Effects of various meteorological conditions and spatial emission resolutions on the ozone concentration & ROG/NO_x limitation in the Milan area (I)

International audienceThe three-dimensional photochemical model UAM-V is used to investigate the effects of various meteorological conditions and of the coarseness of emission inventories on the ozone concentration and ROG/NOx limitation of the ozone production in the Po Basin in the northern part of Italy. As a base case, the high ozone episode with up to 200 ppb on 13 May 1998 was modelled and previously thoroughly evaluated with measurements gained during a large field experiment. The performed variations in meteorology are applied to mixing height, air temperature, specific humidity and wind speed. Three coarser emission inventories are obtained by resampling from 3×3 km2 up to 54×54 km2 emission grids. The model results show that changes in meteorological input files have the largest effect on peak ozone. In the modelled ozone plume a slope of 10.1 ppb ozone/°C and in Milan of 2.8 ppb ozone/°C were found. The net ozone formation in northern Italy is more strongly temperature than humidity dependent, while the humidity is very important for the ROG/NOx limitation of the ozone production. For each of the meteorological variations (e.g. doubling the mixing height), the modelled ozone plume remains ROG limited for this case. A strong change towards NOx sensitivity in the ROG limited areas is only found if much coarser emission inventories were applied. Increasing ROG limited areas with increasing wind speed are found, because the ROG limited ozone chemistry induced by point sources is spread over a larger area. Simulations without point sources tend to increase the NOx limited areas

Changes in ozone and PM2.5 in Europe during the period of 1990-2030 : Role of reductions in land and ship emissions

Air pollution is among the top threats to human health and ecosystems despite the substantial decrease in anthropogenic emissions. Meanwhile, the role of ship emissions on air quality is becoming increasingly important with the growing maritime transport and less strict regulations. In this study, we modeled the air quality in Europe between 1990 and 2030 with ten-year intervals, using the regional air quality model CAMx version 6.50, to investigate the changes in the past (1990-2010) as well as the effects of different land and ship emission scenarios in the future (2020,2030). The modeled mean ozone levels decreased slightly during the first decade but then started increasing again especially in polluted areas. Results from the future scenarios suggest that by 2030 the peak ozone would decrease, leading to a decrease in the days exceeding the maximum daily 8-h average ozone (MDA8) limit values (60 ppb) by 51% in southern Europe relative to 1990. The model results show a decrease of 56% (6.3 mu g m(-3)) in PM2.5 concentrations from 1990 to 2030 under current legislation, mostly due to a large drop in sulfate (representing up to 44% of the total PM2.5 decrease during 1990-2000) while nitrate concentrations were predicted to go down with an increasing rate (10% of total PM2.5 decrease during 1990-2000 while 36% during 2020-2030). The ship emissions if reduced according to the maximum technically feasible reduction (MTFR) scenario were predicted to contribute up to 19% of the decrease in the PM2.5 concentrations over land between 2010 and 2030. Ship emission reductions according to the MTFR scenario would lead to a decrease in the days with MDA8 exceeding EU limits by 24-28% (10-14 days) around the coastal regions. The results obtained in our study show the increasing importance of ship emission reductions, after a relatively large decrease in land emissions was achieved in Europe. (c) 2020 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).Peer reviewe

AEROSOL MEASUREMENTS IN THE RHINE VALLEY DURING FOEHN – ANOTHER FORM PERSPECTIVE

While the main focus of the MAP subproject FORM (Foehn in the Rhine Valley during MAP) was on atmospheric dynamics, numerous measurements of chemical constituents of the atmosphere have been performed with various instruments on different platforms. Aerosol measurements have been obtained with routinely operated conventional surface stations, in-situ airborne particle counters and a backscatter lidar. For the MAP SOP it was found that near-surface aerosol concentrations are reduced by the foehn, i.e. they are lowest at the day after the foehn event, especially in the late fall when the valley inversion becomes stronger. A case study for 2 Oct 1999 (IOP 5) reveals considerable spatial variability in aerosol concentrations and shows interactions of the aerosols with the humidity field

Non-linear photochemical pathways in laser induced atmospheric aerosol formation

We measured the chemical composition and the size distribution of aerosols generated by femtosecond-Terawatt laser pulses in the atmosphere using an aerosol mass spectrometer (AMS). We show that nitric acid condenses in the form of ammonium nitrate, and that oxidized volatile organics also contribute to particle growth. These two components account for two thirds and one third, respectively, of the dry laser-condensed mass. They appear in two different modes centred at 380 nm and 150 nm. The number concentration of particles between 25 and 300 nm increases by a factor of 15. Pre-existing water droplets strongly increase the oxidative properties of the laser-activated atmosphere, substantially enhancing the condensation of organics under laser illumination.Comment: 19 pages, 5 figure

Source apportionment of submicron organic aerosols at an urban site by linear unmixing of aerosol mass spectra

International audienceSubmicron ambient aerosol was characterized in summer 2005 at an urban background site in Zurich, Switzerland, during a three-week measurement campaign. Highly time-resolved samples of non-refractory aerosol components were analyzed with an Aerodyne aerosol mass spectrometer (AMS). Positive matrix factorization (PMF) was used for the first time for AMS data to identify the main components of the total organic aerosol and their sources. The PMF retrieved factors were compared to measured reference mass spectra and were correlated with tracer species of the aerosol and gas phase measurements from collocated instruments. Six factors were found to explain virtually all variance in the data and could be assigned either to sources or to aerosol components such as oxygenated organic aerosol (OOA). Our analysis suggests that at the measurement site only a small (1 originates from freshly emitted fossil fuel combustion. Other primary sources identified to be of similar or even higher importance are charbroiling (10?15%) and wood burning (~10%), along with a minor source interpreted to be influenced by food cooking (6%). The fraction of all identified primary sources is considered as primary organic aerosol (POA). This interpretation is supported by calculated ratios of the modelled POA and measured primary pollutants such as elemental carbon (EC), NOx, and CO, which are in good agreement to literature values. A high fraction (60?69%) of the measured organic aerosol mass is OOA which is interpreted mostly as secondary organic aerosol (SOA). This oxygenated organic aerosol can be separated into a highly aged fraction, OOA I, (40?50%) with low volatility and a mass spectrum similar to fulvic acid, and a more volatile and probably less processed fraction, OOA II (on average 20%). This is the first publication of a multiple component analysis technique to AMS organic spectral data and also the first report of the OOA II component

Surface ozone at the Caucasian site Kislovodsk High Mountain Station and the Swiss Alpine site Jungfaujoch: data analysis and trends (1990–2006)

Long-term ozone measurements of two background mountain sites, namely the Kislovodsk High Mountain Station in Caucasus, Russia (KHMS, 43.70° N, 42.70° E, 2070 m a.s.l.) and the Jungfraujoch in Switzerland (JFJ, 46.55° N, 7.98° E, 3580 m a.s.l.) are compared. Despite of more than 1.5 km altitude difference ozone mixing ratios are comparable at JFJ an KHMS in the beginning of measurements (1990–1993) while the annually averaged levels at JFJ are around 15 ppb higher than the ones at KHMS for the most recent years (1997–2006). The seasonal cycle of the surface ozone mixing ratios is characterized by a double spring-summer maximum at both sites with a spring one being more pronounced for the air masses with the longest contact with the upper free troposphere and stratosphere. Ozone mixing ratio increased at JFJ but decreased at KHMS for the period 1990–2006. Trends are more pronounced for the 1990s (+0.73±0.20 ppb/year at JFJ and −0.91±0.17 ppb/year at KHMS for the period 1991–2001) in comparison with the later years (+0.04±0.21 ppb/year at JFJ and −0.37±0.14 ppb/year at KHMS for the period 1997–2006). Trends show a distinct seasonality, which is different for the different periods. To investigate possible reasons for this remarkable trends difference 3-D trajectories using LAGRANTO trajectory model are used. Effects of horizontal and vertical transport on ozone trends are considered. No substantial systematic changes in the transport patterns were detected which could lead to strong changes in the trend magnitude between 1991–2001 and 1997–2006. The geographical position of the sites relative to the main topographic features and emission sources as well as distance from the coast are interpreted to be among the main reasons for the opposite surface ozone trends. During the 90s the JFJ trend reflects increase of the ozone in the upper free troposphere/lower stratosphere, while KHMS is not sensitive to this change or even showing the opposite tendency. The analysis provided evidence for a stronger influence of processes in the lower troposphere, in particular the dramatic emission decrease in the earlier 1990s in former USSR and emissions regulations in Western Europe on the surface ozone trend at KHMS.ISSN:1680-7375ISSN:1680-736

Modeling the effect of reduced traffic due to COVID-19 measures on air quality using a chemical transport model : Impacts on the Po Valley and the Swiss Plateau regions

Publisher Copyright: © 2021 The Author(s).The spread of COVID-19 has posed serious challenges for the global communities. To reduce the circulation of the infection, governmental bodies have imposed different lockdown measures at various levels of complexity and duration. As a result, a substantial reduction in mobility might have important, yet unknown, implications for air quality. In this study, we applied the Comprehensive Air quality Model with eXtensions (CAMx) to investigate potential changes in air quality and its chemical composition over northern Italy and Switzerland during periods when lockdown measures were enforced. Our results indicated that lockdown measures reduced nitrogen dioxide (NO2) air concentrations by up to 46% and 25% in the Po Valley and Swiss Plateau regions, respectively, whereas fine particulate matter (PM2.5) air concentrations were reduced only by up to 10% and 6%. This highlights the importance of other emission categories other than traffic for the total PM2.5 levels. The analysis of the PM2.5 components indicated that elemental carbon (EC) and particulate nitrate (NO3 -) were the species most affected by the lockdown measures, whereas a mild increase in the secondary organic aerosol (SOA) concentrations occurred in the Po Valley, and specifically over the metropolitan area of Milan. Our results indicated that an increase in the oxidation capacity of the atmosphere, i.e. in the cOH and cNO3 radicals, was mainly responsible for the mild increase in SOA concentrations.Peer reviewe

Quantitative sampling and analysis of trace elements in atmospheric aerosols: impactor characterization and Synchrotron-XRF mass calibration.

he presented work is partly funded by theSwiss Federal Roads Office (ASTRA), the Swiss Federal Office forthe Environment (BAFU) and a post-doc contract sponsored by theSpanish Ministry of Science and Innovation (MICINN). Parts ofthe work were performed at the Swiss Light Source, Paul ScherrerInstitut, Villigen, Switzerland.We thank Andreas Jaggi fortechnical support at the beamline X05DA. Portions of this researchwere carried out at the light source facility DORIS III at HASY-LAB/DESY. DESY is a member of the Helmholtz Association(HGF)

Chemical characterization of secondary organic aerosol at a rural site in the southeastern US: insights from simultaneous high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and FIGAERO chemical ionization mass spectrometer (CIMS) measurements

The formation and evolution of secondary organic aerosol (SOA) were investigated at Yorkville, GA, in late summer (mid-August to mid-October 2016). The organic aerosol (OA) composition was measured using two online mass spectrometry instruments, the high-resolution time-of-flight aerosol mass spectrometer (AMS) and the Filter Inlet for Gases and AEROsols coupled to a high-resolution time-of-flight iodide-adduct chemical ionization mass spectrometer (FIGAERO-CIMS). Through analysis of speciated organics data from FIGAERO-CIMS and factorization analysis of data obtained from both instruments, we observed notable SOA formation from isoprene and monoterpenes during both day and night. Specifically, in addition to isoprene epoxydiol (IEPOX) uptake, we identified isoprene SOA formation from non-IEPOX pathways and isoprene organic nitrate formation via photooxidation in the presence of NO_x and nitrate radical oxidation. Monoterpenes were found to be the most important SOA precursors at night. We observed significant contributions from highly oxidized acid-like compounds to the aged OA factor from FIGAERO-CIMS. Taken together, our results showed that FIGAERO-CIMS measurements are highly complementary to the extensively used AMS factorization analysis, and together they provide more comprehensive insights into OA sources and composition