Author
Nicholas Marsden
Bio: Nicholas Marsden is an academic researcher from University of Manchester. The author has contributed to research in topics: Mineral dust & Bioaerosol. The author has an hindex of 7, co-authored 12 publications receiving 445 citations.
Topics: Mineral dust, Bioaerosol, Aerosol, Spectrometer, Environmental science
Papers
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University of Lyon1, University of Cambridge2, University of Antwerp3, University of Manchester4, University of York5, Aarhus University6, University of Mainz7, Leibniz Institute for Neurobiology8, Alion Science and Technology9, Max Planck Society10, Ghent University11, Finnish Meteorological Institute12, University of North Carolina at Chapel Hill13, University of Bern14, University of Oslo15
TL;DR: Atmosphere: State of the Art and Challenges Barbara Nozier̀e,*,† Markus Kalberer,*,‡ Magda Claeys,* James Allan, Barbara D’Anna,† Stefano Decesari, Emanuela Finessi, Marianne Glasius, Irena Grgic,́ Jacqueline F.
Abstract: Atmosphere: State of the Art and Challenges Barbara Nozier̀e,*,† Markus Kalberer,*,‡ Magda Claeys,* James Allan, Barbara D’Anna,† Stefano Decesari, Emanuela Finessi, Marianne Glasius, Irena Grgic,́ Jacqueline F. Hamilton, Thorsten Hoffmann, Yoshiteru Iinuma, Mohammed Jaoui, Ariane Kahnt, Christopher J. Kampf, Ivan Kourtchev,‡ Willy Maenhaut, Nicholas Marsden, Sanna Saarikoski, Jürgen Schnelle-Kreis, Jason D. Surratt, Sönke Szidat, Rafal Szmigielski, and Armin Wisthaler †Ircelyon/CNRS and Universite ́ Lyon 1, 69626 Villeurbanne Cedex, France ‡University of Cambridge, Cambridge CB2 1EW, United Kingdom University of Antwerp, 2000 Antwerp, Belgium The University of Manchester & National Centre for Atmospheric Science, Manchester M13 9PL, United Kingdom Istituto ISAC C.N.R., I-40129 Bologna, Italy University of York, York YO10 5DD, United Kingdom University of Aarhus, 8000 Aarhus C, Denmark National Institute of Chemistry, 1000 Ljubljana, Slovenia Johannes Gutenberg-Universitaẗ, 55122 Mainz, Germany Leibniz-Institut für Troposphar̈enforschung, 04318 Leipzig, Germany Alion Science & Technology, McLean, Virginia 22102, United States Max Planck Institute for Chemistry, 55128 Mainz, Germany Ghent University, 9000 Gent, Belgium Finnish Meteorological Institute, FI-00101 Helsinki, Finland Helmholtz Zentrum München, D-85764 Neuherberg, Germany University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States University of Bern, 3012 Bern, Switzerland Institute of Physical Chemistry PAS, Warsaw 01-224, Poland University of Oslo, 0316 Oslo, Norway
390 citations
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TL;DR: The recent EUREC$^4$A campaign as discussed by the authors was a turning point in our ability to study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper ocean processes or the life cycle of particulate matter.
Abstract: The science guiding the EUREC$^4$A campaign and its measurements is presented. EUREC$^4$A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and
southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC$^4$A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced groundbased cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC$^4$A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC$^4$A’s outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement
84 citations
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TL;DR: In this article, measurements of aerosol and cloud properties were conducted off the coast of west Africa as part of the ICE-D and AERosol properties (AER-D) campaigns.
Abstract: . During the summertime, dust from the Sahara can be efficiently transported
westwards within the Saharan air layer (SAL). This can lead to high aerosol
loadings being observed above a relatively clean marine boundary layer (MBL)
in the tropical Atlantic Ocean. These dust layers can impart significant
radiative effects through strong visible and IR light absorption and
scattering, and can also have indirect impacts by altering cloud properties.
The processing of the dust aerosol can result in changes in both direct and
indirect radiative effects, leading to significant uncertainty in climate
prediction in this region. During August 2015, measurements of aerosol and
cloud properties were conducted off the coast of west Africa as part of the
Ice in Cloud Experiment – Dust (ICE-D) and AERosol properties – Dust
(AER-D) campaigns. Observations were obtained over a 4-week period using the
UK Facility for Atmospheric Airborne Measurements (FAAM) BAe 146 aircraft
based on Santiago Island, Cabo Verde. Ground-based observations were
collected from Praia (14 ∘ 57 ′ N, 23 ∘ 29 ′ W;
100 m a.s.l.), also located on Santiago Island. The dust in the SAL was
mostly sampled in situ at altitudes of 2–4 km, and the potential dust age
was estimated by backward trajectory analysis. The particle mass
concentration (at diameter d = 0.1–20 µm ) decreased with
transport time. Mean effective diameter ( Deff ) for supermicron
SAL dust ( d = 1–20 µm ) was found to be 5–6 µm
regardless of dust age, whereas submicron Deff
( d = 0.1–1 µm ) showed a decreasing trend with longer
transport. For the first time, an airborne laser-induced incandescence instrument (the
single particle soot photometer – SP2) was deployed to measure the hematite
content of dust. For the Sahel-influenced dust in the SAL, the observed
hematite mass fraction of dust ( FHm ) was found to be
anti-correlated with the single scattering albedo (SSA,
λ = 550 nm, for particles d µm ); as
potential dust age increased from 2 to 7 days, FHm increased from
2.5 to 4.5 %, SSA decreased from 0.97 to 0.93 and the derived imaginary
part ( k ) of the refractive index at 550 nm increased from 0.0015 to
0.0035. However, the optical properties of Sahara-influenced plumes (not
influenced by the Sahel) were independent of dust age and hematite content
with SSA ∼ 0.95 and k ∼ 0.0028 . This indicates that the
absorbing component of dust may be source dependent, or that gravitational
settling of larger particles may lead to a higher fraction of more absorbing
clay–iron aggregates at smaller sizes. Mie calculation using the measured
size distribution and size-resolved refractive indices of the absorbing
components (black carbon and hematite) reproduces the measured SSA to within
± 0.02 for SAL dust by assuming a goethite ∕ hematite mass ratio of 2.
Overall, hematite and goethite constituted 40–80 % of the absorption for
particles d µm , and black carbon (BC) contributed
10–37 %. This highlights the importance of size-dependent composition in
determining the optical properties of dust and also the contribution from BC
within dust plumes.
44 citations
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TL;DR: In this paper, the FIGAERO-HR-To-F-CIMS was used to extract vapour pressures (VPs) of polyethylene glycols (PEG) from the filter inlet for gases and AEROsols.
Abstract: . The Filter Inlet for Gases and AEROsols (FIGAERO) is an inlet specifically
designed to be coupled with the Aerodyne High-Resolution Time-of-Flight
Chemical Ionization Mass Spectrometer (HR-ToF-CIMS). The FIGAERO-HR-ToF-CIMS
provides simultaneous molecular information relating to both the gas- and
particle-phase samples and has been used to extract vapour pressures (VPs) of
the compounds desorbing from the filter whilst giving quantitative
concentrations in the particle phase. However, such extraction of vapour
pressures of the measured particle-phase components requires use of
appropriate, well-defined, reference compounds. Vapour pressures for the
homologous series of polyethylene glycols (PEG)
(( H - ( O - CH 2 - CH 2 ) n - OH ) for n=3 to n=8 ), covering a range
of vapour pressures (VP) (10 −1 to 10 −7 Pa) that are
atmospherically relevant, have been shown to be reproduced well by a range of
different techniques, including Knudsen Effusion Mass Spectrometry (KEMS).
This is the first homologous series of compounds for which a number of vapour
pressure measurement techniques have been found to be in agreement,
indicating the utility as a calibration standard, providing an ideal set of
benchmark compounds for accurate characterization of the FIGAERO for
extracting vapour pressure of measured compounds in chambers and the real
atmosphere. To demonstrate this, single-component and mixture vapour pressure
measurements are made using two FIGAERO-HR-ToF-CIMS instruments based on a
new calibration determined from the PEG series. VP values extracted from both
instruments agree well with those measured by KEMS and reported values from
literature, validating this approach for extracting VP data from the FIGAERO.
This method is then applied to chamber measurements, and the vapour pressures
of known products are estimated.
38 citations
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TL;DR: In this article, the authors used online single-particle mass spectrometry (SPMS) and traditional offline scanning electron microscopy (SEM) techniques to measure the mineralogy and mixing state of the fine fraction ( µm ) in laboratory-suspended dust from PSAs in north Africa.
Abstract: . The mineralogy and mixing state of dust particles originating from the
African continent influences climate and marine ecosystems in the North
Atlantic due to its effect on radiation, cloud properties and biogeochemical
cycling. However, these processes are difficult to constrain because of large
temporal and spatial variability, and the lack of in situ measurements of
dust properties at all stages of the dust cycle. This lack of measurements is
in part due to the remoteness of potential source areas (PSAs) and transport
pathways but also because of the lack of an efficient method to report the
mineralogy and mixing state of single particles with a time resolution
comparable to atmospheric processes, which may last a few hours or less.
Measurements are equally challenging in laboratory simulations where dust
particles need to be isolated and characterised in low numbers whilst
conditions are dynamically controlled and monitored in real time. This is
particularly important in controlled expansion cloud chambers (CECCs) where
ice-nucleating properties of suspended dust samples are studied in cold and
mixed phase cloud conditions. In this work, the mineralogy and mixing state of the fine fraction ( µm )
in laboratory-suspended dust from PSAs in north Africa were made using
novel techniques with online single-particle mass spectrometry (SPMS) and
traditional offline scanning electron microscopy (SEM). A regional
difference in mineralogy was detected, with material sourced from Morocco
containing a high number fraction of illite-like particles in contrast to
Sahelian material which contains potassium- and sodium-depleted clay minerals
like kaolinite. Single-particle mixing state had a much greater local
variation than mineralogy, particularly with respect to organic–biological
content. Applying the same methods to ambient measurement of transported dust
in the marine boundary layer at Cabo Verde in the remote North Atlantic
enabled the number fractions of illite/smectite clay mineral (ISCM),
non-ISCM and calcium-containing particles to be reported at a 1 h time
resolution over a 20-day period. Internal mixing of silicate particles with
nitrate, chlorine and organic–biological material was also measured and
compared to that in the suspended soils. The results show SPMS and SEM techniques are complementary and demonstrate
that SPMS can provide a meaningful high-resolution measurement of
single-particle mineralogy and mixing state in laboratory and ambient
conditions. In most cases, the differences in the mineralogical composition
between particles within a soil sample were small. Thus, particles were not
composed of discrete mineral phases. In ambient measurements, the ISCM and
nitrate content was found to change significantly between distinct dust
events, indicating a shift in source and transport pathways which may not be
captured in offline composition analysis or remote sensing techniques.
27 citations
Cited by
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TL;DR: A copy of the Guangbo jiemu bao [Broadcast Program Report] was being passed from hand to hand among a group of young people eager to be the first to read the article introducing the program "What Is Revolutionary Love?".
Abstract: A copy of Guangbo jiemu bao [Broadcast Program Report] was being passed from hand to hand among a group of young people eager to be the first to read the article introducing the program "What Is Revolutionary Love?" It said: "… Young friends, you are certainly very concerned about this problem'. So, we would like you to meet the young women workers Meng Xiaoyu and Meng Yamei and the older cadre Miss Feng. They are the three leading characters in the short story ‘The Place of Love.’ Through the description of the love lives of these three, the story induces us to think deeply about two questions that merit further examination.
1,528 citations
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TL;DR: Understanding of the climate-related properties of atmospheric OC is still incomplete and the specific ways in which OC impacts atmospheric environment and climate forcing are just beginning to be understood.
Abstract: Organic carbon (OC) accounts for a large fraction of atmospheric aerosol and has profound effects on air quality, atmospheric chemistry and climate forcing. Molecular composition of the OC and its evolution during common processes of atmospheric aging have been a subject of extensive research over the last decade (see reviews of Ervens et al.,1 Hallquist et al.,2 Herckes et al.,3 Carlton et al.,4 Kroll and Seinfeld,5 Rudich et al.,6 and Kanakidou et al.7). Even though many fundamental advances have been reported in these studies, our understanding of the climate-related properties of atmospheric OC is still incomplete and the specific ways in which OC impacts atmospheric environment and climate forcing are just beginning to be understood. This review covers one topic of particular interest in this area –environmental chemistry of light-absorbing aerosol OC and its impact on radiative forcing.
1,026 citations
01 Dec 2006
TL;DR: This paper showed that reactive anthropogenic VOCs (AVOCs) produce much larger amounts of SOA than these models predict, even shortly after sunrise, and a significant fraction of the excess SOA is formed from first-generation AVOC oxidation products.
Abstract: [1] The atmospheric chemistry of volatile organic compounds (VOCs) in urban areas results in the formation of ‘photochemical smog’, including secondary organic aerosol (SOA). State-of-the-art SOA models parameterize the results of simulation chamber experiments that bracket the conditions found in the polluted urban atmosphere. Here we show that in the real urban atmosphere reactive anthropogenic VOCs (AVOCs) produce much larger amounts of SOA than these models predict, even shortly after sunrise. Contrary to current belief, a significant fraction of the excess SOA is formed from first-generation AVOC oxidation products. Global models deem AVOCs a very minor contributor to SOA compared to biogenic VOCs (BVOCs). If our results are extrapolated to other urban areas, AVOCs could be responsible for additional 3–25 Tg yr−1 SOA production globally, and cause up to −0.1 W m−2 additional top-of-the-atmosphere radiative cooling.
947 citations
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TL;DR: The results suggest that mitigation strategies aimed at reducing the mass concentrations of particulate matter alone may not reduce the oxidative potential concentration, and it may be more effective to control specific sources of particulates matter rather than overall particulate mass.
Abstract: Particulate matter is a component of ambient air pollution that has been linked to millions of annual premature deaths globally1–3. Assessments of the chronic and acute effects of particulate matter on human health tend to be based on mass concentration, with particle size and composition also thought to play a part4. Oxidative potential has been suggested to be one of the many possible drivers of the acute health effects of particulate matter, but the link remains uncertain5–8. Studies investigating the particulate-matter components that manifest an oxidative activity have yielded conflicting results7. In consequence, there is still much to be learned about the sources of particulate matter that may control the oxidative potential concentration7. Here we use field observations and air-quality modelling to quantify the major primary and secondary sources of particulate matter and of oxidative potential in Europe. We find that secondary inorganic components, crustal material and secondary biogenic organic aerosols control the mass concentration of particulate matter. By contrast, oxidative potential concentration is associated mostly with anthropogenic sources, in particular with fine-mode secondary organic aerosols largely from residential biomass burning and coarse-mode metals from vehicular non-exhaust emissions. Our results suggest that mitigation strategies aimed at reducing the mass concentrations of particulate matter alone may not reduce the oxidative potential concentration. If the oxidative potential can be linked to major health impacts, it may be more effective to control specific sources of particulate matter rather than overall particulate mass. Observations and air-quality modelling reveal that the sources of particulate matter and oxidative potential in Europe are different, implying that reducing mass concentrations of particulate matter alone may not reduce oxidative potential.
282 citations
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TL;DR: This Review discusses the latest instrument development and characterization work on PTR-MS instruments, including the use of time-of-flight mass analyzers and new types of ion guiding interfaces, and reviews what has been learned about the specificity of different product ion signals for important atmospheric VOCs.
Abstract: Proton-transfer-reaction mass spectrometry (PTR-MS) has been widely used to study the emissions, distributions, and chemical evolution of volatile organic compounds (VOCs) in the atmosphere. The applications of PTR-MS have greatly promoted understanding of VOC sources and their roles in air-quality issues. In the past two decades, many new mass spectrometric techniques have been applied in PTR-MS instruments, and the performance of PTR-MS has improved significantly. This Review summarizes these developments and recent applications of PTR-MS in the atmospheric sciences. We discuss the latest instrument development and characterization work on PTR-MS instruments, including the use of time-of-flight mass analyzers and new types of ion guiding interfaces. Here we review what has been learned about the specificity of different product ion signals for important atmospheric VOCs. We present some of the recent highlights of VOC research using PTR-MS including new observations in urban air, biomass-burning plumes,...
254 citations