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• 1. [Article] The response of atmospheric nitrous oxide to climate variations during the last glacial period

  To the best of our knowledge, one or more authors of this paper were federal employees when contributing to this work. This is the publisher’s final pdf. The published article is copyrighted by the American ...

  Citation × Citation Citation Abstract Copy Title: The response of atmospheric nitrous oxide to climate variations during the last glacial period Author: Schwander, Jakob, Baumgartner, Matthias, Eicher, Olivier, Stocker, Thomas F., Schilt, Adrian, Chappellaz, Jérôme, Fischer, Hubertus To the best of our knowledge, one or more authors of this paper were federal employees when contributing to this work. This is the publisher’s final pdf. The published article is copyrighted by the American Geophysical Union and can be found at: http://www.agu.org/journals/gl/. Title: The response of atmospheric nitrous oxide to climate variations during the last glacial period Author: Schwander, Jakob, Baumgartner, Matthias, Eicher, Olivier, Stocker, Thomas F., Schilt, Adrian, Chappellaz, Jérôme, Fischer, Hubertus To the best of our knowledge, one or more authors of this paper were federal employees when contributing to this work. This is the publisher’s final pdf. The published article is copyrighted by the American Geophysical Union and can be found at: http://www.agu.org/journals/gl/. Close

• 2. [Article] Augmenting and interpreting ice core greenhouse gas records

  The three studies that comprise this dissertation seek to answer significant questions in paleoclimatology through unconventional applications of ice core greenhouse gas data. These studies involve different ...

  Citation × Citation Citation Abstract Copy Title: Augmenting and interpreting ice core greenhouse gas records Author: Rosen, Julia L The three studies that comprise this dissertation seek to answer significant questions in paleoclimatology through unconventional applications of ice core greenhouse gas data. These studies involve different gases and span the interval of time between the Last Glacial Maximum and the Industrial Revolution, but are united by their nontraditional use of greenhouse gases and their attempt to realize the potential for greenhouse gases to reveal important information about Earth’s climate. Ever since their discovery, the abrupt climate changes of the last glacial period known as Dansgaard-Oeschger (D-O) events have proved challenging to explain. The dominant hypothesis involves periodic freshwater discharges into the North Atlantic, which may regulate the strength of the Meridional Overturning Circulation (MOC) and its role in transporting heat to high latitudes. These events were not restricted to the North Atlantic, and can also be recognized in paleoclimate archives around the world. However, numerous uncertainties surrounding the mechanism behind D-O events remain, including how they are communicated to low latitudes and whether other hypotheses can be definitively ruled out. To constrain the mechanism behind abrupt climate changes, we investigate the phasing of climate changes in high- and low-latitude regions at the Bølling Transition, the penultimate abrupt warming event of the last glacial period. We use methane and the ¹⁵N/¹⁴N ratio of N₂ from the North Greenland Eemian (NEEM) ice core, which serve as proxies for tropical climate and Greenland temperature, respectively. We find that these gases change synchronously in the ice core record, and use a firn air model together with a Monte Carlo approach to constrain the phase lag to within several decades. Our results indicate that the mechanism behind the Bølling Transition was capable of rapidly transmitting the climate signal across the planet in a matter of years, and must therefore involve components of the climate system that are suitably reactive. The glacial-interglacial change in atmospheric methane concentrations revealed in ice core records has spurred a decade of debate about its cause. The most likely explanations involve dramatic changes in methane emissions, which originate from both high- and low-latitude wetlands. One method of investigating the changing latitudinal distribution of methane sources is to quantify the difference in methane concentrations between Greenland and Antarctica, which changes in proportion to the fraction of methane produced at high northern latitudes. Previous attempts to determine the methane interpolar difference (IPD) abound, but many have been hampered by complications in synchronizing bipolar ice core records and analytical uncertainties. We present the first continuous estimate of the methane IPD across the termination using high-resolution methane data from the NEEM and West Antarctic Ice Sheet (WAIS) Divide ice cores. Our results reveal the dominant role of tropical sources in driving abrupt changes in atmospheric methane concentrations, and show that boreal methane sources were surprisingly insensitive to dramatic climate changes. We hypothesize that changes in Northern Hemisphere snow and ice cover exerted strong control over tropical methane emissions, while gradually increasing solar insolation and land area allowed boreal sources to grow during the termination. We also investigate the IPD across the major climate transitions of the termination, and during four centennial-scale methane variations, and find opposing trends in boreal and tropical source strengths during these transient events. We propose that temporary decoupling of the locus of interhemispheric mixing, the position of the Intertropical Convergence Zone, and tropical precipitation may explain these results. Atmospheric concentrations of nitrous oxide (N₂O) have risen by ~20% from preindustrial to modern times, but the cause of this increase is not fully understood. The change has been previously attributed to various agricultural activities which perturb microbial processes in soils, but exactly how remains an outstanding question with important implications for future mitigation of N₂O emissions. We present the first measurements of the isotopomers of tropospheric N₂O over the interval from 1450 to 1920 CE. Our results confirm that the preindustrial atmosphere was enriched in all isotopes relative to the modern atmosphere. Furthermore, we estimate that the net anthropogenic source of nitrous oxide must be depleted in all heavy isotopes and have a strong site preference, consistent with a strong role for agricultural emissions and characteristic of N₂O derived from nitrification. We also find a large oscillation in the site preference of the ¹⁵N in N₂O during the Little Ice Age between 1500 and 1700 CE. We hypothesize that this excursion may be due to changing climate conditions that led to an increase in the amount of N₂O produced by nitrification vs. denitrification. Title: Augmenting and interpreting ice core greenhouse gas records Author: Rosen, Julia L The three studies that comprise this dissertation seek to answer significant questions in paleoclimatology through unconventional applications of ice core greenhouse gas data. These studies involve different gases and span the interval of time between the Last Glacial Maximum and the Industrial Revolution, but are united by their nontraditional use of greenhouse gases and their attempt to realize the potential for greenhouse gases to reveal important information about Earth’s climate. Ever since their discovery, the abrupt climate changes of the last glacial period known as Dansgaard-Oeschger (D-O) events have proved challenging to explain. The dominant hypothesis involves periodic freshwater discharges into the North Atlantic, which may regulate the strength of the Meridional Overturning Circulation (MOC) and its role in transporting heat to high latitudes. These events were not restricted to the North Atlantic, and can also be recognized in paleoclimate archives around the world. However, numerous uncertainties surrounding the mechanism behind D-O events remain, including how they are communicated to low latitudes and whether other hypotheses can be definitively ruled out. To constrain the mechanism behind abrupt climate changes, we investigate the phasing of climate changes in high- and low-latitude regions at the Bølling Transition, the penultimate abrupt warming event of the last glacial period. We use methane and the ¹⁵N/¹⁴N ratio of N₂ from the North Greenland Eemian (NEEM) ice core, which serve as proxies for tropical climate and Greenland temperature, respectively. We find that these gases change synchronously in the ice core record, and use a firn air model together with a Monte Carlo approach to constrain the phase lag to within several decades. Our results indicate that the mechanism behind the Bølling Transition was capable of rapidly transmitting the climate signal across the planet in a matter of years, and must therefore involve components of the climate system that are suitably reactive. The glacial-interglacial change in atmospheric methane concentrations revealed in ice core records has spurred a decade of debate about its cause. The most likely explanations involve dramatic changes in methane emissions, which originate from both high- and low-latitude wetlands. One method of investigating the changing latitudinal distribution of methane sources is to quantify the difference in methane concentrations between Greenland and Antarctica, which changes in proportion to the fraction of methane produced at high northern latitudes. Previous attempts to determine the methane interpolar difference (IPD) abound, but many have been hampered by complications in synchronizing bipolar ice core records and analytical uncertainties. We present the first continuous estimate of the methane IPD across the termination using high-resolution methane data from the NEEM and West Antarctic Ice Sheet (WAIS) Divide ice cores. Our results reveal the dominant role of tropical sources in driving abrupt changes in atmospheric methane concentrations, and show that boreal methane sources were surprisingly insensitive to dramatic climate changes. We hypothesize that changes in Northern Hemisphere snow and ice cover exerted strong control over tropical methane emissions, while gradually increasing solar insolation and land area allowed boreal sources to grow during the termination. We also investigate the IPD across the major climate transitions of the termination, and during four centennial-scale methane variations, and find opposing trends in boreal and tropical source strengths during these transient events. We propose that temporary decoupling of the locus of interhemispheric mixing, the position of the Intertropical Convergence Zone, and tropical precipitation may explain these results. Atmospheric concentrations of nitrous oxide (N₂O) have risen by ~20% from preindustrial to modern times, but the cause of this increase is not fully understood. The change has been previously attributed to various agricultural activities which perturb microbial processes in soils, but exactly how remains an outstanding question with important implications for future mitigation of N₂O emissions. We present the first measurements of the isotopomers of tropospheric N₂O over the interval from 1450 to 1920 CE. Our results confirm that the preindustrial atmosphere was enriched in all isotopes relative to the modern atmosphere. Furthermore, we estimate that the net anthropogenic source of nitrous oxide must be depleted in all heavy isotopes and have a strong site preference, consistent with a strong role for agricultural emissions and characteristic of N₂O derived from nitrification. We also find a large oscillation in the site preference of the ¹⁵N in N₂O during the Little Ice Age between 1500 and 1700 CE. We hypothesize that this excursion may be due to changing climate conditions that led to an increase in the amount of N₂O produced by nitrification vs. denitrification. Close

• 3. [Article] Sequence of events from the onset to the demise of the Last Interglacial: Evaluating strengths and limitations of chronologies used in climatic archives

  This is the publisher’s final pdf. The published article is copyrighted by the author(s) and published by Elsevier. The published article can be found at: http://www.journals.elsevier.com/quaternary-sc...

  Citation × Citation Citation Abstract Copy Title: Sequence of events from the onset to the demise of the Last Interglacial: Evaluating strengths and limitations of chronologies used in climatic archives Author: Masson-Delmotte, V., Waelbroeck, C., Blunier, T., Capron, E., Tzedakis, P. C., Hillaire-Marcel, C., Seidenkrantz, M.-S., Zahn, R., Ghaleb, B., Veres, D., Bazin, L., Bassinot, F., Jimenez-Amat, P., Landais, A., Govin, A., St-Onge, G., Martrat, B., Parrenin, F., Genty, D., Verheyden, S., Stoner, J. S., Gersonde, R., Combourieu-Nebout, N., El Ouahabi, A. This is the publisher’s final pdf. The published article is copyrighted by the author(s) and published by Elsevier. The published article can be found at: http://www.journals.elsevier.com/quaternary-science-reviews/ Title: Sequence of events from the onset to the demise of the Last Interglacial: Evaluating strengths and limitations of chronologies used in climatic archives Author: Masson-Delmotte, V., Waelbroeck, C., Blunier, T., Capron, E., Tzedakis, P. C., Hillaire-Marcel, C., Seidenkrantz, M.-S., Zahn, R., Ghaleb, B., Veres, D., Bazin, L., Bassinot, F., Jimenez-Amat, P., Landais, A., Govin, A., St-Onge, G., Martrat, B., Parrenin, F., Genty, D., Verheyden, S., Stoner, J. S., Gersonde, R., Combourieu-Nebout, N., El Ouahabi, A. This is the publisher’s final pdf. The published article is copyrighted by the author(s) and published by Elsevier. The published article can be found at: http://www.journals.elsevier.com/quaternary-science-reviews/ Close

• 4. [Article] Carbon cycle variability during the last millennium and last deglaciation

  The exchange of carbon on earth is one of the fundamental processes that sustains life and regulates climate. Since the onset of the Industrial Revolution, the burning of fossil fuels and anthropogenic ...

  Citation × Citation Citation Abstract Copy Title: Carbon cycle variability during the last millennium and last deglaciation Author: Bauska, Thomas K. The exchange of carbon on earth is one of the fundamental processes that sustains life and regulates climate. Since the onset of the Industrial Revolution, the burning of fossil fuels and anthropogenic land conversion have altered the carbon cycle, increasing carbon dioxide in the atmosphere to levels that are unprecedented in the last 800,000 years. This rapid rise in atmospheric carbon dioxide is driving current climate change and further increases are projected to dominate future climate change. However, the fate of the carbon cycle in response to climate change remains uncertain. Insight into how the carbon cycle may change in the future can come from an understanding how it has changed in the past. Key constraints on past carbon cycle variability come from the concentration and stable isotopic composition of atmospheric carbon dioxide recorded in polar ice cores, but reconstructing these histories has been a significant analytical challenge. This thesis presents a new, more precise method for measuring the stable isotopic composition of carbon in carbon dioxide (δ¹³C of CO₂) from polar ice. The new method is then used to reconstruct the atmospheric history of δ¹³C of CO₂ during the last millennium (~770-1900 C.E.) and last deglaciation (~20,000-10,000 years before present). Previously, methods for measuring the δ¹³C of CO₂ had been limited to precision of greater than ±0.05‰. The method presented here combines an ice grater air extraction method and micro-volume equipped dual-inlet mass spectrometer to make high-precision measurements on very small samples of fossil CO₂. The precision as determined by replicate analysis is ±0.018‰. The method also provides high-precision measurements of the CO₂ (±2 ppm) and N2O (±4 ppb). A new high-resolution (~20 year spacing) record of the δ¹³C of CO₂ from 770-1900 C.E is presented that suggests land carbon controlled atmospheric CO₂ variability prior to the Industrial Revolution. A deconvolution of the CO₂ fluxes to the atmosphere provides a well-constrained estimate of the evolution of land carbon stocks. The relationship between climate and land carbon for this time period constrains future climate-carbon cycle sensitivity, but an additional process affecting land carbon is required to explain the data. This missing process may be related to early anthropogenic land cover change or patterns of drought. A long-standing problem in the field of paleoclimatology is a complete mechanistic understanding of the 80 ppm increase in atmospheric CO₂ during the last deglaciation. A horizontal ice core on the Taylor Glacier in Antarctica allowed for the recovery of well-dated, large ice samples spanning the last deglaciation. From this unique archive, a new δ¹³C of CO₂ of very high resolution (50-150 year spacing) is reconstructed. A box model of the carbon cycle is used to construct a framework of the evolution of the carbon cycle during deglaciation. During the Last Glacial Maximum, the lower CO₂ concentration accompanied by only a minor shift in δ¹³C of CO₂ relative to the early Holocene is consistent with a more efficient biological pump in the Southern ocean, limited air-sea gas exchange around Antarctica, and colder ocean temperatures. The temporal evolution of these factors, as informed by timing of proxy data, reconciles the non-linear relationship between CO₂ and δ¹³C of CO₂ from the Last Glacial Maximum to the pre-Industrial. However, the data also reveal very fast changes in δ¹³C of CO₂ that suggest a rapid emission of depleted carbon to the atmosphere on the centennial timescale that is not captured in current models. Title: Carbon cycle variability during the last millennium and last deglaciation Author: Bauska, Thomas K. The exchange of carbon on earth is one of the fundamental processes that sustains life and regulates climate. Since the onset of the Industrial Revolution, the burning of fossil fuels and anthropogenic land conversion have altered the carbon cycle, increasing carbon dioxide in the atmosphere to levels that are unprecedented in the last 800,000 years. This rapid rise in atmospheric carbon dioxide is driving current climate change and further increases are projected to dominate future climate change. However, the fate of the carbon cycle in response to climate change remains uncertain. Insight into how the carbon cycle may change in the future can come from an understanding how it has changed in the past. Key constraints on past carbon cycle variability come from the concentration and stable isotopic composition of atmospheric carbon dioxide recorded in polar ice cores, but reconstructing these histories has been a significant analytical challenge. This thesis presents a new, more precise method for measuring the stable isotopic composition of carbon in carbon dioxide (δ¹³C of CO₂) from polar ice. The new method is then used to reconstruct the atmospheric history of δ¹³C of CO₂ during the last millennium (~770-1900 C.E.) and last deglaciation (~20,000-10,000 years before present). Previously, methods for measuring the δ¹³C of CO₂ had been limited to precision of greater than ±0.05‰. The method presented here combines an ice grater air extraction method and micro-volume equipped dual-inlet mass spectrometer to make high-precision measurements on very small samples of fossil CO₂. The precision as determined by replicate analysis is ±0.018‰. The method also provides high-precision measurements of the CO₂ (±2 ppm) and N2O (±4 ppb). A new high-resolution (~20 year spacing) record of the δ¹³C of CO₂ from 770-1900 C.E is presented that suggests land carbon controlled atmospheric CO₂ variability prior to the Industrial Revolution. A deconvolution of the CO₂ fluxes to the atmosphere provides a well-constrained estimate of the evolution of land carbon stocks. The relationship between climate and land carbon for this time period constrains future climate-carbon cycle sensitivity, but an additional process affecting land carbon is required to explain the data. This missing process may be related to early anthropogenic land cover change or patterns of drought. A long-standing problem in the field of paleoclimatology is a complete mechanistic understanding of the 80 ppm increase in atmospheric CO₂ during the last deglaciation. A horizontal ice core on the Taylor Glacier in Antarctica allowed for the recovery of well-dated, large ice samples spanning the last deglaciation. From this unique archive, a new δ¹³C of CO₂ of very high resolution (50-150 year spacing) is reconstructed. A box model of the carbon cycle is used to construct a framework of the evolution of the carbon cycle during deglaciation. During the Last Glacial Maximum, the lower CO₂ concentration accompanied by only a minor shift in δ¹³C of CO₂ relative to the early Holocene is consistent with a more efficient biological pump in the Southern ocean, limited air-sea gas exchange around Antarctica, and colder ocean temperatures. The temporal evolution of these factors, as informed by timing of proxy data, reconciles the non-linear relationship between CO₂ and δ¹³C of CO₂ from the Last Glacial Maximum to the pre-Industrial. However, the data also reveal very fast changes in δ¹³C of CO₂ that suggest a rapid emission of depleted carbon to the atmosphere on the centennial timescale that is not captured in current models. Close