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Climatic variabilities on millennial and longer time scales with a bipolar seesaw pattern have been documented in paleoclimatic records, but their frequencies, relationships with mean climatic state, and mechanisms remain unclear. Understanding the processes and sensitivities that underlie these changes will underpin better understanding of the climate system and projections of its future change. We investigate the long-term characteristics of climatic variability using a new ice-core record from Dome Fuji, East Antarctica, combined with an existing long record from the Dome C ice core. Antarctic warming events over the past 720, 000 years are most frequent when the Antarctic temperature is slightly below average on orbital time scales, equivalent to an intermediate climate during glacial periods, whereas interglacial and fully glaciated climates are unfavourable for a millennial-scale bipolar seesaw. Numerical experiments using a fully coupled atmosphere-ocean general circulation model with freshwater hosing in the northern North Atlantic showed that climate becomes most unstable in intermediate glacial conditions associated with large changes in sea ice and the Atlantic Meridional Overturning Circulation. Model sensitivity experiments suggest that the prerequisite for the most frequent climate instability with bipolar seesaw pattern during the late Pleistocene era is associated with reduced atmospheric CO2 concentration via global cooling and sea ice formation in the North Atlantic, in addition to extended Northern Hemisphere ice sheets.

Climatic variabilities on millennial and longer time scales with a bipolar seesaw pattern have been documented in paleoclimatic records, but their frequencies, relationships with mean climatic state, and mechanisms remain unclear. Understanding the processes and sensitivities that underlie these changes will underpin better understanding of the climate system and projections of its future change. We investigate the long-term characteristics of climatic variability using a new ice-core record from Dome Fuji, East Antarctica, combined with an existing long record from the Dome C ice core. Antarctic warming events over the past 720,000 years are most frequent when the Antarctic temperature is slightly below average on orbital time scales, equivalent to an intermediate climate during glacial periods, whereas interglacial and fully glaciated climates are unfavourable for a millennial-scale bipolar seesaw. Numerical experiments using a fully coupled atmosphere-ocean general circulation model with freshwater hosing in the northern North Atlantic showed that climate becomes most unstable in intermediate glacial conditions associated with large changes in sea ice and the Atlantic Meridional Overturning Circulation. Model sensitivity experiments suggest that the prerequisite for the most frequent climate instabilitywith bipolar seesaw pattern during the late Pleistocene era is associated with reduced atmospheric CO2 concentration via global cooling and sea ice formation in the North Atlantic, in addition to extended Northern Hemisphere ice sheets.

The flux and chemical composition of aerosols impact the climate. Antarctic ice cores preserve the record of past atmospheric aerosols, providing useful information about past atmospheric environments. However, few studies have directly measured the chemical composition of aerosol particles preserved in ice cores. Here we present the chemical compositions of sulfate and chloride salts from aerosol particles in the Dome Fuji ice core. The analysis method involves ice sublimation, and the period covers the last termination, 25.0-11.0 thousand years before present (kyr B.P.), with a 350 year resolution. The major components of the soluble particles are CaSO4, Na2SO4, and NaCl. The dominant sulfate salt changes at 16.8 kyr B.P. from CaSO4, a glacial type, to Na2SO4, an interglacial type. The sulfate salt flux (CaSO4 plus Na2SO4) inversely correlates with delta O-18 in Dome Fuji over millennial timescales. This correlation is consistent with the idea that sulfate salt aerosols contributed to the last deglacial warming of inland Antarctica by reducing the aerosol indirect effect. Between 16.3 and 11.0 kyr B.P., the presence of NaCl suggests that winter atmospheric aerosols are preserved. A high NaCl/Na2SO4 fraction between 12.3 and 11.0 kyr B.P. indicates that the contribution from the transport of winter atmospheric aerosols increased during this period.

Most of the aerosol particles present in the surface snow and ice of inland Antarctica come from primary sea salt (sodium chloride) and marine biological activity (methansulfonic and sulfuric acids). Melted water from surface snow, firn, and Holocene ice contains mainly sodium, chloride, and sulfate ions. Although it is well known that sea salt aerosols react rapidly with sulfuric acid, a process known as sulfatization, it is not known when this process takes place. In this research we undertake to measure the proportion of sea salt aerosols that undergo sulfatization in the atmosphere and surface snow, as opposed to deeper ice, in order to understand the suitability of sea salt aerosols as a proxy for past climates in deep ice cores. We directly measure the sulfatization rates in recently fallen snow (0-4 m in depth) collected at the Dome Fuji station, using X-ray dispersion spectroscopy to determine the constituent elements of soluble particles and computing the molar ratios of sodium chloride and sodium sulfate. We estimate that about 90% of the initial sea salt aerosols sulfatize as they are taken up by precipitation over Dome Fuji or in the snowpack within one year after being deposited on the ice sheet., 10

Most of the aerosol particles present in the surface snow and ice of inland Antarctica come from primary sea salt (sodium chloride) and marine biological activity (methansulfonic and sulfuric acids). Melted water from surface snow, firn, and Holocene ice contains mainly sodium, chloride, and sulfate ions. Although it is well known that sea salt aerosols react rapidly with sulfuric acid, a process known as sulfatization, it is not known when this process takes place. In this research we undertake to measure the proportion of sea salt aerosols that undergo sulfatization in the atmosphere and surface snow, as opposed to deeper ice, in order to understand the suitability of sea salt aerosols as a proxy for past climates in deep ice cores. We directly measure the sulfatization rates in recently fallen snow (0-4 m in depth) collected at the Dome Fuji station, using X-ray dispersion spectroscopy to determine the constituent elements of soluble particles and computing the molar ratios of sodium chloride and sodium sulfate. We estimate that about 90% of the initial sea salt aerosols sulfatize as they are taken up by precipitation over Dome Fuji or in the snowpack within one year after being deposited on the ice sheet.

We describe in detail our method of measuring the chemical forms of microparticles in polar ice samples through micro-Raman spectroscopy. The method is intended for solid ice samples, an important point because melting the ice can result in dissociation, contamination, and chemical reactions prior to or during a measurement. We demonstrate the technique of measuring the chemical forms of these microparticles and show that the reference spectra of those salts expected to be common in polar ice are unambiguously detected. From our measurements, Raman intensity of sulfate salts is relatively higher than insoluble dust due to the specific Raman scattering cross-section of chemical forms of microparticles in ice.

We provide the first direct evidence that a number of water-soluble compounds, in particular calcium sulfate (CaSO4·2H2O) and calcium carbonate (CaCO3), are present as solid, micron-sized inclusions within the Greenland GRIP ice core. The compounds are detected by two independent methods: micro-Raman spectroscopy of a solid ice sample, and energy-dispersive X-ray spectroscopy of individual inclusions remaining after sublimation. CaSO4·2H2O is found in abundance throughout the Holocene and the last glacial period, while CaCO3 exists mainly in the glacial period ice. We also present size and spatial distributions of the micro-inclusions. These results suggest that water-soluble aerosols in the GRIP ice core are dependable proxies for past atmospheric conditions. Udgivelsesdato: December

We have proposed a method of deducing the chemical compounds found in deep polar ice cores by analyzing the balance between six major ions (Cl-, NO3 -, SO4 2-, Na+, Mg2+, and Ca2+). The method is demonstrated for the Holocene and last glacial maximum regions of the Dome Fuji and GRIP ice cores. The dominant compounds depend only on the ion balance and the sequence of chemical reactions. In priority order, the principle salts are calcium sulfate, other sulfates, nitrate, chloride, and carbonate. The chemical abundances deduced by this method agree well with the results of Raman spectroscopy on individual salt inclusions. The abundances in the ice cores are shown to reflect differences in climatic periods (the acidic environment of the Holocene versus the reductive environment of the last glacial maximum) and regional conditions (the marine environment of Antarctica versus the continental environment of Greenland). Udgivelsesdato: April 4