ORCID Profile
0000-0002-1487-0969
Current Organisation
The University of Edinburgh
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Publisher: Copernicus GmbH
Date: 19-12-2013
DOI: 10.5194/ACP-13-12451-2013
Abstract: Abstract. In situ airborne measurements were made over eastern Canada in summer 2011 as part of the BORTAS experiment (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites). In this paper we present observations of greenhouse gases (CO2 and CH4) and other biomass burning tracers (CO, HCN and CH3CN), both climatologically and through case studies, as recorded on board the FAAM BAe-146 research aircraft. Vertical profiles of CO2 were generally characterised by depleted boundary layer concentrations relative to the free troposphere, consistent with terrestrial biospheric uptake. In contrast, CH4 concentrations were found to rise with decreasing altitude due to strong local and regional surface sources. BORTAS observations were found to be broadly comparable with both previous measurements in the region during the regional burning season and with reanalysed composition fields from the EU Monitoring Atmospheric Composition and Change (MACC) project. We use coincident tracer–tracer correlations and a Lagrangian trajectory model to characterise and differentiate air mass history of intercepted plumes. In particular, CO, HCN and CH3CN were used to identify air masses that have been recently influenced by biomass burning. Examining in idual cases we were able to quantify emissions from biomass burning. Using both near-field ( 1 day) and far-field ( 1 day) s ling, boreal forest fire plumes were identified throughout the troposphere. Fresh plumes from fires in northwestern Ontario yield emission factors for CH4 and CO2 of 8.5 ± 0.9 g (kg dry matter)−1 and 1512 ± 185 g (kg dry matter)−1, respectively. We have also investigated the efficacy of calculating emission factors from far-field s ling, in which there might be expected to be limited mixing with background and other characteristic air masses, and we provide guidance on best practice and limitations in such analysis. We have found that for measurements within plumes that originated from fires in northwestern Ontario 2–4 days upwind, emission factors can be calculated that range between 1618 ± 216 and 1702 ± 173 g (kg dry matter)−1 for CO2 and 1.8 ± 0.2 and 6.1 ± 1 g (kg dry matter)−1 for CH4.
Publisher: Copernicus GmbH
Date: 30-07-2013
Abstract: Abstract. The source attribution of observed variability of total PM2.5 concentrations over Halifax, Nova Scotia, was investigated between 11 July and 26 August 2011 using measurements of PM2.5 mass and PM2.5 chemical composition (black carbon, organic matter, anions, cations and 33 elements). This was part of the BORTAS-B (quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which investigated the atmospheric chemistry and transport of seasonal boreal wildfire emissions over eastern Canada in 2011. The US EPA Positive Matrix Factorization (PMF) receptor model was used to determine the average mass (percentage) source contribution over the 45 days, which was estimated to be as follows: long-range transport (LRT) pollution: 1.75 μg m−3 (47%) LRT pollution marine mixture: 1.0 μg m−3 (27.9%) vehicles: 0.49 μg m−3 (13.2%) fugitive dust: 0.23 μg m−3 (6.3%) ship emissions: 0.13 μg m−3 (3.4%) and refinery: 0.081 μg m−3 (2.2%). The PMF model describes 87% of the observed variability in total PM2.5 mass (bias = 0.17 and RSME = 1.5 μg m−3). The factor identifications are based on chemical markers, and they are supported by air mass back trajectory analysis and local wind direction. Biomass burning plumes, found by other surface and aircraft measurements, were not significant enough to be identified in this analysis. This paper presents the results of the PMF receptor modelling, providing valuable insight into the local and upwind sources impacting surface PM2.5 in Halifax and a vital comparative data set for the other collocated ground-based observations of atmospheric composition made during BORTAS-B.
Publisher: Copernicus GmbH
Date: 04-04-2019
Abstract: Abstract. We present a method to derive atmospheric-observation-based estimates of carbon dioxide (CO2) fluxes at the national scale, demonstrated using data from a network of surface tall-tower sites across the UK and Ireland over the period 2013–2014. The inversion is carried out using simulations from a Lagrangian chemical transport model and an innovative hierarchical Bayesian Markov chain Monte Carlo (MCMC) framework, which addresses some of the traditional problems faced by inverse modelling studies, such as subjectivity in the specification of model and prior uncertainties. Biospheric fluxes related to gross primary productivity and terrestrial ecosystem respiration are solved separately in the inversion and then combined a posteriori to determine net ecosystem exchange of CO2. Two different models, Data Assimilation Linked Ecosystem Carbon (DALEC) and Joint UK Land Environment Simulator (JULES), provide prior estimates for these fluxes. We carry out separate inversions to assess the impact of these different priors on the posterior flux estimates and evaluate the differences between the prior and posterior estimates in terms of missing model components. The Numerical Atmospheric dispersion Modelling Environment (NAME) is used to relate fluxes to the measurements taken across the regional network. Posterior CO2 estimates from the two inversions agree within estimated uncertainties, despite large differences in the prior fluxes from the different models. With our method, averaging results from 2013 and 2014, we find a total annual net biospheric flux for the UK of 8±79 Tg CO2 yr−1 (DALEC prior) and 64±85 Tg CO2 yr−1 (JULES prior), where negative values represent an uptake of CO2. These biospheric CO2 estimates show that annual UK biospheric sources and sinks are roughly in balance. These annual mean estimates consistently indicate a greater net release of CO2 than the prior estimates, which show much more pronounced uptake in summer months.
Publisher: Copernicus GmbH
Date: 19-12-2011
DOI: 10.5194/ACP-11-12813-2011
Abstract: Abstract. A chemistry-transport model (CTM) intercomparison experiment (TransCom-CH4) has been designed to investigate the roles of surface emissions, transport and chemical loss in simulating the global methane distribution. Model simulations were conducted using twelve models and four model variants and results were archived for the period of 1990–2007. All but one model transports were driven by reanalysis products from 3 different meteorological agencies. The transport and removal of CH4 in six different emission scenarios were simulated, with net global emissions of 513 ± 9 and 514 ± 14 Tg CH4 yr−1 for the 1990s and 2000s, respectively. Additionally, sulfur hexafluoride (SF6) was simulated to check the interhemispheric transport, radon (222Rn) to check the subgrid scale transport, and methyl chloroform (CH3CCl3) to check the chemical removal by the tropospheric hydroxyl radical (OH). The results are compared to monthly or annual mean time series of CH4, SF6 and CH3CCl3 measurements from 8 selected background sites, and to satellite observations of CH4 in the upper troposphere and stratosphere. Most models adequately capture the vertical gradients in the stratosphere, the average long-term trends, seasonal cycles, interannual variations (IAVs) and interhemispheric (IH) gradients at the surface sites for SF6, CH3CCl3 and CH4. The vertical gradients of all tracers between the surface and the upper troposphere are consistent within the models, revealing vertical transport differences between models. An average IH exchange time of 1.39 ± 0.18 yr is derived from SF6 time series. Sensitivity simulations suggest that the estimated trends in exchange time, over the period of 1996–2007, are caused by a change of SF6 emissions towards the tropics. Using six sets of emission scenarios, we show that the decadal average CH4 growth rate likely reached equilibrium in the early 2000s due to the flattening of anthropogenic emission growth since the late 1990s. Up to 60% of the IAVs in the observed CH4 concentrations can be explained by accounting for the IAVs in emissions, from biomass burning and wetlands, as well as meteorology in the forward models. The modeled CH4 budget is shown to depend strongly on the troposphere-stratosphere exchange rate and thus on the model's vertical grid structure and circulation in the lower stratosphere. The 15-model median CH4 and CH3CCl3 atmospheric lifetimes are estimated to be 9.99 ± 0.08 and 4.61 ± 0.13 yr, respectively, with little IAV due to transport and temperature.
Publisher: Copernicus GmbH
Date: 11-11-2022
DOI: 10.5194/ESSD-14-4811-2022
Abstract: Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate is critical to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesize data sets and methodologies to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on land use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly, and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) is estimated with global ocean biogeochemistry models and observation-based data products. The terrestrial CO2 sink (SLAND) is estimated with dynamic global vegetation models. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the year 2021, EFOS increased by 5.1 % relative to 2020, with fossil emissions at 10.1 ± 0.5 GtC yr−1 (9.9 ± 0.5 GtC yr−1 when the cement carbonation sink is included), and ELUC was 1.1 ± 0.7 GtC yr−1, for a total anthropogenic CO2 emission (including the cement carbonation sink) of 10.9 ± 0.8 GtC yr−1 (40.0 ± 2.9 GtCO2). Also, for 2021, GATM was 5.2 ± 0.2 GtC yr−1 (2.5 ± 0.1 ppm yr−1), SOCEAN was 2.9 ± 0.4 GtC yr−1, and SLAND was 3.5 ± 0.9 GtC yr−1, with a BIM of −0.6 GtC yr−1 (i.e. the total estimated sources were too low or sinks were too high). The global atmospheric CO2 concentration averaged over 2021 reached 414.71 ± 0.1 ppm. Preliminary data for 2022 suggest an increase in EFOS relative to 2021 of +1.0 % (0.1 % to 1.9 %) globally and atmospheric CO2 concentration reaching 417.2 ppm, more than 50 % above pre-industrial levels (around 278 ppm). Overall, the mean and trend in the components of the global carbon budget are consistently estimated over the period 1959–2021, but discrepancies of up to 1 GtC yr−1 persist for the representation of annual to semi-decadal variability in CO2 fluxes. Comparison of estimates from multiple approaches and observations shows (1) a persistent large uncertainty in the estimate of land-use change emissions, (2) a low agreement between the different methods on the magnitude of the land CO2 flux in the northern extratropics, and (3) a discrepancy between the different methods on the strength of the ocean sink over the last decade. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set. The data presented in this work are available at 0.18160/GCP-2022 (Friedlingstein et al., 2022b).
Publisher: Copernicus GmbH
Date: 02-10-2020
Publisher: Copernicus GmbH
Date: 26-01-2023
Publisher: Springer Science and Business Media LLC
Date: 28-10-2020
DOI: 10.1038/S41586-020-2849-9
Abstract: Limiting the rise in global mean temperatures relies on reducing carbon dioxide (CO
Publisher: Authorea, Inc.
Date: 11-09-2023
Publisher: Copernicus GmbH
Date: 05-11-2021
DOI: 10.5194/ACP-21-16257-2021
Abstract: Abstract. Atmospheric measurements can be used as a tool to evaluate national greenhouse gas inventories through inverse modelling. Using 8 years of continuous methane (CH4) concentration data, this work assesses the United Kingdom's (UK) CH4 emissions over the period 2013–2020. Using two different inversion methods, we find mean emissions of 2.10 ± 0.09 and 2.12 ± 0.26 Tg yr−1 between 2013 and 2020, an overall trend of −0.05 ± 0.01 and −0.06 ± 0.04 Tg yr−2 and a 2 %–3 % decrease each year. This compares with the mean emissions of 2.23 Tg yr−1 and the trend of −0.03 Tg yr−2 (1 % annual decrease) reported in the UK's 2021 inventory between 2013 and 2019. We examine how sensitive these estimates are to various components of the inversion set-up, such as the measurement network configuration, the prior emissions estimate, the inversion method and the atmospheric transport model used. We find the decreasing trend to be due, primarily, to a reduction in emissions from England, which accounts for 70 % of the UK CH4 emissions. Comparisons during 2015 demonstrate consistency when different atmospheric transport models are used to map the relationship between sources and atmospheric observations at the aggregation level of the UK. The posterior annual national means and negative trend are found to be consistent across changes in network configuration. We show, using only two monitoring sites, that the same conclusions on mean UK emissions and negative trend would be reached as using the full six-site network, albeit with larger posterior uncertainties. However, emissions estimates from Scotland fail to converge on the same posterior under different inversion set-ups, highlighting a shortcoming of the current observation network in monitoring all of the UK. Although CH4 emissions in 2020 are estimated to have declined relative to previous years, this decrease is in line with the longer-term emissions trend and is not necessarily a response to national lockdowns.
Publisher: Copernicus GmbH
Date: 02-05-2011
Abstract: Abstract. Observations of atmospheric carbon monoxide (CO) can only be made on continental and global scales by remote sensing instruments situated in space. One such instrument is the Infrared Atmospheric Sounding Interferometer (IASI), producing spectrally resolved, top-of-atmosphere radiance measurements from which CO vertical layers and total columns can be retrieved. This paper presents a technique for intercomparisons of satellite data with low vertical resolution. The ex le in the paper also generates the first intercomparison between an IASI CO data set, in this case that produced by the University of Leicester IASI Retrieval Scheme (ULIRS), and the V3 and V4 operationally retrieved CO products from the Measurements Of Pollution In The Troposphere (MOPITT) instrument. The comparison is performed for a localised region of Africa, primarily for an ocean day-time configuration, in order to develop the technique for instrument intercomparison in a region with well defined a priori. By comparing both the standard data and a special version of MOPITT data retrieved using the ULIRS a priori for CO, it is shown that standard intercomparisons of CO are strongly affected by the differing a priori data of the retrievals, and by the differing sensitivities of the two instruments. In particular, the differing a priori profiles for MOPITT V3 and V4 data result in systematic retrieved profile changes as expected. An application of averaging kernels is used to derive a difference quantity which is much less affected by smoothing error, and hence more sensitive to systematic error. These conclusions are confirmed by simulations with model profiles for the same region. This technique is used to show that for the data that has been processed the systematic bias between MOPITT V4 and ULIRS IASI data, at MOPITT vertical resolution, is less than 7 % for the comparison data set, and on average appears to be less than 4 %. The results of this study indicate that intercomparisons of satellite data sets with low vertical resolution should ideally be performed with: retrievals using a common a priori appropriate to the geographic region studied the application of averaging kernels to compute difference quantities with reduced a priori influence and a comparison with simulated differences using model profiles for the target gas in the region.
Publisher: Copernicus GmbH
Date: 29-09-2022
Abstract: Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate is critical to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesise data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on land-use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly, and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) is estimated with global ocean biogeochemistry models and observation-based data-products. The terrestrial CO2 sink (SLAND) is estimated with dynamic global vegetation models. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the year 2021, EFOS increased by 5.1 % relative to 2020, with fossil emissions at 10.1 ± 0.5 GtC yr-1 (9.9 ± 0.5 GtC yr-1 when the cement carbonation sink is included), ELUC was 1.1 ± 0.7 GtC yr-1, for a total anthropogenic CO2 emission of 11.1 ± 0.8 GtC yr-1 (40.8 ± 2.9 GtCO2). Also, for 2021, GATM was 5.2 ± 0.2 GtC yr-1 (2.5 ± 0.1 ppm yr-1), SOCEAN was 2.9 ± 0.4 GtC yr-1 and SLAND was 3.5 ± 0.9 GtC yr-1, with a BIM of -0.6 GtC yr-1 (i.e. total estimated sources too low or sinks too high). The global atmospheric CO2 concentration averaged over 2021 reached 414.71 ± 0.1 ppm. Preliminary data for 2022, suggest an increase in EFOS relative to 2021 of +1.1 % (0 % to 1.7 %) globally, and atmospheric CO2 concentration reaching 417.3 ppm, more than 50 % above pre-industrial level. Overall, the mean and trend in the components of the global carbon budget are consistently estimated over the period 1959–2021, but discrepancies of up to 1 GtC yr-1 persist for the representation of annual to semi-decadal variability in CO2 fluxes. Comparison of estimates from multiple approaches and observations shows: (1) a persistent large uncertainty in the estimate of land-use changes emissions, (2) a low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) a discrepancy between the different methods on the strength of the ocean sink over the last decade. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set (Friedlingstein et al., 2022a Friedlingstein et al., 2020 Friedlingstein et al., 2019 Le Quéré et al., 2018b, 2018a, 2016, 2015b, 2015a, 2014, 2013). The data presented in this work are available at 0.18160/GCP-2022 (Friedlingstein et al., 2022b).
Publisher: Copernicus GmbH
Date: 05-06-2019
Abstract: Abstract. The Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme is an international collaborative project focusing on understanding the sources, processes and health effects of air pollution in the Beijing megacity. APHH-Beijing brings together leading China and UK research groups, state-of-the-art infrastructure and air quality models to work on four research themes: (1) sources and emissions of air pollutants (2) atmospheric processes affecting urban air pollution (3) air pollution exposure and health impacts and (4) interventions and solutions. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 to develop cost-effective air pollution mitigation solutions. This paper provides an introduction to (i) the rationale of the APHH-Beijing programme and (ii) the measurement and modelling activities performed as part of it. In addition, this paper introduces the meteorology and air quality conditions during two joint intensive field c aigns – a core integration activity in APHH-Beijing. The coordinated c aigns provided observations of the atmospheric chemistry and physics at two sites: (i) the Institute of Atmospheric Physics in central Beijing and (ii) Pinggu in rural Beijing during 10 November–10 December 2016 (winter) and 21 May–22 June 2017 (summer). The c aigns were complemented by numerical modelling and automatic air quality and low-cost sensor observations in the Beijing megacity. In summary, the paper provides background information on the APHH-Beijing programme and sets the scene for more focused papers addressing specific aspects, processes and effects of air pollution in Beijing.
Publisher: Copernicus GmbH
Date: 15-10-2018
DOI: 10.5194/ACP-2018-922
Abstract: Abstract. APHH-Beijing (Atmospheric Pollution and Human Health in a Chinese Megacity) is an international collaborative project to examine the emissions, processes and health effects of air pollution in Beijing. The four research themes of APHH-China are: (1) sources and emissions of urban atmospheric pollution (2) processes affecting urban atmospheric pollution (3) exposure science and impacts on health and (4) interventions and solutions to reduce health impacts. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 on the development of cost-effective solutions. A key activity within APHH-Beijing was the two month-long intensive field c aigns at two sites: (i) central Beijing, and (ii) rural Pinggu. The coordinated c aigns provided observations of the atmospheric chemistry and physics in and around Beijing during November–December 2016 and May–June 2017. The c aigns were complemented by numerical air quality modelling and air quality and meteorology data at the 12 national monitoring stations in Beijing. This introduction paper provides an overview of (i) APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it in Beijing, and (iii) the air quality and meteorological conditions during the two field c aigns. The winter c aign was characterized by high PM2.5 pollution events whereas the summer experienced high ozone pollution events. Air quality was poor during the winter c aign, but less severe than in the same period in 2015 when there were a number of major pollution episodes. PM2.5 levels were relatively low during the summer period, matching the cleanest periods over the previous five years. Synoptic scale meteorological analysis suggests that the greater stagnation and weak southerly circulation in November/December 2016 may have contributed to the poor air quality.
Publisher: Copernicus GmbH
Date: 29-09-2022
Publisher: American Geophysical Union (AGU)
Date: 2008
DOI: 10.1029/2007GL031394
Publisher: Copernicus GmbH
Date: 11-12-2020
DOI: 10.5194/ESSD-12-3269-2020
Abstract: Abstract. Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere in a changing climate – the “global carbon budget” – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe and synthesize data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. Fossil CO2 emissions (EFOS) are based on energy statistics and cement production data, while emissions from land-use change (ELUC), mainly deforestation, are based on land use and land-use change data and bookkeeping models. Atmospheric CO2 concentration is measured directly and its growth rate (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) and terrestrial CO2 sink (SLAND) are estimated with global process models constrained by observations. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2010–2019), EFOS was 9.6 ± 0.5 GtC yr−1 excluding the cement carbonation sink (9.4 ± 0.5 GtC yr−1 when the cement carbonation sink is included), and ELUC was 1.6 ± 0.7 GtC yr−1. For the same decade, GATM was 5.1 ± 0.02 GtC yr−1 (2.4 ± 0.01 ppm yr−1), SOCEAN 2.5 ± 0.6 GtC yr−1, and SLAND 3.4 ± 0.9 GtC yr−1, with a budget imbalance BIM of −0.1 GtC yr−1 indicating a near balance between estimated sources and sinks over the last decade. For the year 2019 alone, the growth in EFOS was only about 0.1 % with fossil emissions increasing to 9.9 ± 0.5 GtC yr−1 excluding the cement carbonation sink (9.7 ± 0.5 GtC yr−1 when cement carbonation sink is included), and ELUC was 1.8 ± 0.7 GtC yr−1, for total anthropogenic CO2 emissions of 11.5 ± 0.9 GtC yr−1 (42.2 ± 3.3 GtCO2). Also for 2019, GATM was 5.4 ± 0.2 GtC yr−1 (2.5 ± 0.1 ppm yr−1), SOCEAN was 2.6 ± 0.6 GtC yr−1, and SLAND was 3.1 ± 1.2 GtC yr−1, with a BIM of 0.3 GtC. The global atmospheric CO2 concentration reached 409.85 ± 0.1 ppm averaged over 2019. Preliminary data for 2020, accounting for the COVID-19-induced changes in emissions, suggest a decrease in EFOS relative to 2019 of about −7 % (median estimate) based on in idual estimates from four studies of −6 %, −7 %, −7 % (−3 % to −11 %), and −13 %. Overall, the mean and trend in the components of the global carbon budget are consistently estimated over the period 1959–2019, but discrepancies of up to 1 GtC yr−1 persist for the representation of semi-decadal variability in CO2 fluxes. Comparison of estimates from erse approaches and observations shows (1) no consensus in the mean and trend in land-use change emissions over the last decade, (2) a persistent low agreement between the different methods on the magnitude of the land CO2 flux in the northern extra-tropics, and (3) an apparent discrepancy between the different methods for the ocean sink outside the tropics, particularly in the Southern Ocean. This living data update documents changes in the methods and data sets used in this new global carbon budget and the progress in understanding of the global carbon cycle compared with previous publications of this data set (Friedlingstein et al., 2019 Le Quéré et al., 2018b, a, 2016, 2015b, a, 2014, 2013). The data presented in this work are available at 0.18160/gcp-2020 (Friedlingstein et al., 2020).
Publisher: American Geophysical Union (AGU)
Date: 13-05-2013
DOI: 10.1002/JGRD.50380
Publisher: Copernicus GmbH
Date: 29-05-2013
DOI: 10.5194/ACPD-13-14069-2013
Abstract: Abstract. In situ airborne measurements were made over Eastern Canada in summer 2011 as part of the BORTAS experiment (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and~Satellites). In this paper we present observations of greenhouse gases (CO2 and CH4) and other biomass burning tracers and related trace gases, both climatologically and through case studies, as recorded on board the FAAM BAe-146 research aircraft. Vertical profiles of CO2 were generally characterised by depleted boundary layer concentrations relative to the free troposphere, consistent with terrestrial biospheric uptake. In contrast, CH4 concentrations were found to rise with decreasing altitude due to strong local and regional surface sources. We use coincident tracer-tracer correlations and a Lagrangian trajectory model to characterise and differentiate air mass history of intercepted plumes. In particular, CO, HCN and CH3CN were used to identify air masses that have been recently influenced by biomass burning. Concentrations of CO2 were found to have a mean tropospheric, c aign-average concentration of 384.8 ppm (ranging between 371.5 and 397.1 ppm), whilst CH4 concentrations had a mean value of 1859 ppb (ranging between 1797 and 1968 ppb), representing the episodic s ling of local fire plumes. CH4 and CO2 concentrations during BORTAS were found to be broadly comparable to previous measurements in the region during the regional burning season and with reanalysed composition fields from the EU Monitoring Atmospheric Composition and Change (MACC) project. By examining in idual case studies we were able to quantify emissions from biomass burning. Using both near-field ( day) and far-field ( day) s ling, boreal forest fire plumes were identified throughout the troposphere. Fresh plumes from fires in Northwest Ontario yield emission factors for CH4 and CO2 of 8.5 ± 0.9 g (kg dry matter)−1 and 1512 g ± 185 g (kg dry matter)−1, respectively. We have also investigated the efficacy of calculating emission factors from far-field s ling, in which there might be expected to be limited mixing with background and other characteristic air masses and we provide guidance on best practice and limitations in such analysis. We have found that for measurements within plumes that originated from fires in Northwest Ontario 2–4 days upwind, emission factors can be calculated that range between 1618 ± 216 and 1702 ± 173 g (kg dry matter)−1 for CO2 and 1.8 ± 0.2 and 6.1± 1 g (kg dry matter)−1 for CH4.
Publisher: Springer Science and Business Media LLC
Date: 22-09-2013
DOI: 10.1038/NGEO1955
Publisher: Copernicus GmbH
Date: 27-09-2011
Abstract: Abstract. Near global upper tropospheric concentrations of carbon monoxide (CO), ethane (C2H6) and ethyne (C2H2) from ACE (Atmospheric Chemistry Experiment) Fourier transform spectrometer on board the Canadian satellite SCISAT-1 are presented and compared with the output from the Chemical Transport Model (CTM) GEOS-Chem. The retrievals of ethane and ethyne from ACE have been improved for this paper by using new sets of microwindows compared with those for previous versions of ACE data. With the improved ethyne retrieval we have been able to produce a near global upper tropospheric distribution of C2H2 from space. Carbon monoxide, ethane and ethyne concentrations retrieved using ACE spectra show the expected seasonality linked to variations in the anthropogenic emissions and destruction rates as well as seasonal biomass burning activity. The GEOS-Chem model was run using the dicarbonyl chemistry suite, an extended chemical mechanism in which ethyne is treated explicitly. Seasonal cycles observed from satellite data are well reproduced by the model output, however the simulated CO concentrations are found to be systematically biased low over the Northern Hemisphere. An average negative global mean bias of 12% and 7% of the model relative to the satellite observations has been found for CO and C2H6 respectively and a positive global mean bias of 1% has been found for C2H2. ACE data are compared for validation purposes with MkIV spectrometer data and Global Tropospheric Experiment (GTE) TRACE-A c aign data showing good agreement with all of them.
Publisher: Copernicus GmbH
Date: 05-10-2023
Publisher: Copernicus GmbH
Date: 02-2013
Abstract: Abstract. A modified cumulus convection parametrisation scheme is presented. This scheme computes the mass of air transported upward in a cumulus cell using conservation of moisture and a detailed distribution of convective precipitation provided by a reanalysis dataset. The representation of vertical transport within the scheme includes entrainment and detrainment processes in convective updrafts and downdrafts. Output from the proposed parametrisation scheme is employed in the National Institute for Environmental Studies (NIES) global chemical transport model driven by JRA-25/JCDAS reanalysis. The simulated convective precipitation rate and mass fluxes are compared with observations and reanalysis data. A simulation of the short-lived tracer 222Rn is used to further evaluate the performance of the cumulus convection scheme. Simulated distributions of 222Rn are evaluated against observations at the surface and in the free troposphere, and compared with output from models that participated in the TransCom-CH4 Transport Model Intercomparison. From this comparison, we demonstrate that the proposed convective scheme in general is consistent with observed and modeled results.
Publisher: Copernicus GmbH
Date: 13-06-2013
Abstract: Abstract. We use an ensemble Kalman filter (EnKF), together with the GEOS-Chem chemistry transport model, to estimate regional monthly methane (CH4) fluxes for the period June 2009–December 2010 using proxy dry-air column-averaged mole fractions of methane (XCH4) from GOSAT (Greenhouse gases Observing SATellite) and/or NOAA ESRL (Earth System Research Laboratory) and CSIRO GASLAB (Global Atmospheric S ling Laboratory) CH4 surface mole fraction measurements. Global posterior estimates using GOSAT and/or surface measurements are between 510–516 Tg yr−1, which is less than, though within the uncertainty of, the prior global flux of 529 ± 25 Tg yr−1. We find larger differences between regional prior and posterior fluxes, with the largest changes in monthly emissions (75 Tg yr−1) occurring in Temperate Eurasia. In non-boreal regions the error reductions for inversions using the GOSAT data are at least three times larger (up to 45%) than if only surface data are assimilated, a reflection of the greater spatial coverage of GOSAT, with the two exceptions of latitudes ° associated with a data filter and over Europe where the surface network adequately describes fluxes on our model spatial and temporal grid. We use CarbonTracker and GEOS-Chem XCO2 model output to investigate model error on quantifying proxy GOSAT XCH4 (involving model XCO2) and inferring methane flux estimates from surface mole fraction data and show similar resulting fluxes, with differences reflecting initial differences in the proxy value. Using a series of observing system simulation experiments (OSSEs) we characterize the posterior flux error introduced by non-uniform atmospheric s ling by GOSAT. We show that clear-sky measurements can theoretically reproduce fluxes within 10% of true values, with the exception of tropical regions where, due to a large seasonal cycle in the number of measurements because of clouds and aerosols, fluxes are within 15% of true fluxes. We evaluate our posterior methane fluxes by incorporating them into GEOS-Chem and s ling the model at the location and time of surface CH4 measurements from the AGAGE (Advanced Global Atmospheric Gases Experiment) network and column XCH4 measurements from TCCON (Total Carbon Column Observing Network). The posterior fluxes modestly improve the model agreement with AGAGE and TCCON data relative to prior fluxes, with the correlation coefficients (r2) increasing by a mean of 0.04 (range: −0.17 to 0.23) and the biases decreasing by a mean of 0.4 ppb (range: −8.9 to 8.4 ppb).
Publisher: Copernicus GmbH
Date: 26-01-2023
Abstract: Abstract. Quantification of land surface-atmosphere fluxes of carbon dioxide (CO2) fluxes and their trends and uncertainties is essential for monitoring progress of the EU27+UK bloc as it strives to meet ambitious targets determined by both international agreements and internal regulation. This study provides a consolidated synthesis of fossil sources (CO2 fossil) and natural sources and sinks over land (CO2 land) using bottom-up (BU) and top-down (TD) approaches for the European Union and United Kingdom (EU27+UK), updating earlier syntheses (Petrescu et al., 2020, 2021b). Given the wide scope of the work and the variety of approaches involved, this study aims to answer essential questions identified in the previous syntheses and understand the differences between datasets, particularly for poorly characterized fluxes from managed ecosystems. The work integrates updated emission inventory data, process-based model results, data-driven sectoral model results, and inverse modeling estimates, extending the previous period 1990–2018 to the year 2020 to the extent possible. BU and TD products are compared with European National Greenhouse Gas Inventories (NGHGIs) reported by Parties including the year 2019 under the United Nations Framework Convention on Climate Change (UNFCCC). The uncertainties of the EU27+UK NGHGI were evaluated using the standard deviation reported by the EU Member States following the guidelines of the Intergovernmental Panel on Climate Change (IPCC) and harmonized by gap-filling procedures. Variation in estimates produced with other methods, such as atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), originate from within-model uncertainty related to parameterization as well as structural differences between models. By comparing NGHGIs with other approaches, key sources of differences between estimates arise primarily in activities. System boundaries and emission categories create differences in CO2 fossil datasets, while different land use definitions for reporting emissions from Land Use, Land Use Change and Forestry (LULUCF) activities result in differences for CO2 land. The latter has important consequences for atmospheric inversions, leading to inversions reporting stronger sinks in vegetation and soils than are reported by the NGHGI. For CO2 fossil emissions, after harmonizing estimates based on common activities and selecting the most recent year available for all datasets, the UNFCCC NGHGI for the EU27+UK accounts for 3392 ± 49 Tg CO2 yr-1 (926 ± 13 Tg C yr-1), while eight other BU sources report a mean value of 3340 [3238,3401] [25th,75th percentile] Tg CO2 yr-1 (948 [937,961] Tg C yr-1). The sole top-down inversion of fossil emissions currently available accounts for 3800 Tg CO2 yr-1 (1038 Tg C yr-1), a value close to that of the NGHGI, but for which uncertainty estimates are not yet available. For the net CO2 land fluxes, during the most recent five-year period including the NGHGI estimates, the NGHGI accounted for -91 ± 32 Tg C yr-1 while six other BU approaches reported a mean sink of -62 [-117,-49] Tg C yr-1 and a 15-member ensemble of dynamic global vegetation models (DGVMs) reported -69 [-152,-5] Tg C yr-1. The five-year mean of three TD regional ensembles combined with one non-ensemble inversion of -73 Tg C yr-1 has a slightly smaller spread (0th–100th percentile of [-135,45] Tg C yr-1), and was calculated after removing land-atmosphere CO2 fluxes caused by lateral transport of carbon (crops, wood trade and inland waters) resulting in increased agreement with the the NGHGI and bottom-up approaches. Results at the sub-sector level (Forestland, Cropland, Grassland) show generally good agreement between the NGHGI and sub-sector-specific models, but results for a DGVM are mixed. Overall, for both CO2 fossil and net CO2 land fluxes, we find current independent approaches are consistent with the NGHGI at the scale of the EU27+UK. We conclude that CO2 emissions from fossil sources have decreased over the past 30 years in the EU27+UK, while large uncertainties on net uptake of CO2 by the land surface prevent trend identification. In addition, a gap on the order of 1000 Tg C yr-1 between CO2 fossil emissions and net CO2 uptake by the land exists regardless of the type of approach (NGHGI, TD, BU), falling well outside all available estimates of uncertainties. However, uncertainties in top-down approaches to estimate CO2 fossil emissions remain uncharacterized and are likely substantial. The data used to plot the figures are available at 0.5281/zenodo.7365863.
Publisher: American Geophysical Union (AGU)
Date: 15-03-2011
DOI: 10.1029/2010JD014483
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Paul Palmer.