scholarly journals Northern Hemisphere atmospheric history of carbon monoxide since preindustrial times reconstructed from multiple Greenland ice cores

2021 ◽  
Author(s):  
Xavier Faïn ◽  
Rachael H. Rhodes ◽  
Place Philip ◽  
Vasilii V. Petrenko ◽  
Kévin Fourteau ◽  
...  

Abstract. Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. Obtaining a reliable record of atmospheric CO mixing ratios since pre-industrial times is necessary to evaluate climate-chemistry models in conditions different from today and to constrain past CO sources. We present high-resolution measurements of CO mixing ratios from ice cores drilled at five different sites on the Greenland ice sheet which experience a range of snow accumulation rates, mean surface temperatures, and different chemical compositions. An optical-feedback cavity-enhanced absorption spectrometer (OF-CEAS) was coupled to continuous melter systems and operated during four analytical campaigns conducted between 2013 and 2019. Overall, continuous flow analyses (CFA) of CO were carried out on over 700 m of ice. The CFA-based CO measurements exhibit excellent external precision (ranging 3.3-6.6 ppbv, 1sigma), and achieve consistently low blanks (ranging from 4.1+/-1.2 to 12.6+/-4.4 ppbv), enabling paleo-atmospheric interpretations. However the five CO records all exhibit variability too large and rapid to reflect past atmospheric mixing ratio changes. Complementary tests conducted on discrete ice samples demonstrate that these variations are not artifacts of the analytical method (i.e., production of CO from organics in the ice during melting), but very likely are related to in situ CO production within the ice before analysis. Evaluation of signal resolution and co-investigation of high-resolution records of CO and TOC show that past atmospheric CO variations can be extracted from the records’ baselines at four sites with accumulation rates higher than 20 cm water equivalent per year (weq yr-1). However, such baselines should be taken as upper bounds of past atmospheric CO burden. Baseline CO records from four sites are combined to produce a multisite average ice core reconstruction of past atmospheric CO for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE. From 1700 to 1875 CE, the record reveals stable or slightly increasing values in the 100-115 ppbv range. From 1875 to 1957 CE, the record indicates a monotonic increase from 114+/-4 ppbv to 147+/-6 ppbv. The ice-core multisite CO record exhibits an excellent overlap with the atmospheric CO record from Greenland firn air which spans the 1950-2010 time period. The combined ice-core and firn air CO history, spanning 1700-2010 CE provides useful constraints for future model studies of atmospheric changes since the preindustrial period.

2021 ◽  
Author(s):  
Xavier Faïn ◽  
Rachael Rhodes ◽  
Philip Place ◽  
Vasilii Petrenko ◽  
Kévin Fourteau ◽  
...  

<p>Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. Obtaining a reliable record of atmospheric CO mixing ratios since pre-industrial times is necessary to evaluate climate-chemistry models in conditions different from today. We present high-resolution measurements of CO mixing ratios from ice cores drilled at five different sites on the Greenland ice sheet which experience a range of snow accumulation rates, mean surface temperatures, and different chemical compositions. An optical-feedback cavity-enhanced absorption spectrometer (OF-CEAS) was coupled to continuous melter systems and operated during four analytical campaigns conducted between 2013 and 2019. The CFA-based CO measurements exhibit excellent external precision (ranging 3.3 - 6.6 ppbv, 1σ), and achieve consistently low blanks (ranging from 4.1±1.2 to 12.6±4.4 ppbv). Good accuracy and absolute calibration of CFA-based CO records enable paleo-atmospheric interpretations. The five CO records all exhibit variability in CO mixing ratios that is too large and rapid to reflect past atmospheric mixing ratio changes. Complementary tests conducted on discrete ice samples demonstrate that such patterns are not related to the analytical process (i.e., production of CO from organics in the ice during melting), but very likely are related to in situ CO production within the ice before analyses. Evaluation of signal resolution and co-investigation of high-resolution records of CO and TOC show that past atmospheric CO concentration can be extracted from the records’ baselines at four sites with accumulation rates higher than 20 cm water equivalent per year (weq yr<sup>-1</sup>). However, such baselines should be taken as upper bounds of past atmospheric CO burden. CO records from four sites are combined to produce a multisite average ice core reconstruction of past atmospheric CO for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE. From 1700 to 1875 CE, this record reveals stable or slightly increasing values remaining in the 100-115 ppbv range. From 1875 to 1957 CE, the record indicates a monotonic increase from 114±4 ppbv to 147±6 ppbv. The ice-core multisite CO record exhibits an excellent overlap with the atmospheric CO record from Greenland firn air which span the 1950-2010 time period. The combined ice-core and firn air CO history, spanning 1700-2010 CE, largely exhibits patterns that are consistent with the recent anthropogenic and biomass burning CO emission inventories. This brand new time series will be compared with the most recent results from Earth System Models involved in the CMIP6-AerChemMIP multi-model exercise.</p>


2021 ◽  
Author(s):  
Pete D. Akers ◽  
Joël Savarino ◽  
Nicolas Caillon ◽  
Mark Curran ◽  
Tas Van Ommen

<p>Precise Antarctic snow accumulation estimates are needed to understand past and future changes in global sea levels, but standard reconstructions using water isotopes suffer from competing isotopic effects external to accumulation. We present here an alternative accumulation proxy based on the post-depositional photolytic fractionation of nitrogen isotopes (d<sup>15</sup>N) in nitrate. On the high plateau of East Antarctica, sunlight penetrating the uppermost snow layers converts snow-borne nitrate into nitrogen oxide gas that can be lost to the atmosphere. This nitrate loss favors <sup>14</sup>NO<sub>3</sub><sup>-</sup> over <sup>15</sup>NO<sub>3</sub><sup>-</sup>, and thus the d<sup>15</sup>N of nitrate remaining in the snow will steadily increase until the nitrate is eventually buried beneath the reach of light. Because the duration of time until burial is dependent upon the rate of net snow accumulation, sites with lower accumulation rates have a longer burial wait and thus higher d<sup>15</sup>N values. A linear relationship (r<sup>2</sup> = 0.86) between d<sup>15</sup>N and net accumulation<sup>-1</sup> is calculated from over 120 samples representing 105 sites spanning East Antarctica. These sites largely encompass the full range of snow accumulation rates observed in East Antarctica, from 25 kg m-<sup>2</sup> yr<sup>-1</sup> at deep interior sites to >400 kg m-<sup>2</sup> yr<sup>-1</sup> at near coastal sites. We apply this relationship as a transfer function to an Aurora Basin ice core to produce a 700-year record of accumulation changes. Our nitrate-based estimate compares very well with a parallel reconstruction for Aurora Basin that uses volcanic horizons and ice-penetrating radar. Continued improvements to our database may enable precise independent estimates of millennial-scale accumulation changes using deep ice cores such as EPICA Dome C and Beyond EPICA-Oldest Ice.</p>


2020 ◽  
Vol 16 (2) ◽  
pp. 503-522
Author(s):  
Kévin Fourteau ◽  
Patricia Martinerie ◽  
Xavier Faïn ◽  
Alexey A. Ekaykin ◽  
Jérôme Chappellaz ◽  
...  

Abstract. We measured the methane mixing ratios of enclosed air in five ice core sections drilled on the East Antarctic Plateau. Our work aims to study two effects that alter the recorded gas concentrations in ice cores: layered gas trapping artifacts and firn smoothing. Layered gas trapping artifacts are due to the heterogeneous nature of polar firn, where some strata might close early and trap abnormally old gases that appear as spurious values during measurements. The smoothing is due to the combined effects of diffusive mixing in the firn and the progressive closure of bubbles at the bottom of the firn. Consequently, the gases trapped in a given ice layer span a distribution of ages. This means that the gas concentration in an ice layer is the average value over a certain period of time, which removes the fast variability from the record. Here, we focus on the study of East Antarctic Plateau ice cores, as these low-accumulation ice cores are particularly affected by both layering and smoothing. We use high-resolution methane data to test a simple trapping model reproducing the layered gas trapping artifacts for different accumulation conditions typical of the East Antarctic Plateau. We also use the high-resolution methane measurements to estimate the gas age distributions of the enclosed air in the five newly measured ice core sections. It appears that for accumulations below 2 cm ice equivalent yr−1 the gas records experience nearly the same degree of smoothing. We therefore propose to use a single gas age distribution to represent the firn smoothing observed in the glacial ice cores of the East Antarctic Plateau. Finally, we used the layered gas trapping model and the estimation of glacial firn smoothing to quantify their potential impacts on a hypothetical 1.5-million-year-old ice core from the East Antarctic Plateau. Our results indicate that layering artifacts are no longer individually resolved in the case of very thinned ice near the bedrock. They nonetheless contribute to slight biases of the measured signal (less than 10 ppbv and 0.5 ppmv in the case of methane using our currently established continuous CH4 analysis and carbon dioxide, respectively). However, these biases are small compared to the dampening experienced by the record due to firn smoothing.


2014 ◽  
Vol 10 (3) ◽  
pp. 987-1000 ◽  
Author(s):  
X. Faïn ◽  
J. Chappellaz ◽  
R. H. Rhodes ◽  
C. Stowasser ◽  
T. Blunier ◽  
...  

Abstract. We present high-resolution measurements of carbon monoxide (CO) concentrations from a shallow ice core of the North Greenland Eemian Ice Drilling project (NEEM-2011-S1). An optical-feedback cavity-enhanced absorption spectrometer (OF-CEAS) coupled to a continuous melter system performed continuous, online analysis during a four-week measurement campaign. This analytical setup generated stable measurements of CO concentrations with an external precision of 7.8 ppbv (1σ), based on repeated analyses of equivalent ice core sections. However, this first application of this measurement technique suffered from a poorly constrained procedural blank of 48 ± 25 ppbv and poor accuracy because an absolute calibration was not possible. The NEEM-2011-S1 CO record spans 1800 yr and the long-term trends within the most recent section of this record (i.e., post 1700 AD) resemble the existing discrete CO measurements from the Eurocore ice core. However, the CO concentration is highly variable (75–1327 ppbv range) throughout the ice core with high frequency (annual scale), high amplitude spikes characterizing the record. These CO signals are too abrupt and rapid to reflect atmospheric variability and their prevalence largely prevents interpretation of the record in terms of atmospheric CO variation. The abrupt CO spikes are likely the result of in situ production occurring within the ice itself, although the unlikely possibility of CO production driven by non-photolytic, fast kinetic processes within the continuous melter system cannot be excluded. We observe that 68% of the CO spikes are observed in ice layers enriched with pyrogenic aerosols. Such aerosols, originating from boreal biomass burning emissions, contain organic compounds, which may be oxidized or photodissociated to produce CO within the ice. However, the NEEM-2011-S1 record displays an increase of ~0.05 ppbv yr−1 in baseline CO level prior to 1700 AD (129 m depth) and the concentration remains elevated, even for ice layers depleted in dissolved organic carbon (DOC). Thus, the processes driving the likely in situ production of CO within the NEEM ice may involve multiple, complex chemical pathways not all related to past fire history and require further investigation.


2004 ◽  
Vol 39 ◽  
pp. 214-218 ◽  
Author(s):  
Gordon S. Hamilton

AbstractSnow-accumulation rates are known to be sensitive to local changes in ice-sheet surface slope because of the effect of katabatic winds. These topographic effects can be preserved in ice cores that are collected at non-ice-divide locations. The trajectory of an ice-core site at South Pole is reconstructed using measurements of ice-sheet motion to show that snow was probably deposited at places of different surface slope during the past 1000 years. Recent accumulation rates, derived from shallow firn cores, vary along this trajectory according to surface topography, so that on a relatively steep flank mean annual accumulation is ∼18% smaller than on a nearby topographic depression. These modern accumulation rates are used to reinterpret the cause of accumulation rate variability with time in the long ice-core record as an ice-dynamics effect and not a climate-change signal. The results highlight the importance of conducting ancillary ice-dynamics measurements as part of ice-coring programs so that topographic effects can be deconvolved from potential climate signals.


2020 ◽  
Author(s):  
Diana Vladimirova ◽  
Xavier Faïn ◽  
Patrick Ginot ◽  
Stanislav Kutuzov ◽  
Vladimir Mikhalenko

<p>Methane (CH<sub>4</sub>) is the third most powerful greenhouse gas. However, its warming potential is two orders of magnitude higher than of carbon dioxide and its residence time in the atmosphere is only 9.1 ± 0.9 years. It makes CH<sub>4</sub> a good indicator of rapid climate variations both under natural conditions and due to the anthropogenic influence.</p><p>The Elbrus ice core was drilled in 2009 on the Western Plato (43°20’53.9’’N, 42°25’36.0’’E) at elevation 5115 m a.s.l. It is 182 m long and is dated back to 280 ± 400 CE (Common Era). The CH<sub>4</sub> mixing ratios were analyzed using a continuous flow analysis (CFA) system paired with optical-feedback cavity-enhanced absorption spectroscopy. The measurements campaign was organized at Institut des Géosciences de l'Environnement (IGE), Grenoble, France. This is a first high-resolution mid-latitude CH<sub>4</sub> record. The record aims to better constrain the past evolution of mid-latitude methane sources.</p><p>Here we present preliminary results of the methane concentration measurements of the Elbrus ice core in high-resolution (CFA CH<sub>4</sub> record). We observe in situ production (max level 2900 ppb) and a baseline. We inspect a potential origin of the multiple spikes in the high-resolution record. Supposedly, either an in-situ production in the dust-rich layers occurred or a gas dissolution in the melt layers took place. However, the possibility of in-situ production during continuous gas extraction has to be further studied. The identified melt layers can serve as an indicator of interrupted stable water isotopic signal and may be supportive in the regional temperature reconstructions based on the Elbrus ice core record. A cleaned off the spikes record is inspected for the natural variability of the CH<sub>4</sub> baseline concentration related to the short-term climate and methane emissions variability.</p>


2013 ◽  
Vol 9 (3) ◽  
pp. 2817-2857 ◽  
Author(s):  
X. Faïn ◽  
J. Chappellaz ◽  
R. H. Rhodes ◽  
C. Stowasser ◽  
T. Blunier ◽  
...  

Abstract. We present high-resolution measurements of carbon monoxide (CO) concentrations from continuous analysis of a shallow ice core from the North Greenland Eemian Ice Drilling project (NEEM-2011-S1). An Optical Feedback – Cavity Enhanced Absorption Spectrometer (OF-CEAS) was coupled to a continuous melter system during a 4-week laboratory-based measurement campaign. This analytical setup generates highly stable measurements of CO concentrations with an external precision of 7.8 ppbv (1 sigma) based on a comparison of replicate cores. The NEEM-2011-S1 CO record spans 1800 yr and exhibits highly variable concentrations at the scale of annual layers, ranging from 75 to 1327 ppbv. The most recent section of this record (i.e. since 1700 AD) agrees with existing discrete CO measurements from the Eurocore ice core and the deep NEEM firn. However, it is difficult to interpret in terms of atmospheric CO variation due to high frequency, high amplitude spikes in the data. 68% of the elevated CO spikes are observed in ice layers enriched with pyrogenic aerosols. Such aerosols, originating from boreal biomass burning emissions, contain organic compounds, which can be oxidized or photodissociated to produce CO in-situ. We suggest that elevated CO concentration features could present a new integrative proxy for past biomass burning history. Furthermore, the NEEM-2011-S1 record reveals an increase in baseline CO level prior to 1700 AD (129 m depth), with the concentration remaining high even for ice layers depleted in dissolved organic carbon (DOC). Overall, the processes driving in-situ production of CO within the NEEM ice are complex and may involve multiple chemical pathways.


2021 ◽  
Vol 15 (7) ◽  
pp. 3181-3205
Author(s):  
Enrico Mattea ◽  
Horst Machguth ◽  
Marlene Kronenberg ◽  
Ward van Pelt ◽  
Manuela Bassi ◽  
...  

Abstract. Our changing climate is expected to affect ice core records as cold firn progressively transitions to a temperate state. Thus, there is a need to improve our understanding and to further develop quantitative process modeling, to better predict cold firn evolution under a range of climate scenarios. Here we present the application of a distributed, fully coupled energy balance model, to simulate cold firn at the high-alpine glaciated saddle of Colle Gnifetti (Swiss–Italian Alps) over the period 2003–2018. We force the model with high-resolution, long-term, and extensively quality-checked meteorological data measured in the closest vicinity of the firn site, at the highest automatic weather station in Europe (Capanna Margherita, 4560 m a.s.l.). The model incorporates the spatial variability of snow accumulation rates and is calibrated using several partly unpublished high-altitude measurements from the Monte Rosa area. The simulation reveals a very good overall agreement in the comparison with a large archive of firn temperature profiles. Our results show that surface melt over the glaciated saddle is increasing by 3–4 mm w.e. yr−2 depending on the location (29 %–36 % in 16 years), although with large inter-annual variability. Analysis of modeled melt indicates the frequent occurrence of small melt events (<4 mm w.e.), which collectively represent a significant fraction of the melt totals. Modeled firn warming rates at 20 m depth are relatively uniform above 4450 m a.s.l. (0.4–0.5 ∘C per decade). They become highly variable at lower elevations, with a marked dependence on surface aspect and absolute values up to 2.5 times the local rate of atmospheric warming. Our distributed simulation contributes to the understanding of the thermal regime and evolution of a prominent site for alpine ice cores and may support the planning of future core drilling efforts. Moreover, thanks to an extensive archive of measurements available for comparison, we also highlight the possibilities of model improvement most relevant to the investigation of future scenarios, such as the fixed-depth parametrized routine of deep preferential percolation.


2016 ◽  
Vol 16 (5) ◽  
pp. 2819-2842 ◽  
Author(s):  
Maria Zatko ◽  
Lei Geng ◽  
Becky Alexander ◽  
Eric Sofen ◽  
Katarina Klein

Abstract. The formation and recycling of reactive nitrogen (NO, NO2, HONO) at the air–snow interface has implications for air quality and the oxidation capacity of the atmosphere in snow-covered regions. Nitrate (NO3−) photolysis in snow provides a source of oxidants (e.g., hydroxyl radical) and oxidant precursors (e.g., nitrogen oxides) to the overlying boundary layer, and alters the concentration and isotopic (e.g., δ15N) signature of NO3− preserved in ice cores. We have incorporated an idealized snowpack with a NO3− photolysis parameterization into a global chemical transport model (Goddard Earth Observing System (GEOS) Chemistry model, GEOS-Chem) to examine the implications of snow NO3− photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core NO3− in ice cores across Antarctica and Greenland, where observations of these parameters over large spatial scales are difficult to obtain. A major goal of this study is to examine the influence of meteorological parameters and chemical, optical, and physical snow properties on the magnitudes and spatial patterns of snow-sourced NOx fluxes and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland. Snow-sourced NOx fluxes are most influenced by temperature-dependent quantum yields of NO3− photolysis, photolabile NO3− concentrations in snow, and concentrations of light-absorbing impurities (LAIs) in snow. Despite very different assumptions about snowpack properties, the range of model-calculated snow-sourced NOx fluxes are similar in Greenland (0.5–11 × 108 molec cm−2 s−1) and Antarctica (0.01–6.4 × 108 molec cm−2 s−1) due to the opposing effects of higher concentrations of both photolabile NO3− and LAIs in Greenland compared to Antarctica. Despite the similarity in snow-sourced NOx fluxes, these fluxes lead to smaller factor increases in mean austral summer boundary layer mixing ratios of total nitrate (HNO3+ NO3−), NOx, OH, and O3 in Greenland compared to Antarctica because of Greenland's proximity to pollution sources. The degree of nitrogen recycling in the snow is dependent on the relative magnitudes of snow-sourced NOx fluxes versus primary NO3− deposition. Recycling of snow NO3− in Greenland is much less than in Antarctica Photolysis-driven loss of snow NO3− is largely dependent on the time that NO3− remains in the snow photic zone (up to 6.5 years in Antarctica and 7 months in Greenland), and wind patterns that redistribute snow-sourced reactive nitrogen across Antarctica and Greenland. The loss of snow NO3− is higher in Antarctica (up to 99 %) than in Greenland (up to 83 %) due to deeper snow photic zones and lower snow accumulation rates in Antarctica. Modeled enrichments in ice-core δ15N(NO3−) due to photolysis-driven loss of snow NO3− ranges from 0 to 363 ‰ in Antarctica and 0 to 90 ‰ in Greenland, with the highest fraction of NO3− loss and largest enrichments in ice-core δ15N(NO3−) at high elevations where snow accumulation rates are lowest. There is a strong relationship between the degree of photolysis-driven loss of snow NO3− and the degree of nitrogen recycling between the air and snow throughout all of Greenland and in Antarctica where snow accumulation rates are greater than 130 kg m−2 a−1 in the present day.


2002 ◽  
Vol 48 (162) ◽  
pp. 417-424 ◽  
Author(s):  
Anja Pälli ◽  
Jack C. Kohler ◽  
Elisabeth Isaksson ◽  
John C. Moore ◽  
Jean Francis Pinglot ◽  
...  

AbstractA 50 MHz ground-penetrating radar was used to detect horizontal layers in the snowpack along a longitudinal profile on Nordenskjöldbreen, a Svalbard glacier. The profile passed two shallow and one deep ice-core sites. Two internal radar reflection layers were dated using parameters measured in the deep core. Radar travel times were converted to water equivalent, yielding snow-accumulation rates along the profile for three time periods: 1986–99, 1963–99 and 1963–86. The results show 40–60% spatial variability in snow accumulation over short distances along the profile. The average annual accumulation rate for 1986–99 was found to be about 12% higher than for the period 1963–86, which indicates increased accumulation in the late 1980s and 1990s.


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