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16 result(s) for "Lunder, Chris Rene"
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Atmospheric new particle formation characteristics in the Arctic as measured at Mount Zeppelin, Svalbard, from 2016 to 2018
We conducted continuous measurements of nanoparticles down to 3 nm size in the Arctic at Mount Zeppelin, Ny Ålesund, Svalbard, from October 2016 to December 2018, providing a size distribution of nanoparticles (3–60 nm). A significant number of nanoparticles as small as 3 nm were often observed during new particle formation (NPF), particularly in summer, suggesting that these were likely produced near the site rather than being transported from other regions after growth. The average NPF frequency per year was 23 %, having the highest percentage in August (63 %). The average formation rate (J) and growth rate (GR) for 3–7 nm particles were 0.04 cm−3 s−1 and 2.07 nm h−1, respectively. Although NPF frequency in the Arctic was comparable to that in continental areas, the J and GR were much lower. The number of nanoparticles increased more frequently when air mass originated over the south and southwest ocean regions; this pattern overlapped with regions having strong chlorophyll a concentration and dimethyl sulfide (DMS) production capacity (southwest ocean) and was also associated with increased NH3 and H2SO4 concentration, suggesting that marine biogenic sources were responsible for gaseous precursors to NPF. Our results show that previously developed NPF occurrence criteria (low loss rate and high cluster growth rate favor NPF) are also applicable to NPF in the Arctic.
Historical greenhouse gas concentrations for climate modelling (CMIP6)
Atmospheric greenhouse gas (GHG) concentrations are at unprecedented, record-high levels compared to the last 800 000 years. Those elevated GHG concentrations warm the planet and – partially offset by net cooling effects by aerosols – are largely responsible for the observed warming over the past 150 years. An accurate representation of GHG concentrations is hence important to understand and model recent climate change. So far, community efforts to create composite datasets of GHG concentrations with seasonal and latitudinal information have focused on marine boundary layer conditions and recent trends since the 1980s. Here, we provide consolidated datasets of historical atmospheric concentrations (mole fractions) of 43 GHGs to be used in the Climate Model Intercomparison Project – Phase 6 (CMIP6) experiments. The presented datasets are based on AGAGE and NOAA networks, firn and ice core data, and archived air data, and a large set of published studies. In contrast to previous intercomparisons, the new datasets are latitudinally resolved and include seasonality. We focus on the period 1850–2014 for historical CMIP6 runs, but data are also provided for the last 2000 years. We provide consolidated datasets in various spatiotemporal resolutions for carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O), as well as 40 other GHGs, namely 17 ozone-depleting substances, 11 hydrofluorocarbons (HFCs), 9 perfluorocarbons (PFCs), sulfur hexafluoride (SF6), nitrogen trifluoride (NF3) and sulfuryl fluoride (SO2F2). In addition, we provide three equivalence species that aggregate concentrations of GHGs other than CO2, CH4 and N2O, weighted by their radiative forcing efficiencies. For the year 1850, which is used for pre-industrial control runs, we estimate annual global-mean surface concentrations of CO2 at 284.3 ppm, CH4 at 808.2 ppb and N2O at 273.0 ppb. The data are available at https://esgf-node.llnl.gov/search/input4mips/ and http://www.climatecollege.unimelb.edu.au/cmip6 . While the minimum CMIP6 recommendation is to use the global- and annual-mean time series, modelling groups can also choose our monthly and latitudinally resolved concentrations, which imply a stronger radiative forcing in the Northern Hemisphere winter (due to the latitudinal gradient and seasonality).
Estimation of the atmospheric hydroxyl radical oxidative capacity using multiple hydrofluorocarbons (HFCs)
The hydroxyl radical (OH) largely determines the atmosphere's oxidative capacity and, thus, the lifetimes of numerous trace gases, including methane (CH4). Hitherto, observation-based approaches for estimating the atmospheric oxidative capacity have primarily relied on using methyl chloroform (MCF), but as the atmospheric abundance of MCF has declined, the uncertainties associated with this method have increased. In this study, we examine the use of five hydrofluorocarbons (HFCs) (HFC-134a, HFC-152a, HFC-365mfc, HFC-245fa, and HFC-32) in multi-species inversions, which assimilate three HFCs simultaneously, as an alternative method to estimate atmospheric OH. We find robust estimates of OH regardless of which combination of the three HFCs are used in the inversions. Our results show that OH has remained fairly stable during our study period from 2004 to 2021, with variations of
Consumption of CH3Cl, CH3Br, and CH3I and emission of CHCl3, CHBr3, and CH2Br2 from the forefield of a retreating Arctic glacier
The Arctic is one of the most rapidly warming regions of the Earth, with predicted temperature increases of 5–7 ∘C and the accompanying extensive retreat of Arctic glacial systems by 2100. Retreating glaciers will reveal new land surfaces for microbial colonisation, ultimately succeeding to tundra over decades to centuries. An unexplored dimension to these changes is the impact upon the emission and consumption of halogenated organic compounds (halocarbons). Halocarbons are involved in several important atmospheric processes, including ozone destruction, and despite considerable research, uncertainties remain in the natural cycles of some of these compounds. Using flux chambers, we measured halocarbon fluxes across the glacier forefield (the area between the present-day position of a glacier's ice-front and that at the last glacial maximum) of a high-Arctic glacier in Svalbard, spanning recently exposed sediments (<10 years) to approximately 1950-year-old tundra. Forefield land surfaces were found to consume methyl chloride (CH3Cl) and methyl bromide (CH3Br), with both consumption and emission of methyl iodide (CH3I) observed. Bromoform (CHBr3) and dibromomethane (CH2Br2) have rarely been measured from terrestrial sources but were here found to be emitted across the forefield. Novel measurements conducted on terrestrial cyanobacterial mats covering relatively young surfaces showed similar measured fluxes to the oldest, vegetated tundra sites for CH3Cl, CH3Br, and CH3I (which were consumed) and for CHCl3 and CHBr3 (which were emitted). Consumption rates of CH3Cl and CH3Br and emission rates of CHCl3 from tundra and cyanobacterial mat sites were within the ranges reported from older and more established Arctic tundra elsewhere. Rough calculations showed total emissions and consumptions of these gases across the Arctic were small relative to other sources and sinks due to the small surface area represented by glacier forefields. We have demonstrated that glacier forefields can consume and emit halocarbons despite their young age and low soil development, particularly when cyanobacterial mats are present.
Aerosol and dynamical contributions to cloud droplet formation in Arctic low-level clouds
The Arctic is one of the most rapidly warming regions of the globe. Low-level clouds and fog modify the energy transfer from and to space and play a key role in the observed strong Arctic surface warming, a phenomenon commonly termed “Arctic amplification”. The response of low-level clouds to changing aerosol characteristics throughout the year is therefore an important driver of Arctic change that currently lacks sufficient constraints. As such, during the NASCENT campaign (Ny-Ålesund AeroSol Cloud ExperimeNT) extending over a full year from October 2019 to October 2020, microphysical properties of aerosols and clouds were studied at the Zeppelin station (475 m a.s.l.), Ny-Ålesund, Svalbard, Norway. Particle number size distributions obtained from differential mobility particle sizers as well as chemical composition derived from filter samples and an aerosol chemical speciation monitor were analyzed together with meteorological data, in particular vertical wind velocity. The results were used as input to a state-of-the-art cloud droplet formation parameterization to investigate the particle sizes that can activate to cloud droplets, the levels of supersaturation that can develop, the droplet susceptibility to aerosol and the role of vertical velocity. We evaluate the parameterization and the droplet numbers calculated through a droplet closure with in-cloud in situ measurements taken during nine flights over 4 d. A remarkable finding is that, for the clouds sampled in situ, closure is successful in mixed-phase cloud conditions regardless of the cloud glaciation fraction. This suggests that ice production through ice–ice collisions or droplet shattering may have explained the high ice fraction, as opposed to rime splintering that would have significantly reduced the cloud droplet number below levels predicted by warm-cloud activation theory. We also show that pristine-like conditions during fall led to clouds that formed over an aerosol-limited regime, with high levels of supersaturation (generally around 1 %, although highly variable) that activate particles smaller than 20 nm in diameter. Clouds formed in the same regime in late spring and summer, but aerosol activation diameters were much larger due to lower cloud supersaturations (ca. 0.5 %) that develop because of higher aerosol concentrations and lower vertical velocities. The contribution of new particle formation to cloud formation was therefore strongly limited, at least until these newly formed particles started growing. However, clouds forming during the Arctic haze period (winter and early spring) can be limited by updraft velocity, although rarely, with supersaturation levels dropping below 0.1 % and generally activating larger particles (20 to 200 nm), including pollution transported over a long range. The relationship between updraft velocity and the limiting cloud droplet number agrees with previous observations of various types of clouds worldwide, which supports the universality of this relationship.
Tracing biomass burning aerosol from South America to Troll Research Station, Antarctica
The atmospheric observatory at the Norwegian Research Station Troll in Queen Maud Land, Antarctica, holds, since February 2007, the first all-year Antarctic atmospheric aerosol particle number size distribution measurements. These are colocated with measurements of the aerosol absorption and spectral scattering coefficients. In June 2007, this instrument set observed an aerosol whose properties were indicative of a biomass burning aerosol. These properties included two log-normal size distribution modes with median particle diameters of 0.105 μm and 0.36 μm, sharply falling off to smaller and larger sizes, and peaks in scattering and absorption coefficient. With backward plume calculations of the Lagrangian transport model FLEXPART and the MODIS fire activity product, a source-receptor relationship was established between biomass burning events in Central Brazil and the aerosol seen at Troll. This is the first direct evidence that the Antarctic continent is susceptible to emissions from as far north as Southern tropical latitudes.
Atmospheric histories and global emissions of the anthropogenic hydrofluorocarbons HFC-365mfc, HFC-245fa, HFC-227ea, and HFC-236fa
We report on ground‐based atmospheric measurements and emission estimates of the four anthropogenic hydrofluorocarbons (HFCs) HFC‐365mfc (CH3CF2CH2CF3, 1,1,1,3,3‐pentafluorobutane), HFC‐245fa (CHF2CH2CF3, 1,1,1,3,3‐pentafluoropropane), HFC‐227ea (CF3CHFCF3, 1,1,1,2,3,3,3‐heptafluoropropane), and HFC‐236fa (CF3CH2CF3, 1,1,1,3,3,3‐hexafluoropropane). In situ measurements are from the global monitoring sites of the Advanced Global Atmospheric Gases Experiment (AGAGE), the System for Observations of Halogenated Greenhouse Gases in Europe (SOGE), and Gosan (South Korea). We include the first halocarbon flask sample measurements from the Antarctic research stations King Sejong and Troll. We also present measurements of archived air samples from both hemispheres back to the 1970s. We use a two‐dimensional atmospheric transport model to simulate global atmospheric abundances and to estimate global emissions. HFC‐365mfc and HFC‐245fa first appeared in the atmosphere only ∼1 decade ago; they have grown rapidly to globally averaged dry air mole fractions of 0.53 ppt (in parts per trillion, 10−12) and 1.1 ppt, respectively, by the end of 2010. In contrast, HFC‐227ea first appeared in the global atmosphere in the 1980s and has since grown to ∼0.58 ppt. We report the first measurements of HFC‐236fa in the atmosphere. This long‐lived compound was present in the atmosphere at only 0.074 ppt in 2010. All four substances exhibit yearly growth rates of >8% yr−1 at the end of 2010. We find rapidly increasing emissions for the foam‐blowing compounds HFC‐365mfc and HFC‐245fa starting in ∼2002. After peaking in 2006 (HFC‐365mfc: 3.2 kt yr−1, HFC‐245fa: 6.5 kt yr−1), emissions began to decline. Our results for these two compounds suggest that recent estimates from long‐term projections (to the late 21st century) have strongly overestimated emissions for the early years of the projections (∼2005–2010). Global HFC‐227ea and HFC‐236fa emissions have grown to average values of 2.4 kt yr−1 and 0.18 kt yr−1 over the 2008–2010 period, respectively. Key Points Four anthropogenic greenhouse gases in the atmosphere are reported on Global emissions are determined using inverse modeling techniques Atmospheric burden grows rapidly, but by far not as fast as recently predicted