Measurement report: Photochemical production and loss rates of formaldehyde and ozone across Europe

Various atmospheric sources and sinks regulate the abundance of tropospheric formaldehyde (HCHO), which is an important trace gas impacting the HOx (≡ HO2 + OH) budget and the concentration of ozone (O3). In this study, we present the formation and destruction terms of ambient HCHO and O3 calculated from in situ observations of various atmospheric trace gases measured at three different sites across Europe during summertime. These include a coastal site in Cyprus, in the scope of the Cyprus Photochemistry Experiment (CYPHEX) in 2014, a mountain site in southern Germany, as part of the Hohenpeißenberg Photochemistry Experiment (HOPE) in 2012, and a forested site in Finland, where measurements were performed during the Hyytiälä United Measurements of Photochemistry and Particles (HUMPPA) campaign in 2010. We show that, at all three sites, formaldehyde production from the OH oxidation of methane (CH4), acetaldehyde (CH3CHO), isoprene (C5H8) and methanol (CH3OH) can almost completely balance the observed loss via photolysis, OH oxidation and dry deposition. Ozone chemistry is clearly controlled by nitrogen oxides (NOx ≡ NO + NO2) that include O3 production from NO2 photolysis and O3 loss via the reaction with NO. Finally, we use the HCHO budget calculations to determine whether net ozone production is limited by the availability of VOCs (volatile organic compounds; VOC-limited regime) or NOx (NOx-limited regime). At the mountain site in Germany, O3 production is VOC limited, whereas it is NOx limited at the coastal site in Cyprus. The forested site in Finland is in the transition regime.

Measurement report: New particle formation characteristics at an urban and a mountain station in northern China

Atmospheric new particle formation (NPF) events have attracted increasing attention for their contribution to the global aerosol number budget and therefore their effects on climate, air quality and human health. NPF events are regarded as a regional phenomenon, occurring over a large area. Most observations of NPF events in Beijing and its vicinity were conducted in populated areas, whereas observations of NPF events on mountaintops with low anthropogenic emissions are still rare in China. The spatial variation of NPF event intensity has not been investigated in detail by incorporating both urban areas and mountain measurements in Beijing. Here, we provide NPF event characteristics in summer 2018 and 2019 at urban Beijing and a comparison of NPF event characteristics – NPF event frequency, formation rate and growth rate – by comparing an urban Beijing site and a background mountain site separated by ∼80 km from 14 June to 14 July 2019, as well as giving insights into the connection between both locations. During parallel measurements at urban Beijing and mountain background areas, although the median condensation sink during the first 2 h of the common NPF events was around 0.01 s−1 at both sites, there were notable differences in formation rates between the two locations (median of 5.42 cm−3 s−1 at the urban site and 1.13 cm−3 s−1 at the mountain site during the first 2 h of common NPF events). In addition, the growth rates in the 7–15 nm range for common NPF events at the urban site (median of 7.6 nm h−1) were slightly higher than those at the mountain site (median of 6.5 nm h−1). To understand whether the observed events were connected, we compared air mass trajectories as well as meteorological conditions at both stations. Favorable conditions for the occurrence of regional NPF events were largely affected by air mass transport. Overall, our results demonstrate a clear inhomogeneity of regional NPF within a distance of ∼100 km, possibly due to the discretely distributed emission sources.

Measurement report: Photochemical production and loss rates of formaldehyde and ozone across Europe

Various atmospheric sources and sinks regulate the abundance of tropospheric formaldehyde (HCHO) which is an important trace gas impacting the HOx (≡ HO2 + OH) budget and the concentration of ozone (O3). In this study, we present the formation and destruction terms of ambient HCHO and O3 calculated from in-situ observations of various atmospheric trace gases measured at three different sites across Europe during summer time. These include a coastal site in Cyprus in the scope of the Cyprus Photochemistry Experiment (CYPHEX) in 2014, a mountain site in Southern Germany as part of the Hohenpeißenberg Photochemistry Experiment (HOPE) in 2012 and a forested site in Finland where measurements were performed during the Hyytiälä United Measurements of Photochemistry and Particles (HUMPPA) campaign in 2010. We show that at all three sites formaldehyde production from the OH oxidation of methane (CH4), acetaldehyde (CH3CHO), isoprene (C5H8) and methanol (CH3OH) can almost completely balance the observed loss via photolysis, OH oxidation and dry deposition. Ozone chemistry is clearly controlled by nitrogen oxides (NOx ≡ NO + NO2) that includes O3 production from NO2 photolysis and O3 loss via the reaction with NO. Finally, we use the HCHO budget calculations to determine whether net ozone production is limited by the availability of VOCs (VOC limited regime) or NOx (NOx limited regime). At the mountain site in Germany O3 production is VOC limited, whereas it is NOx limited at the coastal site in Cyprus. The forested site in Finland is in the transition regime.

Measurement Report: New particle formation characteristics at an urban and a mountain station in Northern China

Atmospheric new particle formation (NPF) events have attracted increasing attention for their contribution to the global aerosol number budget, and therefore their effects on climate, air quality, and human health. NPF events are regarded as a regional phenomenon, occurring over a large area. However, the spatial variation of NPF intensity has not been investigated in detail by incorporating both urban and regional measurements. Urban environments have more heterogeneous and freshly emitted NPF precursors as compared to environments with less anthropogenic activity. Here, we provide a comparison of NPF event characteristics – NPF event frequency, particle formation rate, and growth rate – by comparing an urban Beijing site and a background mountain site separated by ~80 km from June 14 to July 14, 2019 as well as give insights into the connection between both locations. During the measurement period, 12 and 13 NPF events were observed at the urban and background mountain sites, respectively, with 9 NPF events observed on the same day at both sites. Although the median condensation sink during the first two hours of the common NPF events was around 0.01 s−1 at both sites, there were notable differences in particle formation rates between the two locations (median of 5.42 cm−3 s−1 at the urban site and 1.13 cm−3 s−1 at the mountain site during the first two hours of common NPF events). Yet, the particle growth rates in the 7–15 nm range for common NPF events were comparable (median of 7.6 nm.h−1 at the urban site and 6.5 nm.h−1 at the mountain site as median values). To understand whether the observed events were connected, we compared air mass trajectories as well as meteorological conditions at both stations. Favorable conditions for the occurrence of regional NPF events were largely affected by air mass transport. Overall, our results demonstrate a clear inhomogeneity of regional NPF within a distance of ~100 km, which should be considered in regional-scale aerosol models when estimating the budget of aerosol load and cloud condensation nuclei.

Influence of NPF events on the CCN concentration at a high-altitude site in southern Europe

<p>The Cloud Condensation Nuclei (CCN) budget, the aerosol particles population that could become cloud droplets, can be influenced by primary aerosol particles emitted by different sources (anthropogenic or biogenic) or by secondary particles that have undergone growth processes or chemical transformations. Aerosol particles originated by nucleation of precursor gases in the atmosphere have been identified as an important source of CCN particles. The influence of New Particle Formation (NPF) events to CCN concentrations is highly dependent on the environment where it takes place. Specifically, the study of the influence of NPF events on CCN concentration at high-altitude sites, where atmospheric conditions favor the formation of clouds, is a very interesting scientific goal.</p><p> </p><p>This study presents CCN measurements combined with aerosol size distribution at a high-altitude station in the South East of Spain: a remote high mountain site (Sierra Nevada; SNS, 2500 m a.s.l.). Due to its high altitude, the aerosol particles over SNS station are often representative of pristine free troposphere conditions, especially in winter and nighttime. During summer, SNS station is frequently influenced by transport of pollutants from Granada city to Sierra Nevada station as a result of mixing layer growth and the activation of the mountain-valley breeze phenomenon as well as by NPF events at midday (De Arruda Moreira et al., 2019; Casquero-Vera et al., 2020).</p><p> </p><p>In this study, we analyze the influence of NPF events to CCN concentrations during summer 2019 at the SNS high-altitude station. The study period (from June to August of 2019) was characterized by 67 NPF events, 16 undefined events and 13 non-events days. Following Rose et al. (2017) criteria, only those NPF events referred as type I, i.e. with clear particle growth from smallest sizes, were selected to investigate the contribution of NPF events on CCN concentrations. In this sense, we selected the 15 clearest NPF events for this analysis.</p><p> </p><p>Results show clear differences in the diurnal evolution of CCN concentration between NPF event and non-event days, demonstrating the large influence of NPF to CCN concentrations, especially at high supersaturations (Rejano et al., 2021). NPF events have been estimated to increase the CCN concentrations by 175% at SS=0.5%, evidencing NPF events as one of the major CCN source at this mountain site</p><p> </p><p> </p><p><strong>Acknowledgments</strong>: This work was supported by the European Union's Horizon 2020 research and innovation programme through project ACTRIS 2 (grant agreement No 654109), by the Spanish Ministry of Economy and Competitiveness through projects CGL2016-81092-R, CGL2017-90884-REDT and RTI2018-101154-A-I00 and by University of Granada Plan Propio through Visiting Scholars program. The Spanish Ministry of Universities funds Fernando Rejano under the predoctoral program FPU (FPU19/05340).</p><p> </p><p><strong>References</strong></p><p>Casquero-Vera, et al. (2020) Atmos. Chem. Phys. <strong>20, </strong>14253–14271.</p><p>De Arruda Moreira et al. (2019) Atmos. Chem. Phys. <strong>19</strong>, 1263-1280.</p><p>Rejano et al. (2021) Sci. Tot Envi., <strong>762</strong>, 143100.</p><p>Rose et al. (2017) Atmos. Chem. Phys. <strong>17</strong>, 1529-1541.</p><p>tract HTML here.</p>