ALBERT

Description: Tunable laser direct absorption spectroscopy is a widely used technique for the in situ sensing of atmospheric composition. Aircraft deployment poses a challenging operating environment for instruments measuring climatologically relevant gases in the Earth's atmosphere. Here, we demonstrate the successful adaption of a commercially available continuous wave quantum cascade laser (QCL) and interband cascade laser (ICL) based spectrometer for airborne in situ trace gas measurements with a local to regional focus. The instrument measures methane, ethane, carbon dioxide, carbon monoxide, nitrous oxide and water vapor simultaneously, with high 1 s–1σ precision (740 ppt, 205 ppt, 460 ppb, 2.2 ppb, 137 ppt and 16 ppm, respectively) and high frequency (2 Hz). We estimate a total 1 s–1σ uncertainty of 1.85 ppb, 1.6 ppb, 1.0 ppm, 7.0 ppb and 0.8 ppb in CH4, C2H6, CO2, CO and N2O, respectively. The instrument enables simultaneous and continuous observations for all targeted species. Frequent calibration allows for a measurement duty cycle ≥90 %. Custom retrieval software has been implemented and instrument performance is reported for a first field deployment during NASA's Atmospheric Carbon and Transport – America (ACT-America) campaign in fall 2017 over the eastern and central USA. This includes an inter-instrumental comparison with a calibrated cavity ring-down greenhouse gas analyzer (operated by NASA Langley Research Center, Hampton, USA) and periodic flask samples analyzed at the National Oceanic and Atmospheric Administration (NOAA). We demonstrate good agreement of the QCL- and ICL-based instrument to these concurrent observations within the combined measurement uncertainty after correcting for a constant bias. We find that precise knowledge of the δ13C of the working standards and the sampled air is needed to enhance CO2 compatibility when operating on the 2227.604 cm−1 13C16O2 absorption line.

Description: Atmospheric inversions have been used to assess biosphere–atmosphere CO2 surface exchanges at various scales, but variability among inverse flux estimates remains significant, especially at continental scales. Atmospheric transport errors are one of the main contributors to this variability. To characterize transport errors and their spatiotemporal structures, we present an objective method to generate a calibrated ensemble adjusted with meteorological measurements collected across a region, here the upper US Midwest in midsummer. Using multiple model configurations of the Weather Research and Forecasting (WRF) model, we show that a reduced number of simulations (less than 10 members) reproduces the transport error characteristics of a 45-member ensemble while minimizing the size of the ensemble. The large ensemble of 45 members was constructed using different physics parameterization (i.e., land surface models (LSMs), planetary boundary layer (PBL) schemes, cumulus parameterizations and microphysics parameterizations) and meteorological initial/boundary conditions. All the different models were coupled to CO2 fluxes and lateral boundary conditions from CarbonTracker to simulate CO2 mole fractions. Observed meteorological variables critical to inverse flux estimates, PBL wind speed, PBL wind direction and PBL height are used to calibrate our ensemble over the region. Two optimization techniques (i.e., simulated annealing and a genetic algorithm) are used for the selection of the optimal ensemble using the flatness of the rank histograms as the main criterion. We also choose model configurations that minimize the systematic errors (i.e., monthly biases) in the ensemble. We evaluate the impact of transport errors on atmospheric CO2 mole fraction to represent up to 40 % of the model–data mismatch (fraction of the total variance). We conclude that a carefully chosen subset of the physics ensemble can represent the uncertainties in the full ensemble, and that transport ensembles calibrated with relevant meteorological variables provide a promising path forward for improving the treatment of transport uncertainties in atmospheric inverse flux estimates.

Description: Livestock numbers are increasing to supply the growing demand for meat-rich diets. The sustainability of this trend has been questioned, and future environmental changes, such as climate change, may cause some regions to become less suitable for livestock. Livestock and wild herbivores are strongly dependent on the nutritional chemistry of forage plants. Nutrition is positively linked to weight gains, milk production and reproductive success, and nutrition is also a key determinant of enteric methane production. In this meta-analysis, we assessed the effects of growing conditions on forage quality by compiling published measurements of grass nutritive value and combining these data with climatic, edaphic and management information. We found that forage nutritive value was reduced at higher temperatures and increased by nitrogen fertiliser addition, likely driven by a combination of changes to species identity and changes to physiology and phenology. These relationships were combined with multiple published empirical models to estimate forage- and temperature-driven changes to cattle enteric methane production. This suggested a previously undescribed positive climate change feedback, where elevated temperatures reduce grass nutritive value and correspondingly may increase methane production by 0.9 % with a 1 °C temperature rise and 4.5 % with a 5 °C rise (model average), thus creating an additional climate forcing effect. Future methane production increases are expected to be largest in parts of North America, central and eastern Europe and Asia, with the geographical extent of hotspots increasing under a high emissions scenario. These estimates require refinement and a greater knowledge of the abundance, size, feeding regime and location of cattle, and the representation of heat stress should be included in future modelling work. However, our results indicate that the cultivation of more nutritious forage plants and reduced livestock farming in warming regions may reduce this additional source of pastoral greenhouse gas emissions.

Description: Natural gas infrastructure releases methane (CH4), a potent greenhouse gas, into the atmosphere. The estimated emission rate associated with the production and transportation of natural gas is uncertain, hindering our understanding of its greenhouse footprint. This study presents a new application of inverse methodology for estimating regional emission rates from natural gas production and gathering facilities in north-eastern Pennsylvania. An inventory of CH4 emissions was compiled for major sources in Pennsylvania. This inventory served as input emission data for the Weather Research and Forecasting model with chemistry enabled (WRF-Chem), and atmospheric CH4 mole fraction fields were generated at 3 km resolution. Simulated atmospheric CH4 enhancements from WRF-Chem were compared to observations obtained from a 3-week flight campaign in May 2015. Modelled enhancements from sources not associated with upstream natural gas processes were assumed constant and known and therefore removed from the optimization procedure, creating a set of observed enhancements from natural gas only. Simulated emission rates from unconventional production were then adjusted to minimize the mismatch between aircraft observations and model-simulated mole fractions for 10 flights. To evaluate the method, an aircraft mass balance calculation was performed for four flights where conditions permitted its use. Using the model optimization approach, the weighted mean emission rate from unconventional natural gas production and gathering facilities in north-eastern Pennsylvania approach is found to be 0.36 % of total gas production, with a 2σ confidence interval between 0.27 and 0.45 % of production. Similarly, the mean emission estimates using the aircraft mass balance approach are calculated to be 0.40 % of regional natural gas production, with a 2σ confidence interval between 0.08 and 0.72 % of production. These emission rates as a percent of production are lower than rates found in any other basin using a top-down methodology, and may be indicative of some characteristics of the basin that make sources from the north-eastern Marcellus region unique.

Description: Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS – soot particle aerosol mass spectrometer – or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition. The second phase appears as a transitional phase during the extended polar sunrise. The third phase is marked by an increased importance of biogenically derived sulfate to the total aerosol population (photolysis of dimethyl sulfate and methanesulfonic acid (DMS and MSA)). The increased importance of MSA is identified both through the direct, real-time measurement of aerosol MSA and through the use of positive matrix factorization on the sulfur-containing ions in the high-resolution mass-spectral data. Given the importance of sub-250 nm particles, the aforementioned second phase suggests that early austral spring is the season where new particle formation mechanisms are likely to have the largest contribution to the aerosol population in Antarctica.

Description: This paper presents the physical basis of the Earth Polychromatic Imaging Camera (EPIC) cloud product algorithms and an initial evaluation of their performance. Since June 2015, EPIC has been providing observations of the sunlit side of the Earth with its 10 spectral channels ranging from the UV to the near-infrared. A suite of algorithms has been developed to generate the standard EPIC Level 2 cloud products that include cloud mask, cloud effective pressure/height, and cloud optical thickness. The EPIC cloud mask adopts the threshold method and utilizes multichannel observations and ratios as tests. Cloud effective pressure/height is derived with observations from the O2 A-band (780 and 764 nm) and B-band (680 and 688 nm) pairs. The EPIC cloud optical thickness retrieval adopts a single-channel approach in which the 780 and 680 nm channels are used for retrievals over ocean and over land, respectively. Comparison with co-located cloud retrievals from geosynchronous earth orbit (GEO) and low earth orbit (LEO) satellites shows that the EPIC cloud product algorithms are performing well and are consistent with theoretical expectations. These products are publicly available at the Atmospheric Science Data Center at the NASA Langley Research Center for climate studies and for generating other geophysical products that require cloud properties as input.

Description: We investigated the possibility of bacterial symbiosis in Globigerina bulloides, a palaeoceanographically important, planktonic foraminifer. This marine protist is commonly used in micropalaeontological investigations of climatically sensitive subpolar and temperate water masses as well as wind-driven upwelling regions of the world's oceans. G. bulloides is unusual because it lacks the protist algal symbionts that are often found in other spinose species. In addition, it has a large offset in its stable carbon and oxygen isotopic compositions compared to other planktonic foraminifer species, and also that predicted from seawater equilibrium. This is suggestive of novel differences in ecology and life history of G. bulloides, making it a good candidate for investigating the potential for bacterial symbiosis as a contributory factor influencing shell calcification. Such information is essential to evaluate fully the potential response of G. bulloides to ocean acidification and climate change. To investigate possible ecological interactions between G. bulloides and marine bacteria, 18S rRNA gene sequencing, fluorescence microscopy, 16S rRNA gene metabarcoding and transmission electron microscopy (TEM) were performed on individual specimens of G. bulloides (type IId) collected from two locations in the California Current. Intracellular DNA extracted from five G. bulloides specimens was subjected to 16S rRNA gene metabarcoding and, remarkably, 37–87 % of all 16S rRNA gene sequences recovered were assigned to operational taxonomic units (OTUs) from the picocyanobacterium Synechococcus. This finding was supported by TEM observations of intact Synechococcus cells in both the cytoplasm and vacuoles of G. bulloides. Their concentrations were up to 4 orders of magnitude greater inside the foraminifera than those reported for the California Current water column and approximately 5 % of the intracellular Synechococcus cells observed were undergoing cell division. This suggests that Synechococcus is an endobiont of G. bulloides type IId, which is the first report of a bacterial endobiont in the planktonic foraminifera. We consider the potential roles of Synechococcus and G. bulloides within the relationship and the need to determine how widespread the association is within the widely distributed G. bulloides morphospecies. The possible influence of Synechococcus respiration on G. bulloides shell geochemistry is also explored.

Description: Air quality is a major environmental concern in China, where premature deaths due to air pollution have exceeded 1 million people per year in recent years. Here, using a novel coupling of economic, physical and epidemiological models, we estimate the premature mortality related to anthropogenic outdoor PM2.5 air pollution in seven regions of China in 2010 and show for the first time how the distribution of these deaths in China is determined by a combination of economic activities and physical transport of pollution in the atmosphere. We find that 33 % (338 600 premature deaths) of China's PM2.5-related premature mortality in 2010 were caused by pollutants emitted in a different region of the country and transported in the atmosphere, especially from north to south and from east to west. Trade further extended the cross-regional impact; 56 % of (568 900 premature deaths) China's PM2.5-related premature mortality was related to consumption in another region, including 423 800 (42 % of total) and 145 100 (14 %) premature deaths from domestic consumption and international trade respectively. Our results indicate that multilateral and multi-stage cooperation under a regional sustainable development framework is in urgent need to mitigate air pollution and related health impacts, and efforts to reduce the health impacts of air pollution in China should be prioritized according to the source and location of emissions, the type and economic value of the emitting activities, and the related patterns of consumption.

Description: Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 km altitude (5 and 1 hPa). Near 2 hPa (42 km), ozone has been increasing by about 1.5 % per decade in the tropics (20° S to 20° N), and by 2 to 2.5 % per decade in the 35 to 60° latitude bands of both hemispheres. At levels below 35 km (5 hPa), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2 hPa in the 35 to 60° latitude bands from about ±5 % (2σ) in Harris et al. (2015) to less than ±2 % (2σ). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected.

Description: Reanalysis data sets are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. In this paper, we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere–troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. We also provide a systematic documentation of the treatment of WV and O3 in current reanalyses to aid future research and guide the interpretation of differences amongst reanalysis fields.The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. However, significant biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses.In contrast to O3, reanalysis estimates of stratospheric WV are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore mainly dependent on the reanalyses' representation of the physical drivers that influence stratospheric WV, such as temperatures in the tropical tropopause layer, methane oxidation, and the stratospheric overturning circulation. The lack of assimilated observations and known deficiencies in the representation of stratospheric transport in reanalyses result in much poorer agreement amongst observational and reanalysis estimates of stratospheric WV. Hence, stratospheric WV products from the current generation of reanalyses should generally not be used in scientific studies.