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Buseck, Peter

Publications and source records attributed to Buseck, Peter.

Superstoichiometric Alloying of H and Close‐Packed Fe‐Ni Metal Under High Pressures: Implications for Hydrogen Storage in Planetary Core

Although high pressure enables alloying between hydrogen and iron, hydrogen-to-iron molar ratio (H/Fe) so far found in experiments is mostly limited to 1 in the close-packed iron metal under high pressure. We report a H/(Fe + Ni) ratio of 1.8 ± 0.1 from (Fe,Ni)H x (or x ≥ 1.8) quenched from liquid, exceeding the amounts so far reported for densely packed Fe alloys. From the metastable behavior of the frozen (Fe,Ni)Hx liquid during decompression, we infer that the amount is a lower bound and therefore even a greater amount of H can be dissolved in the liquid part of Fe-rich cores of planets. The significant H storage capacity of liquid Fe-Ni alloy is important to consider for potential storage of H in the interiors of low-density planets as well as rocky planets.

58 GEOSCIENCES↗

Understanding the Evolution of Biomass Burning Particles in the Atmosphere: Analysis of BBOP Data, Laboratory Experiments, and Model Integration

Submicron particles in the atmosphere can have a profound influence on Earth’s climate [Stocker et al., 2013]. Particulate matter (PM) affects climate via both direct effects (scattering or absorption of radiation) and indirect effects (changes to the formation and properties of clouds). Biomass burning (BB) is the largest global source of submicron, carbonaceous particles [Wiedinmyer et al., 2011]. Field campaigns have shown that BB aerosol (BBA) can evolve through rapid transformations and removal processes in the atmosphere, with changing radiative and hygroscopic properties, but these processes are not well characterized. Better understanding of the evolution of biomass burning PM in the atmosphere is critical for improving the accuracy of regional to global climate models. In order to address uncertainties in the initial physical, chemical and radiative forcing of BBA and the evolution of these parameters, DOE ASR conducted an airborne field campaign, the Biomass Burning Observation Project (BBOP), during the summer and fall of 2013 to make measurements in the plumes of northwest U.S. wildfires and southeast U.S. agricultural burns. BBOP provided unique, extremely detailed trace gas and particle measurements in fresh biomass burning plumes and captured large, rapid downwind transformations within a few hours of the sources. These fast changes in properties have also been observed in laboratory-generated BB smoke in a smog chamber, but in general the controlling factors and most likely outcomes in the real atmosphere are still not clear. The goals of this project were to 1) analyze and interpret the BBOP measurements in detail, 2) conduct laboratory experiments to explore the formation of tar balls, and 3) to incorporate our findings into improved models of biomass burning emissions and aging. This research focuses on understanding the chemical, physical and optical properties and transformations of BB emissions in the near-field within hours downwind of the burn and on a more regional scale and, in turn, how BB emissions relate to climate forcing. Analysis of the BBOP data paid particular attention to relating SOA production, changes in size distribution, and mixing state to the environmental conditions (gas-phase precursors, relative humidity, radiation, oxidants, NO x , etc.). This project included subcontracts and unfunded collaborations with many of the key participants in the BBOP campaign. Professor Robert Yokelson at the University of Montana is an expert on biomass burning fuels and emissions and participated in BBOP as an unfunded collaborator. Professor Peter Buseck at Arizona State University collected particle samples during BBOP and analyzed some of them as part of this project. Unfunded collaborators include Dr. Arthur Sedlacek, III at Brookhaven National Laboratory (BNL) and Dr. Rahul Zaveri at the Pacific Northwest National Laboratory (PNNL) who were both principal investigators in the BBOP campaign, focusing on measurements and modeling, respectively. We are also working closely with Prof. Qi Zhang at UC Davis to coordinate analysis of BBOP flight data and data from the Mt. Bachelor Observatory (MBO), and with Dr. Kouji Adachi at the Meteorological Institute (Japan) to analyze laboratory-generated tar ball samples.

09 BIOMASS FUELS↗

Observations and Modeling of the Green Ocean Amazon 2014/15: Transmission Electron Microscopy Analysis of Aerosol Particles Field Campaign Report

During two Intensive Operational Periods (IOP), we collected samples at 3-hour intervals for transmission electron microscopy analysis. The resulting transmission electron microscopy images and compositions were analyzed for the samples of interest. Further analysis will be done especially for the plume of interest. We found solid spherical organic particles from rebounded samples collected with Professor Scot Martin’s group (Harvard University). Approximately 30% of the rebounded particles at 95% relative humidity were spherical organic particles. Their sources and formation process are not known, but such spherical particles could be solid and will have heterogeneous chemical reactions. We observed many organic particles that are internally mixed with inorganic elements such as potassium and nitrogen. They are either homogeneously mixed or have inorganic cores with organic aerosol coatings. Samples collected from the Manaus, Brazil, pollution plume included many nano-size soot particles mixed with organic material and sulfate. Aerosol particles from clean periods included organic aerosol particles, sulfate, sea salt, dust, and primary biogenic aerosol particles. There was more dust, primary biogenic aerosol, and tar balls in samples taken during IOP1 than those taken during IOP2. Many dust particles were found between March 2 and 3.

spherical organic particles, Manaus pollution plum↗

Campaign datasets for Observations and Modeling of the Green Ocean Amazon (GOAMAZON)

The hydrologic cycle of the Amazon Basin is one of the primary heat engines of the Southern Hemisphere. Any accurate climate model must succeed in a good description of the Basin, both in its natural state and in states perturbed by regional and global human activities. At the present time, however, tropical deep convection in a natural state is poorly understood and modeled, with insufficient observational data sets for model constraint. Furthermore, future climate scenarios resulting from human activities globally show the possible drying and the eventual possible conversion of rain forest to savanna in response to global climate change. Based on our current state of knowledge, the governing conditions of this catastrophic change are not defined. Human activities locally, including the economic development activities that are growing the population and the industry within the Basin, also have the potential to shift regional climate, most immediately by an increment in aerosol number and mass concentrations, and the shift is across the range of values to which cloud properties are most sensitive. The ARM Climate Research Facility in the Amazon Basin seeks to understand aerosol and cloud life cycles, particularly the susceptibility to cloud aerosol precipitation interactions, within the Amazon Basin.

54 ENVIRONMENTAL SCIENCES↗

Campaign datasets for Biomass Burning Observation Project (BBOP)

This field campaign will address multiple uncertainties in aerosol intensive properties, which are poorly represented in climate models, by means of aircraft measurements in biomass burning plumes. Key topics to be investigated are: 1. Aerosol mixing state and morphology 2. Mass absorption coefficients (MACs) 3. Chemical composition of non-refractory material associated with light-absorbing carbon (LAC) 4. Production rate of secondary organic aerosol (SOA) 5. Microphysical processes relevant to determining aerosol size distributions and single scattering albedo (SSA) 6. CCN activity. These topics will be investigated through measurements near active fires (0-5 hours downwind), where limited observations indicate rapid changes in aerosol properties, and in biomass burning plumes aged >5 hours. Aerosol properties and their time evolution will be determined as a function of fire type, defined according to fuel and the mix of flaming and smoldering combustion at the source.

54 ENVIRONMENTAL SCIENCES↗

Transmission electron microscope (TEM), BBOP

These transmission electron microscopy (TEM) images indicate representative particle shapes and mixing states collected during the BBOP campaign. Aerosol particles were collected onto lacey-carbon substrates.

54 ENVIRONMENTAL SCIENCES↗