Firn Research Articles

Emissions halted of the potent greenhouse gas SF<sub>5</sub>CF<sub>3</sub>

Abstract. Long term measurements in background air (Cape Grim, Tasmania) and firn air (NEEM, Greenland) of the potent long-lived greenhouse gas SF5CF3 show that emissions declined after the late 1990s, having grown since the 1950s, and became indistinguishable from zero after 2003. The timing of this decline suggests that emissions of this gas may have been related to the production of certain fluorochemicals; production of which have been recently phased out. An earlier observation of closely correlated atmospheric abundances of SF5CF3 and SF6 are shown here to have likely been purely coincidental, as their respective trends diverged after 2002. Due to its long lifetime (ca. 900 yr), atmospheric concentrations of SF5CF3 have not declined, and it is now well mixed between hemispheres, as is also shown here from interhemispheric aircraft measurements. Total cumulative emissions of SF5CF3 amount to around 5 kT.

Evidence from firn air for recent decreases in non-methane hydrocarbons and a 20th century increase in nitrogen oxides in the northern hemisphere

The atmospheric evolution of eight non-methane hydrocarbons (ethane, acetylene, propane, n-butane, isobutane, n-pentane, isopentane and benzene) and five alkyl nitrates (2-propyl, 2-butyl, 3-methyl-2-butyl and the sum of 2+3-pentyl nitrates) are reconstructed for the latter half of the 20th century based on Arctic firn air measurements. The reconstructed trends of the non-methane hydrocarbons (NMHCs) show increasing concentrations from 1950 to a maximum in 1980 before declining towards the end of last century. These observations provide direct evidence that NMHCs in the northern hemisphere have declined substantially during the period 1980–2001. Benzene concentrations show a smaller increase between 1950 and 1980 than the other NMHCs indicating that additional sources of benzene, other than fossil fuel combustion, were likely important contributors to the benzene budget prior to and during this period. The declining benzene concentrations from 1980 to 2001 would suggest that biomass burning is unlikely to be important in the benzene budget as biomass burning emissions were reportedly increasing over the same period. Methyl and ethyl nitrate show growth patterns in the firn that suggested perturbation by in-situ production from an unidentified mechanism. However, the higher alkyl nitrates show evidence for increasing concentrations from 1950 to maxima in the mid 1990s before decreasing slightly toward the end of the last century. The differing atmospheric evolution of the alkyl nitrates relative to their parent hydrocarbons indicate an increase in their production efficiency per hydrocarbon molecule. Using a steady state analysis of hydrocarbon oxidation and alkyl nitrate production and loss we show that reactive nitrogen oxide (NOx) concentrations in the northern hemisphere have likely increased considerably between 1950 and 2001.

On the impact of impurities on the densification of polar firn

Understanding polar firn densification is crucial for reconstructing the age of greenhouse gas concentrations extracted from ice cores, and for the interpretation of air in ice as a dating tool or as a climate proxy. Firn densification is generally modeled as a steady burial and sintering process of defined layers, where the structure of the layering is maintained along the whole firn and ice column. However, available high-resolution density data, as well as firn air samples, question this picture and point to a lack of understanding of firn densification. Based on analysis of high-resolution density and calcium concentration records from Antarctic and Greenland ice cores, we show for the first time that also impurities may have a significant impact on the densification. Analysis of firn cores shows a correlation between density and the calcium ion (Ca++) concentration, and this correlation increases with depth. The existence of this relationship is independent of the local climatic conditions at the core sites analyzed. The strong positive correlation between the density and the logarithm of Ca++ concentration indicates that impurities induce softening and lead to faster densification over a wide range of concentrations. In one core, the impurity effect manifests itself so strongly that the density develops a seasonal cycle closely following the seasonal cycle of Ca++. Our results clearly show that the structure of the firn layering changes with depth and suggest that the increased variability in density observed in deep firn, recently described as a universal feature of polar firn, may arise from the influence of Ca++ and/or other impurities. The impurity effect is likely to have direct implications on our understanding of glacial firn densification and on glacial gas age estimates.

Synthetic Aperture Radar Measurements of a Retreating Firn Line on a Temperate Icecap

The firn line, like other glacier facies, is mapped operationally as part of glacier monitoring activities for glaciological and climate studies. Synthetic aperture radar (SAR) images are commonly used to determine the firn line in dry snow imagery. The radiometric response of retreating firn has not previously been investigated. Rather, it has been assumed that firn line mapping is only useful where large scale advances or retreats of the lower limit of continuous firn have occurred. In this paper the radiometric signal of retreating firn on an icecap in north Norway is analyzed using multi-temporal SAR imagery. Using comparisons with firn well above the firn line and field investigations of the firn properties, backscattering mechanisms are inferred. It is found that retreating firn has a distinctive radiometric signal that can be used to identify the inception and progression of firn down-wasting prior to and during firn line retreat.

Chemical signals of past climate and environment from polar ice cores and firn air

Chemical and isotopic records obtained from polar ice cores have provided some of the most iconic datasets in Earth system science. Here, I discuss how the different records are formed in the ice sheets, emphasising in particular the contrast between chemistry held in the snow/ice phase, and that which is trapped in air bubbles. Air diffusing slowly through the upper firn layers of the ice sheet can also be sampled in large volumes to give more recent historical information on atmospheric composition. The chemical and geophysical issues that have to be solved to interpret ice core data in terms of atmospheric composition and emission changes are also highlighted. Ice cores and firn air have provided particularly strong evidence about recent changes (last few decades to centuries), including otherwise inaccessible data on increases in compounds that are active as greenhouse gases or as agents of stratospheric depletion. On longer timescales (up to 800,000 years in Antarctica), ice cores reveal major changes in biogeochemical cycling, which acted as feedbacks on the very major changes in climate between glacial and interglacial periods.

Controls on the movement and composition of firn air at the West Antarctic Ice Sheet Divide

Abstract. We sampled interstitial air from the perennial snowpack (firn) at a site near the West Antarctic Ice Sheet Divide (WAIS-D) and analyzed the air samples for a wide variety of gas species and their isotopes. We find limited convective influence (1.4–5.2 m, depending on detection method) in the shallow firn, gravitational enrichment of heavy species throughout the diffusive column in general agreement with theoretical expectations, a ~10 m thick lock-in zone beginning at ~67 m, and a total firn thickness consistent with predictions of Kaspers et al. (2004). Our modeling work shows that the air has an age spread (spectral width) of 4.8 yr for CO2 at the firn-ice transition. We also find that advection of firn air due to the 22 cm yr−1 ice-equivalent accumulation rate has a minor impact on firn air composition, causing changes that are comparable to other modeling uncertainties and intrinsic sample variability. Furthermore, estimates of Δage (the gas age/ice age difference) at WAIS-D appear to be largely unaffected by bubble closure above the lock-in zone. Within the lock-in zone, small gas species and their isotopes show evidence of size-dependent fractionation due to permeation through the ice lattice with a size threshold of 0.36 nm, as at other sites. We also see an unequivocal and unprecedented signal of oxygen isotope fractionation within the lock-in zone, which we interpret as the mass-dependent expression of a size-dependent fractionation process.

Snow optical properties at Dome C (Concordia), Antarctica; implications for snow emissions and snow chemistry of reactive nitrogen

Abstract. Measurements of e-folding depth, nadir reflectivity and stratigraphy of the snowpack around Concordia station (Dome C, 75.10° S, 123.31° E) were undertaken to determine wavelength dependent coefficients (350 nm to 550 nm) for light scattering and absorption and to calculate potential fluxes (depth-integrated production rates) of nitrogen dioxide (NO2) from the snowpack due to nitrate photolysis within the snowpack. The stratigraphy of the top 80 cm of Dome C snowpack generally consists of three main layers:- a surface of soft windpack (not ubiquitous), a hard windpack, and a hoar-like layer beneath the windpack(s). The e-folding depths are ~10 cm for the two windpack layers and ~20 cm for the hoar-like layer for solar radiation at a wavelength of 400 nm; about a factor 2–4 larger than previous model estimates for South Pole. The absorption cross-section due to impurities in each snowpack layer are consistent with a combination of absorption due to black carbon and HULIS (HUmic LIke Substances), with amounts of 1–2 ng g−1 of black carbon for the surface snow layers. Depth-integrated photochemical production rates of NO2 in the Dome C snowpack were calculated as 5.3 × 1012 molecules m−2 s−1, 2.3 × 1012 molecules m−2 s−1 and 8 × 1011 molecules m−2 s−1 for clear skies and solar zenith angles of 60°, 70° and 80° respectively using the TUV-snow radiative-transfer model. Depending upon the snowpack stratigraphy, a minimum of 85% of the NO2 may originate from the top 20 cm of the Dome C snowpack. It is found that on a multi-annual time-scale photolysis can remove up to 80% of nitrate from surface snow, confirming independent isotopic evidence that photolysis is an important driver of nitrate loss occurring in the EAIS (East Antarctic Ice Sheet) snowpack. However, the model cannot completely account for the total observed nitrate loss of 90–95 % or the shape of the observed nitrate concentration depth profile. A more complete model will need to include also physical processes such as evaporation, re-deposition or diffusion between the quasi-liquid layer on snow grains and firn air to account for the discrepancies.

Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air

Methane and ethane are the most abundant hydrocarbons in the atmosphere and they affect both atmospheric chemistry and climate. Both gases are emitted from fossil fuels and biomass burning, whereas methane (CH(4)) alone has large sources from wetlands, agriculture, landfills and waste water. Here we use measurements in firn (perennial snowpack) air from Greenland and Antarctica to reconstruct the atmospheric variability of ethane (C(2)H(6)) during the twentieth century. Ethane levels rose from early in the century until the 1980s, when the trend reversed, with a period of decline over the next 20 years. We find that this variability was primarily driven by changes in ethane emissions from fossil fuels; these emissions peaked in the 1960s and 1970s at 14-16 teragrams per year (1 Tg = 10(12) g) and dropped to 8-10 Tg yr(-1) by the turn of the century. The reduction in fossil-fuel sources is probably related to changes in light hydrocarbon emissions associated with petroleum production and use. The ethane-based fossil-fuel emission history is strikingly different from bottom-up estimates of methane emissions from fossil-fuel use, and implies that the fossil-fuel source of methane started to decline in the 1980s and probably caused the late twentieth century slow-down in the growth rate of atmospheric methane.

Measuring the air content of the Larsen Ice Shelf

The surface elevation of the Larsen Ice Shelf in the Antarctic Peninsula has decreased by about 0.1 meter per year since 1992. This could be caused either by an increase in the density of firn (compacted snow) at the surface of the ice shelf or by an increase in melting of ice at the base of the shelf. Attributing the observed decrease to one of these causes would help researchers to know whether atmospheric or ocean warming is affecting the ice shelf. To do this, it is necessary to know the density or air content of the firn. However, firn air content has been measurable only with labor‐intensive ground‐based techniques. To overcome those challenges, Holland et al. developed a new method that uses radar sounding measurements to estimate air content. Using this approach, they observed spatial variations in the air content of the shelf. Overall, they found that the air content suggested that loss of air (increased firn density) could account for the observed lowering of the surface of the ice shelf, though the result does not rule out a contribution from melting at the base of the ice shelf. (Geophysical Research Letters, doi:10.1029/2011GL047245, 2011)

First record of testate amoebae on glaciers and description of a new species Puytoracia jenswendti nov. sp. (Rhizaria, Euglyphida)

This study documents for the first time the presence of testate amoebae on glaciers. Three shallow firn cores of 10 m depth were obtained from the Mocho-Choshuenco and Osorno volcanoes, Southern Andes, Chile, in October and November, 2005. Euglyphid testate amoebae were detected in 28 samples that correspond to the spring-summer layers of the firn cores. Inspection of 454 collected individuals reveals the presence of four different taxa. Three of these taxa, Trinema lineare, Trinema enchelys and Puytoracia bergeri have previously been reported in ice-free environments. The fourth taxon corresponds to a new species Puytoracia jenswendti nov. sp. The observation of food content and reproductive activities in a significant fraction of specimens evidence that testate amoebae are competent to inhabit glaciers. The testate amoebae found in the firn cores display clear seasonal variations in abundance indicating that these records can provide a new and novel proxy as paleoindicator for firn/ice core dating and for estimation of past glacier mass balance.

The air content of Larsen Ice Shelf

[1] The air content of glacial firn determines the effect and attribution of observed changes in ice surface elevation, but is currently measurable only using labor-intensive ground-based techniques. Here a novel method is presented for using radar sounding measurements to decompose the total thickness of floating ice shelves into thicknesses of solid ice and firn air (or firn water). The method is applied to a 1997/98 airborne survey of Larsen Ice Shelf, revealing large spatial gradients in air content that are consistent with existing measurements and local meteorology. The gradients appear to be governed by meltwater-induced firn densification. We find sufficient air in Larsen C Ice Shelf for increased densification to account for its previously observed surface lowering, and the rate of lowering superficially agrees with published trends in melting. This does not preclude a contribution to the lowering from oceanic basal melting, but a modern repeat of the survey could conclusively distinguish atmosphere-led from ocean-led change. The technique also holds promise for the calibration of firn-density models, derivation of ice thickness from surface elevation measurements, and calculation of the sea-level contribution of changes in grounded-ice discharge.

Mass change detection in Antarctic ice sheet using ICESat block analysis techniques from 2003-2008

In this paper,the ICESat laser altimetry data is used to obtain an estimate of the mass balance of Antarctic ice sheet from February 2003 to March 2008.The time series of elevation change in Antarctic ice sheet are derived by the block crossover analysis using the ICESat nadir ground track,and the calculation of the campaign basis is discussed.A least square regression of crossover difference is applied to calculate the average elevation change trend and the seasonal cycle,and then the mass changes of Antarctic ice sheet are estimated by combining the elevation change rate with the surface firn density model.The result shows that seasonal cycle signals are obvious in Antarctic ice sheet height changes,and the average annual amplitude is about 2.21 cm.On the coast of the Antarctica continent,there are significant thinning and thickening, especially near the Amundsen Sea embayment of west Antarctic and Antarctic Peninsula. Considering the influence of GIA(three public GIA models),our best estimate of the mass change in Antarctic ice sheet is about -82～-73Gt/yr.For the ICESat,the ice sheet surface firn density model and the GIA model are the main factors in the mass change estimates.

THE GLACIER COMPLEXES OF THE MOUNTAIN MASSIFS OF THE NORTH-WEST OF INNER ASIA AND THEIR DYNAMICS

The subject of this paper is the glaciation of the mountain massifs Mongun-Taiga, Tavan-Boghd-Ola, Turgeni-Nuru, and Harhira-Nuru. The glaciation is represented mostly by small forms that sometimes form a single complex of dome-shaped peaks. According to the authors, the modern glaciated area of the mountain massifs is 21.2 km 2 (Tavan-Boghd-Ola), 20.3 km 2 (Mongun-Taiga), 42 km 2 (Turgeni-Nuru), and 33.1 km 2 (Harhira-Nuru). The area of the glaciers has been shrinking since the mid 1960’s. In 1995–2008, the rate of reduction of the glaciers’ area has grown considerably: valley glaciers were rapidly degrading and splitting; accumulation of morainic material in the lower parts of the glaciers accelerated. Small glaciers transformed into snowfields and rock glaciers. There has been also a degradation of the highest parts of the glaciers and the collapse of the glacial complexes with a single zone of accumulation into isolated from each other glaciers. Reduced snow cover area has led to a rise in the firn line and the disintegration of a common accumulation area of the glacial complex. In the of the Mongun-Taiga massif, in 1995–2008, the firn line rose by 200–300 m. The reduction of the glaciers significantly lagged behind the change in the position of the accumulation area boundary. In the past two years, there has been a significant recovery of the glaciers that could eventually lead to their slower degradation or stabilization of the glaciers in the study area.

Bromide and other ions in the snow, firn air, and atmospheric boundary layer at Summit during GSHOX

Abstract. Measurements of gas phase soluble bromide in the boundary layer and in firn air, and Br− in aerosol and snow, were made at Summit, Greenland (72.5° N, 38.4° W, 3200 m a.s.l.) as part of a larger investigation into the influence of Br chemistry on HOx cycling. The soluble bromide measurements confirm that photochemical activation of Br− in the snow causes release of active Br to the overlying air despite trace concentrations of Br− in the snow (means 15 and 8 nmol Br− kg−1 of snow in 2007 and 2008, respectively). Mixing ratios of soluble bromide above the snow were also found to be very small (mean <1 ppt both years, with maxima of 3 and 4 ppt in 2007 and 2008, respectively), but these levels clearly oxidize and deposit long-lived gaseous elemental mercury and may perturb HOx partitioning. Concentrations of Br− in surface snow tended to increase/decrease in parallel with the specific activities of the aerosol-associated radionuclides 7Be and 210Pb. Earlier work has shown that ventilation of the boundary layer causes simultaneous increases in 7Be and 210Pb at Summit, suggesting there is a pool of Br in the free troposphere above Summit in summer time. Speciation and the source of this free tropospheric Br− are not well constrained, but we suggest it may be linked to extensive regions of active Br chemistry in the Arctic basin which are known to cause ozone and mercury depletion events shortly after polar sunrise. If this hypothesis is correct, it implies persistence of the free troposphere Br− for several months after peak Br activation in March/April. Alternatively, there may be a ubiquitous pool of Br− in the free troposphere, sustained by currently unknown sources and processes.

Accelerating growth of HFC-227ea (1,1,1,2,3,3,3-heptafluoropropane) in the atmosphere

Abstract. We report the first measurements of 1,1,1,2,3,3,3-heptafluoropropane (HFC-227ea), a substitute for ozone depleting compounds, in air samples originating from remote regions of the atmosphere and present evidence for its accelerating growth. Observed mixing ratios ranged from below 0.01 ppt in deep firn air to 0.59 ppt in the current northern mid-latitudinal upper troposphere. Firn air samples collected in Greenland were used to reconstruct a history of atmospheric abundance. Year-on-year increases were deduced, with acceleration in the growth rate from 0.029 ppt per year in 2000 to 0.056 ppt per year in 2007. Upper tropospheric air samples provide evidence for a continuing growth until late 2009. Furthermore we calculated a stratospheric lifetime of 370 years from measurements of air samples collected on board high altitude aircraft and balloons. Emission estimates were determined from the reconstructed atmospheric trend and suggest that current "bottom-up" estimates of global emissions for 2005 are too high by a factor of three.

Post-coring entrapment of modern air in some shallow ice cores collected near the firn-ice transition: evidence from CFC-12 measurements in Antarctic firn air and ice cores

Abstract. In this study, we report measurements of CFC-12 (CCl2F2) in firn air and in air extracted from shallow ice cores from three Antarctic sites. The firn air data are consistent with the known atmospheric history of CFC-12. In contrast, some of the ice core samples collected near the firn-ice transition exhibit anomalously high CFC-12 levels. Together, the ice core and firn air data provide evidence for the presence of modern air entrapped in the shallow ice core samples that likely contained open pores at the time of collection. We propose that this is due to closure of the open pores after drilling, entrapping modern air and resulting in elevated CFC-12 mixing ratios. Our results reveal that open porosity can exist below the maximum depth at which firn air samples can be collected, particularly at sites with lower accumulation rates. CFC-12 measurements demonstrate that post-drilling closure of open pores can lead to a change in the composition of bubble air in shallow ice cores through purely physical processes. The results have implications for investigations involving trace gas composition of bubbles in shallow ice cores collected near the firn-ice transition.

Deep air convection in the firn at a zero-accumulation site, central Antarctica

Ice cores provide unique archives of past atmospheres and climate, but interpretation of trapped-gas records and their climatic significance has been hampered by a poor knowledge of the prevalence of air convection in the firn layer on top of polar ice sheets. In particular, the phasing of greenhouse gases and climate from ice cores has been obscured by a discrepancy between empirical and model-based estimates of the age difference between trapped gases and enclosing ice, which may be due to air convection. Here we show that deep air convection (>23m) occurs at a windy, near-zero-accumulation rate site in central Antarctica known informally as the Megadunes site (80.77914°S, 124.48796°E). Deep convection is evident in depth profiles of air withdrawn from the firn layer, in the observed pattern of the nitrogen isotope ratio 15N/14N, the argon isotope ratio 40Ar/36Ar, and in the mixing ratios of the anthropogenic halocarbons methyl chloroform (CH3CCl3) and HFC-134a (CH2FCF3). Transport parameters (diffusivities) were inferred and air was dated using measured carbon dioxide (CO2) and methane (CH4) mixing ratios, by comparing with the Law Dome atmospheric record, which shows that these are the oldest firn air samples ever recovered (CO2 mean age=1863AD). The low accumulation rate and the consequent intense metamorphism of the firn (due to prolonged exposure to seasonal temperature cycling) likely contribute to deep air convection via large grain size and vertical cracks that act as conduits for vigorous air motion. The Megadunes site provides a possible modern analog for the glacial conditions in the Vostok, Dome Fuji, and Dome C ice core records and a possible explanation for lower-than-expected 15N/14N ratios in trapped air bubbles at these times. A general conclusion is that very low accumulation rate causes deep air convection via its effect on firn structural characteristics.

Estimating the equilibrium line of Devon Ice Cap, Nunavut, from RADARSAT-1 ScanSAR wide imagery

C-band synthetic aperture radar (SAR) imagery from RADARSAT-1 is used to estimate the equilibrium line of Devon Ice Cap, Nunavut, over 3 years (2004–2006). The equilibrium line is determined from the interpretation of radar glacier zones and the transient snow line (TSL). Winter SAR data cannot be used to accurately estimate the equilibrium line because the firn line obscures the end-of-summer TSL, and accumulated superimposed ice cannot be identified. A methodology to estimate the equilibrium line from frequent summer SAR acquisitions is proposed. The TSL is tracked through the ablation season, and the equilibrium line is estimated as being equal to its maximum elevation. The summer SAR data are compared with near-surface air temperatures, QuikSCAT backscatter, optical imagery, and in situ mass balance measurements. The summer SAR-derived equilibrium line altitude (ELA) is always estimated as being above the in situ measured ELA because accumulated superimposed ice cannot be identified. Uncertainty in the equilibrium line estimation is reduced where slopes face the radar look direction. The summer SAR data provide a more accurate estimation of the equilibrium line than winter data, and the estimated equilibrium line can be used to infer relative changes in net balance between years.

Polar firn air reveals large-scale impact of anthropogenic mercury emissions during the 1970s

Mercury (Hg) is an extremely toxic pollutant, and its biogeochemical cycle has been perturbed by anthropogenic emissions during recent centuries. In the atmosphere, gaseous elemental mercury (GEM; Hg degrees ) is the predominant form of mercury (up to 95%). Here we report the evolution of atmospheric levels of GEM in mid- to high-northern latitudes inferred from the interstitial air of firn (perennial snowpack) at Summit, Greenland. GEM concentrations increased rapidly after World War II from approximately 1.5 ng m(-3) reaching a maximum of approximately 3 ng m(-3) around 1970 and decreased until stabilizing at approximately 1.7 ng m(-3) around 1995. This reconstruction reproduces real-time measurements available from the Arctic since 1995 and exhibits the same general trend observed in Europe since 1990. Anthropogenic emissions caused a two-fold rise in boreal atmospheric GEM concentrations before the 1970s, which likely contributed to higher deposition of mercury in both industrialized and remotes areas. Once deposited, this toxin becomes available for methylation and, subsequently, the contamination of ecosystems. Implementation of air pollution regulations, however, enabled a large-scale decline in atmospheric mercury levels during the 1980s. The results shown here suggest that potential increases in emissions in the coming decades could have a similar large-scale impact on atmospheric Hg levels.

Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn

Abstract. The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are small. Our results indicate that the emissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6 are well constrained, whereas it is not the case for CFC-114 and CCl4. Significant emission-dependent changes in the lifetimes of halocarbons destroyed in the stratosphere were obtained. Those result from the time needed for their transport from the surface where they are emitted to the stratosphere where they are destroyed. Efforts should be made to update and reduce the large uncertainties on CFC lifetimes.