JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 PAGES 2303–2331 2001 Geochemical Evolution of Akagi Volcano, NE Japan: Implications for Interaction Between Island-arc Magma and Lower Crust, and Generation of Isotopically Various Magmas KATSURA KOBAYASHI∗ AND EIZO NAKAMURA PHEASANT MEMORIAL LABORATORY OF GEOCHEMISTRY AND COSMOCHEMISTRY, INSTITUTE FOR STUDY OF THE EARTH’S INTERIOR, OKAYAMA UNIVERSITY AT MISASA, TOTTORI, 682-0193, JAPAN RECEIVED APRIL 30, 2000; REVISED TYPESCRIPT ACCEPTED JUNE 10, 2001 Major and trace element, and Sr, Nd and Pb isotopic compositions were determined for whole-rock samples from the ‘isotopically anomalous’ Akagi volcano in the volcanic front of the NE Japan arc. Sr and Nd isotopic compositions of phenocrysts were also analyzed together with their major and trace element compositions. Compared with the other volcanoes from the volcanic front, the whole-rock isotope compositions of Akagi show highly enriched characteristics; 87Sr/86Sr = 0·7060–0·7088, Nd = −0·40 to −8·6, and 208Pb/204Pb = 38·4–38·8. The rare earth element (REE) patterns are characterized by heavy REE (HREE) depletions with U-shaped patterns from middle REE (MREE) to HREE, suggesting that amphibole fractionation was induced by a reaction between clinopyroxene and H2O-rich magma in the lower crust. The integrated isotope and trace elements systematics, and tectonic structure beneath Akagi volcano, suggest that lower-crustal assimilation by the H2O-rich primary magma could have been affected by the double subduction of Philippine Sea and Pacific oceanic plates. This double subduction could have supplied larger amounts of water to the magma source region in the wedge mantle than in the case of a single subduction zone. Significant differences in isotopic compositions are observed between phenocrysts and the coexisting melts. Such isotopic disequilibrium may have resulted from magma mixing between an isotopically depleted aphyric and an enriched porphyritic magma in a shallow magma chamber. The geochemical characteristics of these end-member magmas were retained in the lower crust, despite differing extents of lower-crustal assimilation by the H2O-rich magmas. Island-arc volcanism has been considered to result from partial melting of the wedge mantle induced by addition of slab-derived fluid-rich materials in subduction zones. This general model is supported by many geochemical studies employing major and trace element compositions, and radiogenic isotope systematics of arc volcanic ejecta (e.g. Nakamura et al., 1985; Woodhead & Fraser, 1985; Tatsumi et al., 1986; Ishikawa & Nakamura, 1994; Miller et al., 1994; Ryan et al., 1995; Shibata & Nakamura, 1997). These previous works mainly focused on the source characteristics in relation to the evolution of the mantle wedge in subduction zones. The magmatic evolution of individual volcanoes, after partial melting of the wedge mantle, and in shallow magma chambers has received less attention. Isotope and trace element geochemistry has typically been restricted to basaltic volcanic rocks, not the felsic rocks, to avoid the complexities of processes such as crystal fractionation, magma mixing and crustal assimilation. It is, however, essential to characterize the shallower magmatic processes along with the source characteristics. Magmas erupted at the Earth’s surface ∗Corresponding author. E-mail: [email protected] Oxford University Press 2001 Akagi volcano; H2O-rich magma; isotopic disequilibrium; lower-crustal assimilation; magma mixing KEY WORDS: INTRODUCTION JOURNAL OF PETROLOGY VOLUME 42 possess original source-related characteristics considerably modified by post-melting physico-chemical processes that may obscure the source signature. In this study, Akagi volcano in the NE Japan arc was investigated because of its distinctive isotopic composition relative to neighboring volcanoes from the volcanic front of the NE Japan arc. This arc is one of the ideal localities for discussing island-arc magmatism, because the structure of the subduction zone is well defined by abundant seismological data (e.g. Utsu, 1974; Yoshii, 1979; Zhao et al., 1990; Zhao, 1992). Moreover, systematic acrossarc variations of chemical and isotopic compositions were correlated with the depth of the Wadati–Benioff Zone (Notsu, 1983; Nakamura et al., 1985; Sakuyama & Nesbitt, 1986; Shibata & Nakamura, 1997). These across-arc systematics have been explained by continuous dehydration of the subducting oceanic slab resulting in a continuous decrease in the slab component in the source region with increasing depth to the subducted slab (Shibata & Nakamura, 1997). Volcanoes in the northern part of the volcanic front show a relatively narrow range of 87 Sr/86Sr ratio (0·7038–0·7045) (Notsu, 1983; Shibata & Nakamura, 1997). However, the Sr isotope composition in the southern part of the volcanic front increases to the south and has the highest 87Sr/86Sr ratio of >0·7087 at Akagi volcano (Notsu, 1983; Kersting et al., 1996). According to Gust et al. (1997), such systematic isotopic change along the volcanic front in the NE Japan arc could be explained by the contribution of subcontinental lithospheric mantle with some crustal contamination based on Sr–Nd–Pb isotope systematics and trace element geochemistry. They also suggested that the primary magmas of the volcanoes located south of the Tanakura Tectonic Line might have been involved with IndianOcean-type mantle, although they pointed out the possibility of lower-crustal contamination in the petrogenesis of the felsic volcanic rocks. However, their data are limited for individual volcanoes (only one to four samples without petrological description), making it difficult to discriminate samples that might have been involved with crustal contamination. It is, therefore, risky to discuss their source materials in the mantle beneath individual volcanic centers based on previous studies with insufficient petrological description of samples or a systematic dataset for each volcano. From such a point of view, we investigated Akagi volcano, measuring major and trace element compositions and multi-isotope compositions including Sr, Nd and Pb isotopes for whole-rock samples, to comprehensively understand the magmatic processes involved in the formation of the isotopically most anomalous volcano in the volcanic front of the NE Japan arc, and to assess the mechanisms of along-arc variation with respect to tectonic setting. In addition, the trace element, NUMBER 12 DECEMBER 2001 and Sr and Nd isotope compositions of phenocryst minerals were determined to further understand the shallow magma chamber processes and thereby elucidate the genesis of andesite magma in subduction zones. Geological and petrological features of Akagi volcano Akagi volcano (36°33′N, 139°12′E) is located in the southern part of the volcanic front of the NE Japan arc (Fig. 1). This area is characterized by the presence of many Quaternary volcanoes (e.g. Haruna, Hotaka, Nikko-Shirane volcano), and is one of the most volcanically active regions in Japan. As illustrated in Fig. 1, an unusual structure exists in the mantle wedge beneath the volcanic area including Akagi volcano; that is, a double subduction zone, in which the Philippine Sea plate is subducted into the wedge mantle above the Pacific plate (Ishida, 1991). The tip of the Philippine Sea plate is subducted to depth of >90 km just under Akagi volcano, and it probably adheres closely to the subducting Pacific plate, of which the interface depth is >110 km. Moreover, the depth of the Moho under Akagi volcano is >39 km, some 4 km deeper than is typical beneath the volcanic front of the NE Japan arc (Zhao et al., 1990; Zhao, 1992). These unusual tectonic conditions probably contribute to the formation of the distinctive geochemical characteristics of Akagi volcano. Although Akagi volcano is known to be mostly Quaternary in age, the lack of systematic radiometric ages precludes a clear understanding of the commencement of volcanic activity. On the basis of stratigraphical relationships between Akagi volcano (Moriya, 1968) and the neighboring Komochi volcano (Iizuka, 1996), the activity of Akagi volcano is thought to have started before 350 ka, and lasted intermittently to 30 ka. The latter age is based on the only available radiometric age, determined by the 14C method by Koga (1981). The volcanic history of Akagi volcano is divided into three main stages based on the eruption style: the older stratovolcano formation stage (O) characterized by the eruption of andesitic lava flow and ejecta of scoria, the younger stratovolcano formation stage (Y) characterized by pyroclastics without lava flows, and the central cone formation stage (Cc) (Moriya, 1968). The older stratovolcano formation stage (O) is further divided into three substages based on the volcanic stratigraphy: the early (Oe), middle (Om) and late (Ol) substages. The main volcanic stages and substages are geologically distinguishable. However, the eruptive sequence of volcanic ejecta within each stage is unclear based on stratigraphy. The present volcanic flank is mainly formed of pyroclastics of the Y stage and of secondary deposits. Lava flows can be observed in the caldera, which formed after the activity of the Y stage, and near the caldera wall. 2304 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Fig. 1. Geological and sample locality maps for Akagi volcano. The geological map is modified from Moriya (1968). In the inset diagram the volcanic front of the NE Japan arc and depth contours of the Wadati–Benioff Zone of the Philippine Sea plate (Ishida, 1992) are shown. Sample locality and description To investigate the magmatic processes of Akagi volcano, volcanic ejecta were collected based on the volcano stratigraphy established by Moriya (1968). The sampling localities are presented in Fig. 1. Samples were picked from fresh parts of outcrops to minimize alteration effects, and examined under the petrographic microscope to confirm the absence of significant secondary alteration. Petrographic observations indicate that the Akagi rock samples are highly porphyritic, with phenocrysts mainly consisting of plagioclase, hypersthene, augite and opaque minerals (see Table 1). Some of the felsic samples with SiO2 contents exceeding 58 wt % in the Ol substage and Y and Cc stages contain phenocrysts of hornblende instead of augite, even without quartz phenocrysts. Olivine phenocrysts are absent in the studied samples except for a sample AK1303, which contains an olivine pseudomorph surrounded by orthopyroxene. The mineral assemblage in the groundmass of the Oe and Om substages is plagioclase + pigeonite ± augite ± hypersthene. In contrast, samples from the Ol substage and the Y and Cc stage samples do not contain groundmass pigeonite. Sample preparation In the preparation of whole-rock samples for major, trace element and isotope analyses, chunks free from surface alteration were picked. These unaltered chunks were washed with Milli-Q water using an ultrasonic bath, and dried. Then, they were ground to fine powders with grain sizes under 200 mesh using a silicon nitride mortar. To separate phenocrysts, rock powders obtained using a disk mill were sieved to collect materials with grain size ranging from 100 to 200 mesh, as the average grain size of phenocrysts of plagioclase, orthopyroxene, and clinopyroxene or hornblende is >500 m. The sieved fraction was then processed to purify the minerals using conventional heavy liquid methods followed by an isodynamic separator. The mineral separation was finally 2305 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Table 1: Phenocryst assemblages and modal compositions of the studied samples Sample no. Pl Opx Cpx Ol Hb Mt 15·1 0·9 — — 1·8 0·5 AK2605 32·5 6·7 3·4 — tr. 1·7 AK2602 28·4 4·7 1·6 — 1·1 1·2 AK2603W 28·0 3·8 1·8 — — 1·0 AK2603G 29·5 3·2 1·1 — — 1·0 AK2603B 33·4 4·6 1·0 — — 1·0 AK2601 14·1 3·2 0·5 — — 0·5 AK1202 32·6 5·0 3·4 — tr. 2·0 AK1108 22·6 2·4 — — 2·1 0·9 AK1102 31·5 4·1 0·6 — — 1·2 AK1201 31·2 7·6 0·7 — — 1·3 AK1012 36·4 9·6 1·9 — — 1·8 AK-A 35·7 6·8 2·7 — — 1·6 AK1010 21·8 3·6 0·5 — — 0·6 AK0910 29·9 8·6 0·7 — — 1·0 AK1103 30·1 1·3 tr. — — 0·3 AK1011 30·1 2·6 tr. — — 0·9 AK1004 28·8 0·5 0·1 — — 0·3 AK1002 32·3 2·6 0·2 — — 0·2 AK2604 23·0 3·6 2·0 — — 1·1 AK1302 28·4 1·1 0·4 — — 0·6 AK1303 19·5 5·7 1·5 tr. — 1·9 Cc AK0807 Y Ol Om Oe Pl, plagioclase; Opx, orthopyroxene; Cpx, clinopyroxene; Ol, olivine; Hb, hornblende; Mt, magnetite; tr., trace (<0·1 vol. %). accomplished by hand-picking, and the purity is regarded as being better than 99%. Analytical methods All geochemical analyses were carried out at the Pheasant Memorial Laboratory (PML), Institute for Study of the Earth’s Interior, Okayama University at Misasa. Major element compositions of whole rocks were determined by X-ray fluorescence (XRF) using a Philips PW-2400 system; details of the analytical procedure are described elsewhere (Takei et al., in preparation). Trace element analyses of the whole rocks were performed by inductively coupled plasma mass spectrometry (ICP-MS) using a Yokogawa PMS 2000 instrument with a flow-injection method developed by Makishima & Nakamura (1997). The analytical reproducibility for trace element analyses of andesitic samples was <5%, and typically >3% (Makishima & Nakamura, 1997). The analytical procedures, including the chemical separations and mass spectrometry utilized in this study, are from Yoshikawa & Nakamura (1993), Makishima & Nakamura (1991a, 1991b) and Koide & Nakamura (1990) for Sr, Nd and Pb isotope analysis, respectively. Mass spectrometry was carried out on Finnigan MAT 261 and MAT 262 instruments equipped with five Faraday cups, applying a static-multi-collection mode. Normalizing factors used to correct isotopic fractionation of Sr and Nd are 86Sr/88Sr = 0·1194 and 146Nd/144Nd = 0·7219, respectively. The Pb isotope analyses were carried out with a nearly fixed filament temperature of >1200°C. Measured ratios of reference materials were 87Sr/86Sr = 0·710233 ± 8 (2m) for 100 ng of NIST SRM 987, 143 Nd/144Nd = 0·511818 ± 13 (2m) for 30 ng of La Jolla, and 206Pb/204Pb = 16·940 ± 15 (2m), 207Pb/ 2306 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Pb = 15·494 ± 16 (2m) and 208Pb/204Pb = 36·709 ± 38 (2m) for 100 ng of NIST SRM 981. Major element compositions of phenocrysts were determined by electron probe microanalysis (EMPA), using a JEOL JXA-8800R instrument, at Misasa following the techniques of Iizuka (1996). Trace element analyses of clinopyroxene, orthopyroxene and plagioclase phenocrysts were carried out employing a Cameca ims 5f ion microprobe at PML, Misasa, following procedures described by Nakamura & Kushiro (1997, 1998). Standard materials used for the calibration of trace element compositions were clinopyroxene from mantle xenoliths for pyroxene and hornblende analyses, and labradorite megacrysts for plagioclase analyses. These standards have been well characterized in terms of homogeneity and concentrations by both ion microprobe and ICP-MS. Clinopyroxene phenocrysts in the thin sections were sputtered with an O− primary beam of >10 nA intensity, resulting in >10 m beam diameter, and orthopyroxene and plagioclase with 15–20 nA intensity, resulting in >15 m beam diameter. Positive secondary ions were collected by ion counting using an energy offset of −60 V for Si, Rb, Sr, Y and Zr, and of −45 V for other elements from 4500 V acceleration with an energy bandpass of ±10 V. These operational conditions resulted in (1−2) × 105 c.p.s. for 30Si secondary ion in the analysis of phenocrysts. Analytical reproducibilities (RSD 1%, n = 10) for trace elements in the clinopyroxene standard were typically >5%, except for Ba (60%), and for the labradorite standard also typically >5%, except for Zr, Nb, Sm and heavy rare earth elements (HREE) (20–30%). 204 RESULTS AND DISCUSSION Major element compositions of whole-rock samples Major and trace element compositions of the Akagi samples are given in Table 2. Selected major element oxides are plotted against SiO2 content in Fig. 2, classifying the samples into the five stages defined by Moriya (1968) with reference to the Nasu volcanic zone, which forms the volcanic front of NE Japan (Kawano et al., 1961). As shown in Fig. 2, the range of SiO2 contents of the Akagi samples is between 53·4 and 71·4 wt %, consistent with those of previous studies, indicating that basaltic rocks have not been discovered at Akagi (Koga, 1984; Yamaguchi, 1990). TiO2, Fe2O3, MgO and CaO show negative trends against SiO2, and these trends are essentially consistent with those of the Nasu volcanic zone. Two different trends, the relatively steeper trend formed by the samples in the Oe and Om stages and that in the Ol, Y and Cc stages, can be recognized in the Fe2O3 and MgO diagrams, as well as in the Na2O diagram. The Al2O3–SiO2 diagram shows a more complicated feature, with a positive trend for the earlier stages of Oe and Om, and a negative trend for the later stages of Ol, Y and Cc. The former positive trend may be explained by considerable plagioclase accumulation in a shallow magma chamber, as the deduced Al2O3 contents in the melts obtained by subtracting the phenocryst compositions from those of the whole rocks form a negative trend against SiO2 overlapping the samples from the later stages as shown in Fig. 3. The major element compositions, after subtraction of the phenocrysts in Adatara volcano (the neighboring volcano located in the volcanic front of NE Japan), are also shown based on the data given by Fujinawa (1988, 1990). The corrected Al2O3 concentrations for Akagi volcano indicate a similar negative trend to that of Adatara volcano; however, that of Akagi is still systematically higher than for Adatara at similar SiO2 contents. The relatively high content of Al2O3 in the Akagi samples is consistent with the results of Yamaguchi (1990). The differentiation trend of corrected CaO against SiO2 (Fig. 3), which is also influenced by plagioclase accumulation, shows similar negative trends with increasing SiO2 content. However, the corrected Na2O contents are scattered and the differentiation trends are less obvious. Two distinct trends in the co-variation of FeO∗ (total Fe as FeO) and MgO of Akagi volcano can be divided into different rock series using the Miyashiro diagram (Fig. 4a; Miyashiro, 1974). In this diagram, the Oe and Om suites belong to the tholeiitic rock series, and the Ol, Y and Cc suites to the calc-alkaline rock series. On the other hand, although the Oe and Om suites are slightly less depleted in FeO∗ than the Ol, Y and Cc suites, the entire Akagi volcanic suite follows a calcalkaline differentiation trend in the AFM diagram (Fig. 4b). These major element characteristics of Akagi volcano cannot be explained by a simple magmatic differentiation process, because there appear to be considerable gaps in the SiO2 and total alkali contents in the transition from the Om to the Ol suites (Figs 2 and 4a). It may be, therefore, necessary to invoke more complex processes, such as magma mixing and crustal contamination associated with crystal fractionation. Moreover, the difference in the eruption style, which is the basis for the discrimination of the stages, does not correspond to the characteristics of the major element compositions. It may thus be more suitable to discuss the geochemical evolution of Akagi volcano without distinctions between stages and substages. Here, we discriminate simply between samples from the five stages (Oe, Om, Ol, Y, Cc), which are distinguishable by geological discontinuities. Trace element compositions Trace element compositions of whole rocks are listed in Table 1, and are plotted in primitive mantle 2307 AK1303 53·4 0·82 19·8 2·93 5·51 0·15 4·04 9·87 2·57 0·45 0·12 0·04 1·18 100·9 2·02 11·9 370 18·9 45·5 1·76 0·915 146 6·21 14·4 2·00 9·67 2·46 0·918 2·71 0·474 3·07 0·648 1·78 0·275 1·92 0·277 1·33 0·117 3·63 0·700 0·227 Sample no.: wt % SiO2 TiO2 Al2O3 Fe2O3 FeO MnO MgO CaO Na2O K 2O P 2O 5 H 2O− H 2O+ Total FeO∗/MgO ppm Rb Sr Y Zr Nb Cs Ba La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Hf Ta Pb Th U Oe 27·0 327 15·7 81·4 3·03 1·33 227 9·89 21·8 2·61 11·4 2·58 0·855 2·71 0·454 2·84 0·594 1·58 0·251 1·69 0·257 2·09 0·231 5·54 2·38 0·629 58·5 0·67 18·8 3·34 3·63 0·14 2·73 7·37 3·11 1·06 0·11 0·09 1·03 100·5 2·43 AK1302 17·8 357 15·8 63·1 2·18 0·892 185 7·57 17·4 2·24 9·85 2·40 0·813 2·46 0·416 2·58 0·558 1·48 0·236 1·59 0·237 1·86 0·150 4·27 1·69 0·381 56·3 0·66 19·1 3·38 3·88 0·14 3·10 7·87 2·73 0·66 0·13 0·24 2·10 100·3 2·23 AK2604 Om 24·3 379 23·7 107·7 4·04 0·539 280 12·83 24·6 3·29 14·2 3·22 1·01 3·31 0·579 3·26 0·703 1·90 0·290 2·02 0·298 2·58 0·257 4·53 2·43 0·507 57·1 0·79 19·2 2·70 4·39 0·13 2·73 7·67 3·10 0·95 0·18 0·17 1·16 100·3 2·49 AK1002 20·2 439 18·5 98·3 3·75 0·792 286 13·10 27·7 3·48 15·3 3·40 1·12 3·37 0·543 3·19 0·663 1·73 0·266 1·83 0·267 2·55 0·244 4·89 2·29 0·466 57·9 0·65 19·9 2·56 3·52 0·12 2·12 8·24 3·24 0·81 0·19 0·16 0·56 100·0 2·75 AK1004 23·1 436 19·2 92·3 3·50 0·713 280 11·99 25·6 3·31 14·6 3·06 1·04 3·07 0·489 2·93 0·610 1·55 0·239 1·66 0·245 2·31 0·223 5·38 2·14 0·483 58·2 0·64 19·9 2·25 3·55 0·11 1·94 7·95 3·24 0·86 0·20 0·20 0·86 99·8 2·88 AK1011 24·3 383 17·8 68·6 2·78 0·839 227 9·45 21·8 2·74 12·0 2·79 0·979 2·85 0·496 2·91 0·615 1·70 0·243 1·77 0·257 2·02 0·201 4·22 2·20 0·505 59·5 0·51 20·7 1·95 2·29 0·09 1·36 7·82 3·34 0·91 0·16 0·17 0·96 99·7 2·97 AK1103 19·5 340 16·3 64·7 2·06 0·494 180 8·04 17·7 2·33 10·3 2·52 0·868 2·57 0·414 2·74 0·556 1·47 0·225 1·55 0·232 1·63 0·142 4·10 1·66 0·374 53·6 0·82 19·1 3·58 5·84 0·16 4·53 8·55 2·52 0·43 0·14 0·12 0·75 100·2 2·00 AK0910 Ol 14·2 379 16·5 84·0 3·12 0·183 222 11·70 25·6 3·22 14·7 3·27 1·06 3·27 0·539 3·13 0·640 1·68 0·257 1·76 0·259 2·12 0·188 4·01 1·45 0·334 55·7 0·77 18·5 3·95 4·76 0·15 3·85 7·12 2·82 0·66 0·17 0·41 1·45 100·4 2·16 AK1010 Table 2: Major and trace element compositions of whole-rock samples from Akagi volcano 22·9 310 16·9 66·6 2·59 0·495 188 8·11 17·8 2·28 9·95 2·29 0·794 2·33 0·400 2·49 0·517 1·42 0·219 1·55 0·229 1·82 0·191 4·03 1·84 0·469 56·0 0·77 18·0 3·86 4·90 0·16 4·08 8·11 2·80 0·67 0·14 0·03 0·36 99·9 2·05 AK-A 22·0 325 15·6 70·7 3·17 0·475 201 8·67 18·8 2·37 10·4 2·46 0·830 2·61 0·429 2·64 0·537 1·42 0·211 1·44 0·217 1·99 0·245 6·63 2·06 0·476 56·4 0·77 18·0 4·61 3·78 0·15 4·05 7·72 2·82 0·80 0·13 0·07 0·71 100·0 1·96 AK1012 8·5 369 15·1 47·9 1·72 0·255 169 6·59 15·2 2·07 9·38 2·36 0·883 2·51 0·421 2·66 0·568 1·54 0·233 1·65 0·227 1·32 0·112 2·41 0·832 0·179 56·5 0·69 18·0 3·95 4·32 0·16 3·84 7·40 2·76 0·83 0·13 0·30 1·56 100·4 2·05 AK1201 22·0 383 25·5 95·1 4·08 1·08 334 16·7 31·4 4·39 19·0 4·03 1·22 4·18 0·684 4·12 0·876 2·26 0·358 2·46 0·372 2·56 0·247 4·85 2·46 0·522 59·5 0·62 17·6 4·29 2·69 0·13 2·70 6·49 2·83 0·75 0·15 0·48 1·68 99·9 2·42 AK1102 33·3 414 18·8 82·10 4·43 0·802 393 16·9 36·8 4·43 18·8 3·76 1·10 3·51 0·533 3·13 0·600 1·46 0·234 1·57 0·203 2·97 0·260 8·25 1·90 0·535 62·1 0·49 16·2 2·76 2·13 0·11 1·56 5·58 3·13 1·09 0·15 0·20 3·77 99·3 2·97 AK1108 JOURNAL OF PETROLOGY VOLUME 42 2308 NUMBER 12 DECEMBER 2001 AK1202 58·0 0·69 18·0 3·29 3·54 0·13 3·06 6·96 2·78 0·86 0·12 0·62 1·90 100·0 2·12 22·4 316 17·4 101 3·17 1·19 351 13·6 28·8 3·34 13·8 2·93 0·941 3·05 0·477 2·96 0·637 1·69 0·266 1·87 0·274 2·71 0·194 6·29 3·15 0·704 Sample no.: wt % SiO2 TiO2 Al2O3 Fe2O3 FeO MnO MgO CaO Na2O K 2O P 2O 5 H 2O− H 2O+ Total FeO∗/MgO ppm Rb Sr Y Zr Nb Cs Ba La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Hf Ta Pb Th U Y 31·4 377 18·0 89·1 3·78 1·61 370 13·4 28·0 3·27 13·7 2·77 0·910 2·73 0·434 2·58 0·551 1·51 0·240 1·65 0·250 2·50 0·291 7·05 3·39 0·660 59·3 0·54 18·0 3·50 3·05 0·14 3·00 6·96 2·86 1·04 0·13 0·13 1·17 99·8 2·07 AK2601 31·0 391 14·1 79·3 3·37 1·61 351 12·6 27·4 3·03 12·2 2·46 0·840 2·34 0·379 2·22 0·480 1·27 0·201 1·43 0·215 2·23 0·246 7·47 3·46 0·627 60·3 0·57 17·1 3·25 3·35 0·14 3·03 6·59 2·98 1·10 0·14 0·03 0·97 99·6 2·07 AK2603B 30·9 369 17·2 93·1 3·66 1·68 422 13·6 28·6 3·25 13·5 2·70 0·859 2·62 0·415 2·43 0·535 1·45 0·222 1·62 0·232 2·51 0·264 7·20 3·79 0·617 60·5 0·56 17·8 3·23 2·78 0·12 2·44 6·84 3·06 1·12 0·14 0·03 0·81 99·4 2·33 AK2603G 31·9 366 17·8 89·5 3·51 1·55 356 13·5 27·7 3·30 13·5 2·88 0·894 2·63 0·428 2·59 0·545 1·47 0·238 1·64 0·249 2·29 0·240 5·45 3·41 0·659 60·6 0·53 17·6 2·73 3·30 0·13 2·72 6·82 3·04 1·08 0·13 0·08 0·99 99·8 2·12 32·2 386 17·8 92·9 3·80 1·58 377 14·6 29·4 3·57 14·5 2·97 0·957 2·88 0·470 2·63 0·602 1·62 0·256 1·78 0·262 2·46 0·289 6·86 3·38 0·654 61·1 0·55 17·1 3·33 2·92 0·13 2·95 6·63 2·86 1·10 0·12 0·09 0·94 99·8 2·00 AK2603W AK2602 30·1 341 13·8 92·7 2·84 1·31 353 12·7 27·5 3·12 12·4 2·54 0·892 2·52 0·380 2·39 0·483 1·36 0·213 1·48 0·219 2·50 0·193 5·97 3·44 0·692 62·0 0·55 17·5 2·61 2·73 0·11 2·36 6·42 3·20 1·17 0·12 0·18 0·83 99·8 2·15 AK2605 64·1 276 11·5 92·7 4·92 1·74 459 16·1 31·4 3·41 12·5 2·17 0·676 2·05 0·323 1·85 0·407 1·13 0·183 1·39 0·198 2·44 0·489 11·1 5·59 1·50 71·4 0·30 15·1 1·21 1·22 0·08 0·78 3·48 3·84 2·01 0·09 0·03 1·03 100·5 2·98 AK0807 Cc KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO 2309 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Fig. 2. Major element variation against SiO2 (wt %) content in Akagi samples. Dark and light gray shaded areas are the tholeiite and calcalkali rock series of the Nasu Volcanic zone in NE Japan, respectively [data from Kawano et al. (1961)]. (PM)-normalized diagrams in Fig. 5. The contents of incompatible elements are enriched compared with most basaltic rocks of the volcanic front of the NE Japan arc (Shibata & Nakamura, 1997). However, the less incompatible elements such as the HREE are less enriched. These trace element characteristics cannot be explained by simple fractional crystallization from a common primary basaltic magma in the volcanic front using the phenocryst assemblage in the Akagi volcanic rocks. Such a fractionation process should increase not only the most incompatible trace elements but also the HREE. The behavior of REE in the Akagi samples is discussed below in more detail in a section describing their isotopic compositions. With progress within a volcanic stage, the contents of highly incompatible elements become gradually higher. However, no correlation is observed between trace elements and SiO2 contents in the Om and Ol stages. Akagi volcanic rocks show positive spikes of Sr and Pb, and remarkably negative spikes for Nb and Ta, consistent with the general features of trace elements in island-arc volcanic rocks (e.g. Wood et al., 1979; Perfit et al., 1979; Sakuyama & Nesbitt, 1986; Shibata & Nakamura, 1997; Woodhead et al., 1998). Sr–Nd–Pb isotope systematics of Akagi volcano The whole-rock Sr, Nd and Pb isotopic compositions are listed in Table 3 and are plotted in Fig. 6 along with the reference variations of volcanic rocks from the NE Japan arc, lower-crustal materials, oceanic sediments and 2310 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Fig. 3. Corrected Al2O3, CaO and Na2O contents plotted against SiO2 content by the subtraction of phenocryst compositions from the bulk Akagi samples. Symbols are the same as in Fig. 2. The continuous and broken lines indicate corrected compositions of the tholeiite and calcalkali rock series of Adatara volcano, respectively (Fujinawa, 1988, 1990). MORBs. The 87Sr/86Sr ratios of the Akagi samples vary widely from 0·70603 to 0·70879, consistent with the data reported by Notsu et al. (1985), and are significantly higher than those of other typical volcanoes in the northern part of Tanakura Tectonic Line in the volcanic front of the NE Japan arc, which have an average 87Sr/86Sr ratio of >0·7045 (Notsu, 1983; Gust et al., 1997; Shibata & Nakamura, 1997). The Nd isotopic compositions of Akagi range from −0·4 to −8·6 in Nd, and are much lower than those of other volcanoes in the northern part of the volcanic front with Nd of 3–10 (Gust et al., 1997; Shibata & Nakamura, 1997). The 206Pb/204Pb, 207Pb/204Pb and 208 Pb/204Pb ratios vary in the range of 18·21–18·44, 15·56–15·64 and 38·44–38·79, respectively (Fig. 6b and c). These isotope characteristics of Akagi, therefore, are regarded as ‘unusual’ in the NE Japan arc, confirming the original observations based on Sr isotopic compositions by Notsu et al. (1985). Fig. 4. (a) FeO∗/MgO plotted against SiO2 for Akagi volcano. The TH series and CA series were defined by Miyashiro (1974), and the boundary line is defined by FeO∗/MgO = 0·1562 × SiO2 − 6·685. (b) AFM diagram for Akagi volcano. A, Na2O + K2O; F, FeO + 0·9Fe2O3; M, MgO. Symbols are as in (a). The boundary line between the TH and CA series is based on the definition of Gill (1981). In the Sr and Nd isotope diagram (Fig. 6a), the Akagi samples have a linear trend with an extremely isotopically enriched signature compared with those of other ‘typical’ volcanoes in the volcanic front of the NE Japan arc, which have simple isotopic across-arc variations (Shibata & Nakamura, 1997). These isotopic compositions are widely varied not only over the entire history of the volcano but also with each volcanic stage of Akagi volcano. An extrapolation of the Akagi trend to the depleted direction nearly intersects the isotopic trend of the NE Japan arc at a value typical of volcanoes on the front. As is shown in Fig. 6b and c, the Pb isotopic compositions of the Akagi samples form clusters that are clearly distinct from the isotopic trend of the NE Japan arc (Shibata & Nakamura, 1997). The 206Pb/204Pb ratios 2311 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Fig. 5. Primitive mantle (PM)-normalized trace element patterns for whole-rock samples from Akagi volcano. The PM normalization values are from McDonough & Sun (1995) in this and subsequent figures. The shaded area shows a range of samples from the Iwate and Funagata volcanoes in the volcanic front of the NE Japan arc (Shibata & Nakamura, 1997). are lower, whereas the 207Pb/204Pb and 208Pb/204Pb ratios are higher than those of the ‘typical’ volcanoes on the front. In the Nd–206Pb/204Pb diagram (Fig. 6d), the Akagi data also define a linear trend clearly different from the tendency in the isotope variations of other primary magmas in the northern part of the NE Japan arc, and which extrapolates to the values characteristic of the volcanic front. The above isotope systematics suggest that the Akagi volcanic rocks were formed by two-component mixing of an isotopically depleted and an enriched end-member. Intersections between the ‘typical’ trend of the NE Japan arc and the extrapolations of the Akagi trends in the Sr–Nd and Nd–Pb diagrams indicate that the depleted end-member is similar to the primary magma in the volcanic front of the NE Japan arc, which was defined by Shibata & Nakamura (1997). It is, however, still difficult to identify the source of the enriched end-member using these isotope systematics. On the basis of the existence of an enriched component deduced from the isotope systematics and the tectonic setting of the Akagi volcano, the following candidates for the enriched end-member can be postulated: (1) oceanic sediments; (2) upper crust; (3) lower crust. Isotopic variations of oceanic sediments in the NW Pacific and lower-crustal materials are shown in Fig. 6. The isotopic composition of JG-1, the granitic standard of the Geological Survey of Japan, which outcrops near Akagi volcano and is considered to be the upper-crustal basement of Akagi, is shown in the diagrams. It should be noted that the JG-1 composition lies within the field for oceanic sediments (data from Nohda & Wasserberg, 1981; Koide & Nakamura, 1990), therefore the uppercrustal field is not shown in Fig. 6. The isotopic characteristics of lower-crust materials under the NE Japan arc have not been well understood. The lower crust under the arc might be considered as a fragment of continental material and/or a piled-up sequence of young 2312 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Table 3: Sr, Nd and Pb isotopic compositions of whole-rock samples from Akagi volcano Sample no. 87 Sr/86Sr 143 Nd/144Nd Nd 206 Pb/204Pb 207 Pb/204Pb 208 Pb/204Pb Cc 0·706852±9 0·512437±12 −3·92 18·444±9 15·600±7 38·667±18 AK2605 0·707414±10 0·512297±11 −6·65 18·290±7 15·573±6 38·599±15 AK2602 0·708087±11 0·512248±12 −7·61 18·268±35 15·592±29 38·695±73 AK2603W 0·707774±10 0·512274±12 −7·10 18·280±13 15·578±11 38·630±27 AK2603G 0·707774±9 0·512233±10 −7·90 18·285±24 15·583±21 38·645±52 AK2603B 0·707800±11 0·512296±9 −6·67 18·294±23 15·594±20 38·677±49 AK2601 0·708114±11 0·512209±13 −8·37 18·290±64 15·609±55 38·732±135 AK1202 0·707385±10 0·512336±12 −5·89 18·309±12 15·577±10 38·605±24 AK1108 0·708792±12 0·512199±13 −8·56 18·262±20 15·583±16 38·625±42 AK1102 0·708244±10 0·512210±10 −8·35 18·259±19 15·584±18 38·634±41 AK1201 0·706833±8 0·512442±12 −3·82 18·366±20 15·576±4 38·580±9 AK0807 Y Ol AK1012 0·707119±8 0·512392±10 −4·80 18·327±29 15·576±24 38·597±60 AK-A 0·706765±8 0·512423±11 −4·19 18·341±79 15·602±65 38·642±165 AK1010 0·708632±9 0·512224±12 −8·08 18·242±74 15·605±61 38·684±156 AK0910 0·706857±9 0·512430±10 −4·06 18·279±75 15·575±65 38·556±157 AK1103 0·706840±9 0·512440±9 −3·86 18·380±50 15·637±39 38·794±105 AK1011 0·708705±9 0·512213±10 −8·29 18·206±22 15·583±19 38·643±47 AK1004 0·708716±10 0·512210±8 −8·35 18·253±16 15·625±91 38·734±156 AK1002 0·707532±8 0·512381±10 −5·01 18·302±20 15·579±16 38·615±41 AK2604 0·706972±10 0·512388±12 −4·88 18·334±97 15·614±81 38·665±204 AK1302 0·707207±8 0·512387±10 −4·90 18·375±45 15·600±38 38·556±95 AK1303 0·706034±10 0·512618±11 −0·39 18·354±29 15·561±23 38·436±60 Om Oe Isotopic fractionation was normalized to 86Sr/88Sr = 0·1194, 2 mean. Nd/144Nd = 0·7219. Analytical precisions for isotope data are 146 metamorphic rocks originally derived from the arc magmas (Arculus & Johnson, 1981). In the latter case, the isotopic characteristics should be similar to those of the arc volcanic rocks, as a result of less time-integrated isotopic evolution. We prefer, therefore, that the isotopic characteristics of the lower-crustal materials are similar to ‘continental’ type lower crust in Fig. 6. In the Sr–Nd diagram (Fig. 6a), the isotopic compositions of oceanic sediments and lower crust overlap, making it difficult to unambiguously identify an enriched end-member. However, the Pb–Pb and Nd–Pb diagrams clearly discriminate between lower crust and oceanic sediments and/or upper crust. On the basis of Fig. 6b–d, it appears that oceanic sediments and/or upper crust are not possible candidates for the enriched end-member. In practice, the isotopic compositions of sediments, which occur on the Philippine Sea plate, cannot be the enriched end-member for Akagi volcano. Consequently, it is most likely that the enriched end-member involved in magma formation of Akagi volcano is lower-crustal material, although Notsu et al. (1985) proposed a sediment component derived from the subducting Philippine Sea plate as the enriched end-member in Akagi volcano based on 87 Sr/86Sr and 18O data. The complete Sr, Nd and Pb isotopic dataset from the along-arc volcanoes by Kersting et al. (1996) and Gust et al. (1997) is also shown in Fig. 6. The isotopic trends defined by the volcanoes located to the south of the Tanakura Tectonic Line (STTL: Akagi, Nikkoshirane, Nantai, Takahara, Nasu) essentially have the same direction as those of the primary magmas in the volcanic front of the NE Japan arc (Fig. 6). Therefore, it is likely that the depleted end-member for 2313 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Fig. 6. Nd–Sr–Pb isotope systematics of the Akagi samples. Symbols are as in Fig. 2. Nd isotope ratios are normalized to CHUR ( 143Nd/ 144 Nd = 0·512638). The large open circle represents the isotopic composition of the inferred primary magma of the NE Japan arc, and the thick continuous line extending from the open circle indicates the across-arc variation in the NE Japan arc (Shibata & Nakamura, 1991, 1997). The fields ‘N’ and ‘S’ represent the along-arc variations of the magmatic suites from north and south of the Tanakura Tectonic Line (NTTL and STTL), respectively (Kersting et al., 1996; Gust et al., 1997). ×, isotopic composition of JG-1, the granitic rock standard material of the Geological Survey of Japan (Nohda & Wasserburg, 1981; Koide & Nakamura, 1990). The range of isotopic variation of MORB, oceanic sediments including those on the Philippine Sea plate and the lower crust are also shown. Data source for MORB: Cohen et al. (1980), Dupre & Allègre (1980), White & Hofmann (1982), Le Roex et al. (1983); oceanic sediments: O’Nions et al. (1978), White & Patchett (1984), Woodhead & Fraser (1985), White & Dupre (1986), Ben Othman et al. (1989), Cousens et al. (1994), Shimoda et al. (1998); lower crust: Zartman & Doe (1981), Rudnick et al. (1986), Zartman & Haines (1988), Stoltz & Davies (1989), Kempton et al. (1990), Rudnick & Goldstein (1990), Downes et al. (1991). the source of the volcanoes from the STTL also is similar to the MORB-type wedge mantle metasomatized by the fluid derived from dehydration of the subducted slab as proposed by Shibata & Nakamura (1997) for the primary magma source of the NE Japan arc. Moreover, the Nd–Pb diagram (Fig. 6d) for the STTL group clearly indicates the involvement of lower-crustal materials as an enriched end-member, as well as at Akagi volcano. It is, therefore, not necessary to introduce a unique mantle source such as Indian Ocean-type mantle beneath the volcanoes from the STTL to explain the isotope systematics of the STTL group based on the dataset given in this study and in previous studies (Kersting et al., 1996; Gust et al., 1997). Major and trace element compositions of phenocrysts Seven samples from the Ol stage, which is characterized by large variations in whole-rock major element and isotopic composition (SiO2 = 55·8–63·5 wt %, 87Sr/ 86 Sr = 0·70683–0·70879), were selected to investigate detailed magmatic processes based on the chemical and isotopic compositions of phenocrysts. Phenocrysts in Akagi volcano rocks are always zoned. The mg-numbers [defined as 100 × Mg/(Mg + Fe2+)] of cores in orthopyroxene and clinopyroxene are 75–65 and 80–73, respectively. Reverse zoning is commonly observed in the pyroxene of samples AK1102, AK0910, AK1010 and AK1108. The an-number in the cores of 2314 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO plagioclase phenocrysts does not have a bimodal signature, which has been regarded as evidence of magma mixing according to Sakuyama (1981). Hornblende phenocrysts occur in only the most siliceous sample in this stage. The hornblende phenocrysts have a zonal structure with decreasing mg-number and edenite component from core to rim, and a pseudomorph of hornblende phenocrysts, consisting of fine-grained plagioclase + orthopyroxene + clinopyroxene + opaque minerals, also occurs in five siliceous samples listed in Table 1. Trace element compositions of orthopyroxene, clinopyroxene and plagioclase phenocrysts in the Ol stage are given in Table 4 and their primitive mantle-normalized patterns are shown in Figs 7 and 8. The trace element patterns of pyroxenes show clear negative Sr and Nb spikes. Experimental determinations of the Kd for Sr between pyroxenes and silicate melt show no Sr depletion compared with the adjacent elements Pr and Nd (Green, 1994). The Sr depletion, therefore, indicates that the pyroxenes crystallized from Sr-depleted melts, although Sr enrichment is observed in whole-rock analyses of the Ol samples (see Fig. 5). Such Sr enrichment could be expected as a result of the accumulation of plagioclase, which is characterized by a strong Sr positive spike (Fig. 8). The influence of plagioclase accumulation is expected based on the major element compositions of the wholerock samples (see Fig. 3). The positive Sr spikes are removed by consideration of phenocryst subtraction; for example, Sr/Sr∗ value [Sr∗ is defined as (Pr + Nd)/2 on the primitive mantle-normalized value] of the melt part in AK-A decreases from 2·0 to 0·7. The Nb depletions in the phenocrysts can be attributed to the whole-rock compositions that are unique to islandarc volcanic rocks (see also Fig. 5). The Zr depletion in clinopyroxene and the slightly positive Zr spike in orthopyroxene may be simply explained by the difference in Kd [i.e. KdHFSE/KdLILE,LREE >1 for orthopyroxene, KdHFSE/ KdLILE,LREE <1 for clinopyroxene (where HFSE indicates high field strength elements, LILE indicates large ion lithophile elements and LREE are light REE); Green, 1994]. The Y depletion in the plagioclase phenocrysts may be a characteristic feature of plagioclase, because such depletion is always observed in the plagioclases used for our secondary ion mass spectrometry standards (also precisely characterized by ICP-MS). In samples AK1010 and AK1108, the incompatible elements in the orthopyroxene rims are significantly depleted compared with those of the core. This is consistent with reverse zoning (based on mg-number) in the pyroxene of these samples. Sr and Nd isotope compositions of phenocrysts in the Ol stage The isotopic compositions of Sr and Nd for phenocrysts in the Ol stage are given in Table 5 and plotted in a Sr–Nd isotope diagram in Fig. 9. In this diagram, the isotopic compositions of the melts are calculated using the Sr and Nd isotopic and elemental compositions of the whole rocks, and the modal abundance, densities, isotopic and elemental compositions of the phenocrysts. The results are given in Table 6. The isotopic compositions of the phenocrysts tend to have more enriched compositions, especially for Sr, exceeding the analytical uncertainties, than the calculated compositions of the melts. In other words, the phenocrysts are isotopically in disequilibrium with the surrounding melt. The uncertainty of calculated melt isotopic compositions mainly depends on the measured modal abundance of the phenocrysts, especially plagioclase, which is a main sink for Sr. The statistical error of the plagioclase modal abundance is estimated to be >3%, based on the counting statistics. This uncertainty affects the 87Sr/86Sr ratio of melts up to ±>0·0002 for AK-A and AK1012, but the uncertainties in the others are less than ±0·0001. In contrast, the calculated Nd isotopic compositions of the melts are not significantly affected by the uncertainty in the modal abundance. Heterogeneity in the sample also causes the error in the estimation of the Sr and Nd isotopic composition of the melt. However, the distributions of phenocrysts are homogeneous in the samples from the Ol stage. Therefore, the isotopically depleted characteristics of the calculated melts compared with the phenocrysts are apparently significant except in sample AK1010. In AK1010, the Sr isotopic composition of the melt is identical to that of the phenocrysts within the analytical uncertainties. However, the Nd isotopic composition of the plagioclase is significantly lower than that of the calculated melt. INTERACTION BETWEEN ISLANDARC MAGMA AND LOWER CRUST In Fig. 10, chondrite-normalized REE patterns of Akagi volcano samples are compared with those for Adatara volcano (Fujinawa, 1992), which is a neighboring volcano in the volcanic front of the NE Japan arc and has similar petrological and mineralogical features to those of Akagi. This comparison shows that Akagi samples have (1) significantly lower HREE abundance, (2) significantly higher LREE/HREE ratios, and (3) U-shaped REE patterns between the middle REE (MREE) and HREE. The REE patterns from Adatara volcano were explained by crystal fractionation (Fujinawa, 1992). However, the REE characteristics of Akagi volcano cannot be formed by such a simple fractionation involving removal of minerals such as plagioclase, orthopyroxene, clinopyroxene and opaque minerals occurring as phenocrysts in the Akagi samples. Because the mineral–melt partition coefficients of the REE are much smaller than one, 2315 2316 43·4 25·6 12·5 0·002 27·1 1·00 3·93 0·825 5·27 2·37 0·935 3·44 3·81 2·03 2·16 0·317 ppm Sr Y Zr Nb Ba La Ce Pr Nd Sm Eu Gd Dy Er Yb Lu 21·3 37·3 23·3 0·001 0·492 1·93 7·78 1·76 10·8 5·06 1·21 5·90 7·50 3·29 4·00 0·516 20·7 34·1 21·4 0·002 0·284 1·73 7·13 1·89 11·6 4·74 1·26 5·80 7·22 3·21 3·52 0·470 core 0·207 4·15 1·54 0·001 0·225 0·018 0·045 0·013 0·109 0·081 0·027 0·140 0·479 0·348 0·511 0·074 0·291 3·33 1·18 0·001 0·489 0·030 0·072 0·010 0·100 0·068 0·028 0·163 0·297 0·276 0·449 0·075 core rim 0·204 5·89 1·54 n.d. 0·016 0·014 0·078 0·023 0·170 0·090 0·046 0·207 0·697 0·416 0·642 0·121 rim 0·557 5·46 2·98 0·001 0·687 0·037 0·074 0·025 0·157 0·137 0·046 0·208 0·610 0·476 0·587 0·094 orthopyroxene 16·7 21·4 10·8 0·001 2·63 1·08 3·42 0·711 4·73 2·30 0·579 2·71 3·15 1·68 1·91 0·274 525 0·054 0·490 0·193 12·1 0·903 1·70 0·197 0·948 0·191 0·430 0·222 0·085 0·031 0·033 0·004 rim plagioclase 558 0·026 0·032 0·065 8·81 0·639 1·14 0·156 0·647 0·095 0·254 0·038 0·032 0·019 0·008 0·003 rim plagioclase 596 0·031 0·091 0·032 11·7 1·75 2·88 0·365 1·16 0·189 0·539 0·087 0·080 0·033 0·006 0·002 core 621 0·056 0·324 0·152 11·8 2·28 4·12 0·433 1·69 0·276 0·496 0·219 0·054 0·028 0·015 0·003 core 25·6 31·7 29·0 0·002 0·106 1·71 7·72 1·53 10·8 4·19 1·20 5·27 5·51 2·93 2·79 0·392 core 22·0 33·9 22·3 0·002 0·403 1·48 6·01 1·44 10·1 3·98 0·960 5·39 5·54 2·91 2·91 0·445 rim 19·2 34·1 23·2 0·002 2·66 1·49 6·47 1·65 10·1 4·25 1·04 5·87 6·80 3·55 3·21 0·479 core clinopyroxene AK1012 28·4 25·3 21·6 0·005 0·96 1·40 6·22 1·40 9·53 3·05 1·00 4·24 3·81 2·20 2·05 0·289 rim clinopyroxene AK1010 0·889 3·46 2·02 0·001 1·20 0·037 0·091 0·028 0·112 0·080 0·025 0·196 0·415 0·327 0·421 0·077 core 0·226 4·82 1·92 0·001 0·108 0·012 0·063 0·013 0·089 0·052 0·062 0·154 0·478 0·485 0·856 0·134 rim 0·205 4·10 1·51 0·001 0·231 0·011 0·064 0·015 0·114 0·046 0·047 0·198 0·492 0·394 0·576 0·089 core orthopyroxene 0·207 2·62 1·49 0·001 0·037 0·012 0·026 0·009 0·052 0·109 0·029 0·162 0·305 0·247 0·300 0·041 rim orthopyroxene 596 0·043 0·194 0·137 17·0 1·75 3·43 0·360 1·44 0·287 0·526 0·287 0·082 0·033 0·026 0·004 rim plagioclase 667 0·051 0·355 0·0821 38·5 2·78 5·00 0·621 1·85 0·333 1·24 0·317 0·186 0·068 0·037 0·004 rim plagioclase 583 0·097 2·77 0·607 24·9 2·59 4·35 0·487 1·87 0·213 0·710 0·261 0·125 0·033 0·017 0·004 core 655 0·091 0·282 0·181 11·8 1·46 2·78 0·367 1·50 0·211 0·504 0·183 0·107 0·026 0·025 0·002 core VOLUME 42 clinopyroxene Sample no.: AK-A ppm Sr Y Zr Nb Ba La Ce Pr Nd Sm Eu Gd Dy Er Yb Lu core rim rim core orthopyroxene clinopyroxene Sample no.: AK0910 Table 4: Trace element compositions of phenocrysts from Ol stage samples obtained by ion microprobe JOURNAL OF PETROLOGY NUMBER 12 DECEMBER 2001 2317 ppm Sr Y Zr Nb Ba La Ce Pr Nd Sm Eu Gd Dy Er Yb Lu 61·4 188·8 81·8 0·335 81·4 8·33 37·0 8·90 58·0 20·5 4·39 32·1 29·5 15·4 16·0 2·56 58·4 191·8 81·3 0·312 72·8 7·49 32·8 7·83 53·1 18·4 4·24 28·1 29·4 14·8 15·9 2·31 0·154 5·72 3·75 0·001 0·071 0·011 0·049 0·013 0·139 0·125 0·035 0·143 0·611 0·573 0·811 0·140 0·176 5·86 2·83 0·001 0·102 0·101 0·297 0·042 0·250 0·174 0·041 0·370 0·602 0·599 0·918 0·137 core rim core 0·447 6·63 2·74 0·001 0·928 0·022 0·090 0·012 0·131 0·118 0·047 0·286 0·720 0·552 0·852 0·115 rim 0·162 6·47 3·48 0·001 0·106 0·008 0·071 0·015 0·173 0·099 0·037 0·322 0·727 0·513 0·776 0·115 orthopyroxene AK1108 Sample: 21·1 27·9 14·6 0·002 0·046 1·09 5·09 1·30 7·89 3·28 0·972 4·20 5·92 2·51 2·57 0·424 hornblende 22·1 32·6 19·4 0·002 0·231 1·48 6·14 1·45 9·62 3·75 1·05 6·01 6·34 3·28 3·07 0·478 ppm Sr Y Zr Nb Ba La Ce Pr Nd Sm Eu Gd Dy Er Yb Lu core rim rim core orthopyroxene clinopyroxene Sample no.: AK1201 764 0·040 0·351 0·114 17·6 3·67 5·96 0·645 2·23 0·269 0·933 0·172 0·069 0·041 0·010 0·003 rim plagioclase 612 0·043 0·840 0·043 10·4 1·48 2·66 0·301 1·00 0·186 0·492 0·253 0·079 0·026 0·007 0·001 rim plagioclase 800 0·036 0·082 0·070 10·8 2·94 4·49 0·560 1·61 0·300 0·638 0·292 0·045 0·030 0·006 0·002 core 527 0·030 0·012 0·022 2·49 0·391 0·791 0·082 0·375 0·099 0·180 0·105 0·025 0·010 0·006 n.d. core 26·1 46·8 41·9 0·008 22·4 2·61 10·6 2·42 16·3 5·92 1·39 7·47 8·23 3·92 3·69 0·643 rim 17·0 42·7 25·1 0·002 4·13 1·89 8·53 2·10 13·3 4·58 1·47 5·48 8·73 4·02 4·21 0·583 core clinopyroxene AK1102 0·177 5·67 2·33 0·001 0·097 0·020 0·107 0·027 0·164 0·073 0·017 0·177 0·454 0·658 0·783 0·131 rim 0·140 5·09 2·71 0·001 0·073 0·005 0·032 0·010 0·084 0·032 0·034 0·167 0·370 0·477 0·752 0·110 core orthopyroxene 681 0·052 0·153 0·057 12·9 2·16 3·88 0·437 1·62 0·248 0·644 0·323 0·055 0·040 0·017 0·003 rim plagioclase 774 0·034 0·046 n.d. 12·0 3·37 5·46 0·588 1·84 0·274 0·752 0·029 0·056 0·025 0·014 0·002 core KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Fig. 7. PM-normalized trace element patterns of clinopyroxene and orthopyroxene phenocrysts in Ol stage samples. For the AK1108 sample, hornblende data are represented instead of clinopyroxene, because there are no clinopyroxene phenocrysts in this sample. Open and filled symbols indicate the rim and core of phenocrysts, respectively. fractional crystallization in a shallow magma chamber would increase the total REE with LREE enrichment, as is observed in Adatara volcano. This mechanism, therefore, cannot explain characteristics (1) and (2) of Akagi’s REE compositions. On the basis of a high-pressure melting experiment involving a basaltic composition, Forden & Green (1992) suggested that the liquidus phase is clinopyroxene under high-H2O conditions in the lower-crustal environment, and olivine is the liquidus phase at lower pressure conditions. When the temperature of the melts drops, clinopyroxene becomes unstable, and reacts with the melt to form amphibole, resulting in the evolved melt being more siliceous and decreasing the H2O content of the magma itself. The lower-crustal granulites commonly contain clinopyroxene; ascending H2O-rich magma from the mantle, therefore, might react with the clinopyroxene and fractionate amphibole as a residual phase. The MREE are preferentially partitioned into amphibole, with mineral–melt partition coefficients greater than one (Adam & Green, 1994; Sisson, 1994; Witt-Eickschen & Harte, 1994). Consequently, the evolved magma acquires a U-shaped REE pattern because of the buffering effect of residual amphibole. Partial melting experiments on lower-crustal materials under high-pressure conditions indicate that the resultant liquid has a felsic composition caused by the persistence of mafic minerals in the residue (e.g. Beard & Lofgren, 1991; Beard et al., 1993, 1994). Although amphibole fractionation processes in shallow magma chambers could also explain the U-shaped REE patterns, the occurrence of hornblende phenocrysts is rare and only very small amounts occur in felsic samples in the later volcanic stages (Table 1). This process is, therefore, unlikely to explain the overall U-shaped signature retained in the Akagi volcanic rocks. If the interaction between H2O-rich magma and lowercrustal material is a major process controlling the REE patterns of Akagi volcano, a process of ‘assimilation– fractional crystallization’ (AFC, DePaolo, 1981) under 2318 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Fig. 8. PM-normalized trace element patterns of plagioclase phenocrysts in Ol stage samples. Open and filled symbols indicate the rim and core of phenocrysts, respectively. lower-crustal conditions might be invoked. To examine the assimilation process in the lower crust, the AFC model (DePaolo, 1981) was applied to the isotope and trace element systematics in the Akagi volcano. In this model calculation, a primary magma deduced from ‘normal’ primary magma on the northern part of the volcanic front in the NE Japan arc, defined by Shibata & Nakamura (1997), is assumed as an ‘assimilator’. It is, however, difficult to determine the other parameters such as isotope and element ratios of assimilated material (hereafter denoted as ‘assimilant’) under Akagi volcano, and bulk partition coefficients between the melt and the assimilant. Thus, we fixed these parameters, and only evaluated the assimilation rate (r) as given by r = Ma(t)/Mc(t) (DePaolo, 1981) where Ma(t) and Mc(t) represent a rate (mass/unit time) of wallrock assimilation and a rate of fractionation of crystallizing phases, respectively. Thus, the assimilation rate implies the rate of contribution of masses controlled by the assimilation and the crystal fractionation to the total mass of magma. Furthermore, the assimilation rate is an essential parameter to evaluate the temperature conditions at which the AFC takes place. The averages of element ratios of lower-crustal materials compiled by Rudnick & Fountain (1995) are used for the assimilant. The isotopic compositions of the assimilant are obtained by the extrapolation of the linear correlations in the multi-isotope systematics of Akagi volcano. The bulk partition coefficients between magma and the assimilant were obtained by using the modal abundance of residual phases consisting of plagioclase, amphibole, clinopyroxene and orthopyroxene, as determined by hydrous melting experiments at lower-crustal conditions by Beard & Lofgren (1991). The REE signature of Akagi volcanic rocks indicates that amphibole fractionation was involved in the evolution of magma under lower-crustal conditions as discussed in the previous sections. All parameters used in the AFC calculations are compiled in Table 7. 2319 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Table 5: Isotopic analyses of phenocysts in Ol stage samples 87 Sample no. AK1108 AK1102 AK1201 AK1012 AK-A AK1010 AK0910 Sr/86Sr 143 Nd/144Nd Nd Pl 0·709051±10 0·512218±7 −8·19 Opx 0·708974±11 0·512195±7 −8·64 Hb 0·708919±10 0·512143±7 −9·66 Pl 0·708570±10 0·512191±16 −8·72 Opx 0·708228±9 0·512216±18 −8·23 Cpx 0·708221±7 0·512212±17 −8·31 Pl 0·707046±12 0·512422±12 −4·21 Opx 0·707267±13 0·512455±30 −3·57 Cpx 0·707310±10 0·512364±6 −5·34 Pl 0·707596±11 0·512401±9 −4·62 Opx 0·707275±13 0·512381±11 −5·01 Cpx 0·707375±9 0·512401±32 −4·62 Pl 0·707200±10 0·512371±10 −5·21 Opx 0·706833±9 0·512420±31 −4·25 Cpx 0·707245±11 0·512384±6 −4·95 Pl 0·708631±10 0·512139±12 −9·73 Opx 0·708790±20 0·512234±21 −7·88 Cpx 0·708786±26 0·512277±11 −7·04 Pl 0·707032±11 0·512434±11 −3·98 Opx 0·706928±9 0·512429±10 −4·08 Cpx 0·707086±39 0·512445±12 −3·76 Pl, plagioclase; Opx, orthopyroxene; Cpx, clinopyroxene; Hb, hornblende. Isotopic fractionation was normalized to 86Sr/ 88 Sr = 0·1194, 146Nd/144Nd = 0·7219. Analytical precisions for isotope data are 2 mean. Representative results from the AFC model calculations are presented together with data for Akagi, Adatara and other volcanoes from NE Japan in Fig. 11a–d. There appear to be correlations between isotope and element ratios in the arc data, although the correlation is poor for Pb isotopes, probably as a result of the small variation of Pb isotope compositions and the small differences between those of the lower crust and the primary magma. These correlations are obviously different from those of basaltic rocks elsewhere in the NE Japan arc and at Adatara volcano, for which the source heterogeneity and crystal fractionation processes have caused variations in isotope and elemental ratios without crustal assimilation (Shibata & Nakamura 1997). As shown in Fig. 11, most of the Akagi data plot near the mixing lines with an assimilation rate of 0·9, although those of the earliest and final stages tend to plot above the mixing lines with assimilation rates <0·9. This observation indicates that the extent of crustal assimilation relative to the crystallization in the middle stage is larger than in the earliest Fig. 9. Sr and Nd isotope systematics of phenocryst minerals in Ol stage samples. Data from the same sample are connected by tie-lines. The bulk-rock and calculated melt isotopic compositions (see text) are also shown. and latest stages of Akagi volcano. In the middle stage, therefore, the enrichment of incompatible elements together with isotope variations may largely have resulted from significant lower-crustal assimilation by primary magma similar to ‘normal’ basaltic magmas in the northern part of the volcanic front in the NE Japan arc. 2320 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Table 6: Calculated Sr and Nd compositions, and isotope compositions of melt part in Ol stage samples Sample no. Sr (ppm) 87 AK1108 323 AK1102 231 AK1201 Sr/86Sr Nd/144Nd Nd Nd (ppm) 143 0·70859 24·5 0·51220 −8·5 0·70770 29·5 0·51221 −8·3 360 0·70667 15·8 0·51244 −3·8 AK1012 246 0·70632 19·2 0·51239 −4·8 AK-A 199 0·70591 17·5 0·51243 −4·1 AK1010 327 0·70863 19·7 0·51223 −8·0 AK0910 278 0·70666 16·8 0·51243 −4·1 Phenocryst mode as in Table 1. Sr and Nd isotope compositions of whole rocks and phenocrysts as in Tables 3 and 5. Trace element compositions of whole rocks and phenocrysts as in Tables 2 and 4. Densities (in g/cm3): melt, 2·6; pl, 2·6; cpx and opx, 3·4; hb,3·0. When the assimilation rate is nearly 1·0, the latent heat of crystallization and the heat of fusion for the assimilation process are thermally balanced, approximately. Such a circumstance is likely to be achieved under lower-crustal conditions, because the geotherm in the lower crust is such that temperatures are 600–700°C, making it feasible to reach the solidus temperature of the assimilant by intrusion of magma and with less heat loss. On the other hand, the latent heat of crystallization could be mostly consumed by raising the temperature of the wallrock to its solidus, when assimilation occurs under shallower crustal conditions. Consequently, this results in an assimilation rate smaller than that occurring under lower-crustal conditions. From the above discussion based on the AFC model calculations, it may be concluded that the assimilation occurred primarily in the lowercrustal region, resulting in the unique isotope characteristics of the magmas of Akagi volcano. The seismologically determined Moho depth gradually increases from the northern part of NE Japan along the volcanic front, and it shows the maximum value beneath Akagi volcano (>38 km, >1·3 GPa), which is >4 km deeper than the typical depth beneath the volcanic front of the NE Japan arc (Zhao et al., 1992). Hildreth & Moorbath (1988) suggested that chemical interaction between magma and crust is closely related to the crustal thickness in the Andean arc. The thicker crust might effectively increase the assimilation rate, because the higher temperatures in the bottom of the crust mean that it more easily attains its solidus temperature. Consequently, volcanoes such as Akagi located on thicker crust might experience a larger effect of assimilation of lower crust on their trace element and isotope compositions. EXISTENCE OF A WATER-RICH MAGMA The above discussion based on isotope and trace element systematics requires a primary magma sufficiently enriched in H2O to stabilize amphibole in the lower crust. It is, therefore, essential to understand the mechanism whereby an H2O-rich source region for the primary magma in the mantle wedge beneath Akagi volcano could form. Fig. 10. Chondrite-normalized REE patterns for the TH and CA series of Akagi samples. The normalizing values are from McDonough & Sun (1995). The shaded area shows the range of REE patterns for the TH and CA series samples from Adatara volcano (Fujinawa, 1992). 2321 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Table 7: The parameters used for model calculation and the lower-crustal assimilation Element Plag. Kd∗ Cpx Kd† Opx Kd† Amph. Kd‡ Whole-rock Calc. melt composition§ composition (ppm) (ppm) La 0·15 0·04 0·008 0·16 8 35 Sr 3·1 0·12 0·018 0·50 348 297 11 Nd 0·12 0·19 0·030 0·77 Pb 0·39 0·10 0·015 0·40 4·2 32 12 (La/Nd)CH 1·40 2·10 (La/Sr)PM 0·71 3·65 (La/Pb)PM 0·51 0·78 ∗Calculated by the method of Bindeman et al. (1998); XAn = 0·57; T = 1173 K. †Green (1994). ‡Sisson et al. (1994), Kd for Pb is calculated by interpolation. § Average value of the lower crust by Rudnick & Fountain (1995). On the basis of petrological observations, quartz phenocrysts generally occur in felsic volcanic rocks without hydrous phenocrysts in the volcanic front of the NE Japan arc (Sakuyama, 1979). However, quartz does not appear as a phenocryst in Akagi samples, even in the felsic samples. Sakuyama (1979, 1983a, 1983b) determined the H2O content of magmas based on the crystallization sequence of phenocrysts. Following his definition, the Akagi volcanic rocks belong to Type II–III, which allows magmas to contain >3–4 wt % of H2O at >0·5 GPa. This suggests that the H2O content of the Akagi magmas is considerably higher than that of the Type I volcanoes, typical of the volcanic front in NE Japan, which contain <3 wt % of H2O. Yamaguchi (1990) inferred that the groundmass in the Akagi volcanic rocks has a significantly higher Al2O3 content than that of the adjacent Hotaka volcano. This is because the plagioclase stability field becomes narrower relative to the diopside stability field with increasing H2O content in the magma. This observation is also consistent with the hypothesis that the primary magma of Akagi is enriched in H2O relative to other volcanoes in the volcanic front in NE Japan. The peculiar petrological and geochemical characteristics of Akagi volcano discussed above might be explained by the development of the unusual tectonic setting beneath Akagi volcanic area, where the Philippine Sea plate overlaps onto the Pacific plate. Such a tectonic setting might lead to a significantly larger amount of water in the magma source region than that expected from subduction of a single Pacific plate. EVOLUTION OF MAGMA IN THE Ol STAGE Recently, magma mixing at Akagi has been discussed, on the basis of the major element composition of phenocrysts and their textures, in the pumice from the Y stage, by Horio & Umino (1995) and Umino & Horio (1998). Those workers have suggested that high-T, less fractionated magma was periodically injected into a low-T, silicic, mushy magma in a shallow magma chamber. However, previous studies have not addressed the origin of these two different magmas because of the limited geochemical information available, especially isotope compositions, for Akagi volcano. On the basis of the major element compositions of pyroxenes, the temperatures of the magmas in the Ol stage were determined by using the QUILF program of Andersen et al. (1993). Average compositions of the rims of clinopyroxene and orthopyroxene were used for the temperature estimation. Ferric–ferrous ratios were calculated to satisfy the stoichiometry of the pyroxenes. The samples investigated from the Ol stage can be divided into high-T (1000–1200°C) and low-T (<1000°C) groups, and tend to have a negative correlation between calculated temperature and Sr isotopic composition (Table 8 and Fig. 12). This indicates that such a variation in magma temperatures is not a consequence of the simple cooling process in the shallow magma chamber. In the Ol samples, melts are isotopically more depleted than the coexisting phenocrysts (Fig. 9) as discussed in the previous section. Such isotopic disequilibrium observed could be explained only by a mechanical mixing 2322 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Fig. 11. Trajectories of AFC model calculation for Akagi volcanic rocks. The parameter r = Ma(t)/Mc(t) is defined as the assimilation rate, and the numbers on the trajectories show the proportion of remaining magma (Mm/Mm0) defined by DePaolo (1981). The variation of trace element ratios of Adatara volcano are calculated from Fujinawa (1992), and the Nd and Sr isotopic compositions are based on unpublished data. The other parameters are compiled in Table 7. In the case where the assimilation rate is small (r = 0·2), the concentration ratios increase rapidly without large isotopic differences. When the assimilation and fractionation are nearly balanced (r = 0·9), the trajectories appear to explain moderately well the variation observed in the Akagi volcanic rocks. between the isotopically enriched magma equilibrated with the phenocrysts and the relatively depleted aphyric magma. Mass-balance calculations, based on the trace element composition and modal abundance of the phenocrysts, indicate that the Sr/Nd ratio in the glass of the phenocryst-rich rock is lower than that in the aphyricprimary magma as a result of the equilibration of phenocrysts, especially plagioclase. If the aphyric-primary magma has a more depleted isotopic signature than the phenocryst-rich magma, the mixing curve forms a convex hyperbola in the Sr and Nd isotope diagram (Fig. 13a). That is, the Sr isotopic compositions of glasses are characteristically more depleted than those of the coexisting phenocrysts. However, the difference in Nd isotopic composition between them is smaller than the difference in Sr isotopic composition. These observations, together with model mixing, may suggest that the involvement of depleted aphyric magma mixed with phenocryst-rich magma was relatively small, and that isotopic re-equilibration among the phenocrysts and the mixed melt has not been achieved. To examine the above argument further, a model calculation was carried out using the samples with remarkable isotope disequilibrium in Sr between melt and phenocrysts (AK1012 and AK1102) representing the high-T and the low-T group, respectively. The results are presented in Fig. 13b, based on the parameters given in Table 9. In this model, the isotope and trace element compositions of the primary aphyric magma are assumed to be those of the primary basaltic magma (a depleted end-member, Pm) in the volcanic front of NE Japan (Shibata & Nakamura, 1997). The isotopic compositions of two end-members (Fm1 and Fm2) are represented by the values of the most enriched phenocrysts in AK1012 2323 JOURNAL OF PETROLOGY VOLUME 42 Table 8: Magmatic temperatures obtained for Ol stage samples at 1 atm and 2 kbar Sample no. 1 atm 2 kbar T (°C) T (°C) AK1108 808∗ 814∗ AK1102 931±21 938±23 AK0910 1196±11 1206±10 AK1012 1069±20 1076±22 AK1201 1038±19 1045±21 AK-A 1068±12 1076±14 AK1010 1005±12 1012±14 ∗Error not determined. and AK1102, assuming that the phenocrysts in the enriched end-members were isotopically equilibrated with their host melts, when the phenocrysts crystallized. The Sr and Nd abundances in Fm1 and Fm2 were obtained by the subtraction of phenocryst compositions from the whole rock of the most mafic sample AK0910 in the Ol stage. In this model, clinopyroxene and opaque phenocrysts are not considered. Because the Kd values of Sr and Nd for clinopyroxene are almost identical (Green, 1994), and because of the extremely low concentrations NUMBER 12 DECEMBER 2001 of these elements in the opaque minerals, very little change in Sr/Nd is produced. The amounts of phenocrysts subtracted are assumed to be 30 wt % of plagioclase for Fm1, and 40 wt % of plagioclase and 10 wt % of hornblende for Fm2. After subtraction of the phenocrysts, the resulting major element compositions are similar to the whole-rock composition of the examined samples, AK1012 and AK1102, except for Mg and Fe (e.g. calculated CSiO2Fm1 = 55·8, CSiO2Fm2 = 59·2 wt %, and the whole rocks 56·4 and 59·5 wt %, respectively). In Fig. 13b, the calculated isotopic compositions of melts in AK1012 and AK1102 are plotted near the fractions of 0·25 (Mm1) and 0·12 (Mm2) of the Pm component on the mixing curves 1 and 2, respectively. The Sr isotopic compositions show significantly more depleted signatures than those of the whole rocks with less variation in Nd isotopic composition. This is consistent with the observation that the Sr isotopic compositions of most of the glasses are characteristically more depleted than those of the whole rocks and their constituent phenocryst minerals. As shown in Fig. 9, the differences in both Sr and Nd isotopic compositions between glasses and phenocrysts are variable from sample to sample. This may be attributed to the extent of mixing of the depleted aphyric magma with the enriched porphyritic magma and/or to the residence time after mixing in the magma chamber, or to the evolution of the primary magma by reaction with lower-crustal materials. Although reverse zoning of pyroxenes is believed to be evidence of magma mixing (i.e. Sakuyama 1979, Fig. 12. Magmatic temperature vs Sr isotopic composition of whole rock, clinopyroxene and orthopyroxene phenocrysts in the Ol stage. The magmatic temperature is determined using the QUILF program (Andersen et al., 1993). 2324 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Fig. 13. (a) Schematic illustration, in a Sr–Nd isotope diagram, of two-component mixing (after DePaolo & Wasserburg, 1979). K, Sr/Nd ratio in component A relative to component B; F, fraction of component A in product magma. (b) Model calculation of mixing between the aphyric, isotopically depleted melt (Pm) and the isotopically enriched melts (Fm1, Fm2). The chemical parameters are summarized in Table 9. The numbers beside each curve represent the weight fraction of Pm in the mixed melt. The mixing trajectories are concave hyperbolae, and the K values of Curve 1 and Curve 2 are 3·8 and 3·4, respectively. A relatively small amount of injection of the isotopically depleted primitive magma (Pm) can produce the depleted melt part for Sr isotopes (Mm1 and Mm2) as a result of the mixing. 1981), such a signature was not observed in the sample belonging to the high-T group, AK1012. If the depleted primary magma (Pm), derived from a strongly metasomatized wedge mantle as a result of the double subduction, is less affected by assimilation processes in the lower crust, the mode of phenocrysts could be smaller than for anhydrous magma under the same temperature conditions. This is because the liquidus temperature falls with increasing H2O contents in melt (e.g. >1100°C at >3 wt % H2O; Baker & Eggler, 1983). It may, therefore, be reasonable that a depleted primary magma enriched in water can cool without crystallization to a temperature 2325 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Table 9: The compositions assumed for the end-member components in the mixing calculation End-member Pm Fm1 Fm2 Mm1 Mm2 Sr (ppm) 290 230 160 245 173 87 Sr/86Sr 0·70430 Nd (ppm) 4·6 143 0·51282 Nd/144Nd Nd Sr/Nd 3·6 63 0·7072 0·70857 13·9 8·5 0·51236 0·51219 0·7063 11·6 0·5124 0·7077 8·0 0·5122 −5·5 −8·7 −4·5 −7·9 16·5 18·8 21·2 21·9 similar to that of the isotopically enriched end-member (Fm1) of the high-T group. This consequently reduces the temperature difference between the aphyric-depleted and the enriched magma, making it difficult to form reverse zoning in pyroxenes. On the other hand, the low-T group represented by AK1102 commonly contains pyroxenes with reverse zoning and hornblendes surrounded by pyroxene reaction rims. Under low-pressure conditions, the hornblende stability field is sensitive to magmatic temperature, and it dissociates to form crystal aggregates of pyroxene and melts above >900–1000°C (Boettcher, 1977). Thus, the occurrence of both reaction rims in hornblende and reverse zoning of pyroxenes also indicates that the temperature of the enriched endmember (Fm2) was significantly lower than that for Pm and Fm1. Furthermore, the temperature of Fm2 was raised by mixing with Pm. It is, however, difficult to produce Fm2 directly from Fm1 by simple cooling processes associated with fractional crystallization in a shallow magma chamber, because of the significant difference in isotopic composition between them (Fig. 12). It is more likely that the high-T and low-T magmas behaved independently in the shallow region through the Ol stage. The temperature and isotopic differences between the high-T and low-T magmas could have depended on the difference in the degree of assimilation in the lower crust, before their migration into the shallow magma chamber. On the other hand, it may be possible to produce a highT magma from a low-T magma, when a single magma batch such as low-temperature Fm2 is repeatedly injected by a ‘hotter’ primary magma (Pm) in the shallow magma chamber, resulting in rising magmatic temperature and increasing isotopic depletion. However, a relatively large discontinuity in isotopic composition and magmatic temperature exists between the high-T and low-T groups (Fig. 12), indicating that two enriched magma reservoirs have been involved in the formation of the Ol stage magmas. The relatively small variations of isotopic compositions and temperature in each group may have been caused by more complicated processes such as repeated injections of relatively small amounts of new hot magma into the enriched reservoirs in the shallow magma chamber. It may be concluded that the isotopic variations and disequilibrium between glass and coexisting phenocrysts in the Ol stage were caused by two-component mixing of relatively depleted aphyric magma and enriched phenocryst-rich magma in the shallow magma chamber. These two magmas evolved independently in the lower crust before their mixing. This model is, therefore, different from that for the generation of calc-alkaline series magmas proposed by Sakuyama (1979, 1981), in which the original and its fractionated daughter magmas are mixed, so that isotopic variations are not expected. Our model is rather similar to the models of Eichelberger (1978) and Takahashi (1986) based on petrological arguments, proposing a mixing of magma derived from the mantle and a partially fused lower crust. TEMPORAL ISOTOPIC VARIATION OF AKAGI VOLCANO The isotope signatures changed temporally during the activity of Akagi volcano. The early stage volcanic rocks are isotopically most depleted and the final stage becomes depleted again, whereas the middle stage has more enriched signatures (Fig. 14). These temporal variations are probably attributable to the evolution of the interface (wall rock) between lower crust and the magma derived from the mantle wedge beneath Akagi. When magma starts to intrude into the lower crust, the margins of the magma conduit could be chilled as a result of the significant temperature difference between the basaltic magma and the lower crust. This could have led to less interaction between the lower crust and the magma or less assimilation by the magma resulting in a relatively depleted isotopic signature at the early stage of Akagi volcano. Repeated injection of magma should raise the temperature of the wall rock near the magma conduit and exceed the solidus temperatures of the surrounding wall-rock materials in the lower crust. Thus, the volcanic 2326 KOBAYASHI AND NAKAMURA EVOLUTION OF AKAGI VOLCANO Fig. 14. Temporal variation of Sr, Nd and Pb isotopic compositions in the Akagi volcano. rocks of the middle stage could have acquired the relatively enriched isotopic signature by lower-crustal assimilation relative to magmas of the early stage (Fig. 14). In addition to the thermal evolution of the wall rock in the lower crust, the interface between the magma and the lower crust may have compositionally evolved, as a result of the solidification of magma and the formation of amphibole by the reaction between a water-rich primary magma and pyroxene in the lower crust (see discussion in previous section). Such an evolved interface could act as an insulator that would prevent interaction between the lower crust and the magma. Therefore, the isotope signature in the final stage would become similar to that of the early stage, with depleted isotope characteristics relative to the middle stages (Fig. 14). CONCLUSIONS The evolution of magma to form Akagi volcano is schematically summarized in Fig. 15. The major element compositions and the phenocryst assemblages of Akagi volcano indicate that water content in the magma is significantly higher than that of other volcanoes in the volcanic front in the NE Japan arc. This may be attributed to the unique geometry of subduction beneath Akagi volcano. The Philippine Sea plate subducts into the mantle wedge above the downgoing Pacific plate underneath Akagi. Such double subduction of the oceanic plates should provide a larger amount of water as a result of the dehydration of hydrous minerals in the slabs, to be contributed to the source region of magmas for Akagi volcano, than in the case of single subduction of the Pacific plate, which produced other volcanoes in the volcanic front in NE Japan. On the other hand, multi-isotope and trace element systematics of Akagi volcano clearly require interaction between the water-rich magma and the lower crust along with amphibole fractionation. Such assimilation– fractional crystallization in the lower crust may largely have been induced by a fall in the solidus temperature of the lower crust as a result of the higher water content in the primary magma of this volcano relative to that of other volcanoes in the volcanic front. The AFC model calculation suggests that the latent heat of crystallization and the heat of fusion for the wall rock were nearly balanced in the lower crust, implying that assimilation proceeded easily because of the high temperature in the lower crust and the high water content in the magma. Isotope disequilibrium was observed between phenocrysts formed in the shallow magma chamber and the coexisting melts. Furthermore, the apparent magma temperatures correlate with Sr isotope compositions but to a lesser extent with Nd isotope compositions. These observations suggest that at least two recognizable and distinct magmas, which had been separately evolving in the lower crust, existed in the shallow magma chamber in a single stage. Then, the magmas were mixed independently with injections of isotopically depleted aphyric magmas. Although the other stages were not examined for phenocryst geochemistry in this study, it may be also possible, on the contrary, that the depleted magma is mixed by the injection of enriched magma. Such a difference should be attributable to the residence time of magma, and the evolution of the interface between the magma and the wall rock in the lower crust. Therefore, we conclude that the evolution of Akagi volcano has been strongly controlled by the assimilation process in the lower crust induced by the water-rich magma compositions. 2327 JOURNAL OF PETROLOGY VOLUME 42 NUMBER 12 DECEMBER 2001 Fig. 15. Schematic representation of the magma differentiation process, including assimilation and amphibole fractionation by water-rich magma in the lower crust under Akagi volcano. Overlapping of the Pacific and Philippine Sea plates may be an important mechanism for supplying fluid to form the H2O-rich primary magmas. Finally, fractional crystallization and repeated magma mixing processes in a shallow magma chamber produced the various geochemical characteristics of the Akagi volcanic rocks. As mentioned repeatedly in this paper, a primary factor in enhancing assimilation in the lower crust is the higher water content in the primary magma than that in magmas producing the surrounding volcanoes in the volcanic front. If this is the case, the along-arc Sr isotope variation, which decreases on either side of the ‘unique’ Akagi volcano in the volcanic front, may indicate a decrease in the extent of assimilation in the lower crust as a result of a decrease in the water content of the primary magmas. This may be due to the location of Akagi volcano, which stands above the top of a ‘tongue’ of the Philippine Sea plate. The position of this feature is shown by the isodepths to the subducting plate in Fig. 1. This would further increase the water content in the source region of the primary magma by the dehydration of the Philippine Sea plate, in addition to the water from the Pacific plate. If this is true, it may be possible to more clearly deduce the extent of the Philippine Sea plate in the mantle wedge of the Pacific plate and the role of water in the generation of island-arc magmas by extending detailed trace element and multi-isotope systematics to the volcanoes in central Japan as has been performed for Akagi volcano in this study. ACKNOWLEDGEMENTS We thank T. Shibata, M. Yoshikawa and A. Makishima for their technical help in isotopic analyses and ICP-MS analysis. Thanks are also due to our many colleagues with whom we have discussed various issues during the course of this study. We are deeply indebted to Professor I. Kushiro for his encouragement. Professor I. Moriya is also sincerely thanked for geological information on the study area. Dr G. E. Bebout is also acknowledged for improving the manuscript. 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