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Here we use high-precision carbon isotope data (δ13C-CO2) to show atmospheric CO2 during Marine Isotope Stage 4 (MIS 4, ~70.5-59 ka) was controlled by a succession of millennial-scale processes. Enriched δ13C-CO2 during peak glaciation suggests increased ocean carbon storage. Variations in δ13C-CO2 in early MIS 4 suggest multiple processes were active during CO2 drawdown, potentially including decreased land carbon and decreased Southern Ocean air-sea gas exchange superposed on increased ocean carbon storage. CO2 remained low during MIS 4 while δ13C-CO2 fluctuations suggest changes in Southern Ocean and North Atlantic air-sea gas exchange. A 7 ppm increase in CO2 at the onset of Dansgaard-Oeschger event 19 (72.1 ka) and 27 ppm increase in CO2 during late MIS 4 (Heinrich Stadial 6, ~63.5-60 ka) involved additions of isotopically light carbon to the atmosphere. The terrestrial biosphere and Southern Ocean air-sea gas exchange are possible sources, with the latter event also involving decreased ocean carbon storage.

Abstract. Deglaciations are characterized by relatively fast and near-synchronous changes in ice sheet volume, ocean temperature, and atmospheric greenhouse gas concentrations, but glacial inceptions occur more gradually. Understanding the evolution of ice sheet, ocean, and atmospheric conditions from interglacial to glacial maximum provides important insight into the interplay of these components of our climate system. Using noble gas measurements in ancient ice samples, we reconstruct mean ocean temperature (MOT) from 74 to 59.5 ka BP, covering the Marine Isotope Stage (MIS) 5-4 boundary, MIS 4, and part of the MIS 4-3 transition. Comparing this MOT reconstruction to previously published MOT reconstructions from the last glacial cycle, we find that the majority of interglacial-glacial ocean cooling occurred across MIS 5, and MOT reached full glacial levels by MIS 4 (−2.7 ± 0.3 °C relative to the Holocene). Comparing MOT to contemporaneous records of CO2 and benthic ?18O, we find that ocean cooling and the solubility pump can explain most of the CO2 drawdown and increase in ?18O across MIS 5. The timing of ocean warming and cooling in our record indicates that millennial scale climate variability plays a crucial role in setting mean ocean temperature during this interval, as seen during other periods, such as the last deglaciation.

Abstract. Deglaciations are characterized by relatively fast andnear-synchronous changes in ice sheet volume, ocean temperature, andatmospheric greenhouse gas concentrations, but glacial inception occurs moregradually. Understanding the evolution of ice sheet, ocean, and atmosphereconditions from interglacial to glacial maximum provides insight into theinterplay of these components of the climate system. Using noble gasmeasurements in ancient ice samples, we reconstruct mean ocean temperature(MOT) from 74 to 59.7 ka, covering the Marine Isotope Stage (MIS) 5a–4boundary, MIS 4, and part of the MIS 4–3 transition. Comparing this MOTreconstruction to previously published MOT reconstructions from the last andpenultimate deglaciation, we find that the majority of the lastinterglacial–glacial ocean cooling must have occurred within MIS 5. MOTreached equally cold conditions in MIS 4 as in MIS 2 (−2.7 ± 0.3 ∘C relative to the Holocene, −0.1 ± 0.3 ∘Crelative to MIS 2). Using a carbon cycle model to quantify the CO2 solubility pump, we show that ocean cooling can explain most of theCO2 drawdown (32 ± 4 of 40 ppm) across MIS 5. Comparing MOT tocontemporaneous records of benthic δ18O, we find that ocean coolingcan also explain the majority of the δ18O increase across MIS 5 (0.7 ‰of 1.3 ‰). The timing of ocean warming and cooling inthe record and the comparison to coeval Antarctic isotope data suggest anintimate link between ocean heat content, Southern Hemisphere high-latitude climate,and ocean circulation on orbital and millennial timescales.

Abstract. We reconstruct atmospheric abundances of the potentgreenhouse gas c-C4F8 (perfluorocyclobutane, perfluorocarbonPFC-318) from measurements of in situ, archived, firn, and aircraft airsamples with precisions of ∼1 %–2 % reported on the SIO-14gravimetric calibration scale. Combined with inverse methods, we found near-zero atmospheric abundances from the early 1900s to the early 1960s, afterwhich they rose sharply, reaching 1.66 ppt (parts per trillion dry-air molefraction) in 2017. Global c-C4F8 emissions rose from near zero inthe 1960s to 1.2±0.1 (1σ) Gg yr−1 in the late 1970s tolate 1980s, then declined to 0.77±0.03 Gg yr−1 in the mid-1990sto early 2000s, followed by a rise since the early 2000s to 2.20±0.05 Gg yr−1 in 2017. These emissions are significantly larger thaninventory-based emission estimates. Estimated emissions from eastern Asiarose from 0.36 Gg yr−1 in 2010 to 0.73 Gg yr−1 in 2016 and 2017,31 % of global emissions, mostly from eastern China. We estimateemissions of 0.14 Gg yr−1 from northern and central India in 2016 andfind evidence for significant emissions from Russia. In contrast, recentemissions from northwestern Europe and Australia are estimated to be small(≤1 % each). We suggest that emissions from China, India, and Russiaare likely related to production of polytetrafluoroethylene (PTFE,“Teflon”) and other fluoropolymers and fluorochemicals that are based onthe pyrolysis of hydrochlorofluorocarbon HCFC-22 (CHClF2) in whichc-C4F8 is a known by-product. The semiconductor sector, wherec-C4F8 is used, is estimated to be a small source, at least inSouth Korea, Japan, Taiwan, and Europe. Without an obvious correlation withpopulation density, incineration of waste-containing fluoropolymers isprobably a minor source, and we find no evidence of emissions fromelectrolytic production of aluminum in Australia. While many possibleemissive uses of c-C4F8 are known and though we cannotcategorically exclude unknown sources, the start of significant emissionsmay well be related to the advent of commercial PTFE production in 1947.Process controls or abatement to reduce the c-C4F8 by-product wereprobably not in place in the early decades, explaining the increase inemissions in the 1960s and 1970s. With the advent of by-product reportingrequirements to the United Nations Framework Convention on Climate Change(UNFCCC) in the 1990s, concern about climate change and product stewardship,abatement, and perhaps the collection of c-C4F8 by-product for usein the semiconductor industry where it can be easily abated, it isconceivable that emissions in developed countries were stabilized and thenreduced, explaining the observed emission reduction in the 1980s and 1990s.Concurrently, production of PTFE in China began to increase rapidly. Withoutemission reduction requirements, it is plausible that global emissions todayare dominated by China and other developing countries. We predict thatc-C4F8 emissions will continue to rise and that c-C4F8will become the second most important emitted PFC in terms ofCO2-equivalent emissions within a year or two. The 2017 radiativeforcing of c-C4F8 (0.52 mW m−2) is small but emissions ofc-C4F8 and other PFCs, due to their very long atmosphericlifetimes, essentially permanently alter Earth's radiative budget and shouldbe reduced. Significant emissions inferred outside of the investigatedregions clearly show that observational capabilities and reportingrequirements need to be improved to understand global and country-scaleemissions of PFCs and other synthetic greenhouse gases and ozone-depletingsubstances.

New ice cores retrieved from the Taylor Glacier (Antarctica) blue ice area contain ice and air spanning the Marine Isotope Stage (MIS) 5-4 transition, a period of global cooling and ice sheet expansion. We determine chronologies for the ice and air bubbles in the new ice cores by visually matching variations in gas- and ice-phase tracers to preexisting ice core records. The chronologies reveal an ice age-gas age difference (Δage) approaching 10 ka during MIS 4, implying very low snow accumulation in the Taylor Glacier accumulation zone. A revised chronology for the analogous section of the Taylor Dome ice core (84 to 55 ka), located to the south of the Taylor Glacier accumulation zone, shows that Δage did not exceed 3 ka. The difference in Δage between the two records during MIS 4 is similar in magnitude but opposite in direction to what is observed at the Last Glacial Maximum. This relationship implies that a spatial gradient in snow accumulation existed across the Taylor Dome region during MIS 4 that was oriented in the opposite direction of the accumulation gradient during the Last Glacial Maximum.

Abstract. A new ice core retrieved from the Taylor Glacier blue ice area contains ice and air spanning the Marine Isotope Stage (MIS) 5/4 transition (74 to 65 ka), a period of global cooling and glacial inception. Dating the ice and air bubbles in the new ice core reveals an ice age-gas age difference (Δage) approaching 10 ka during MIS 4, implying very low accumulation at the Taylor Glacier accumulation zone on the northern flank of Taylor Dome. A revised chronology for the Taylor Dome ice core (80 to 55 ka), situated to the south of the Taylor Glacier accumulation zone, shows that Δage did not exceed 2.5 ka at that location. The difference in Δage between the new Taylor Glacier ice core and the Taylor Dome ice core implies a spatial gradient in snow accumulation across Taylor Dome that intensified during the last glacial inception and through MIS 4.

Methane (CH4) is a powerful greenhouse gas and plays a key part in global atmospheric chemistry. Natural geological emissions (fossil methane vented naturally from marine and terrestrial seeps and mud volcanoes) are thought to contribute around 52 teragrams of methane per year to the global methane source, about 10 per cent of the total, but both bottom-up methods (measuring emissions) and top-down approaches (measuring atmospheric mole fractions and isotopes) for constraining these geological emissions have been associated with large uncertainties. Here we use ice core measurements to quantify the absolute amount of radiocarbon-containing methane (14CH4) in the past atmosphere and show that geological methane emissions were no higher than 15.4 teragrams per year (95 per cent confidence), averaged over the abrupt warming event that occurred between the Younger Dryas and Preboreal intervals, approximately 11,600 years ago. Assuming that past geological methane emissions were no lower than today, our results indicate that current estimates of today's natural geological methane emissions (about 52 teragrams per year) are too high and, by extension, that current estimates of anthropogenic fossil methane emissions are too low. Our results also improve on and confirm earlier findings that the rapid increase of about 50 per cent in mole fraction of atmospheric methane at the Younger Dryas-Preboreal event was driven by contemporaneous methane from sources such as wetlands; our findings constrain the contribution from old carbon reservoirs (marine methane hydrates, permafrost and methane trapped under ice) to 19 per cent or less (95 per cent confidence). To the extent that the characteristics of the most recent deglaciation and the Younger Dryas-Preboreal warming are comparable to those of the current anthropogenic warming, our measurements suggest that large future atmospheric releases of methane from old carbon sources are unlikely to occur.

Abstract. Old ice for paleo-environmental studies, traditionally accessed through deep core drilling on domes and ridges on the large ice sheets, can also be retrieved at the surface from ice sheet margins and blue ice areas. The practically unlimited amount of ice available at these sites satisfies a need in the community for studies of trace components requiring large sample volumes. For margin sites to be useful as ancient ice archives, the ice stratigraphy needs to be understood and age models need to be established. We present measurements of trapped gases in ice from Taylor Glacier, Antarctica, to date the ice and assess the completeness of the stratigraphic section. Using δ18O of O2 and methane concentrations, we unambiguously identify ice from the last glacial cycle, covering every climate interval from the early Holocene to the penultimate interglacial. A high-resolution transect reveals the last deglaciation and the Last Glacial Maximum (LGM) in detail. We observe large-scale deformation in the form of folding, but individual stratigraphic layers do not appear to have undergone irregular thinning. Rather, it appears that the entire LGM-deglaciation sequence has been transported from the interior of the ice sheet to the surface of Taylor Glacier relatively undisturbed. We present an age model that builds the foundation for gas studies on Taylor Glacier. A comparison with the Taylor Dome ice core confirms that the section we studied on Taylor Glacier is better suited for paleo-climate reconstructions of the LGM due to higher accumulation rates.

Galactic cosmic rays (GCRs) interact with matter in the atmosphere and at the surface of the Earth to produce a range of cosmogenic nuclides. Measurements of cosmogenic nuclides produced in surface rocks have been used to study past land ice extent as well as to estimate erosion rates. Because the GCR flux reaching the Earth is modulated by magnetic fields (solar and Earth's), records of cosmogenic nuclides produced in the atmosphere have also been used for studies of past solar activity. Studies utilizing cosmogenic nuclides assume that the GCR flux is constant in time, but this assumption may be uncertain by 30 % or more. Here we propose that measurements of 14 C of carbon monoxide (14 CO) in ice cores at low-accumulation sites can be used as a proxy for variations in GCR flux on timescales of several thousand years. At low-accumulation ice core sites, 14 CO in ice below the firn zone originates almost entirely from in situ cosmogenic production by deep-penetrating secondary cosmic ray muons. The flux of such muons is almost insensitive to solar and geomagnetic variations and depends only on the primary GCR flux intensity. We use an empirically constrained model of in situ cosmogenic 14 CO production in ice in combination with a statistical analysis to explore the sensitivity of ice core 14 CO measurements at Dome C, Antarctica, to variations in the GCR flux over the past ≈ 7000 years. We find that Dome C 14 CO measurements would be able to detect a linear change of 6 % over 7 ka, a step increase of 6 % at 3.5 ka or a transient 100-year spike of 190 % at 3.5 ka at the 3 σ significance level. The ice core 14 CO proxy therefore appears promising for the purpose of providing a high-precision test of the assumption of GCR flux constancy over the Holocene. [ABSTRACT FROM AUTHOR]

An understanding of the mechanisms that control CO2 change during glacial-interglacial cycles remains elusive. Here we help to constrain changing sources with a high-precision, high-resolution deglacial record of the stable isotopic composition of carbon in CO2(δ(13)C-CO2) in air extracted from ice samples from Taylor Glacier, Antarctica. During the initial rise in atmospheric CO2 from 17.6 to 15.5 ka, these data demarcate a decrease in δ(13)C-CO2, likely due to a weakened oceanic biological pump. From 15.5 to 11.5 ka, the continued atmospheric CO2 rise of 40 ppm is associated with small changes in δ(13)C-CO2, consistent with a nearly equal contribution from a further weakening of the biological pump and rising ocean temperature. These two trends, related to marine sources, are punctuated at 16.3 and 12.9 ka with abrupt, century-scale perturbations in δ(13)C-CO2 that suggest rapid oxidation of organic land carbon or enhanced air-sea gas exchange in the Southern Ocean. Additional century-scale increases in atmospheric CO2 coincident with increases in atmospheric CH4 and Northern Hemisphere temperature at the onset of the Bølling (14.6-14.3 ka) and Holocene (11.6-11.4 ka) intervals are associated with small changes in δ(13)C-CO2, suggesting a combination of sources that included rising surface ocean temperature.

Nitrous oxide (N2O) is an important greenhouse gas and ozone-depleting substance that has anthropogenic as well as natural marine and terrestrial sources. The tropospheric N2O concentrations have varied substantially in the past in concert with changing climate on glacial-interglacial and millennial timescales. It is not well understood, however, how N2O emissions from marine and terrestrial sources change in response to varying environmental conditions. The distinct isotopic compositions of marine and terrestrial N2O sources can help disentangle the relative changes in marine and terrestrial N2O emissions during past climate variations. Here we present N2O concentration and isotopic data for the last deglaciation, from 16,000 to 10,000 years before present, retrieved from air bubbles trapped in polar ice at Taylor Glacier, Antarctica. With the help of our data and a box model of the N2O cycle, we find a 30 per cent increase in total N2O emissions from the late glacial to the interglacial, with terrestrial and marine emissions contributing equally to the overall increase and generally evolving in parallel over the last deglaciation, even though there is no a priori connection between the drivers of the two sources. However, we find that terrestrial emissions dominated on centennial timescales, consistent with a state-of-the-art dynamic global vegetation and land surface process model that suggests that during the last deglaciation emission changes were strongly influenced by temperature and precipitation patterns over land surfaces. The results improve our understanding of the drivers of natural N2O emissions and are consistent with the idea that natural N2O emissions will probably increase in response to anthropogenic warming.

Measurements of carbon-14-containing carbon monoxide (14 CO) in glacial ice are useful for studies of the past oxidative capacity of the atmosphere as well as for reconstructing the past cosmic ray flux. The 14 CO abundance in glacial ice represents the combination of trapped atmospheric 14 CO and in situ cosmogenic 14 CO. The systematics of in situ cosmogenic 14 CO production and retention in ice are not fully quantified, posing an obstacle to interpretation of ice core 14 CO measurements. Here we provide the first comprehensive characterization of 14 CO at an ice accumulation site (Summit, Greenland), including measurements in the ice grains of the firn matrix, firn air and bubbly ice below the firn zone. The results are interpreted with the aid of a firn gas transport model into which we implemented in situ cosmogenic 14 C. We find that almost all (≈ 99.5 %) of in situ 14 CO that is produced in the ice grains in firn is very rapidly (in <1 year) lost to the open porosity and from there mostly vented to the atmosphere. The timescale of this rapid loss is consistent with what is expected from gas diffusion through ice. The small fraction of in situ 14 CO that initially stays in the ice grains continues to slowly leak out to the open porosity at a rate of ≈ 0.6 % yr -1. Below the firn zone we observe an increase in 14 CO content with depth that is due to in situ 14 CO production by deep-penetrating muons, confirming recent estimates of 14 CO production rates in ice via the muon mechanisms and allowing for narrowing constraints on these production rates. [ABSTRACT FROM AUTHOR]

Global chemistry-climate models (CCMs) play an important role in assessing the climate and air pollution implications of aerosols and chemically reactive gases. Evaluating these models under past conditions and constraining historical sources and sinks necessitates reliable records of atmospheric mixing ratios spanning preindustrial times. Such precious records were recently obtained for carbon monoxide (CO) documenting for the first time the evolution of this reactive compound over the industrial era. In this study, we compare the simulated atmospheric surface CO mixing ratios ([CO]) from two different sets of CCMs and emissions in the frame of CMIP5 and of CMIP6 (Coupled Model Intercomparison Project Phases 5 and 6) with recent bipolar ice archive reconstructions for the period spanning 1850 to present. We analyze how historical (1850-2014) [CO] outputs from 16 (Atmospheric Chemistry and Climate Model Intercomparison Project) models and 6 AerChemMIP (Aerosol Chemistry Model Intercomparison Project) models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. While most models underestimate [CO] at high northern latitudes, a reduction in this bias is observed from ACCMIP to AerChemMIP exercises. Over the 1980-2010 CE period, trends in ice archive and firn air observations and AerChemMIP outputs align remarkably well at high northern and southern latitudes, indicating improved quantification of CO anthropogenic emissions and the main CO sink (OH oxidation) compared to ACCMIP. From 1850 to 1980 CE, AerChemMIP models and observations consistently show increasing [CO] in both the Northern Hemisphere (NH) and Southern Hemisphere (SH), suggesting a robust understanding of the CO budget evolution. However, a divergence in the [CO] growth rate emerges in NH between models and observations over the 1920-1975 CE period, attributed to uncertainties in CO emission factors (EF), particularly EF for RCO (Residential, Commercial and Others) and transportation sectors, although we cannot totally rule out that the CO record based on Greenland ice archives may be biased high by CO chemical production processes occurring in the ice prior the measurements (i.e., in situ CO production). In the Southern Hemisphere, AerChemMIP models simulate an increase in atmospheric [CO] from 1850 to 1980 CE closely reproducing the observations (22±10 ppb and 13±7 ppb, respectively). Such agreement supports CMIP6 biomass burning CO emission inventories which do not reveal a peak in CO emissions in the late 19th century. Furthermore, both SH models and observations reveal an accelerated growth rate in [CO] during 1945-1980 CE relative to 1980-1945 CE, likely linked to increased anthropogenic transportation emissions. [ABSTRACT FROM AUTHOR]

Galactic cosmic rays (GCRs) interact with matter in the atmosphere and at the surface of the Earth to produce a range of cosmogenic nuclides. Measurements of cosmogenic nuclides produced in surface rocks have been used to study past land ice extent as well as to estimate erosion rates. Because the GCR flux reaching the Earth is modulated by magnetic fields (solar and Earth's), records of cosmogenic nuclides produced in the atmosphere have also been used for studies of past solar activity. Studies utilizing cosmogenic nuclides assume that the GCR flux is constant in time, but this assumption may be uncertain by 30% or more. Here we propose that measurements of 14C of carbon monoxide (14CO) in ice cores at low-accumulation sites can be used as a proxy for variations in GCR flux on timescales of several thousand years. At low-accumulation ice core sites, 14CO in ice below the firn zone originates almost entirely from in situ cosmogenic production by deep-penetrating secondary cosmic ray muons. The flux of such muons is insensitive to solar and geomagnetic variations, and depends only on the primary GCR flux intensity. We use an empirically-constrained model of in situ cosmogenic 14CO production in ice in combination with a statistical analysis to explore the sensitivity of ice core 14CO measurements at Dome C, Antarctica to variations in the GCR flux over the past ≈7000 years. We find that Dome C 14CO measurements would be able to detect a linear change of 4%, a step increase of 4% or a transient 100-year spike of 250% at the 3 σ significance level. The ice core 14CO proxy therefore appears promising for the purpose of providing a high-precision test of the assumption of GCR flux constancy over the Holocene. [ABSTRACT FROM AUTHOR]

Historical atmospheric H 2 levels were reconstructed using firn air measurements from two sites in Greenland (NEEM and Summit) and two sites in Antarctica (South Pole and Megadunes). A joint reconstruction based on the two Antarctic sites yields H 2 levels monotonically increasing from about 330 ppb in 1900 to 550 ppb in the late 1990s, leveling off thereafter. These results are similar to individual reconstructions published previously (Patterson et al., 2020, 2021). Interpretation of the Greenland firn air measurements is complicated by challenges in modeling enrichment induced by pore close-off at these sites. We used observations of neon enrichment at NEEM and Summit to tune the parameterization of enrichment induced by pore close-off in our firn air model. The joint reconstruction from the Greenland data shows H 2 levels rising 30 % between 1950 and the late 1980s, reaching a maximum of 530 ppb. After 1990, reconstructed atmospheric H 2 levels over Greenland are roughly constant, with a small decline of 3 % over the next 25 years. The reconstruction shows good agreement with the available flask measurements of H 2 at high northern latitudes. [ABSTRACT FROM AUTHOR]

Author(s): Vasilii V. Petrenko (corresponding author) [1]; Andrew M. Smith [2]; Hinrich Schaefer [3]; Katja Riedel [3]; Edward Brook [4]; Daniel Baggenstos [5, 6]; Christina Harth [5]; Quan Hua [2]; [...]

Measurements of carbon-14-containing carbon monoxide (14CO) in glacial ice are useful for studies of the past oxidative capacity of the atmosphere as well as for reconstructing the past cosmic ray flux. 14CO abundance in glacial ice represents the combination of trapped atmospheric 14CO and in situ cosmogenic 14CO. The systematics of in situ cosmogenic 14CO production and retention in ice are not fully quantified, posing an obstacle to interpretation of ice core 14CO measurements. Here we provide the first comprehensive characterization of 14CO at an ice accumulation site (Summit, Greenland), including measurements in the ice grains of the firn matrix, firn air and bubbly ice below the firn zone. The results are interpreted with the aid of a firn gas transport model into which we implemented in situ cosmogenic 14C. We find that almost all (≈99.5%) of in situ 14CO that is produced in the ice grains in firn is very rapidly (in <1 year) lost to the open porosity and from there mostly vented to the atmosphere. The time scale of this rapid loss is consistent with what is expected from gas diffusion through ice. The small fraction of in situ 14CO that initially stays in the ice grains continues to slowly leak out to the open porosity at a rate of ≈0.6% per year. Below the firn zone we observe an increase in 14CO content with depth that is due to in situ 14CO production by deep-penetrating muons, confirming recent estimates of production rates in ice via the muon mechanisms and allowing for narrowing constraints on these production rates. [ABSTRACT FROM AUTHOR]

Historical hemispheric atmospheric H2 levels since 1930 were reconstructed using the UCI_2 firn air model and firn air measurements from three sites in Greenland: (NEEM, Summit, and Tunu) and two sites in Antarctica (South Pole and Megadunes). A joint reconstruction based on the two Antarctic sites yields H2 levels monotonically increasing from about 350 ppb in 1900 to 550 ppb in the late 1990's, levelling off thereafter. These results are similar to individual reconstructions published previously (Patterson et al., 2020; 2021). Reconstruction of the Greenland data is complicated by a systematic bias between Tunu and the other sites. The Tunu reconstruction shows substantially lower historical H2 levels than the other two sites, a difference we attribute to possible bias in the calibration of the Tunu measurements. All three reconstructions show a late 20th century maximum in H2 levels over Greenland. A joint reconstruction of the Greenland data shows H2 levels rising 40% from 1930-1990, reaching a maximum of 550 ppb. After 1990, reconstructed atmospheric H2 decrease by 6% over the next 20 years. The reconstruction deviates by at most 4% from the few available surface air measurements of atmospheric H2 levels over Greenland from 1998-2004. However, the longer instrumental records from sampling sites outside of Greenland show a more rapid decrease and stabilization after 1990 compared to the reconstruction. We explore the possibility that this difference is an artefact caused by the firn air model underestimating pore close-off induced enrichment, evidenced by a mismatch between measured and modelled Ne in firn air. We developed new parameterizations which more accurately capture pore close-off induced enrichment at the Greenland sites. Incorporating those 30 parameterizations into the UCI_2 model yields reconstructions with lower H2 levels throughout the mid-late 20th century and more stable H2 levels during the 1990's, in better agreement with the flask measurements. [ABSTRACT FROM AUTHOR]