Peter H. McMurry

Final Report: "Collaborative Project. Understanding the Chemical Processes That Affect Growth Rates of Freshly Nucleated Particles"

This final technical report describes our research activities that have, as the ultimate goal, the development of a model that explains growth rates of freshly nucleated particles. The research activities, which combine field observations with laboratory experiments, explore the relationship between concentrations of gas-phase species that contribute to growth and the rates at which those species are taken up. We also describe measurements of the chemical composition of freshly nucleated particles in a variety of locales, as well as properties (especially hygroscopicity) that influence their effects on climate. Our measurements include a self-organized, DOE-ARM funded project at the Southern Great Plains site, the New Particle Formation Study (NPFS), which took place during spring 2013. NPFS data are available to the research community on the ARM data archive, providing a unique suite observations of trace gas and aerosols that are associated with the formation and growth of atmospheric aerosol particles.

Final Report: " Growth Rates of Freshly Nucleated Particles"

This report lists of archival journal articles that were written with support from this grant. Research objectives from the original proposal are given, along with papers that were written to meet each of those objectives. The papers are all available in the archival literature.

Final Report "Nucleation and Growth of Atmospheric Aerosols" DOE Grant No. DE-FG02-98ER62556

Research that was supported by this contract has contributed substantially to progress in our understanding of new particle formation in the atmosphere. Objectives included the development of new measurement methods, the application of those new instrument systems in atmospheric field studies, and the interpretation of results from those studies. We developed the Nano TDMA to measure the hygroscopicity and volatility of 4-20 nm particles. We used this instrument system to characterize properties of atmospheric particles in the Atlanta atmosphere in July/August 2002 as well as to study properties of diesel exhaust particles. We also developed the thermal desorption chemical ionization mass spectrometer (TDCIMS) to measure the chemical composition of nanoparticles as small as 7 nm with a time resolution of 10-20 minutes. The TDCIMS is currently the only instrument that can perform such measurements. Atmospheric field measurements were carried out in Atlanta (July/August 2002; we refer to this as the ANARChE study) and in Boulder, CO (2003/04). In the ANARChE study we measured, for the first time, the composition of freshly nucleated particles as small as 7 nm using the TDCIMS. The ANARChE study also included the first nano-TDMA measurements of the volatility and hygroscopicity of freshly nucleated particles asmorexa0» small as 4 nm. Other parameters that were measured included particle size distributions (3 nm-2 µm), and sulfuric acid and ammonia concentrations. Key discoveries from the ANARChE study are: (1) freshly nucleated particles in Atlanta consist primarily of ammonium and sulfate; evidence for significant amounts of other species such as organics and nitrates was not found; (2) new particle formation occurs when rates of cluster loss to preexisting particles are small compared to rates of lost to the next larger cluster size by growth; a dimensionless parameter L describes the ratio of these rates, and measurements showed that new particle formation was always observed when L was less than one and not when L was greater than one; (3) growth rates of freshly nucleated particles could be explained by condensation of sulfuric acid and coagulation of the newly formed nucleation mode in the mornings when particles were small (<20 nm), but at midday when particles had growth to larger sizes measured growth rates were often five times greater than calculated growth rates suggesting that species in addition to sulfuric acid were contributing to growth. This contract also supported TDCIMS and aerosol physical property measurements performed at NCARs Mesa Laboratory in Boulder, CO, intermittently since the Spring of 2002. The TDCIMS measurements were made on sub-20 nm diameter atmospheric particles, and have uncovered many intriguing questions that warrant further investigation. For example, unlike the case in Atlanta where primarily ammonium was observed in the positive ion spectrum for ambient aerosol, Boulder aerosols appear to be composed of a variety of compounds most of which have not been identified. In the negative ion spectrum, Boulder sub-20 nm diameter particles are characterized by large nitrate peaks, with integrated areas up to 3 orders of magnitude greater than aerosol sulfate.«xa0less

Ultrafine aerosol size distribution: A study of new particle formation in the atmosphere. Final report on DOE Grant number: DE-FG02-91ER61205

This project involved studies pertinent to the formation of new particles by homogeneous nucleation in the atmosphere. The research focused on (1) the development of instrumentation to measure size distributions of freshly nucleated particles in the 3 to 10 nm diameter range, (2) laboratory studies of particle thermodynamic and transport properties relevant to nucleation in the atmosphere, and (3) field measurements of new particle formation by homogeneous nucleation. Highlights of the achievements under this grant are summarized briefly. A complete list of publications and presentations supported by the grant is given.