Daniel G. Partridge

Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability

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.

Strong Constraints on Aerosol-Cloud Interactions from Volcanic Eruptions

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol–cloud interactions. Here we show that the massive 2014–2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets—consistent with expectations—but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around −0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.&NA; Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol‐cloud interactions. Here we show that the massive 2014‐2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets—consistent with expectations—but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global‐mean radiative forcing of around −0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid‐water‐path response. Investigations of an Icelandic volcanic eruption confirm that sulfate aerosols caused a discernible yet transient brightening effect, as predicted, but their effect on the liquid water path was unexpectedly negligible.

Nitrate dry deposition in Svalbard

ABSTRACT Arctic regions are generally nutrient limited, receiving an extensive part of their bio-available nitrogen from the deposition of atmospheric reactive nitrogen. Reactive nitrogen oxides, as nitric acid (HNO3) and nitrate aerosols (p-NO3), can either be washed out from the atmosphere by precipitation or dry deposited, dissolving to nitrate ( ). During winter, is accumulated in the snowpack and released as a pulse during spring melt. Quantification of deposition is essential to assess impacts on Arctic terrestrial ecology and for ice core interpretations. However, the individual importance of wet and dry deposition is poorly quantified in the high Arctic regions where in-situ measurements are demanding. In this study, three different methods are employed to quantify dry deposition around the atmospheric and ecosystem monitoring site, Ny-Ålesund, Svalbard, for the winter season (September 2009 to May 2010): (1) A snow tray sampling approach indicates a dry deposition of –10.27±3.84 mg m−2 (± S.E.); (2) A glacial sampling approach yielded somewhat higher values –30.68±12.00 mg m−2; and (3) Dry deposition was also modelled for HNO3 and p-NO3 using atmospheric concentrations and stability observations, resulting in a total combined nitrate dry deposition of –10.76±1.26 mg m−2. The model indicates that deposition primarily occurs via HNO3 with only a minor contribution by p-NO3. Modelled median deposition velocities largely explain this difference: 0.63 cm s−1 for HNO3 while p-NO3 was 0.0025 and 0.16 cm s−1 for particle sizes 0.7 and 7 µm, respectively. Overall, the three methods are within two standard errors agreement, attributing an average 14% (total range of 2–44%) of the total nitrate deposition to dry deposition. Dry deposition events were identified in association with elevated atmospheric concentrations, corroborating recent studies that identified episodes of rapid pollution transport and deposition to the Arctic.

Revising the hygroscopicity of inorganic sea salt particles

Sea spray is one of the largest natural aerosol sources and plays an important role in the Earth’s radiative budget. These particles are inherently hygroscopic, that is, they take-up moisture from the air, which affects the extent to which they interact with solar radiation. We demonstrate that the hygroscopic growth of inorganic sea salt is 8–15% lower than pure sodium chloride, most likely due to the presence of hydrates. We observe an increase in hygroscopic growth with decreasing particle size (for particle diameters <150 nm) that is independent of the particle generation method. We vary the hygroscopic growth of the inorganic sea salt within a general circulation model and show that a reduced hygroscopicity leads to a reduction in aerosol-radiation interactions, manifested by a latitudinal-dependent reduction of the aerosol optical depth by up to 15%, while cloud-related parameters are unaffected. We propose that a value of κs=1.1 (at RH=90%) is used to represent the hygroscopicity of inorganic sea salt particles in numerical models.

Constraining the instantaneous aerosol influence on cloud albedo

Significance Uncertainties in the strength of aerosol–cloud interactions drive the current uncertainty in the anthropogenic forcing of the climate. Previous studies have highlighted shortcomings in using satellite data for determining the forcing, which underestimate the strength of the aerosol forcing. This work demonstrates that the component of the radiative forcing from aerosol–cloud interactions due to the instantaneous effect on cloud reflectivity (RFaci) can be calculated to within 20%, using only present-day observations of the variability of aerosol and cloud properties, provided the anthropogenic component of the aerosol is known. The model results are combined with satellite data to provide an improved observations-based estimate of the RFaci, paving the way for more accurate estimates of the aerosol influence on climate. Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration (Nd), previous studies have used the sensitivity of the Nd to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol and cloud properties in the present-day climate may not be suitable for determining the sensitivity of the Nd to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between Nd and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. The accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.

Microphysical explanation of the RH‐dependent water affinity of biogenic organic aerosol and its importance for climate

Abstract A large fraction of atmospheric organic aerosol (OA) originates from natural emissions that are oxidized in the atmosphere to form secondary organic aerosol (SOA). Isoprene (IP) and monoterpenes (MT) are the most important precursors of SOA originating from forests. The climate impacts from OA are currently estimated through parameterizations of water uptake that drastically simplify the complexity of OA. We combine laboratory experiments, thermodynamic modeling, field observations, and climate modeling to (1) explain the molecular mechanisms behind RH‐dependent SOA water‐uptake with solubility and phase separation; (2) show that laboratory data on IP‐ and MT‐SOA hygroscopicity are representative of ambient data with corresponding OA source profiles; and (3) demonstrate the sensitivity of the modeled aerosol climate effect to assumed OA water affinity. We conclude that the commonly used single‐parameter hygroscopicity framework can introduce significant error when quantifying the climate effects of organic aerosol. The results highlight the need for better constraints on the overall global OA mass loadings and its molecular composition, including currently underexplored anthropogenic and marine OA sources.

Erratum: Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability (Proceedings of the National Academy of Sciences of the United States of America (2016) 113 (5804-5811))

COLLOQUIUM Correction for “Challenges in constraining anthropogenic aerosol effects on cloud radiative forcing using present-day spatiotemporal variability,” by Steven Ghan, Minghuai Wang, Shipeng Zhang, Sylvaine Ferrachat, Andrew Gettelman, Jan Griesfeller, Zak Kipling, Ulrike Lohmann, Hugh Morrison, David Neubauer, Daniel G. Partridge, Philip Stier, Toshihiko Takemura, Hailong Wang, and Kai Zhang, which appeared in issue 21, May 24, 2016, of Proc Natl Acad Sci USA (113:5804–5811; first published February 26, 2016; 10.1073/pnas.1514036113). The authors note the order of affiliations for Minghuai Wang appeared incorrectly: this author’s first affiliation should be listed as Institute for Climate and Global Change Research, Nanjing University. The corrected author and affiliation lines appear below. The online version has been corrected. The authors also note that, due to a printer’s error, Eq. 3 appeared incorrectly. The corrected equation appears below. The online version has been corrected.