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E Avasimibe site between IC1 and IC4 is the prominence of hydrogenous nO2 precipitation that uptakes Ce preferentially via oxidation of Ce (III) to Ce (IV), which might be attributed to the variation in concentration of dissolved Fe and Mn, including colloids, in water masses36,45,46; the regional variation in supply of teeth/bone debris of marine vertebrates to the sediment; or differences in the sedimentation rate which may affect accumulation of the hydrogenous component. In addition, an increase in the depositional flux of biogenic Ca-phosphate likely coincided with an increased supply of organic matter to the seafloor, although the sedimentation rate was likely held at a sufficiently lower level than those of calcareous/siliceous ooze and near-shore Necrosulfonamide site terrigenous detrital sediment. The increased deposition of organic matter might have caused relatively oxygen-poor (suboxic) conditions near the sediment surface and enhancement of the geochemical interactions between sediments and ferromanganese nodules during early diagenetic processes17,47, which partially explains the geographical overlap of REY-controlling IC signals and ferromanganese nodules on the seafloor. As the next step, ICA on a higher dimensional dataset including various transition metals involved in ferromanganese nodules, such as Co, Ni, Cu, and Zn, would likely extract another characteristic signature of the geochemical processes. On the basis of the statistical analysis of the integrated dataset, we can also deduce regional features from a global perspective. Among all of the samples analysed in the present study, the highest concentration of REY, 2,800 ppm, occurred at DSDP Site 596 in the central South Pacific Ocean. Site 596 is one of a few sites where the sediment column of pelagic clay throughout the Cenozoic was recovered almost completely. The downhole variation of total REY contents in bulk sediments at the comparable Site U13658 drilled during Integrated Ocean Drilling Program Expedition 329 shows the essentially same profile. At Site 596, IC1-type REY-rich mud containing >2,000 ppm of REY plus Ce was deposited during the Palaeogene (i.e. 66 to 23 Ma; Fig. 5a). In a previous work48, temporal variations in the relative mass fractions of inferred sediment end-member components at Site 596 were calculated by using the total inversion method. The profile of our IC1 scores at Site 596 almost correlates with both the calculated hydrogenous and phosphate components (Fig. 5b ). This confirms that the commingled accumulation of these two components18 extracted as IC1 generated the very high-grade REY-rich mud in the South Pacific during the Palaeogene. The occurrence of such mud might be explained by the absence of the major source of terrigenous aeolian dust and volcanic ashes that represent a significant fraction of pelagicScientific RepoRts | 6:29603 | DOI: 10.1038/srepDiscussionwww.nature.com/scientificreports/Figure 5. Temporal variations of REY content, IC1 score, and inferred relative mass fractions of sediment end-member components48 at Deep Sea Drilling Project (DSDP) Site 596, central South Pacific. (a) Bulk REY plus Ce contents and (b) IC1 scores (this study). (c) Hydrogenous, (d) phosphate, and (e) detrital (sum of aeolian dust and andesitic materials from magmatic arc) components calculated by using the total inversion method48. Age was determined on the basis of a constant Co-flux model48. (f) Geographical relationship between the Australian continent and DSDP Site 5.E between IC1 and IC4 is the prominence of hydrogenous nO2 precipitation that uptakes Ce preferentially via oxidation of Ce (III) to Ce (IV), which might be attributed to the variation in concentration of dissolved Fe and Mn, including colloids, in water masses36,45,46; the regional variation in supply of teeth/bone debris of marine vertebrates to the sediment; or differences in the sedimentation rate which may affect accumulation of the hydrogenous component. In addition, an increase in the depositional flux of biogenic Ca-phosphate likely coincided with an increased supply of organic matter to the seafloor, although the sedimentation rate was likely held at a sufficiently lower level than those of calcareous/siliceous ooze and near-shore terrigenous detrital sediment. The increased deposition of organic matter might have caused relatively oxygen-poor (suboxic) conditions near the sediment surface and enhancement of the geochemical interactions between sediments and ferromanganese nodules during early diagenetic processes17,47, which partially explains the geographical overlap of REY-controlling IC signals and ferromanganese nodules on the seafloor. As the next step, ICA on a higher dimensional dataset including various transition metals involved in ferromanganese nodules, such as Co, Ni, Cu, and Zn, would likely extract another characteristic signature of the geochemical processes. On the basis of the statistical analysis of the integrated dataset, we can also deduce regional features from a global perspective. Among all of the samples analysed in the present study, the highest concentration of REY, 2,800 ppm, occurred at DSDP Site 596 in the central South Pacific Ocean. Site 596 is one of a few sites where the sediment column of pelagic clay throughout the Cenozoic was recovered almost completely. The downhole variation of total REY contents in bulk sediments at the comparable Site U13658 drilled during Integrated Ocean Drilling Program Expedition 329 shows the essentially same profile. At Site 596, IC1-type REY-rich mud containing >2,000 ppm of REY plus Ce was deposited during the Palaeogene (i.e. 66 to 23 Ma; Fig. 5a). In a previous work48, temporal variations in the relative mass fractions of inferred sediment end-member components at Site 596 were calculated by using the total inversion method. The profile of our IC1 scores at Site 596 almost correlates with both the calculated hydrogenous and phosphate components (Fig. 5b ). This confirms that the commingled accumulation of these two components18 extracted as IC1 generated the very high-grade REY-rich mud in the South Pacific during the Palaeogene. The occurrence of such mud might be explained by the absence of the major source of terrigenous aeolian dust and volcanic ashes that represent a significant fraction of pelagicScientific RepoRts | 6:29603 | DOI: 10.1038/srepDiscussionwww.nature.com/scientificreports/Figure 5. Temporal variations of REY content, IC1 score, and inferred relative mass fractions of sediment end-member components48 at Deep Sea Drilling Project (DSDP) Site 596, central South Pacific. (a) Bulk REY plus Ce contents and (b) IC1 scores (this study). (c) Hydrogenous, (d) phosphate, and (e) detrital (sum of aeolian dust and andesitic materials from magmatic arc) components calculated by using the total inversion method48. Age was determined on the basis of a constant Co-flux model48. (f) Geographical relationship between the Australian continent and DSDP Site 5.

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