Neodymium (Nd) isotopes have been increasingly used to trace the modern and past ocean circulation. This assumes that seawater Nd isotope ratios (εNd) effectively fingerprint different water masses and approximate expected values from water mass mixing. However, the decoupling of Nd isotopes and Nd concentration (the “Nd paradox”) in the water column, and the lack of understanding of sources and sinks of Nd, restrain our understanding of the “quasi-conservative” behavior of εNd in seawater. Nd is one of the lanthanide rare earth elements (REEs) with similar chemical characteristics that undergo some degree of fractionation. The shale-normalized REE patterns and REE ratios can be used to investigate potential sources/sinks of REEs. Combining REEs with εNd will provide additional information to study REE cycling in the ocean. To better understand the reliability of εNd as a water mass tracer, 17 high-resolution seawater profiles were sampled meridionally in the Southwest Atlantic (GEOTRACES GA02 Leg 3; RRS James Cook 057) and measured for εNd. This region involves the major water masses in the Atlantic Meridional Overturning Circulation: southward flowing North Atlantic Deep Water (NADW), northward flowing Antarctic Intermediate Water (AAIW) and Antarctic Bottom Water (AABW). Along the cruise track, there are potential sources (eolian dusts, marginal sediments, oceanic volcanism, and nepheloid layer) that could add external Nd to seawater and disturb the “quasi-conservative” behavior of εNd. Our results show strikingly that the Southwest Atlantic transect confirms “quasi-conservative” behavior of εNd in intermediate and deep water. Our evaluations of Nd isotopic deviations (ΔεNd) from conservative behavior show that out of 198 intermediate and deep samples, 49% of ΔεNd-values are within ± 0.25 εNd units (< analytical error: ± 0.30 εNd units) and 84% of ΔεNd-values are within ± 0.75 εNd units. Potential sources that could add external Nd to seawater from oceanic volcanism and the nepheloid layer do not show impact on seawater εNd. Terrigenous sources of Nd (e.g. eolian dusts from Africa and Patagonia, marginal sediments from South America) show influence on surface/subsurface water εNd but this εNd signature is not transferred to intermediate and deep water. To better understand the conservative vs. non-conservative behavior of REEs in the ocean, the dissolved REE concentrations were analyzed for the 17 seawater profiles in the Southwest Meridional Atlantic Transect (GEOTRACES GA02 Leg 3). The shale-normalized REE patterns are consistent with typical seawater patterns. To investigate whether and how much REE concentrations deviate from conservative water mass mixing, the REE concentration deviations were calculated for the intermediate and deep water. It is shown that within the SAMT, the intermediate and deep water REEs generally reflect water mass mixing and nearly conservative behavior. Along this transect, the potential sources that could add external REEs to seawater are dissolution of REEs from eolian dust to the surface/subsurface water, REEs released from dissolution of Fe-Mn oxides in the oxygen depleted zone, REEs from sediments near the continental margin, and dissolution of REEs from deep sea sediments. REEs and Nd isotopes of most intermediate and deep water masses passing the volcanic Rio Grande Rise (RGR) and Vitória-Trindade Ridge (VTR) do not show influence from RGR and VTR. REEs and Nd isotopes of the bottom water Lower Circumpolar Deep Water (LCDW) and AABW passing the RGR are influenced by dissolved REEs from the deep sea sediments. LCDW and AABW passing the VTR are influenced by dissolved REEs from the deep sea sediments as well as the volcanic VTR. In order to better understand the oceanic Nd cycling in the North Pacific, its sources and sinks in seawater must be better characterized. The high εNd of North Pacific Deep Water (NPDW, ~ −4) has been difficult to reconcile with the eolian inputs as reflected in surface waters (e.g. Jones et al., 2008), which have much lower εNd (~ −10), indicating potential addition of a component from Pacific volcanism. In order to constrain the REE sources in the North Pacific, we measured εNd and REEs of seawater from five stations across the subarctic North Pacific sampled by the Innovative North Pacific Experiment (INOPEX) Cruise SO202 (2009). In the surface water (~10 m), the highest εNd is observed at the station closest to the Aleutian-Kamchatka volcanic margin (Northwest station SO202-5), suggesting higher contribution of external REEs from volcanic ashes compared to the other stations. In the shallow water (100-400 m, depending on location), remineralization of REEs from volcanic ashes prevails over Asian dusts at Northwest station SO202-5 and near Japan stations SO202-44, 41, and 39, whereas remineralization of REEs from Asian dusts prevails over volcanic ashes at the Northeast station SO202-32 in the open ocean of the Alaska Peninsula. From the depths of North Pacific Intermediate Water (NPIW) to NPDW, seawater εNd and REEs show conservative water mass mixing of NPIW-NPDW. They also show conservative behavior along the water mass transport paths of NPIW and NPDW. Below the depths of NPDW, addition of external REEs is observed in the vertical profiles of εNd and REEs as well as along the transport path of LCDW. The potential sources that add external REEs to the bottom water are (1) sediments on the Kuril-Kamchatka-Aleutian volcanic margin along the LCDW transport path, and (2) sediments on the seafloor, both of which could interact with seawater and modify the seawater εNd and REE signatures.

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L’objectif de cette thèse est d’apporter de nouvelles contraintes sur l’hydrologie de l’Atlantique Nord-Est et de la Méditerranée occidentale depuis la dernière période glaciaire à partir de l’analyse de la composition isotopique du Nd (εNd) dans des échantillons d’eau de mer ainsi que des coraux profonds et des foraminifères, prélevés dans des carottes sédimentaires marines. Les changements de l’hydrologie des masses d’eau intermédiaire (LIW, MSW, AAIW et masses d’eau intermédiaire des gyres subtropical et subpolaire) ont été plus particulièrement étudiés car leur rôle sur les transferts de sels en Atlantique Nord et in fine sur l’AMOC est actuellement mal contraint. Ce travail a été mené au cours des périodes de changements hydrologiques majeurs et abrupts de l’océan qui se sont produits lors des variations climatiques rapides de la dernière période glaciaire (événements d’Heinrich et cycles de Dansgaard-Oeschger) et lors du dépôt du Sapropel S1 en Méditerranée orientale. Dans un premier volet, nous avons amélioré la couverture spatiale des valeurs d’εNd des masses d’eau de l’Atlantique Nord-Est et de la mer d’Alboran, préalable indispensable pour restituer l’hydrologie passée de ces régions avec le traceur εNd. Nous avons ensuite mis en évidence un changement majeur du schéma de circulation de la Méditerranée occidentale durant la période de dépôt du sapropel S1, marquée par une forte réduction des masses d’eau de la Méditerranée orientale (LIW) au sud de la Sardaigne au profit de celles provenant du Golfe du Lion (WIW). Ce changement hydrologique ainsi que ceux qui s’opèrent en Méditerranée depuis la dernière période glaciaire ne sont pas associés à de fortes modifications des valeurs d’εNd de la LIW de la mer d’Alboran et de la mer des Baléares, suggérant une stabilité de la signature isotopique en Nd de la MOW au cours du temps. Ceci a permis, à partir d’un enregistrement d’εNd obtenus sur des coraux profonds du Golfe de Cadix, de mettre en évidence une contribution plus importante de l’AAIW plus radiogénique et donc une pénétration plus marquée en Atlantique Nord de cette masse d’eau lors des périodes de fortes réductions de l’AMOC, liées à la déstabilisation des calottes de glace de l’Hémisphère Nord. / : The purpose of this thesis is to constrain the hydrology of the North-East Atlantic and western Mediterranean Sea since the last glacial period from neodymium isotopic composition (εNd) measured on seawater, cold water corals and foraminifera. In particular, hydrological changes of intermediate water masses (LIW, AAIW, MSW, mid-subtropical and subpolar gyre water) have been studied as their role on salt budget in North Atlantic and ultimately on AMOC are currently poorly constrained. This work has been conducted at times of major and abrupt hydrological changes that occurred during rapid climatic variations of the last glacial period (Heinrich and Dansgaard-Oeschger events) and during the last sapropel deposit (S1) in eastern Mediterranean Sea. In a first step, we have improved the spatial distribution of water masses εNd values in North-east Atlantic and Alboran Sea, what is an absolute prerequisite in order to track past hydrological changes in these areas with εNd proxy. Next, we have highlighted a major change of the western Mediterranean circulation pattern during the sapropel S1 deposit, which is marked south of Sardinia by a strong reduction of eastern-sourced water masses (LIW) in favor of western-sourced water masses (WIW). This hydrological change as well as those occurring in Mediterranean Sea since the last glacial period was not associated with strong modifications of εNd values in Alboran and Balearic Sea, suggesting a stability of Nd isotopic signature of MOW over the time. This has highlighted, from an εNd record obtained on cold water corals in the Gulf of Cadiz, an enhanced contribution of more radiogenic AAIW and therefore a stronger northward penetration in North Atlantic at times of reduced AMOC linked to iceberg discharges from Northern Hemisphere ice sheets.

Afin d’étudier les changements hydrologiques passés du « lac Noir » (dernière phase lacustre de la mer Noire) et l’expression de la Dernière Déglaciation en Europe centrale, des techniques analytiques variées ont été mises en œuvre sur la carotte MD04-2790 : modélisation, développement de méthodes statistiques, géochimie élémentaire et isotopique. La reconstitution de l’évolution des âges réservoir du « lac Noir » au cours des 30 derniers millénaires a permis de mieux comprendre les réponses hydrologiques du bassin aux changements climatiques (variations du niveau du plan d’eau, phases de stratification, possible déstabilisation d’hydrates de gaz). L’âge de la dernière reconnexion du « lac Noir » avec la mer Méditerranée a été révisé à 9 000 ans BP. L’interprétation des isotopes du Nd en termes de provenance des sédiments a permis de mettre en évidence que les pulses d’eaux de fonte arrivant dans le « lac Noir » au cours de l’événement de Heinrich 1 provenaient de la désintégration de la calotte fennoscandinave. Un mécanisme régional d’interactions climatiques entre lacs proglaciaires et atmosphère a été proposé pour expliquer l’organisation temporelle particulière des pulses d’eaux de fonte. Nos résultats renforcent le paradigme de Denton qui suggère que des stades prolongés sont nécessaires au passage du mode climatique glaciaire au mode interglaciaire. / In order to study the past hydrologic changes of the Black Sea “Lake”, various analytical techniques were applied to study the core MD04-2790: modelling, development of statistical approaches, elemental and isotopic geochemistry. The reconstructed reservoir age changes of the Black Sea “Lake” were interpreted in terms of the hydrologic responses of the lake to glacial/deglacial climate changes (water level change, water column stratification, possible chlatrate dissociation). Calendar age of the Black Sea “Lake” last reconnection to global ocean was also revised to 9,000 yr BP. Finally, drastic changes in &#949;Nd values strongly suggest that sediments deposited in response to Deglacial Water Pulses (DWP) during Heinrich Event 1 (HE1) originated from the Fennoscandian Ice Sheet (FIS), providing the first direct evidence that the Black Sea “Lake” recorded the collapse of the FIS. The peculiar temporal organisation of DWPs suggests outbursts of proglacial lakes into Dniepr catchment as well as regional climatic interactions between proglacial lakes and atmosphere. The HE1-timing of the DWPs occurrence would indicate that FIS was involved in the N-Atlantic circulation reduction that shifted Earth climatic machine towards interglacial conditions in accordance with Denton’s paradigm.

Le Crétacé est décrit comme la période la plus chaude des derniers 300 millions d’années. La circulation océanique et l’origine des eaux profondes alimentant les bassins restent mal connues pour le Crétacé, alors qu’elles sont capitales dans la compréhension du rôle de l’océan dans l’évolution du climat à cette époque. Les isotopes du néodyme (Nd) permettent de tracer la circulation océanique et les échanges entre les masses d’eau, et ont été utilisés pour explorer la circulation océanique globale des océans actuels et dans le passé. La composition isotopique en Nd (εNd) des océans dérive de celle des continents qui les entourent. Les courants océaniques exportent cette signature, et les eaux profondes de chaque bassin océanique ont une composition en Nd qui leur est propre. L’interprétation du signal du Nd des eaux océaniques au Crétacé est rendue difficiles du fait de l'insuffisance de la couverture spatiale et temporelle des données existantes. L’objectif de cette thèse est l’acquisition la signature en Nd sur les marges continentales et dans les régions dépourvues de données pour le Crétacé, en se focalisant prioritairement sur les zones potentielles de production d’eau profonde. L’εNd est analysé à partir d’échantillons de dents de poissons, d’oxydes encroûtant les tests de foraminifères et de fraction détritique extraits des sédiments. Les résultats sont comparés aux données de la littérature afin d’identifier les sources des eaux profondes et leur évolution au cours du Crétacé. Les liens entre les changements océanographiques, paléogéographiques et climatiques sont explorés avec un modèle climatique couplé océan-atmosphère. / The Cretaceous is depicted as the warmest period of the last 300 Ma. The oceanic circulation and location of the source zones of deep-waters are essential to understand the role of oceans in the evolution of the climate during the Cretaceous, yet they remain unclear for this period. The neodymium (Nd) isotopes are used to track oceanic circulation and exchanges between water masses, in both past and modern oceans. The Nd isotope composition (εNd) in the ocean is related to the nature of the surrounding continental landmasses. The oceanic currents transport this isotopic signature, thus every oceanic basin acquires a singular εNd. Unequivocal interpretations of the Cretaceous seawater εNd values stem from the insufficient spatial and temporal cover of available data. This PhD thesis intents to collect the Nd signature of continental margins and in regions without data for the Cretaceous, with special attention given to the potential source zones of deep-water production. Fossil fish teeth, coatings on foraminifera tests and detrital fraction from Cretaceous sediments are analyzed for their εNd. The results are compared to published data sets, in order to identify deep-waters source zones and their evolution throughout the Cretaceous. The links connecting oceanographic, palaeogeographic and climatic changes are investigated with a coupled ocean-atmosphere circulation model.