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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 2 ( 2022-01-31), p. 1495-1514
    Abstract: Abstract. We investigated the distribution of polycyclic aromatic hydrocarbons (PAHs) on individual ambient aerosol particles at the Swedish western coast in a pristine environment for 10 d in October 2019. The measurements were carried out using new technology with single-particle mass spectrometry (SPMS) that reveals both the inorganic particle composition as well as the particle-bound PAHs (Schade et al., 2019). More than 290 000 particles were characterized; 4412 of them reveal PAH signatures. Most of the PAH-containing particles were internal mixtures of carbonaceous material, secondary nitrate and metals from distant sources in central and eastern Europe. We characterize the aerosol with respect to the inorganic composition, comparable to conventional SPMS, before we discuss the distribution of PAHs within this particle ensemble. Vice versa, we analyze the single-particle PAH spectra for characteristic patterns and discuss the inorganic composition, origin and atmospheric processing of the respective particles. The study period comprised different meteorological situations: clean air conditions with winds from the North Sea/Kattegat and little terrestrial air pollution, long-range transport from eastern Europe and southern Sweden, and transport of aerosols from central Europe over the sea. For all meteorological conditions, PAHs were detected in particles whose inorganic content indicates traffic emissions, such as combinations of soot, iron and calcium as well as in particles with biomass-burning signatures. However, there were variations in their amounts, dependent on the geographic origin. Because of strong mixing, rapid degradation and speciation limits, e.g., for PAHs of the same nominal mass, the application of diagnostic ratios for source apportionment is limited under the conditions of our study. Nevertheless, the combination with the inorganic content and meteorological data provides unique insights into the particles' origin, aging and mixing state. We exemplarily show how the observation of PAH profiles and inorganic secondary components on a single-particle level can open a new door to investigate aerosol aging processes. To our best knowledge, we herewith present the first comprehensive study on the single-particle distribution of PAHs in ambient air as well as the first set of combined data on PAHs and inorganic composition on a single-particle level.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 2
    In: Environmental Science: Atmospheres, Royal Society of Chemistry (RSC), Vol. 3, No. 8 ( 2023), p. 1134-1144
    Abstract: Using novel ionization technologies in single-particle mass spectrometry (SPMS), we analyzed the polycyclic aromatic hydrocarbons (PAHs) on individual particles from a research ship engine running on marine gasoil (MGO). We found a rather uniform PAH signature on the majority of particles. The PAH pattern is stable for all engine loads and particle sizes and differs from typical signatures of other pyrogenic and petrogenic PAH sources. Based on this observation, we conducted a field experiment and observed that the appearance of this PAH signature is associated with marine air masses. Moreover, we could detect the plume of a single ship passage at 15–20 km distance by the transient appearance of particles with the same distinct PAH profile. Consequently, we suggest the use of the specific PAH pattern as a new marker to detect and monitor ship emissions, independent of the conventional metal signatures that are not applicable for compliant fuels in emission control areas and coastal waters.
    Type of Medium: Online Resource
    ISSN: 2634-3606
    Language: English
    Publisher: Royal Society of Chemistry (RSC)
    Publication Date: 2023
    detail.hit.zdb_id: 3057711-1
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  • 3
    In: Chemical Science, Royal Society of Chemistry (RSC), Vol. 10, No. 12 ( 2019), p. 3486-3493
    Type of Medium: Online Resource
    ISSN: 2041-6520 , 2041-6539
    Language: English
    Publisher: Royal Society of Chemistry (RSC)
    Publication Date: 2019
    detail.hit.zdb_id: 2559110-1
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 12 ( 2020-06-18), p. 7139-7152
    Abstract: Abstract. We describe resonance effects in laser desorption–ionization (LDI) of particles that substantially increase the sensitivity and selectivity to metals in single-particle mass spectrometry (SPMS). Within the proposed scenario, resonant light absorption by ablated metal atoms increases their ionization rate within a single laser pulse. By choosing the appropriate laser wavelength, the key micronutrients Fe, Zn and Mn can be detected on individual aerosol particles with considerably improved efficiency. These ionization enhancements for metals apply to natural dust and anthropogenic aerosols, both important sources of bioavailable metals to marine environments. Transferring the results into applications, we show that the spectrum of our KrF-excimer laser is in resonance with a major absorption line of iron atoms. To estimate the impact of resonant LDI on the metal detection efficiency in SPMS applications, we performed a field experiment on ambient air with two alternately firing excimer lasers of different wavelengths. Herein, resonant LDI with the KrF-excimer laser (248.3 nm) revealed iron signatures for many more particles of the same aerosol ensemble compared to the more common ArF-excimer laser line of 193.3 nm (nonresonant LDI of iron). Many of the particles that showed iron contents upon resonant LDI were mixtures of sea salt and organic carbon. For nonresonant ionization, iron was exclusively detected in particles with a soot contribution. This suggests that resonant LDI allows a more universal and secure metal detection in SPMS. Moreover, our field study indicates relevant atmospheric iron transport by mixed organic particles, a pathway that might be underestimated in SPMS measurements based on nonresonant LDI. Our findings show a way to improve the detection and source attribution capabilities of SPMS for particle-bound metals, a health-relevant aerosol component and an important source of micronutrients to the surface oceans affecting marine primary productivity.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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