Publications by authors named "Donahue N"

Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon and the Atlantic and Pacific oceans. Although the vapours involved remain unknown, recent satellite observations have revealed surprisingly high night-time isoprene mixing ratios of up to 1 part per billion by volume (ppbv) in the tropical upper troposphere. Here, in experiments performed with the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber, we report new particle formation initiated by the reaction of hydroxyl radicals with isoprene at upper-tropospheric temperatures of -30 °C and -50 °C.

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  • Ammonia emissions in Southeast Asia significantly impact air pollution and the development of the Asian Tropopause Aerosol Layer (ATAL), particularly during summer when the South Asian monsoon is active.
  • The study utilizes the EMAC chemistry-climate model to analyze how ammonia influences particle formation, revealing a tenfold increase in particle creation during the day, especially within the monsoon's upper troposphere and lower stratosphere (UTLS).
  • Findings indicate that while ammonia enhances cloud condensation nuclei (CCN) concentrations and aerosol optical depth (AOD), its effect on aerosol mass in the ATAL is comparatively limited, suggesting a complex relationship between ammonia, particle growth, and aerosol composition.
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  • Haze in Beijing is primarily due to harmful secondary organic aerosols formed from solid-fuel emissions and secondary processes involving aromatic compounds.
  • In winter, pollution is mainly from solid-fuel combustion, with severe haze linked to aerosols transported from surrounding areas.
  • In summer, aromatic emissions from nearby regions increase secondary organic aerosol levels, indicating that regional emission control strategies are essential for effective pollution management.
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Isoprene affects new particle formation rates in environments and experiments also containing monoterpenes. For the most part, isoprene reduces particle formation rates, but the reason is debated. It is proposed that due to its fast reaction with OH, isoprene may compete with larger monoterpenes for oxidants.

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A key challenge in aerosol pollution studies and climate change assessment is to understand how atmospheric aerosol particles are initially formed. Although new particle formation (NPF) mechanisms have been described at specific sites, in most regions, such mechanisms remain uncertain to a large extent because of the limited ability of atmospheric models to simulate critical NPF processes. Here we synthesize molecular-level experiments to develop comprehensive representations of 11 NPF mechanisms and the complex chemical transformation of precursor gases in a fully coupled global climate model.

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  • * The study found that particle formation rates due to ion-induced processes are stable across temperature changes, while neutral particle formation rates increase significantly when temperatures drop from +10 °C to -10 °C.
  • * Despite higher ionization rates, the formation of charged clusters is unlikely to be enhanced in upper tropospheric conditions; instead, neutral nucleation is expected to dominate, with humidity having little effect unless extremely low.
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A comprehensive understanding of the full volatility spectrum of organic oxidation products from the benzene series precursors is important to quantify the air quality and climate effects of secondary organic aerosol (SOA) and new particle formation (NPF). However, current models fail to capture the full volatility spectrum due to the absence of important reaction pathways. Here, we develop a novel unified model framework, the integrated two-dimensional volatility basis set (I2D-VBS), to simulate the full volatility spectrum of products from benzene series precursors by simultaneously representing first-generational oxidation, multigenerational aging, autoxidation, dimerization, nitrate formation, etc.

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Cancer nanomedicines predominately rely on transport processes controlled by tumor-associated endothelial cells to deliver therapeutic and diagnostic payloads into solid tumors. While the dominant role of this class of endothelial cells for nanoparticle transport and tumor delivery is established in animal models, the translational potential in human cells needs exploration. Using primary human breast cancer as a model, the differential interactions of normal and tumor-associated endothelial cells with clinically relevant nanomedicine formulations are explored and quantified.

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Highly oxygenated organic molecules (HOMs) are a major source of new particles that affect the Earth's climate. HOM production from the oxidation of volatile organic compounds (VOCs) occurs during both the day and night and can lead to new particle formation (NPF). However, NPF involving organic vapors has been reported much more often during the daytime than during nighttime.

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The main nucleating vapor in the atmosphere is thought to be sulfuric acid (HSO), stabilized by ammonia (NH). However, in marine and polar regions, NH is generally low, and HSO is frequently found together with iodine oxoacids [HIO, i.e.

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Asphalt is ubiquitous across cities and a source of organic compounds spanning a wide range of volatility and may be an overlooked source of urban organic aerosols. The emission rate and composition depend strongly on temperature, but emissions have been observed at both application temperatures and surface temperatures during warm sunny days. Here we report primary organic aerosol (POA) emissions and secondary organic aerosol (SOA) production from asphalt.

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The pressure dependence of carbonyl oxide (Criegee intermediate) stabilization can be measured via HSO detection using chemical ionization mass spectrometry. By selectively scavenging OH radicals in a flow reactor containing an alkene, O, and SO, we measure an HSO ratio related to the Criegee intermediate stabilization, and by performing experiments at multiple pressures, we constrain the pressure dependence of the stabilization. Here, we present results from a set of monoterpenes as well as isoprene, along with previously published results from tetramethylethylene and a sequence of symmetrical trans alkenes.

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Biogenic vapors form new particles in the atmosphere, affecting global climate. The contributions of monoterpenes and isoprene to new particle formation (NPF) have been extensively studied. However, sesquiterpenes have received little attention despite a potentially important role due to their high molecular weight.

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Atmospheric simulation chambers continue to be indispensable tools for research in the atmospheric sciences. Insights from chamber studies are integrated into atmospheric chemical transport models, which are used for science-informed policy decisions. However, a centralized data management and access infrastructure for their scientific products had not been available in the United States and many parts of the world.

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  • The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO) is crucial for creating highly oxygenated organic molecules (HOM), which are essential for forming secondary organic aerosols.
  • New experiments show that low levels of NO (0 - 82 pptv) can actually boost HOM production by affecting RO loss and promoting alkoxy radical formation, which continues to react and form more HOM.
  • These findings reveal that HOM yields in boreal forest emissions can range from 2.5%-6.5%, and high NO levels do not completely stop HOM formation, challenging previous beliefs about NO's role in lowering HOM yields, especially in environments with low NO.
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Impairment in persons with multiple sclerosis (PwMS) can often be attributed to symptoms of motor instability and fatigue. Symptom monitoring and queued interventions often target these symptoms. Clinical metrics are currently limited to objective physician assessments or subjective patient reported measures.

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Super-resolution microscopy can transform our understanding of nanoparticle-cell interactions. Here, we established a super-resolution imaging technology to visualize nanoparticle distributions inside mammalian cells. The cells were exposed to metallic nanoparticles and then embedded within different swellable hydrogels to enable quantitative three-dimensional (3D) imaging approaching electron-microscopy-like resolution using a standard light microscope.

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Typical assessments of balance impairment are subjective or require data from cumbersome and expensive force platforms. Researchers have utilized lower back (sacrum) accelerometers to enable more accessible, objective measurement of postural sway for use in balance assessment. However, new sensor patches are broadly being deployed on the chest for cardiac monitoring, opening a need to determine if measurements from these devices can similarly inform balance assessment.

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  • The study investigates how high relative humidity (RH) influences the partitioning of biogenic oxidized organic molecules into secondary organic aerosols (SOA) using real-time measurements in a controlled lab setting.
  • Results show significant increases in SOA mass (45%-85%) as RH rises from low to high levels, with semi-volatile compounds playing a key role in this process.
  • The research explains that higher RH alters the chemical composition of aerosols, shifting toward more volatile species, and emphasizes the critical role of water content in promoting organic aerosol growth.
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Iodine is a reactive trace element in atmospheric chemistry that destroys ozone and nucleates particles. Iodine emissions have tripled since 1950 and are projected to keep increasing with rising O surface concentrations. Although iodic acid (HIO) is widespread and forms particles more efficiently than sulfuric acid, its gas-phase formation mechanism remains unresolved.

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Secondary organic aerosol (SOA) is a significant component of atmospheric fine particulate matter. Mobile sources have historically been a major source of SOA precursors in urban environments, but decades of regulations have reduced their emissions. Less regulated sources, such as volatile chemical products (VCPs), are of growing importance.

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Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the atmosphere. However, the acid-base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain the measured high formation rate of new particles.

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  • The study explores how nitrogen oxides (NO) affect the formation of reactive oxygen species (ROS) and environmentally persistent free radicals (EPFR) during the photooxidation of α-pinene and naphthalene, which are important for understanding aerosol chemistry and health effects.
  • It was found that while naphthalene SOA contains low levels of EPFR, NO has minimal impact on EPFR concentrations and oxidative potential, with ROS generation greatly reduced under high NO conditions.
  • High-resolution mass spectrometry revealed that high NO levels lead to the formation of nitroaromatics and organic nitrates, and modeling showed that peroxy radicals react with NO instead of hydroxyl radicals, resulting in decreased hydroperoxide formation and
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