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Pierce, Jeffrey R.

Publications and source records attributed to Pierce, Jeffrey R..

12 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Kinetic Modeling of Secondary Organic Aerosol in a Weather-Chemistry Model: Parameterizations, Processes, and Predictions for GOAmazon

Secondary organic aerosol (SOA) forms and evolves in the atmosphere through many pathways and processes, over diverse spatial and time scales. Hence, there is a need to represent these widely-varying kinetic processes in large-scale atmospheric models to allow for accurate predictions of the abundance, properties, and impacts of SOA. In this work, we integrated a kinetic, process-level model (simpleSOM-MOSAIC) into a weather-chemistry model (WRF-Chem) to simulate the oxidation chemistry and microphysics of atmospheric SOA. simpleSOM-MOSAIC simulates multigenerational gas-phase chemistry, autoxidation reactions, heterogeneous oxidation, oligomerization, and phase-state-influenced gas/particle partitioning of SOA. As a case study, the integrated WRF-Chem-simpleSOM-MOSAIC (WC-SSM) model was used to simulate the photochemical evolution downwind of a large city (Manaus, Brazil) in the Amazon and, in turn, study the anthropogenic and biogenic interactions in an otherwise pristine environment. Consistent with previous work, we found that OA was enhanced by up to a factor of four in the urban plume due to elevated hydroxyl radical (OH) concentrations, relative to the background, and that this OA was dominated by SOA from biogenic precursors (80%). Further, in addition to accurately simulating the OA enhancement in the urban plume, the model reproduced the magnitude of the OA oxygen-to-carbon (O:C) ratio and broadly tracked the evolution of the aerosol size distribution. Our work highlights the importance of including an integrated, kinetic representation of SOA processes in an atmospheric model

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Anthropogenic extremely low volatility organics (ELVOCs) Govern the Growth of Molecular Clusters over the Southern Great Plains during the Springtime

New particle formation (NPF) and growth govern cloud condensation nuclei (CCN) concentrations in many regions. The mechanisms governing the nucleation of molecular clusters vary substantially in different regions of the atmosphere. Additionally, the growth of these clusters from ~2 to 20 nm sizes is often governed by the availability of extremely low volatility organic vapours (ELVOCs). While the pathways to ELVOC formation from the oxidation of biogenic monoterpenes with ozone is better understood, the chemical and mechanistic pathways for ELVOC formation from oxidation of anthropogenic organics are not well understood. We integrate measurements and three-dimensional regional model simulations with the Weather Research and Forecasting Model coupled to chemistry (WRF-Chem) to understand the processes governing new particle formation and growth and secondary organic aerosol (SOA) formation during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) field campaign at the Southern Great Plains (SGP) observatory in Oklahoma, and contrast it with a site within the Bankhead National Forest (BNF), Alabama in Southeast USA, where 5-year long measurements will begin in 2024. Simulations show that nucleation rates are at least an order of magnitude higher at SGP compared to BNF during the springtime days (April 28 and May 14, 2016), largely due to lower H2SO4 concentrations at BNF, which are needed for nucleation. In addition, the larger CS at BNF (compared to SGP) increase the loss of molecular clusters by coagulation to pre-existing particles. Among the 8 different nucleation mechanisms in WRF-Chem, we find that the amine+H2SO4 nucleation mechanism dominates at the SGP site, while the pure organic ion induced nucleation mechanism dominates over BNF. Through various WRF-Chem sensitivity simulations, we find that anthropogenic ELVOCs are critical for explaining the growth of newly formed particles and the resulting number size distribution observed near the surface at the SGP site during the daytime. In addition, we show that treating organic particles as semisolid, with strong diffusion-limited uptake of organic vapours, brings model predictions into closer agreement with the observed evolution of particle size distribution. Simulations also predict that anthropogenic SOA, formed by the oxidation of aromatic volatile organic compounds (VOCs), is the dominant organic aerosol component at SGP, while biogenic SOA dominates particle composition at the BNF site in Southeast USA on these days.

Shrivastava, ManishKumar B.↗
DOE OSTI2024

Constraining Present‐Day Anthropogenic Total Iron Emissions Using Model and Observations

Abstract Iron emissions from human activities, such as oil combustion and smelting, affect the Earth's climate and marine ecosystems. These emissions are difficult to quantify accurately due to a lack of observations, particularly in remote ocean regions. In this study, we used long‐term, near‐source observations in areas with a dominance of anthropogenic iron emissions in various parts of the world to better estimate the total amount of anthropogenic iron emissions. We also used a statistical source apportionment method to identify the anthropogenic components and their sub‐sources from bulk aerosol observations in the United States. We find that the estimates of anthropogenic iron emissions are within a factor of 3 in most regions compared to previous inventory estimates. Under‐ or overestimation varied by region and depended on the number of sites, interannual variability, and the statistical filter choice. Smelting‐related iron emissions are overestimated by a factor of 1.5 in East Asia compared to previous estimates. More long‐term iron observations and the consideration of the influence of dust and wildfires could help reduce the uncertainty in anthropogenic iron emissions estimates.

Meteorology & Atmospheric Sciences↗
DOE OSTI2024

Intense formation of secondary ultrafine particles from Amazonian vegetation fires and their invigoration of deep clouds and precipitation

New particle formation (NPF) in fire smoke is thought to be unlikely due to large condensation and coagulation sinks that scavenge molecular clusters. We analyze aircraft measurements over the Amazon and find that fires significantly enhance NPF and ultrafine particle (UFP < 50 nm diameter) numbers compared to background conditions, contrary to previous understanding. We identify that the nucleation of dimethylamine with sulfuric acid, which is aided by the formation of extremely low volatility organics in biomass-burning smoke, can overcome the large condensation and coagulation sinks and explain aircraft observations. We show that freshly formed clusters rapidly grow to UFP sizes through biomass-burning secondary organic aerosol formation, leading to a 10-fold increase in UFP number concentrations. Here, we find a contrasting effect of UFPs on deep convective clouds compared to the larger particles from primary emissions for the case investigated here. UFPs intensify the deep convective clouds and precipitation due to increased condensational heating, while larger particles delay and reduce precipitation.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2019

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

cloud droplets↗
NASA NTRS2010

Efficient Formation of Stratospheric Aerosol for Climate Engineering by Emission of Condensible Vapor from Aircraft

Recent analysis suggests that the effectiveness of stratospheric aerosol climate engineering through emission of non-condensable vapors such as SO2 is limited because the slow conversion to H2SO4 tends to produce aerosol particles that are too large; SO2 injection may be so inefficient that it is difficult to counteract the radiative forcing due to a CO2 doubling. Here we describe an alternate method in which aerosol is formed rapidly in the plume following injection of H2SO4, a condensable vapor, from an aircraft. This method gives better control of particle size and can produce larger radiative forcing with lower sulfur loadings than SO2 injection. Relative to SO2 injection, it may reduce some of the adverse effects of geoengineering such as radiative heating of the lower stratosphere. This method does not, however, alter the fact that such a geoengineered radiative forcing can, at best, only partially compensate for the climate changes produced by CO2.

Pierce, Jeffrey R.↗
NASA NTRS2010

Detecting Thin Cirrus in Multiangle Imaging Spectroradiometer Aerosol Retrievals

Thin cirrus clouds (optical depth (OD) < 03) are often undetected by standard cloud masking in satellite aerosol retrieval algorithms. However, the Mu]tiangle Imaging Spectroradiometer (MISR) aerosol retrieval has the potential to discriminate between the scattering phase functions of cirrus and aerosols, thus separating these components. Theoretical tests show that MISR is sensitive to cirrus OD within Max{0.05 1 20%l, similar to MISR's sensitivity to aerosol OD, and MISR can distinguish between small and large crystals, even at low latitudes, where the range of scattering angles observed by MISR is smallest. Including just two cirrus components in the aerosol retrieval algorithm would capture typical MISR sensitivity to the natural range of cinus properties; in situations where cirrus is present but the retrieval comparison space lacks these components, the retrieval tends to underestimate OD. Generally, MISR can also distinguish between cirrus and common aerosol types when the proper cirrus and aerosol optical models are included in the retrieval comparison space and total column OD is >-0.2. However, in some cases, especially at low latitudes, cirrus can be mistaken for some combinations of dust and large nonabsorbing spherical aerosols, raising a caution about retrievals in dusty marine regions when cirrus is present. Comparisons of MISR with lidar and Aerosol Robotic Network show good agreement in a majority of the cases, but situations where cirrus clouds have optical depths >0.15 and are horizontally inhomogeneous on spatial scales shorter than 50 km pose difficulties for cirrus retrieval using the MISR standard aerosol algorithm..

Pierce, Jeffrey R.↗