Isotope and trace element geochemistry of Colorado Plateau volcanics

Basalts from the San Francisco Peaks and North Rim of Grand Canyon, nephelinites from the Hopi Buttes and Navajo minettes (Colorado Plateau) have been analyzed for trace element contents and Sr, Nd, Pb isotope compositions. The ages increase eastward from the Quaternary (basalt) to 5 Ma (nephelinite) and 30 Ma (minette) as does the depth of melt generation inferred from xenolith mineralogy and major element geochemistry.

The three rock types present an enrichment of incompatible elements (although minettes present negative concentration spikes for Nb, Zr, Ti, Ba, Sr) relative to other magma types. The chondrite-normalized Ce/Yb ratio changes from 8–22 (basalt) to 25–30 (nephelinite) and 33–60 (minette) and reflects small degrees of partial melting of a mantle source with a garnet/clinopyroxene ratio increasing with depth. The negative Eu anomaly present in minette, the low Sr/Nd and high Pb/Ce suggest the presence of a recycled continental crust component in their mantle source.

The ⁸⁷Sr/⁸⁶Sr ratio varies from 0.7032-0.7045 (basalt and nephelinite) to 0.7052-0.7071 (minette), while ε_Nd is remarkably more constant at +0.8 to +3.7 (nephelinite) and −2.6 to +2.2 (basalt and minette). Good linear correlations are observed in both ²⁰⁷Pb/²⁰⁴Pb and ²⁰⁸Pb/²⁰⁴Pb vs. ²⁰⁶Pb/²⁰⁴Pb diagrams with basalt being the least and nephelinite the most radiogenic and indicate a 2.3 ±0.1 Ga age and a Th/U of 3.4.

Three lithospheric source components are indicated: a) an OIB-type depleted mantle source, b) an end-member with unradiogenic Sr, Nd and Pb for basalt and nephelinite and c) a recycled crustal component for minette.     

Sterol geochemistry of sediments from the western North Atlantic Ocean and adjacent coastal areas

Core sections from coastal bay, continental slope, and continental rise surface sediments of the western North Atlantic were analyzed for sterols. Changing rate or type of sediment input, bioturbation, and chemical conversion appear to be processes important in controlling the distribution of sterols in these sediments. Comparisons of individual sterol distributions and variations in the ratio of Soxhlet-extractable to non-extractable saponified sterols indicate that for the western North Atlantic, the extent to which each process is dominant varies with proximity to shore. Evidence is presented to show that sterols in the deep sea may be at least partially terrigenous in origin and not all biogenically derived in the surface waters. These sterols, and by analogy other labile organic compounds, may serve as a source of carbon for benthic organism metabolism.     

Isotope and Trace Element Geochemistry of Fuchuan Ophiolite Suite,Anhui,China

The Fuchuan ophiolite suite in Shexian County, Anhui Province, was formed in the Middle-Late Proterozoic. It is characterized by varying Nd [∈_Nd (T) =0.7−3.8], Sr [∈_Sr(T) = 30.7−53.9] and O(δ¹⁸O=3.2−11.0%.) and low ratios of Nd/La (<0.8), Ti/Y (<350) and Ti/V (<30). These characteristics, in combination with geological features, indicate that the ophiolite suite was formed in the axial part of the back-arc basin of the Jiangnan ancient island arc at the southeastern margin of the Yangtze Plate. The varying ∈_Nd (T) was caused by the contamination of the underlying inmature sialic crust during the formation of the ophiolite and variations in ∈_Sr(T) and δ¹⁸ O may have resulted from hydrothermal alteration by seawater during or shortly after its formation.     

Mineralogy and trace element geochemistry of sulfide minerals from the Wocan Hydrothermal Field on the slow-spreading Carlsberg Ridge,Indian Ocean

The basalt-hosted Wocan Hydrothermal Field (WHF), located on the NW slope of an axial volcanic ridge at a depth of ∼3000 m at 6°22′N on the slow-spreading Carlsberg Ridge, northwest Indian Ocean, was discovered in 2013 during Chinese DY28th cruise. Preliminary investigations show that the field consists of two hydrothermal sites: Wocan-1, which shows indications for recent high-temperature hydrothermal activity, is located near the peak of the axial volcanic ridge at a water depth of 2970–2990 m, and Wocan-2 site, located at a water depth of 3100 m, ∼1.7 km to the northwest of Wocan-1. The recovered hydrothermal precipitates can be classified into four groups: (i) Cu-rich chimneys; (ii) Cu-rich massive sulfides; (iii) Fe-rich massive sulfides; and (iv) silicified massive sulfides. We conducted mineral texture and assemblage observation and Laser-ablation ICP-MS analyses of the hydrothermal precipitates to study the mineralization processes. Our results show that there are distinct systematic trace element distributions throughout the different minerals in the four sample groups. In general, chalcopyrite from the group (i) is enriched in Pb, As, Mo, Ga, Ge, V, and Sb, metals that are commonly referred to as medium- to low-temperature elements. In contrast these elements are present in low contents in the chalcopyrite grains from other sample groups. Selenium, a typical high-temperature metal, is enriched in chalcopyrite from groups (ii) and (iv), whereas Ag and Sn are enriched only in some silicified massive sulfides. As with chalcopyrite, pyrite also shows distinct trace element associations in grains with different habitus. The low-temperature association of elements (Pb, Mo, Mn, U, Mg, Ag, and Tl) is typically present in colloform/framboidal pyrite, whereas the high-temperature association (Se, Co, and Bi) is enriched in euhedral pyrite. Sphalerite in the groups (i) and (iii) at Wocan-1 is characterized by high concentrations of Ga, Ge, Pb, Cd, As, and Sb, indicating that sphalerite in these sample groups likely precipitated at intermediate temperatures. Early bornite, which mainly occurs in the central part of the Cu-rich chimney, is typically enriched in Sn and In compared to the other minerals. In contrast, late bornite that likely formed during increasing interaction of hydrothermal fluids with cold, oxygenated seawater has low Sn and In, but significantly higher concentrations of Ag, Au, Mo and U. Digenite, also forming in the exterior parts of the samples during the late stages of hydrothermal fluid venting, is poor in most trace elements, except Ag and U. The notable Ag enrichment in the late-stage mineral assemblages at both Wocan-1 and Wocan-2 may therefore be related to lower temperatures and elevated pH. Our results indicate that Wocan-1 has experienced a cycle of heating with Cu-rich chimney growth and subsequent cooling, followed by late seafloor weathering, while Wocan-2 has seen intermediate- to high-temperature mineralization followed by intense silicification of sulfides. Seafloor weathering processes or mixing of hydrothermal fluids with seawater during the waning stages of hydrothermal fluid flow result in significant redistributions of trace elements in sulfide minerals.     

黄河、长江与韩国Keum、Yeongsan江沉积物常量元素地球化学特征

运用同样的样品采集和测试方法比较分析了我国的长江和黄河以及韩国的Keum和Yeongsan江的常量元素地球化学特征。韩国河流沉积物中Ca及碳酸盐含量显著低于长江和黄河,而其他元素含量则在二者之间;黄河沉积物以总无机碳(TIC)、Na和Ca含量高为特征,而长江沉积物则显著富集Ti和P。Keum和Yeongsan江沉积物中P、Ca、Fe和Mg在酸溶相中比例可达30％～66％,而K、Al和Ti则富集在残渣相中。韩国河流沉积物极低的Ca含量同流域缺乏碳酸盐源岩密切相关,其沉积物主要由侏罗一晚白垩纪的花岗岩经过中等程度的化学风化而成。虽然Ca在中韩河流沉积物之间含量差异显著,但必须谨慎运用全钙含量来识别海区物源。而沉积物中非碳酸盐态钙(Ca^*)及相应的K／Ca^*和Al／Ca^*比更适合用来示踪黄河及Keum和Yeongsan江沉积物;Ti则可以用来区分长江与其他河流沉积物。     

Assessment of trace element geochemistry of Hampton Roads harbor and lower Chesapeake Bay area sediments

Acid extractable Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb. and Zn were determined in sediments from the Inner Virginia Shelf, and from shipping channels in the lower Chesapeake Bay and Hampton Roads, Virginia, harbor system. Data were evaluated by a variety of techniques Levels of Cd, Cu, Pb, and Zn exceeded average crustal abundances for most of the study sites. Cumulative frequency curves suggested that there were two major populations for all metals and perhaps a third and smaller, one for Cd, Cr, and Mn Plots of metal vs Fe indicated no anthropogenic inputs of metals for shelf and Chesapeake Bay channel sites, but suggested anthropogenic influences for all metals in several of the inshore sites. Enrichment factor calculations showed enrichment of Cd, Pb, and Zn with respect to average crustal abundances for all sites and of Cu for the industrial harbor system. A recommendation of this study for evaluation of environmental geochemical metals data is to utilize mean concentrations, cumulative frequency plots, and metal vs Fe and/or enrichment factor calculations when evaluating the pollution status of sediments.     

Mineralogy,major and trace element geochemistry of riverbed sediments in the headwaters of the Yangtze,Tongtian River and Jinsha River

We collected riverbed sediments of the headwaters of the Yangtze River (Chumaer River, Tuotuo River, Gaerqu River and Buqu River), Tongtian River and Jinsha River (HTJR) flowing on the eastern Tibetan Plateau and analyzed their mineralogical features, major and trace element contents. The results show: (i) very poor correlations of Na₂O, K₂O, CaO, Ba, and Sr to SiO₂, LREE to Th, HREE to Hf, and Ta/La to Ti, and characteristics of Eu anomaly (the ratios of (Eu/Eu^*)_N range from 0.60 to 0.83 with an average value of 0.71) all indicate that the Jinsha River sediments have not undergone much mineralogical sorting; (ii) illite and chlorite are predominant clay minerals, and quartz, calcite, dolomite, albite, and K-feldspar are prevailing non-clay minerals. The characteristics of mineral assemblage indicate relatively weak chemical weathering degree in these river basins; (iii) very high contents of Fe₂O₃, MgO, TiO₂, Sc, V, Cr, Co, and Ni at Panzhihua mainly result from the huge-sized V–Ti magnetite deposits occurred in layered gabbroic intrusion; and (iv) the chemical alteration index (CIA) in the HTJR ranges from 46.5 to 69.2 and with an average value of 60.5 which indicates relatively weak weathering degree.     

The trace element geochemistry of Corsican ophiolites

Ultramafic rocks, gabbros, plagiogranites, dolerites and basaltic dikes and pillows lavas of the ophiolite slices of eastern Corsica have been metamorphosed in both oceanic and orogenic environments. The trace element content of the metabasaltic rocks which exhibit a tholeiitic differentiation trend towards a ferrobasaltic composition, is similar to that of oceanic basalts. The cumulate sequence is interpreted to have been formed by fractional crystallization from an olivine-tholeiite magma. The troctolites representing cumulates derived from melts representing liquid fractions in the range F=1-0.85, gabbros from melts with F=0.85-0.45, and ferrogabbros and plagiogranites from melts with F<0.45. An oceanic environment with moderate spreading rates and magmatic processes similar to present-day normal oceanic ridge segments is considered the more probable original setting of the Corsican ophiolites.Financial support by C.N.R. (Italy) and A.T.P. Géodynamique de la Méditerranée Occidentale C.N.R.S. (France)     

西藏松多榴辉岩的矿物原位微量元素地球化学研究

对松多榴辉岩中单矿物进行的LA-ICP-MS原位微区微量元素分析研究结果表明,石榴石主要富集中、重稀土元素和Y,同时具有高丰度的Sc、V、Cr和Co等元素;绿辉石中的微量元素以中稀土元素、Sr、Sc、V、Cr、Co、Ni和Ti为主,含有一定量的Zr、Hf等。石榴石、绿辉石、角闪石和绿帘石中均显示轻稀土元素亏损的特点,表明在退变质过程中没有发生明显的富轻稀土元素的外来流体交代作用,因而其微量元素矿物地球化学的某些特点不同于苏鲁地区的榴辉岩。石榴石变斑晶中某些元素(如Ti、Zr)的分带性暗示了榴辉岩在紧随峰期变质之后的折返过程中发生了降压增温过程。榴辉岩主要变质矿物中微量元素的分配显然受到矿物主量元素的分配所控制,如MgO在石榴石和绿辉石之间的分配对Ni、Co、Ti分配的控制以及CaO的分配对Sr、Y、REE分配的控制等。退变质过程中矿物的形成或分解以及物理化学条件的改变都可以引起矿物间微量元素的重新分配。由绿辉石退变质而形成的角闪石,较之原先的绿辉石,其微量元素配分曲线总体特征会发生变化,但元素总体丰度相近,某些元素特点相似,又反映了绿辉石和角闪石之间的成生联系。金红石是Ti、Nb、Ta、Zr、Hf的主要赋存矿物,而与之共生的绿帘石所表现出来的高场强元素的亏损特征表明了金红石的存在所带来的影响。     

Genesis,evolution and tectonic significance of K-rich volcanics from the Alban Hills (Roman comagmatic region) as inferred from trace element geochemistry

Trace element data are reported in 21 lava samples from the Alban Hills, one of the most important volcanic complexes of the Roman comagmatic region. The samples consist mostly of tephritic leucitites with minor phonolitic tephrites and tephritic phonolites emplaced during two distinct phases of activity, separated by a caldera collapse. The ferromagnesian element contents are variable (Ni=93-26 ppm; Co=37-20 ppm; Cr=359-5 ppm; Sc=35-6 ppm) and tend to have higher values in the post-caldera rocks. Rb, Cs, Th, Sr, and LREE are extremely enriched in all the samples analyzed, with the pre-caldera rocks displaying a lower content of Rb and Cs and a higher abundance of Th, light REE and La/Yb ratio. Ta and Hf are not so high and are more enriched in the pre-caldera samples. Sr displays comparable values in the two groups of rocks. The trace element variation indicates that the rocks from the Alban Hills represent two distinct series of liquids formed by crystal/liquid fractionation processes starting from two parental magmas. The genesis of the primary melts is hypothesized as due to a low degree of partial melting of a mantle peridotite enriched in incompatible elements. All of the studied samples have distribution patterns of incompatible elements normalized against a hypothetical primordial mantle composition, which are similar to that displayed by the aeolian calc-alkaline and leucite-tephritic products and distinctively different from those of typical K-rich volcanics from an intraplate rift environment. This strongly supports the hypothesis that there is a close genetic connection between Roman magmatism and subductionrelated processes.     

Metabasalts from the Troodos Massif,Cyprus: Genetic implication deduced from petrography and trace element geochemistry

A wide variety of data support the contention that the Troodos massif, Cyprus is a fragment of oceanic lithosphere formed at a constructive margin some 85 m.y. ago. However, Troodos rocks differ significantly in major and trace element content and mineral parageneses from those formed at present day active constructive margins. It is here argued that the geochemical and petrographic characteristics of the massif are compatible with its formation at the axis of a slow spreading ridge within a small, marginal ocean basin.     

Petrology and trace element geochemistry of the Papuan Ultramafic Belt

New petrologic and geochemical data are presented for a suite of rocks from the Papuan Ultramafic Belt (PUB), Papua New Guinea. Tectonite harzburgites at the base of the ophiolite have extremely refractory, uniform mineralogy, and are exceptionally depleted in lithophile elements. These features are consistent with the proposed origin of these rocks as depleted upper mantle, residual after extraction of a basaltic melt. The tectonite peridotites are overlain by a thick sequence of layered ultramafic and mafic cumulates containing olivine, orthopyroxene, clinopyroxene and plagioclase as the major cumulus phases. Early cumulates are characterized by magnesian olivine Mg₉₀, orthopyroxene Mg₉₀ and calcic plagioclase An₈₆, and exhibit cryptic variation towards more iron-rich and sodic compositions. Abundances of incompatible elements in the cumulates are extremely low which, together with the nature of the cumulus phases, points to a magnesian olivine-poor tholeiite or magnesian quartz tholeiite parent magma(s) strongly depleted in incompatible elements. Highly fractionated iron-rich products of this parent magma type are represented by the LREE-depleted lavas in the overlying basalt sequence which, although resembling the most depleted mid-ocean ridge basalts (MORB) in terms of their low abundances of incompatible elements, have higher abundances of transition metals and lower abundances of Ti, HREE and other high valence cations compared to common MORB of similar Mg/(Mg+Fe) ratio.Eocene tonalites intruding the PUB are genetically unrelated to the ophiolites, and appear to be related to the Ti-poor high-Mg andesites of Cape Vogel and similar andesites and dacites at the northern end of the PUB. These rocks are considered to represent the early stages of island-arc magmatism associated with a northeastward-dipping subduction zone in the early Eocene immediately prior to emplacement of the PUB.     

Terrigenous organic matter sources in mid-pleistocene sediments from the orphan knoll,Northwest Atlantic Ocean

The concentration and composition of lignin-derived phenols, which are often used as biomarkers for terrigenous organic matter (OM) inputs, were examined in North Atlantic Ocean sediments from IODP core U1302A (50°9.985′N, 45°38.271′W, 3568 m water depth), Orphan Knoll, 650 km NE of St. John’s, Newfoundland, Canada for the period of ca. 1100–810 ka BP. Lignin-derived phenols were extracted from sediments using CuO oxidation which yielded eight characteristic phenols. The majority of sediments have low syringyl phenol to vanillyl phenol (S/V) ratios and high cinnamyl phenol to vanillyl phenol (C/V) ratios, suggesting predominant concentrations of gymnosperm-derived organic matter inputs from adjacent continents (most likely eastern Canada and possibly southern Greenland). The S/V values were lower for the period of ca. 958–840 ka BP relative to ca. 1090–1078, 1042–958 and 840–818 ka BP, indicating fluctuations in the proportion of angiosperm- and gymnosperm-derived lignin delivery to the ocean. The greater fraction of gymnosperms for the period of 958–840 ka BP likely reflects the response of vegetation in source regions to climate cooling in the early part of the mid-Pleistocene. Lignin-derived phenol concentrations also displayed high variability during the investigated period, which did not show positive correlations with magnetic susceptibility or Gamma Ray Attenuation density. Considering that a fundamental climate change (41–100 ka cyclicity) occurred within the mid-Pleistocene, large variations in abundance and composition of lignin-derived phenols in core U1302A is likely indicative of dynamic environmental conditions, reflected by the variability in both concentrations and types of vegetation on adjacent continents and/or different mechanisms to transport terrigenous organic matter to the deep ocean.     

On the occurrence,trace element geochemistry,and crystallization history of zircon from in situ ocean lithosphere

We characterize the textural and geochemical features of ocean crustal zircon recovered from plagiogranite, evolved gabbro, and metamorphosed ultramafic host-rocks collected along present-day slow and ultraslow spreading mid-ocean ridges (MORs). The geochemistry of 267 zircon grains was measured by sensitive high-resolution ion microprobe-reverse geometry at the USGS-Stanford Ion Microprobe facility. Three types of zircon are recognized based on texture and geochemistry. Most ocean crustal zircons resemble young magmatic zircon from other crustal settings, occurring as pristine, colorless euhedral (Type 1) or subhedral to anhedral (Type 2) grains. In these grains, Hf and most trace elements vary systematically with Ti, typically becoming enriched with falling Ti-in-zircon temperature. Ti-in-zircon temperatures range from 1,040 to 660°C (corrected for a _TiO2 ≈ 0.7, a _SiO2 ≈ 1.0, pressure ≈ 2 kbar); intra-sample variation is typically ~60–150°C. Decreasing Ti correlates with enrichment in Hf to ~2 wt%, while additional Hf-enrichment occurs at relatively constant temperature. Trends between Ti and U, Y, REE, and Eu/Eu* exhibit a similar inflection, which may denote the onset of eutectic crystallization; the inflection is well-defined by zircons from plagiogranite and implies solidus temperatures of ~680–740°C. A third type of zircon is defined as being porous and colored with chaotic CL zoning, and occurs in ~25% of rock samples studied. These features, along with high measured La, Cl, S, Ca, and Fe, and low (Sm/La)_N ratios are suggestive of interaction with aqueous fluids. Non-porous, luminescent CL overgrowth rims on porous grains record uniform temperatures averaging 615 ± 26°C (2SD, n = 7), implying zircon formation below the wet-granite solidus and under water-saturated conditions. Zircon geochemistry reflects, in part, source region; elevated HREE coupled with low U concentrations allow effective discrimination of ~80% of zircon formed at modern MORs from zircon in continental crust. The geochemistry and textural observations reported here serve as an important database for comparison with detrital, xenocrystic, and metamorphosed mafic rock-hosted zircon populations to evaluate provenance.     

Historical trace element distribution in sediments from the Mississippi River delta

Five sediment cores were collected on the shelf of the inner Mississippi Bight in June 2003 for a suite of radionuclides to establish geochronologies and trace elements to examine patterns of contaminant deposition and accumulation. Core sites were chosen to reflect a matrix of variable water depths, proximity to the Mississippi River mouth as the primary source for terrigenous particles, and extent and duration of summertime water column hypoxia. The vertical distribution of^239,240Pu and²¹⁰Pb_xs(=²¹⁰Pb_total−²²⁶Ra) provided reliable geochronological age constraints to develop models for mass accumulation rates and historic trace element inputs and variations. Mass accumulation rates ranged from 0.27 to 0.87 g cm⁻²yr⁻¹ and were internally consistent using either²¹⁰Pb_xs or^239,240Pu. Measured inventories of¹³⁷Cs,^239,240Pu, and²¹⁰Pb_xs were compared to atmospheric deposition rates to quantify potential sediment focusing or winnowing. Observed variability in calculated mass accumulation rates may be attributed foremost to site-specific proximity to the river mouth (i.e., sediment source), variability in water depth, and enhanced sediment focusing at the Mississippi River canyon site. Trace element concentrations were first normalized to Al, and then Al-normalized enrichment factors (ANEF) were calculated based on preanthropogenic and crustal trace element abundances. These ANEFs were typically >1 for V and Ba, while for most other elements studied, either no enrichment or depletion was observed. The enrichment of Ba may be related, in part, to the seasonal occurrence of oxygen-depleted subsurface waters off the Mississippi River delta, as well as being an ubiquitous byproduct of the petroleum industry.     

The geochemistry of redox sensitive trace metals in sediments

We analyzed the redox sensitive elements V, Mo, U, Re and Cd in surface sediments from the Northwest African margin, the U.S. Northwest margin and the Arabian Sea to determine their response under a range of redox conditions. Where oxygen penetrates 1 cm or less into the sediments, Mo and V diffuse to the overlying water as Mn is reduced and remobilized. Authigenic enrichments of U, Re and Cd are evident under these redox conditions. With the onset of sulfate reduction, all of the metals accumulate authigenically with Re being by far the most enriched. General trends in authigenic metal accumulation are described by calculating authigenic fluxes for the 3 main redox regimes: oxic, reducing where oxygen penetrates ≤1 cm, and anoxic conditions. Using a simple diagenesis model and global estimates of organic carbon rain rate and bottom water oxygen concentrations, we calculate the area of sediments below 1000 m water depth in which oxygen penetration is ≤1 cm to be 4% of the ocean floor. We conclude that sediments where oxygen penetrates ≤1 cm release Mn, V and Mo to seawater at rates of 140%–260%, 60%–150% and 5%–10% of their respective riverine fluxes, using the authigenic metal concentrations and accumulation rates from this work and other literature. These sediments are sinks for Re, Cd and U, with burial fluxes of 70%–140%, 30%–80% and 20%–40%, respectively, of their dissolved riverine inputs. We modeled the sensitivity of the response of seawater Re, Cd and V concentrations to changes in the area of reducing sediments where oxygen penetrates ≤1 cm. Our analysis suggests a negligible change in seawater Re concentration, whereas seawater concentrations of Cd and V could have decreased and increased, respectively, by 5%–10% over 20 kyr if the area of reducing sediments increased by a factor of 2 and by 10%–20% if the area increased by a factor of 3. The concentration variations for a factor of 2 increase in the area of reducing sediments are at about the level of uncertainty of Cd/Ca and V/Ca ratios observed in foraminifera shells over the last 40 kyr. This implies that the area of reducing sediments in the ocean deeper than 1000 m (4%) has not been greater than twice the present value in the recent past.     

The minor and trace element geochemistry of volcanic rocks from Truk,Ponape and Kusaie,Eastern Caroline Islands; the evolution of a young hot spot trace across Old Pacific Ocean Crust

Recent paleomagnetic and K-Ar age dating studies in the Caroline Islands show that the high volcanic islands of Truk, Panape and Kusaie formed at the same shallow latitude and display a progression of ages increasing westward from 1 m.y. (Kusaie), through 6 m.y. (Ponape) to 12 m.y. (Truk). These data suggest that the islands were formed by a young hotspot or melting anomaly. One hundred and fifty volcanic rocks from these three islands have been analysed for major and 15 trace elements and results indicate that shield-building lavas on each island (1) evolved by low-pressure open-system fractional crystallisation of a small range of partial melts and (2) became more alkaline with time from Truk to Kusaie. The secular geochemical variation along the Caroline chain may represent a hotspot trace whose magma production was slowly declining over the past 14 m.y.