Clear-sky vertical profiles of trace gases as influenced by upstream convective activity

1989 ◽  
Vol 94 (D12) ◽  
pp. 14879-14892 ◽  
Author(s):  
Kenneth E. Pickering ◽  
Russell R. Dickerson ◽  
Winston T. Luke ◽  
Linda J. Nunnermacker
2021 ◽  
Author(s):  
Yvette Gramlich ◽  
Sophie Haslett ◽  
Karolina Siegel ◽  
Gabriel Freitas ◽  
Radovan Krejci ◽  
...  

<p>The number of cloud seeds, e.g. cloud condensation nuclei (CCN) and ice nucleation particles (INP), in the pristine Arctic shows a large range throughout the year, thereby influencing the radiative properties of Arctic clouds. However, little is known about the chemical properties of CCN and INP in this region. This study aims to investigate the chemical properties of aerosol particles and trace gases that are of importance for cloud formation in the Arctic environment, with focus on the organic fraction.</p><p>Over the course of one full year (fall 2019 until fall 2020), we deployed a filter-inlet for gases and aerosols coupled to a chemical ionization high-resolution time-of-flight mass spectrometer (FIGAERO-CIMS) using iodide as reagent ion at the Zeppelin Observatory in Svalbard (480 m a.s.l.), as part of the Ny-Ålesund Aerosol Cloud Experiment (NASCENT). The FIGAERO-CIMS is able to measure organic trace gases and aerosol particles semi-simultaneously. The instrument was connected to an inlet switching between a counterflow virtual impactor (CVI) inlet and a total air inlet. This setup allows to study the differences in chemical composition of organic aerosol particles and trace gases at molecular level that are involved in Arctic cloud formation compared to ambient non-activated aerosol.</p><p>We observed organic signal above background in both gas and particle phase all year round. A comparison between the gas phase mass spectra of cloud-free and cloudy conditions shows lower signal for some organics inside the cloud, indicating that some trace gases are scavenged by cloud hydrometeors whilst others are not. In this presentation we will discuss the chemical characteristics of the gases exhibiting different behavior during clear sky and cloudy conditions, and the implications for partitioning of organic compounds between the gas, aerosol particle and cloud hydrometeor (droplet/ice) phase.</p>


2018 ◽  
Author(s):  
Yang Wang ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Sebastian Böhnke ◽  
Isabelle De Smedt ◽  
...  

Abstract. A Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18° N, 114.36° E) in the suburban area of Xingtai (one of the most polluted cities in China) during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ~ 3.5 ppb. Underestimates of MAX-DOAS results compared to in situ measurements of NO2 (~ 60 %), SO2 (~ 20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2, SO2 are reasonably consistent with those measured by a collocated Raman Lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO, and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ~ 1.4 km) than did NO2, SO2, and HONO (with 75 % integrated column below ~ 0.5 km) under polluted condition. Lifted layers were systematically observed for all species, (except HONO), indicating accumulation, secondary formation, or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2, SO2, and HONO, but around noon for aerosols, HCHO, and CHOCHO, mainly dominated by photochemistry, characteristic upslope/downslope circulation and PBL dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution from the southern areas such as industrialized Wuan. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases, and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations of HCHO, CHOCHO and aerosols.


2011 ◽  
Vol 11 (9) ◽  
pp. 4491-4503 ◽  
Author(s):  
J. Worden ◽  
D. Noone ◽  
J. Galewsky ◽  
A. Bailey ◽  
K. Bowman ◽  
...  

Abstract. The Aura satellite Tropospheric Emission Spectrometer (TES) instrument is capable of measuring the HDO/H2O ratio in the lower troposphere using thermal infrared radiances between 1200 and 1350 cm−1. However, direct validation of these measurements is challenging due to a lack of in situ measured vertical profiles of the HDO/H2O ratio that are spatially and temporally co-located with the TES observations. From 11 October through 5 November 2008, we undertook a campaign to measure HDO and H2O at the Mauna Loa observatory in Hawaii for comparison with TES observations. The Mauna Loa observatory is situated at 3.1 km above sea level or approximately 680 hPa, which is approximately the altitude where the TES HDO/H2O observations show the most sensitivity. Another advantage of comparing in situ data from this site to estimates derived from thermal IR radiances is that the volcanic rock is heated by sunlight during the day, thus providing significant thermal contrast between the surface and atmosphere; this thermal contrast increases the sensitivity to near surface estimates of tropospheric trace gases. The objective of this inter-comparison is to better characterize a bias in the TES HDO data, which had been previously estimated to be approximately 5 % too high for a column integrated value between 850 hPa and 500 hPa. We estimate that the TES HDO profiles should be corrected downwards by approximately 4.8 % and 6.3 % for Versions 3 and 4 of the data respectively. These corrections must account for the vertical sensitivity of the TES HDO estimates. We estimate that the precision of this bias correction is approximately 1.9 %. The accuracy is driven by the corrections applied to the in situ HDO and H2O measurements using flask data taken during the inter-comparison campaign and is estimated to be less than 1 %. Future comparisons of TES data to accurate vertical profiles of in situ measurements are needed to refine this bias estimate.


2013 ◽  
Vol 6 (6) ◽  
pp. 10297-10360 ◽  
Author(s):  
T. Wagner ◽  
S. Beirle ◽  
S. Dörner ◽  
U. Friess ◽  
J. Remmers ◽  
...  

Abstract. Multi-AXis-Differential Optical Absorption Spectroscopy (MAX-DOAS) observations of aerosols and trace gases can be strongly influenced by clouds. Thus it is important to identify clouds and characterise their properties. In this study we investigate the effects of clouds on several quantities which can be derived from MAX-DOAS observations, like the radiance, the colour index (radiance ratio at two selected wavelengths), the absorption of the oxygen dimer O4 and the fraction of inelastically scattered light (Ring effect). To identify clouds, these quantities can be either compared to their corresponding clear sky reference values, or their dependencies on time or viewing direction can be analysed. From the investigation of the temporal variability the influence of clouds can be identified even for individual measurements. Based on our investigations we developed a cloud classification scheme, which can be applied in a flexible way to MAX-DOAS or zenith DOAS observations: in its simplest version, zenith observations of the colour index are used to identify the presence of clouds (or high aerosol load). In more sophisticated versions, also other quantities and viewing directions are considered, which allows sub-classifications like e.g. thin or thick clouds, or fog. We applied our cloud classification scheme to MAX-DOAS observations during the CINDI campaign in the Netherlands in Summer 2009 and found very good agreement with sky images taken from ground.


2013 ◽  
Vol 6 (3) ◽  
pp. 719-739 ◽  
Author(s):  
S. Baidar ◽  
H. Oetjen ◽  
S. Coburn ◽  
B. Dix ◽  
I. Ortega ◽  
...  

Abstract. The University of Colorado Airborne Multi-Axis Differential Optical Absorption Spectroscopy (CU AMAX-DOAS) instrument uses solar stray light to detect and quantify multiple trace gases, including nitrogen dioxide (NO2), glyoxal (CHOCHO), formaldehyde (HCHO), water vapor (H2O), nitrous acid (HONO), iodine monoxide (IO), bromine monoxide (BrO), and oxygen dimers (O4) at multiple wavelengths (absorption bands at 360, 477, 577, 632 nm) simultaneously in the open atmosphere. The instrument is unique as it (1) features a motion compensation system that decouples the telescope field of view from aircraft movements in real time (<0.35° accuracy), and (2) includes measurements of solar stray light photons from nadir, zenith, and multiple elevation angles forward and below the plane by the same spectrometer/detector system. Sets of solar stray light spectra collected from nadir to zenith scans provide some vertical profile information within 2 km above and below the aircraft altitude, and the vertical column density (VCD) below the aircraft is measured in nadir view. Maximum information about vertical profiles is derived simultaneously for trace gas concentrations and aerosol extinction coefficients over similar spatial scales and with a vertical resolution of typically 250 m during aircraft ascent/descent. The instrument is described, and data from flights over California during the CalNex (California Research at the Nexus of Air Quality and Climate Change) and CARES (Carbonaceous Aerosols and Radiative Effects Study) air quality field campaigns is presented. Horizontal distributions of NO2 VCD (below the aircraft) maps are sampled with typically 1 km resolution, and show good agreement with two ground-based MAX-DOAS instruments (slope = 0.95 ± 0.09, R2 = 0.86). As a case study vertical profiles of NO2, CHOCHO, HCHO, and H2O concentrations and aerosol extinction coefficients, ε, at 477 nm calculated from O4 measurements from a low approach at Brackett airfield inside the South Coast Air Basin (SCAB) are presented. These profiles contain ~12 degrees of freedom (DOF) over a 3.5 km altitude range, an independent information approximately every 250 m. The boundary layer NO2 concentration, and the integral aerosol extinction over height (aerosol optical depth, AOD) agrees well with nearby ground-based in situ NO2 measurement, and AERONET station. The detection limits of NO2, CHOCHO, HCHO, H2O442, &amp;varepsilon;360, &amp;varepsilon;477 for 30 s integration time spectra recorded forward of the plane are 5 ppt, 3 ppt, 100 ppt, 42 ppm, 0.004 km−1, 0.002 km−1 in the free troposphere (FT), and 30 ppt, 16 ppt, 540 ppt, 252 ppm, 0.012 km−1, 0.006 km−1 inside the boundary layer (BL), respectively. Mobile column observations of trace gases and aerosols are complimentary to in situ observations, and help bridge the spatial scales that are probed by satellites and ground-based observations, and predicted by atmospheric models.


2013 ◽  
Vol 13 (5) ◽  
pp. 12287-12336 ◽  
Author(s):  
M. Michael ◽  
A. Yadav ◽  
S. N. Tripathi ◽  
V. P. Kanawade ◽  
A. Gaur ◽  
...  

Abstract. The "online" meteorological and chemical transport Weather Research and Forecasting/Chemistry (WRF-Chem) model has been implemented over the Indian subcontinent for three consecutive summers in 2008, 2009 and 2010 to study the aerosol properties over the domain. The initial and boundary conditions are obtained from NCAR reanalysis data. The emission rates of sulfur dioxide, black carbon, organic carbon and PM2.5, which are developed over India at a grid resolution of 0.25° × 0.25° have been used in the present study. The remaining emissions are obtained from global inventories (RETRO and EDGAR). The model simulated the meteorological parameters, trace gases and particulate matter. Predicted mixing ratios of trace gases (Ozone, carbon monoxide and sulfur dioxide) are compared with ground based observations over Kanpur. Simulated aerosol optical depth are compared with those observed at nine Aerosol Robotic Network stations (AERONET). The simulations show that the aerosol optical depth of the less polluted regions is better simulated compared to that of the locations where the aerosol loading is very high. The vertical profiles of extinction coefficient observed at Kanpur Micropulse Lidar Network (MPLNET) station is in agreement with the simulated values for altitudes greater than 1.5 km and qualitatively simulate the elevated layers of aerosols. The simulated mass concentration of black carbon shows very good correlation with observations, due to the better local emission inventory used. The vertical profiles of black carbon at various locations have also been compared with observations from aircraft campaign held during pre-monsoon period of 2008 and 2009 resulting in good agreement. This study shows that WRF-Chem model captures many important features of the observations and therefore can be used for understanding and predicting regional atmospheric composition over Indian subcontinent.


Author(s):  
Melanie Müller ◽  
Martin Strunk ◽  
Andreas Engel ◽  
Ulrich Schmidt

2020 ◽  
Author(s):  
Michael Revesz ◽  
Stefan F. Schreier ◽  
Philipp Weihs ◽  
Tim Bösch ◽  
Kezia Lange ◽  
...  

&lt;p&gt;Within the project VINDOBONA (VIenna horizontal aNd vertical Distribution OBservations Of Nitrogen dioxide and Aerosols), a method was developed to retrieve the spatial distribution of trace gases using data from three ground based MAX-DOAS instruments and was applied on the example of NO&lt;sub&gt;2&lt;/sub&gt;. At three different locations in Vienna (Austria) MAX-DOAS instruments were installed performing measurements in the visible and UV spectral range. Currently, each instrument is set up to determine the column densities in different azimuthal directions and low elevation angles within approximately a horizontal plane. The different lines of sight of the three instruments intersect horizontally and can be used to estimate the horizontal spatial distribution of trace gases. With the knowledge of vertical profiles, even the vertical distribution can be estimated using this method.&amp;#160;&lt;/p&gt;&lt;p&gt;The intersections of the different lines of sight define segments along the slant columns for which the mass concentrations can be estimated. Knowledge about the vertical profiles for a chosen trace gas can be used to correct the retrieved trace gas concentration to specific altitudes above ground. Such corrections are also required since the three instruments were set up at different heights above ground, at different altitudes relative to sea level and with different elevation angles of the lowest viewing direction. One open issue for the retrieval process is the terrain in Vienna in combination with the prevailing wind condition that impacts the horizontal and vertical trace gas distribution and make the retrieval challenging.&amp;#160;&lt;/p&gt;


2014 ◽  
Vol 7 (1) ◽  
pp. 431-482 ◽  
Author(s):  
M. Michael ◽  
A. Yadav ◽  
S. N. Tripathi ◽  
V. P. Kanawade ◽  
A. Gaur ◽  
...  

Abstract. The "online" meteorological and chemical transport Weather Research and Forecasting/Chemistry (WRF-Chem) model has been implemented over the Indian subcontinent for three consecutive summers in 2008, 2009 and 2010 to study the aerosol properties over the domain. The model simulated the meteorological parameters, trace gases and particulate matter. Predicted mixing ratios of trace gases (Ozone, carbon monoxide and sulfur dioxide) are compared with ground based observations over Kanpur. Simulated aerosol optical depth are compared with those observed at nine Aerosol Robotic Network stations (AERONET). The simulations show that the aerosol optical depth of the less polluted regions is better simulated compared to that of the locations where the aerosol loading is very high. The vertical profiles of extinction coefficient observed at the Kanpur Micropulse Lidar Network (MPLNET) station is underpredicted by the model by 10 to 50% for altitudes greater than 1.5 km and qualitatively simulate the elevated layers of aerosols. The simulated mass concentration of black carbon shows a correlation coefficient of 0.4 with observations. Vertical profiles of black carbon at various locations have also been compared with observations from an aircraft campaign held during pre-monsoon period of 2008 and 2009. This study shows that WRF-Chem model captures many important features of the observed atmospheric composition during the pre-monsoon season in India.


2015 ◽  
Vol 15 (6) ◽  
pp. 8283-8328 ◽  
Author(s):  
C. Di Biagio ◽  
L. Doppler ◽  
C. Gaimoz ◽  
N. Grand ◽  
G. Ancellet ◽  
...  

Abstract. In this study we present airborne observations of aerosol and trace gases obtained over the sea in the Western Mediterranean Basin during the TRAQA (TRansport and Air QuAlity) and SAFMED (Secondary Aerosol Formation in the MEDiterranean) campaigns in summers 2012 and 2013. A total of 23 vertical profiles were measured up to 5000 m a.s.l. over an extended area (40–45° N latitude and 2° W–12° E longitude) including the Gulf of Genoa, Southern France, the Gulf of Lion, and the Spanish coast. TRAQA and SAFMED successfully measured a wide range of meteorological conditions which favoured the pollution export from different sources located around the basin. Also, several events of dust outflows were measured during the campaigns. Observations from the present study indicate that continental pollution largely affects the Western Mediterranean both close to coastal regions and in the open sea as far as ~250 km from the coastline. Aerosol layers not specifically linked with Saharan dust outflows are distributed ubiquitously which indicates quite elevated levels of background pollution throughout the Western Basin. The measured aerosol scattering coefficient varies between ~20 and 120 M m−1, while carbon monoxide (CO) and ozone (O3) mixing ratios are in the range of 60–170 and 30–85 ppbv, respectively. Pollution reaches 3000–4000 m in altitude and presents a very complex and highly stratified structure characterized by fresh and aged layers both in the boundary layer and in the free troposphere. Within pollution plumes the measured particle concentration in the Aitken (0.004–0.1 μm) and accumulation (0.1–1.0 μm) modes is between $\\sim 100$ and 5000–6000 s cm−3 (standard cm−3), which is comparable to the aerosol concentration measured in continental urban areas. Additionally, our measurements indicate the presence of highly concentrated Aitken layers (10 000–15 000 s cm−3) observed both close to the surface and in the free troposphere, possibly linked to the influence of new particle formation (NPF) episodes over the basin.


Sign in / Sign up

Export Citation Format

Share Document