Publications by authors named "Douglas R Worsnop"

Article Synopsis
  • 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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Dinitrogen pentoxide (NO) plays an essential role in tropospheric chemistry, serving as a nocturnal reservoir of reactive nitrogen and significantly promoting nitrate formations. However, identifying key environmental drivers of NO formation remains challenging using traditional statistical methods, impeding effective emission control measures to mitigate NO-induced air pollution. Here, we adopted machine learning assisted by steady-state analysis to elucidate the driving factors of NO before and during the 2022 Winter Olympics (WO) in Beijing.

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  • Researchers observed pure biogenic new particle formation (NPF) driven by highly oxygenated organic molecules (HOMs) in a peatland in southern Finland, indicating a possible mechanism for aerosol formation similar to pre-industrial times.
  • The study found that meteorological conditions created an "air pocket" at night, allowing NPF to initiate solely from biogenic HOM, providing a rare look at a pristine atmospheric environment.
  • This research offers insights into how pre-industrial aerosols were formed, helping improve our understanding of the effects of aerosols on climate today and in the future, especially as air pollution mitigation efforts may return conditions closer to those of the past.
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  • * The study investigated how titanium dioxide (TiO) photocatalytic seeds can reduce secondary organic aerosol (SOA) formation from the oxidation of α-pinene and toluene under UV light.
  • * Results showed a marked reduction in SOA particles—53.7% for α-pinene SOA directly and 21.9% for externally mixed SOA, demonstrating the potential of TiO in air pollution control and its implications for climate interactions.
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  • Aerosols from gas-to-particle processes significantly contribute to urban smog and haze, particularly through the formation of ammonium nitrate, which can thrive in polluted city conditions.
  • Urban areas face complex variations in temperature and gas concentrations, influencing how quickly aerosols can form and grow.
  • Experimental results from CERN's CLOUD chamber reveal that rapid temperature fluctuations can enhance nanoparticle growth, highlighting the influence of inconsistent ammonia emissions in cities on aerosol dynamics.
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Biogenic and anthropogenic organic vapors are crucial precursors of ozone and secondary organic aerosol (SOA) in the atmosphere. Here we conducted real-time measurements of gaseous organic compounds using a Vocus proton-transfer-reaction mass spectrometer (Vocus PTR-MS) at the Shanghuang mountain site (1128 m a.s.

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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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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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Oxygenated organic molecules (OOMs) are critical intermediates linking volatile organic compound oxidation and secondary organic aerosol (SOA) formation. Yet, the understanding of OOM components, formation mechanism, and impacts are still limited, especially for urbanized regions with a cocktail of anthropogenic emissions. Herein, ambient measurements of OOMs were conducted at a regional background site in South China in 2018.

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Article Synopsis
  • 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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Alkaline gases, including NH, C-amines, C-amides, and C-imines, were measured using a water cluster-CIMS in urban Beijing during the wintertime of 2018, with a campaign average of 2.8 ± 2.0 ppbv, 5.

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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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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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  • Dimethyl sulfide (DMS) contributes to climate change by affecting cloud formation through its oxidation products, primarily methanesulfonic acid (MSA) and sulfuric acid (HSO), but predicting their levels accurately is difficult.
  • Experiments conducted at CERN's CLOUD chamber showed that lowering the temperature significantly boosts the production of MSA from DMS oxidation, while HSO production remains relatively stable, resulting in a lower HSO/MSA ratio at cold temperatures.
  • The research introduces a new DMS oxidation mechanism that increases MSA production estimates, significantly higher than previous models, revealing MSA's crucial role in the sulfur cycle and its impact on cloud condensation nuclei.
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Nucleation of neutral iodine particles has recently been found to involve both iodic acid (HIO) and iodous acid (HIO). However, the precise role of HIO in iodine oxoacid nucleation remains unclear. Herein, we probe such a role by investigating the cluster formation mechanisms and kinetics of (HIO)(HIO) ( = 0-4, = 0-4) clusters with quantum chemical calculations and atmospheric cluster dynamics modeling.

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Article Synopsis
  • New particle formation events occur frequently in polluted environments, despite high loss rates of tiny clusters, suggesting scavenging by larger particles or unknown growth mechanisms might be less effective than anticipated.
  • Experiments in the CLOUD chamber at CERN showed that the creation of new particles from human-made vapors significantly drops when there are many pre-existing particles, proving they effectively scavenge smaller molecular clusters.
  • In conditions with high levels of nitric acid and ammonia, newly formed particles can grow rapidly and maintain their numbers, even in heavily polluted air, which helps explain why these particles survive in haze-like situations.
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New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN). However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components.

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Oxygenated volatile organic compounds (OVOCs) and secondary organic aerosol (SOA) formation potential of ambient air in Guangzhou, China was investigated using a field-deployed oxidation flow reactor (OFR). The OFR was used to mimic hours to weeks of atmospheric exposure to hydroxyl (OH) radicals within the 2-3 min residence time. A comprehensive investigation on the variation of VOCs and OVOCs as a function of OH exposure is shown.

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Article Synopsis
  • - Understanding the formation of secondary organic aerosols (SOA) at a molecular level is challenging due to unclear mechanisms and inadequate analytical methods, particularly in developing countries where haze impacts climate and health significantly.
  • - This study includes simultaneous measurements of volatile organic compounds (VOCs), oxygenated organic molecules (OOMs), and SOA particles in Beijing, revealing that OOMs are responsible for 26-39% of organic aerosol mass growth.
  • - The findings indicate that the contribution of OOMs to SOA increases during severe haze episodes, establishing a clear link from emissions to the formation of haze through condensable organic oxidation products.
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Medical shortages during the COVID-19 pandemic saw numerous efforts to 3D print personal protective equipment and treatment supplies. There is, however, little research on the potential biocompatibility of 3D-printed parts using typical polymeric resins as pertaining to volatile organic compounds (VOCs), which have specific relevance for respiratory circuit equipment. Here, we measured VOCs emitted from freshly printed stereolithography (SLA) replacement medical parts using proton transfer reaction mass spectrometry and infrared differential absorption spectroscopy, and particulates using a scanning mobility particle sizer.

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Aerosol particles negatively affect human health while also having climatic relevance due to, for example, their ability to act as cloud condensation nuclei. Ultrafine particles (diameter < 100 nm) typically comprise the largest fraction of the total number concentration, however, their chemical characterization is difficult because of their low mass. Using an extractive electrospray time-of-flight mass spectrometer (EESI-TOF), we characterize the molecular composition of freshly nucleated particles from naphthalene and β-caryophyllene oxidation products at the CLOUD chamber at CERN.

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Gas-phase oxygenated organic molecules (OOMs) can contribute substantially to the growth of newly formed particles. However, the characteristics of OOMs and their contributions to particle growth rate are not well understood in urban areas, which have complex anthropogenic emissions and atmospheric conditions. We performed long-term measurement of gas-phase OOMs in urban Beijing during 2018-2019 using nitrate-based chemical ionization mass spectrometry.

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Molecular clustering is the initial step of atmospheric new particle formation (NPF) that generates numerous secondary particles. Using two online mass spectrometers with and without a chemical ionization inlet, we characterized the neutral clusters and the naturally charged ion clusters during NPF periods in urban Beijing. In ion clusters, we observed pure sulfuric acid (SA) clusters, SA-amine clusters, SA-ammonia (NH) clusters, and SA-amine-NH clusters.

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Article Synopsis
  • - Iodic acid (HIO) can rapidly form aerosol particles in coastal areas, with nucleation rates surpassing those of sulfuric acid-ammonia under similar conditions.
  • - Ion-induced nucleation involves the initial formation of IO followed by the addition of HIO, occurring efficiently at temperatures below +10°C, while neutral nucleation relies on a different process involving iodous acid.
  • - Freshly formed HIO particles significantly contribute to fast particle growth and can effectively compete with sulfuric acid particle formation in unpolluted atmospheric regions.
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