Plume-lithosphere interaction beneath Mt. Cameroon volcano, West Africa: Constraints from U-Th-Ra and Sr-Nd-Pb isotope systematics

Precise measurements of ²³⁸U-²³⁰Th-²²⁶Ra disequilibria in lavas erupted within the last 100 yr on Mt. Cameroon are presented, together with major and trace elements, and Sr-Nd-Pb isotope ratios, to unravel the source and processes of basaltic magmatism at intraplate tectonic settings. All samples possess ²³⁸U-²³⁰Th-²²⁶Ra disequilibria with ²³⁰Th (18-24%) and ²²⁶Ra (9-21%) excesses, and there exists a positive correlation in a (²²⁶Ra/²³⁰Th)-(²³⁰Th/²³⁸U) diagram. The extent of ²³⁸U-²³⁰Th-²²⁶Ra disequilibria is markedly different in lavas of individual eruption ages, although the (²³⁰Th/²³²Th) ratio is constant irrespective of eruption age. When U-series results are combined with Pb isotope ratios, negative correlations are observed in the (²³⁰Th/²³⁸U)-(²⁰⁶Pb/²⁰⁴Pb) and (²²⁶Ra/²³⁰Th)-(²⁰⁶Pb/²⁰⁴Pb) diagrams. Shallow magma chamber processes like magma mixing, fractional crystallization and wall rock assimilation do not account for the correlations. Crustal contamination is not the cause of the observed isotopic variations because continental crust is considered to have extremely different Pb isotope compositions and U/Th ratios. Melting of a chemically heterogeneous mantle might explain the Mt. Cameroon data, but dynamic melting under conditions of high D_U and D_U/D_Th, long magma ascent time, or disequilibrium mineral/melt partitioning, is required. The most plausible scenario to produce the geochemical characteristics of Mt. Cameroon samples is the interaction of melt derived from the asthenospheric mantle with overlying sub-continental lithospheric mantle which has elevated U/Pb (>0.75) and Pb isotope ratios (²⁰⁶Pb/²⁰⁴Pb > 20.47) due to late Mesozoic metasomatism.     

Timescales of magma differentiation from basalt to andesite beneath Hekla Volcano, Iceland: Constraints from U-series disequilibria in lavas from the last quarter-millennium flows

Measurements of ²³⁸U-²³⁰Th-²²⁶Ra disequilibria, Sr-Nd-Pb-Hf isotopes and major-trace elements have been conducted for lavas erupted in the last quarter-millennium at Hekla volcano, Iceland. The volcanic rocks range from basalt to dacite. Most of the lavas (excluding dacitic samples) display limited compositional variations in radiogenic Sr-Nd-Pb-Hf isotopes (⁸⁷Sr/⁸⁶Sr = 0.70319-0.70322; ¹⁴³Nd/¹⁴⁴Nd = 0.51302-0.51305; ²⁰⁶Pb/²⁰⁴Pb = 19.04-19.06; ²⁰⁷Pb/²⁰⁴Pb = 15.53-15.54; ²⁰⁸Pb/²⁰⁴Pb = 38.61-38.65; ¹⁷⁶Hf/¹⁷⁷Hf = 0.28311-0.28312). All the samples possess (²³⁰Th/²³⁸U) disequilibrium with ²³⁰Th excesses, and they show systematic variations in (²³⁰Th/²³²Th) and (²³⁸U/²³²Th) ratios. The highest ²²⁶Ra excesses occur in the basalt and most differentiated andesite lavas, while some basaltic-andesite lavas have (²²⁶Ra/²³⁰Th) ratio that are close to equilibrium. The ²³⁸U-²³⁰Th-²²⁶Ra disequilibria variations cannot be produced by simple closed-system fractional crystallization with radioactive decay of ²³⁰Th and ²²⁶Ra in a magma chamber. A closed-system fractional crystallization model and assimilation and fractional crystallization (AFC) model indicate that the least differentiated basaltic andesites were derived from basalt by fractional crystallization with a differentiation age of ∼24 ± 11 kyr, whereas the andesites were formed by assimilation of crustal material and fractionation of the basaltic-andesites within 2 kyr. Apatite is inferred to play a key role in fractionating the parent-daughter nuclides in ²³⁰Th-²³⁸U and ²²⁶Ra-²³⁰Th to make the observed variations. Our proposed model is that several batches of basaltic-andesite magmas that formed by fractional crystallization of a basaltic melt from a deeper reservoir, were periodically injected into the shallow crust to form individual magma pockets, and subsequently modifying the original magma compositions via simultaneous assimilation and fractional crystallization. The assimilant is the dacitic melt, which formed by partial melting of the crust.     

The effect of assimilation, fractional crystallization, and ageing on U-series disequilibria in subduction zone lavas

Although most arc lavas have experienced significant magma differentiation, the effect of the differentiation process on U-series disequilibria is still poorly understood. Here we present a numerical model for simulating the effect of time-dependent magma differentiation processes on U-series disequilibria in lavas from convergent margins. Our model shows that, in a closed system with fractional crystallization, the ageing effect can decrease U-series disequilibria via radioactive decay while in an open system, both ageing and bulk assimilation of old crustal material serve to reduce the primary U-series disequilibria. In contrast, with recharge of refresh magma, significant ²²⁶Ra excess in erupted lavas can be maintained even if the average residence time is longer than 8000 years.The positive correlations of (²²⁶Ra/²³⁰Th) between Sr/Th or Ba/Th in young lavas from convergent margins have been widely used as evidence of fluid addition generating the observed ²²⁶Ra excess in subduction zones. We assess to what extent the positive correlations of (²²⁶Ra/²³⁰Th) with Sr/Th and Ba/Th observed in the Tonga arc could reflect AFC process. Results of our model show that these positive correlations can be produced during time-dependent magma differentiation at shallow crustal levels. Specifically, fractional crystallization of plagioclase and amphibole coupled with contemporaneous decay of ²²⁶Ra can produce positive correlations between (²²⁶Ra/²³⁰Th) and Sr/Th or Ba/Th (to a lesser extent). Therefore, the correlations of (²²⁶Ra/²³⁰Th) with Sr/Th and Ba/Th cannot be used to unambiguously support the fluid addition model, and the strength of previous conclusions regarding recent fluid addition and ultra-fast ascent rates of arc magmas is significantly lessened.     

The extent of U-series disequilibria produced during partial melting of the lower crust with implications for the formation of the Mount St. Helens dacites

The extent to which U-series disequilibria can be produced during partial melting of mafic lower crust is quantified using a simple batch melting model and both experimental and theoretical partition coefficients for U, Th and Ra. We show that partial melting of mafic lower crust can only produce small disequilibria between ²³⁸U, ²³⁰Th and ²²⁶Ra. Crystallisation of basalt and mixing between young basalt and crustal derived melts will have a similar or smaller effect. Consequently, U-series disequilibrium in arc andesites and dacites can generally only be an inherited feature derived from a mantle parent, unless the timescales of silicic magma production within the crust are short compared to the half-life of ²²⁶Ra. Our results have profound implications for several recent models of silicic magma production by thermal incubation and partial melting of the lower crust. We show that the ²²⁶Ra excess observed in most arc andesites and dacites requires extremely rapid differentiation and/or the involvement of mantle derived basalts less than a few thousand years old. Application to Mount St. Helens suggests that crystallisation of young mantle-derived magma is likely to be the dominant process in the formation of these dacites.     

U-series disequilibria in Kick’em Jenny submarine volcano lavas: A new view of time-scales of magmatism in convergent margins

We present data for U and its decay series nuclides ²³⁰Th, ²²⁶Ra, ²³¹Pa, and ²¹⁰Po for 14 lavas from Kick’em Jenny (KEJ) submarine volcano to constrain the time-scales and processes of magmatism in the Southern Lesser Antilles, the arc having the globally lowest plate convergence rate. Although these samples are thought to have been erupted in the last century, most have (²²⁶Ra)/(²¹⁰Po) within ±15% of unity. Ten out of 14 samples have significant ²²⁶Ra excesses over ²³⁰Th, with (²²⁶Ra)/(²³⁰Th) up to 2.97, while four samples are in ²²⁶Ra-²³⁰Th equilibrium within error. All KEJ samples have high (²³¹Pa)/(²³⁵U), ranging from 1.56 to 2.64 and high ²³⁸U excesses (up to 43%), providing a global end-member of high ²³⁸U and high ²³¹Pa excesses. Negative correlations between Sr, sensitive to plagioclase fractionation, and Ho/Sm, sensitive to amphibole fractionation, or K/Rb, sensitive to open system behavior, indicate that differentiation at KEJ lavas was dominated by amphibole fractionation and open-system assimilation. While (²³¹Pa)/(²³⁵U) does not correlate with differentiation indices such as Ho/Sm, (²³⁰Th)/(²³⁸U) shows a slight negative correlation, likely due to assimilation of materials with slightly higher (²³⁰Th)/(²³⁸U). Samples with ²²⁶Ra excess have higher Sr/Th and Ba/Th than those in ²²⁶Ra-²³⁰Th equilibrium, forming rough positive correlations of (²²⁶Ra)/(²³⁰Th) with Sr/Th and Ba/Th similar to those observed in many arc settings. We interpret these correlations to reflect a time-dependent magma differentiation process at shallow crustal levels and not the process of recent fluid addition at the slab-wedge interface.The high ²³¹Pa excesses require an in-growth melting process operating at low melting rates and small residual porosity; such a model will also produce significant ²³⁸U-²³⁰Th and ²²⁶Ra-²³⁰Th disequilibrium in erupted lavas, meaning that signatures of recent fluid addition from the slab are unlikely to be preserved in KEJ lavas. We instead propose that most of the ²³⁸U-²³⁰Th, ²²⁶Ra-²³⁰Th, and ²³⁵U-²³¹Pa disequilibria in erupted KEJ lavas reflect the in-growth melting process in the mantle wedge (reflecting variations in U/Th, daughter-parent ratios, fO₂, and thermal structure), followed by modification by magma differentiation at crustal depths. Such a conclusion reconciles the different temporal implications from different U-series parent-daughter pairs and relaxes the time constraint on mass transfer from slab to eruption occurring in less than a few thousand years imposed by models whereby ²²⁶Ra excess is derived from the slab.     

Ra-excess during the 1631-1944 activity period of Vesuvius (Italy): A model of alpha-recoil enrichment in a metasomatized mantle and implications on the current state of the magmatic system

The origin of the ²²⁶Ra-excess during the last cycle of Vesuvius activity was investigated by high-resolution γ-spectrometry, TIMS and EDXRF. Lavas display high initial ²²⁶Ra-excess (500-1000%), similar (²³⁰Th/²³²Th) activity ratios (0.87-0.91) and most samples show significant ²³⁸U-excess. During the period 1631-1944 the initial absolute ²²⁶Ra-excess reached the highest values (19-44 dpm g⁻¹) recorded for earth volcanoes. Crystal fractionation and particularly leucite floating did not cause the ²²⁶Ra-excess in spite of the high ²²⁶Ra activity (21-85 dpm g⁻¹) in leucite. The presence of phlogopite in the mantle source, documented by field and petrological evidences on local mantle-derived xenoliths, rules out that equilibrium partial melting can be responsible for the ²²⁶Ra-excess. This primary feature may be explained by a multistage process involving metasomatic mantle fluids (MMFs) flowing through a mantle wedge where U is concentrated as U-accessory minerals deposited along microfractures. Fluids, passing through the mantle wedge, are supplied of ²²⁶Ra, ²³⁰Th and ²³⁴U by α-decay recoil of parent nuclides from U-enriched microfractures. This model calculates that the ascent time of fluids through the mantle wedge was ≤ 12 ka. Successively MMFs mixed with mantle-derived melts, giving rise to ²²⁶Ra-enriched magmas, which entered the Vesuvius plumbing system less than 7 ka. Crystal fractionation did not affect extensively the initial ²²⁶Ra/Ba ratio, which varied in the 1631-1944 period according to a pattern reflecting periodic inputs of ²²⁶Ra-enriched magma, variable reservoir volumes and residence times in magmatic chamber(s). The temporal trend of the reservoir volumes, extrapolated to the present time, indicates a volume of magma of ∼ 0.021 km³, stored most probably in a shallow chamber.     

U- and Th-decay series constraints on the timescales of crystal fractionation to produce the phonolite erupted in 2004 near Tristan da Cunha, South Atlantic Ocean

Phonolite pumice found floating offshore of Tristan da Cunha following intense seismic activity southeast of the island July 29-30, 2004 was analyzed for ²³⁸U- and ²³²Th-series nuclides to determine initial ²³⁰Th, ²²⁶Ra, ²¹⁰Pb, ²¹⁰Po, ²²⁸Ra, and ²²⁸Th activities. The initial (²¹⁰Po/²¹⁰Pb) value of 0.15 for the phonolite shows that, like most subaerial lavas, this subaqueous tephra degassed most of its ²¹⁰Po upon eruption. The (²³⁰Th/²³²Th) and (²³⁸U/²³²Th) values for the phonolite are similar to those of the trachyandesites erupted in 1961 from Tristan da Cunha. However, the relative activities of ²¹⁰Pb, ²²⁶Ra, and ²³⁰Th in the phonolite contrast with those of the trachyandesites, in that ²¹⁰Pb and ²³⁰Th are both strongly enriched with respect to ²²⁶Ra. In addition, the phonolite had a small deficit in ²²⁸Ra with respect to ²³²Th. The Ra deficits likely resulted from partitioning into feldspars and hornblende in a time frame that extended over several decades to a century. These disequilibria can be explained by crystal fractionation at a decreasing rate through time at an average of 3-5 × 10⁻³ year⁻¹. The calculated crystallization rate is about an order of magnitude faster than has been calculated for most other phonolites and trachytes, and about half that calculated for crystallization of the Makaopuhi lava lake. These data imply that the 2004 magma was not the differentiated cap of a much larger body that remained at depth. Instead, it was likely the residue of a relatively small body of more mafic magma that was injected into the crust southeast Tristan and underwent extensive and rapid crystal fractionation before it erupted.     

Chemical and isotopic constraints on the generation and transport of magma beneath the East Pacific Rise

Interpretation of U-series disequilibria in midocean ridge basalts is highly dependent on the bulk partition coefficients for U and Th and therefore the mineralogy of the mantle source. Distinguishing between the effect of melting processes and variable source compositions on measured disequilibria (²³⁸U-²³⁰Th-²²⁶Ra and ²³⁵U-²³¹Pa) requires measurement of the radiogenic isotopes Hf, Nd, Sr, and Pb. Here, we report measurements of ²³⁸U-²³⁰Th-²²⁶Ra and ²³⁵U-²³¹Pa disequilibria; Hf, Nd, Sr, and Pb isotopic; and major and trace element compositions for a suite of 20 young midocean ridge basalts from the East Pacific Rise axis between 9°28′ and 9°52′N. All of the samples were collected within the axial summit trough using the submersible Alvin. The geological setting and observational data collected during sampling operations indicate that all the rocks are likely to have been erupted from 1991 to 1992 or within a few decades of that time. In these samples, ²³⁰Th excesses and ²²⁶Ra excesses are variable and inversely correlated. Because the eruption ages of the samples are much less than the half-life of ²²⁶Ra, this inverse correlation between ²³⁰Th and ²²⁶Ra excesses can be considered a primary feature of these lavas. For the lava suite analyzed in this study, ²²⁶Ra and ²³⁰Th excesses also vary with lava composition: ²²⁶Ra excesses are negatively correlated with Na₈ and La/Yb and positively correlated with Mg#. Conversely, ²³⁰Th excesses are positively correlated with Na₈ and La/Yb and negatively correlated with Mg#. Th/U, ²³⁰Th/²³²Th, and ²³⁰Th excesses are also variable and correlated to one another. ²³¹Pa excesses are large but relatively constant and independent of Mg#, La/Yb, Th/U, and Na₈. The isotope ratios ¹⁴³Nd/¹⁴⁴Nd, ¹⁷⁶Hf/¹⁷⁷Hf, ⁸⁷Sr/⁸⁶Sr, and ²⁰⁸Pb/²⁰⁶Pb are constant within analytical uncertainty, indicating that they were derived from a common source. The source is homogeneous with respect to parent/daughter ratios Lu/Hf, Sm/Nd, Rb/Sr, and Th/U; therefore, the measured variations of Th/U, ²³⁰Th, and ²²⁶Ra excesses and major and trace element compositions in these samples are best explained by polybaric melting of a homogeneous source, not by mixing of compositionally distinct sources.     

Using short-lived nuclides of the U- and Th-series to probe the kinetics of colloid migration in forested soils

The recent chemical dynamics of a podzolic forest soil section (from the Strengbach watershed, France) was investigated using U- and Th-series nuclides. Analyses of (²³⁸U), (²³⁰Th), (²²⁶Ra), (²³²Th), (²²⁸Ra) and (²²⁸Th) activities in the soil particles, the seepage waters, and the mature leaves of the beech trees growing on this soil were performed by TIMS or gamma spectrometry. The simultaneous analysis of the different soil (sl) compartments allows to demonstrate that a preferential Th leaching over Ra must be assumed to explain the (²²⁶Ra/²³⁰Th), (²²⁸Ra/²³²Th) and (²²⁸Th/²²⁸Ra) disequilibria recorded in the soil particles. The overall Ra- and Th- transfer schemes are entirely consistent with the prevailing acido-complexolysis weathering mechanism in podzols. Using a continuous open-system leaching model, the (²²⁶Ra/²³⁰Th) and (²²⁸Ra/²³²Th) disequilibria measured in the different soil layers enable dating of the contemporary processes occurring in this soil. In this way, we have determined that a preferential Th-leaching from the shallow Ah horizon, due to a strong complexation with organic colloids, began fairly recently (18 years ago at most). The continual increase in pH recorded in precipitations over the last 20 years is assumed to be the cause of this enhanced organic complexation. A lower soil horizon (50-60 cm) is also affected by preferential Th leaching, though lasting over several centuries at least, with a much smaller leaching rate. The migration of Th isotopes through this soil section might hence be used as a tracer for the organic colloids migration and the induced radioactive disequilibria demonstrate to be useful for assessing the colloidal migration kinetics in a forested soil.Ra and Th isotopic ratios also appear to be valuable tracers of some mineral-water-plant interactions occurring in soil. The (²²⁸Ra/²²⁶Ra) ratio enables discrimination of the Ra flux originating from leaf degradation from that originating from mineral weathering in shallow −10 cm seepage soil waters. It appears that, at least in some cases, the Ra-isotopic ratio measured in forest-soil seepage waters may not be representative of the Ra-isotopic ratio released from mineral weathering, indicating that the different origins of the dissolved ²²⁶Ra and ²²⁸Ra must be taken into account.     

U-TH-PA-RA study of the Kamchatka arc: new constraints on the genesis of arc lavas

The ²³⁸U-²³⁰Th-²²⁶Ra and ²³⁵U-²³¹Pa disequilibria have been measured by mass spectrometry in historic lavas from the Kamchatka arc. The samples come from three closely located volcanoes in the Central Kamchatka Depression (CKD), the most active region of subducted-related volcanism in the world. The large excesses of ²²⁶Ra over ²³⁰Th found in the CKD lavas are believed to be linked to slab dehydration. Moreover, the samples show the uncommon feature of (²³⁰Th/²³⁸U) activity ratios both lower and higher than 1. The U-series disequilibria are characterized by binary trends between activity ratios, with (²³¹Pa/²³⁵U) ratios all >1. It is shown that these correlations cannot be explained by a simple process involving a combination of slab dehydration and melting. We suggest that they are more likely to reflect mixing between two end-members: a high-magnesia basalt (HMB) end-member with a clear slab fluid signature and a high-alumina andesite (HAA) end-member reflecting the contribution of a slab-derived melt. The U-Th-Ra characteristics of the HMB end-member can be explained either by a two-step fluid addition with a time lag of 150 ka between each event or by continuous dehydration. The inferred composition for the dehydrating slab is a phengite-bearing eclogite. Equilibrium transport or dynamic melting can both account for ²³¹Pa excess over ²³⁵U in HMB end-member. Nevertheless, dynamic melting is preferred as equilibrium transport melting requires unrealistically high upwelling velocities to preserve fluid-derived ²²⁶Ra/²³⁰Th. A continuous flux melting model is also tested. In this model, ²³¹Pa-²³⁵U is quickly dominated by fluid addition and, for realistic extents of melting, this process cannot account for (²³¹Pa/²³⁵U) ratios as high as 1.6, as observed in the HMB end-member.The involvement of a melt derived from the subducted oceanic crust is more likely for explaining the HAA end-member compositions than crustal assimilation. Melting of the oceanic crust is believed to occur in presence of residual phengite and rutile, resulting in no ²²⁶Ra-²³⁰Th disequilibrium and low ²³¹Pa excess over ²³⁵U in the high-alumina andesites. Consequently, it appears that high-alumina andesites and high-magnesia basalts have distinct origins: the former being derived from melting of the subducted oceanic crust and the latter from hydrated mantle. It seems that there is no genetic link between these two magma types, in contrast with what was previously believed.     

Diffusive fractionation of U-series radionuclides during mantle melting and shallow-level melt-cumulate interaction

U-series radioactive disequilibria in basaltic lavas have been used to infer many important aspects of melt generation and extraction processes in Earth’s mantle and crust, including the porosity of the melting zone, the solid mantle upwelling rate, and the melt transport rate. Most of these inferences have been based on simplified theoretical treatments of the fractionation process, which assume equilibrium partitioning of U-series nuclides among minerals and melt. We have developed a numerical model in which solid-state diffusion controls the exchange of U-series nuclides among multiple minerals and melt. First the initial steady-state distribution of nuclides among the phases, which represents a balance between diffusive fluxes and radioactive production and decay, is calculated. Next, partial melting begins, or a foreign melt is introduced into the system, and nuclides are again redistributed among the phases via diffusion. U-series nuclides can be separated during this stage due to differences in their diffusivity; radium in particular, and possibly protactinium as well, can be strongly fractionated from slower-diffusing thorium and uranium. We show that two distinct processes are not required for the generation of ²²⁶Ra and ²³⁰Th excesses in mid-ocean ridge basalts, as has been argued previously; instead the observed negative correlations of the (²²⁶Ra/²³⁰Th) activity ratio with (²³⁰Th/²³⁸U) and with the extent of trace element enrichment may result from diffusive fractionation of Ra from Th during partial melting of the mantle. Alternatively, the (²²⁶Ra/²³⁰Th) disequilibrium in mid-ocean ridge basalts may result from diffusive fractionation during shallow-level interaction of mantle melts with gabbroic cumulates, and we show that the results of the interaction have a weak dependence on the age of the cumulate if both plagioclase and clinopyroxene are present.     

U-series disequilibria in volcanic rocks from the Canary Islands: Plume versus lithospheric melting

U-series disequilibria are presented for Holocene samples from the Canary Islands and interpreted with special emphasis on the separate roles of plume vs. lithospheric melting processes. We report Th and U concentrations and (²³⁸U)/(²³²Th), (²³⁰Th)/(²³²Th), (²³⁰Th)/(²³⁸U) and (²³⁴U)/(²³⁸U) for 43 samples, most of which are minimally differentiated, along with (²²⁶Ra)/(²³⁰Th) and (²³¹Pa)/(²³⁵U) for a subset of these samples, measured by thermal ionization mass spectrometry (TIMS). Th and U concentrations range between 2 and 20 ppm and 0.5 and 6 ppm, respectively. Initial (²³⁰Th)/(²³⁸U) ranges from 1.1 to 1.6. (²²⁶Ra)/(²³⁰Th)_o ranges between 0.9 and 1.8 while (²³¹Pa)/(²³⁵U)_o ranges between 1.0 and 2.0.Our interpretation of results is based on a three-fold division of samples as a function of incompatible element ratio, such as Nb/U. The majority of samples have Nb/U = 47 ± 10, similar to most MORB and OIB. Higher ratios are found exclusively in alkali basalts and tholeiites from the eastern Canary Islands whereas lower ratios are exclusively found in differentiated rocks from the western Canary Islands. Those with ordinary Nb/U ratios are attributed to melting within the slowly ascending HIMU-dominated Canary plume.Higher Nb/U, generally found in more silica rich basalts from the eastern islands, is attributed to lithospheric contamination. Based on their trace element characteristics, two possible contaminants are amphibole veins (± other minerals) crystallized in the mantle from previous plume-derived basanite or re-melted plume-derived intrusive rocks. The high Nb/U signature of these materials is imparted on a melt of the lithosphere created either by the diffusive infiltration of alkalis or by direct reaction between basanites and peridotite. Mixing between plume-derived basanite and lithospheric melt accounts for the U-series systematics of most eastern island magmas including the well-known Timanfaya eruption. Lower Nb/U ratios in differentiated rocks from the western islands are attributed to fractional crystallization of amphibole ± phlogopite ± sphene from basanite during its ascent through the lithosphere. Based on changes in disequilibria, phonolites and tephrites are interpreted to result from rapid differentiation of primitive parents within millennia.     

高分辨电感耦合等离子体质谱法测定铀矿石样品中234U/238U、230Th/232Th和228Ra/226Ra同位素比值 

采用氢氟酸-硝酸-盐酸混合酸密闭消解含铀矿石样品,用阴离子交换树脂、阳离子交换树脂和锶特效树脂逐级分离富集铀、钍和镭。使用高分辨电感耦合等离子体质谱(HR-ICPMS)测定分离纯化液中234U/238U2、30Th/232Th和228Ra/226Ra同位素。比值的测量精密度取决于比值的大小和对应核素浓度的大小。对质量浓度为10 ng/mL天然铀测量液,234U/238U的测量精密度优于1.2%;对230Th质量浓度为0.6ng/mL且230Th和232Th质量浓度接近的测量液,230Th/232Th的测量精密度为1.2%;对228Ra质量浓度为0.48 pg/mL且228Ra和226Ra质量浓度接近的测量液,228Ra/226Ra的测量精密度为4.0%。     

(Pa/U)-(Th/U) of young mafic volcanic rocks from Nicaragua and Costa Rica and the influence of flux melting on U-series systematics of arc lavas

We present U, Th, and Pa isotope data for young lavas from Costa Rica and Nicaragua in the Central American arc. Thorium isotopic ratios for Costa Rica and Nicaragua differ dramatically: Costa Rican lavas are characterized by low (²³⁰Th/²³²Th) (1 to 1.2) and, for four out of five lavas, (²³⁰Th/²³⁸U) greater than unity. Nicaraguan lavas have high (²³⁰Th/²³²Th) (2.2 to 2.7) and, for five of six samples, (²³⁰Th/²³⁸U) less than unity. All lavas have (²³¹Pa/²³⁵U) greater than unity, with initial values ranging from 1.27 to 1.77, but those from Costa Rica have larger ²³¹Pa excesses. There is a broad positive correlation between (²³¹Pa/²³⁵U) and (²³⁰Th/²³⁸U) similar to the worldwide trend for arcs outlined by Pickett and Murrell (1997), although many of the Nicaraguan lavas skirt the high end of that trend. In greater detail, the Central American data appear to divide into separate high-(²³¹Pa/²³⁵U) and low-(²³¹Pa/²³⁵U) tiers. These tiers may be different because of either different residence times in the crust or different proportions of sedimentary components from the slab.Substantial (²³¹Pa/²³⁵U) excesses (>1.5) in both Costa Rica and Nicaragua require a melting process that allows for enhanced daughter (²³¹Pa) ingrowth. With increasing U addition, (²³¹Pa/²³⁰Th) increases in a manner that cannot be explained adequately by aging of fluid components before partial melting and eruption. Thus, either some ²³¹Pa is added from the slab, or melting-enhanced ²³¹Pa ingrowth is greater in sources that have experienced a larger amount of slab-derived flux and a higher extent of melting. These observations can be explained if regions that have undergone greater extents of fluxing and melting have experienced these processes over a longer time interval than those that have had little flux added and little melt extracted. We propose a flux-ingrowth melting model in which corner flow in the mantle wedge supplies fresh hot mantle into a zone of slab fluid addition. Partial melting occurs in response to this fluxing. We assume critical melting at low porosity (∼10⁻³), rapid fluid flux to the melting region, and rapid melt transport. Solid mantle traverses the melting region over 10⁵ to 10⁶ yr, thereby allowing ²³¹Pa and ²³⁰Th ingrowth from U retained in the residues of melt extraction. Magmas are aggregated from all parts of the melting regime, mixing melts from incipiently fluxed regions with those from sources that have experienced more extensive fluid addition, partial melting, and daughter nuclide ingrowth. With suitable assumptions about component addition from the slab, this flux-ingrowth model matches a wide range of U-series and trace element data from Costa Rican and Nicaraguan lavas, with required average extents of melting of ∼1 to 3% and 7 to 15%, respectively. Upwelling and/or extensive melt-rock reaction are not required to explain large (²³¹Pa/²³⁵U) excesses in Central America or other arcs. On Th isotope equiline plots, the model produces linear arrays that resemble isochrons but that have no age significance. Instead, these arrays are generated by mixing of melts from sources that have experienced fluid addition and partial melting over a range of time intervals, as seems likely in arc source regions. Finally, the flux-ingrowth model predicts considerable ²²⁶Ra excesses for integrated magmas. If we assume that ²²⁶Ra is added continuously with the slab-derived fluid, the model predicts large and increasing (²²⁶Ra/²³⁰Th) with increasing melting and slab-component addition, without requiring the addition of a distinct late fluid.     

Factors controlling the groundwater transport of U, Th, Ra, and Rn

A model for the groundwater transport of naturally occurring U, Th, Ra, and Rn nuclides in the²³⁸U and²³²Th decay series is discussed. The model developed here takes into account transport by advection and the physico-chemical processes of weathering, decay, α-recoil, and sorption at the water-rock interface. It describes the evolution along a flowline of the activities of the²³⁸U and²³²Th decay series nuclides in groundwater. Simple sets of relationships governing the activities of the various species in solution are derived, and these can be used both to calculate effective retardation factors and to interpret groundwater data. For the activities of each nuclide, a general solution to the transport equation has been obtained, which shows that the activities reach a constant value after a distance ϰ_i, characteristic of each nuclide. Where ϰ_i is much longer than the aquifer length, (for²³⁸U,²³⁴U, and²³²Th), the activities grow linearly with distance. Where gKⁱ is short compared to the aquifer length, (for²³⁴Th,²³⁰Th,²²⁸Th,²²⁸Ra, and²²⁴Ra), the activities rapidly reach a constant or quasi-constant activity value. For²²⁶Ra and²²²Rn, the limiting activity is reached after 1 km. High δ²³⁴U values (proportional to the ratio^ɛ234Th/^W238U) can be obtained through high recoil fraction and/or low weathering rates. The activity ratios²³⁰Th/²³²Th,²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra have been considered in the cases where either weathering or recoil is the predominant process of input from the mineral grain. Typical values for weathering rates and recoil fractions for a sandy aquifer indicate that recoil is the dominant process for Th isotopic ratios in the water. Measured data for Ra isotope activity ratios indicate that recoil is the process generally controlling the Ra isotopic composition in water. Higher isotopic ratios can be explained by different desorption kinetics of Ra. However, the model does not provide an explanation for²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra activity ratios less than unity. From the model, the highest²²²Rn emanation equals 2ɛ. This is in agreement with the hypothesis that²²²Rn activity can be used as a first approximation for input by recoil (Krishnaswamiet al 1982). However, high²²²Rn emanation cannot be explained by production from the surface layer as formulated in the model. Other possibilities involve models including surface precipitation, where the surface layer is not in steady-state.     

Rates and Timescales of Fractional Crystallization from 238U-230Th-226Ra Disequilibria in Trachyte Lavas from Longonot Volcano, Kenya

A suite of peralkaline trachytes from Longonot volcano, Kenya,which erupted during the last 6000 years, has been analysedfor major and trace elements, Pb and Nd isotopes, and U–Th–Radisequilibria. The lavas are divided into three stratigraphicgroups of trachytes (Lt²a, Lt²b and Lt³), and hybrid lavas,designated LMx¹ and LMx², which, respectively, pre-date andpost-date the Lt² lavas. Major and trace elements are consistent,with up to 37% within-group fractional crystallization of predominantlyalkali feldspar. The parental magma for the different trachytegroups had a more mafic composition—probably hawaiitic.Nd and Pb isotopes show minimal variation, both within and betweenmagma groups, and indicate that up to 10% comendite magma fromthe neighbouring Olkaria volcanic field may have intermixedwith the Longonot magma. (²³⁰Th/²³⁸U) disequilibria indicatethat limited U/Th fractionation occurred during the past 10kyr, whereas (²²⁶Ra/²³⁰Th) disequilibria reflect the effectof alkali feldspar fractionation >8 kyr ago in the Lt²a lavas,between 3 and 7 kyr ago in the Lt²b lavas and in the past 3kyr for the Lt³ lavas. (²²⁶Ra/²³⁰Th) disequilibria in the Lt²blavas are interpreted using a model that combines the equationsof radioactive decay and in-growth with Rayleigh crystallizationto give fractionation rates of about 0·2 x 10^–4/yearfor the evolution of hawaiite to trachyte, but more rapid ratesof up to 3 x 10^–4/year for fractionation within the trachytesequence. (²²⁶Ra/²³⁰Th) from two whole-rock–alkali feldsparpairs are interpreted to show the crystals formed at 5800 yearsBP (Lt²b) and 2800 years BP (Lt³), implying that phenocrystformation continued almost up to the time of eruption. The resultsstrongly indicate that fractionated magmas can be stored forperiods on the order of 1000–2500 years prior to eruption,whereas other magmas were erupted as fractionation was proceeding. KEY WORDS: trachyte; magma chambers; u-series; Kenya     

Porosity of the melting zone and variations in the solid mantle upwelling rate beneath Hawaii: inferences from 238U-230Th-226Ra and 235U-231Pa disequilibria

Measurements of ²³⁸U-²³⁰Th-²²⁶Ra and ²³⁵U-²³¹Pa disequilibria in a suite of tholeiitic-to-basanitic lavas provide estimates of porosity, solid mantle upwelling rate and melt transport times beneath Hawaii. The observation that (²³⁰Th/²³⁸U) > 1 indicates that garnet is required as a residual phase in the magma sources for all of the lavas. Both chromatographic porous flow and dynamic melting of a garnet peridotite source can adequately explain the combined U-Th-Ra and U-Pa data for these Hawaiian basalts. For chromatographic porous flow, the calculated maximum porosity in the melting zone ranges from 0.3–3% for tholeiites and 0.1–1% for alkali basalts and basanites, and solid mantle upwelling rates range from 40 to 100 cm yr⁻¹ for tholeiites and from 1 to 3 cm yr⁻¹ for basanites. For dynamic melting, the escape or threshold porosity is 0.5–2% for tholeiites and 0.1–0.8% for alkali basalts and basanites, and solid mantle upwelling rates range from 10 to 30 cm yr⁻¹ for tholeiites and from 0.1 to 1 cm yr⁻¹ for basanites. Assuming a constant melt productivity, calculated total melt fractions range from 15% for the tholeiitic basalts to 3% for alkali basalts and basanites.     

中国东部全新世火山的镭-钍同位素年代学

活火山是指1万年来有过喷发历史的全新世火山。火山的高分辨年代学对火山灾害评估和火山分类具有重要意义。对于缺乏历史记载的全新世火山,直接对火山岩进行同位素定年很困难。本文利用具有高时间分辨率的镭-钍-铀非平衡确定中国东部年轻火山的年龄。根据镭-钍-铀同位素,海南岛的马鞍岭和雷虎岭是全新世火山(马鞍岭:4.3ka;雷虎岭:4.7ka);镜泊湖火山(4.9ka)也是全新世火山;龙岗火山存在晚更新世和全新世活动(7.0ka,15.0ka);大兴安岭阿尔山和诺敏河Ra/Th非平衡消失但~(230)Th/~(238)U非平衡显著,属于晚更新世喷发(阿尔山:63ka;诺敏河:71ka)。海南岛的马鞍岭火山、雷虎岭火山和东北地区的龙岗火山、镜泊湖火山,是4座活火山。至于东北地区的阿尔山和诺敏河火山是否是活火山,有待测试更多样品的Ra/Th同位素。五大连池老黑山和火烧山有历史喷发记录,这与它们都存在显著Ra/Th非平衡一致。五大连池老黑山和火烧山的岩浆滞留年龄分别小于4.2ka和3.2ka,岩浆上升速率 18～23m/y。     

TIMS测定铀矿石样品中^234U/^238U、^230Th/^232Th、^228Ra/^226Ra的方法研究

研究了TIMS测定铀矿石样品中234U/238U、230Th/232Th、228Ra/226Ra的方法。建立了铀矿石密闭混酸一次溶样的方法和采用阴离子、阳离子和Sr特效树脂逐级离子交换分离纯化U、Th和Ra的流程,满足了TIMS测量要求。测定结果表明：100～1000 ng的天然铀中234U/238U,其测量精密度从静态多接收的2.34%提高到动态多接收的0.47%;对230Th与232Th丰度接近、质量为1μg左右的钍,采用三带点样技术和法拉第多接收技术测定230Th/232Th,其内精度平均值为0.0048%,外精度为0.028%;采用单带加钽发射剂,ETP跳峰测定50～100 fg镭-228稀释剂中的228Ra/226Ra,其内精度小于0.10%,外精度小于0.20%。比较TIMS和HR-ICP-MS、α能谱法测定234U/238U、230Th/232Th、228Ra/226Ra结果,三者结果相吻合。TIMS测量法样品用量少、快速、准确、精密度高,是U、Th、Ra同位素比值测定方法的又一补充。     

Consequences of diffuse and channelled porous melt migration on uranium series disequilibria

Magmas erupted at mid-ocean ridges (MORB) result from decompression melting of upwelling mantle. However, the mechanism of melt transport from the source region to the surface is poorly understood. It is debated whether melt is transported through melt-filled conduits or cracks on short time scales (<∼ 10³ yrs), or whether there is a significant component of slow, equilibrium porous flow on much longer time scales (>∼ 10³-10⁴ yrs). Radiogenic excess ²²⁶Ra in MORB indicates that melt is transported from the melting region on time scales less than the half life of ²²⁶Ra (∼1600 yrs), and has been used to argue for fast melt transport from the base of the melting column. However, excess ²²⁶Ra can be generated at the bottom of the melt column, during the onset of melting, and at the top of the melt column by reactive porous flow. Determining the depth at which ²²⁶Ra is generated is critical to interpreting the rate and mechanism of magma migration. A recent compilation of high quality U-series isotope data show that in many young basalts, ²²⁶Ra excess in MORB is negatively correlated with ²³⁰Th excess. The data suggest that ²²⁶Ra excess is generated independently of ²³⁰Th excess, and cannot be explained by “dynamic” or fractional melting, where observed radiogenic excesses are all generated at the base of the melt column. One explanation is that the negative correlation of activity ratios is a result of mixing of slow moving melt that has travelled through reactive, low-porosity pathways and relatively fast moving melt that has been transported in unreactive high-porosity channels. We investigate this possibility by calculating U-series disequilibria in a melting column in which high-porosity, unreactive channels form within a low-porosity matrix that is undergoing melting. The results show that the negative correlation of ²²⁶Ra and ²³⁰Th excesses observed in MORB can be produced if ∼60% of the total melt flux travels through the low-porosity matrix. This melt maintains ²²⁶Ra excesses via chromatographic fractionation of Ra and Th during equilibrium transport. Melt that travels through the unreactive, high-porosity channels is not able to maintain significant ²²⁶Ra excesses because Ra and Th are not fractionated from each other during transport and the transport time for melt in the channels to reach the top of the melt column is longer than the time scale for ²²⁶Ra excesses to decay. Mixing of melt from the high porosity channels with melt from the low-porosity matrix at the top of the melting column can produce a negative correlation of ²²⁶Ra and ²³⁰Th excesses with the slope and magnitude observed in MORB. This transport process can also account for other aspects of the geochemistry of MORB, such as correlations between La/Yb, α_Sm/Nd, and Th/U and ²²⁶Ra and ²³⁰Th excess.