skip to main content

Search for: All records

Creators/Authors contains: "Bell, David M."

Note: When clicking on a Digital Object Identifier (DOI) number, you will be taken to an external site maintained by the publisher. Some full text articles may not yet be available without a charge during the embargo (administrative interval).
What is a DOI Number?

Some links on this page may take you to non-federal websites. Their policies may differ from this site.

  1. Free, publicly-accessible full text available November 1, 2023
  2. Abstract 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 3 surface concentrations. Although iodic acid (HIO 3 ) is widespread and forms particles more efficiently than sulfuric acid, its gas-phase formation mechanism remains unresolved. Here, in CLOUD atmospheric simulation chamber experiments that generate iodine radicals at atmospherically relevant rates, we show that iodooxy hypoiodite, IOIO, is efficiently converted into HIO 3 via reactions (R1) IOIO + O 3  → IOIO 4 and (R2) IOIO 4  + H 2 O → HIO 3  + HOI +  (1) O 2 . The laboratory-derived reaction rate coefficients are corroborated by theory and shown to explain field observations of daytime HIO 3 in the remote lower free troposphere. The mechanism provides a missing link between iodine sources and particle formation. Because particulate iodate is readily reduced, recycling iodine back into the gas phase, our results suggest a catalytic role of iodine in aerosol formation.
    Free, publicly-accessible full text available November 14, 2023
  3. Intense new particle formation events are regularly observed under highly polluted conditions, despite the high loss rates of nucleated clusters. Higher than expected cluster survival probability implies either ineffective scavenging by pre-existing particles or missing growth mechanisms. Here we present experiments performed in the CLOUD chamber at CERN showing particle formation from a mixture of anthropogenic vapours, under condensation sinks typical of haze conditions, up to 0.1 s −1 . We find that new particle formation rates substantially decrease at higher concentrations of pre-existing particles, demonstrating experimentally for the first time that molecular clusters are efficiently scavenged by larger sized particles. Additionally, we demonstrate that in the presence of supersaturated gas-phase nitric acid (HNO 3 ) and ammonia (NH 3 ), freshly nucleated particles can grow extremely rapidly, maintaining a high particle number concentration, even in the presence of a high condensation sink. Such high growth rates may explain the high survival probability of freshly formed particles under haze conditions. We identify under what typical urban conditions HNO 3 and NH 3 can be expected to contribute to particle survival during haze.
    Free, publicly-accessible full text available May 19, 2023
  4. Abstract. Extractive electrospray ionization (EESI) has been a well-knowntechnique for high-throughput online molecular characterization of chemicalreaction products and intermediates, detection of native biomolecules, invivo metabolomics, and environmental monitoring with negligible thermal andionization-induced fragmentation for over two decades. However, the EESIextraction mechanism remains uncertain. Prior studies disagree on whetherparticles between 20 and 400 nm diameter are fully extracted or if theextraction is limited to the surface layer. Here, we examined the analyteextraction mechanism by assessing the influence of particle size and coatingthickness on the detection of the molecules therein. We find that particlesare extracted fully: organics-coated NH4NO3 particles with afixed core volume (156 and 226 nm in diameter without coating) showedconstant EESI signals for NH4NO3 independent of the shell coatingthickness, while the signals of the secondary organic molecules comprisingthe shell varied proportionally to the shell volume. We also found that theEESI sensitivity exhibited a strong size dependence, with an increase insensitivity by 1–3 orders of magnitude as particle size decreasedfrom 300 to 30 nm. This dependence varied with the electrospray (ES)droplet size, the particle size and the residence time for coagulation in theEESI inlet, suggesting that the EESI sensitivity was influenced by thecoagulation coefficient between particles and ES droplets. Overall, ourresults indicate that, inmore »the EESI, particles are fully extracted by the ESdroplets regardless of the chemical composition, when they are collected bythe ES droplets. However, their coalescence is not complete and dependsstrongly on their size. This size dependence is especially relevant whenEESI is used to probe size-varying particles as is the case in aerosolformation and growth studies with size ranges below 100 nm.« less
  5. Free, publicly-accessible full text available March 15, 2023
  6. 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 D p < 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. We perform a detailed intercomparison of the organic aerosol chemical composition measured by the EESI-TOF and an iodide adduct chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols (FIGAERO-I-CIMS). We also use an aerosol growth model based on the condensation of organic vapors to show that the chemical composition measured by the EESI-TOF is consistent with the expected condensed oxidation products. This agreement could be further improved by constraining the EESI-TOF compound-specific sensitivity or considering condensed-phase processes. Our results show that the EESI-TOF can obtain the chemical composition of particles as small as 20 nm in diameter with mass loadings as low as hundreds of ng m −3 in real time. This was until nowmore »difficult to achieve, as other online instruments are often limited by size cutoffs, ionization/thermal fragmentation and/or semi-continuous sampling. Using real-time simultaneous gas- and particle-phase data, we discuss the condensation of naphthalene oxidation products on a molecular level.« less
  7. Abstract Detecting and understanding disturbance is a challenge in ecology that has grown more critical with global environmental change and the emergence of research on social–ecological systems. We identify three areas of research need: developing a flexible framework that incorporates feedback loops between social and ecological systems, anticipating whether a disturbance will change vulnerability to other environmental drivers, and incorporating changes in system sensitivity to disturbance in the face of global changes in environmental drivers. In the present article, we review how discoveries from the US Long Term Ecological Research (LTER) Network have influenced theoretical paradigms in disturbance ecology, and we refine a framework for describing social–ecological disturbance that addresses these three challenges. By operationalizing this framework for seven LTER sites spanning distinct biomes, we show how disturbance can maintain or alter ecosystem state, drive spatial patterns at landscape scales, influence social–ecological interactions, and cause divergent outcomes depending on other environmental changes.