Relaxed Eddy Accumulation Method Research Articles

A Single Compartment Relaxed Eddy Accumulation Method

AbstractThe relaxed eddy accumulation (REA) method is a widely‐known technique that measures turbulent fluxes of scalar quantities. The REA technique has been used to measure turbulent fluxes of various compounds, such as methane, ethene, propene, butene, isoprene, nitrous oxides, ozone, and others. The REA method requires the accumulation of scalar concentrations in two separate compartments that conditionally sample updrafts and downdraft events. It is demonstrated here that the assumptions behind the conventional or two‐compartment REA approach allow for one‐compartment sampling, therefore called a one compartment or 1‐C‐REA approach, thereby expanding its operational utility. The one‐compartment sampling method is tested across various land cover types and atmospheric stability conditions, and it is found that the one‐compartment REA can provide results comparable to those determined from conventional two‐compartment REA. This finding enables rapid expansion and practical utility of REA in studies of surface‐atmosphere exchanges, interactions, and feedbacks.

The Relaxed Eddy Accumulation Method Over the Amazon Forest: The Importance of Flux Strength on Individual and Aggregated Flux Estimates

The Relaxed Eddy Accumulation Method Over the Amazon Forest: The Importance of Flux Strength on Individual and Aggregated Flux Estimates

Discerning the Concentration and Bi‐Directional Flux of Ammonia in an Urban Estuary Using the Relaxed Eddy Accumulation Method

AbstractNarragansett Bay, the largest estuary in New England, is a heavily urbanized watershed impacted by deposition and runoff. Nutrient budgets and local policy rely on deposition data from a 1990 study that did not include any direct observations of dry deposition of gaseous ammonia (NH3(g)) and particulate ammonium (p‐NH4+) due to uncertainties in their flux direction and measurement difficulty. Recent work has shown that wet deposition of ammonium (NH4+) to the Bay has increased by a factor of 6 over the past three decades, leading to a 2.5‐fold increase in wet nitrogen (N) deposition. This documented increase in wet deposition of NH4+ is concurrent with managed nutrient reductions in urbanized estuaries but has potentially increased the impacts of atmospheric N deposition, including the dry deposition of NH3(g) and p‐NH4+. However, the lack of NH3(g) and p‐NH4+ measurements hinders our interpretation of this important N source. For the first time over Narragansett Bay, and to our knowledge over open water, dry (particulate and gas phase) total ammonia (NHx = NH3(g) + p‐NH4+) and the bidirectional NH3(g) flux were quantified using a relaxed eddy accumulation sampling technique. We find that dry deposition of NHx comprises 9.6% of total (wet + dry) N deposition. During the fall season, the dominant flux direction for NH3(g) is upward, which also has implications for urban air quality. We estimate that NH3(g) emitted from the Bay to the atmosphere makes up to 10% of the local NH3(g) emission budget for fall.

Relaxed Eddy Accumulation Outperforms Monin‐Obukhov Flux Models Under Non‐Ideal Conditions

AbstractThe Monin‐Obukhov Similarity Theory (MOST) links turbulent statistics to surface fluxes through universal functions. Here, we investigate its performance over a large lake, where none of its assumptions (flat homogeneous surface) are obviously violated. We probe the connection between the variance budget terms and departure from the nondimensional flux‐variance function for CO2, water vapor, and temperature. Our results indicate that both the variance storage and its vertical transport affect MOST, and these terms are most significant when small fluxes and near neutral conditions were prevalent. Such conditions are common over lakes and oceans, especially for CO2, underlining the limitation of using any MOST‐based methods to compute small fluxes. We further show that the relaxed eddy accumulation (REA) method is more robust and less sensitive to storage and transport, adequately reproducing the eddy‐covariance fluxes even for the smallest flux magnitudes. Therefore, we recommend REA over MOST methods for trace‐gas flux estimation.

Ammonia fluxes over an agricultural field in growing and fallow periods using relaxed eddy accumulation

Asia has a considerable risk of nitrogen deposition effects on ecosystems due to the high deposition amounts. Ammonia (NH3) emissions, primarily from agricultural production, have increased in East Asia, and the increasing contribution of NH3 deposition to the total nitrogen deposition is concerning. However, NH3 deposition in this region is uncertain due to lacking flux measurements and the complex bidirectional nature of NH3 atmosphere−surface exchange. To better understand the NH3 deposition in this region, we investigated NH3 fluxes over an agricultural field in Tokyo, Japan. Fluxes were determined using the relaxed eddy accumulation method incorporating the denuder/filter-pack sampling technique and continuously conducting daytime and nighttime measurements in soybean-growing (July 28–August 5, 2020) and fallow (March 4–March 10, 2021) periods. NH3 fluxes were mostly downward in both periods, indicating that the agricultural field was a sink for NH3 during the periods (mean flux = −0.091 μg m−2 s−1). The deposition velocities in the growing period were lower than in the fallow period possibly due to the smaller turbulence. The deposition velocities correlated positively with friction velocity, indicating that the turbulence is the dominant factor driving NH3 deposition. We compared inferred fluxes using a compensation point model with the measured fluxes. The model did not reproduce the observation results when using default inputs, but showed a mean NH3 emission of 0.054 μg m−2 s−1. Revised inputs considering on-site soil and foliage information improved the model's results; however, the inferred fluxes were still smaller than the measured fluxes (mean flux = −0.017 μg m−2 s−1). These results indicate that there were possibly other processes enhancing NH3 deposition in the agricultural field.

Choosing an optimal <i>β</i> factor for relaxed eddy accumulation applications across vegetated and non-vegetated surfaces

Abstract. Accurately measuring the turbulent transport of reactive and conservative greenhouse gases, heat, and organic compounds between the surface and the atmosphere is critical for understanding trace gas exchange and its response to changes in climate and anthropogenic activities. The relaxed eddy accumulation (REA) method enables measuring the land surface exchange when fast-response sensors are not available, broadening the suite of trace gases that can be investigated. The β factor scales the concentration differences to the flux, and its choice is central to successfully using REA. Deadbands are used to select only certain turbulent motions to compute the flux. This study evaluates a variety of different REA approaches with the goal of formulating recommendations applicable over a wide range of surfaces and meteorological conditions for an optimal choice of the β factor in combination with a suitable deadband. Observations were collected across three contrasting ecosystems offering stark differences in scalar transport and dynamics: a mid-latitude grassland ecosystem in Europe, a loose gravel surface of the Dry Valleys of Antarctica, and a spruce forest site in the European mid-range mountains. We tested a total of four different REA models for the β factor: the first two methods, referred to as model 1 and model 2, derive βp based on a proxy p for which high-frequency observations are available (sensible heat Ts). In the first case, a linear deadband is applied, while in the second case, we are using a hyperbolic deadband. The third method, model 3, employs the approach first published by Baker et al. (1992), which computes βw solely based upon the vertical wind statistics. The fourth method, model 4, uses a constant βp, const derived from long-term averaging of the proxy-based βp factor. Each β model was optimized with respect to deadband size before intercomparison. To our best knowledge, this is the first study intercomparing these different approaches over a range of different sites. With respect to overall REA performance, we found that the βw and constant βp, const performed more robustly than the dynamic proxy-dependent approaches. The latter models still performed well when scalar similarity between the proxy (here Ts) and the scalar of interest (here water vapor) showed strong statistical correlation, i.e., during periods when the distribution and temporal behavior of sources and sinks were similar. Concerning the sensitivity of the different β factors to atmospheric stability, we observed that βT slightly increased with increasing stability parameter z/L when no deadband is applied, but this trend vanished with increasing deadband size. βw was unrelated to dynamic stability and displayed a generally low variability across all sites, suggesting that βw can be considered a site-independent constant. To explain why the βw approach seems to be insensitive towards changes in atmospheric stability, we separated the contribution of w′ kurtosis to the flux uncertainty. For REA applications without deeper site-specific knowledge of the turbulent transport and degree of scalar similarity, we recommend using either the βp, const or βw models when the uncertainty of the REA flux quantification is not limited by the detection limit of the instrument. For conditions when REA sampling differences are close to the instrument's detection limit, the βp models using a hyperbolic deadband are the recommended choice.

Recent advances in understanding and measurement of Hg in the environment: Surface-atmosphere exchange of gaseous elemental mercury (Hg0)

The atmosphere is the major transport pathway for distribution of mercury (Hg) globally. Gaseous elemental mercury (GEM, hereafter Hg0) is the predominant form in both anthropogenic and natural emissions. Evaluation of the efficacy of reductions in emissions set by the UN's Minamata Convention (UN-MC) is critically dependent on the knowledge of the dynamics of the global Hg cycle. Of these dynamics including e.g. red-ox reactions, methylation-demethylation and dry-wet deposition, poorly constrained atmosphere–surface Hg0 fluxes especially limit predictability of the timescales of its global biogeochemical cycle. This review focuses on Hg0 flux field observational studies, namely the theory, applications, strengths, and limitations of the various experimental methodologies applied to gauge the exchange flux and decipher active sub-processes. We present an in-depth review, a comprehensive literature synthesis, and methodological and instrumentation advances for terrestrial and marine Hg0 flux studies in recent years. In particular, we outline the theory of a wide range of measurement techniques and detail the operational protocols. Today, the most frequently used measurement techniques to determine the net Hg0 flux (>95% of the published flux data) are dynamic flux chambers for small-scale and micrometeorological approaches for large-scale measurements. Furthermore, top-down approaches based on Hg0 concentration measurements have been applied as tools to better constrain Hg emissions as an independent way to e.g. challenge emission inventories. This review is an up-dated, thoroughly revised edition of Sommar et al. 2013 (DOI: 10.1080/10643389.2012.671733). To the tabulation of >100 cited flux studies 1988–2009 given in the former publication, we have here listed corresponding studies published during the last decade with a few exceptions (2008–2019). During that decade, Hg stable isotope ratios of samples involved in atmosphere-terrestrial interaction is at hand and provide in combination with concentration and/or flux measurements novel constraints to quantitatively and qualitatively assess the bi-directional Hg0 flux. Recent efforts in the development of relaxed eddy accumulation and eddy covariance Hg0 flux methods bear the potential to facilitate long-term, ecosystem-scale flux measurements to reduce the prevailing large uncertainties in Hg0 flux estimates. Standardization of methods for Hg0 flux measurements is crucial to investigate how land-use change and how climate warming impact ecosystem-specific Hg0 sink-source characteristics and to validate frequently applied model parameterizations describing the regional and global scale Hg cycle.

True eddy accumulation trace gas flux measurements: proof of concept

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.

Implementation of the effect of urease inhibitor on ammonia emissions following urea-based fertilizer application at a Zea mays field in central Illinois: A study with SURFATM-NH3 model

Agriculture is the main source of ammonia (NH3) emissions in the atmosphere. NH3 is precursor to secondary fine particulate matter, which is of concern for its impacts on health and visibility. There are a limited number of field measurements of NH3 emissions from fertilizer application in the US, and this limits our understanding of the importance of individual NH3 source and sink processes in controlling timing and magnitude of NH3 emissions. In this study, a new parameterization of the effect of urease inhibitor on NH3 emissions from urea-based fertilizer was developed on the basis of experimental results found in the literature. This parameterization was combined with an existing operational parameterization of soil and stomatal emission potentials (Γg, Γs) and was implemented in a surface-atmosphere transfer model for NH3 (SURFATM-NH3) in order to evaluate the bi-directional fluxes of NH3 at the field scale. The model was evaluated with field measurements obtained by the flux-gradient (FG) and relaxed eddy accumulation (REA) methods in a fertilized corn field in central Illinois. By integrating the effect of urease inhibitor, the timing of the highest NH3 emission peak was successfully predicted and its magnitude was close to that measured (predicted 2106 ng m−2 s−1, measured by FG 2312 ± 582 ng m−2 s−1). Based on the model results, urease inhibitor has a considerable effect on the dynamics and order of magnitude of NH3 fluxes. Furthermore, the model simulated the inhibiting action of N-(n-butyl) thiophosphoric (nBTPT) and suggests that it can reduce NH3 volatilization by 32%. The model also successfully predicted environmental parameters, such as soil temperature. Finally, this new version of SURFATM-NH3 is a valuable tool to estimate the NH3 bi-directional fluxes at the field scale, which describes dynamic modeling of Γs and Γg by taking into account the effect of urease inhibitor which is commonly used in the US to improve the efficiency of urea fertilizers.

Ammonia flux measurements above a corn canopy using relaxed eddy accumulation and a flux gradient system

Studies of NH3 flux over agricultural ecosystems in the USA are limited by low temporal resolution (typically hours or days) and sparse spatial coverage, with no studies over corn in the Midwest USA. We report on NH3 flux measurements over a corn canopy in Central Illinois, USA, using the relaxed eddy accumulation (REA) and flux gradient (FG) methods, providing measurements at 4 h and 0.5 h intervals, respectively. The REA and FG systems were operated for the duration of the 2014 corn-growing season. Flux-footprint analysis was used to select data from both systems, resulting in 82 concurrent measurements. Mean NH3 flux of concurrent measurements was 205 ± 300 ng m−2 s−1 from REA and 110 ± 256 ng m−2 s−1 from FG for all concurrent samples. Results from both methods were not significantly different at a 95% confidence level for all concurrent measurements. The FG system resolved NH3 emission peaks at 0.5 h averaging time that were otherwise un-observed with 4 h REA averaging. Two early-season peak emission periods were identified (DOY 130-132 and 140-143), where the timing and intensity of such emissions were attributed to a combination of urease inhibitor, applied as a field-management decision, and localized soil temperature and precipitation. Given the dependence of NH3 fluxes on multiple parameters, this study further highlights the need for increased spatial coverage and high temporal resolution (e.g., <1 h) of measurements to better understand the impact of agricultural NH3 emissions on air quality and the global nitrogen cycle. Such measurements are also needed for evaluation of models describing surface-atmosphere exchange of NH3.

Ecosystem‐Scale Measurements of Methyl Halide Fluxes From a Brackish Tidal Marsh Invaded With Perennial Pepperweed (Lepidium latifolium)

AbstractNatural methyl chloride (CH3Cl) and methyl bromide (CH3Br) emissions from coastal marsh ecosystems may constitute a significant proportion of stratospheric chlorine and bromine, which catalyze ozone depletion. Current inventories involve substantial uncertainties associated with upscaling plot‐scale footprints (i.e., ≤1 m2). Here we present net ecosystem flux measurements of methyl halides from a brackish tidal marsh on the west coast of the United States between April 2016 and June 2017 using the relaxed eddy accumulation method. The measurement footprint encompasses a large part of the studied tidal marsh, including roughly 20 vascular plant species, open water, and soil surfaces. On the annual scale, ecosystem methyl halide emissions showed the strongest relationships to temperature and the growth cycle of halophyte vegetation, whereas on diurnal time scales, fluxes correlated the most with evapotranspiration. The maximum seasonal emissions occurred during the flowering season of Lepidium latifolium (perennial pepperweed), one of the most abundant halophytes on site. The maximum hourly emissions of 111 μg CH3Cl · m−2 s· hr−1 and 38 μg CH3Br · m−2 · hr−1 were observed during a heat wave in early June. Annually integrated emissions were 135 mg/m2 for CH3Cl and 21 mg/m2 for CH3Br, scaling up to 621 and 96 kg over the entire marsh. We provide a global salt marsh emission inventory that takes into account the spatial distribution of salt marshes in different climate zones, yielding a global salt marsh source of 31 Gg/year CH3Cl (range: 10 to 77) and 3 Gg/year CH3Br (range: 1 to 8).

A cool-temperate young larch plantation as a net methane source - A 4-year continuous hyperbolic relaxed eddy accumulation and chamber measurements

Upland forests are thought to be methane (CH4) sinks due to oxidation by methanotrophs in aerobic soils. However, CH4 budget for upland forests are not well quantified at the ecosystem scale, when possible CH4 sources, such as small wet areas, exists in the ecosystem. Here, we quantified CH4 fluxes in a cool-temperate larch plantation based on four-year continuous measurements using the hyperbolic relaxed eddy accumulation (HREA) method and dynamic closed chambers with a laser-based analyzer. After filling data gaps for half-hourly data using machine-learning-based regressions, we found that the forest acted as a net CH4 source at the canopy scale: 30 ± 11 mg CH4 m−2 yr−1 in 2014, 56 ± 8 mg CH4 m−2 yr−1 in 2015, 154 ± 5 mg CH4 m−2 yr−1 in 2016, and 132 ± 6 mg CH4 m−2 yr−1 in 2017. Hotspot emissions from the edge of the pond could strongly contribute to the canopy-scale emissions. The magnitude of the hotspot emissions was 10–100 times greater than the order of the canopy-scale and chamber-based CH4 fluxes at the dry soils. The high temperatures with wet conditions stimulated the hotspot emissions, and thus induced canopy-scale CH4 emissions in the summer. Understanding and modeling the dynamics of hotspot emissions are important for quantifying CH4 budgets of upland forests. Micrometeorological measurements at various forests are required for revisiting CH4 budget of upland forests.

Continuous flow hygroscopicity-resolved relaxed eddy accumulation (Hy-Res REA) method of measuring size-resolved sodium chloride particle fluxes.

The accurate representation of aerosols in climate models requires direct ambient measurement of the size- and composition-dependent particle production fluxes. Here, we present the design, testing, and analysis of data collected through the first instrument capable of measuring hygroscopicity-based, size-resolved particle fluxes using a continuous-flow Hygroscopicity-Resolved Relaxed Eddy Accumulation (Hy-Res REA) technique. The Hy-Res REA system used in this study includes a 3D sonic anemometer, two fast-response solenoid valves, two condensation particle counters, a scanning mobility particle sizer, and a hygroscopicity tandem differential mobility analyzer. The different components of the instrument were tested inside the US Environmental Protection Agency's Aerosol Test Facility for sodium chloride and ammonium sulfate particle fluxes. The new REA system design does not require particle accumulation, and therefore avoids the diffusional wall losses associated with long residence times of particles inside the air collectors of traditional REA devices. A linear relationship was found between the sodium chloride particle fluxes measured by eddy covariance and REA techniques. The particle detection limit of the Hy-Res REA flux system is estimated to be ~3 × 105 m-2 s-1. The estimated sodium chloride particle classification limit, for the mixture of sodium chloride and ammonium sulfate particles of comparable concentrations, is ~6 × 106 m-2 s-1.

The non‐local character of turbulence asymmetry in the convective atmospheric boundary layer

The inadequacy of conventional gradient diffusion in closure modelling of turbulent heat fluxes within the convective atmospheric boundary layer is often alleviated by accounting for non‐local transport effects, such as Deardorff's counter‐gradient models, Wyngaard's transport asymmetry closures or mass‐flux parametrization. This concept of large‐eddy flux transport is examined here with the principal aim of unifying these seemingly different models. Using large‐eddy simulation (LES) runs for the atmospheric boundary layer, spanning weakly to strongly convective conditions, a generic diagnostic framework that encodes the role of third‐order moments in non‐local transport is developed and tested. The premise is that these non‐local effects are responsible for the inherent asymmetry in vertical transport and hence the necessary non‐Gaussian nature of the joint probability density function (JPDF) of vertical velocity and potential temperature must account for these effects. Conditional sampling (quadrant analysis) of this JPDF and the imbalance between the flow mechanisms of ejections and sweeps are used to characterize this asymmetry, which is then linked to the third‐order moments using a cumulant‐discard method for the Gram–Charlier expansion of the JPDF. While the concept of ejection‐sweep events used here is not a simple extension of that commonly used in the surface layer, their connection to third‐order moments shows that the concepts of bottom‐up/top‐down diffusion or updraught/downdraught models are accounted for by various quadrants of the JPDF. An analogy between mass‐flux models and the relaxed eddy accumulation method reveals that there is a seemingly implicit assumption of a Gaussian JPDF in the former.

Methane uptake in a temperate forest soil using continuous closed-chamber measurements

Methane (CH4) fluxes were continuously measured in a temperate forest soil using six dynamic closed chambers with a laser-based analyzer. CH4 uptake increased with an increase in soil temperature and a decrease in volumetric water content, where multiple linear regressions using the two variables explained approximately 80% of the seasonal variations. Based on the measurements, our forest acted as an annual CH4 sink with a spatial variation of 25%. The calculated annual CH4 sink significantly decreased by increasing the chamber deployment period: 8–13mg CH4m−2yr−1min−1. The annual CH4 sink was significantly different using different calculation methods for the initial slope: 898±11mg CH4m−2yr−1 using a linear regression, 924±8mg CH4m−2yr−1 using a quadratic regression, and 975±10mg CH4m−2yr−1 using an exponential model. These results indicate that underestimations due to disturbing the CH4 gradient between chamber headspaces and soils were significant despite of the short deployment periods of 4–10min. Chamber-based fluxes were consistent with canopy-scale CH4 fluxes by the micrometeorological hyperbolic relaxed eddy accumulation method: sink of 731±38 to 888±87mg CH4m−2yr−1. Continuous dynamic closed chambers with laser-based analyzers are a powerful tool to understand CH4 fluxes in temperate forest soils, as long as a range of uncertainties are carefully evaluated.

Mercury vapor air–surface exchange measured by collocated micrometeorological and enclosure methods – Part II: Bias and uncertainty analysis

Abstract. Dynamic flux chambers (DFCs) and micrometeorological (MM) methods are extensively deployed for gauging air–surface Hg0 gas exchange. However, a systematic evaluation of the precision of the contemporary Hg0 flux quantification methods is not available. In this study, the uncertainty in Hg0 flux measured by the relaxed eddy accumulation (REA) method, the aerodynamic gradient method (AGM), the modified Bowen ratio (MBR) method, as well as DFC of traditional (TDFC) and novel (NDFC) designs, are assessed using a robust data set from two field intercomparison campaigns. The absolute precision in Hg0 concentration difference (ΔC) measurements is estimated at 0.064 ng m−3 for the gradient-based MBR and AGM systems. For the REA system, the parameter is Hg0 concentration (C) dependent at 0.069 + 0.022C. During the campaigns, 57 and 62 % of the individual vertical gradient measurements are found to be significantly different from 0, while for the REA technique, the percentage of significant observations is lower. For the chambers, non-significant fluxes are confined to a few night-time periods with varying ambient Hg$^{0}$ concentrations. Relative bias for DFC-derived fluxes is estimated to be ~ ±10, and ~ 85% of the flux bias is within ±2 ng m−2 h−1 in absolute terms. The DFC flux bias follows a diurnal cycle, which is largely affected by the forced temperature and irradiation bias in the chambers. Due to contrasting prevailing micrometeorological conditions, the relative uncertainty (median) in turbulent exchange parameters differs by nearly a factor of 2 between the campaigns, while that in ΔC measurement is fairly consistent. The estimated flux uncertainties for the triad of MM techniques are 16–27, 12–23 and 19–31% (interquartile range) for the AGM, MBR and REA methods, respectively. This study indicates that flux-gradient-based techniques (MBR and AGM) are preferable to REA in quantifying Hg0 flux over ecosystems with low vegetation height. A limitation of all Hg0 flux measurement systems investigated is their inability to obtain synchronous samples for the calculation of ΔC. This reduces the precision of flux quantification, particularly in the MM systems under non-stationarity of ambient Hg0 concentration. For future applications, it is recommended to accomplish ΔC derivation from simultaneous collected samples.

Dry deposition of PM2.5 sulfate above a hilly forest using relaxed eddy accumulation

Sulfur compounds continue to be an important component of atmospheric deposition in East Asia. In order to better understand the dry deposition of PM2.5 sulfate, which is one of the most significant transboundary air pollutants in this region, we measured the dry deposition flux of PM2.5 sulfate above a hilly forest of the Field Museum Tamakyuryo (FM Tama) site in suburban Tokyo. We used the relaxed eddy accumulation (REA) method and took measurements during the summer, from 26 July to 2 August 2013, and the autumn, from 18 to 22 November 2013. We primarily focused on the evaluation of dry deposition above a forest on complex terrain. The total flux and 80% of the runs showed downward flux. The deposition velocities measured by the REA method during times when the wind direction was from a relatively uniform sloping surface over the forest were more reasonable than those measured when the wind direction was from a more complex surface. Using a resistance model that includes the effect of growth of hygroscopic aerosols, we inferred the deposition velocities during two experimental periods. When the fluxes were averaged for a long time (i.e., about 2 weeks) the inferred fluxes and deposition velocities were in reasonable agreement with the measurements. Although averages over long periods showed good agreement, the measured deposition velocities were distributed in a wider range than those inferred by the model. An increased range of deposition velocities was associated with flux footprints from complex terrain. It is possible that the agreements between measured and inferred fluxes or deposition velocities at the site are because the depositions of sulfate are largely controlled by surface factors rather than aerodynamic resistance.

Inferring methane fluxes at a larch forest using Lagrangian, Eulerian, and hybrid inverse models

AbstractMeasuring methane (CH4) flux at upland forests is challenging due to high levels of heterogeneity in upscaling chamber measurements and the detection limits of currently available micrometeorological methods. We estimated CH4 fluxes in an upland forest from vertical concentration profiles using three different inverse multilayer models: the Lagrangian localized near field theory, Eulerian, and hybrid Lagrangian‐Eulerian models. The approach could estimate spatially representative fluxes, and use of higher gradients within canopies than above them could minimize uncertainties associated with sensor noises. Comparing fluxes by the models and measurements by the micrometeorological hyperbolic relaxed eddy accumulation and chamber methods, daytime fluxes were reasonably reproduced, but nighttime fluxes were overestimated most likely due to an underestimation of stable conditions and storage effects. The models and measurements show that the forest acted as a CH4 sink during the study period, and the soil acted as the dominant sink. The estimated sink increased with increasing soil temperatures and decreasing soil water content. The CH4 sink estimated during the study period were 1.5 ± 0.2 nmol m−2 s−1 by the micrometeorological method, 2.4 ± 0.5 nmol m−2 s−1 by chambers, 2.8 ± 1.1 nmol m−2 s−1 by the Lagrangian model, 2.7 ± 1.0 nmol m−2 s−1 by the Eulerian model, and 3.7 ± 2.8 nmol m−2 s−1 by the hybrid model. The performance of the Lagrangian and hybrid models increased when the CH4 sink/source was assumed to only exist in the soil.

Application of a GC-ECD for measurements of biosphere–atmosphere exchange fluxes of peroxyacetyl nitrate using the relaxed eddy accumulation and gradient method

Abstract. Peroxyacetyl nitrate (PAN) may constitute a significant fraction of reactive nitrogen in the atmosphere. Current knowledge about the biosphere–atmosphere exchange of PAN is limited, and only few studies have investigated the deposition of PAN to terrestrial ecosystems. We developed a flux measurement system for the determination of biosphere–atmosphere exchange fluxes of PAN using both the hyperbolic relaxed eddy accumulation (HREA) method and the modified Bowen ratio (MBR) method. The system consists of a modified, commercially available gas chromatograph with electron capture detection (GC-ECD, Meteorologie Consult GmbH, Germany). Sampling was performed by trapping PAN onto two pre-concentration columns; during HREA operation one was used for updraft and one for downdraft events, and during MBR operation the two columns allowed simultaneous sampling at two measurement heights. The performance of the PAN flux measurement system was tested at a natural grassland site, using fast-response ozone (O3) measurements as a proxy for both methods. The measured PAN fluxes were comparatively small (daytime PAN deposition was on average −0.07 nmol m−2 s−1) and, thus, prone to significant uncertainties. A major challenge in the design of the system was the resolution of the small PAN mixing ratio differences. Consequently, the study focuses on the performance of the analytical unit and a detailed analysis of errors contributing to the overall uncertainty. The error of the PAN mixing ratio differences ranged from 4 to 15 ppt during the MBR and between 18 and 26 ppt during the HREA operation, while during daytime measured PAN mixing ratios were of similar magnitude. Choosing optimal settings for both the MBR and HREA method, the study shows that the HREA method did not have a significant advantage towards the MBR method under well-mixed conditions as was expected.

Is the empirical coefficient b for the relaxed eddy accumulation method constant?

The relaxed eddy accumulation (REA) method is an attractive alternative to the eddy covariance method to measure trace-gas flux, because it allows the use of analyzers with an optimal integration time to reduce the noise. However, the use of an empirical coefficient b results in uncertainties in the REA method. The consistency of b for temperature was investigated using a 1 year dataset obtained at three forest sites in East Asia: a temperate evergreen coniferous forest, a tropical evergreen broadleaf forest, and a cool-temperate deciduous coniferous forest. The observational b ranged from 0.54 to 0.57 under unstable conditions. Although the values for observational b were within narrow ranges among the sites, there were slight site-specific differences. We introduced new expression of b, similarity b, based on scalar similarity using the integral turbulence characteristics to investigate the nature of b. Both the observational and similarity b increased with increasing atmospheric stability under stable conditions, when lower values for the standard deviation of the vertical wind velocity resulted in higher values for b. The variations in b under stable conditions differed among sites. There were no seasonal variations in the observational b at all sites. Consequently, the present study recommends determining the coefficient b for unstable conditions for each site and considering changes in b associated with atmospheric stability in order to minimize errors in the REA method.