Showing papers by "Karl D. Froyd published in 2020"

Widespread biomass burning smoke throughout the remote troposphere

Abstract: Biomass burning emits ~34–41 Tg yr−1 of smoke aerosol to the atmosphere. Biomass burning aerosol directly influences the Earth’s climate by attenuation of solar and terrestrial radiation; however, its abundance and distribution on a global scale are poorly constrained, particularly after plumes dilute into the background remote troposphere and are subject to removal by clouds and precipitation. Here we report global-scale, airborne measurements of biomass burning aerosol in the remote troposphere. Measurements were taken during four series of seasonal flights over the Pacific and Atlantic Ocean basins, each with near pole-to-pole latitude coverage. We find that biomass burning particles in the remote troposphere are dilute but ubiquitous, accounting for one-quarter of the accumulation-mode aerosol number and one-fifth of the aerosol mass. Comparing our observations with a high-resolution global aerosol model, we find that the model overestimates biomass burning aerosol mass in the remote troposphere with a mean bias of >400%, largely due to insufficient wet removal by in-cloud precipitation. After updating the model’s aerosol removal scheme we find that, on a global scale, dilute smoke contributes as much as denser plumes to biomass burning’s scattering and absorption effects on the Earth’s radiation field. Aerosol particles produced by biomass burning are ubiquitous in the remote troposphere, according to global airborne measurements over remote ocean regions.

Characterization of organic aerosol across the global remote troposphere: a comparison of ATom measurements and global chemistry models

Abstract: . The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm−3 ). Lower concentrations ( ∼0.1 –0.3 µg sm−3 ) are observed in the northern middle and high latitudes and very low concentrations ( µg sm−3 ) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA ∕ OC) ratios of ∼2.2 –2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations.

Global Measurements of Brown Carbon and Estimated Direct Radiative Effects

Abstract: Brown carbon (BrC) is an organic aerosol material that preferentially absorbs light of shorter wavelengths. Global-scale radiative impacts of BrC have been difficult to assess due to the lack of BrC observational data. To address this, aerosol filters were continuously collected with near pole-to-pole latitudinal coverage over the Pacific and Atlantic basins in three seasons as part of the Atmospheric Tomography Mission. BrC chromophores in filter extracts were measured. We find that globally, BrC was highly spatially heterogeneous, mostly detected in air masses that had been transported from regions of extensive biomass burning. We calculate the average direct radiative effect due to BrC absorption accounted for approximately 7% to 48% of the top of the atmosphere clear-sky instantaneous forcing by all absorbing carbonaceous aerosols in the remote atmosphere, indicating that BrC from biomass burning is an important component of the global radiative balance.

A biogenic secondary organic aerosol source of cirrus ice nucleating particles

Abstract: Atmospheric ice nucleating particles (INPs) influence global climate by altering cloud formation, lifetime, and precipitation efficiency. The role of secondary organic aerosol (SOA) material as a source of INPs in the ambient atmosphere has not been well defined. Here, we demonstrate the potential for biogenic SOA to activate as depositional INPs in the upper troposphere by combining field measurements with laboratory experiments. Ambient INPs were measured in a remote mountaintop location at –46 °C and an ice supersaturation of 30% with concentrations ranging from 0.1 to 70 L–1. Concentrations of depositional INPs were positively correlated with the mass fractions and loadings of isoprene-derived secondary organic aerosols. Compositional analysis of ice residuals showed that ambient particles with isoprene-derived SOA material can act as depositional ice nuclei. Laboratory experiments further demonstrated the ability of isoprene-derived SOA to nucleate ice under a range of atmospheric conditions. We further show that ambient concentrations of isoprene-derived SOA can be competitive with other INP sources. This demonstrates that isoprene and potentially other biogenically-derived SOA materials could influence cirrus formation and properties. Ice nucleating particles impact the global climate by altering cloud formation and properties, but the sources of these emissions are not completely characterized. Here, the authors show that secondary organic aerosols formed from the oxidation of organic gases in the atmosphere can be a source of ice nucleating particles.

The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere

Abstract: . Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003