| 1. |
- Acosta Navarro, Juan Camilo, 1983-
(författare)
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Anthropogenic influence on climate through changes in aerosol emissions from air pollution and land use change
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Particulate matter suspended in air (i.e. aerosol particles) exerts a substantial influence on the climate of our planet and is responsible for causing severe public health problems in many regions across the globe. Human activities have altered the natural and anthropogenic emissions of aerosol particles through direct emissions or indirectly by modifying natural sources. The climate effects of the latter have been largely overlooked. Humans have dramatically altered the land surface of the planet causing changes in natural aerosol emissions from vegetated areas. Regulation on anthropogenic and natural aerosol emissions have the potential to affect the climate on regional to global scales. Furthermore, the regional climate effects of aerosol particles could potentially be very different than the ones caused by other climate forcers (e.g. well mixed greenhouse gases). The main objective of this work was to investigate the climatic effects of land use and air pollution via aerosol changes.Using numerical model simulations it was found that land use changes in the past millennium have likely caused a positive radiative forcing via aerosol climate interactions. The forcing is an order of magnitude smaller and has an opposite sign than the radiative forcing caused by direct aerosol emissions changes from other human activities. The results also indicate that future reductions of fossil fuel aerosols via air quality regulations may lead to an additional warming of the planet by mid-21st century and could also cause an important Arctic amplification of the warming. In addition, the mean position of the intertropical convergence zone and the Asian monsoon appear to be sensitive to aerosol emission reductions from air quality regulations. For these reasons, climate mitigation policies should take into consideration aerosol air pollution, which has not received sufficient attention in the past.
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| 2. |
- Acosta Navarro, Juan C., et al.
(författare)
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Future response of temperature and precipitation to reduced aerosol emissions as compared with increased greenhouse gas concentrations
- 2017
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Ingår i: Journal of Climate. - 0894-8755 .- 1520-0442. ; 30:3, s. 939-954
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Tidskriftsartikel (refereegranskat)abstract
- Experiments with a climate model (NorESM1) were performed to isolate the effects of aerosol particles and greenhouse gases on surface temperature and precipitation in simulations of future climate. The simulations show that by 2025-2049, a reduction of aerosol emissions from fossil fuels following a maximum technically feasible reduction (MFR) scenario could lead to a global and Arctic warming of 0.26 K and 0.84 K, respectively; as compared with a simulation with fixed aerosol emissions at the level of 2005. If fossil fuel emissions of aerosols follow a current legislation emissions (CLE) scenario, the NorESM1 model simulations yield a non-significant change in global and Arctic average surface temperature as compared with aerosol emissions fixed at year 2005. The corresponding greenhouse gas effect following the RCP4.5 emission scenario leads to a global and Arctic warming of 0.35 K and 0.94 K, respectively.The model yields a marked annual average northward shift in the inter-tropical convergence zone with decreasing aerosol emissions and subsequent warming of the northern hemisphere. The shift is most pronounced in the MFR scenario but also visible in the CLE scenario. The modeled temperature response to a change in greenhouse gas concentrations is relatively symmetric between the hemispheres and there is no marked shift in the annual average position of the inter-tropical convergence zone. The strong reduction in aerosol emissions in MFR also leads to a net southward cross-hemispheric energy transport anomaly both in the atmosphere and ocean, and enhanced monsoon circulation in Southeast and East Asia causing an increase in precipitation over a large part of this region.
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| 3. |
- Acosta Navarro, Juan Camilo, et al.
(författare)
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Global emissions of terpenoid VOCs from terrestrial vegetation in the last millennium
- 2014
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Ingår i: Journal of Geophysical Research - Atmospheres. - : Wiley-Blackwell. - 2169-897X .- 2169-8996. ; 119:11, s. 6867-6885
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Tidskriftsartikel (refereegranskat)abstract
- We investigated the millennial variability (1000 A.D.-2000 A.D.) of global biogenic volatile organic compound (BVOC) emissions by using two independent numerical models: The Model of Emissions of Gases and Aerosols from Nature (MEGAN), for isoprene, monoterpene, and sesquiterpene, and Lund-Potsdam-Jena-General Ecosystem Simulator (LPJ-GUESS), for isoprene and monoterpenes. We found the millennial trends of global isoprene emissions to be mostly affected by land cover and atmospheric carbon dioxide changes, whereas monoterpene and sesquiterpene emission trends were dominated by temperature change. Isoprene emissions declined substantially in regions with large and rapid land cover change. In addition, isoprene emission sensitivity to drought proved to have significant short-term global effects. By the end of the past millennium MEGAN isoprene emissions were 634 TgC yr-1 (13% and 19% less than during 1750-1850 and 1000-1200, respectively), and LPJ-GUESS emissions were 323 TgC yr-1(15% and 20% less than during 1750-1850 and 1000-1200, respectively). Monoterpene emissions were 89 TgC yr-1(10% and 6% higher than during 1750-1850 and 1000-1200, respectively) in MEGAN, and 24 TgC yr-1 (2% higher and 5% less than during 1750-1850 and 1000-1200, respectively) in LPJ-GUESS. MEGAN sesquiterpene emissions were 36 TgC yr-1(10% and 4% higher than during 1750-1850 and 1000-1200, respectively). Although both models capture similar emission trends, the magnitude of the emissions are different. This highlights the importance of building better constraints on VOC emissions from terrestrial vegetation.
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| 4. |
- Acosta Navarro, Juan Camilo
(författare)
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Historical anthropogenic radiative forcing of changes in biogenic secondary organic aerosol
- 2015
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Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Human activities have lead to changes in the energy balance of the Earth and the global climate. Changes in atmospheric aerosols are the second largest contributor to climate change after greenhouse gases since 1750 A.D. Land-use practices and other environmental drivers have caused changes in the emission of biogenic volatile organic compounds (BVOCs) and secondary organic aerosol (SOA) well before 1750 A.D, possibly causing climate effects through aerosol-radiation and aerosol-cloud interactions. Two numerical emission models LPJ-GUESS and MEGAN were used to quantify the changes in aerosol forming BVOC emissions in the past millennium. A chemical transport model of the atmosphere (GEOS-Chem-TOMAS) was driven with those BVOC emissions to quantify the effects on radiation caused by millennial changes in SOA.The specific objectives of this licentiate thesis are: 1) to understand what drove the changes in aerosol-forming BVOC emissions (i.e. isoprene, monoterpenes and sesquiterpenes) and to quantify these changes; 2) to calculate for the first time the combined historical aerosol direct and aerosol-cloud albedo effects on radiation from changing BVOC emissions through SOA formation; 3) to investigate how important the biological climate feedback associated to BVOC emissions and SOA formation is from a global climate perspective.We find that global isoprene emissions decreased after 1800 A.D. by about 12% - 15%. This decrease was dominated by losses of natural vegetation, whereas monoterpene and sesquiterpene emissions increased by about 2% - 10%, driven mostly by rising surface air temperatures. From 1000 A.D. to 1800 A.D, isoprene, monoterpene and sesquiterpene emissions decline by 3% - 8% driven by both, natural vegetation losses, and the moderate global cooling between the medieval climate anomaly and the little ice age. The millennial reduction in BVOC emissions lead to a 0.5% to 2% reduction in climatically relevant aerosol particles (> 80 nm) and cause a direct radiative forcing between +0.02 W/m² and +0.07 W/m², and an indirect radiative forcing between -0.02 W/m² and +0.02 W/m². The suggested biological climate feedback seems to be too small to have observable consequences on the global climate in the recent past.
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| 5. |
- Ahlm, Lars, et al.
(författare)
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Particle number concentrations over Europe in 2030 : the role of emissions and new particle formation
- 2013
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Ingår i: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 13:20, s. 10271-10283
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Tidskriftsartikel (refereegranskat)abstract
- The aerosol particle number concentration is a key parameter when estimating impacts of aerosol particles on climate and human health. We use a three-dimensional chemical transport model with detailed microphysics, PMCAMx-UF, to simulate particle number concentrations over Europe in the year 2030, by applying emission scenarios for trace gases and primary aerosols. The scenarios are based on expected changes in anthropogenic emissions of sulfur dioxide, ammonia, nitrogen oxides, and primary aerosol particles with a diameter less than 2.5 mu m (PM2.5) focusing on a photochemically active period, and the implications for other seasons are discussed. For the baseline scenario, which represents a best estimate of the evolution of anthropogenic emissions in Europe, PMCAMx-UF predicts that the total particle number concentration (N-tot) will decrease by 30-70% between 2008 and 2030. The number concentration of particles larger than 100 nm (N-100), a proxy for cloud condensation nuclei (CCN) concentration, is predicted to decrease by 40-70% during the same period. The predicted decrease in N-tot is mainly a result of reduced new particle formation due to the expected reduction in SO2 emissions, whereas the predicted decrease in N-100 is a result of both decreasing condensational growth and reduced primary aerosol emissions. For larger emission reductions, PMCAMx-UF predicts reductions of 60-80% in both N-tot and N-100 over Europe. Sensitivity tests reveal that a reduction in SO2 emissions is far more efficient than any other emission reduction investigated, in reducing N-tot. For N-100, emission reductions of both SO2 and PM2.5 contribute significantly to the reduced concentration, even though SO2 plays the dominant role once more. The impact of SO2 for both new particle formation and growth over Europe may be expected to be somewhat higher during the simulated period with high photochemical activity than during times of the year with less incoming solar radiation. The predicted reductions in both N-tot and N-100 between 2008 and 2030 in this study will likely reduce both the aerosol direct and indirect effects, and limit the damaging effects of aerosol particles on human health in Europe
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| 6. |
- Almeida, Joao, et al.
(författare)
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Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
- 2013
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 502:7471, s. 359-
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Tidskriftsartikel (refereegranskat)abstract
- 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(4-16), 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.
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| 7. |
- Artaxo, Paulo, et al.
(författare)
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Tropical and Boreal Forest – Atmosphere Interactions : A Review
- 2022
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Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 74:1, s. 24-163
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Forskningsöversikt (refereegranskat)abstract
- This review presents how the boreal and the tropical forests affect the atmosphere, its chemical composition, its function, and further how that affects the climate and, in return, the ecosystems through feedback processes. Observations from key tower sites standing out due to their long-term comprehensive observations: The Amazon Tall Tower Observatory in Central Amazonia, the Zotino Tall Tower Observatory in Siberia, and the Station to Measure Ecosystem-Atmosphere Relations at Hyytiäla in Finland. The review is complemented by short-term observations from networks and large experiments.The review discusses atmospheric chemistry observations, aerosol formation and processing, physiochemical aerosol, and cloud condensation nuclei properties and finds surprising similarities and important differences in the two ecosystems. The aerosol concentrations and chemistry are similar, particularly concerning the main chemical components, both dominated by an organic fraction, while the boreal ecosystem has generally higher concentrations of inorganics, due to higher influence of long-range transported air pollution. The emissions of biogenic volatile organic compounds are dominated by isoprene and monoterpene in the tropical and boreal regions, respectively, being the main precursors of the organic aerosol fraction.Observations and modeling studies show that climate change and deforestation affect the ecosystems such that the carbon and hydrological cycles in Amazonia are changing to carbon neutrality and affect precipitation downwind. In Africa, the tropical forests are so far maintaining their carbon sink.It is urgent to better understand the interaction between these major ecosystems, the atmosphere, and climate, which calls for more observation sites, providing long-term data on water, carbon, and other biogeochemical cycles. This is essential in finding a sustainable balance between forest preservation and reforestation versus a potential increase in food production and biofuels, which are critical in maintaining ecosystem services and global climate stability. Reducing global warming and deforestation is vital for tropical forests.
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| 8. |
- Bannan, Thomas J., et al.
(författare)
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Measured Saturation Vapor Pressures of Phenolic and Nitro-aromatic Compounds
- 2017
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 51:7, s. 3922-3928
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Tidskriftsartikel (refereegranskat)abstract
- Phenolic and nitro-aromatic compounds are extremely toxic components of atmospheric aerosol that are currently not well understood. In this Article, solid and subcooled-liquid-state saturation vapor pressures of phenolic and nitro-aromatic compounds are measured using Knudsen Effusion Mass Spectrometry (KEMS) over a range of temperatures (298-318 K). Vapor pressure estimation methods, assessed in this study, do not replicate the observed dependency on the relative positions of functional groups. With a few exceptions, the estimates are biased toward predicting saturation vapor pressures that are too high, by 5-6 orders of magnitude in some cases. Basic partitioning theory comparisons indicate that overestimation of vapor pressures in such cases would cause us to expect these compounds to be present in the gas state, whereas measurements in this study suggest these phenolic and nitro-aromatic will partition into the condensed state for a wide range of ambient conditions if absorptive partitioning plays a dominant role. While these techniques might have both structural and parametric uncertainties, the new data presented here should support studies trying to ascertain the role of nitrogen containing organics on aerosol growth and human health impacts.
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| 9. |
- Baranizadeh, Elham, et al.
(författare)
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Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe
- 2016
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Ingår i: Geoscientific Model Development. - : Copernicus GmbH. - 1991-959X .- 1991-9603. ; 9:8, s. 2741-2754
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Tidskriftsartikel (refereegranskat)abstract
- The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4-NH3-H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions-Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.
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| 10. |
- Bardakov, Roman, et al.
(författare)
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A Novel Framework to Study Trace Gas Transport in Deep Convective Clouds
- 2020
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Ingår i: Journal of Advances in Modeling Earth Systems. - 1942-2466. ; 12:5
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Tidskriftsartikel (refereegranskat)abstract
- Deep convective clouds reach the upper troposphere (8-15 km height). In addition to moisture and aerosol particles, they can bring aerosol precursor gases and other reactive trace gases from the planetary boundary layer to the cloud top. In this paper, we present a method to estimate trace gas transport based on the analysis of individual air parcel trajectories. Large eddy simulation of an idealized deep convective cloud was used to provide realistic environmental input to a parcel model. For a buoyant parcel, we found that the trace gas transport approximately follows one out of three scenarios, determined by a combination of the equilibrium vapor pressure (containing information about water-solubility and pure component saturation vapor pressure) and the enthalpy of vaporization. In one extreme, the trace gas will eventually be completely removed by precipitation. In the other extreme, there is almost no vapor condensation on hydrometeors and most of the gas is transported to the top of the cloud. The scenario in between these two extremes is also characterized by strong gas condensation, but a small fraction of the trace gas may still be transported aloft. This approach confirms previously suggested patterns of inert trace gas behavior in deep convective clouds, agrees with observational data, and allows estimating transport in analytically simple and computationally efficient way compared to explicit cloud-resolving model calculations.
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