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1.
Proc Natl Acad Sci U S A ; 121(5): e2315492121, 2024 Jan 30.
Artículo en Inglés | MEDLINE | ID: mdl-38252841

RESUMEN

The Earth's radiative cooling is a key driver of climate. Determining how it is affected by greenhouse gas concentration is a core question in climate-change sciences. Due to the complexity of radiative transfer processes, current practices to estimate this cooling require the development and use of a suite of radiative transfer models whose accuracy diminishes as we move from local, instantaneous estimates to global estimates over the whole globe and over long periods of time (decades). Here, we show that recent advances in nonlinear Monte Carlo methods allow a paradigm shift: a completely unbiased estimate of the Earth's infrared cooling to space can be produced using a single model, integrating the most refined spectroscopic models of molecular gas energy transitions over a global scale and over years, all at a very low computational cost (a few seconds).

2.
Proc Natl Acad Sci U S A ; 119(46): e2210481119, 2022 Nov 16.
Artículo en Inglés | MEDLINE | ID: mdl-36343255

RESUMEN

How clouds respond to anthropogenic sulfate aerosols is one of the largest sources of uncertainty in the radiative forcing of climate over the industrial era. This uncertainty limits our ability to predict equilibrium climate sensitivity (ECS)-the equilibrium global warming following a doubling of atmospheric CO2. Here, we use satellite observations to quantify relationships between sulfate aerosols and low-level clouds while carefully controlling for meteorology. We then combine the relationships with estimates of the change in sulfate concentration since about 1850 to constrain the associated radiative forcing. We estimate that the cloud-mediated radiative forcing from anthropogenic sulfate aerosols is [Formula: see text] W m-2 over the global ocean (95% confidence). This constraint implies that ECS is likely between 2.9 and 4.5 K (66% confidence). Our results indicate that aerosol forcing is less uncertain and ECS is probably larger than the ranges proposed by recent climate assessments.


Asunto(s)
Clima , Meteorología , Aerosoles , Sulfatos , Océanos y Mares
3.
Proc Natl Acad Sci U S A ; 119(22): e2123536119, 2022 05 31.
Artículo en Inglés | MEDLINE | ID: mdl-35605122

RESUMEN

The ongoing and projected impacts from human-induced climate change highlight the need for mitigation approaches to limit warming in both the near term (<2050) and the long term (>2050). We clarify the role of non-CO2 greenhouse gases and aerosols in the context of near-term and long-term climate mitigation, as well as the net effect of decarbonization strategies targeting fossil fuel (FF) phaseout by 2050. Relying on Intergovernmental Panel on Climate Change radiative forcing, we show that the net historical (2019 to 1750) radiative forcing effect of CO2 and non-CO2 climate forcers emitted by FF sources plus the CO2 emitted by land-use changes is comparable to the net from non-CO2 climate forcers emitted by non-FF sources. We find that mitigation measures that target only decarbonization are essential for strong long-term cooling but can result in weak near-term warming (due to unmasking the cooling effect of coemitted aerosols) and lead to temperatures exceeding 2 °C before 2050. In contrast, pairing decarbonization with additional mitigation measures targeting short-lived climate pollutants and N2O, slows the rate of warming a decade or two earlier than decarbonization alone and avoids the 2 °C threshold altogether. These non-CO2 targeted measures when combined with decarbonization can provide net cooling by 2030 and reduce the rate of warming from 2030 to 2050 by about 50%, roughly half of which comes from methane, significantly larger than decarbonization alone over this time frame. Our analysis demonstrates the need for a comprehensive CO2 and targeted non-CO2 mitigation approach to address both the near-term and long-term impacts of climate disruption.


Asunto(s)
Calentamiento Global , Gases de Efecto Invernadero , Dióxido de Carbono/análisis , Clima , Combustibles Fósiles , Calentamiento Global/prevención & control
4.
Glob Chang Biol ; 30(7): e17388, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-38967139

RESUMEN

Permafrost thaw in northern peatlands causes collapse of permafrost peat plateaus and thermokarst bog development, with potential impacts on atmospheric greenhouse gas exchange. Here, we measured methane and carbon dioxide fluxes over 3 years (including winters) using static chambers along two permafrost thaw transects in northwestern Canada, spanning young (~30 years since thaw), intermediate and mature thermokarst bogs (~200 years since thaw). Young bogs were wetter, warmer and had more hydrophilic vegetation than mature bogs. Methane emissions increased with wetness and soil temperature (40 cm depth) and modelled annual estimates were greatest in the young bog during the warmest year and lowest in the mature bog during the coolest year (21 and 7 g C-CH4 m-2 year-1, respectively). The dominant control on net ecosystem exchange (NEE) in the mature bog (between +20 and -54 g C-CO2 m-2 year-1) was soil temperature (5 cm), causing net CO2 loss due to higher ecosystem respiration (ER) in warmer years. In contrast, wetness controlled NEE in the young and intermediate bogs (between +55 and -95 g C-CO2 m-2 year-1), where years with periodic inundation at the beginning of the growing season caused greater reduction in gross primary productivity than in ER leading to CO2 loss. Winter fluxes (November-April) represented 16% of annual ER and 38% of annual CH4 emissions. Our study found NEE of thermokarst bogs to be close to neutral and rules out large CO2 losses under current conditions. However, high CH4 emissions after thaw caused a positive net radiative forcing effect. While wet conditions favouring high CH4 emissions only persist for the initial young bog period, we showed that continued climate warming with increased ER, and thus, CO2 losses from the mature bog can cause net positive radiative forcing which would last for centuries after permafrost thaw.


Asunto(s)
Dióxido de Carbono , Cambio Climático , Gases de Efecto Invernadero , Metano , Hielos Perennes , Humedales , Metano/análisis , Metano/metabolismo , Dióxido de Carbono/análisis , Gases de Efecto Invernadero/análisis , Temperatura , Suelo/química , Canadá , Estaciones del Año
5.
Environ Res ; : 119629, 2024 Jul 16.
Artículo en Inglés | MEDLINE | ID: mdl-39025349

RESUMEN

From the beginning of May 2023 to the end of August 2023, the Northern Hemisphere experienced significant wildfire activity with the most widespread fires occurring in Canada. Forest fires in Canada destroyed more than 15.6 million hectares of forests. These wildfires worsened air quality across the region and other parts of the world. The smoke reached southern Europe by the end of June 2023. To better understand the consequences of such forest fires far from the site of origin, aerosol optical, microphysical and radiative properties were analyzed during this event for southern Europe using data from the Visible Infrared Imaging Radiometer Suite (VIIRS), TROPOspheric Monitoring Instrument (TROPOMI), and Aerosol Robotic Network (AERONET). TROPOMI aerosol index (AI) and the carbon monoxide (CO) product confirm that the smoke originated directly from these forest fires. AERONET data from the El Arenosillo site in southern Spain showed maximum aerosol optical depth (AOD) values on June 27 reached 2.36. Data on Angstrom Exponent (AE), aerosol volume size distribution (VSD), single scattering albedo (SSA), fine mode fraction (FMF), volume particle concentration, effective radius (REff), absorption AOD (AAOD), extinction AE (EAE) and absorption AE (AAE) showed that fine-mode particles with carbonaceous aerosols contribution predominated in the atmosphere above the El Arenosillo site. Direct aerosol radiative forcing (DARF) at the top (DARFTOA) and bottom of atmosphere (DARFBOA) were -103.1 and -198.93 Wm-2, respectively. The atmospheric aerosol radiative forcing (DARFATM) was found to be 95.83 Wm-2 and with a heating rate 2.69 K day-1, which indicates the resulting warming of the atmosphere.

6.
Proc Natl Acad Sci U S A ; 118(15)2021 04 13.
Artículo en Inglés | MEDLINE | ID: mdl-33876752

RESUMEN

Knowing the historical relative contribution of greenhouse gases (GHGs) and short-lived climate forcers (SLCFs) to global radiative forcing (RF) at the regional level can help understand how future GHGs emission reductions and associated or independent reductions in SLCFs will affect the ultimate purpose of the Paris Agreement. In this study, we use a compact Earth system model to quantify the global RF and attribute global RF to individual countries and regions. As our evaluation, the United States, the first 15 European Union members, and China are the top three contributors, accounting for 21.9 ± 3.1%, 13.7 ± 1.6%, and 8.6 ± 7.0% of global RF in 2014, respectively. We also find a contrast between developed countries where GHGs dominate the RF and developing countries where SLCFs including aerosols and ozone are more dominant. In developing countries, negative RF caused by aerosols largely masks the positive RF from GHGs. As developing countries take measures to improve the air quality, their negative contributions from aerosols will likely be reduced in the future, which will in turn enhance global warming. This underlines the importance of reducing GHG emissions in parallel to avoid any detrimental consequences from air quality policies.

7.
Environ Sci Technol ; 57(6): 2506-2515, 2023 02 14.
Artículo en Inglés | MEDLINE | ID: mdl-36734358

RESUMEN

Fuel combustion provides basic energy for the society but also produces CO2 and incomplete combustion products that threaten human survival, climate change, and global sustainability. A variety of fuels burned in different facilities expectedly have distinct impacts on climate, which remains to be quantitatively assessed. This study uses updated emission inventories and an earth system model to evaluate absolute and relative contributions in combustion emission-associated climate forcing by fuels, sectors, and regions. We showed that, from 1970 to 2014, coal burned in the energy sector and oil used in the transportation sector contributed comparable energies consumed (24 and 20% of the total) but had distinct climate forcing (1 and 40%, respectively). Globally, coal burned for energy production had negative impacts on climate forcing but positive effects in the residential sector. In many developing countries, coal combustion in the energy sector had negative radiative forcing (RF) per unit energy consumed due to insufficient controls on sulfur and scattering aerosol levels, but oils in the transportation sector had high positive RF values. These results had important implications on the energy transition and emission reduction actions in response to climate change. Distinct climate efficiencies of energies and the spatial heterogeneity implied differentiated energy utilization strategies and pollution control policies by region and sector.


Asunto(s)
Contaminación del Aire , Carbón Mineral , Humanos , Carbón Mineral/análisis , Fenómenos Físicos
8.
Environ Sci Technol ; 57(23): 8691-8700, 2023 06 13.
Artículo en Inglés | MEDLINE | ID: mdl-37259829

RESUMEN

Black carbon (BC) plays a vital role in Arctic warming. Extensive investigations have been conducted to elucidate the source-receptor relationships of BC between the Arctic and mid-/high-latitude sources. However, it is unclear to what extent source relocation under globalization could disturb Arctic BC contamination and climate forcing from anthropogenic BC emissions. Here, we show that the global supply chain (GSC) relocation featured by the southward shift of industries from high-latitude developed countries to low-latitude developing countries markedly reduces the BC burden in the Arctic using a global chemical transport model (GEOS-Chem) and a multiregional input-output analysis (MRIO). We find that Arctic annual mean BC concentration associated with the GSC relocation drops by ∼15% from the case without the GSC relocation. The total net BC level declines 7% over the entire Arctic and 16% in the European Arctic. We also observed markedly declining BC deposition as well as direct and snow albedo radiative forcing in the Arctic. We show that the Arctic BC burden would be further reduced by decreasing BC emissions in China, attributable to its emission reduction and ongoing shift of the GSC from China to southern and southeastern Asia.


Asunto(s)
Clima , Modelos Químicos , China , Hollín/análisis , Carbono
9.
Environ Sci Technol ; 57(44): 16834-16842, 2023 11 07.
Artículo en Inglés | MEDLINE | ID: mdl-37856673

RESUMEN

Tar balls are brown carbonaceous particles that are highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are also believed to have a significant impact on the Earth's radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we used two nighttime samples to investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory "Ottavio Vittori" on Mt. Cimone, Italy, using multimodal microspectroscopy. In our two samples, tar balls contributed 50% of carbonaceous particles by number. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index (RI) for a wavelength range from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average RI of inhomogeneously and homogeneously mixed tar balls (1.40-0.03i and 1.36-0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 W m-2 (on a clear sky day) to 9.5 W m-2 (when clouds are below the aerosol layer). Understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.


Asunto(s)
Contaminantes Atmosféricos , Clima , Atmósfera/química , Aerosoles/análisis , Italia , Contaminantes Atmosféricos/análisis
10.
Environ Res ; 238(Pt 1): 117105, 2023 12 01.
Artículo en Inglés | MEDLINE | ID: mdl-37689338

RESUMEN

We analyse the long-term (1980-2020) changes in aerosols over the Third Pole (TP) and assess the changes in radiative forcing (RF) using satellite, ground-based and reanalysis data. The annual mean aerosol optical depth (AOD) varies from 0.06 to 0.24, with the highest values of around 0.2 in the north and southwest TP, which are dominated by dust from Taklimakan and Thar deserts, respectively. However, Organic Carbon (OC), Black Carbon (BC) and sulphate aerosols have significant contributions to the total AOD in the south and east TP. High amounts of dust are observed in spring and summer, but BC in winter. Trajectory analysis reveals that the air mass originated from East and South Asia carries BC and OC, whereas the air from South Asia, Central Asia and Middle East brings dust to TP. Significant positive trends in AOD is found in TP, with high values of about 0.002/yr in the eastern and southern TP. There is a gradual increase in BC and OC concentrations during 1980-2020, but the change from 2000 is phenomenal. The RF at the top of the atmosphere varies from -10 to 2 W/m2 in TP, and high positive RF of about 2 W/m2 is estimated in Pamir, Karakoram and Nyainquentanglha mountains, where the massive glacier mass exists. The RF has increased in much of TP during recent decades (2001-2020) with respect to previous decades (1981-2000), which can be due to the rise in BC and dust during the latter period. Therefore, the positive trend in BC and its associated change in RF can amplify the regional warming, and thus, the melting of glaciers or ice in TP. This is a great concern as it is directly connected to the water security of many South Asian countries.


Asunto(s)
Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Cambio Climático , Polvo/análisis , Estaciones del Año , Aerosoles/análisis , Carbono/análisis , Monitoreo del Ambiente/métodos
11.
Proc Natl Acad Sci U S A ; 117(30): 17591-17598, 2020 07 28.
Artículo en Inglés | MEDLINE | ID: mdl-32661149

RESUMEN

Anthropogenic aerosols are hypothesized to enhance planetary albedo and offset some of the warming due to the buildup of greenhouse gases in Earth's atmosphere. Aerosols can enhance the coverage, reflectance, and lifetime of warm low-level clouds. However, the relationship between cloud lifetime and aerosol concentration has been challenging to measure from polar orbiting satellites. We estimate two timescales relating to the formation and persistence of low-level clouds over [Formula: see text] spatial domains using multiple years of geostationary satellite observations provided by the Clouds and Earth's Radiant Energy System (CERES) Synoptic (SYN) product. Lagrangian trajectories spanning several days along the classic stratus-to-cumulus transition zone are stratified by aerosol optical depth and meteorology. Clouds forming in relatively polluted trajectories tend to have lighter precipitation rates, longer average lifetime, and higher cloud albedo and cloud fraction compared with unpolluted trajectories. While liquid water path differences are found to be negligible, we find direct evidence of increased planetary albedo primarily through increased drop concentration ([Formula: see text]) and cloud fraction, with the caveat that the aerosol influence on cloud fraction is positive only for stable atmospheric conditions. While the increase in cloud fraction can be large typically in the beginning of trajectories, the Twomey effect accounts for the bulk (roughly 3/4) of the total aerosol indirect radiative forcing estimate.

12.
Proc Natl Acad Sci U S A ; 117(10): 5196-5203, 2020 03 10.
Artículo en Inglés | MEDLINE | ID: mdl-32098848

RESUMEN

Black carbon (BC) absorbs solar radiation, leading to a strong but uncertain warming effect on climate. A key challenge in modeling and quantifying BC's radiative effect on climate is predicting enhancements in light absorption that result from internal mixing between BC and other aerosol components. Modeling and laboratory studies show that BC, when mixed with other aerosol components, absorbs more strongly than pure, uncoated BC; however, some ambient observations suggest more variable and weaker absorption enhancement. We show that the lower-than-expected enhancements in ambient measurements result from a combination of two factors. First, the often used spherical, concentric core-shell approximation generally overestimates the absorption by BC. Second, and more importantly, inadequate consideration of heterogeneity in particle-to-particle composition engenders substantial overestimation in absorption by the total particle population, with greater heterogeneity associated with larger model-measurement differences. We show that accounting for these two effects-variability in per-particle composition and deviations from the core-shell approximation-reconciles absorption enhancement predictions with laboratory and field observations and resolves the apparent discrepancy. Furthermore, our consistent model framework provides a path forward for improving predictions of BC's radiative effect on climate.

13.
Proc Natl Acad Sci U S A ; 117(32): 18998-19006, 2020 08 11.
Artículo en Inglés | MEDLINE | ID: mdl-32719114

RESUMEN

The change in planetary albedo due to aerosol-cloud interactions during the industrial era is the leading source of uncertainty in inferring Earth's climate sensitivity to increased greenhouse gases from the historical record. The variable that controls aerosol-cloud interactions in warm clouds is droplet number concentration. Global climate models demonstrate that the present-day hemispheric contrast in cloud droplet number concentration between the pristine Southern Hemisphere and the polluted Northern Hemisphere oceans can be used as a proxy for anthropogenically driven change in cloud droplet number concentration. Remotely sensed estimates constrain this change in droplet number concentration to be between 8 cm-3 and 24 cm-3 By extension, the radiative forcing since 1850 from aerosol-cloud interactions is constrained to be -1.2 W⋅m-2 to -0.6 W⋅m-2 The robustness of this constraint depends upon the assumption that pristine Southern Ocean droplet number concentration is a suitable proxy for preindustrial concentrations. Droplet number concentrations calculated from satellite data over the Southern Ocean are high in austral summer. Near Antarctica, they reach values typical of Northern Hemisphere polluted outflows. These concentrations are found to agree with several in situ datasets. In contrast, climate models show systematic underpredictions of cloud droplet number concentration across the Southern Ocean. Near Antarctica, where precipitation sinks of aerosol are small, the underestimation by climate models is particularly large. This motivates the need for detailed process studies of aerosol production and aerosol-cloud interactions in pristine environments. The hemispheric difference in satellite estimated cloud droplet number concentration implies preindustrial aerosol concentrations were higher than estimated by most models.

14.
Environ Monit Assess ; 195(2): 256, 2023 Jan 03.
Artículo en Inglés | MEDLINE | ID: mdl-36595082

RESUMEN

The present investigation outlines the crucial factors that influence the black carbon (BC) concentrations over a polluted metropolis, Kolkata (22.57° N, 88.37° E), India. Located in the eastern part of the Indo Gangetic Plain (IGP) outflow region and close to the land-ocean boundary, Kolkata is subject to contrasting seasonal maritime airflow from the Bay of Bengal and continental air mass from the IGP and Tibetan plateau region, which modulates the local concentration of BC. The origin of aerosol transport and associated atmospheric dynamics with high and low BC activities over Kolkata are examined during 2012-2015 using data from multi-technique sources which include measurements of ground-based instruments of aethalometer and multi-frequency microwave radiometer, reanalysis data from ERA-5 and MEERA-2, and model outputs from HYPSLIT back trajectory model simulations. The study highlights the control of IGP wind inflow on the occurrence of anomalous enhancements in BC concentration during weekends and holidays when local emissions are low. High BC events are associated with enhanced atmospheric heating below the boundary layer (2000 m) and significant negative surface radiative forcing. The response of the boundary layer to high and low BC episodes, shown in the diurnal variation in comparison with the seasonal mean, is investigated. Dominant suppression of morning and night-time boundary layer height is observed on high BC days. During the daytime in pre-monsoon, post-monsoon, and winter seasons, boundary layer height peaks are found to be strongly controlled by high BC episode occurrences as obtained from the hourly data of ERA-5.


Asunto(s)
Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente/métodos , Estaciones del Año , Viento , Hollín/análisis , Aerosoles/análisis , India , Carbono/análisis
15.
Glob Chang Biol ; 28(21): 6349-6365, 2022 11.
Artículo en Inglés | MEDLINE | ID: mdl-35904068

RESUMEN

Peatland rewetting has been proposed as a vital climate change mitigation tool to reduce greenhouse gas emissions and to generate suitable conditions for the return of carbon (C) sequestration. In this study, we present annual C balances for a 5-year period at a rewetted peatland in Ireland (rewetted at the start of the study) and compare the results with an adjacent drained area (represents business-as-usual). Hydrological modelling of the 230-hectare site was carried out to determine the likely ecotopes (vegetation communities) that will develop post-rewetting and was used to inform a radiative forcing modelling exercise to determine the climate impacts of rewetting this peatland under five high-priority scenarios (SSP1-1.9, SS1-2.6, SSP2-4.5, SSP3-7.0 and SSP5-8.5). The drained area (marginal ecotope) was a net C source throughout the study and emitted 157 ± 25.5 g C m-2  year-1 . In contrast, the rewetted area (sub-central ecotope) was a net C sink of 78.0 ± 37.6 g C m-2  year-1 , despite relatively large annual methane emissions post-rewetting (average 19.3 ± 5.2 g C m-2  year-1 ). Hydrological modelling predicted the development of three key ecotopes at the site, with the sub-central ecotope predicted to cover 24% of the site, the sub-marginal predicted to cover 59% and the marginal predicted to cover 16%. Using these areal estimates, our radiative forcing modelling projects that under the SSP1-1.9 scenario, the site will have a warming effect on the climate until 2085 but will then have a strong cooling impact. In contrast, our modelling exercise shows that the site will never have a cooling impact under the SSP5-8.5 scenario. Our results confirm the importance of rapid rewetting of drained peatland sites to (a) achieve strong C emissions reductions, (b) establish optimal conditions for C sequestration and (c) set the site on a climate cooling trajectory.


Asunto(s)
Carbono , Gases de Efecto Invernadero , Dióxido de Carbono/análisis , Irlanda , Metano/análisis , Suelo , Humedales
16.
Glob Chang Biol ; 28(13): 4069-4084, 2022 07.
Artículo en Inglés | MEDLINE | ID: mdl-35377520

RESUMEN

Reconstructions of past climate impact, that is, radiative forcing (RF), of peatland carbon (C) dynamics show that immediately after peatland initiation the climate warming effect of CH4 emissions exceeds the cooling effect of CO2 uptake, but thereafter the net effect of most peatlands will move toward cooling, when RF switches from positive to negative. Reconstructing peatland C dynamics necessarily involves uncertainties related to basic assumptions on past CO2  flux, CH4 emission and peatland expansion. We investigated the effect of these uncertainties on the RF of three peatlands, using either apparent C accumulation rates, net C balance (NCB) or NCB plus C loss during fires as basis for CO2 uptake estimate; applying a plausible range for CH4 emission; and assuming linearly interpolated expansion between basal dates or comparatively early or late expansion. When we factored that some C would only be stored temporarily (NCB and NCB+fire), the estimated past cooling effect of CO2 uptake increased, but the present-day RF was affected little. Altering the assumptions behind the reconstructed CO2  flux or expansion patterns caused the RF to peak earlier and advanced the switch from positive to negative RF by several thousand years. Compared with NCB, including fires had only small additional effect on RF lasting less than 1000 year. The largest uncertainty in reconstructing peatland RF was associated with CH4 emissions. As shown by the consistently positive RF modelled for one site, and in some cases for the other two, peatlands with high CH4 emissions and low C accumulation rates may have remained climate warming agents since their initiation. Although uncertainties in present-day RF were mainly due to the assumed CH4 emission rates, the uncertainty in lateral expansion still had a significant effect on the present-day RF, highlighting the importance to consider uncertainties in the past peatland C balance in RF reconstructions.


Asunto(s)
Dióxido de Carbono , Metano , Carbono , Dióxido de Carbono/análisis , Suelo , Incertidumbre
17.
Environ Sci Technol ; 56(12): 8610-8618, 2022 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-35652563

RESUMEN

The climate models of the Intergovernmental Panel on Climate Change list black carbon (BC) as an important contributor to global warming based on its radiative forcing (RF) impact. Examining closely these models, it becomes apparent that they might underpredict significantly the direct RF for BC, largely due to their assumed spherical BC morphology. Specifically, the light absorption and direct RF of BC agglomerates are enhanced by light scattering between their constituent primary particles as determined by the Rayleigh-Debye-Gans theory interfaced with discrete dipole approximation and recent relations for the refractive index and lensing effect. The light absorption of BC is enhanced by about 20% by the multiple light scattering between BC primary particles regardless of the compactness of their agglomerates. The resulting light absorption agrees very well with the observed absorption aerosol optical depth of BC. ECHAM-HAM simulations accounting for the realistic BC morphology and its coatings reveal high direct RF = 3-5 W/m2 in East, South Asia, sub-Sahara, western Africa, and the Arabian peninsula. These results are in agreement with satellite and AERONET observations of RF and indicate a regional climate warming contribution by 0.75-1.25 °C, solely due to BC emissions.

18.
Environ Sci Technol ; 56(3): 1586-1593, 2022 02 01.
Artículo en Inglés | MEDLINE | ID: mdl-35038862

RESUMEN

Atmospheric black carbon (BC) has a large yet highly uncertain contribution to global warming. When mixed with non-BC/coating material during atmospheric aging, the BC light absorption can be enhanced through the lensing effect. Laboratory and modeling studies have consistently found strong BC absorption enhancement, while the results in ambient measurements are conflicting, with some reporting weak absorption enhancement even for particles with large bulk coating amounts. Here, from our direct field observations, we report both large and minor absorption enhancement factors for different BC-containing particle populations with large bulk non-BC-to-BC mass ratios. By gaining insights into the measured coating material distribution across each particle population, we find that the level of absorption enhancement is strongly dependent on the particle-resolved mixing state. Our study shows that the greater mixing-state heterogeneity results in the larger difference between observed and predicted absorption enhancement. We demonstrate that by considering the variability in coating material thickness in the optical model, the previously observed model measurement discrepancy of absorption enhancement can be reconciled. The observations and improved optical models reported here highlight the importance of mixing-state heterogeneity on BC's radiative forcing, which should be better resolved in large-scale models to increase confidence when estimating the aerosol radiation effect.


Asunto(s)
Carbono , Hollín , Aerosoles/análisis , Calentamiento Global
19.
Environ Sci Technol ; 56(2): 761-769, 2022 01 18.
Artículo en Inglés | MEDLINE | ID: mdl-34941248

RESUMEN

With urbanization worldwide in recent decades, anthropogenic dust (AD) emissions due to heavy urban construction and off-road vehicle use have been increasing. Its perturbations on urban air pollution at the global scale are still unclear. Based on observations, we found that a high urban AD optical depth is often accompanied by severe non-dust aerosol optical depth in the planetary boundary layer (PBL), both magnitudes even comparable. To investigate the causes, an AD emission inventory constrained by satellite retrievals is implemented in a global climate model. The results show that AD-induced surface radiative cooling of up to -15.9 ± 4.0 W m-2 regionally leads to reduced PBL height, which deteriorates non-dust pollution, especially over India and northern China, in addition to the tremendous direct AD contribution to pollutants. The estimated global total premature mortality due to AD is 0.8 million deaths per year and is more severe in populous regions.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , Polvo/análisis , Monitoreo del Ambiente/métodos
20.
Geophys Res Lett ; 49(11): e2022GL098102, 2022 Jun 16.
Artículo en Inglés | MEDLINE | ID: mdl-35859851

RESUMEN

This study employs a fully coupled meteorology-chemistry-snow model to investigate the impacts of light-absorbing particles (LAPs) on snow darkening in the Sierra Nevada. After comprehensive evaluation with spatially and temporally complete satellite retrievals, the model shows that LAPs in snow reduce snow albedo by 0.013 (0-0.045) in the Sierra Nevada during the ablation season (April-July), producing a midday mean radiative forcing of 4.5 W m-2 which increases to 15-22 W m-2 in July. LAPs in snow accelerate snow aging processes and reduce snow cover fraction, which doubles the albedo change and radiative forcing caused by LAPs. The impurity-induced snow darkening effects decrease snow water equivalent and snow depth by 20 and 70 mm in June in the Sierra Nevada bighorn sheep habitat. The earlier snowmelt reduces root-zone soil water content by 20%, deteriorating the forage productivity and playing a negative role in the survival of bighorn sheep.

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