Felicia Kolonjari

Comparison of upper tropospheric carbon monoxide from MOPITT, ACE-FTS, and HIPPO-QCLS

Products from the Measurements Of Pollution In The Troposphere (MOPITT) instrument are regularly validated using in situ airborne measurements. However, few of these measurements reach into the upper troposphere, thus hindering MOPITT validation in that region. Here we evaluate upper tropospheric (~500 hPa to the tropopause) MOPITT CO profiles by comparing them to satellite Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) retrievals and to measurements from the High-performance Instrumented Airborne Platform for Environmental Research Pole to Pole Observations (HIPPO) Quantum Cascade Laser Spectrometer (QCLS). Direct comparison of colocated v5 MOPITT thermal infrared-only retrievals, v3.0 ACE-FTS retrievals, and HIPPO-QCLS measurements shows a slight positive MOPITT CO bias within its 10% accuracy requirement with respect to the other two data sets. Direct comparison of colocated ACE-FTS and HIPPO-QCLS measurements results in a small number of samples due to the large disparity in sampling pattern and density of these data sets. Thus, two additional indirect techniques for comparison of noncoincident data sets have been applied: tracer-tracer (CO-O3) correlation analysis and analysis of profiles in tropopause coordinates. These techniques suggest a negative bias of ACE-FTS with respect to HIPPO-QCLS; this could be caused by differences in resolution (horizontal, vertical) or by deficiencies in the ACE-FTS CO retrievals below ~20 km of altitude, among others. We also investigate the temporal stability of MOPITT and ACE-FTS data, which provide unique global CO records and are thus important in climate analysis. Our results indicate that the relative bias between the two data sets has remained generally stable during the 2004–2010 period.

An idealized stratospheric model useful for understanding differences between long‐lived trace gas measurements and global chemistry‐climate model output

We use a modified version of the tropical leaky pipe (TLP) model of the stratosphere to explore how well an idealized model can (1) reproduce global chemistry-climate model (CCM) output and (2) constrain transport characteristics necessary to replicate measurements of long-lived trace gases. The version of the TLP model we use includes the simulation of long-lived trace gases, such as SF6 and CO2, as well as photochemically active trace gases such as CFC-11, CFC-12, and N2O. The TLP model was found to accurately replicate trace gas output from the Canadian Middle Atmosphere Model (CMAM) for time-averaged profiles in the tropics and each extratropical region. Given confidence that the TLP model represents the basic transport features in CMAMwe then used the TLP model to interpret differences between CMAM output and measurements from the Atmospheric Chemistry Experiment and balloons. The TLP model is shown to uniquely determine residual mean circulation and recirculation (mixing between the extratropics and tropics) changes necessary for CMAM to more accurately simulate the measurements. Such guidance on these transport parameters is novel due to the relatively high precision and the simultaneous derivation of important parameters, as compared to previous studies. The TLP model can ideally be used as a bridge between measurements and CCMs to potentially allow more targeted modification of the CCMs than would otherwise be possible.

Characterization of aerosol growth events over Ellesmere Island during the summers of 2015 and 2016

The occurrence of frequent aerosol nucleation and growth events in the Arctic during summertime may impact the region’s climate through increasing the number of cloud condensation nuclei in the Arctic atmosphere. Measurements of aerosol size distributions and aerosol composition were taken during the summers of 2015 and 2016 at Eureka and Alert on 15 Ellesmere Island in Nunavut, Canada. The corresponding results provide a better understanding of the frequency and spatial extent of these nucleation and growth events as well as of the composition and sources of aerosol mass during particle growth. These events are observed beginning in June with the melting of the sea ice rather than with polar sunrise, which strongly suggests emissions from marine sources are the primary cause of the events. Frequent particle nucleation followed by growth occurs throughout the summer. Correlated particle growths events at the two sites, separated by 480 km, indicate 20 conditions existing over such large scales play a key role in determining the timing and the characteristics of the events. In addition, aerosol mass spectrometry measurements are used to analyze the size-resolved chemical composition of aerosols during two selected growth events. It is found that particles with diameters smaller than 100 nm are predominately organic with only a small sulphate contribution. The oxidation of the organic fraction also changes with particle size with larger particles containing a greater fraction of organic acids relative to other non-acid oxygenates (e.g. alcohols or 25 aldehydes). It is also observed that the relative amount of m/z 44 in the measured mass spectra increases during the growth events suggesting increases in organic acid concentrations in the particle phase. The nucleation and growth events at Eureka are observed most often when the temperature inversion between the sea and the measurement site (at 610 m ASL) is non-existent or weak allowing presumably fresh marine emissions to be mixed upward to the observatory altitude. While the nature of the gaseous precursors responsible for the growth events are 30 poorly understood, oxidation of dimethyl sulphide alone to produce particle phase sulphate or methanesulphonic acid is not consistent with the measured aerosol composition, suggesting the importance of condensation of other gas phase organic compounds for particle growth. 1 Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-428 Manuscript under review for journal Atmos. Chem. Phys. Discussion started: 8 May 2018 c

Multi-year comparisons of ground-based and space-borne Fourier Transform Spectrometers in the high Arctic between 2006 and 2013

This paper presents 8 years (2006–2013) of measurements obtained from Fourier transform spectrometers (FTSs) in the high Arctic at the Polar Environment Atmospheric Research Laboratory (PEARL; 80.05 N, 86.42W). These measurements were taken as part of the Canadian Arctic ACE (Atmospheric Chemistry Experiment) validation campaigns that have been carried out since 2004 during the polar sunrise period (from mid-February to mid-April). Each spring, two ground-based FTSs were used to measure total and partial columns of HF, O3, and trace gases that impact O3 depletion, namely, HCl and HNO3. Additionally, some tropospheric greenhouse gases and pollutant species were measured, namely CH4, N2O, CO, and C2H6. During the same time period, the satellite-based ACE-FTS made measurements near Eureka and provided profiles of the same trace gases. Comparisons have been carried out between the measurements from the Portable Atmospheric Research Interferometric Spectrometer for the InfraRed (PARIS-IR) and the co-located high-resolution Bruker 125HR FTS, as well as with the latest version of the ACE-FTS retrievals (v3.5). The total column comparison between the two colocated ground-based FTSs, PARIS-IR and Bruker 125HR, found very good agreement for most of these species (except HF), with differences well below the estimated uncertainties (≤ 6%) and with high correlations (R ≥ 0.8). Partial columns have been used for the ground-based to space-borne comparison, with coincident measurements selected based on time, distance, and scaled potential vorticity (sPV). The comparisons of the ground-based measurements with ACEFTS show good agreement in the partial columns for most species within 6 % (except for C2H6 and PARIS-IR HF), which is consistent with the total retrieval uncertainty of the ground-based instruments. The correlation coefficients (R) of the partial column comparisons for all eight species range from approximately 0.75 to 0.95. The comparisons show no notable increases of the mean differences over these 8 years, indicating the consistency of these datasets and suggesting that the space-borne ACE-FTS measurements have been stable over this period. In addition, changes in the amounts of these trace gases during springtime between 2006 and 2013 are presented and discussed. Increased O3 (0.9%yr−1), HCl (1.7%yr−1), HF (3.8%yr−1), CH4 (0.5 % yr−1), and C2H6 (2.3%yr−1, 2009–2013) have been found with the PARIS-IR dataset, the longer of the two ground-based records. Published by Copernicus Publications on behalf of the European Geosciences Union. 3274 D. Griffin et al.: Ground-based and space-borne FTS comparisons in the high Arctic (2006–2013)