New approaches to quantifying aerosol influence on the cloud radiative effect.
Ontology highlight
ABSTRACT: The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical properties, cloud condensation, and ice nucleation potential, along with the global distribution of these properties, controlled by emissions, transport, transformation, and sinks. Equally daunting is that clouds themselves are complex, turbulent, microphysical entities and, by their very nature, ephemeral and hard to predict. Atmospheric general circulation models represent aerosol-cloud interactions at ever-increasing levels of detail, but these models lack the resolution to represent clouds and aerosol-cloud interactions adequately. There is a dearth of observational constraints on aerosol-cloud interactions. We develop a conceptual approach to systematically constrain the aerosol-cloud radiative effect in shallow clouds through a combination of routine process modeling and satellite and surface-based shortwave radiation measurements. We heed the call to merge Darwinian and Newtonian strategies by balancing microphysical detail with scaling and emergent properties of the aerosol-cloud radiation system.
Project description:This study examines the atmospheric properties of weather states (WSs) derived from the International Satellite Cloud Climatology Project over the Western North Atlantic Ocean. In particular, radiation and aerosol data corresponding to two sites in the study domain, Pennsylvania State University and Bermuda, were examined to characterize the atmospheric properties of the various satellite-derived WSs. At both sites, the fair weather WS was most prevalent, followed by the cirrus WS. Differences in the seasonality of the various WSs were observed at the two sites. Fractional sky cover and effective shortwave cloud transmissivity derived from ground-based radiation measurements were able to capture differences among the satellite-derived WSs. Speciated aerosol optical thicknesses (AOT) from the Modern-Era Retrospective Analysis for Research and Applications, version 2 were used to investigate potential differences in aerosol properties among the WSs. The clear sky WS exhibited below-average seasonal values of AOT at both sites year-round, as well as relatively high rates of occurrence with low AOT events. In addition, the clear sky WS showed above-average contributions from dust and black carbon to the total AOT year-round. Finally, transitions between various WSs were examined under low, high, and midrange AOT conditions. The most common pathway was for the WSs to remain in the same state after a 3 h interval. Some WSs, such as mid latitude storms, deep convection, middle top, and shallow cumulus, were more prevalent as ending states under high AOT conditions. This work motivates examining differences in aerosol properties between WSs in other regions.
Project description: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.
Project description:There is a lack of satellite-based aerosol retrievals in the vicinity of low-topped clouds, mainly because reflectance from aerosols is overwhelmed by three-dimensional cloud radiative effects. To account for cloud radiative effects on reflectance observations, we develop a Convolutional Neural Network and retrieve aerosol optical depth (AOD) with 100-500 m horizontal resolution for all cloud-free regions regardless of their distances to clouds. The retrieval uncertainty is 0.01 + 5%AOD, and the mean bias is approximately -2%. In an application to satellite observations, aerosol hygroscopic growth due to humidification near clouds enhances AOD by 100% in regions within 1 km of cloud edges. The humidification effect leads to an overall 55% increase in the clear-sky aerosol direct radiative effect. Although this increase is based on a case study, it highlights the importance of aerosol retrievals in near-cloud regions, and the need to incorporate the humidification effect in radiative forcing estimates.
Project description:Satellite-based estimates of radiative forcing by aerosol-cloud interactions (RFaci) are consistently smaller than those from global models, hampering accurate projections of future climate change. Here we show that the discrepancy can be substantially reduced by correcting sampling biases induced by inherent limitations of satellite measurements, which tend to artificially discard the clouds with high cloud fraction. Those missed clouds exert a stronger cooling effect, and are more sensitive to aerosol perturbations. By accounting for the sampling biases, the magnitude of RFaci (from -0.38 to -0.59 W m-2) increases by 55 % globally (133 % over land and 33 % over ocean). Notably, the RFaci further increases to -1.09 W m-2 when switching total aerosol optical depth (AOD) to fine-mode AOD that is a better proxy for CCN than AOD. In contrast to previous weak satellite-based RFaci, the improved one substantially increases (especially over land), resolving a major difference with models.
Project description:A large number of processes are involved in the chain from emissions of aerosol precursor gases and primary particles to impacts on cloud radiative forcing. Those processes are manifest in a number of relationships that can be expressed as factors dlnX/dlnY driving aerosol effects on cloud radiative forcing. These factors include the relationships between cloud condensation nuclei (CCN) concentration and emissions, droplet number and CCN concentration, cloud fraction and droplet number, cloud optical depth and droplet number, and cloud radiative forcing and cloud optical depth. The relationship between cloud optical depth and droplet number can be further decomposed into the sum of two terms involving the relationship of droplet effective radius and cloud liquid water path with droplet number. These relationships can be constrained using observations of recent spatial and temporal variability of these quantities. However, we are most interested in the radiative forcing since the preindustrial era. Because few relevant measurements are available from that era, relationships from recent variability have been assumed to be applicable to the preindustrial to present-day change. Our analysis of Aerosol Comparisons between Observations and Models (AeroCom) model simulations suggests that estimates of relationships from recent variability are poor constraints on relationships from anthropogenic change for some terms, with even the sign of some relationships differing in many regions. Proxies connecting recent spatial/temporal variability to anthropogenic change, or sustained measurements in regions where emissions have changed, are needed to constrain estimates of anthropogenic aerosol impacts on cloud radiative forcing.
Project description:Marine cloud brightening (MCB) is proposed to offset global warming by emitting sea salt aerosols to the tropical marine boundary layer, which increases aerosol and cloud albedo. Sea salt aerosol is the main source of tropospheric reactive chlorine (Cl y ) and bromine (Br y ). The effects of additional sea salt on atmospheric chemistry have not been explored. We simulate sea salt aerosol injections for MCB under two scenarios (212-569 Tg/a) in the GEOS-Chem global chemical transport model, only considering their impacts as a halogen source. Globally, tropospheric Cl y and Br y increase (20-40%), leading to decreased ozone (-3 to -6%). Consequently, OH decreases (-3 to -5%), which increases the methane lifetime (3-6%). Our results suggest that the chemistry of the additional sea salt leads to minor total radiative forcing compared to that of the sea salt aerosol itself (~2%) but may have potential implications for surface ozone pollution in tropical coastal regions.
Project description:The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.
Project description:The climate effects of atmospheric aerosol particles serving as cloud condensation nuclei (CCN) depend on chemical composition and hygroscopicity, which are highly variable on spatial and temporal scales. Here we present global CCN measurements, covering diverse environments from pristine to highly polluted conditions. We show that the effective aerosol hygroscopicity, κ, can be derived accurately from the fine aerosol mass fractions of organic particulate matter (ϵorg) and inorganic ions (ϵinorg) through a linear combination, κ = ϵorg ⋅ κorg + ϵinorg ⋅ κinorg. In spite of the chemical complexity of organic matter, its hygroscopicity is well captured and represented by a global average value of κorg = 0.12 ± 0.02 with κinorg = 0.63 ± 0.01 as the corresponding value for inorganic ions. By showing that the sensitivity of global climate forcing to changes in κorg and κinorg is small, we constrain a critically important aspect of global climate modelling.
Project description:Climate models simulate a wide range of temperatures in the Arctic. Here we investigate one of the main drivers of changes in surface temperature: the net surface heat flux in the models. We show that in the winter months of the dark Arctic, there is a more than two-fold difference in the net surface heat fluxes among the models, and this difference is dominated by the downward infrared radiation from clouds. Owing to the small amount of water vapor in the winter Arctic, infrared radiation from clouds transmits more easily to the surface in the Arctic than at other latitudes, resulting in large cloud radiative effect at the surface. The dominant role of the cloud effect is also found in the transient variability of the net surface heat flux. Results demonstrate that accurate simulation of clouds is crucial for determining the net surface heat flux, which in turn affects surface temperature and sea ice properties in the Arctic.
Project description:Cloud droplet relative dispersion, defined as the standard deviation over the mean cloud droplet size, is of central importance in determining and understanding aerosol indirect effects. In recent work, it was found that cloud droplet size distributions become broader as a result of supersaturation variability and that the sensitivity of this effect is inversely related to cloud droplet number density. The subject is investigated in further detail using an extensive dataset from a laboratory cloud chamber capable of producing steady-state turbulence. An extended stochastic theory is found to successfully describe properties of the droplet size distribution, including an analytical expression for the relative dispersion. The latter is found to depend on the cloud droplet removal time, which in turn increases with the cloud droplet number density. The results show that relative dispersion decreases monotonically with increasing droplet number density, consistent with some recent atmospheric observations. Experiments spanning fast to slow microphysics regimes are reported. The observed dispersion is used to estimate time scales for autoconversion, demonstrating the important role of the turbulence-induced broadening effect on precipitation development. An initial effort is made to extend the stochastic theory to an atmospheric context with a steady updraft, for which autoconversion time is the controlling factor for droplet lifetime. As in the cloud chamber, relative dispersion is found to increase with decreasing cloud droplet number density.