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

2015 ◽  
Vol 15 (10) ◽  
pp. 5359-5376 ◽  
Author(s):  
W. Zhu ◽  
J. Sommar ◽  
C.-J. Lin ◽  
X. Feng

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.

2015 ◽  
Vol 15 (4) ◽  
pp. 4627-4676
Author(s):  
W. Zhu ◽  
J. Sommar ◽  
C.-J. Lin ◽  
X. Feng

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 relaxed eddy accumulation (REA) method, aerodynamic gradient method (AGM), modified Bowen-ratio (MBR) method, as well as DFC of traditional (TDFC) and novel (NDFC) designs is assessed using a robust data-set from two field intercomparison campaigns. The absolute precision in Hg0 concentration difference (Δ C) measurements is estimated at 0.064 ng m−3 for the gradient-based MBR and AGM system. For the REA system, the parameter is Hg0 concentration (C) dependent at 0.069+0.022C. 57 and 62% of the individual vertical gradient measurements were found to be significantly different from zero during the campaigns, while for the REA-technique the percentage of significant observations was lower. For the chambers, non-significant fluxes are confined to a few nighttime periods with varying ambient Hg0 concentration. Relative bias for DFC-derived fluxes is estimated to be ~ ±10%, and ~ 85% of the flux bias are within ±2 ng m−2 h−1 in absolute term. The DFC flux bias follows a diurnal cycle, which is largely dictated by temperature controls on the enclosed volume. Due to contrasting prevailing micrometeorological conditions, the relative uncertainty (median) in turbulent exchange parameters differs by nearly a factor of two between the campaigns, while that in Δ C measurements is fairly stable. 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 method, 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 incapability to obtain synchronous samples for the calculation of Δ C. This reduces the precision of flux quantification, particularly the MM-systems under non-stationarity of ambient Hg0 concentration. For future applications, it is recommended to accomplish Δ C derivation from simultaneous collected samples.


2021 ◽  
Author(s):  
Thomas Cropper ◽  
Elizabeth Kent ◽  
David Berry ◽  
Richard Cornes ◽  
Beatriz Recinos-Rivas

<p>Accurate, long-term time series of near-surface air temperature (AT) are the fundamental datasets on which the magnitude of anthropogenic climate change is scientifically and societally addressed. Across the ocean, these (near-surface) climate records use Sea Surface Temperature (SST) instead of Marine Air Temperature (MAT) and blend the SST and AT over land to create datasets. MAT has often been overlooked as a data choice as daytime MAT observations from ships are known to contain warm biases due to the storage of accumulated solar energy. Two recent MAT datasets, CLASSnmat (1881 – 2019) and UAHNMAT (1900 – 2018), both use night-time MAT observations only. Daytime MAT observations in the International Comprehensive Ocean–Atmosphere Data Set (ICOADS) account for over half of the MAT observations in ICOADS, and this proportion increases further back in time (i.e. pre-1850s). If long-term MAT records over the ocean are to be extended, the use of daytime MAT is vital.</p><p> </p><p>To adjust for the daytime MAT heating bias, and apply it to ICOADS, we present the application of a physics-based model, which accounts for the accumulated energy storage throughout the day. As the ‘true’ diurnal cycle of MAT over the ocean has not been, to-date, adequately quantified, our approach also removes the diurnal cycle from ICOADS observations and generates a night-time equivalent MAT for all observations. We fit this model to MAT observations from groups of ships in ICOADS that share similar heating biases and metadata characteristics. This enables us to use the empirically derived coefficients (representing the physical energy transfer terms of the heating model) obtained from the fit for use in removal of the heating bias and diurnal cycle from ship-based MAT observations throughout ICOADS which share similar characteristics (i.e. we can remove the diurnal cycle from a ship which only reports once daily at noon). This adjustment will create an MAT record of night-time-equivalent temperatures that will enable an extension of the marine surface AT record back into the 18<sup>th</sup> century.</p>


2016 ◽  
Author(s):  
W. Zhu ◽  
C.-J. Lin ◽  
X. Wang ◽  
J. Sommar ◽  
X. W. Fu ◽  
...  

Abstract. Reliable quantification of air-surfaces flux of elemental Hg vapor (Hg0) is crucial for understanding mercury (Hg) global biogeochemical cycles. There have been extensive measurements and modeling efforts devoting to estimating the exchange fluxes between the atmosphere and various surfaces (e.g., soil, canopies, water, snow, etc.) in past three decades. However, large uncertainty remains due to the complexity of Hg0 bi-directional exchange, limitations of flux quantification techniques and challenges in model parameterization. In this study, we provide a comprehensive review on the state of science in the atmosphere-surface exchange of Hg0. Specifically, the advancement of flux quantification techniques, mechanisms in driving the air-surfaces Hg exchange, and modeling efforts are presented. Due to the semi-volatile nature of Hg0 and redox transformation of Hg in environmental media, Hg deposition and evasion are influenced by multiple environmental variables including seasonality, vegetative coverage and its life cycle, temperature, light, moisture, atmospheric turbulence, presence of reactants (e.g., O3, radicals, etc.) that drives the physicochemical process of Hg in the media where Hg0 exchange occurs. However, effects of these processes on flux have not been fundamentally and quantitatively determined, which limits the accuracy of flux modeling. In this study, we compile an up-to-date global observational flux database and discuss the implication of flux data on global Hg budget. Mean Hg0 flux obtained by micrometeorological measurement did not appear to be significantly greater than the flux measured by dynamic flux chamber methods over unpolluted surfaces (p=0.16, one-tailed, Mann-Whitney U test). The spatio-temporal coverage of existing Hg0 flux measurements is highly heterogeneous with large data gaps existing in multiple continents (Africa, South Asia, Middle East, South America and Australia). The magnitude of evasion flux is strongly enhanced by human activities, particularly at contaminated sites. Hg0 flux observations in East Asia are comparatively larger in magnitude than the rest of the world, suggesting substantial reemission of previously deposited mercury from anthropogenic sources. Hg0 exchange over pristine surfaces (e.g., background soil and water) and vegetation need better constrains for global analysis of atmospheric Hg budget. The existing knowledge gap and the associated research needs for future measurements and modeling efforts for the air-surface exchange of Hg0 are discussed.


2010 ◽  
Vol 3 (1) ◽  
pp. 187-208 ◽  
Author(s):  
V. Wolff ◽  
I. Trebs ◽  
C. Ammann ◽  
F. X. Meixner

Abstract. The aerodynamic gradient method is widely used for flux measurements of ammonia, nitric acid, particulate ammonium nitrate (the NH3-HNO3-NH4NO3 triad) and other water-soluble reactive trace compounds. The surface exchange flux is derived from a measured concentration difference and micrometeorological quantities (turbulent exchange coefficient). The significance of the measured concentration difference is crucial for the significant determination of surface exchange fluxes. Additionally, measurements of surface exchange fluxes of ammonia, nitric acid and ammonium nitrate are often strongly affected by phase changes between gaseous and particulate compounds of the triad, which make measurements of the four individual species (NH3, HNO3, NH4+, NO3− necessary for a correct interpretation of the measured concentration differences. We present here a rigorous analysis of results obtained with a multi-component, wet-chemical instrument, able to simultaneously measure gradients of both gaseous and particulate trace substances. Basis for our analysis are two field experiments, conducted above contrasting ecosystems (grassland, forest). Precision requirements of the instrument as well as errors of concentration differences and micrometeorological exchange parameters have been estimated, which, in turn, allows the establishment of thorough error estimates of the derived fluxes of NH3, HNO3, NH4+, and NO3−. Derived median flux errors for the grassland and forest field experiments were: 39% and 50% (NH3), 31% and 38% (HNO3), 62% and 57% (NH4+), and 47% and 68% (NO3−), respectively. Additionally, we provide the basis for using field data to characterize the instrument performance, as well as subsequent quantification of surface exchange fluxes and underlying mechanistic processes under realistic ambient measurement conditions.


2016 ◽  
Vol 9 (7) ◽  
pp. 2947-2959 ◽  
Author(s):  
Maxime Hervo ◽  
Yann Poltera ◽  
Alexander Haefele

Abstract. Imperfections in a lidar's overlap function lead to artefacts in the background, range and overlap-corrected lidar signals. These artefacts can erroneously be interpreted as an aerosol gradient or, in extreme cases, as a cloud base leading to false cloud detection. A correct specification of the overlap function is hence crucial in the use of automatic elastic lidars (ceilometers) for the detection of the planetary boundary layer or of low cloud. In this study, an algorithm is presented to correct such artefacts. It is based on the assumption of a homogeneous boundary layer and a correct specification of the overlap function down to a minimum range, which must be situated within the boundary layer. The strength of the algorithm lies in a sophisticated quality-check scheme which allows the reliable identification of favourable atmospheric conditions. The algorithm was applied to 2 years of data from a CHM15k ceilometer from the company Lufft. Backscatter signals corrected for background, range and overlap were compared using the overlap function provided by the manufacturer and the one corrected with the presented algorithm. Differences between corrected and uncorrected signals reached up to 45 % in the first 300 m above ground. The amplitude of the correction turned out to be temperature dependent and was larger for higher temperatures. A linear model of the correction as a function of the instrument's internal temperature was derived from the experimental data. Case studies and a statistical analysis of the strongest gradient derived from corrected signals reveal that the temperature model is capable of a high-quality correction of overlap artefacts, in particular those due to diurnal variations. The presented correction method has the potential to significantly improve the detection of the boundary layer with gradient-based methods because it removes false candidates and hence simplifies the attribution of the detected gradients to the planetary boundary layer. A particularly significant benefit can be expected for the detection of shallow stable layers typical of night-time situations. The algorithm is completely automatic and does not require any on-site intervention but requires the definition of an adequate instrument-specific configuration. It is therefore suited for use in large ceilometer networks.


2006 ◽  
Vol 21 (22) ◽  
pp. 1761-1768 ◽  
Author(s):  
S. DEV ◽  
SANJEEV KUMAR ◽  
SURENDER VERMA

We perform the most general model-independent analysis of the latest 391-Day Salt Phase SNO Data Set incorporating the super-Kamiokande ES flux measurement and obtain bounds on the antineutrino and sterile neutrino flux in the solar 8 B neutrino flux reaching the detectors on the earth. The muon/tauon antineutrino flux is found to be disallowed at 1.4σ C.L. The sterile flux is found to be nonzero at about 1.26 standard deviations.


Geophysics ◽  
2009 ◽  
Vol 74 (6) ◽  
pp. WCB1-WCB10 ◽  
Author(s):  
Cédric Taillandier ◽  
Mark Noble ◽  
Hervé Chauris ◽  
Henri Calandra

Classical algorithms used for traveltime tomography are not necessarily well suited for handling very large seismic data sets or for taking advantage of current supercomputers. The classical approach of first-arrival traveltime tomography was revisited with the proposal of a simple gradient-based approach that avoids ray tracing and estimation of the Fréchet derivative matrix. The key point becomes the derivation of the gradient of the misfit function obtained by the adjoint-state technique. The adjoint-state method is very attractive from a numerical point of view because the associated cost is equivalent to the solution of the forward-modeling problem, whatever the size of the input data and the number of unknown velocity parameters. An application on a 2D synthetic data set demonstrated the ability of the algorithm to image near-surface velocities with strong vertical and lateral variations and revealed the potential of the method.


2018 ◽  
Vol 14 (2) ◽  
pp. 233-258 ◽  
Author(s):  
Efthimia Mavridou ◽  
Konstantinos M. Giannoutakis ◽  
Dionysios Kehagias ◽  
Dimitrios Tzovaras ◽  
George Hassapis

Purpose Semantic categorization of Web services comprises a fundamental requirement for enabling more efficient and accurate search and discovery of services in the semantic Web era. However, to efficiently deal with the growing presence of Web services, more automated mechanisms are required. This paper aims to introduce an automatic Web service categorization mechanism, by exploiting various techniques that aim to increase the overall prediction accuracy. Design/methodology/approach The paper proposes the use of Error Correcting Output Codes on top of a Logistic Model Trees-based classifier, in conjunction with a data pre-processing technique that reduces the original feature-space dimension without affecting data integrity. The proposed technique is generalized so as to adhere to all Web services with a description file. A semantic matchmaking scheme is also proposed for enabling the semantic annotation of the input and output parameters of each operation. Findings The proposed Web service categorization framework was tested with the OWLS-TC v4.0, as well as a synthetic data set with a systematic evaluation procedure that enables comparison with well-known approaches. After conducting exhaustive evaluation experiments, categorization efficiency in terms of accuracy, precision, recall and F-measure was measured. The presented Web service categorization framework outperformed the other benchmark techniques, which comprise different variations of it and also third-party implementations. Originality/value The proposed three-level categorization approach is a significant contribution to the Web service community, as it allows the automatic semantic categorization of all functional elements of Web services that are equipped with a service description file.


Geophysics ◽  
2014 ◽  
Vol 79 (1) ◽  
pp. J1-J9 ◽  
Author(s):  
Meixia Geng ◽  
Qingjie Yang ◽  
Yuan Yuan

Geophysical data have to be modeled on a regular grid for various numerical procedures. However, airborne data tend to be collected with fine spacing along traverses but with much coarser spacing between traverses. Gridding only honors flight-line data when the mesh size is close to the sample spacing; otherwise, high-frequency information is always lost, which creates aliasing artifacts. For example, linear trends at an acute angle with respect to flight lines are imaged as “bull’s-eyes,” which resemble a boudinage at line intersections. The presence of boudinage artifacts can significantly distort anomalies of interest and thus lead to incorrect interpretation of shapes or sizes of causative bodies. We evaluated a method called constrained coherence-enhancing diffusion filtering that only diffuses the image in specific areas where strong anisotropy is detected. This method was tested on synthetic and field data set. Results indicated that the method can be efficiently used to enhance linear structure in multiple local directions. The images derived from this grid, such as the vertical gradient map, are also significantly improved. The original line data are honored by the constraints applied. We also used a field data set to compare the proposed approach with the approach used when diffusion is applied uniformly in all areas, irrespective of anisotropy. The proposed method was proven to produce better results with fewer artifacts.


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