Physical science research needed to evaluate the viability and risks of marine cloud brightening.

Marine cloud brightening (MCB) is the deliberate injection of aerosol particles into shallow marine clouds to increase their reflection of solar radiation and reduce the amount of energy absorbed by the climate system. From the physical science perspective, the consensus of a broad international group of scientists is that the viability of MCB will ultimately depend on whether observations and models can robustly assess the scale-up of local-to-global brightening in today's climate and identify strategies that will ensure an equitable geographical distribution of the benefits and risks associated with projected regional changes in temperature and precipitation. To address the physical science knowledge gaps required to assess the societal implications of MCB, we propose a substantial and targeted program of research-field and laboratory experiments, monitoring, and numerical modeling across a range of scales.

Aerosol effects on clouds are concealed by natural cloud heterogeneity and satellite retrieval errors.

One major source of uncertainty in the cloud-mediated aerosol forcing arises from the magnitude of the cloud liquid water path (LWP) adjustment to aerosol-cloud interactions, which is poorly constrained by observations. Many of the recent satellite-based studies have observed a decreasing LWP as a function of cloud droplet number concentration (CDNC) as the dominating behavior. Estimating the LWP response to the CDNC changes is a complex task since various confounding factors need to be isolated. However, an important aspect has not been sufficiently considered: the propagation of natural spatial variability and errors in satellite retrievals of cloud optical depth and cloud effective radius to estimates of CDNC and LWP. Here we use satellite and simulated measurements to demonstrate that, because of this propagation, even a positive LWP adjustment is likely to be misinterpreted as negative. This biasing effect therefore leads to an underestimate of the aerosol-cloud-climate cooling and must be properly considered in future studies.

Shipping regulations lead to large reduction in cloud perturbations.

Global shipping accounts for 13% of global emissions of SO2, which, once oxidized to sulfate aerosol, acts to cool the planet both directly by scattering sunlight and indirectly by increasing the albedo of clouds. This cooling due to sulfate aerosol offsets some of the warming effect of greenhouse gasses and is the largest uncertainty in determining the change in the Earth's radiative balance by human activity. Ship tracks-the visible manifestation of the indirect of effect of ship emissions on clouds as quasi-linear features-have long provided an opportunity to quantify these effects. However, they have been arduous to catalog and typically studied only in particular regions for short periods of time. Using a machine-learning algorithm to automate their detection we catalog more than 1 million ship tracks to provide a global climatology. We use this to investigate the effect of stringent fuel regulations introduced by the International Maritime Organization in 2020 on their global prevalence since then, while accounting for the disruption in global commerce caused by COVID-19. We find a marked, but clearly nonlinear, decline in ship tracks globally: An 80% reduction in SO[Formula: see text] emissions causes only a 25% reduction in the number of tracks detected.

Opportunistic experiments to constrain aerosol effective radiative forcing.

Aerosol-cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide "opportunistic experiments" (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred. These perturbations cover a wide range of locations and spatiotemporal scales, including point sources such as volcanic eruptions or industrial sources, plumes from biomass burning or forest fires, and tracks from individual ships or shipping corridors. We review the different experimental conditions and conduct a synthesis of the available satellite datasets and field campaigns to place these opportunistic experiments on a common footing, facilitating new insights and a clearer understanding of key uncertainties in aerosol radiative forcing. Cloud albedo perturbations are strongly sensitive to background meteorological conditions. Strong liquid water path increases due to aerosol perturbations are largely ruled out by averaging across experiments. Opportunistic experiments have significantly improved process-level understanding of ACI, but it remains unclear how reliably the relationships found can be scaled to the global level, thus demonstrating a need for deeper investigation in order to improve assessments of aerosol radiative forcing and climate change.

Surprising similarities in model and observational aerosol radiative forcing estimates.

The radiative forcing from aerosols (particularly through their interaction with clouds) remains one of the most uncertain components of the human forcing of the climate. Observation-based studies have typically found a smaller aerosol effective radiative forcing than in model simulations and were given preferential weighting in the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment Report (AR5). With their own sources of uncertainty, it is not clear that observation-based estimates are more reliable. Understanding the source of the model and observational differences is thus vital to reduce uncertainty in the impact of aerosols on the climate. These reported discrepancies arise from the different methods of separating the components of aerosol forcing used in model and observational studies. Applying the observational decomposition to global climate model (GCM) output, the two different lines of evidence are surprisingly similar, with a much better agreement on the magnitude of aerosol impacts on cloud properties. Cloud adjustments remain a significant source of uncertainty, particularly for ice clouds. However, they are consistent with the uncertainty from observation-based methods, with the liquid water path adjustment usually enhancing the Twomey effect by less than 50%. Depending on different sets of assumptions, this work suggests that model and observation-based estimates could be more equally weighted in future synthesis studies.

Analysis of polarimetric satellite measurements suggests stronger cooling due to aerosol-cloud interactions.

Anthropogenic aerosol emissions lead to an increase in the amount of cloud condensation nuclei and consequently an increase in cloud droplet number concentration and cloud albedo. The corresponding negative radiative forcing due to aerosol cloud interactions (RF[Formula: see text]) is one of the most uncertain radiative forcing terms as reported in the 5th Assessment Report of the Intergovernmental Panel on Climate Change (IPCC). Here we show that previous observation-based studies underestimate aerosol-cloud interactions because they used measurements of aerosol optical properties that are not directly related to cloud formation and are hampered by measurement uncertainties. We have overcome this problem by the use of new polarimetric satellite retrievals of the relevant aerosol properties (aerosol number, size, shape). The resulting estimate of RF[Formula: see text] = -1.14 Wm[Formula: see text] (range between -0.84 and -1.72 Wm[Formula: see text]) is more than a factor 2 stronger than the IPCC estimate that includes also other aerosol induced changes in cloud properties.

Constraining the instantaneous aerosol influence on cloud albedo.

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.