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Made available in DSpace on 2014-10-09T12:32:11Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:09:36Z (GMT). No. of bitstreams: 1 02469.pdf: 6886157 bytes, checksum: 5f8e19151fe770d09c221c405058d58e (MD5) / Tese (Doutoramento) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Changes in monsoon patterns not only affect ecosystems and societies but also the global climate system in terms of heat energy and humidity transfer from the equator to higher latitudes. However, understanding the mechanisms that drive monsoon variability on longer timescales remains a challenge, partly due to sparse paleoenvironmental and paleoclimatic data. This thesis, which contributes new hydroclimate data sets for the Asian monsoon region, seeks to advance our understanding of the mechanisms that contributed to Southeast Asian summer monsoon variability in the past. Moreover, it explores how past climatic conditions may have impacted societies and ecosystems. In this study lake sediment and peat sequences from northeastern and southern Thailand have been investigated using organic geochemistry, and more specifically the stable carbon and hydrogen isotopic composition of specific biomarkers (n-alkanes, botryococcenes, and highly branched isoprenoids). The hydrogen isotopic composition of leaf waxes (δDwax) in Thailand was shown to relate to the amount of precipitation and the extent of the El Niño Southern Oscillation.  Higher values of δDwax can be interpreted as reflecting relatively dry climatic conditions, whereas lower values relate to wetter conditions. The hydroclimate reconstruction for northeastern Thailand, based on the sedimentary record of Lake Kumphawapi, suggests higher moisture availability between ca. 10,700 cal. BP and ca. 7,000 cal. BP likely related to a strengthened early Holocene summer monsoon. Moisture availability decreased during the mid-Holocene, but seems to have increased again around 2,000 years ago and has fluctuated since. The high-resolution Lake Pa Kho peat sequence, which allows for a sub-centennial reconstruction of moisture availability, indicates that the wettest period occurred between ca. 700 and ca. 1000 CE whereas driest intervals were from ca. 50 BCE to ca. 700 CE and from ca. 1300 to ca. 1500 CE. Hydroclimate comparison of Pa Kho’s δDwax record with other paleoclimate records from the Asian-Pacific region suggests that El Niño-like conditions led to Northeastern Thailand being wetter, whereas La Niña-like conditions led to drier conditions. Regional hydroclimate variability also greatly influenced the Angkor Civilization, which flourished between ca. 845 and ca. 1450 CE. The shift from drier to wetter conditions coincided in time with the rise of the Angkor Civilization and likely favored the intense agriculture needed to sustain the empire. The gradual decline in moisture availability, which started after ca. 1000 years CE, could have stretched the hydrological capacity of Angkor to its limit. It is suggested that Angkor’s population resorted to unconventional water sources, such as wetlands, as population growth continued, but summer monsoon rains weakened. The 150-year long record of Lake Nong Thale Prong in southern Thailand offers insights into decadal-scale hydroclimatic changes that can be connected to the instrumental record. δDwax-based hydroclimate was drier from ~1857 to 1916 CE and ~1970 to 2010 CE and wetter from ~1916 to 1969 CE. Drier climatic conditions between ~1857 and 1916 CE coincided with oligotrophic lake waters and a dominance of the green algae Botryococcus braunii. Higher rainfall between ~1916 and 1969 CE concurred with an increase in diatom blooms while eutrophic lake water conditions were established between ~1970–2010 CE. / <p>At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 2: Submitted. Paper 3: Manuscript.</p> / Monsoon project

The large amount of turquoise artifacts recovered from archaeological sites in the American Southwest and Mesoamerica suggests that turquoise was an important commodity in pre-Columbian trade networks. However, the spatial and temporal patterns of turquoise exchange networks and the provenance regions of the turquoise in the southwestern United States and Mesoamerica are poorly understood. Turquoise (CuAl6(PO4)4(OH)8•4(H2O)) is a supergene mineral that forms from meteoric water along fractures that are often associated with copper porphyry deposits. This copper-rich mineral can range in color and chemistry within a single sample or deposit. The ability to identify the turquoise resource areas of turquoise artifacts using the stable isotopes of hydrogen (2H/1H) and copper (65Cu/63Cu) has overcome many of the limitations of trace element analyses of complex minerals such as turquoise. The geography and geology of turquoise deposits dictate the isotopic composition of turquoise. Employing the Secondary Ion Mass Spectrometry (SIMS) technique to measure the hydrogen and copper stable isotope ratios in turquoise samples, a comparative reference database consisting of 876 analyses from 21 turquoise resource areas in the western United States was established. Sixty-two turquoise artifacts recovered from Aztec Ruin, Salmon Ruin, and nine sites in Chaco Canyon were analyzed and their isotopic signatures were compared to the reference database identifying the turquoise resource areas of 35 artifacts. These results were compared to pre-existing models of trade and exchange in the American Southwest and models that explain the complex culture history of the inhabitants of these sites. The results showed that turquoise was obtained from several different turquoise provenance regions across the western United States and there are notable differences in the turquoise procurement patterns between the three major great houses and between Pueblo Bonito and the small sites within Chaco Canyon. The results from this study improved the understanding of turquoise trade and relationships among the occupants of important Ancestral Puebloan sites in northwestern New Mexico. The development of the turquoise comparative reference database established the foundation of future research for reconstruction of ancient turquoise trade networks and investigation of turquoise procurement strategies in the American Southwest and Mesoamerica.

The large amount of turquoise artifacts recovered from archaeological sites in the American Southwest and Mesoamerica suggests that turquoise was an important commodity in pre-Columbian trade networks. However, the spatial and temporal patterns of turquoise exchange networks and the provenance regions of the turquoise in the southwestern United States and Mesoamerica are poorly understood. Turquoise (CuAl6(PO4)4(OH)8•4(H2O)) is a supergene mineral that forms from meteoric water along fractures that are often associated with copper porphyry deposits. This copper-rich mineral can range in color and chemistry within a single sample or deposit. The ability to identify the turquoise resource areas of turquoise artifacts using the stable isotopes of hydrogen (2H/1H) and copper (65Cu/63Cu) has overcome many of the limitations of trace element analyses of complex minerals such as turquoise. The geography and geology of turquoise deposits dictate the isotopic composition of turquoise. Employing the Secondary Ion Mass Spectrometry (SIMS) technique to measure the hydrogen and copper stable isotope ratios in turquoise samples, a comparative reference database consisting of 876 analyses from 21 turquoise resource areas in the western United States was established. Sixty-two turquoise artifacts recovered from Aztec Ruin, Salmon Ruin, and nine sites in Chaco Canyon were analyzed and their isotopic signatures were compared to the reference database identifying the turquoise resource areas of 35 artifacts. These results were compared to pre-existing models of trade and exchange in the American Southwest and models that explain the complex culture history of the inhabitants of these sites. The results showed that turquoise was obtained from several different turquoise provenance regions across the western United States and there are notable differences in the turquoise procurement patterns between the three major great houses and between Pueblo Bonito and the small sites within Chaco Canyon. The results from this study improved the understanding of turquoise trade and relationships among the occupants of important Ancestral Puebloan sites in northwestern New Mexico. The development of the turquoise comparative reference database established the foundation of future research for reconstruction of ancient turquoise trade networks and investigation of turquoise procurement strategies in the American Southwest and Mesoamerica.

No description available.

During the "Green Sahara" period (11,000 to 5000 years before the present), the Sahara desert received high amounts of rainfall, supporting diverse vegetation, permanent lakes, and human populations. Our knowledge of rainfall rates and the spatiotemporal extent of wet conditions has suffered from a lack of continuous sedimentary records. We present a quantitative reconstruction of western Saharan precipitation derived from leaf wax isotopes in marine sediments. Our data indicate that the Green Sahara extended to 31 degrees N and likely ended abruptly. We find evidence for a prolonged "pause" in Green Sahara conditions 8000 years ago, coincident with a temporary abandonment of occupational sites by Neolithic humans. The rainfall rates inferred from our data are best explained by strong vegetation and dust feedbacks; without these mechanisms, climate models systematically fail to reproduce the Green Sahara. This study suggests that accurate simulations of future climate change in the Sahara and Sahel will require improvements in our ability to simulate vegetation and dust feedbacks.

Ce travail a pour objectif de développer un nouvel indicateur quantitatif des conditions hydrologiques passées fondé sur la composition isotopique en hydrogène (δD) d’un biomarqueur sédimentaire spécifique du millet commun (Panicum miliaceum), la miliacine. L’étude de la pertinence spatio-temporelle de cet indicateur révèle que le δD miliacine de plants de millet dans un champ, bien que dispersé, suit une loi gaussienne. Le δD miliacine du sol correspond au δD miliacine des plantes cultivées l’année précédente. L’évolution interannuelle du δD miliacine est globallement parallèle à celle du δD des eaux météoriques, les différences pouvant être attribuées à des différences d’humidité. La comparaison des valeurs de δD miliacine dans des sédiments du même âge prélevés sur deux archives distinctes dans le Lac du Bourget témoigne que l’archivage de cet indicateur est intègre de manière homogène les conditions climatiques ayant régné dans le bassin versant. La culture de millet en chambre climatique démontre que, si le δD de l’eau de source est le principal facteur controlant le δD miliacine, ce dernier est très étroitement corrélé au δD de l’eau de la feuille. De légères différences de fractionnement biosynthétique net entre n-alcanes et miliacine sous deux conditions d’humidité laissent supposer que l’analyse combinée de biomarqueurs sédimentaires issus de voies synthétiques distinctes permettrait d’accéder à la fois aux variables paléoenvironnementales clé que sont le δD de l’eau de source et l’humidité. / This work aims at developing a new proxy of past hydrological conditions based on the hydrogen isotopic composition (δD) of a sedimentary biomarker that is specific for broomcorn millet (Panicum miliaceum), miliacin. Analysing the spatio-temporal relevancy of this proxy reveals that miliacin δD values of plants cultivated in the field, although dispersed, follow a Gaussian law. Soil miliacin δD values are the same as those found for plants grown the year before. Interannual variations in plant miliacin δD values roughly parallel those of precipitation δD values, slight differences being attributed to differences in relative humidity. The comparison of miliacin δD values in sediments deposited in two distinct settings at the same time in Lake le Bourget attests that this proxy homogeneously integrates climatic conditions over the whole catchment. Cultivation of millet plants in climatic chambers allowed demonstrating that, although source water δD is the principal controlling miliacin δD values, this later is closely correlated to leaf water δD. Slight differences in net biosynthetic fractionation between n-alcanes and miliacin under two relative humidity levels imply that the combined analysis of sedimentary biomarkers produced through distinct biosynthetic pathways could help discriminating between source water δD and relative humidity in paleoenvironmental studies.

The electric charge distribution of molecules such as H₂ and D₂ is inversion-symmetric so that permanent dipole moments do not exist: such molecules are infrared-inactive. It is therefore interesting that gaseous, liquid, and solid hydrogen and its isotopes actually absorb infrared radiation, for example if gas densities are sufficiently high. The observed absorption arises from electric dipole moments induced by intermolecular interactions. It is of a supermolecular origin, due to binary (or higher-order) molecular complexes that may be transient (i.e., in a collisional encounter) or relatively stable (van-der-Waals molecule). Interaction-induced electric dipoles arise from the same mechanisms that generate the intermolecular forces: exchange forces, dispersion forces, and multipolar induction. Recently the induced dipole and potential energy surfaces of H₂ pairs have been obtained by advanced quantum-chemical calculations. Interaction-induced absorption, more commonly called collision-induced absorption (CIA), by H₂ pairs is an important opacity source in the atmospheres of various types of planets and cool stars, such as late stars, low-mass stars, brown dwarfs, certain white dwarfs, etc., and therefore of special astronomical interest. The emission spectra of cool white dwarf stars differ significantly from the expected blackbody spectra of their cores, mainly due to collision-induced absorption by collisional complexes of hydrogen and helium in the stellar atmospheres. Before proceeding to the frequencies and temperatures of interest it is good to check the new potential energy surface and induced dipole surface in all possible ways by comparison with existing isotopic laboratory measurements. Furthermore, the new potential energy surface is directly compared with previously available, well established intermolecular potential energy surfaces. The electric charge distributions of deuterium and hydrogen are very similar. The new potential energy and induced dipole surfaces were originally obtained to facilitate the computation of the collision-induced absorption of hydrogen. However, by replacing the rotovibrational wavefunctions of H₂ with those of D₂ the surfaces can also be used to calculate the collision-induced absorption of deuterium pairs, thereby probing them further. At the temperature of 298K existing measurements of the collision-induced absorption of D₂--D₂ gas are compared with our quantum scattering calculations in the D₂ fundamental band (approximately 2,500cm⁻¹ to 4,500cm⁻¹). Furthermore, measurements of the collision-induced absorption of deuterium (D₂) in the D₂ first overtone band (about 5,250cm⁻¹ to 7,250cm⁻¹) at 201K are reported. These measurements are compared with ab initio calculations of the absorption spectra. Close agreement of measured and calculated spectra is seen.

Lors de l’opération d’ITER, des flux importants d’isotopes d’hydrogène (HI) constituant le fuel interagissent avec les composants face au plasma (CFP) de la machine. Dans le cas du Tungstène (W) composant le divertor qui est la zone la plus exposée aux interactions plasma paroi, le flux incident est implanté et diffuse ensuite dans le corps du matériau entrainant un piégeage du fuel. Pour des raisons de sureté, l’inventaire de Tritium retenu dans les parois d’ITER est limité. De plus, le dégazage du fuel depuis les parois vers le plasma, lors des opérations plasma peut avoir un impact sur le contrôle global du plasma. Le but de cette thèse est d’abord de déterminer les paramètres de piégeages du fuel dans le W (énergies/températures de dépiégeage, concentrations de pièges) grâce à la modélisation de résultats expérimentaux. Ces simulations de résultats expérimentaux montrent que l’implantation d’HIs dans le W peut induire, sous certaines conditions, la formation de lacunes contenant des impuretés. En plus de ce piège induit par l’implantation d’ions, 2 pièges intrinsèques sont présents dans le W. Ces 3 pièges retiennent les HIs jusqu’à 700 K. Enfin, il est montré que le W endommagé par des ions lourds ou des neutrons contient des dislocations, des boucles de dislocations et des cavités retenant les HIs jusqu’à 1000 K.Après avoir déterminé ces paramètres de piégeages des HIs dans le W, la rétention des HIs durant l’opération d’ITER est estimée. Lors de cette opération, la température des CFP W atteint environ 1000 K. Les simulations montrent donc que la rétention dans les CFPs non endommagé est bien plus faible que dans le cas d’un CFP endommagé. / During ITER operation, important flux of Hydrogen Isotopes (HIs) constituting the fuel interact with the plasma facing components (PFC) of the machine. In the case of tungsten (W) making the divertor which is the most exposed area to the plasma wall interaction, the incident flux can be implanted and diffuse inside the bulk material inducing a trapping of the fuel. To safety issue, the tritium inventory retained in ITER’s PFC is limited. In addition, the outgassing of the fuel during plasma operation can impact the edge plasma control.The aim of this PhD project is first to determined relevant trapping parameters of the fuel in W (detrapping energies/temperatures and trap concentrations) by modelling experimental results. The simulations of experimental results shows that under specific condition, the HI implantation can induce the formation of mono-vacancies containing impurities. In addition to this induced trap, 2 intrinsic traps are present in W. This 3 traps retain HIs up to 700 K. Finally, it has been shown that the damaged W by heavy ions or neutrons contains dislocations, dislocation loops and cavities that can trap HIs up to 1000 K.After determining the fuel retention properties of W, the HIs retention during ITER operation is estimated. During this operation, the PFC temperature reaches around 1000 K so the simulations show that the damaged W retains much more HIs than the undamaged W.