scholarly journals Tunable diode laser in-situ CH<sub>4</sub> measurements aboard the CARIBIC passenger aircraft: instrument performance assessment

2013 ◽  
Vol 6 (5) ◽  
pp. 9225-9261 ◽  
Author(s):  
C. Dyroff ◽  
A. Zahn ◽  
S. Sanati ◽  
E. Christner ◽  
A. Rauthe-Schöch ◽  
...  
Keyword(s):  
Lower Troposphere ◽  
Correlation Study ◽  
Tunable Diode Laser ◽  
Long Distance ◽  
Airborne Measurements ◽  
Mixing Ratios ◽  
Laboratory Characterization ◽  
Passenger Aircraft ◽  
The Tropics

Abstract. A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyzer (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne employment. The modified instrument is described. A laboratory characterization was performed to determine the instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation a calibration strategy is described, that utilizes CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppbv for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppbv. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately considered and the uncertainty is estimated to be 12.4 ppbv. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppbv at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.

scholarly journals Tunable diode laser in-situ CH<sub>4</sub> measurements aboard the CARIBIC passenger aircraft: instrument performance assessment

2014 ◽  
Vol 7 (3) ◽  
pp. 743-755 ◽  
Author(s):  
C. Dyroff ◽  
A. Zahn ◽  
S. Sanati ◽  
E. Christner ◽  
A. Rauthe-Schöch ◽  
...  
Keyword(s):  
Lower Troposphere ◽  
Correlation Study ◽  
Tunable Diode Laser ◽  
Long Distance ◽  
Airborne Measurements ◽  
Mixing Ratios ◽  
Flight Level ◽  
Passenger Aircraft ◽  
The Tropics

Abstract. A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.

scholarly journals Representativeness of the IAGOS airborne measurements in the lower troposphere

Elem Sci Anth ◽  
2018 ◽  
Vol 6 ◽  
Author(s):  
H. Petetin ◽  
M. Jeoffrion ◽  
B. Sauvage ◽  
G. Athier ◽  
R. Blot ◽  
...  
Keyword(s):  
Air Quality ◽  
Lower Troposphere ◽  
Monitoring Network ◽  
Ratio Distribution ◽  
Airborne Measurements ◽  
Mixing Ratios ◽  
The Difference ◽  
The Vertical Distribution ◽  
Local Emissions

In the framework of the In Service Aircraft for Global Observing System (IAGOS) program, airborne in-situ O3 and CO measurements are performed routinely using in-service aircraft, providing vertical profiles from the surface to about 10–12 km. Due to the specificity of IAGOS measurements (measurements around busy international airports), uncertainties exist on their representativeness in the lower troposphere as they may be impacted by emissions related to airport activities and/or other aircraft. In this study, we thus investigate how the IAGOS measurements in the lower troposphere compare with nearby surface stations (from the local Air Quality monitoring network (AQN)) and more distant regional surface stations (from the Global Atmospheric Watch (GAW) network). The study focuses on Frankfurt but some results at other European airports (Vienna, Paris) are also discussed. Results indicate that the IAGOS observations close to the surface do not appear to be strongly impacted by local emissions related to airport activities. In terms of mixing ratio distribution, seasonal variations and trends, the CO and O3 mixing ratios measured by IAGOS in the first few hundred metres above the surface have similar characteristics to the mixing ratios measured at surrounding urban background stations. Higher in altitude, both the difference with data from the local AQN and the consistency with the GAW regional stations are higher, which indicates a larger representativeness of the IAGOS data. Despite few quantitative differences with Frankfurt, consistent results are obtained in the two other cities Vienna and Paris. Based on 11 years of data (2002–2012), this study thus demonstrates that IAGOS observations in the lowest troposphere can be used as a complement to surface stations to study the air quality in/around the agglomeration, providing important information on the vertical distribution of pollution.

scholarly journals Tracer measurements in the tropical tropopause layer during the AMMA/SCOUT-O3 aircraft campaign

2010 ◽  
Vol 10 (8) ◽  
pp. 3615-3627 ◽  
Author(s):  
C. D. Homan ◽  
C. M. Volk ◽  
A. C. Kuhn ◽  
A. Werner ◽  
J. Baehr ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Deep Convection ◽  
Transport Processes ◽  
Gradual Transition ◽  
Tropical Tropopause Layer ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
Multidisciplinary Analysis ◽  
The Tropics

Abstract. We present airborne in situ measurements made during the AMMA (African Monsoon Multidisciplinary Analysis)/SCOUT-O3 campaign between 31 July and 17 August 2006 on board the M55 Geophysica aircraft, based in Ouagadougou, Burkina Faso. CO2 and N2O were measured with the High Altitude Gas Analyzer (HAGAR), CO was measured with the Cryogenically Operated Laser Diode (COLD) instrument, and O3 with the Fast Ozone ANalyzer (FOZAN). We analyse the data obtained during five local flights to study the dominant transport processes controlling the tropical tropopause layer (TTL, here ~350–375 K) and lower stratosphere above West-Africa: deep convection up to the level of main convective outflow, overshooting of deep convection, and horizontal inmixing across the subtropical tropopause. Besides, we examine the morphology of the stratospheric subtropical barrier. Except for the flight of 13 August, distinct minima in CO2 mixing ratios indicate convective outflow of boundary layer air in the TTL. The CO2 profiles show that the level of main convective outflow was mostly located at potential temperatures between 350 and 360 K, and for 11 August reached up to 370 K. While the CO2 minima indicate quite significant convective influence, the O3 profiles suggest that the observed convective signatures were mostly not fresh, but of older origin (several days or more). When compared with the mean O3 profile measured during a previous campaign over Darwin in November 2005, the O3 minimum at the main convective outflow level was less pronounced over Ouagadougou. Furthermore O3 mixing ratios were much higher throughout the whole TTL and, unlike over Darwin, rarely showed low values observed in the regional boundary layer. Signatures of irreversible mixing following overshooting of convective air were scarce in the tracer data. Some small signatures indicative of this process were found in CO2 profiles between 390 and 410 K during the flights of 4 and 8 August, and in CO data at 410 K on 7 August. However, the absence of expected corresponding signatures in other tracer data makes this evidence inconclusive, and overall there is little indication from the observations that overshooting convection has a profound impact on gas-phase tracer TTL composition during AMMA. We find the amount of photochemically aged air isentropically mixed into the TTL across the subtropical tropopause to be not significant. Using the N2O observations we estimate the fraction of aged extratropical stratospheric air in the TTL to be 0.0±0.1 up to 370 K during the local flights. Above the TTL this fraction increases to 0.3±0.1 at 390 K. The subtropical barrier, as indicated by the slope of the correlation between N2O and O3 between 415 and 490 K, does not appear as a sharp border between the tropics and extratropics, but rather as a gradual transition region between 10° N and 25° N where isentropic mixing between these two regions may occur.

scholarly journals Aircraft validation of Aura Tropospheric Emission Spectrometer retrievals of HDO / H<sub>2</sub>O

2014 ◽  
Vol 7 (9) ◽  
pp. 3127-3138 ◽  
Author(s):  
R. L. Herman ◽  
J. E. Cherry ◽  
J. Young ◽  
J. M. Welker ◽  
D. Noone ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Water Vapor ◽  
Standard Deviation ◽  
Lower Troposphere ◽  
Temporal Variations ◽  
Observation Error ◽  
Free Troposphere ◽  
Data Set ◽  
Airborne Measurements

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.

scholarly journals Oxygenated compounds in aged biomass burning plumes over the Eastern Mediterranean: evidence for strong secondary production of methanol and acetone

2005 ◽  
Vol 5 (1) ◽  
pp. 39-46 ◽  
Author(s):  
R. Holzinger ◽  
J. Williams ◽  
G. Salisbury ◽  
T. Klüpfel ◽  
M. de Reus ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Secondary Production ◽  
Eastern Mediterranean ◽  
Proton Transfer Reaction ◽  
Tunable Diode Laser ◽  
Airborne Measurements ◽  
Mixing Ratios ◽  
Oxygenated Compounds ◽  
Laser Absorption ◽  
Secondary Formation

Abstract. Airborne measurements of acetone, methanol, PAN, acetonitrile (by Proton Transfer Reaction Mass Spectrometry), and CO (by Tunable Diode Laser Absorption Spectroscopy) have been performed during the Mediterranean Intensive Oxidants Study (MINOS August 2001). We have identified ten biomass burning plumes from strongly elevated acetonitrile mixing ratios. The characteristic biomass burning signatures obtained from these plumes reveal secondary production of acetone and methanol, while CO photochemically declines in the plumes. Mean excess mixing ratios - normalized to CO - of 1.8%, 0.20%, 3.8%, and 0.65% for acetone, acetonitrile, methanol, and PAN, respectively, were found. By scaling to an assumed global annual source of 663-807Tg CO, biomass burning emissions of 25-31 and 29-35 Tg/yr for acetone and methanol are estimated, respectively. Our measurements suggest that the present biomass burning contributions of acetone and methanol are significantly underestimated due to the neglect of secondary formation within the plume. Median acetonitrile mixing ratios throughout the troposphere were around 150pmol/mol, in accord with current biomass burning inventories and an atmospheric lifetime of ~6 months.

scholarly journals Evaluation of balloon and satellite water vapour measurements in the Southern tropical UTLS during the HIBISCUS campaign

2007 ◽  
Vol 7 (3) ◽  
pp. 6037-6075 ◽  
Author(s):  
N. Montoux ◽  
A. Hauchecorne ◽  
J.-P. Pommereau ◽  
G. Durry ◽  
B. Morel ◽  
...  
Keyword(s):  
Remote Sensing ◽  
Water Vapour ◽  
Transport Model ◽  
Tunable Diode Laser ◽  
Upper Troposphere ◽  
Satellite Systems ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
Dry Bias

Abstract. Among the objectives of the HIBISCUS campaign was the study of water vapour in the tropical upper troposphere and lower stratosphere (UTLS) by balloon borne in situ and remote sensing, offering a unique opportunity for evaluating the performances of balloon and satellite water vapour data available at the southern tropics in February-April 2004. Instruments evaluated include balloon borne in situ tunable diode laser spectrometer (μ SDLA) and surface acoustic wave hygrometer (SAW), and remote sensing with a near IR spectrometer (SAOZ) flown on a circumnavigating long duration balloon. The satellite systems available are those of AIRS/AMSU (v4), SAGE-II (v6.2), HALOE (v19), MIPAS (v4.62) and GOMOS (v6.0). In the stratosphere between 20–25 km, three satellite instruments, HALOE, SAGE-II and MIPAS, are showing very consistent results (nearly constant mixing ratios), while AIRS, GOMOS and the SAOZ balloon are displaying a slight increase with altitude. Considering the previous studies, the first three appear the most precise at this level, HALOE being the less variable (5%), close to the atmospheric variability shown by the REPROBUS/ECMWF Chemistry-Transport model. The three others are showing significantly larger variability, AIRS being the most variable (35%), followed by GOMOS (25%) and SAOZ (20%). Lower down in the Tropical Tropopause Layer between 14–20 km, HALOE and SAGE-II are showing marked minimum mixing ratios around 17–19 km, not seen by all others. For HALOE, this might be related to an altitude registration error already identified on ozone, while for SAGE-II, a possible explanation could be the persistence of the dry bias displayed by previous retrieval versions, not completely removed in version 6.2. On average, MIPAS is consistent with AIRS, GOMOS and SAOZ, not displaying the dry bias observed in past versions, but a fast degradation of precision below 20 km. Compared to satellites, the μ SDLA measurements shows systematically larger humidity although this conclusion may be biased by the fact that the balloon flights were carried out intentionally next or above strong convective systems where remote observations from space are difficult. In the upper troposphere below 14 km, all remote sensing measurements (except MIPAS of limited precision, and AIRS/AMSU) become rare, dry biased and less variable compared to ECMWF, but particularly HALOE and SAGE-II. The main reason for that is the frequent masking by clouds within which no remote measurements could be performed except by the AMSU microwave. Water vapour remote sensing profiles are representative of cloud free conditions only and thus dryer and less variable on average than ECMWF and AIRS/AMSU. Always in the upper troposphere, two in-situ instruments, μ SDLA and SAW, flown on the same balloon agree each other, displaying water vapour mixing ratios 100–200% larger than that of HALOE and MIPAS, which could be explained by the large ice supersaturation of the layer up to the tropopause, hardly detectable from the orbit.

scholarly journals TransCom N<sub>2</sub>O model inter-comparison – Part 1: Assessing the influence of transport and surface fluxes on tropospheric N<sub>2</sub>O variability

2014 ◽  
Vol 14 (2) ◽  
pp. 2307-2362 ◽  
Author(s):  
R. L. Thompson ◽  
P. K. Patra ◽  
K. Ishijima ◽  
E. Saikawa ◽  
M. Corazza ◽  
...  
Keyword(s):  
Northern Hemisphere ◽  
Seasonal Cycle ◽  
Large Scale ◽  
Atmospheric Transport ◽  
Lower Troposphere ◽  
Vertical Gradient ◽  
Surface Fluxes ◽  
Meridional Transport ◽  
Mixing Ratios

Abstract. We present a comparison of chemistry-transport models (TransCom-N2O) to examine the importance of atmospheric transport and surface fluxes on the variability of N2O mixing ratios in the troposphere. Six different models and two model variants participated in the inter-comparison and simulations were made for the period 2006 to 2009. In addition to N2O, simulations of CFC-12 and SF6 were made by a subset of four of the models to provide information on the models proficiency in stratosphere-troposphere exchange (STE) and meridional transport, respectively. The same prior emissions were used by all models to restrict differences among models to transport and chemistry alone. Four different N2O flux scenarios totalling between 14 and 17 Tg N yr−1 (for 2005) globally were also compared. The modelled N2O mixing ratios were assessed against observations from in-situ stations, discrete air sampling networks, and aircraft. All models adequately captured the large-scale patterns of N2O and the vertical gradient from the troposphere to the stratosphere and most models also adequately captured the N2O tropospheric growth rate. However, all models underestimated the inter-hemispheric N2O gradient by at least 0.33 ppb (equivalent to 1.5 Tg N), which, even after accounting for an overestimate of emissions in the Southern Ocean of circa 1.0 Tg N, points to a likely underestimate of the Northern Hemisphere source by up to 0.5 Tg N and/or an overestimate of STE in the Northern Hemisphere. Comparison with aircraft data reveal that the models overestimate the amplitude of the N2O seasonal cycle at Hawaii (21° N, 158° W) below circa 6000 m, suggesting an overestimate of the importance of stratosphere to troposphere transport in the lower troposphere at this latitude. In the Northern Hemisphere, most of the models that provided CFC-12 simulations captured the phase of the CFC-12, seasonal cycle, indicating a reasonable representation of the timing of STE. However, for N2O all models simulated a too early minimum by 2 to 3 months owing to errors in the seasonal cycle in the prior soil emissions, which is still not adequately represented by terrestrial biosphere models. In the Southern Hemisphere, most models failed to capture the N2O and CFC-12 seasonality at Cape Grim, Tasmania, and all failed at the South Pole, whereas for SF6, all models could capture the seasonality at all sites, suggesting that there are large errors in modeled vertical transport in high southern latitudes.

scholarly journals Attribution and evolution of ozone from Asian wild fires using satellite and aircraft measurements during the ARCTAS campaign

2012 ◽  
Vol 12 (1) ◽  
pp. 169-188 ◽  
Author(s):  
R. Dupont ◽  
B. Pierce ◽  
J. Worden ◽  
J. Hair ◽  
M. Fenn ◽  
...  
Keyword(s):  
Lower Troposphere ◽  
Dynamical Evolution ◽  
Mixing Ratios ◽  
In Situ Data ◽  
Photochemical Production ◽  
The Pacific ◽  
Western Asia ◽  
Quality Modeling ◽  
Low Sensitivity

Abstract. We use ozone and carbon monoxide measurements from the Tropospheric Emission Spectrometer (TES), model estimates of Ozone, CO, and ozone pre-cursors from the Real-time Air Quality Modeling System (RAQMS), and data from the NASA DC8 aircraft to characterize the source and dynamical evolution of ozone and CO in Asian wildfire plumes during the spring ARCTAS campaign 2008. On the 19 April, NASA DC8 O3 and aerosol Differential Absorption Lidar (DIAL) observed two biomass burning plumes originating from North-Western Asia (Kazakhstan) and South-Eastern Asia (Thailand) that advected eastward over the Pacific reaching North America in 10 to 12 days. Using both TES observations and RAQMS chemical analyses, we track the wildfire plumes from their source to the ARCTAS DC8 platform. In addition to photochemical production due to ozone pre-cursors, we find that exchange between the stratosphere and the troposphere is a major factor influencing O3 concentrations for both plumes. For example, the Kazakhstan and Siberian plumes at 55 degrees North is a region of significant springtime stratospheric/tropospheric exchange. Stratospheric air influences the Thailand plume after it is lofted to high altitudes via the Himalayas. Using comparisons of the model to the aircraft and satellite measurements, we estimate that the Kazakhstan plume is responsible for increases of O3 and CO mixing ratios by approximately 6.4 ppbv and 38 ppbv in the lower troposphere (height of 2 to 6 km), and the Thailand plume is responsible for increases of O3 and CO mixing ratios of approximately 11 ppbv and 71 ppbv in the upper troposphere (height of 8 to 12 km) respectively. However, there are significant sources of uncertainty in these estimates that point to the need for future improvements in both model and satellite observations. For example, it is challenging to characterize the fraction of air parcels from the stratosphere versus those from the fire because of the low sensitivity of the TES CO estimates used to mark stratospheric air versus air parcels affected by the smoke plume. Model transport uncertainties, such as too much dispersion, results in a broad plume structure from the Kazakhstan fires that is approximately 2 km lower than the plume observed by aircraft. Consequently, the model and TES data do not capture the photochemical production of ozone in the Kazakhstan plume that is apparent in the aircraft in situ data. However, ozone and CO distributions from TES and RAQMS model estimates of the Thailand plume are within the uncertainties of the TES data. Therefore, the RAQMS model is better able to characterize the emissions from this fire, the mixing of ozone from the stratosphere to the plume, and the photochemical production and transport of ozone and ozone pre-cursors as the plume moves across the Pacific.

scholarly journals Methane source attribution in a U.S. dry gas basin using spatial patterns of ground and airborne ethane and methane measurements

Elem Sci Anth ◽  
2019 ◽  
Vol 7 ◽  
Author(s):  
Ingrid Mielke-Maday ◽  
Stefan Schwietzke ◽  
Tara I. Yacovitch ◽  
Benjamin Miller ◽  
Steve Conley ◽  
...  
Keyword(s):  
Source Attribution ◽  
Bottom Up ◽  
Fayetteville Shale ◽  
Airborne Measurements ◽  
Ch4 Emissions ◽  
Mixing Ratios ◽  
Methane Source ◽  
Methane Enhancement ◽  
Western Half

An intensive coordinated airborne and ground-based measurement study was conducted in the Fayetteville Shale in northwestern Arkansas during September and October 2015 to compare and explain potential discrepancies between top-down and bottom-up estimates of regional natural gas (NG) methane (CH4) emissions. In situ mobile downwind measurements are used to document the ethane to methane enhancement ratios (ERs) in emission plumes from NG operations in the region. Enhancement ratios are low (&lt;2% for 87% of NG sources sampled) in this dry gas-producing region and normally distributed around 1.3% in the western half of the study area. A few sampled landfills emitted CH4 but no ethane (C2H6). Sampling drives around large chicken farms, prevalent in the region, did not detect significant downwind CH4 enhancements. In situ airborne measurements of C2H6 and CH4 from area-scale surveys over and downwind of the region documented the resulting ERs from a mix of CH4 sources. Based on these measurements, we show that on average during the measurement windows 85–95% of total CH4 emissions in the western half of the Fayetteville Shale originated from NG sources, which agrees well with bottom-up estimates from the same field study. Lower mixing ratios measured over the eastern half of the region did not support the ER analysis due to the low signal-to-noise on C2H6 measurements.

scholarly journals HO<sub>x</sub> measurements in the summertime upper troposphere over Europe: a comparison of observations to a box model and a 3-D model

2012 ◽  
Vol 12 (11) ◽  
pp. 30619-30660 ◽  
Author(s):  
E. Regelin ◽  
H. Harder ◽  
M. Martinez ◽  
D. Kubistin ◽  
C. Tatum Ernest ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Circulation Model ◽  
Box Model ◽  
Measurement Unit ◽  
Data Set ◽  
Upper Troposphere ◽  
Sources And Sinks ◽  
Airborne Measurements ◽  
Mixing Ratios

Abstract. In-situ airborne measurements of OH and HO2 with the HORUS (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy) instrument were performed in the summertime upper troposphere across Europe during the HOOVER 2 (HOx OVer EuRope) campaign in July 2007. Complementary measurements of trace gas species and photolysis frequencies were conducted to obtain a broad data set, which has been used to quantify the significant HOx sources and sinks. In this study we compare the in-situ measurement of OH and HO2 with simulated mixing ratios from the constrained box model CAABA/MECCA (Chemistry As A Box Model Application/Module Efficiently Calculating the Chemistry of the Atmosphere), and the global circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry Model). The constrained box model reproduces the observed OH and HO2 mixing ratios with better agreement (obs/mod median 98% OH, 96% HO2) than the global model (median 76% OH, 59% HO2). The observations and the computed HOx sources and sinks are used to identify deviations between the models and their impacts on the calculated HOx budget.

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