scholarly journals Airborne observations of newly formed boundary layer aerosol particles under cloudy conditions

2018 ◽  
Vol 18 (11) ◽  
pp. 8249-8264 ◽  
Author(s):  
Barbara Altstädter ◽  
Andreas Platis ◽  
Michael Jähn ◽  
Holger Baars ◽  
Janine Lückerath ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Ultrafine Particles ◽  
Aerosol Particles ◽  
Inversion Layer ◽  
Time Intervals ◽  
Flight Duration ◽  
Airborne Measurements ◽  
Stratocumulus Clouds ◽  
Short Time

Abstract. This study describes the appearance of ultrafine boundary layer aerosol particles under classical “non-favourable” conditions at the research site of TROPOS (Leibniz Institute for Tropospheric Research). Airborne measurements of meteorological and aerosol properties of the atmospheric boundary layer (ABL) were repeatedly performed with the unmanned aerial system ALADINA (Application of Light-weight Aircraft for Detecting IN-situ Aerosol) during three seasons between October 2013 and July 2015. More than 100 measurement flights were conducted on 23 different days with a total flight duration of 53 h. In 26 % of the cases, maxima of ultrafine particles were observed close to the inversion layer at altitudes between 400 and 600 m and the particles were rapidly mixed vertically and mainly transported downwards during short time intervals of cloud gaps. This study focuses on two measurement days affected by low-level stratocumulus clouds, but different wind directions (NE, SW) and minimal concentrations (< 4.6 µg m−3) of SO2, as a common indicator for precursor gases at ground. Taken from vertical profiles, the onset of clouds led to a non-linearity of humidity that resulted in an increased turbulence at the local-scale and caused fast nucleation (e.g. Bigg, 1997; Wehner et al., 2010), but in relation to rapid dilution of surrounding air, seen in sporadic clusters of ground data, so that ultrafine particles disappeared in the verticality. The typical “banana shape” (Heintzenberg et al., 2007) of new particle formation (NPF) and growth was not seen at ground and thus these days might not have been classified as NPF event days by pure surface studies.

scholarly journals Airborne observations of newly formed boundary layer aerosol particles under cloudy conditions

2018 ◽  
Author(s):  
Barbara Altstädter ◽  
Andreas Platis ◽  
Michael Jähn ◽  
Holger Baars ◽  
Janine Lückerath ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atmospheric Boundary Layer ◽  
Aerosol Particles ◽  
Inversion Layer ◽  
Particle Formation ◽  
Small Scale ◽  
New Particle Formation ◽  
Pressure System ◽  
Flight Duration ◽  
Airborne Measurements

Abstract. This study describes the formation of freshly formed boundary layer aerosol particles under classical called non favourable conditions by the existence of low-level strato cumulus clouds. Airborne measurements for vertical profiling atmospheric boundary layer properties and aerosol particles in the diameter range between 5 nm and 10 μm were repeatedly performed with the unmanned aerial system ALADINA (Application of Light-weight Aircraft for Detecting IN-situ Aerosol) at the research site of TROPOS (Leibniz Institute for Tropospheric Research) in Melpitz during three seasons between October 2013 and July 2015. More than 100 measurement flights were performed during this period on 23 different days with a total flight duration of 53 h. On 26 % of the measurement days, new particle formation was measured close to the inversion layer and was observed to be transported downwards during short time intervals of cloud gaps. However, the typical banana shape of new particle formation and growth was not seen at ground, only sporadic events appeared with low particle growth rate and thus might not have been classified as NPF by pure surface studies. This presentation focuses on two cases influenced by the passage of a low pressure system and minimal concentrations of SO2 as indicator for precursor gases at ground; I) on April 4, 2014 by east wind and II) on June 21, 2015 under south-west wind. For a closure, an LES-model output was used for the second study in order to derive a full analysis of atmospheric boundary layer growth over the measurement site at small-scale with high spatial resolution. Pronounced turbulent fluxes of sensible and latent heat in the vertical distribution initiated fast mixing processes of freshly formed boundary layer aerosol. Furthermore, CO2 and particle fluxes indicated downward transport and high deposition during sporadic nucleation events, so that NPF occurrence above with subsequent downward transport was clearly identified.

scholarly journals Aerosol particle characteristics measured in the United Arab Emirates and their response to mixing in the boundary layer

2021 ◽  
Author(s):  
Jutta Kesti ◽  
John Backman ◽  
Ewan James O'Connor ◽  
Anne Hirsikko ◽  
Eija Asmi ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Aerosol Particle ◽  
United Arab Emirates ◽  
Wind Direction ◽  
Aerosol Particles ◽  
Surface Wind ◽  
Number Concentration ◽  
Particle Properties ◽  
Boundary Layer Height

Abstract. Aerosol particles play an important in role in the microphysics of clouds and hence on their likelihood to precipitate. In the changing climate already dry areas such as the United Arab Emirates (UAE) are predicted to become even drier. Comprehensive observations of the daily and seasonal variation in aerosol particle properties in such locations are required reducing the uncertainty in such predictions. We analyse observations from a one-year measurement campaign at a background location in the United Arab Emirates to investigate the properties of aerosol particles in this region, study the impact of boundary layer mixing on background aerosol particle properties measured at the surface and study the temporal evolution of the aerosol particle cloud formation potential in the region. We used in-situ aerosol particle measurements to characterise the aerosol particle composition, size, number and cloud condensation nuclei (CCN) properties, in-situ SO2 measurements as an anthropogenic signature and a long-range scanning Doppler lidar to provide vertical profiles of the horizontal wind and turbulent properties to monitor the evolution of the boundary layer. Anthropogenic sulphate dominated the aerosol particle mass composition in this location. There was a clear diurnal cycle in the surface wind direction, which had a strong impact on aerosol particle total number concentration, SO2 concentration and black carbon mass concentration. Local sources were the predominant source of black carbon, as concentrations clearly depended on the presence of turbulent mixing, with much higher values during calm nights. The measured concentrations of SO2, instead, were highly dependent on the surface wind direction as well as on the depth of the boundary layer when entrainment from the advected elevated layers occurred. The wind direction at the surface or of the elevated layer suggests that the cities of Dubai, Abu Dhabi and other coastal conurbations were the remote sources of SO2. We observed new aerosol particle formation events almost every day (on four days out of five on average). Calm nights had the highest CCN number concentrations and lowest κ values and activation fractions. We did not observe any clear dependence of CCN number concentration and κ parameter on the height of the daytime boundary layer, whereas the activation fraction did show a slight increase with increasing boundary layer height, due to the change in the shape of the aerosol particle size distribution where the relative portion of larger aerosol particles increased with increasing boundary layer height. We believe that this indicates that size is more important than chemistry for aerosol particle CCN activation at this site. The combination of instrumentation used in this campaign enabled us to identify periods when anthropogenic pollution from remote sources that had been transported in elevated layers was present, and had been mixed down to the surface in the growing boundary layer.

scholarly journals Cloud Processing of Aerosol Particles in Marine Stratocumulus Clouds

Atmosphere ◽  
2019 ◽  
Vol 10 (9) ◽  
pp. 520 ◽  
Author(s):  
Andrea I. Flossmann ◽  
Wolfram Wobrock
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Numerical Study ◽  
Spatial Scales ◽  
Aerosol Particles ◽  
Cloud Microphysics ◽  
Marine Stratocumulus ◽  
Boundary Layer Clouds ◽  
Cloud Processing ◽  
Stratocumulus Clouds

Cloud processing of aerosol particles is an important process and is, for example, thought to be responsible for the so-called “Hoppel-minimum” in the marine aerosol particle distribution or contribute to the cell organization of marine boundary layer clouds. A numerical study of the temporal and spatial scales of the processing of aerosol particles by typical marine stratocumulus clouds is presented. The dynamical framework is inspired by observations during the VOCALS (Variability of the American Monsoon System Ocean-Cloud-Atmosphere-Land Study) Regional Experiment in the Southeast Pacific. The 3-D mesoscale model version of DESCAM (Detailed Scavenging Model) follows cloud microphysics of the stratocumulus deck in a bin-resolved manner and has been extended to keep track of cloud-processed particles in addition to non-processed aerosol particles in the air and inside the cloud drops. The simulation follows the evolution of the processing of aerosol particles by the cloud. It is found that within one hour almost all boundary layer aerosol particles have passed through at least one cloud cycle. However, as the in-cloud residence times of the particles in the considered case are only on the order of minutes, the aerosol particles remain essentially unchanged. Our findings suggest that in order to produce noticeable microphysical and dynamical effects in the marine boundary layer clouds, cloud processing needs to continue for extended periods of time, exceeding largely the time period considered in the present study. A second model study is dedicated to the interaction of ship track particles with marine boundary layer clouds. The model simulates quite satisfactorily the incorporation of the ship plume particles into the cloud. The observed time and spatial scales and a possible Twomey effect were reproduced.

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 Large-Scale Atmospheric Forcing by Southeast Pacific Boundary Layer Clouds: A Regional Model Study*

2005 ◽  
Vol 18 (7) ◽  
pp. 934-951 ◽  
Author(s):  
Yuqing Wang ◽  
Shang-Ping Xie ◽  
Bin Wang ◽  
Haiming Xu
Keyword(s):  
Boundary Layer ◽  
Large Scale ◽  
Inversion Layer ◽  
Regional Model ◽  
Cloud Layer ◽  
Eastern Pacific ◽  
Radiative Effect ◽  
Boundary Layer Clouds ◽  
Southeast Pacific ◽  
Stratocumulus Clouds

Abstract A regional model is used to study the radiative effect of boundary layer clouds over the southeast Pacific on large-scale atmosphere circulation during August–October 1999. With the standard settings, the model simulates reasonably well the large-scale circulation over the eastern Pacific, precipitation in the intertropical convergence zone (ITCZ) north of the equator, and marine boundary layer stratocumulus clouds to the south. In a sensitivity experiment with the radiative effect of liquid clouds south of the equator over the eastern Pacific artificially removed, boundary layer clouds south of the equator almost disappear and precipitation in the ITCZ is reduced by 15%–20%, indicating that the stratocumulus clouds over the southeast Pacific have both local and cross-equatorial effects. Examination of the differences between the control and sensitivity experiments indicates that clouds exert a net diabatic cooling in the inversion layer. In response to this cloud-induced cooling, an in situ anomalous high pressure system develops in the boundary layer and an anomalous shallow meridional circulation develops in the lower troposphere over the equatorial eastern Pacific. At the lower branch of this shallow circulation, anomalous boundary layer southerlies blow from the boundary layer high toward the northern ITCZ where the air ascends. An anomalous returning flow (northerly) just above the cloud layer closes the shallow circulation. This low-level anomalous shallow circulation enhances the subsidence over the southeast Pacific above the cloud layer, helping to maintain boundary layer clouds and temperature inversion there. Meanwhile, the strengthened cross-equatorial flow near the surface enhances moisture convergence and convection in the ITCZ north of the equator. This in turn strengthens the local, deep Hadley circulation and hence the large-scale subsidence and boundary layer clouds over the southeast Pacific. This positive feedback therefore enhances the interhemispheric climate asymmetry over the tropical eastern Pacific.

scholarly journals Aerosol particle characteristics measured in the United Arab Emirates and their response to mixing in the boundary layer

2022 ◽  
Vol 22 (1) ◽  
pp. 481-503
Author(s):  
Jutta Kesti ◽  
John Backman ◽  
Ewan J. O'Connor ◽  
Anne Hirsikko ◽  
Eija Asmi ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Aerosol Particle ◽  
United Arab Emirates ◽  
Wind Direction ◽  
Aerosol Particles ◽  
Surface Wind ◽  
Number Concentration ◽  
Particle Properties ◽  
Boundary Layer Height

Abstract. Aerosol particles play an important role in the microphysics of clouds and hence in their likelihood to precipitate. In the changing climate already-dry areas such as the United Arab Emirates (UAE) are predicted to become even drier. Comprehensive observations of the daily and seasonal variation in aerosol particle properties in such locations are required, reducing the uncertainty in such predictions. We analyse observations from a 1-year measurement campaign at a background location in the United Arab Emirates to investigate the properties of aerosol particles in this region, study the impact of boundary layer mixing on background aerosol particle properties measured at the surface, and study the temporal evolution of the aerosol particle cloud formation potential in the region. We used in situ aerosol particle measurements to characterise the aerosol particle composition, size, number, and cloud condensation nuclei (CCN) properties; in situ SO2 measurements as an anthropogenic signature; and a long-range scanning Doppler lidar to provide vertical profiles of the horizontal wind and turbulent properties to monitor the evolution of the boundary layer. Anthropogenic sulfate dominated the aerosol particle mass composition in this location. There was a clear diurnal cycle in the surface wind direction, which had a strong impact on aerosol particle total number concentration, SO2 concentration, and black carbon mass concentration. Local sources were the predominant source of black carbon as concentrations clearly depended on the presence of turbulent mixing, with much higher values during calm nights. The measured concentrations of SO2, instead, were highly dependent on the surface wind direction as well as on the depth of the boundary layer when entrainment from the advected elevated layers occurred. The wind direction at the surface or of the elevated layer suggests that the oil refineries and the cities of Dubai and Abu Dhabi and other coastal conurbations were the remote sources of SO2. We observed new-aerosol-particle formation events almost every day (on 4 d out of 5 on average). Calm nights had the highest CCN number concentrations and lowest κ values and activation fractions. We did not observe any clear dependence of CCN number concentration and κ parameter on the height of the daytime boundary layer, whereas the activation fraction did show a slight increase with increasing boundary layer height due to the change in the shape of the aerosol particle size distribution where the relative portion of larger aerosol particles increased with increasing boundary layer height. We believe that this indicates that size is more important than chemistry for aerosol particle CCN activation at this site. The combination of instrumentation used in this campaign enabled us to identify periods when anthropogenic pollution from remote sources that had been transported in elevated layers was present and had been mixed down to the surface in the growing boundary layer.

scholarly journals Top-down and Bottom-up aerosol-cloud-closure: towards understanding sources of uncertainty in deriving cloud radiative flux

2017 ◽  
Author(s):  
Kevin J. Sanchez ◽  
Greg C. Roberts ◽  
Radiance Calmer ◽  
Keri Nicoll ◽  
Eyal Hashimshoni ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Radiative Flux ◽  
Research Station ◽  
Top Down ◽  
Bottom Up ◽  
Airborne Measurements ◽  
Aerosol Cloud ◽  
Microphysical Properties ◽  
Holistic Understanding

Abstract. Top-down and bottom-up aerosol-cloud-radiative flux closures were conducted at the Mace Head atmospheric research station in Galway, Ireland in August 2015. This study is part of the BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) European collaborative project, with the goal of understanding key processes affecting aerosol-cloud-radiative flux closures to improve future climate predictions and develop sustainable policies for Europe. Instrument platforms include ground-based, unmanned aerial vehicles (UAV), and satellite measurements of aerosols, clouds and meteorological variables. The ground-based and airborne measurements of aerosol size distributions and cloud condensation nuclei (CCN) concentration were used to initiate a 1D microphysical aerosol-cloud parcel model (ACPM). UAVs were equipped for a specific science mission, with an optical particle counter for aerosol distribution profiles, a cloud sensor to measure cloud extinction, or a 5-hole probe for 3D wind vectors. UAV cloud measurements are rare and have only become possible in recent years through the miniaturization of instrumentation. These are the first UAV measurements at Mace Head. ACPM simulations are compared to in-situ cloud extinction measurements from UAVs to quantify closure in terms of cloud radiative flux. Two out of seven cases exhibit sub-adiabatic vertical temperature profiles within the cloud, which suggests that entrainment processes affect cloud microphysical properties and lead to an overestimate of simulated cloud radiative flux. Including an entrainment parameterization and explicitly calculating the entrainment fraction in the ACPM simulations both improved cloud-top radiative closure. Entrainment reduced the difference between simulated and observation-derived cloud-top radiative flux (δRF) by between 30 W m−2 and 40 W m−2. After accounting for entrainment, satellite-derived cloud droplet number concentrations (CDNC) were within 30 % of simulated CDNC. In cases with a well-mixed boundary layer, δRF is less than 25 W m−2 after accounting for cloud-top entrainment, compared to less than 50 W m−2 when entrainment is not taken into account. In cases with a decoupled boundary layer, cloud microphysical properties are inconsistent with ground-based aerosol measurements, as expected, and δRF is as high as 88 W m−2, even after accounting for cloud-top entrainment. This work demonstrates the need to take in-situ measurements of aerosol properties for cases where the boundary layer is decoupled as well as consider cloud-top entrainment to accurately model stratocumulus cloud radiative flux.

Aircraft measurements of nitrous acid in excess of model predictions in the boundary layer and free troposphere

2020 ◽  
Author(s):  
Benjamin Schreiner ◽  
Klaus Pfeilsticker ◽  
Flora Kluge ◽  
Meike Rotermund ◽  
Andreas Zahn ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Optical Absorption Spectroscopy ◽  
Free Troposphere ◽  
Aerosol Composition ◽  
Transport And Transformation ◽  
Air Masses ◽  
Airborne Measurements ◽  
Photolysis Frequencies ◽  
Model Predictions

&lt;p&gt;Middle and long-term &amp;#160;photo-chemical effects of local and regional pollution are not well quantified and are an area of active study. NO&lt;sub&gt;x&lt;/sub&gt; (here defined as NO, NO&lt;sub&gt;2&lt;/sub&gt;, and HONO) is a regional pollutant, which influences atmospheric oxidation capacity and ozone formation. Airborne measurements of atmospheric trace gases from the HALO (High Altitude Long Range) aircraft, particularly of NO, NO&lt;sub&gt;2&lt;/sub&gt;, and HONO were performed as part of the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) campaign over continental Europe and southeast Asia in July 2017 and April 2018, respectively. NO (and NO&lt;sub&gt;Y&lt;/sub&gt;), O&lt;sub&gt;3&lt;/sub&gt;, and the photolysis frequencies of NO&lt;sub&gt;2&lt;/sub&gt; and HONO were measured in-situ. NO&lt;sub&gt;2&lt;/sub&gt; and HONO were inferred from Limb measurements of the mini-DOAS (Differential Optical Absorption Spectroscopy) instrument, using the novel scaling method (H&amp;#252;neke et al., 2017). These measurements were compared with simulations of the MECO/EMAC models. In relatively polluted air-masses in the boundary layer and free troposphere, HONO measured in excess of model predictions (and previous measurements) suggests an in-situ formation and a significant source of OH as well as a pathway for re-noxification. Aerosol composition simultaneously measured &amp;#160;by the C-Tof-AMS instrument may reveal potential reaction mechanisms to explain the discrepancy.&amp;#160;&lt;/p&gt;

scholarly journals Top-down and bottom-up aerosol–cloud closure: towards understanding sources of uncertainty in deriving cloud shortwave radiative flux

2017 ◽  
Vol 17 (16) ◽  
pp. 9797-9814 ◽  
Author(s):  
Kevin J. Sanchez ◽  
Gregory C. Roberts ◽  
Radiance Calmer ◽  
Keri Nicoll ◽  
Eyal Hashimshoni ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Radiative Flux ◽  
Research Station ◽  
Top Down ◽  
Bottom Up ◽  
Airborne Measurements ◽  
Aerosol Cloud ◽  
Microphysical Properties ◽  
Holistic Understanding

Abstract. Top-down and bottom-up aerosol–cloud shortwave radiative flux closures were conducted at the Mace Head Atmospheric Research Station in Galway, Ireland, in August 2015. This study is part of the BACCHUS (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding) European collaborative project, with the goal of understanding key processes affecting aerosol–cloud shortwave radiative flux closures to improve future climate predictions and develop sustainable policies for Europe. Instrument platforms include ground-based unmanned aerial vehicles (UAVs)1 and satellite measurements of aerosols, clouds and meteorological variables. The ground-based and airborne measurements of aerosol size distributions and cloud condensation nuclei (CCN) concentration were used to initiate a 1-D microphysical aerosol–cloud parcel model (ACPM). UAVs were equipped for a specific science mission, with an optical particle counter for aerosol distribution profiles, a cloud sensor to measure cloud extinction or a five-hole probe for 3-D wind vectors. UAV cloud measurements are rare and have only become possible in recent years through the miniaturization of instrumentation. These are the first UAV measurements at Mace Head. ACPM simulations are compared to in situ cloud extinction measurements from UAVs to quantify closure in terms of cloud shortwave radiative flux. Two out of seven cases exhibit sub-adiabatic vertical temperature profiles within the cloud, which suggests that entrainment processes affect cloud microphysical properties and lead to an overestimate of simulated cloud shortwave radiative flux. Including an entrainment parameterization and explicitly calculating the entrainment fraction in the ACPM simulations both improved cloud-top radiative closure. Entrainment reduced the difference between simulated and observation-derived cloud-top shortwave radiative flux (δRF) by between 25 and 60 W m−2. After accounting for entrainment, satellite-derived cloud droplet number concentrations (CDNCs) were within 30 % of simulated CDNC. In cases with a well-mixed boundary layer, δRF is no greater than 20 W m−2 after accounting for cloud-top entrainment and up to 50 W m−2 when entrainment is not taken into account. In cases with a decoupled boundary layer, cloud microphysical properties are inconsistent with ground-based aerosol measurements, as expected, and δRF is as high as 88 W m−2, even high (> 30 W m−2) after accounting for cloud-top entrainment. This work demonstrates the need to take in situ measurements of aerosol properties for cases where the boundary layer is decoupled as well as consider cloud-top entrainment to accurately model stratocumulus cloud radiative flux. 1The regulatory term for UAV is remotely piloted aircraft (RPA).

scholarly journals Assessment of fossil fuel carbon dioxide and other anthropogenic trace gas emissions from airborne measurements over Sacramento, California in spring 2009

2011 ◽  
Vol 11 (2) ◽  
pp. 705-721 ◽  
Author(s):  
J. C. Turnbull ◽  
A. Karion ◽  
M. L. Fischer ◽  
I. Faloona ◽  
T. Guilderson ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Mole Fraction ◽  
Fossil Fuel ◽  
Trace Gases ◽  
Emission Inventories ◽  
Airborne Measurements ◽  
Boundary Layer Height ◽  
The Difference ◽  
Emission Ratios

Abstract. Direct quantification of fossil fuel CO2 (CO2ff) in atmospheric samples can be used to examine several carbon cycle and air quality questions. We collected in situ CO2, CO, and CH4 measurements and flask samples in the boundary layer and free troposphere over Sacramento, California, USA, during two aircraft flights over and downwind of this urban area during spring of 2009. The flask samples were analyzed for Δ14CO2 and CO2 to determine the recently added CO2ff mole fraction. A suite of greenhouse and other trace gases, including hydrocarbons and halocarbons, were measured in the same samples. Strong correlations were observed between CO2ff and numerous trace gases associated with urban emissions. From these correlations we estimate emission ratios between CO2ff and these species, and compare these with bottom-up inventory-derived estimates. Recent county level inventory estimates for carbon monoxide (CO) and benzene from the California Air Resources Board CEPAM database are in good agreement with our measured emission ratios, whereas older emissions inventories appear to overestimate emissions of these gases by a factor of two. For most other trace species, there are substantial differences (200–500%) between our measured emission ratios and those derived from available emission inventories. For the first flight, we combine in situ CO measurements with the measured CO:CO2ff emission ratio of 14 ± 2 ppbCO/ppmCO2 to derive an estimate of CO2ff mole fraction throughout this flight, and also estimate the biospheric CO2 mixing ratio (CO2bio) from the difference of total and fossil CO2. The resulting CO2bio varies dramatically from up to 8 ± 2 ppm in the urban plume to −6 ± 1 ppm in the surrounding boundary layer air. Finally, we use the in situ estimates of CO2ff mole fraction to infer total fossil fuel CO2 emissions from the Sacramento region, using a mass balance approach. The resulting emissions are uncertain to within a factor of two due to uncertainties in wind speed and boundary layer height. Nevertheless, this first attempt to estimate urban-scale CO2ff from atmospheric radiocarbon measurements shows that CO2ff can be used to verify and improve emission inventories for many poorly known anthropogenic species, separate biospheric CO2, and indicates the potential to constrain CO2ff emissions if transport uncertainties are reduced.

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