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"MCGRATH, Matthew J"
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Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere
by
Schobesberger, Siegfried
,
Ehrhart, Sebastian
,
Curtius, Joachim
in
704/106/35/824
,
Acids
,
Aerosols
2013
Amines at typical atmospheric concentrations of a only few molecules per trillion air molecules combine with sulphuric acid to form highly stable aerosol particles at rates similar to those observed in the lower atmosphere.
Atmospheric chemistry of anthropogenic amines
Amines emitted into the atmosphere from anthropogenic sources are thought to enhance nucleation from trace atmospheric vapours, stimulate particle formation and influence the development and properties of clouds. Direct evidence for this under atmospheric conditions has been lacking; however, this study, using the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN, demonstrates that amines at atmospherically relevant concentrations can sufficiently increase nucleation rates to be able to account for the particle formation rates observed in the atmospheric environment.
Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei
1
. Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes
2
. Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases
2
. However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere
3
. It is thought that amines may enhance nucleation
4
,
5
,
6
,
7
,
8
,
9
,
10
,
11
,
12
,
13
,
14
,
15
,
16
, but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid–amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid–dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
Journal Article
Global Carbon Budget 2022
by
Alin, Simone R
,
Falk, Stefanie
,
Gehlen, Marion
in
Anthropogenic factors
,
Atmosphere
,
Atmospheric models
2022
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 https://doi.org/10.18160/GCP-2022 (Friedlingstein et al., 2022b).
Journal Article
Europe's forest management did not mitigate climate warming
2016
Afforestation and forest management are considered to be key instruments in mitigating climate change. Here we show that since 1750, in spite of considerable afforestation, wood extraction has led to Europe's forests accumulating a carbon debt of 3.1 petagrams of carbon. We found that afforestation is responsible for an increase of 0.12 watts per square meter in the radiative imbalance at the top of the atmosphere, whereas an increase of 0.12 kelvin in summertime atmospheric boundary layer temperature was mainly caused by species conversion. Thus, two and a half centuries of forest management in Europe have not cooled the climate. The political imperative to mitigate climate change through afforestation and forest management therefore risks failure, unless it is recognized that not all forestry contributes to climate change mitigation.
Journal Article
The consolidated European synthesis of CH4 and N2O emissions for the European Union and United Kingdom: 1990–2017
by
Regnier, Pierre
,
Tian, Hanqin
,
Bastviken, David
in
Agriculture
,
Anthropogenic factors
,
Atmospheric models
2021
Reliable quantification of the sources and sinks of greenhouse gases, together with trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Paris Agreement. This study provides a consolidated synthesis of CH4 andN2O emissions with consistently derived state-of-the-art bottom-up (BU) and top-down (TD) data sources for the European Union and UK (EU27 + UK). We integrate recent emission inventory data, ecosystem process-based model results and inverse modeling estimates over the period 1990–2017. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported to the UN climate convention UNFCCC secretariat in 2019. For uncertainties, we used for NGHGIs the standard deviation obtained by varying parameters of inventory calculations, reported by the member states (MSs) following the recommendations of the IPCC Guidelines. For atmospheric inversion models (TD) or other inventory datasets (BU), we defined uncertainties from the spread between different model estimates or model-specific uncertainties when reported. In comparing NGHGIs with other approaches, a key source of bias is the activities included, e.g., anthropogenic versus anthropogenic plus natural fluxes. In inversions, the separation between anthropogenic and natural emissions is sensitive to the geospatial prior distribution of emissions. Over the 2011–2015 period, which is the common denominator of data availability between all sources, the anthropogenic BU approaches are directly comparable, reporting mean emissions of 20.8 TgCH4yr-1 (EDGAR v5.0) and 19.0 TgCH4yr-1 (GAINS), consistent with the NGHGI estimates of 18.9 ± 1.7 TgCH4yr-1. The estimates of TD total inversions give higher emission estimates, as they also include natural emissions. Over the same period regional TD inversions with higher-resolution atmospheric transport models give a mean emission of 28.8 TgCH4yr-1. Coarser-resolution global TD inversions are consistent with regional TD inversions, for global inversions with GOSAT satellite data (23.3 TgCH4yr-1) and surface network (24.4 TgCH4yr-1). The magnitude of natural peatland emissions from the JSBACH–HIMMELI model, natural rivers and lakes emissions, and geological sources together account for the gap between NGHGIs and inversions and account for 5.2 TgCH4yr-1. For N2O emissions, over the 2011–2015 period, both BU approaches (EDGAR v5.0 and GAINS) give a mean value of anthropogenic emissions of 0.8 and 0.9 TgN2Oyr-1, respectively, agreeing with the NGHGI data (0.9 ± 0.6 TgN2Oyr-1). Over the same period, the average of the three total TD global and regional inversions was 1.3 ± 0.4 and 1.3 ± 0.1 TgN2Oyr-1, respectively. The TD and BU comparison method defined in this study can be operationalized for future yearly updates for the calculation of CH4 and N2O budgets both at the EU+UK scale and at the national scale. The referenced datasets related to figures are visualized at 10.5281/zenodo.4590875 (Petrescu et al., 2020b).
Journal Article
Trade-offs in using European forests to meet climate objectives
by
Naudts, Kim
,
Njakou Djomo, Sylvestre
,
Lansø, Anne Sofie
in
21st century
,
631/158/1145
,
704/106/694/682
2018
The Paris Agreement promotes forest management as a pathway towards halting climate warming through the reduction of carbon dioxide (CO
2
) emissions
1
. However, the climate benefits from carbon sequestration through forest management may be reinforced, counteracted or even offset by concurrent management-induced changes in surface albedo, land-surface roughness, emissions of biogenic volatile organic compounds, transpiration and sensible heat flux
2
–
4
. Consequently, forest management could offset CO
2
emissions without halting global temperature rise. It therefore remains to be confirmed whether commonly proposed sustainable European forest-management portfolios would comply with the Paris Agreement—that is, whether they can reduce the growth rate of atmospheric CO
2
, reduce the radiative imbalance at the top of the atmosphere, and neither increase the near-surface air temperature nor decrease precipitation by the end of the twenty-first century. Here we show that the portfolio made up of management systems that locally maximize the carbon sink through carbon sequestration, wood use and product and energy substitution reduces the growth rate of atmospheric CO
2
, but does not meet any of the other criteria. The portfolios that maximize the carbon sink or forest albedo pass only one—different in each case—criterion. Managing the European forests with the objective of reducing near-surface air temperature, on the other hand, will also reduce the atmospheric CO
2
growth rate, thus meeting two of the four criteria. Trade-off are thus unavoidable when using European forests to meet climate objectives. Furthermore, our results demonstrate that if present-day forest cover is sustained, the additional climate benefits achieved through forest management would be modest and local, rather than global. On the basis of these findings, we argue that Europe should not rely on forest management to mitigate climate change. The modest climate effects from changes in forest management imply, however, that if adaptation to future climate were to require large-scale changes in species composition and silvicultural systems over Europe
5
,
6
, the forests could be adapted to climate change with neither positive nor negative climate effects.
Simulations of commonly proposed forest-management portfolios for Europe show that no single portfolio would meet all the requirements of the Paris Agreement, and climate benefits from forest management would be modest and local.
Journal Article
The key role of forest disturbance in reconciling estimates of the northern carbon sink
2024
Northern forests are an important carbon sink, but our understanding of the driving factors is limited due to discrepancies between dynamic global vegetation models (DGVMs) and atmospheric inversions. We show that DGVMs simulate a 50% lower sink (1.1 ± 0.5 PgC yr
−1
over 2001–2021) across North America, Europe, Russia, and China compared to atmospheric inversions (2.2 ± 0.6 PgC yr
−1
). We explain why DGVMs underestimate the carbon sink by considering how they represent disturbance processes, specifically the overestimation of fire emissions, and the lack of robust forest demography resulting in lower forest regrowth rates than observed. We reconcile net sink estimates by using alternative disturbance-related fluxes. We estimate carbon uptake through forest regrowth by combining satellite-derived forest age and biomass maps. We calculate a regrowth flux of 1.1 ± 0.1 PgC yr
−1
, and combine this with satellite-derived estimates of fire emissions (0.4 ± 0.1 PgC yr
−1
), land-use change emissions from bookkeeping models (0.9 ± 0.2 PgC yr
−1
), and the DGVM-estimated sink from CO
2
fertilisation, nitrogen deposition, and climate change (2.2 ± 0.9 PgC yr
−1
). The resulting ‘bottom-up’ net flux of 2.1 ± 0.9 PgC yr
−1
agrees with atmospheric inversions. The reconciliation holds at regional scales, increasing confidence in our results.
A satellite-based estimate of forest regrowth carbon flux across the Northern Hemisphere suggests forest disturbance and regrowth are transient but important aspects of the carbon sink that may explain underestimates from dynamic global vegetation models
Journal Article
Land management and land-cover change have impacts of similar magnitude on surface temperature
2014
The direct effects of land-cover change on surface climate are increasingly well understood, but fewer studies have investigated the consequences of the trend towards more intensive land management practices. Now, research investigating the biophysical effects of temperate land-management changes reveals a net warming effect of similar magnitude to that driven by changing land cover.
Anthropogenic changes to land cover (LCC) remain common, but continuing land scarcity promotes the widespread intensification of land management changes (LMC) to better satisfy societal demand for food, fibre, fuel and shelter
1
. The biophysical effects of LCC on surface climate are largely understood
2
,
3
,
4
,
5
, particularly for the boreal
6
and tropical zones
7
, but fewer studies have investigated the biophysical consequences of LMC; that is, anthropogenic modification without a change in land cover type. Harmonized analysis of ground measurements and remote sensing observations of both LCC and LMC revealed that, in the temperate zone, potential surface cooling from increased albedo is typically offset by warming from decreased sensible heat fluxes, with the net effect being a warming of the surface. Temperature changes from LMC and LCC were of the same magnitude, and averaged 2 K at the vegetation surface and were estimated at 1.7 K in the planetary boundary layer. Given the spatial extent of land management (42–58% of the land surface) this calls for increasing the efforts to integrate land management in Earth System Science to better take into account the human impact on the climate
8
.
Journal Article
Greenhouse gas emissions and their trends over the last 3 decades across Africa
by
Patra, Prabir K.
,
Mostefaoui, Mounia
,
McGrath, Matthew J.
in
Air pollution
,
Anthropogenic factors
,
Atmospheric models
2024
A key goal of the Paris Agreement (PA) is to reach net-zero greenhouse gas (GHG) emissions by 2050 globally, which requires mitigation efforts from all countries. Africa's rapidly growing population and gross domestic product (GDP) make this continent important for GHG emission trends. In this paper, we study the emissions of carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O) in Africa over 3 decades (1990–2018). We compare bottom-up (BU) approaches, including United Nations Convention Framework on Climate Change (UNFCCC) national inventories, FAO, PRIMAP-hist, process-based ecosystem models for CO2 fluxes in the land use, land use change and forestry (LULUCF) sector and global atmospheric inversions. For inversions, we applied different methods to separate anthropogenic CH4 emissions. The BU inventories show that, over the decade 2010–2018, fewer than 10 countries represented more than 75 % of African fossil CO2 emissions. With a mean of 1373 Mt CO2 yr−1, total African fossil CO2 emissions over 2010–2018 represent only 4 % of global fossil emissions. However, these emissions grew by +34 % from 1990–1999 to 2000–2009 and by +31 % from 2000–2009 to 2010–2018, which represents more than a doubling in 30 years. This growth rate is more than 2 times faster than the global growth rate of fossil CO2 emissions. The anthropogenic emissions of CH4 grew by 5 % from 1990–1999 to 2000–2009 and by 14.8 % from 2000–2009 to 2010–2018. The N2O emissions grew by 19.5 % from 1990–1999 to 2000–2009 and by 20.8 % from 2000–2009 to 2010–2018. When using the mean of the estimates from UNFCCC reports (including the land use sector) with corrections from outliers, Africa was a mean source of greenhouse gases of 262221863239 Mt CO2 eq. yr−1 from all BU estimates (the subscript and superscript indicate min–max range uncertainties) and of +263717615873 Mt CO2 eq. yr−1 from top-down (TD) methods during their overlap period from 2001 to 2017. Although the mean values are consistent, the range of TD estimates is larger than the one of the BU estimates, indicating that sparse atmospheric observations and transport model errors do not allow us to use inversions to reduce the uncertainty in BU estimates. The main source of uncertainty comes from CO2 fluxes in the LULUCF sector, for which the spread across inversions is larger than 50 %, especially in central Africa. Moreover, estimates from national UNFCCC communications differ widely depending on whether the large sinks in a few countries are corrected to more plausible values using more recent national sources following the methodology of Grassi et al. (2022). The medians of CH4 emissions from inversions based on satellite retrievals and surface station networks are consistent with each other within 2 % at the continental scale. The inversion ensemble also provides consistent estimates of anthropogenic CH4 emissions with BU inventories such as PRIMAP-hist. For N2O, inversions systematically show higher emissions than inventories, on average about 4.5 times more than PRIMAP-hist, either because natural N2O sources cannot be separated accurately from anthropogenic ones in inversions or because BU estimates ignore indirect emissions and underestimate emission factors. Future improvements can be expected thanks to a denser network of monitoring atmospheric concentrations. This study helps to introduce methods to enhance the scope of use of various published datasets and allows us to compute budgets thanks to recombinations of those data products. Our results allow us to understand uncertainty and trends in emissions and removals in a region of the world where few observations exist and where most inventories are based on default IPCC guideline values. The results can therefore serve as a support tool for the Global Stocktake (GST) of the Paris Agreement. The referenced datasets related to the figures are available at https://doi.org/10.5281/zenodo.7347077 (Mostefaoui et al., 2022).
Journal Article
Harmonising the Land-Use Flux Estimates of Global Models and National Inventories for 2000–2020
by
Falk, Stefanie
,
Sitch, Stephen
,
Cescatti, Alessandro
in
Air pollution
,
Analysis
,
Anthropogenic factors
2023
As the focus of climate policy shifts from pledges to implementation, there is a growing need to track progress on climate change mitigation at the country level, particularly for the land-use sector. Despite new tools and models providing unprecedented monitoring opportunities, striking differences remain in estimations of anthropogenic land-use CO2 fluxes between, on the one hand, the national greenhouse gas inventories (NGHGIs) used to assess compliance with national climate targets under the Paris Agreement and, on the other hand, the Global Carbon Budget and Intergovernmental Panel on Climate Change (IPCC) assessment reports, both based on global bookkeeping models (BMs).
Recent studies have shown that these differences are mainly due to inconsistent definitions of anthropogenic CO2 fluxes in managed forests. Countries assume larger areas of forest to be managed than BMs do, due to a broader definition of managed land in NGHGIs. Additionally, the fraction of the land sink caused by indirect effects of human-induced environmental change (e.g. fertilisation effect on vegetation growth due to increased atmospheric CO2 concentration) on managed lands is treated as non-anthropogenic by BMs but as anthropogenic in most NGHGIs.
We implement an approach that adds the CO2 sink caused by environmental change in countries' managed forests (estimated by 16 dynamic global vegetation models, DGVMs) to the land-use fluxes from three BMs. This sum is conceptually more comparable to NGHGIs and is thus expected to be quantitatively more similar. Our analysis uses updated and more comprehensive data from NGHGIs than previous studies and provides model results at a greater level of disaggregation in terms of regions, countries and land categories (i.e. forest land, deforestation, organic soils, other land uses).
Our results confirm a large difference (6.7 GtCO2 yr−1) in global land-use CO2 fluxes between the ensemble mean of the BMs, which estimate a source of 4.8 GtCO2 yr−1 for the period 2000–2020, and NGHGIs, which estimate a sink of −1.9 GtCO2 yr−1 in the same period. Most of the gap is found on forest land (3.5 GtCO2 yr−1), with differences also for deforestation (2.4 GtCO2 yr−1), for fluxes from other land uses (1.0 GtCO2 yr−1) and to a lesser extent for fluxes from organic soils (0.2 GtCO2 yr−1). By adding the DGVM ensemble mean sink arising from environmental change in managed forests (−6.4 GtCO2 yr−1) to BM estimates, the gap between BMs and NGHGIs becomes substantially smaller both globally (residual gap: 0.3 GtCO2 yr−1) and in most regions and countries. However, some discrepancies remain and deserve further investigation. For example, the BMs generally provide higher emissions from deforestation than NGHGIs and, when adjusted with the sink in managed forests estimated by DGVMs, yield a sink that is often greater than NGHGIs.
In summary, this study provides a blueprint for harmonising the estimations of anthropogenic land-use fluxes, allowing for detailed comparisons between global models and national inventories at global, regional and country levels. This is crucial to increase confidence in land-use emissions estimates, support investments in land-based mitigation strategies and assess the countries' collective progress under the Global Stocktake of the Paris Agreement.
Journal Article
Simulating Ips typographus L. outbreak dynamics and their influence on carbon balance estimates with ORCHIDEE r8627
2024
New (a)biotic conditions resulting from climate change are expected to change disturbance dynamics, such as windthrow, forest fires, droughts, and insect outbreaks, and their interactions. These unprecedented natural disturbance dynamics might alter the capability of forest ecosystems to buffer atmospheric CO2 increases, potentially leading forests to transform from sinks into sources of CO2. This study aims to enhance the ORCHIDEE land surface model to study the impacts of climate change on the dynamics of the bark beetle, Ips typographus, and subsequent effects on forest functioning. The Ips typographus outbreak model is inspired by previous work from Temperli et al. (2013) for the LandClim landscape model. The new implementation of this model in ORCHIDEE r8627 accounts for key differences between ORCHIDEE and LandClim: (1) the coarser spatial resolution of ORCHIDEE; (2) the higher temporal resolution of ORCHIDEE; and (3) the pre-existing process representation of windthrow, drought, and forest structure in ORCHIDEE. Simulation experiments demonstrated the capability of ORCHIDEE to simulate a variety of post-disturbance forest dynamics observed in empirical studies. Through an array of simulation experiments across various climatic conditions and windthrow intensities, the model was tested for its sensitivity to climate, initial disturbance, and selected parameter values. The results of these tests indicated that with a single set of parameters, ORCHIDEE outputs spanned the range of observed dynamics. Additional tests highlighted the substantial impact of incorporating Ips typographus outbreaks on carbon dynamics. Notably, the study revealed that modeling abrupt mortality events as opposed to a continuous mortality framework provides new insights into the short-term carbon sequestration potential of forests under disturbance regimes by showing that the continuous mortality framework tends to overestimate the carbon sink capacity of forests in the 20- to 50-year range in ecosystems under high disturbance pressure compared to scenarios with abrupt mortality events. This model enhancement underscores the critical need to include disturbance dynamics in land surface models to refine predictions of forest carbon dynamics in a changing climate.
Journal Article