Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer

Schulte, Ruben; Zanten, M.C. van; Rutledge, Susanna; Swart, D. P. J.; Kruit, R.J. Wichink; Krol, Maarten; Pul, W.A.J. van; Arellano, Jordi Vilà‐Guerau de

doi:10.1016/j.atmosenv.2020.118153

Cited by 13 publications

(22 citation statements)

References 52 publications

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“…Finally, we filter out the impact of boundary-layer dynamics and variations in the thermodynamic variables with our choice of analysis window, from 14:00 and 17:00 CEST. Bourndary-layer dynamics are especially relevant in the morning, when entrainment is one of the dominant processes driving the NH 3 diurnal variability (Wichink Kruit et al, 2007;Schulte et al, 2021). As shown in Fig.…”

Section: Uncertainty On the Blending-distance Estimationmentioning

confidence: 98%

“…The atmospheric ammonia budget is further governed by surface-atmosphere exchange and chemical gas-particle transformations (Schulte et al, 2021). We use a simplified, yet realistic, approach in our representation of these processes.…”

Section: Nh 3 Turbulent Dispersion In Dalesmentioning

confidence: 99%

“…methane (Shah et al, 2020;Ražnjević et al, 2021). Ammonia is highly reactive: surface-atmosphere exchange and chemical gas-aerosols transformations play an important role in the NH 3 budget (Fowler et al, 1998;Van Oss et al, 1998;Nemitz et al, 2004;aan de Brugh et al, 2013;Behera et al, 2013;Shen et al, 2016;Schulte et al, 2021). Additionally, ammonia emissions in densely agricultuural areas are released and mixed into a background concentration, a result of long range transport of NH 3 (10-100 km).…”

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confidence: 99%

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Assessing representativity of NH<sub>3</sub> measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Schulte

Zanten

Arellano

2021

Preprint

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Abstract. This study presents a fine scale simulation approach to assess the representativity of ammonia (NH3) measurements in proximity of an emission source. Close proximity to emission sources (< 5 km) can introduce a bias in regionally representative measurements of the NH3 molar fraction and flux. Measurement sites should therefore be located a significant distance from emission sources, but such requirements are poorly defined and can be difficult to meet in densely agricultural regions. This study presents a consistent criterium to assess the regional representativity of NH3 measurements in proximity of an emission source, calculating variables that quantify the NH3 plume dispersion using a series of numerical experiments at a fine resolution (20 m). Our fine scale simulation framework with explicitly resolved turbulence enables us to distinguish between the background NH3 and the emission plume, including realistic representations of NH3 deposition and chemical gas-aerosol transformations. We introduce the concept of blending-distance, based on the calculation of turbulent fluctuations, to systematically analyze the impact of the emission plume on simulated measurements, relative to this background NH3. This sensitivity analysis includes systematic experiments varying meteorological factors, emission/deposition and NH3 dependences. Considering these sensitivities, we find that NH3 measurements should be located at a minimum distance of 0.5–2.5 km and 1–3.5 km from an emission source, for NH3 molar fraction and flux measurements respectively. The simulation framework presented here can easily be adapted to local conditions and paves the way for future ammonia research at high spatio-temporal resolution.

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Section: Uncertainty On the Blending-distance Estimationmentioning

confidence: 98%

Section: Nh 3 Turbulent Dispersion In Dalesmentioning

confidence: 99%

mentioning

confidence: 99%

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Assessing representativity of NH<sub>3</sub> measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Schulte

Zanten

Arellano

2021

Preprint

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“…Sutton et al, 2009), half-hour fluxes from eddy-covariance measurements allow for investigating the mechanisms governing the surfaceatmosphere exchange on different temporal scales. For example, high temporal resolution helps to identify the bidirectional exchange of NH 3 (Nemitz et al, 2001;Zhu et al, 2015;Schulte et al, 2021) and reveals phases of net emission vs. net deposition (McGinn et al, 2016;Zöll et al, 2016;Wintjen et al, 2022). A clearer picture can be derived about the interplay of stomatal (Geßler et al, 2002) and non-stomatal pathways (Schrader et al, 2016); the exchange between soil and the atmosphere; seasonal site-specific conditions, e.g.…”

Section: Potential Applicationsmentioning

confidence: 99%

Reactive nitrogen fluxes over peatland and forest ecosystems using micrometeorological measurement techniques

Brümmer¹,

Rüffer²,

Delorme³

et al. 2022

Earth Syst. Sci. Data

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Abstract. Interactions of reactive nitrogen (Nr) compounds between the atmosphere and the earth's surface play a key role in atmospheric chemistry and in understanding nutrient cycling of terrestrial ecosystems. While continuous observations of inert greenhouse gases through micrometeorological flux measurements have become a common procedure, information about temporal dynamics and longer-term budgets of Nr compounds is still extremely limited. Within the framework of the research projects NITROSPHERE and FORESTFLUX, field campaigns were carried out to investigate the biosphere–atmosphere exchange of selected Nr compounds over different land surfaces. The aim of the campaigns was to test and establish novel measurement techniques in eddy-covariance setups for continuous determination of surface fluxes of ammonia (NH3) and total reactive nitrogen (ΣNr) using two different analytical devices. While high-frequency measurements of NH3 were conducted with a quantum cascade laser (QCL) absorption spectrometer, a custom-built converter called Total Reactive Atmospheric Nitrogen Converter (TRANC) connected and operated upstream of a chemiluminescence detector (CLD) was used for the measurement of ΣNr. As high-resolution data of Nr surface–atmosphere exchange are still scarce but highly desired for testing and validating local inferential and larger-scale models, we provide access to campaign data including concentrations, fluxes, and ancillary measurements of meteorological parameters. Campaigns (n=4) were carried out in natural (forest) and semi-natural (peatland) ecosystem types. The published datasets stress the importance of recent advancements in laser spectrometry and help improve our understanding of the temporal variability of surface–atmosphere exchange in different ecosystems, thereby providing validation opportunities for inferential models simulating the exchange of reactive nitrogen. The dataset has been placed in the Zenodo repository (https://doi.org/10.5281/zenodo.4513854; Brümmer et al., 2022) and contains individual data files for each campaign.

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“…(i) During day, agricultural practices and animal activity (Aarnink et al., 1996) are enhanced. (ii) NH 3 emissions from plants and soils increase during the day due to meteorological factors (Schulte et al., 2020). Emissions exhibit in particular an up to exponential increase with temperature (Ernst & Massey, 1960; Schjoerring et al., 1998; Sutton, Reis, et al., 2013; Tevlin & Murphy, 2019; L. Zhang et al., 2010), making it an important driver both for the seasonal and the diel emission cycle.…”

Section: Diel Cyclementioning

confidence: 99%

The Diel Cycle of NH₃ Observed From the FY‐4A Geostationary Interferometric Infrared Sounder (GIIRS)

Clarisse

Damme

Hurtmans

et al. 2021

Geophysical Research Letters

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As the atmosphere's primary base and one of the main reactive nitrogen compounds, ammonia (NH 3 ) plays a key role in our atmosphere and the global nitrogen cycle (Fowler et al., 2013). Emitted in excess, NH 3 can lead to a dramatic loss of biodiversity and deterioration of water, soil and air quality (Bauer et al., 2016;Bobbink et al., 2010;Sutton, Bleeker, et al., 2013). Unlike other primary gaseous pollutants, such as the acidifying NO x and SO 2 (Aas et al., 2019;Georgoulias et al., 2019), concentrations of NH 3 are steadily increasing in large parts of the world (Sutton et al., 2020;Van Damme et al., 2021). NH 3 has stayed under the radar for long, partially as a result of the historic dearth of measurements. Fortunately, thanks to the availability of new and cheaper techniques, large measurement networks of ground-based stations are gradually put in place (Nair & Yu, 2020;Viatte et al., 2021). In addition, since over a decade, satellites equipped with high-resolution infrared spectrometers offer an unprecedented temporal and spatial sampling of the global NH 3 distributions, which has led to important progress in our understanding of its local to global emission and deposition fluxes and how these are evolving over time (e.g.,

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Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer

Cited by 13 publications

References 52 publications

Assessing representativity of NH<sub>3</sub> measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Assessing representativity of NH<sub>3</sub> measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Reactive nitrogen fluxes over peatland and forest ecosystems using micrometeorological measurement techniques

The Diel Cycle of NH₃ Observed From the FY‐4A Geostationary Interferometric Infrared Sounder (GIIRS)

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Unraveling the diurnal atmospheric ammonia budget of a prototypical convective boundary layer

Cited by 13 publications

References 52 publications

Assessing representativity of NH&lt;sub&gt;3&lt;/sub&gt; measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Assessing representativity of NH&lt;sub&gt;3&lt;/sub&gt; measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Reactive nitrogen fluxes over peatland and forest ecosystems using micrometeorological measurement techniques

The Diel Cycle of NH3 Observed From the FY‐4A Geostationary Interferometric Infrared Sounder (GIIRS)

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Assessing representativity of NH<sub>3</sub> measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

Assessing representativity of NH<sub>3</sub> measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source

The Diel Cycle of NH₃ Observed From the FY‐4A Geostationary Interferometric Infrared Sounder (GIIRS)