scholarly journals Observations of iodine monoxide over three summers at the Indian Antarctic bases of Bharati and Maitri

2021 ◽  
Vol 21 (15) ◽  
pp. 11829-11842
Author(s):  
Anoop S. Mahajan ◽  
Mriganka S. Biswas ◽  
Steffen Beirle ◽  
Thomas Wagner ◽  
Anja Schönhardt ◽  
...  

Abstract. Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone in West Antarctica. Here, we present MAX-DOAS-based (multi-axis differential absorption spectroscopy) observations of IO over three summers (2015–2017) at the Indian Antarctic bases of Bharati and Maitri. IO was observed during all the campaigns with mixing ratios below 2 pptv (parts per trillion by volume) for the three summers, which are lower than the peak levels observed in West Antarctica. This suggests that sources in West Antarctica are different or stronger than sources of iodine compounds in East Antarctica, the nature of which is still uncertain. Vertical profiles estimated using a profile retrieval algorithm showed decreasing gradients with a peak in the lower boundary layer. The ground-based instrument retrieved vertical column densities (VCDs) were approximately a factor of 3 to 5 higher than the VCDs reported using satellite-based instruments, which is most likely related to the sensitivities of the measurement techniques. Air mass back-trajectory analysis failed to highlight a source region, with most of the air masses coming from coastal or continental regions. This study highlights the variation in iodine chemistry in different regions in Antarctica and the importance of a long-term dataset to validate models estimating the impacts of iodine chemistry.

2020 ◽  
Author(s):  
Anoop S. Mahajan ◽  
Mriganka S. Biswas ◽  
Steffen Beirle ◽  
Thomas Wagner ◽  
Anja Schönhardt ◽  
...  

Abstract. Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone in West Antarctica. Here, we present multi axis differential absorption spectroscopy (MAX-DOAS) based observations of IO over three summers (2015–2017) at the Indian Antarctic bases, Bharati and Maitri. IO was observed during all the campaigns, with mixing ratios below 2 pptv for the three summers, which are lower than the peak levels observed in West Antarctica. This suggests that sources in West Antarctica are different or stronger than sources of iodine compounds in East Antarctica. Vertical profiles estimated using a profile retrieval algorithm showed decreasing gradients, with a peak in the lower boundary layer. The ground-based instrument retrieved vertical column densities (VCDs) were approximately a factor of three-five higher than the VCDs reported using satellite-based instruments, which is most likely related to the sensitivities of the measurement techniques. Airmass back-trajectory analysis failed to highlight a source region, with most of the airmasses coming from coastal or continental regions. This study highlights the variation in iodine chemistry in different regions in Antarctica and the importance of a long-term dataset to validate models estimating the impacts of iodine chemistry.


2021 ◽  
Author(s):  
Anoop Mahajan ◽  
Mriganka Biswas ◽  
Steffen Beirle ◽  
Thomas Wagner ◽  
Anja Schönhardt ◽  
...  

<p> Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone in West Antarctica. However, observations across Antarctica are still rare, and have hitherto been mostly focused on the West Antarctic, which needs to be addressed in order for comprehensive model validation. Here, we present multi axis differential absorption spectroscopy (MAX-DOAS) based observations of IO over three summers (2015-2017) at the Indian Antarctic bases, Bharati and Maitri. IO was observed during all the campaigns, with mixing ratios below 2 pptv for the three summers, which are lower than the peak levels observed in West Antarctica. This suggests that sources in West Antarctica are different or stronger than sources of iodine compounds in East Antarctica. Vertical profiles estimated using a profile retrieval algorithm showed decreasing gradients, with a peak in the lower boundary layer. The ground-based instrument retrieved vertical column densities (VCDs) were approximately a factor of three-five higher than the VCDs reported using satellite-based instruments, which is most likely related to the sensitivities of the measurement techniques. Airmass back-trajectory analysis failed to highlight a source region, with most of the airmasses coming from coastal or continental regions. This study adds to the sparse observational database of iodine compounds in Antarctica and highlights the variation in iodine chemistry in different regions in Antarctica. It also shines light on the needs of more long-term datasets in different regions to validate models estimating the impacts of iodine chemistry across Antarctica.</p>


2011 ◽  
Vol 11 (23) ◽  
pp. 12475-12498 ◽  
Author(s):  
J. D. Halla ◽  
T. Wagner ◽  
S. Beirle ◽  
J. R. Brook ◽  
K. L. Hayden ◽  
...  

Abstract. Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed in a rural location of southwestern Ontario during the Border Air Quality and Meteorology Study. Slant column densities (SCDs) of NO2 and O4 were determined using the standard DOAS technique. Using a radiative transfer model and the O4 SCDs, aerosol optical depths were determined for clear sky conditions and compared to OMI, MODIS, AERONET, and local PM2.5 measurements. This aerosol information was input to a radiative transfer model to calculate NO2 air mass factors, which were fit to the measured NO2 SCDs to determine tropospheric vertical column densities (VCDs) of NO2. The method of determining NO2 VCDs in this way was validated for the first time by comparison to composite VCDs derived from aircraft and ground-based measurements of NO2. The new VCDs were compared to VCDs of NO2 determined via retrievals from the satellite instruments SCIAMACHY and OMI, for overlapping time periods. The satellite-derived VCDs were higher, with a mean bias of +0.5–0.9×1015 molec cm−2. This last finding is different from previous studies whereby MAX-DOAS geometric VCDs were higher than satellite determinations, albeit for urban areas with higher VCDs. An effective boundary layer height, BLHeff, is defined as the ratio of the tropospheric VCD and the ground level concentration of NO2. Variations of BLHeff can be linked to time of day, source region, stability of the atmosphere, and the presence or absence of elevated NOx sources. In particular, a case study is shown where a high VCD and BLHeff were observed when an elevated industrial plume of NOx and SO2 was fumigated to the surface as a lake breeze impacted the measurement site. High BLHeff values (~1.9 km) were observed during a regional smog event when high winds from the SW and high convection promoted mixing throughout the boundary layer. During this event, the regional line flux of NO2 through the region was estimated to be greater than 112 kg NO2 km−1 h−1.


2015 ◽  
Vol 15 (1) ◽  
pp. 223-240 ◽  
Author(s):  
S. J. Lawson ◽  
P. W. Selleck ◽  
I. E. Galbally ◽  
M. D. Keywood ◽  
M. J. Harvey ◽  
...  

Abstract. The dicarbonyls glyoxal and methylglyoxal have been measured with 2,4-dinitrophenylhydrazine (2,4-DNPH) cartridges and high-performance liquid chromatography (HPLC), optimised for dicarbonyl detection, in clean marine air over the temperate Southern Hemisphere (SH) oceans. Measurements of a range of dicarbonyl precursors (volatile organic compounds, VOCs) were made in parallel. These are the first in situ measurements of glyoxal and methylglyoxal over the remote temperate oceans. Six 24 h samples were collected in summer (February–March) over the Chatham Rise in the south-west Pacific Ocean during the Surface Ocean Aerosol Production (SOAP) voyage in 2012, while 34 24 h samples were collected at Cape Grim Baseline Air Pollution Station in the late winter (August–September) of 2011. Average glyoxal mixing ratios in clean marine air were 7 ppt at Cape Grim and 23 ppt over Chatham Rise. Average methylglyoxal mixing ratios in clean marine air were 28 ppt at Cape Grim and 10 ppt over Chatham Rise. The mixing ratios of glyoxal at Cape Grim are the lowest observed over the remote oceans, while mixing ratios over Chatham Rise are in good agreement with other temperate and tropical observations, including concurrent Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations. Methylglyoxal mixing ratios at both sites are comparable to the only other marine methylglyoxal observations available over the tropical Northern Hemisphere (NH) ocean. Ratios of glyoxal : methylglyoxal > 1 over Chatham Rise but < 1 at Cape Grim suggest that a different formation and/or loss processes or rates dominate at each site. Dicarbonyl precursor VOCs, including isoprene and monoterpenes, are used to calculate an upper-estimate yield of glyoxal and methylglyoxal in the remote marine boundary layer and explain at most 1–3 ppt of dicarbonyls observed, corresponding to 10% and 17% of the observed glyoxal and 29 and 10% of the methylglyoxal at Chatham Rise and Cape Grim, respectively, highlighting a significant but as yet unknown production mechanism. Surface-level glyoxal observations from both sites were converted to vertical columns and compared to average vertical column densities (VCDs) from GOME-2 satellite retrievals. Both satellite columns and in situ observations are higher in summer than winter; however, satellite vertical column densities exceeded the surface observations by more than 1.5 × 1014 molecules cm−2 at both sites. This discrepancy may be due to the incorrect assumption that all glyoxal observed by satellite is within the boundary layer, or it may be due to challenges retrieving low VCDs of glyoxal over the oceans due to interferences by liquid water absorption or the use of an inappropriate normalisation reference value in the retrieval algorithm. This study provides much-needed data to verify the presence of these short-lived gases over the remote ocean and provide further evidence of an as yet unidentified source of both glyoxal and also methylglyoxal over the remote oceans.


2011 ◽  
Vol 11 (4) ◽  
pp. 13035-13097 ◽  
Author(s):  
J. D. Halla ◽  
T. Wagner ◽  
S. Beirle ◽  
J. R. Brook ◽  
K. L. Hayden ◽  
...  

Abstract. Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed in a rural location of southwestern Ontario during the Border Air Quality and Meteorology Study. Slant column densities (SCDs) of NO2 and O4 were determined using the standard DOAS technique. Using a radiative transfer model and the O4 SCDs, aerosol optical depths were determined for clear sky conditions and compared to OMI, MODIS, AERONET, and local PM2.5 measurements. This aerosol information was input to a radiative transfer model to calculate NO2 air mass factors, which were fit to the measured NO2 SCDs to determine tropospheric vertical column densities (VCDs) of NO2. The method of determining NO2 VCDs in this way was validated by comparison to composite VCDs derived from aircraft and ground-based measurements of NO2. The new VCDs were compared to VCDs of NO2 determined via the satellite instruments SCIAMACHY and OMI, for overlapping time periods. The satellite-derived VCDs were higher by 50%, with a mean positive error of 0.5–0.9 × 1015 molec cm−2. This last finding is different from previous studies whereby MAX-DOAS geometric VCDs were higher than satellite determinations, albeit for urban areas with higher VCDs. An effective boundary layer height, BLeff, is defined as the ratio of the tropospheric VCD and the ground level concentration of NO2. Variations of BLeff can be linked to time of day, source region, stability of the atmosphere, and the presence or absence of elevated NOx sources. In particular, a case study is shown where a high VCD and BLeff were observed when an elevated industrial plume of NOx and SO2 was fumigated to the surface as a lake breeze front impacted the measurement site. High BLeff values (~1.9 km) were observed during a regional smog event when high winds from the SW and high convection promoted mixing throughout the boundary layer. During this event, the regional line flux of NO2 through the region was estimated to be greater than 112 kg NO2 km−1 h−1.


2014 ◽  
Vol 14 (15) ◽  
pp. 21659-21708 ◽  
Author(s):  
S. J. Lawson ◽  
P. W. Selleck ◽  
I. E. Galbally ◽  
M. D. Keywood ◽  
M. J. Harvey ◽  
...  

Abstract. Dicarbonyls glyoxal and methylglyoxal have been measured with 2,4-dinitrophenylhydrazine (2,4-DNPH) cartridges and high performance liquid chromatography (HPLC), optimised for dicarbonyl detection, in clean marine air over the temperate Southern Hemisphere (SH) oceans. Measurements of a range of dicarbonyl precursors (volatile organic compounds, VOCs) were made in parallel. These are the first in situ measurements of glyoxal and methylglyoxal over the remote temperate oceans. Six 24 h samples were collected in late summer (February–March) over the Chatham Rise in the South West Pacific Ocean during the Surface Ocean Aerosol Production (SOAP) voyage in 2012, while 34 24 h samples were collected at Cape Grim Baseline Air Pollution Station in late winter (August–September) 2011. Average glyoxal mixing ratios in clean marine air were 7 ppt at Cape Grim, and 24 ppt over Chatham Rise. Average methylglyoxal mixing ratios in clean marine air were 28 ppt at Cape Grim and 12 ppt over Chatham Rise. The mixing ratios of glyoxal at Cape Grim are the lowest observed over the remote oceans, while mixing ratios over Chatham Rise are in good agreement with other temperate and tropical observations, including concurrent MAX-DOAS observations. Methylglyoxal mixing ratios at both sites are comparable to the only other marine methylglyoxal observations available over the tropical Northern Hemisphere (NH) ocean. Ratios of glyoxal : methylglyoxal > 1 over Chatham Rise but < 1 at Cape Grim, suggesting different formation and/or loss processes or rates dominate at each site. Dicarbonyl precursor VOCs, including isoprene and monoterpenes, are used to calculate an upper estimate yield of glyoxal and methylglyoxal in the remote marine boundary layer and explain at most 1–3 ppt of dicarbonyls observed, corresponding to 11 and 17% of the observed glyoxal and 28 and 10% of the methylglyoxal at Chatham Rise and Cape Grim, respectively, highlighting a significant but as yet unknown production mechanism. Glyoxal surface observations from both sites were converted to vertical columns and compared to average vertical column densities (VCDs) from GOME-2 satellite retrievals. Both satellite columns and in situ observations are higher in summer than winter, however satellite vertical column densities exceeded the surface observations by more than 1.5 × 1014 molecules cm−2 at both sites. This discrepancy may be due to the incorrect assumption that all glyoxal observed by satellite is within the boundary layer, or may be due to challenges retrieving low VCDs of glyoxal over the oceans due to interferences by liquid water absorption, or use of an inappropriate normalisation reference value in the retrieval algorithm. This study provides much needed data to verify the presence of these short lived gases over the remote ocean and provide further evidence of an as yet unidentified source of both glyoxal and also methylglyoxal over the remote oceans.


2014 ◽  
Vol 7 (3) ◽  
pp. 3021-3073 ◽  
Author(s):  
M. Grossi ◽  
P. Valks ◽  
D. Loyola ◽  
B. Aberle ◽  
S. Slijkhuis ◽  
...  

Abstract. The knowledge of the total column water vapour (TCWV) global distribution is fundamental for climate analysis and weather monitoring. In this work, we present the retrieval algorithm used to derive the operational TCWV from the GOME-2 sensors and perform an extensive inter-comparison and validation in order to estimate their absolute accuracy and long-term stability. We use the recently reprocessed data sets retrieved by the GOME-2 instruments aboard EUMETSAT's MetOp-A and MetOp-B satellites and generated by DLR in the framework of the O3M-SAF using the GOME Data Processor (GDP) version 4.7. The retrieval algorithm is based on a classical Differential Optical Absorption Spectroscopy (DOAS) method and combines H2O/O2 retrieval for the computation of the trace gas vertical column density. We introduce a further enhancement in the quality of the H2O column by optimizing the cloud screening and developing an empirical correction in order to eliminate the instrument scan angle dependencies. We evaluate the overall consistency between about 8 months measurements from the newer GOME-2 instrument on the MetOp-B platform with the GOME-2/MetOp-A data in the overlap period. Furthermore, we compare GOME-2 results with independent TCWV data from ECMWF and with SSMIS satellite measurements during the full period January 2007–August 2013 and we perform a validation against the combined SSM/I + MERIS satellite data set developed in the framework of the ESA DUE GlobVapour project. We find global mean biases as small as ± 0.03 g cm−2 between GOME-2A and all other data sets. The combined SSM/I-MERIS sample is typically drier than the GOME-2 retrievals (−0.005 g cm−2), while on average GOME-2 data overestimate the SSMIS measurements by only 0.028 g cm−2. However, the size of some of these biases are seasonally dependent. Monthly average differences can be as large as 0.1 g cm−2, based on the analysis against SSMIS measurements, but are not as evident in the validation with the ECMWF and the SSM/I + MERIS data. Studying two exemplary months, we estimate regional differences and identify a very good agreement between GOME-2 total columns and all three independent data sets, especially for land areas, although some discrepancies over ocean and over land areas with high humidity and a relatively large surface albedo are also present.


1986 ◽  
Vol 64 (6) ◽  
pp. 1295-1309 ◽  
Author(s):  
M. M. Chance ◽  
D. A. Craig

Detailed water flow around larvae of Simulium vittatum Zett. (sibling IS-7) was investigated using flow tanks, aluminium flakes, pigment, still photography, cinematography, and video recordings. Angle of deflection of a larva from the vertical has a hyperbolic relationship to water velocity. Velocity profiles around larvae show that the body is in the boundary layer. Frontal area of the body decreases as velocity increases. Disturbed larvae exhibit "avoidance reaction" and pull the body into the lower boundary layer. Longitudinal twisting and yawing of the larval body places one labral fan closer to the substrate, the other near the top of the boundary layer. Models and live larvae were used to demonstrate the basic hydrodynamic phenomenon of downstream paired vortices. Body shape and feeding stance result in one of the vortices remaining in the lower boundary layer. The other rises up the downstream side of the body, passes through the lower fan, then forms a von Karman trail of detaching vortices. This vortex entrains particulate matter from the substrate, which larvae then filter. Discharge of water into this upper vortex remains constant at various velocities and only water between the substrate and top of the posterior abdomen is incorporated into it. The upper fan filters water only from the top of the boundary layer. Formation of vortices probably influences larval microdistribution and filter feeding. Larvae positioned side by side across the flow mutually influence flow between them, thus enhancing feeding. Larvae downstream of one another may use information from the von Karman trail of vortices to position themselves advantageously.


2018 ◽  
Vol 18 (1) ◽  
pp. 3-48
Author(s):  
LMBC Campos ◽  
C Legendre

In this study, the propagation of waves in a two-dimensional parallel-sided nozzle is considered allowing for the combination of: (a) distinct impedances of the upper and lower walls; (b) upper and lower boundary layers with different thicknesses with linear shear velocity profiles matched to a uniform core flow; and (c) a uniform cross-flow as a bias flow out of one and into the other porous acoustic liner. The model involves an “acoustic triple deck” consisting of third-order non-sinusoidal non-plane acoustic-shear waves in the upper and lower boundary layers coupled to convected plane sinusoidal acoustic waves in the uniform core flow. The acoustic modes are determined from a dispersion relation corresponding to the vanishing of an 8 × 8 matrix determinant, and the waveforms are combinations of two acoustic and two sets of three acoustic-shear waves. The eigenvalues are calculated and the waveforms are plotted for a wide range of values of the four parameters of the problem, namely: (i/ii) the core and bias flow Mach numbers; (iii) the impedances at the two walls; and (iv) the thicknesses of the two boundary layers relative to each other and the core flow. It is shown that all three main physical phenomena considered in this model can have a significant effect on the wave field: (c) a bias or cross-flow even with small Mach number [Formula: see text] relative to the mean flow Mach number [Formula: see text] can modify the waveforms; (b) the possibly dissimilar impedances of the lined walls can absorb (or amplify) waves more or less depending on the reactance and inductance; (a) the exchange of the wave energy with the shear flow is also important, since for the same stream velocity, a thin boundary layer has higher vorticity, and lower vorticity corresponds to a thicker boundary layer. The combination of all these three effects (a–c) leads to a large set of different waveforms in the duct that are plotted for a wide range of the parameters (i–iv) of the problem.


2010 ◽  
Vol 10 (16) ◽  
pp. 7709-7722 ◽  
Author(s):  
G.-J. Roelofs ◽  
H. ten Brink ◽  
A. Kiendler-Scharr ◽  
G. de Leeuw ◽  
A. Mensah ◽  
...  

Abstract. In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the associated aerosol optical thickness (AOT) for the campaign period. Synoptic scale meteorology is represented realistically through nudging of the vorticity, the divergence, the temperature and the surface pressure. Simulated concentrations of aerosol sulfate and organics at the surface are generally within a factor of two from observed values. The monthly averaged AOT from the model is 0.33, about 20% larger than observed. For selected periods of the month with relatively dry and moist conditions discrepancies are approximately −30% and +15%, respectively. Discrepancies during the dry period are partly caused by inaccurate representation of boundary layer (BL) dynamics by the model affecting the simulated AOT. The model simulates too strong exchange between the BL and the free troposphere, resulting in weaker concentration gradients at the BL top than observed for aerosol and humidity, while upward mixing from the surface layers into the BL appears to be underestimated. The results indicate that beside aerosol sulfate and organics also aerosol ammonium and nitrate significantly contribute to aerosol water uptake. The simulated day-to-day variability of AOT follows synoptic scale advection of humidity rather than particle concentration. Even for relatively dry conditions AOT appears to be strongly influenced by the diurnal cycle of RH in the lower boundary layer, further enhanced by uptake and release of nitric acid and ammonia by aerosol water.


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