Rock type (number of averaged samples) Pelitic schist (n = 5) Intervening matrix (n = 3) Leucosome (n = 4) Metatexite (n = 8) SiO2 TiO2 Al2O3 Fe2O3 MnO MgO CaO Na2O K2O P2O5 Total B Ba Pb Zr Sr Nb Ni Rb Th Y U Ta La Ce Nd Sm Tb Pr Gd Dy Ho Eu Er Tm Yb Lu La(N) / Yb(N) Eu / Eu* 66.6 0.8 17.0 5.9 0.1 2.2 1.4 2.1 3.8 0.2 99.9 48.2 698.2 20.0 232.9 170.3 13.2 31.3 124.2 14.7 28.8 2.8 1.4 36.0 75.1 32.2 6.2 0.8 8.3 5.7 5.3 1.1 1.2 3.1 0.5 3.1 0.5 8.1 0.62 64.94 0.7 18.5 5.5 0.1 1.8 1.5 2.6 4.2 0.1 100.0 n.a. 729.5 22.4 265.9 154.9 12.1 32.9 117.1 13.8 29.6 3.0 1.5 30.8 67.8 28.6 5.9 0.9 7.4 5.6 5.5 1.1 1.0 3.4 0.5 3.6 0.6 5.8 0.55 74.1 0.1 14.8 0.8 0.0 0.3 0.6 1.6 6.8 0.2 99.4 433.7 1101.8 51.7 32.2 157.5 3.2 16.6 124.7 2.3 10.7 4.0 1.3 6.1 13.9 5.6 1.3 0.3 1.5 1.5 1.9 0.4 0.9 1.2 0.2 1.4 0.2 2.8 1.98 65.3 0.8 17.2 6.1 0.1 2.2 1.8 3.2 3.1 0.1 100.0 2.6 366.5 17.7 271.6 183.8 15.8 34.6 139.0 16.8 28.3 2.6 1.6 38.7 80.2 33.9 6.5 0.8 8.7 5.6 5.3 1.1 1.0 3.3 0.5 3.5 0.5 7.6 0.53 Major element and boron concentrations are from Kawakami (2001b) and this study. wt.% for major elements and ppm for trace elements (B – Lu). Total Fe as Fe2O3. n.a. = not analyzed. melting (that is, Eu may be more rapidly taken into melt than other REE). 5. Discussion 5.1. Leucosomes in interboudin partitions — are they frozen melts? The leucosomes in interboudin partitions now consist of granitic mineral assemblages including euhedral plagioclase. Generally, plagioclase is only rarely euhedral in metamorphic rocks (Spry, 1969), and the euhedral shape implies its growth in free space, melt or fluid. Three-dimensionally closed shape 183 of leucosomes is the supporting evidence that melt or fluid segregated from intervening matrix and that melt or fluid did not contain significant amount of crystals including those formed simultaneously with the melt or fluid, when they were segregated into the interboudin partitions. The normative Qtz –Ab – Or plots of the leucosomes are in good agreement with experimental melt compositions (Fig. 2), showing that the leucosomes can be interpreted to be frozen melts. Although the experiments cited in Fig. 2 were performed at lower pressures (3 kbar) than the estimated pressure of the Aoyama area (¨5 kbar), this difference may not affect the conclusion that the leucosomes possess the composition of frozen melts, because leucosome compositions (SAI series) are plotted near the quartz– orthoclase cotectic line at 5 kbar and because location of the quartz – orthoclase cotectic line in the Qtz –Ab – Or system does not differ very much between 3 to 5 kbar (e.g. Holtz et al., 1992). The only major difference caused by the pressure difference will be the temperature that is needed to produce the same melt composition, and at 5 kbar, the leucosome (melt) compositions of the Aoyama samples may be produced at 700– 740 -C under X(H2O) = 1.0 and at about 820 -C under X(H2O) = 0.7 (Holtz et al., 1992). This is concordant with the temperature estimates of the Aoyama area. The aluminum saturation index [ASI = Al 2O3 / (CaO + Na2O + K2O)] (Zen, 1986) of the leucosomes range from 1.28 to 1.47. Based on Acosta-Vigil et al. (2003), hydrous granitic melts with ASI = 1.28 – 1.47 coexist with tourmaline at about 730– 810 -C at 2 kbar. The normative corundum of the SAIseries leucosomes range from 3.59 to 5.29. Such melts coexist with tourmaline at above 780 -C at 2 kbar. These temperatures are almost concordant with the estimated temperature of the migmatite front (730 -C). Bea (1996) reported that Eu is always essentially contained within feldspars, and epidote may also contain a significant proportion. However, epidote is not contained in the pelitic rocks from the Aoyama area and thus Eu will be mostly contained in feldspars. Therefore, behavior of Eu will be not affected by the disequilibrium melting process related to accessory minerals, and solely controlled by the melting reactions containing feldspars. Positive Eu anomaly of leucosomes and negative Eu anomaly of intervening matrix parts relative to pelitic schists (Fig. 7) suggest that feldspars were consumed in the course of partial melting to produce leucosome melts, and feldspar components are taken into melt. This is the supporting evidence for the model proposed by Kawakami (2001a) that the melt was produced in the intervening matrix parts of boudinaged pelitic samples and segregated into interboudin partitions. From these lines of evidence, leucosomes that are filling the interboudin partitions of boudinaged pelitic schists (SAI-series samples) are interpreted to be nearly frozen melts. The zirconium contents of the leucosomes in interboudin partitions are below the concentration that is required to saturate the peraluminous melt of SiO2 = 73 wt.% in zircon (Watson, 1988), and the calculated Zr / Zr* ratio are 0.16– 0.45. The leucosomes may be classified into a Fdisequilibrium melt_ of Sawyer (1991). 184 T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 Fig. 5. Trace element compositions of (a) leucosomes and metatexites, and (b) inhomogeneous diatexites from the Aoyama area, normalized to Faverage pelitic schist_. 5.2. Estimating degree of partial melting by mass-balance calculation Kawakami (2005) estimated the degree of partial melting of the pelitic rock sample with interboudin partitions filled with leucosome to be 12 wt.%, using average boron contents of the leucosomes in interboudin partitions, the intervening matrix parts, and of the average pelitic schist compositions. He assumed the closed-system behavior of boron and melts within the sample scale. His conclusion can be evaluated utilizing other trace elements, and the new estimates are given below. Under the assumption that SAI-series samples are almost perfectly separated into melt and solid fractions, mass balance can be expressed as C0 ¼ C1 ð1 F Þ þ C2 F where C 0 (ppm) is the whole-rock trace element of the pelitic schists before partial melting, C 1 residues, C 2 is that of the leucosomes, and F is partial melting in wt.% basis (e.g. Prinzhofer ð4Þ concentration is that of the the degree of and Allegre, T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 185 Fig. 6. Chondrite-normalized REE plots of (a) pelitic schists, (b) leucosomes and intervening matrix parts of boudinaged samples, (c) metatexites and (d) inhomogeneous diatexites from the Aoyama area. Chondrite values are taken from Taylor and McLennan (1985). Fig. 7. REE plot of leucosomes and intervening matrix parts of boudinaged samples normalized to Faverage pelitic schist_. 1985). In this study, composition of samples SAITn is used for C 1, and the composition of SAITnB is used for C 2. Using these values, C 0 is calculated for given F (= calculated C 0) and compared with observed C 0 values (= Faverage pelitic schist_ of Table 2). In order to determine which value of F gives the bestfit composition to Faverage pelitic schist_ (= observed C 0), the least square method was used. In this calculation, all the major and trace element compositions available are used and dealt equally. As a result, SAIT1 – SAIT1B and SAIT2 – SAIT2B pairs gave F values of 5 and 11 wt.% (Table 3). A SAIT3 – SAITB3 pair gave F = 0 wt.% to be the best-fit result. This may be due to the inappropriate assumption of protolith composition for a SAIT3 –SAITB3 pair. The degree of partial melting at the migmatite front of the Aoyama area may be estimated to be 5– 11 wt.%. Alternative way of estimating the degree of partial melting is to separate the pure restitic part and analyze its composition to utilize in this calculation. However, it is difficult to do so in the case of Aoyama area because melanosome patches contained in the boudinaged samples are small and irregularly 186 T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 Table 3 Summary of F values calculated by Eq. (4) Protolith (C 0) Average Average Average Average Average Average Average pelitic pelitic pelitic pelitic pelitic pelitic pelitic schist schist schist schist schist schist schist Residue (C 1) Leucosome (C 2) SAIT1 SAIT2 SAIT3 Average Average Average Average SAITB1 SAITB2 SAITB3 SAITB1 SAITB2 SAITB3 Average leucosome migmatite migmatite migmatite migmatite shaped (see Fig. 3b of Kawakami, 2001a). Even if the pure restite parts are successfully separated, one has to be careful because the F value obtained from the mass-balance calculation may represent the degree of partial melting in the specific rock part where partial melting reactions selectively took place (this is why melanosome patches are produced). In order to obtain Fbulk_ degree of partial melting, modal information of restitic part should be taken into account, which will result in lowering the degree of partial melting estimated by this method. Metatexite migmatites are presumably a mixture of residual solid and leucosome, where the leucosome may represent some mixture of residual felsic minerals, early crystallized felsic minerals (cumulates) (Brown, 2001), and possibly unextracted felsic melts. Because SAI-series leucosomes may represent melt compositions that were produced almost in situ at the migmatite front, it is interesting to consider the degree of melt extraction from the metatexite migmatites under some assumptions. The assumptions made here are (i) protolith composition of metatexites are Faverage pelitic schist_, and (ii) melt composition that extracted from metatexites is equivalent to average leucosome compositions of SAI series (Table 2). Following calculation is based on Eq. (4), and composition of average metatexite (Table 2) is used for C 1, and the composition of SAITnB (n = 1, 2 and 3) is used for C 2. In this calculation, F does not represent the degree of partial melting in metatexites but represents the degree of melt extraction (in wt.%) from the metatexites. Then, C 0 is calculated for a given F and compared with observed C 0 values (= Faverage pelitic schist_ of Table 2). In order to determine which value of F gives the best-fit composition to Faverage pelitic schist_, the least square method was used. All the major and trace element compositions available are used and dealt equally. As a result, F values of 12 –14 wt.% are obtained (Table 3). If average leucosome composition (Table 2) is used for C 2 instead of SAITnB, then the F value is 13 wt.%. As some melt probably remained unextracted in metatexites, it may be concluded that the degree of partial melting in most part of the migmatite zone exceeded the degree of melt extraction of 12 –14 wt.%. 5.3. Implications for the source region of tourmaline leucogranites Because pelitic migmatite zones are potential sources for leucogranites, and because the presence of tourmaline-bearing Calculated F (wt.%) 5 11 0 12 13 14 13 leucosome in the migmatite front of the Aoyama area shows that tourmaline – leucogranite was produced there, it is interesting to compare the degree of partial melting of the Aoyama area with that estimated in the tourmaline leucogranite suites. The Harney Peak leucogranite (Nabelek et al., 1992; Wilke et al., 2002) and Himalayan leucogranites (Harris and Inger, 1992) are well-studied examples of tourmaline leucogranites and are considered to have been produced via muscovite dehydration melting reaction. The degrees of partial melting to produce the leucogranites from muscovite schists are estimated to be 10– 14 wt.% for the Harney Peak leucogranite (Nabelek et al., 1992; Wilke et al., 2002), and about 12 wt.% for the Himalayan leucogranites (Harris and Inger, 1992). The result of this study shows that more than 5– 11 wt.% of partial melting in the migmatite front of the Aoyama area, which is quite similar to the values estimated in other leucogranite suites, produced the tourmaline leucogranite although it did not segregate into a pluton scale. The source of boron to produce boron-bearing melt in the Aoyama area is considered to be the breakdown of tourmaline, and other melting reactions involving biotite, such as reactions (1) and (2), are also responsible for the production of melts at that metamorphic grade (Kawakami, 2001a). In the migmatite zone where higher degrees of partial melting are inferred from the calculation given above, no tourmaline-bearing leucogranite is found. This is probably because boron content in the leucosome melt was not high enough to crystallize tourmaline (e.g., Wolf and London, 1997) or high Ti content preferred crystallization of biotite instead of tourmaline (e.g., Nabelek and Bartlett, 1998). Anyway, the mechanism of producing tourmaline leucogranite, including the reaction to produce it, and P – T conditions of its production are different from those considered for the Harney Peak leucogranite and Himalayan leucogranites. The similarity of the degree of partial melting, in spite of these differences, implies that production of the tourmaline leucogranite is limited to low degrees of partial melting (¨10 wt.%) regardless of P – T conditions and reaction by which it is produced. This low degree of melting of ¨10 wt.% is probably controlled by the breakdown of sink minerals of boron such as muscovite and tourmaline at a relatively early stage of the partial melting of the pelitic source rocks. Low-temperature breakdown of tourmaline may require the coexistence with quartz (i.e., breakdown of tourmaline + quartz; von Goerne et al., 1999) and appropriate tourmaline composition, possibly tourmaline with substantial amount of X-site vacancy and schorl component (e.g., T. Kawakami, T. Kobayashi / Gondwana Research 9 (2006) 176 – 188 Schreyer and Werding, 1997; Kawakami, 2001b; Kawakami and Ikeda, 2003). Because of the limited amount of boron originally available in the pelitic source rocks (on average ¨100 ppm; Harder, 1970), ¨10 wt.% of melting requires almost complete breakdown of sink mineral(s) of boron in the source rock in some cases (e.g., Kawakami, 2001a, b; Kawakami and Ikeda, 2003; Wilke et al., 2002), in order to provide sufficient amounts of boron into the melt to saturate in tourmaline, although the concentration of boron required for the tourmaline saturation in leucogranite melts is still controversial (e.g., Benard et al., 1985; Holtz and Johannes, 1991; Scaillet et al., 1995; Spicer et al., 2004; Wolf and London, 1997). This, in turn, means that boron-depleted metapelite regions, except for the boron-depleted contact aureoles around some plutons (e.g., Wilke et al., 2002), are important candidates for source regions of tourmaline leucogranites. Acknowledgements We are grateful to C. Allen and D. Rubatto for the LAICPMS analyses at RSES, ANU, and T. Shibata, K. Sato, Y. Tatsumi and T. Hoshide for the XRF analyses at Kyoto University. We would like to thank T. Ikeda, K. Miyazaki and M. Owada for reading the manuscript and giving us valuable comments. Thanks are also due to I. Buick and M. Brown for constructive reviews and K. Sajeev for editorial efforts. This study was mainly done during T. Kawakami’s stay in DEMS, ANU as a visiting fellow, and was financially supported by the Grant-in-Aid for JSPS Fellows (No. 05864) to T. Kawakami. References Acosta-Vigil, A., London, D., Morgan VI, G.B., Dewers, T.A., 2003. Solubility of excess alumina in hydrous granitic melts in equilibrium with peraluminous minerals at 700 – 800 -C and 200 MPa, and applications of the aluminum saturation index. Contrib. Mineral. Petrol. 146, 100 – 119. Bea, F., 1996. Residence of REE, Y, Th and U in granites and crustal protoliths; implications for the chemistry of crustal melts. J. Petrol. 37, 521 – 552. Benard, F., Moutou, P., Pichavant, M., 1985. 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