scholarly journals Sources of uncertainty in eddy covariance ozone flux measurements made by dry chemiluminescence fast response analysers

2009 ◽  
Vol 2 (5) ◽  
pp. 2241-2280 ◽  
Author(s):  
J. B. A. Muller ◽  
C. J. Percival ◽  
M. W. Gallagher ◽  
D. Fowler ◽  
M. Coyle ◽  
...  

Abstract. Eddy covariance ozone flux measurements are the most direct way to estimate ozone removal near the surface. Over vegetated surfaces, high quality ozone fluxes are required to probe the underlying processes for which it is necessary to separate the flux into the components of stomatal and non-stomatal deposition. Detailed knowledge of the processes that control non-stomatal deposition is limited and more accurate ozone flux measurements are needed to quantify this component of the deposited flux. We present a systematic intercomparison study of eddy covariance ozone flux measurements made using two fast response dry chemiluminescence analysers. Ozone deposition was measured over a well characterised managed grassland near Edinburgh, Scotland, during August 2007. A data quality control procedure specific to these analysers is introduced. Absolute ozone fluxes were calculated based on the relative signals of the dry chemiluminescence analysers using three different calibration methods and the results are compared for both analysers. It is shown that the error in the fitted parameters required for the flux calculations provides a substantial source of uncertainty in the fluxes. The choice of the calculation method itself can also constitute an uncertainty in the flux as the calculated fluxes by the three methods do not agree within error at all times. This finding highlights the need for a consistent and rigorous approach for comparable data-sets, such as e.g. in flux networks. Ozone fluxes calculated by one of the methods were then used to compare the two analysers in more detail. This systematic analyser comparison reveals half-hourly flux values differing by up to a factor of two at times with the difference in mean hourly flux ranging from 0 to 23% with an error in the mean daily flux of ±12%. The comparison of analysers shows that the agreement in fluxes is excellent for some days but that there is an underlying uncertainty as a result of variable analyser performance and/or non-linear behaviour of disc sensitivity.

2010 ◽  
Vol 3 (1) ◽  
pp. 163-176 ◽  
Author(s):  
J. B. A. Muller ◽  
C. J. Percival ◽  
M. W. Gallagher ◽  
D. Fowler ◽  
M. Coyle ◽  
...  

Abstract. We present a systematic intercomparison study of eddy covariance ozone flux measurements made using two fast response dry chemiluminescence analysers. Ozone deposition was measured over a well characterised managed grassland near Edinburgh, Scotland, during August 2007. A data quality control procedure specific to these analysers is introduced. Absolute ozone fluxes were calculated based on the relative signals of the dry chemiluminescence analysers using three different methods and the results are compared for both analysers. It is shown that the error in the fitted analyser calibration parameters required for the flux calculations provides a substantial source of uncertainty in the fluxes. The choice of the calculation method itself can also constitute an uncertainty in the flux as the calculated fluxes by the three methods do not agree within error at all times. This finding highlights the need for a consistent and rigorous approach for comparable datasets, such as e.g. in flux networks. Ozone fluxes calculated by one of the methods were then used to compare the two analysers in more detail. This systematic analyser comparison reveals half-hourly flux values differing by up to a factor of two at times with the difference in mean hourly flux ranging from 0 to 23% with an error in the mean daily flux of ± 12%. The comparison of analysers shows that the agreement in fluxes is excellent for some days but that there is an underlying uncertainty as a result of variable analyser performance and/or non-linear sensitivity.


2010 ◽  
Vol 3 (4) ◽  
pp. 2961-2993 ◽  
Author(s):  
B. Tuzson ◽  
R. V. Hiller ◽  
K. Zeyer ◽  
W. Eugster ◽  
A. Neftel ◽  
...  

Abstract. Fast response optical analyzers based on laser absorption spectroscopy are the preferred tools to measure field-scale mixing ratios and fluxes of a range of trace gases. Several state-of-the-art instruments have become commercially available and are gaining in popularity. This paper aims for a critical field evaluation and intercomparison of two compact, cryogen-free and fast response instruments: a quantum cascade laser based absorption spectrometer from Aerodyne Research, Inc., and an off-axis integrated cavity output spectrometer from Los Gatos Research, Inc. In this paper, both analyzers are characterized with respect to precision, accuracy, response time and also their sensitivity to water vapour. The instruments were tested in a field campaign to assess their behaviour under various meteorological conditions. The instrument's suitability for eddy covariance flux measurements was evaluated by applying an artificial flux of CH4 generated above a managed grassland with otherwise very low methane flux. This allowed an independent verification of the flux measurements accuracy, including the overall eddy covariance setup and data treatment. The retrieved fluxes were in good agreement with the known artificial emission flux, which is more than satisfactory, given that the analyzers were attached to separate sonic anemometers placed on individual eddy towers with different data acquisition systems but similar data treatment that are specific to the best practice used by the involved research teams.


2012 ◽  
Vol 9 (11) ◽  
pp. 4247-4261 ◽  
Author(s):  
C. Ammann ◽  
V. Wolff ◽  
O. Marx ◽  
C. Brümmer ◽  
A. Neftel

Abstract. The (net) exchange of reactive nitrogen (Nr) with the atmosphere is an important driver for ecosystem productivity and greenhouse gas exchange. The exchange of airborne Nr includes various trace compounds that usually require different specific measurement techniques, and up to now fast response instruments suitable for eddy covariance measurements are only available for few of these compounds. Here we present eddy covariance flux measurements with a recently introduced converter (TRANC) for the sum of all Nr compounds (∑Nr). Measurements were performed over a managed grassland field with phases of net emission and net deposition of ∑Nr and alternating dominance of oxidized (NOX) and reduced species (NH3). Spectral analysis of the eddy covariance data exhibited the existence of covariance function peaks at a reasonable time lag related to the sampling tube residence time under stationary conditions. Using ogive analysis, the high-frequency damping was quantified to 19%–26% for a low measurement height of 1.2 m and to about 10% for 4.8 m measurement height. ∑Nr concentrations and fluxes were compared to parallel NO and NO2 measurements by dynamic chambers and NH3 measurements by the aerodynamic gradient technique. The average concentration results indicate that the main compounds NO2 and NH3 were converted by the TRANC system with an efficiency of near 100%. With an optimised sample inlet also the fluxes of these compounds were recovered reasonably well including net deposition and net emission phases. The study shows that the TRANC system is suitable for fast response measurements of oxidized and reduced nitrogen compounds and can be used for continuous eddy covariance flux measurements of total reactive nitrogen.


2019 ◽  
Author(s):  
Lukas Siebicke ◽  
Anas Emad

Abstract. Micrometeorological methods to quantify fluxes of atmospheric constituents are key to understanding and managing the impact of land surface sources and sinks on air quality and atmospheric composition. Important greenhouse gases are water vapor, carbon dioxide, methane, and nitrous oxide. Further important atmospheric constituents are aerosols which impact air quality and cloud formation, and volatile organic compounds. Many atmospheric constituents therefore critically affect the health of ecosystems, and humans as well as climate. The micrometeorological eddy covariance (EC) method has evolved as the method-of-choice for CO2 and water vapor flux measurements using fast-response gas analyzers. While the EC method has also been used to measure other atmospheric constituents including methane, nitrous oxide, and ozone, the often relatively small fluxes of these constituents over ecosystems are much more challenging to measure by eddy covariance than CO2 and water vapor fluxes. For many further atmospheric constituents, eddy covariance is not an option due to the lack of sufficiently accurate and fast-response gas analyzers. Therefore, alternative flux measurement methods are required for the observation of atmospheric constituent fluxes for which no fast-response gas analyzers exist or which require more accurate measurements. True eddy accumulation (TEA) is a direct flux measurement technique capable of using slow-response gas analyzers. Unlike its more frequently used derivative, known as the relaxed eddy accumulation (REA) method, TEA does not require the use of proxies and is therefore superior to the indirect REA method. The true eddy accumulation method is by design ideally suited for measuring a wide range of trace gases and other conserved constituents transported with the air. This is because TEA obtains whole air samples and is, in combination with constituent-specific fast or slow analyzers, a universal method for conserved scalars. Despite the recognized value of the method, true eddy accumulation flux measurements remained very challenging to perform as they require fast and dynamic modulation of the air sampling mass flow rate proportional to the magnitude of the instantaneous vertical wind velocity. Appropriate techniques for dynamic mass flow control have long been unavailable, preventing the unlocking of the TEA method's potential for more than 40 years. Recently, a new dynamic and accurate mass flow controller which can resolve turbulence at a frequency of 10 Hz and higher has been developed by the author. This study presents the proof-of-concept that practical true eddy accumulation trace gas flux measurements are possible today using dynamic mass flow control, advanced real-time processing of wind measurements, and fully automatic gas handling. We describe setup and methods of the TEA and EC reference flux measurements. The experiment was conducted over grassland and comprised seven days of continuous flux measurements at 30-min flux integration intervals. The results show that fluxes obtained by TEA compared favourably to EC reference flux measurements with coefficients of determination of up to 86 % and a slope of 0.98. We present a quantitative analysis of uncertainties of the mass flow control system, the gas analyzer and gas handling system and their impact on trace gas flux uncertainty, the impact of different approaches to coordinate rotation and uncertainties of vertical wind velocity measurements. Challenges of TEA are highlighted and solutions presented. The current results are put into context of previous works. Finally, based on the current successful proof-of-concept, we suggest specific improvements towards long-term and reliable true eddy accumulation flux measurements.


2014 ◽  
Vol 14 (14) ◽  
pp. 20417-20460 ◽  
Author(s):  
H. Huang ◽  
J. Wang ◽  
D. Hui ◽  
D. R. Miller ◽  
S. Bhattarai ◽  
...  

Abstract. Increases in observed atmospheric concentrations of the long-lived greenhouse gas, nitrous oxide (N2O), have been well documented. However, information on event-related instantaneous emissions during fertilizer applications is lacking. With the development of fast-response N2O analyzers, the eddy covariance (EC) technique can be used to gather instantaneous measurements of N2O concentrations to quantify the exchange of nitrogen between the soil and atmosphere. The objectives of this study were to evaluate the performance of a new EC system, to measure the N2O flux with the system, and finally to examine relationships of the N2O flux with soil temperature, soil moisture, precipitation, and fertilization events. We assembled an EC system that included a sonic anemometer and a fast-response N2O analyzer (quantum cascade laser spectrometer) in a cornfield in Nolensville, Tennessee during the 2012 corn growing season (4 April–8 August). Fertilizer amounts totaling 217 kg N ha−1 were applied to the experimental site. The precision of the instrument was 0.066 ppbv for 10 Hz measurements. The seasonal mean detection limit of the N2O flux measurements was 2.10 ng N m−2 s−1. This EC system can be used to provide reliable N2O flux measurements. The cumulative emitted N2O for the entire growing season was 6.87 kg N2O-N ha−1. The 30 min average N2O emissions ranged from 0 to 11 100 μg N2O{-}N m−2 h−1 (mean = 257.5, standard deviation = 817.7). Average daytime emissions were much higher than night emissions (278.8 ± 865.8 vs. 100.0 ± 210.0 μg N2O-N m−2 h−1). Seasonal fluxes were highly dependent on soil moisture rather than soil temperature, although the diurnal flux was positively related to soil temperature. This study was one of the few experiments that continuously measured instantaneous, high-frequency N2O emissions in crop fields over a growing season of more than 100 days.


2012 ◽  
Vol 9 (6) ◽  
pp. 6857-6898 ◽  
Author(s):  
C. Ammann ◽  
V. Wolff ◽  
O. Marx ◽  
C. Brümmer ◽  
A. Neftel

Abstract. The (net) exchange of reactive nitrogen (Nr) with the atmosphere is an important driver for ecosystem productivity and greenhouse gas exchange. The exchange of airborne Nr includes various trace compounds that usually require different specific measurement techniques, and up to now fast response instruments suitable for eddy covariance measurements are only available for few of these compounds. Here we present eddy covariance flux measurements with a recently introduced converter (TRANC) for the sum of all Nr compounds (∑Nr). Measurements were performed over a managed grassland field with phases of net emission and net deposition of ∑Nr and alternating dominance of oxidized (NOx) and reduced species (NH3). Spectral analysis of the eddy covariance data exhibited the existence of covariance function peaks at a reasonable time lag related to the sampling tube residence time under stationary conditions. Using ogive analysis, the high-frequency damping was quantified to 19–26% for a low measurement height of 1.2 m and to about 10% for 4.8 m measurement height. ∑Nr concentrations and fluxes were compared to parallel NO and NO2 measurements by dynamic chambers and NH3 measurements by the aerodynamic gradient technique. The average concentration results indicate that close-to-full conversion of the main compounds NO2 and NH3 was generally obtained by the TRANC system. With an optimised sample inlet also the fluxes of these compounds were recovered fairly including net deposition and net emission phases. The study shows that the TRANC system is suitable for fast response measurements of oxidized and reduced nitrogen compounds and can be used for continuous eddy covariance flux measurements of total reactive nitrogen.


2021 ◽  
Author(s):  
Pascal Wintjen ◽  
Jeremy Rüffer ◽  
Liv Sokolowsky ◽  
Christof Ammann ◽  
Christian Brümmer

<p>We designed a fast-response two-channel converter called NO<sub>y</sub>-TRANC for eddy covariance measurements of reduced and oxidized reactive nitrogen compounds (N<sub>r</sub>). It is a combination of the Total Reactive Atmospheric Nitrogen Converter (TRANC), which converts all reactive forms of nitrogen (ΣN<sub>r</sub>), except for nitrous oxide (N<sub>2</sub>O) and molecular nitrogen (N<sub>2</sub>), to nitrogen monoxide (NO), and a heated gold catalyst, which converts NO<sub>y</sub> to NO. NO<sub>x</sub>, which is the sum of NO and nitrogen dioxide (NO<sub>2</sub>), and higher oxidized nitrogen compounds are described by the term NO<sub>y</sub>. The NO<sub>y</sub>-TRANC is coupled to a two-channel chemiluminescence detector (CLD) for measuring NO. Due to a high sampling frequency and a fast response time, the system meets the requirements for flux calculation based on the eddy-covariance method. With this setup, a separation of ΣN<sub>r</sub> fluxes in reduced and oxidized nitrogen can be done.</p><p>We conducted flux measurements at a typically deeply drained, intensively managed grassland site on peat in an intensive dairy region in Northwest Germany for one year. ΣN<sub>r</sub> concentration was 12.4 ppb and NO<sub>y</sub> concentration was 6.3 ppb on average. We observed mostly emission fluxes at the site after the first fertilization in early spring. The winter month were characterized by slight nitrogen dry deposition. Monthly median of ΣN<sub>r</sub> fluxes ranged from -8 to 57 ng N m<sup>-2</sup>s<sup>-1</sup> with the exchange being enhanced during summer. We found that ΣN<sub>r</sub> and NO<sub>y</sub> dry emission were comparatively higher under dry conditions, i.e., low air humidity and soil moisture. The emission factors of applied nitrogen after the respective fertilization released as NH<sub>x</sub> can reach up to 2.0%.</p><p>Site management included five fertilization events and five grass cuts. The first fertilization event was at the end of March starting with mineral fertilizer followed by organic fertilizer a week later.  The fertilization scheme was the same for second and third event, but approximately two days were between the application of the fertilizer types. The second fertilization was at the end of May, subsequent fertilizations were done in intervals of 4-5 weeks. Only for the fourth and fifth event, organic fertilizer was used. Organic fertilizer was injected in slits made by v-shaped discs, mineral fertilizer was spread on the soil surface. The emission factor was lower after the first fertilization event compared to events in summer probably indicating a beginning nitrogen saturation after the first fertilization.</p><p>Our study demonstrates the application of a novel measurement technique for the determination reactive nitrogen compounds and gives insight into the exchange characteristics of reactive nitrogen under a common agricultural management.</p>


2019 ◽  
Vol 12 (8) ◽  
pp. 4393-4420 ◽  
Author(s):  
Lukas Siebicke ◽  
Anas Emad

Abstract. Micrometeorological methods to quantify fluxes of atmospheric constituents are key to understanding and managing the impact of land surface sources and sinks on air quality and atmospheric composition. Important greenhouse gases are water vapor, carbon dioxide, methane, and nitrous oxide. Further important atmospheric constituents are aerosols, which impact air quality and cloud formation, and volatile organic compounds. Many atmospheric constituents therefore critically affect the health of ecosystems and humans, as well as climate. The micrometeorological eddy covariance (EC) method has evolved as the method of choice for CO2 and water vapor flux measurements using fast-response gas analyzers. While the EC method has also been used to measure other atmospheric constituents including methane, nitrous oxide, and ozone, the often relatively small fluxes of these constituents over ecosystems are much more challenging to measure using eddy covariance than CO2 and water vapor fluxes. For many further atmospheric constituents, eddy covariance is not an option due to the lack of sufficiently accurate and fast-response gas analyzers. Therefore, alternative flux measurement methods are required for the observation of atmospheric constituent fluxes for which no fast-response gas analyzers exist or which require more accurate measurements. True eddy accumulation (TEA) is a direct flux measurement technique capable of using slow-response gas analyzers. Unlike its more frequently used derivative, known as the relaxed eddy accumulation (REA) method, TEA does not require the use of proxies and is therefore superior to the indirect REA method. The true eddy accumulation method is by design ideally suited for measuring a wide range of trace gases and other conserved constituents transported with the air. This is because TEA obtains whole air samples and is, in combination with constituent-specific fast or slow analyzers, a universal method for conserved scalars. Despite the recognized value of the method, true eddy accumulation flux measurements remain very challenging to perform as they require fast and dynamic modulation of the air sampling mass flow rate proportional to the magnitude of the instantaneous vertical wind velocity. Appropriate techniques for dynamic mass flow control have long been unavailable, preventing the unlocking of the TEA method's potential for more than 40 years. Recently, a new dynamic and accurate mass flow controller which can resolve turbulence at a frequency of 10 Hz and higher has been developed by the first author. This study presents the proof of concept that practical true eddy accumulation trace gas flux measurements are possible today using dynamic mass flow control, advanced real-time processing of wind measurements, and fully automatic gas handling. We describe setup and methods of the TEA and EC reference flux measurements. The experiment was conducted over grassland and comprised 7 d of continuous flux measurements at 30 min flux integration intervals. The results show that fluxes obtained by TEA compared favorably to EC reference flux measurements, with coefficients of determination of up to 86 % and a slope of 0.98. We present a quantitative analysis of uncertainties of the mass flow control system, the gas analyzer, and gas handling system and their impact on trace gas flux uncertainty, the impact of different approaches to coordinate rotation, and uncertainties of vertical wind velocity measurements. Challenges of TEA are highlighted and solutions presented. The current results are put into the context of previous works. Finally, based on the current successful proof of concept, we suggest specific improvements towards long-term and reliable true eddy accumulation flux measurements.


2014 ◽  
Vol 11 (12) ◽  
pp. 3163-3186 ◽  
Author(s):  
O. Peltola ◽  
A. Hensen ◽  
C. Helfter ◽  
L. Belelli Marchesini ◽  
F. C. Bosveld ◽  
...  

Abstract. The performance of eight fast-response methane (CH4) gas analysers suitable for eddy covariance flux measurements were tested at a grassland site near the Cabauw tall tower (Netherlands) during June 2012. The instruments were positioned close to each other in order to minimise the effect of varying turbulent conditions. The moderate CH4 fluxes observed at the location, of the order of 25 nmol m−2 s−1, provided a suitable signal for testing the instruments' performance. Generally, all analysers tested were able to quantify the concentration fluctuations at the frequency range relevant for turbulent exchange and were able to deliver high-quality data. The tested cavity ringdown spectrometer (CRDS) instruments from Picarro, models G2311-f and G1301-f, were superior to other CH4 analysers with respect to instrumental noise. As an open-path instrument susceptible to the effects of rain, the LI-COR LI-7700 achieved lower data coverage and also required larger density corrections; however, the system is especially useful for remote sites that are restricted in power availability. In this study the open-path LI-7700 results were compromised due to a data acquisition problem in our data-logging setup. Some of the older closed-path analysers tested do not measure H2O concentrations alongside CH4 (i.e. FMA1 and DLT-100 by Los Gatos Research) and this complicates data processing since the required corrections for dilution and spectroscopic interactions have to be based on external information. To overcome this issue, we used H2O mole fractions measured by other gas analysers, adjusted them with different methods and then applied them to correct the CH4 fluxes. Following this procedure we estimated a bias of the order of 0.1 g (CH4) m−2 (8% of the measured mean flux) in the processed and corrected CH4 fluxes on a monthly scale due to missing H2O concentration measurements. Finally, cumulative CH4 fluxes over 14 days from three closed-path gas analysers, G2311-f (Picarro Inc.), FGGA (Los Gatos Research) and FMA2 (Los Gatos Research), which were measuring H2O concentrations in addition to CH4, agreed within 3% (355–367 mg (CH4) m−2) and were not clearly different from each other, whereas the other instruments derived total fluxes which showed small but distinct differences (±10%, 330–399 mg (CH4) m−2).


2020 ◽  
Author(s):  
Yuan You ◽  
Ralf M. Staebler ◽  
Samar G. Moussa ◽  
James Beck ◽  
Richard L. Mittermeier

Abstract. Tailings ponds in the Alberta Oil Sands Region are significant sources of fugitive emissions of methane to the atmosphere, but detailed knowledge on spatial and temporal variabilities is lacking due to limitations of the methods deployed under current regulatory compliance monitoring programs. To develop more robust and representative methods for quantifying these emissions, three micrometeorological flux methods were applied along with traditional flux chambers to determine fluxes over a 5-week period. Eddy covariance flux measurements provided the benchmark. A method is presented to directly calculate stability-corrected eddy diffusivities that can be applied to vertical gas profiles for gradient flux estimation. Gradient fluxes were shown to agree with eddy covariance within 7 %, and inverse dispersion model fluxes within 11 %, with an overall uncertainty of 28 % for the calculated mean flux. Fluxes were shown to have only a minor diurnal cycle (18 % variability) and to be mostly independent of wind speed, air and water surface temperatures. Flux chambers underestimated the fluxes by a factor of 2 in this particular campaign. These measurements indicate that the larger footprint of micrometeorological measurements results in more robust emission estimates representing the whole pond.


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