SUPPLEMENTARY INFORMATION

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1 SUPPLEMENTARY INFORMATION DOI: /NGEO1250 Intensive hydration of the mantle transition zone beneath China caused by ancient slab stagnation Takeshi Kuritani 1,2 *, Eiji Ohtani 1, and Jun-Ichi Kimura 3 1 Department of Earth and Planetary Materials Science, Graduate School of Science, Tohoku University, Sendai , Japan 2 Division of Biology and Geosciences, Graduate School of Science, Osaka City University, Osaka , Japan 2 Institute for Frontier Research on Earth Evolution, Japan Agency for Marine-Earth Science and Technology, Yokosuka , Japan Supplementary Figure S1 Supplementary Figure S2 Supplementary Figure S3 Supplementary Figure S4 Supplementary Figure S5 Supplementary Figure S6 Supplementary Notes Supplementary References Supplementary Table S1 Supplementary Table S2 *Corresponding author: kuritani@sci.osaka-cu.ac.jp NATURE GEOSCIENCE 1

2 SUPPLEMENTARY FIGURE S1 Figure S1: Whole-rock major element compositions of late Cenozoic basaltic lavas from northeast China. The data are from refs 10, 11, 13, and 31 35, and from this study (Table S1). The classification of rock types was taken from ref

3 SUPPLEMENTARY FIGURE S2 Figure S2: Primitive mantle normalized multi-element concentration diagram for representative lavas from the studied volcanic areas. Significant positive anomalies of Ba, Pb, and Sr are observed. The data are from refs 11, 31, 32, and 34, and from this study (Table S1). Trace element concentrations of primitive mantle are taken from ref

4 SUPPLEMENTARY FIGURE S3 Figure S3: Sr and Nd isotopic compositions of basalts from some of the studied areas shown in a 86 Sr/ 87 Sr versus 143 Nd/ 144 Nd diagram. Quaternary samples are shown with filled circles and Tertiary samples (<10 Ma) and samples of unknown ages are shown with open circles. The data are from refs 11, 13, 32, 34, and 35, and from this study (Table S1). The compositional fields of EM1 and Indian MORB are from ref. 38. Isotopic compositions of Japan Sea basalts, shown with open crosses, are from ref

5 SUPPLEMENTARY FIGURE S4 Figure S4: Compositions of basaltic lavas from the studied volcanic areas. (a) Ba/Th versus SiO 2 diagram. (b) 87 Sr/ 86 Sr versus SiO 2 diagram. (c) SiO 2 versus distance (from Tianchi Volcano) diagram. For clarity, only Quaternary lavas are shown. The symbols for the data are the same as those used in Fig. S1. The samples with significant Eu anomaly (Eu*>1.1 or Eu*<0.9) are not plotted in (a) and (c). The data are from refs 10, 11, 13, 31, 34, and 35, and from this study (Table S1). It is noteworthy that the whole-rock SiO 2 content of the lavas do not show significant spatial variation and the Ba/Th and 87 Sr/ 86 Sr ratios do not vary significantly with increasing SiO 2 content in each volcanic area (except for Kuandian samples). In addition, the Ba/Th and 87 Sr/ 86 Sr ratios show significant spatial variations in Figs. S4a and S4b. These observations suggest that the geochemical features of lavas are not significantly affected by crustal contamination, and that the spatial geochemical variations shown in Figs. 3, 4, and S3 primarily represent a real variation in the ratios in the source mantle. 5

6 SUPPLEMENTARY FIGURE S5 Figure S5: Compositions of basalts from the studied areas, along with those of Gaussberg lamproites, plotted in a Ba/La versus Ba/Th diagram. For northeast China basalts, only Quaternary samples are shown. The compositions of sediment (K-hollandite) and depleted mantle (DM) are taken from ref. 23. The data of Gaussberg lamproites are from ref. 15 and those of northeast China lavas are from refs 10, 11, 13, 31, 34, and 35, and from this study (Table S1). 6

7 SUPPLEMENTARY FIGURE S6 Figure S6: Sr, Nd, and Pb isotopic compositions of basalts from the studied area, along with those of three possible end-member components. Quaternary samples are shown with filled circles and Tertiary samples (<10 Ma) and samples of unknown ages are shown with open circles. Large open circles indicate the compositions of the three end-member components. The tie line between the two sediment components is annotated with the percentage of the ancient sediment component. Dashed lines represent equal percentages of the mixture sediment component (i.e., consisting of the ancient and recent sediment components) added to the DM component. It is noteworthy that most of the data are within the fields formed by the three end-member components, although a few samples are not in (b) and (d). Gray areas show the compositional areas of pelagic sediments 24. For the DM (depleted mantle) component, the elemental 7

8 concentrations of ref. 39 and the Sr and Pb isotopic compositions of the least radiogenic Japan Sea basalts 30 are assumed. The Nd isotopic composition of the component is determined using the Sr isotopic composition of the component 30 and the correlation between the Sr and Nd isotopic compositions of the global MORB data 39. The elemental concentrations and the Sr and Nd isotopic compositions of the recent sediment component are assumed to be those of Pacific sediments 18. For lead isotopic compositions, slightly more radiogenic compositions than the Pacific sediments of ref. 18, which are within the compositional area of pelagic sediments 24, are assumed. The elemental concentrations of the ancient (1.5 Ga) sediment component are assumed to be similar to those of the recent sediment component 18. The present-day Sr and Nd isotopic compositions of this component are taken from ref. 17. The method to determine the present-day Pb isotopic compositions of the 1.5-Ga sediment component is essentially similar to that in ref. 17. However, in the second-stage evolution of the Stacey Kramers model 29, = 9.9 and = 4.1 are assumed, instead of = 9.7 and = 3.8, so that the present-day compositions coincide with those of the recent sediment component. After 1.5 Ga ago, the lead isotopic compositions are assumed to evolve with = 2.0 and = 6.3 according to ref. 17. Present-day lead isotopic compositions of continental crust-derived sediments shown in Fig. 4 (1.5 0 Ga ago) were calculated by the same procedure. The elemental concentrations and isotopic compositions of the three components are listed in Table S2. These compositions have large uncertainties, because we do not consider the elemental fractionation in sediments during subduction processes, and the age of the ancient sediment component is also unknown. However, the composition of Changbaishan lavas can be consistently explained by ~0.5% sediments that consist of ~60% of the ancient sediment component. The data of lavas are from refs 11, 13, 32, 34, and 35, and from this study (Table S1). 8

9 SUPPLEMENTARY NOTES The data source for Fig. 3 The data are from refs 10, 11, 13, and 31-35, and from this study (Table S1). The data source for Fig. 4 The data are from refs 11, 13, 34, and 35, and from this study (Table S1). Unpublished data In this study, four unpublished data of basaltic lavas from the Longgang volcanic field are used. The data are listed in Table S1. The analytical methods are the same as those described in ref

10 SUPPLEMENTARY REFERENCES 31. Liu, C.-Q., Masuda, A. & Xie, G.-H. Major- and trace-element compositions of Cenozoic basalts in eastern China: petrogenesis and mantle source. Chem. Geol. 114, (1994). 32. Hsu, C.-N., Chen, J.-C. & Ho, K.-S. Geochemistry of Cenozoic volcanic rocks from Kirin Province, northeast China. Geochem. J. 34, (2000). 33. Chen, J.-C., Hsu, C.-N. & Ho, K.-S. Geochemistry of Cenozoic volcanic rocks and related ultramafic xenoliths from the Jilin and Heilongjiang provinces, northeast China. J. Asian Earth Sci. 21, (2003). 34. Zou, H., Fan, Q. & Yao, Y. U Th systematic of dispersed young volcanoes in NE China: asthenosphere upwelling caused by pilling up and upward thickening of stagnant Pacific slab. Chem. Geol. 255, (2008). 35. Yan, J. & Zhao, J.-X. Cenozoic alkali basalts from Jingpohu, NE China: the role of lithosphere asthenosphere interaction. J. Asian Earth Sci. 33, (2008). 36. Le Bas, M. J., Le Maitre, R. W., Streckeisen, A. & Zanettin, B. A chemical classification of volcanic rocks based on the total alkalis-silica diagram. J. Petrol. 27, (1986). 37. Sun, S.-S. & McDonough, W. F. in Magmatism in the Ocean Basins (eds. Saunders, A. D. & Norry, M. J.) (Vol. 42 of Spec. Pub, Geol. Soc. London, 1989). 38. Hofmann, A. W. in The Mantle and Core (ed. Carlson, R. W.) (Vol. 2 of Treatise on Geochem., Elsevier-Pergamon, 2005). 39. Workman, R. K. & Hart, S. R. Major and trace element composition of the depleted MORB mantle (DMM). Earth Planet. Sci.Lett. 231, (2005). 10

11 SUPPLEMENTARY TABLE S1 Volcanic field Changbaishan Sample name 92P01 92P02 92P03 92CW19 92CW20 92CW21 92CW22 92CW23 92CW24 CBS-1b CBS-6a Reference ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 10 ref. 10 Distance, km Age SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

12 Volcanic field Changbaishan Sample name CBS-10a CBS-15a CBS-19a CBS-21a CBS-22a HAKU01a HAKU01b HAKU02 HAKU03 HAKU04 HAKU05 Reference ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 Distance, km Age Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

13 Volcanic field Changbaishan Sample name HAKU09 HAKU10 HAKU20 HAKU25 HAKU26 HAKU27 HAKU29 HAKU30a HAKU30b HAKU32a HAKU32b Reference ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 ref. 11 Distance, km Age Quaternary Quaternary 3.1 Ma 3.2 Ma Quaternary 2.7 Ma Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li Rb Sr Y Zr Nb Cs Ba 725 1, ,091 La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Hf Ta Pb Th U Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

14 Volcanic field Changbaishan Zengfengshan Sample name HAKU34 HAKU35 HAKU36 92CW08 92CW09 92CW13 92CW14 92CW15 92CW16 92CW17 Reference ref. 11 ref. 11 ref. 11 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 Distance, km Age Quaternary 4.2 Ma Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

15 Volcanic field Zengfengshan Longgang Sample name CBS-24a CBS-25A 92CW25 92CW26 92CW27 LG02 LG06 LG07 Reference ref. 10 ref. 10 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 33 ref. 33 ref. 33 Distance, km Age SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

16 Volcanic field Longgang Sample name LG08 LG09 LG12 LG13-1 LG17 LG18 LG19 LG20 LG21 LG-1c LG-DLW-1w Reference ref. 33 ref. 33 ref. 33 ref. 33 ref. 33 ref. 33 ref. 33 ref. 33 ref. 33 ref. 10 ref. 10 Distance, km Age Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

17 Volcanic field Longgang Sample name LG-DLW-1p LG-DLW-1aa LG-1a LG-2a LG-3a Lg-4a LG-5b LG-6a LG-6a LG-7b LG9940 Reference ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 34 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li Rb 56 Sr Y Zr Nb Cs Ba La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm 0.25 Yb 1.94 Lu 0.29 Hf Ta Pb 4.39 Th U Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U 3.4 Eu*

18 Volcanic field Longgang Wangqing Sample name LG99L11-1 HJ97001A HJ97034 HJ97044 HAKU39 HAKU40 HAKU42 HAKU45 WQ72 WQ77 Reference ref. 34 ref. 34 ref. 34 ref. 34 This study This study This study This study ref. 31 ref. 31 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

19 Volcanic field Wangqing Jingbohu Sample name WQ84 91WQ1-1 91WQ2-1 91WQ2-3 91WQ2-4 91WQ3-1 91WQ4 91WQ5-1 J01 J02 Reference ref. 31 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 32 ref. 33 ref. 33 Distance, km Age Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li Rb Sr Y Zr Nb Cs Ba La Ce Pr Nd Sm Eu Gd 6.17 Tb Dy 4.8 Ho Er 2.36 Tm Yb Lu Hf Ta Pb Th U Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

20 Volcanic field Jingbohu Sample name J03 J04 J05 J06 JBH-BH-1a JBH-BH-1g JBH-BH-1u JBH-BH-1af JBH-3a JBH-3c JBH-3d Reference ref. 33 ref. 33 ref. 33 ref. 33 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

21 Volcanic field Jingbohu Sample name JBH-1a JBH-2a JBH-3a JBH-3a JBH-4a JBH-5a JBH-6a JBH-7a JBH-8a JBH-HMT-1a JBH-HMT- 2a Reference ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li Rb Sr Y Zr Nb Cs 0.4 Ba La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm 0.26 Yb Lu Hf Ta Pb Th U Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

22 Volcanic field Sample name Jingbohu JBH-HMT- 3a JBH-10a J J J J J J JB11-11 JB-1 JB-2 Reference ref. 10 ref. 10 ref. 34 ref. 34 ref. 34 ref. 34 ref. 34 ref. 34 ref. 34 ref. 35 ref. 35 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

23 Volcanic field Jingbohu Sample name JB-5 JB-7 JB-8 JB-9 JB-11 JB-12 JB-14 JB-15 JB-16A JB-16B JB-17 Reference ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

24 Volcanic field Jingbohu Sample name JB-18 JB-19 JB-20 JB-21 JB-22 JB-23 JB-24 JB-25 JB-26 JB-27 Reference ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 ref. 35 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Miocene Miocene Miocene SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

25 Volcanic field Mudanjiang Sample name BNE1 M37 M38 M43 M45 M55 M62 M64 MDJ-1a MDJ-1a MDJ-2a Reference ref. 31 ref. 31 ref. 31 ref. 31 ref. 31 ref. 31 ref. 31 ref. 31 ref. 10 ref. 10 ref. 10 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li Rb Sr Y Zr Nb Cs 0.6 Ba La Ce Pr Nd Sm Eu Gd Tb Dy Ho Er Tm 0.31 Yb Lu Hf Ta Pb Th U Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

26 Volcanic field Mudanjiang Kuandian Sample name MDJ-3a MDJ-4a MDJ-5a MDJ-6a MDJ-7a BC5-2 BC4-1 BC3-1 BC2-4 BC1-4 Reference ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 13 ref. 13 ref. 13 ref. 13 ref. 13 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

27 Volcanic field Kuandian Sample name KB1 KB2 KB3 KB4 KB5 KD-HY-1d KD-HY-2a KD-HY-3a KD-HY-3b KD-HY-4a KD-HY-4d Reference ref. 31 ref. 31 ref. 31 ref. 31 ref. 31 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 ref. 10 Distance, km Age Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary Quaternary SiO TiO Al2O Fe2O FeO MnO MgO CaO Na2O K2O P2O LOI Total Li 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 Sr/ Sr Nd/ Nd Pb/ Pb Pb/ Pb Pb/ Pb Ba/Th Pb/U Eu*

Supplementary Figure 1 Map of the study area Sample locations and main physiographic features of the study area. Contour interval is 200m (a) and 40m

Supplementary Figure 1 Map of the study area Sample locations and main physiographic features of the study area. Contour interval is 200m (a) and 40m (b). Dashed lines represent the two successive ridge