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result(s) for
"Sanchez-Marroquin, Alberto"
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The ice-nucleating ability of quartz immersed in water and its atmospheric importance compared to K-feldspar
2019
Mineral dust particles are thought to be an important type of ice-nucleating particle (INP) in the mixed-phase cloud regime around the globe. While K-rich feldspar (K-feldspar) has been identified as being a particularly important component of mineral dust for ice nucleation, it has been shown that quartz is also relatively ice-nucleation active. Given quartz typically makes up a substantial proportion of atmospheric desert dust, it could potentially be important for cloud glaciation. Here, we survey the ice-nucleating ability of 10 α-quartz samples (the most common quartz polymorph) when immersed in microlitre supercooled water droplets. Despite all samples being α-quartz, the temperature at which they induce freezing varies by around 12 ∘C for a constant active site density. We find that some quartz samples are very sensitive to ageing in both aqueous suspension and air, resulting in a loss of ice-nucleating activity, while other samples are insensitive to exposure to air and water over many months. For example, the ice-nucleation temperatures for one quartz sample shift down by ∼2 ∘C in 1 h and 12 ∘C after 16 months in water. The sensitivity to water and air is perhaps surprising, as quartz is thought of as a chemically resistant mineral, but this observation suggests that the active sites responsible for nucleation are less stable than the bulk of the mineral. We find that the quartz group of minerals is generally less active than K-feldspars by roughly 7 ∘C, although the most active quartz samples are of a similar activity to some K-feldspars with an active site density, ns(T), of 1 cm−2 at −9 ∘C. We also find that the freshly milled quartz samples are generally more active by roughly 5 ∘C than the plagioclase feldspar group of minerals and the albite end member has an intermediate activity. Using both the new and literature data, active site density parameterizations have been proposed for freshly milled quartz, K-feldspar, plagioclase and albite. Combining these parameterizations with the typical atmospheric abundance of each mineral supports previous work that suggests that K-feldspar is the most important ice-nucleating mineral in airborne mineral dust.
Journal Article
The ice-nucleating activity of African mineral dust in the Caribbean boundary layer
by
Pöhlker, Christopher
,
Murray, Benjamin J.
,
Harrison, Alexander D.
in
Aerosols
,
Atmosphere
,
Atmospheric models
2022
African mineral dust is transported many thousands of kilometres from its source regions, and, because of its ability to nucleate ice, it plays a major role in cloud glaciation around the globe. The ice-nucleating activity of desert dust is influenced by its mineralogy, which varies substantially between source regions and across particle sizes. However, in models it is often assumed that the activity (expressed as active sites per unit surface area as a function of temperature) of atmospheric mineral dust is the same everywhere on the globe. Here, we find that the ice-nucleating activity of African desert dust sampled in the summertime marine boundary layer of Barbados (July and August 2017) is substantially lower than parameterizations based on soil from specific locations in the Sahara or dust sedimented from dust storms. We conclude that the activity of dust in Barbados' boundary layer is primarily defined by the low K-feldspar content of the dust, which is around 1 %. We propose that the dust we sampled in the Caribbean was from a region in western Africa (in and around the Sahel in Mauritania and Mali), which has a much lower feldspar content than other African sources across the Sahara and Sahel.
Journal Article
Newly Identified Climatically and Environmentally Significant High-Latitude Dust Sources
2022
Dust particles from high latitudes have a potentially large local, regional, and global significance to climate and the environment as short-lived climate forcers, air pollutants, and nutrient sources. Identifying the locations of local dust sources and their emission, transport, and deposition processes is important for understanding the multiple impacts of high-latitude dust (HLD) on the Earth’s systems. Here, we identify, describe, and quantify the source intensity (SI) values, which show the potential of soil surfaces for dust emission scaled to values 0 to 1 concerning globally best productive sources, using the Global Sand and Dust Storms Source Base Map (G-SDS-SBM). This includes 64 HLD sources in our collection for the northern (Alaska, Canada, Denmark, Greenland, Iceland, Svalbard, Sweden, and Russia) and southern (Antarctica and Patagonia) high latitudes. Activity from most of these HLD sources shows seasonal character. It is estimated that high-latitude land areas with higher (SI ≥ 0.5), very high (SI ≥ 0.7), and the highest potential (SI ≥ 0.9) for dust emission cover > 1 670 000 km2 , > 560 000 km2 , and > 240 000 km2 , respectively. In the Arctic HLD region (≥ 60◦ N), land area with SI ≥ 0.5 is 5.5 % (1 035 059 km2), area with SI ≥ 0.7 is 2.3 % (440 804 km2), and area with SI ≥ 0.9 is 1.1 % (208 701 km2). Minimum SI values in the northern HLD region are about 3 orders of magnitude smaller, indicating that the dust sources of this region greatly depend on weather conditions. Our spatial dust source distribution analysis modeling results showed evidence supporting a northern HLD belt, defined as the area north of 50◦ N, with a “transitional HLD-source area” extending at latitudes 50–58◦ N in Eurasia and 50–55◦ N in Canada and a “cold HLD-source area” including areas north of 60◦ N in Eurasia and north of 58◦ N in Canada, with currently “no dust source” area between the HLD and low-latitude dust (LLD) dust belt, except for British Columbia. Using the global atmospheric transport model SILAM, we estimated that 1.0 % of the global dust emission originated from the high-latitude regions. About 57 % of the dust deposition in snow- and ice-covered Arctic regions was from HLD sources. In the southern HLD region, soil surface conditions are favorable for dust emission during the whole year. Climate change can cause a decrease in the duration of snow cover, retreat of glaciers, and an increase in drought, heatwave intensity, and frequency, leading to the increasing frequency of topsoil conditions favorable for dust emission, which increases the probability of dust storms. Our study provides a step forward to improve the representation of HLD in models and to monitor, quantify, and assess the environmental and climate significance of HLD.
Journal Article
Gaps in our understanding of ice-nucleating particle sources exposed by global simulation of the UK Earth System Model
by
Pringle, Kirsty J.
,
Murray, Benjamin J.
,
Sanchez-Marroquin, Alberto
in
Aerosols
,
Annual variations
,
Atmosphere
2025
Changes in the availability of a subset of aerosol known as ice-nucleating particles (INPs) can substantially alter cloud microphysical and radiative properties. Despite very large spatial and temporal variability in INP properties, many climate models do not currently represent the link between (i) the global distribution of aerosols and INPs and (ii) primary ice production in clouds. Here we use the UK Earth System Model to simulate the global distribution of dust, marine-sourced, and black carbon INPs suitable for immersion-mode freezing of liquid cloud droplets over an annual cycle. The model captures the overall spatial and temporal distribution of measured INP concentrations, which is strongly influenced by the world's major mineral dust source regions. A negative bias in simulated versus measured INP concentrations at higher freezing temperatures points to incorrectly defined INP properties or a missing source of INPs. We find that the ability of the model to reproduce measured INP concentrations is greatly improved by representing dust as a mixture of mineralogical and organic ice-nucleating components, as present in many soils. To improve the agreement further, we define an optimized hypothetical parameterization of dust INP activity (ns(T)) as a function of temperature with a logarithmic slope of −0.175 K−1, which is much shallower than existing parameterizations (e.g. −0.35 K−1 for the K-feldspar data of Harrison et al., 2019). The results point to a globally important role for an organic component associated with mineral dust.
Journal Article
Aircraft ice-nucleating particle and aerosol composition measurements in the western North American Arctic
by
Murray, Benjamin J.
,
Burke, Ian T.
,
McQuaid, James B.
in
Aerosol composition
,
Aerosol concentrations
,
Aerosol particles
2023
Knowledge of the temperature-dependent concentration of ice-nucleating particles (INPs) is crucial to understanding the properties of mixed-phase clouds. However, the sources, transport and removal of INPs around the globe, and particularly in the Arctic region, are poorly understood. In the Arctic winter and spring, when many local sources are covered by ice and snow, it is not clear which INP types are important. In this study, we present a new dataset of aircraft-based immersion mode INP measurements and aerosol size-resolved composition in the western North American Arctic from 11 to 21 March 2018. Aerosol samples were collected between ∼ 70 and 600 m above the surface on filters that were analysed using both a freezing droplet-based assay and scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS). The measured INP concentrations were at or close to the limit of detection, with concentrations at −20 ∘C of 1 L−1 or below. The size-resolved composition measurements indicates that the aerosol concentrations were low, dominated mostly by sea spray aerosol and mineral dust. Further analysis shows that mineral dust is important for the ice-nucleating properties of our samples, dominating over the sea spray aerosol particles in the four cases we analysed, suggesting that mineral dust is a relevant type of INP in the Alaskan springtime Arctic. Furthermore, the INP concentrations are more consistent with fertile soil dusts that have an ice-active biological component than what would be expected for the ice-active mineral K-feldspar alone. While we cannot rule out local high-latitude sources of dust, the relatively small size of the mineral dust implies that the dust was from distant sources.
Journal Article
Megacity and local contributions to regional air pollution: an aircraft case study over London
2020
In July 2017 three research flights circumnavigating the megacity of London were conducted as a part of the STANCO training school for students and early career researchers organised by EUFAR (European Facility for Airborne Research). Measurements were made from the UK's Facility for Airborne Atmospheric Measurements (FAAM) BAe-146-301 atmospheric research aircraft with the aim to sample, characterise and quantify the impact of megacity outflow pollution on air quality in the surrounding region. Conditions were extremely favourable for airborne measurements, and all three flights were able to observe clear pollution events along the flight path. A small change in wind direction provided sufficiently different air mass origins over the 2 d such that a distinct pollution plume from London, attributable marine emissions and a double-peaked dispersed area of pollution resulting from a combination of local and transported emissions were measured. We were able to analyse the effect of London emissions on air quality in the wider region and the extent to which local sources contribute to pollution events. The background air upwind of London was relatively clean during both days; concentrations of CO were 88–95 ppbv, total (measured) volatile organic compounds (VOCs) were 1.6–1.8 ppbv and NOx was 0.7–0.8 ppbv. Downwind of London, we encountered elevations in all species with CO>100 ppbv, VOCs 2.8–3.8 ppbv, CH4>2080 ppbv and NOx>4 ppbv, and peak concentrations in individual pollution events were higher still. Levels of O3 were inversely correlated with NOx during the first flight, with O3 concentrations of 37 ppbv upwind falling to ∼26 ppbv in the well-defined London plume. Total pollutant fluxes from London were estimated through a vertical plane downwind of the city. Our calculated CO2 fluxes are within the combined uncertainty of those estimated previously, but there was a greater disparity in our estimates of CH4 and CO. On the second day, winds were lighter and downwind O3 concentrations were elevated to ∼39–43 ppbv (from ∼32 to 35 ppbv upwind), reflecting the contribution of more aged pollution to the regional background. Elevations in pollutant concentrations were dispersed over a wider area than the first day, although we also encountered a number of clear transient enhancements from local sources. This series of flights demonstrated that even in a region of megacity outflow, such as the south-east of the UK, local fresh emissions and more distant UK sources of pollution can all contribute substantially to pollution events. In the highly complex atmosphere around a megacity where a high background level of pollution mixes with a variety of local sources at a range of spatial and temporal scales and atmospheric dynamics are further complicated by the urban heat island, the use of pollutant ratios to track and determine the ageing of air masses may not be valid. The individual sources must therefore all be well-characterised and constrained to understand air quality around megacities such as London. Research aircraft offer that capability through targeted sampling of specific sources and longitudinal studies monitoring trends in emission strength and profiles over time.
Journal Article
Characterisation of the filter inlet system on the FAAM BAe-146 research aircraft and its use for size-resolved aerosol composition measurements
by
Murray, Benjamin J.
,
Hedges, Duncan H. P.
,
Sanchez-Marroquin, Alberto
in
Aerosol composition
,
Aerosol particles
,
Aerosols
2019
Atmospheric aerosol particles are important for our planet's climate because they interact with radiation and clouds. Hence, having characterised methods to collect aerosol from aircraft for detailed offline analysis are valuable. However, collecting aerosol, particularly coarse-mode aerosol, onto substrates from a fast-moving aircraft is challenging and can result in both losses and enhancement in particles. Here we present the characterisation of an inlet system designed for collection of aerosol onto filters on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146-301 Atmospheric Research Aircraft. We also present an offline scanning electron microscopy (SEM) technique for quantifying both the size distribution and size-resolved composition of the collected aerosol. We use this SEM technique in parallel with online underwing optical probes in order to experimentally characterise the efficiency of the inlet system. We find that the coarse-mode aerosol is sub-isokinetically enhanced, with a peak enhancement at around 10 µm up to a factor of 2 under recommended operating conditions. Calculations show that the efficiency of collection then decreases rapidly at larger sizes. In order to minimise the isokinetic enhancement of coarse-mode aerosol, we recommend sampling with total flow rates above 50 L min−1; operating the inlet with the bypass fully open helps achieve this by increasing the flow rate through the inlet nozzle. With the inlet characterised, we also present single-particle chemical information obtained from X-ray spectroscopy analysis, which allows us to group the particles into composition categories.
Journal Article
The impact and cost-effectiveness of pneumococcal immunisation strategies for the elderly in England
2024
Pneumococcal disease, presenting as invasive pneumococcal disease (IPD) or community-acquired pneumonia (CAP) is an important cause of illness and hospitalisation in the elderly. To reduce pneumococcal burden, since 2003, 65-year-olds in England have been offered a 23-valent pneumococcal polysaccharide vaccine (PPV23). This study compares the impact and cost-effectiveness (CE) of vaccination with the existing PPV23 vaccine to the new 15-and 20-valent pneumococcal conjugate vaccines (PCV15 and PCV20), targeting adults aged 65 or 75 years old.
We developed a static Markov model for immunisation against pneumococcal disease, capturing different vaccine effectiveness and immunity waning assumptions, projecting the number of IPD/CAP cases averted over the thirty years following vaccination. Using an economic model and probabilistic sensitivity analysis we evaluated the CE of the different immunisation strategies at current vaccine list prices and the willingness-to-pay at a median threshold of £20,000/QALY and an uncertainty threshold of 90% of simulations below £30,000/QALY.
PCV20 averted more IPD and CAP cases than PCV15 or PPV23 over the thirty years following vaccination: 353(360), 145(159) and 150(174) IPD and 581(673), 259(485) and 212(235) CAP cases at a vaccination age of 65(75) under base vaccine effectiveness assumptions. At the listed prices of PCV20 and PPV23 vaccines as of May 2023, both vaccines were cost-effective when vaccinating 65- or 75-year-olds with an ICER threshold of £20,000 per QALY. To achieve the same cost-effectiveness as PPV23, the additional cost of PCV20 should be less than £44(£91) at an ICER threshold of £20,000/QALY (£30,000/QALY) if vaccination age is 65 (or £54(£103) if vaccination age is increased to 75).
We showed that both PPV23 and PCV20 were likely to be cost-effective. PCV20 was likely to avert more cases of pneumococcal disease in elderly adults in England than the current PPV23 vaccine, given input assumptions of a higher vaccine effectiveness and slower waning for PCV20.
Journal Article
Combining models to generate a consensus effective reproduction number R for the COVID-19 epidemic status in England
2024
The effective reproduction number
$ R $
was widely accepted as a key indicator during the early stages of the COVID-19 pandemic. In the UK, the
$ R $
value published on the UK Government Dashboard has been generated as a combined value from an ensemble of epidemiological models via a collaborative initiative between academia and government. In this paper, we outline this collaborative modelling approach and illustrate how, by using an established combination method, a combined
$ R $
estimate can be generated from an ensemble of epidemiological models. We analyse the
$ R $
values calculated for the period between April 2021 and December 2021, to show that this
$ R $
is robust to different model weighting methods and ensemble sizes and that using heterogeneous data sources for validation increases its robustness and reduces the biases and limitations associated with a single source of data. We discuss how
$ R $
can be generated from different data sources and show that it is a good summary indicator of the current dynamics in an epidemic.
Journal Article
Measuring and Identifying Ice-Nucleating Particles in the Atmosphere
2020
A fraction of aerosol particles known as Ice-Nucleating Particles (INPs) has the potential to trigger ice formation in supercooled liquid droplets, dramatically altering the properties of mixed-phase clouds. However, our current knowledge on the way these particles are distributed in the atmosphere is still limited. This thesis aimed to expand our understanding of the sources and concentrations of INPs in the atmosphere at various locations at mid- and high-latitudes. This was done by performing immersion mode INP and aerosol size-resolved composition measurements on board of a research aircraft in three different locations (North-Western Europe, Iceland and the Western North American Arctic). Aerosol measurements were performed on board of the FAAM BAe-146 research aircraft. Hence, I first characterised the biases of the filter inlet system available on board of this aircraft both theoretically and experimentally, providing recommendations on how to operate the system. I also implemented a methodology to study the size-resolved composition of aerosol samples collected on top of filters using Scanning Electron Microscopy with Energy Dispersive Spectroscopy (SEM-EDS). This technique has been applied in parallel with a droplet freezing assay to measure INPs as well as aerosol size-resolved composition in aerosol samples collected on board of the FAAM BAe-146 in different locations. The first area of study was North-Western Europe. The INP concentration was dominated by the presence of mineral dust at the lower end of the temperature spectrum, while an additional source (likely biological) was the main component at higher temperatures. The second area of study was Iceland, where the INP concentrations were dominated by the presence of local dust. The used methodology allowed me to derive a parameterization of the ice-nucleation ability of airborne Icelandic dust. This parameterization was combined with a global aerosol model which included the Icelandic dust emissions, showing that Icelandic dust significantly contributes to the INP population over the North Atlantic and some areas of the Arctic. The INP concentrations in the Western North American Arctic were the lowest I detected, being compatible with the limit of detection in most cases. The SEM-EDS analysed revealed that mineral dust is more important than sea spray aerosol for the INP population. Overall, across the campaigns, I observed large variability in aerosol concentration, aerosol composition and INP concentration. A part of this variability in the INPs can be explained by the presence of surface area of aerosol and dust in the samples.
Dissertation