scholarly journals Tropospheric mercury vertical profiles between 500 and 10 000 m in central Europe

2015 ◽  
Vol 15 (20) ◽  
pp. 28217-28247 ◽  
Author(s):  
A. Weigelt ◽  
R. Ebinghaus ◽  
N. Pirrone ◽  
J. Bieser ◽  
J. Bödewadt ◽  
...  

Abstract. Measurements of the vertical distribution of atmospheric mercury (Hg) are rare, because airborne measurements are expensive and labour intensive. Consequently, only a few vertical Hg profile measurements have been reported since the 1970s. Besides the CARIBIC passenger aircraft observations, the latest vertical profile over Europe was measured in 1996. Within the Global Mercury Observation System (GMOS) project four vertical profiles were taken on board research aircraft (CASA-212) in August 2013 in background air over different locations in Slovenia and Germany. Each vertical profile consists of at least seven 5 min horizontal flight sections from 500 m above ground to 3000 m a.s.l. Gaseous elemental mercury (GEM) was measured with a Tekran 2537X analyser and a Lumex RA-915-AM. Total gaseous mercury (TGM) was measured using a Tekran 2537B analyser and gaseous oxidized mercury (GOM) was sampled onto 8 denuders for post flight analysis (one for each profile, three during the transfer flights, and two blanks). In addition to the mercury measurements, SO2, CO, O3, NO, NO2, as well as basic meteorological parameters (pressure, temperature, relative humidity) have been measured. Additional ground based speciated mercury measurements at the GMOS master site in Waldhof (Germany) were used to extend the profile to the ground. No vertical gradient was found inside the well mixed boundary layer (variation by less than 0.1 ng m-3) at different sites with GEM varying from location to location between 1.4 and 1.6 ng m-3 (STP; standard conditions: p = 1013.25 hPa, T = 273.15 K). At all locations GEM dropped to 1.3 ng m-3 (STP) when entering the free troposphere and remained constant at higher altitudes. The combination of the vertical profile, measured on 21 August 2013, over Leipzig (Germany) with the CARIBIC measurements during ascent and descent to Frankfurt airport (Germany) at approximately the same time provide a unique central European vertical profile from inside the boundary layer (550 m a.s.l.) to the upper free troposphere (10 500 m a.s.l.) and shows a fairly constant free tropospheric TGM concentration of 1.3 ng m-3 (STP). The highest GOM concentrations of up to 60 pg m-3 (STP, denuder samples) were found above the boundary layer during the transfer flights.

2016 ◽  
Vol 16 (6) ◽  
pp. 4135-4146 ◽  
Author(s):  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
Nicola Pirrone ◽  
Johannes Bieser ◽  
Jan Bödewadt ◽  
...  

Abstract. The knowledge of the vertical distribution of atmospheric mercury (Hg) plays an important role in determining the transport and cycling of mercury. However, measurements of the vertical distribution are rare, because airborne measurements are expensive and labour intensive. Consequently, only a few vertical Hg profile measurements have been reported since the 1970s. Besides the Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC) observations, the latest vertical profile over Europe was measured in 1996. Within the Global Mercury Observation System (GMOS) project, four vertical profiles were taken on board research aircraft (CASA-212) in August 2013 in background air over different locations in Slovenia and Germany. Each vertical profile consists of at least seven 5 min horizontal flight sections from 500 m above ground to 3000 m a.s.l. Gaseous elemental mercury (GEM) and total gaseous mercury (TGM) were measured with Tekran 2537X and Tekran 2537B analysers. In addition to the mercury measurements, SO2, CO, O3, NO, and NO2, basic meteorological parameters (pressure, temperature, relative humidity) have been measured. Additional ground-based mercury measurements at the GMOS master site in Waldhof, Germany and measurements onboard the CARIBIC passenger aircraft were used to extend the profile to the ground and upper troposphere respectively. No vertical gradient was found inside the well-mixed boundary layer (variation of less than 0.1 ng m−3) at different sites, with GEM varying from location to location between 1.4 and 1.6 ng m−3 (standard temperature and pressure, STP: T  =  273.15 K, p  =  1013.25 hPa). At all locations GEM dropped to 1.3 ng m−3 (STP) when entering the free troposphere and remained constant at higher altitudes. The combination of the vertical profile, measured on 21 August 2013 over Leipzig, Germany, with the CARIBIC measurements during ascent and descent to Frankfurt Airport, Germany, taken at approximately the same time, provide a unique central European vertical profile from inside the boundary layer (550 m a.s.l) to the upper free troposphere (10 500 m a.s.l.) and show a fairly constant free-tropospheric TGM concentration of 1.3 ng m−3 (STP).


2019 ◽  
Author(s):  
Olivia E. Salmon ◽  
Lisa R. Welp ◽  
Michael Baldwin ◽  
Kristian Hajny ◽  
Brian H. Stirm ◽  
...  

Abstract. We use H2Ov isotopic vertical profile measurements and complementary meteorological observations to examine how boundary layer, cloud, and mixing processes influence the vertical structure of deuterium-excess (d-excess = δD – 8 × δ18O) in the boundary layer, inversion layer, and lower free troposphere. Airborne measurements of water vapor (H2Ov) stable isotopologues were conducted around two continental U.S. cities in February–March 2016. Nine research flights were designed to characterize the δD, δ18O, and d-excess vertical profiles extending from the surface to ≤ 2 km. We examine observations from three unique case study flights in detail. One case study shows H2Ov isotopologue vertical profiles that are consistent with Rayleigh isotopic distillation theory coinciding with clear skies, dry adiabatic lapse rates within the boundary layer, and relatively constant vertical profiles of wind speed and wind direction. The two remaining case studies show that H2Ov isotopic signatures above the boundary layer are sensitive to cloud processes and complex air mass mixing patterns. These two case studies indicate anomalies in the d-excess signature relative to Rayleigh theory, such as low d-excess values at the interface of the inversion layer and the free troposphere, which is possibly indicative of cloud evaporation. We discuss possible explanations for the observed d-excess anomalies, such as cloud evaporation, wind shear, and vertical mixing. In situ H2Ov stable isotope measurements, and d-excess in particular, could be useful for improving our understanding of moisture processing and transport mixing occurring between the boundary layer, inversion layer, and free troposphere.


2019 ◽  
Vol 19 (17) ◽  
pp. 11525-11543 ◽  
Author(s):  
Olivia E. Salmon ◽  
Lisa R. Welp ◽  
Michael E. Baldwin ◽  
Kristian D. Hajny ◽  
Brian H. Stirm ◽  
...  

Abstract. We use airborne measurements of water vapor (H2Ov) stable isotopologues and complementary meteorological observations to examine how boundary layer (BL) dynamics, cloud processing, and atmospheric mixing influence the vertical structure of δD, δ18O, and deuterium excess (d excess =δD–8×δ18O) in the BL, inversion layer (INV), and lower free troposphere (FT). Flights were conducted around two continental US cities in February–March 2016 and included vertical profiles extending from near the surface to ≤2 km. We examine observations from three unique case study flights in detail. One case study shows observations that are consistent with Rayleigh isotopic distillation theory coinciding with clear skies, dry adiabatic lapse rates within the boundary layer, and relatively constant vertical profiles of wind speed and wind direction. This suggests that the air mass retained the isotopic fingerprint of dehydration during moist adiabatic processes upwind of the study area. Also, observed d-excess values in the free troposphere were sometimes larger than Rayleigh theory predicts, which may indicate mixing of extremely dehydrated air from higher altitudes. The two remaining case studies show isotopic anomalies in the d-excess signature relative to Rayleigh theory and indicate cloud processes and complex boundary layer development. The most notable case study with stratocumulus clouds present had extremely low (negative) d-excess values at the interface of the inversion layer and the free troposphere, which is possibly indicative of cloud or rain droplet evaporation. We discuss how in situ H2Ov stable isotope measurements, and d excess in particular, could be useful for improving our understanding of water phase changes, transport, and mixing that occurs between the BL, INV, and FT.


2014 ◽  
Vol 7 (9) ◽  
pp. 3127-3138 ◽  
Author(s):  
R. L. Herman ◽  
J. E. Cherry ◽  
J. Young ◽  
J. M. Welker ◽  
D. Noone ◽  
...  

Abstract. The EOS (Earth Observing System) Aura Tropospheric Emission Spectrometer (TES) retrieves the atmospheric HDO / H2O ratio in the mid-to-lower troposphere as well as the planetary boundary layer. TES observations of water vapor and the HDO isotopologue have been compared with nearly coincident in situ airborne measurements for direct validation of the TES products. The field measurements were made with a commercially available Picarro L1115-i isotopic water analyzer on aircraft over the Alaskan interior boreal forest during the three summers of 2011 to 2013. TES special observations were utilized in these comparisons. The TES averaging kernels and a priori constraints have been applied to the in situ data, using version 5 (V005) of the TES data. TES calculated errors are compared with the standard deviation (1σ) of scan-to-scan variability to check consistency with the TES observation error. Spatial and temporal variations are assessed from the in situ aircraft measurements. It is found that the standard deviation of scan-to-scan variability of TES δD is ±34.1‰ in the boundary layer and ± 26.5‰ in the free troposphere. This scan-to-scan variability is consistent with the TES estimated error (observation error) of 10–18‰ after accounting for the atmospheric variations along the TES track of ±16‰ in the boundary layer, increasing to ±30‰ in the free troposphere observed by the aircraft in situ measurements. We estimate that TES V005 δD is biased high by an amount that decreases with pressure: approximately +123‰ at 1000 hPa, +98‰ in the boundary layer and +37‰ in the free troposphere. The uncertainty in this bias estimate is ±20‰. A correction for this bias has been applied to the TES HDO Lite Product data set. After bias correction, we show that TES has accurate sensitivity to water vapor isotopologues in the boundary layer.


2018 ◽  
Vol 176 ◽  
pp. 05025 ◽  
Author(s):  
Michail Mytilinaios ◽  
Alexandros Papayannis ◽  
Georgios Tsaknakis

A compact ozone differential absorption lidar (DIAL) was implemented at the Laboratory of Laser Remote Sensing of the National Technical University of Athens (NTUA), in Athens, Greece. The DIAL system is based on a Nd:YAG laser emitting at 266 nm. A high-pressure Raman cell, filled with D2, was used to generate the λON and λOFF laser wavelength pairs (i.e., 266-289 nm and 289-316 nm, respectively) based on the Stimulated Raman Scattering (SRS) effect. The system was run during daytime and nighttime conditions to obtain the vertical profile of tropospheric ozone in the Planetary Boundary Layer (PBL) and the adjacent free troposphere.


2020 ◽  
Author(s):  
Mo Wang ◽  
Baiqing Xu ◽  
Song Yang ◽  
Jing Gao ◽  
Taihua Zhang ◽  
...  

<p>Black carbon (BC) can change the energy budget of the earth system by strongly absorbing solar radiation: both suspended in the atmosphere, incorporated into cloud droplets, or deposited onto high-albedo surfaces. BC’s direct radiative forcing is highly dependent on its vertical distribution. However, due to large variabilities and the small number of vertical profile measurements, there is still large uncertainty in this forcing value. Moreover, the vertical profile of BC and its relative elevation to clouds determine BC’s lifetime in the atmosphere and its transport and removal processes. In November-December 2017, a series of tethered balloon flights was launched at the Southeast Tibet Observation and Research Station for the Alpine Environment of the Chinese Academy of Sciences. A cylindrical balloon with a diameter of 7.9 m and maximum volume of 1250 m<sup>3</sup> was used. A 7-channel Aethalometer was installed in the gondola attached to the balloon, together with several other instruments including a GPS for altitude, and sensors for temperature and relative humidity. The airborne Aethalometer measured BC mass concentration (ng/m<sup>3</sup>) on a on a 1-second timebase at 7 wavelengths ranging from 370 nm to 950 nm. Meanwhile, another Aethalometer was used to monitor BC mass concentration near the surface, at a height of about 10 m above the ground. From the tethered balloon flights, we derived three profiles designated as ‘F1’, ‘F3-ASC’, and ‘F3-DES’. The maximum height for the F1 flight was 500 m a.g.l., namely 3800 m a.s.l.; while the maximum height for the F3 flight was 1950 m a.g.l., namely 5250 m a.s.l. Based on the potential temperature and relative humidity data, the profiles were divided into three layers: the stable boundary layer (SBL), the residual layer (RL), and the free troposphere (FT). The vertical distribution of BC shows a prominent peak within the SBL. The mean BC concentration in SBL (1000±750 ng/m<sup>3</sup>) was one order of magnitude higher than in RL and FT, which were 140±40 ng/m<sup>3</sup> and 120±40 ng/m<sup>3</sup>, respectively. The BC concentration measured in the present study in FT over the southeastern Tibetan Plateau is comparable to measurements in Arctic regions, but lower than values in South Asia. Analysis of the wavelength dependence of the data yields an estimate of the biomass burning contribution. This showed a maximum value in SBL of 44±37%, and was 16±6% in RL and 13±5% in FT. Analysis of 24-hour isentropic back trajectories showed that BC in SBL and RL was dominated by local sources, while in the FT, BC is mainly influenced by mid- to long-distant transport by the westerlies. In addition, analysis of the variations of BC concentration and biomass burning contribution on a high-resolution time scale showed that BC concentrations and the nature of their sources are largely influenced by air mass origins and transport. To our knowledge, this is the first ever in situ measurement of BC concentration over the Tibetan Plateau in the atmospheric boundary layer and free troposphere up to 5000 m a.s.l.</p>


2016 ◽  
Vol 16 (6) ◽  
pp. 3743-3760 ◽  
Author(s):  
Sean Coburn ◽  
Barbara Dix ◽  
Eric Edgerton ◽  
Christopher D. Holmes ◽  
Douglas Kinnison ◽  
...  

Abstract. The elevated deposition of atmospheric mercury over the southeastern United States is currently not well understood. Here we measure partial columns and vertical profiles of bromine monoxide (BrO) radicals, a key component of mercury oxidation chemistry, to better understand the processes and altitudes at which mercury is being oxidized in the atmosphere. We use data from a ground-based MAX-DOAS instrument located at a coastal site ∼  1 km from the Gulf of Mexico in Gulf Breeze, FL, where we had previously detected tropospheric BrO (Coburn et al., 2011). Our profile retrieval assimilates information about stratospheric BrO from the WACCM chemical transport model (CTM), and uses only measurements at moderately low solar zenith angles (SZAs) to estimate the BrO slant column density contained in the reference spectrum (SCDRef). The approach has 2.6 degrees of freedom, and avoids spectroscopic complications that arise at high SZA; knowledge about SCDRef further helps to maximize sensitivity in the free troposphere (FT). A cloud-free case study day with low aerosol load (9 April 2010) provided optimal conditions for distinguishing marine boundary layer (MBL: 0–1 km) and free-tropospheric (FT: 1–15 km) BrO from the ground. The average daytime tropospheric BrO vertical column density (VCD) of ∼  2.3  ×  1013 molec cm−2 (SZA  <  70°) is consistent with our earlier reports on other days. The vertical profile locates essentially all tropospheric BrO above 4 km, and shows no evidence for BrO inside the MBL (detection limit  <  0.5 pptv). BrO increases to  ∼  3.5 pptv at 10–15 km altitude, consistent with recent aircraft observations. Our case study day is consistent with recent aircraft studies, in that the oxidation of gaseous elemental mercury (GEM) by bromine radicals to form gaseous oxidized mercury (GOM) is the dominant pathway for GEM oxidation throughout the troposphere above Gulf Breeze. The column integral oxidation rates are about 3.6  × 105 molec cm−2 s−1 for bromine, while the contribution from ozone (O3) is 0.8  ×  105 molec cm−2 s−1. Chlorine-induced oxidation is estimated to add  <  5 % to these mercury oxidation rates. The GOM formation rate is sensitive to recently proposed atmospheric scavenging reactions of the HgBr adduct by nitrogen dioxide (NO2), and to a lesser extent also HO2 radicals. Using a 3-D CTM, we find that surface GOM variations are also typical of other days, and are mainly derived from the FT. Bromine chemistry is active in the FT over Gulf Breeze, where it forms water-soluble GOM that is subsequently available for wet scavenging by thunderstorms or transport to the boundary layer.


2010 ◽  
Vol 10 (5) ◽  
pp. 13609-13642 ◽  
Author(s):  
J. E. Dibb ◽  
L. D. Ziemba ◽  
J. Luxford ◽  
P. Beckman

Abstract. Measurements of gas phase soluble bromide in the boundary layer and in firn air, and Br− in aerosol and snow, were made at Summit, Greenland (72.5° N, 38.4° W, 3200 m a.s.l.) as part of a larger investigation into the influence of Br chemistry on HOx cycling. The soluble bromide measurements confirm that photochemical activation of Br− in the snow causes release of active Br to the overlying air despite trace concentrations of Br− in the snow (means 15 and 8 nmol Br− kg−1 of snow in 2007 and 2008, respectively). Mixing ratios of soluble bromide above the snow were also found to be very small (mean <1 ppt both years, with maxima of 3 and 4 ppt in 2007 and 2008, respectively), but these levels clearly oxidize and deposit long-lived gaseous elemental mercury and may perturb HOx partitioning. Concentrations of Br− in surface snow tended to increase/decrease in parallel with the specific activities of the aerosol-associated radionuclides 7Be and 210Pb. Earlier work has shown that ventilation of the boundary layer causes simultaneous increases in 7Be and 210Pb at Summit, suggesting there is a pool of Br in the free troposphere above Summit in summer time. Speciation and the source of this free tropospheric Br are not well constrained, but we suggest it may be linked to extensive regions of active Br chemistry in the Arctic basin which are known to cause ozone and mercury depletion events shortly after polar sunrise. If this hypothesis is correct, it implies persistence of the free troposphere Br− for several months after peak Br activation in March/April. Alternatively, there may be a~ubiquitous pool of Br− in the free troposphere, sustained by currently unknown sources and processes.


2012 ◽  
Vol 12 (5) ◽  
pp. 11539-11566 ◽  
Author(s):  
L. Haszpra ◽  
M. Ramonet ◽  
M. Schmidt ◽  
Z. Barcza ◽  
Z. Pátkai ◽  
...  

Abstract. Eight years of occasional flask air sampling and 3 yr of frequent in situ measurements of carbon dioxide (CO2) vertical profiles on board of a small aircraft, over a tall tower greenhouse gases monitoring site in Hungary are used for the analysis of the variations of vertical profile of CO2 mole fraction. Using the airborne vertical profiles and the measurements along the 115 m tall tower it is shown that the measurements at the top of the tower estimate the mean boundary layer CO2 mole fraction during the mid-afternoon fairly well, with an underestimation of 0.27–0.85 μmol mol−1 in summer, and an overestimation of 0.66–1.83 μmol mol−1 in winter. The seasonal cycle of CO2 mole fraction is damped with elevation. While the amplitude of the seasonal cycle is 28.5 μmol mol−1 at 10 m above the ground, it is only 10.7 μmol mol−1 in the layer of 2500–3000 m corresponding to the lower free atmosphere above the well-mixed boundary layer. The maximum mole fraction in the layer of 2500–3000 m can be observed around 25 March on average, two weeks ahead of that of the marine boundary layer reference (GLOBALVIEW). By contrast, close to the ground, the maximum CO2 mole fraction is observed late December, early January. The specific seasonal behavior is attributed to the climatology of vertical mixing of the atmosphere in the Carpathian Basin.


2010 ◽  
Vol 10 (6) ◽  
pp. 15167-15196
Author(s):  
J. R. Spackman ◽  
R. S. Gao ◽  
W. D. Neff ◽  
J. P. Schwarz ◽  
L. A. Watts ◽  
...  

Abstract. Understanding the processes controlling black carbon (BC) in the Arctic is crucial for evaluating the impact of anthropogenic and natural sources of BC on Arctic climate. Vertical profiles of BC mass were observed from the surface to near 7-km altitude in April 2008 using a Single-Particle Soot Photometer (SP2) during flights on the NOAA WP-3D research aircraft from Fairbanks, Alaska. These measurements were conducted during the NOAA-sponsored Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project as part of POLARCAT, an International Polar Year (IPY) activity. In the free troposphere, the Arctic air mass was influenced by long-range transport from biomass-burning and anthropogenic source regions at lower latitudes especially during the latter part of the campaign. Maximum average BC mass loadings of 150 ng kg−1 were observed near 5.5-km altitude in the aged Arctic air mass. In biomass-burning plumes, BC was enhanced from near the top of the Arctic boundary layer (ABL) to 5.5 km compared to the aged Arctic air mass. At the bottom of some of the profiles, positive vertical gradients in BC were observed in the vicinity of open leads in the sea-ice. BC mass loadings increased by about a factor of two across the boundary layer transition in the ABL in these cases while carbon monoxide (CO) remained constant, evidence for depletion of BC in the ABL. BC mass loadings were positively correlated with O3 in ozone depletion events (ODEs) for all the observations in the ABL suggesting that BC was removed by dry deposition of BC on the snow or ice because molecular bromine, Br2, which photolyzes and catalytically destroys O3, is thought to be released near the open leads in regions of ice formation. We estimate the deposition flux of BC mass to the snow using a box model constrained by the vertical profiles of BC in the ABL. The open leads may increase vertical mixing in the ABL and entrainment of pollution from the free troposphere possibly enhancing the deposition of BC to the snow.


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