RESUMO
Nitrogen oxides (NO x =NO+NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations in NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements and surface EPA Air Quality System (AQS) observations as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; GOME-2A: Global Ozone Monitoring Experiment - 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument in July 2011 during the DISCOVER-AQ campaign over the Baltimore-Washington region. The model simulations at 36 and 4 km resolutions are in reasonably good agreement with the regional mean temporospatial NO2 observations in the daytime. However, we find significant overestimations (underestimations) of model-simulated NO2 (O3) surface concentrations during night-time, which can be mitigated by enhancing nocturnal vertical mixing in the model. Another discrepancy is that Pandora-measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. The higher-resolution 4 km simulations tend to show larger biases compared to the observations due largely to the larger spatial variations in NO x emissions in the model when the model spatial resolution is increased from 36 to 4 km. OMI, GOME-2A, and the high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than corresponding 36 and 4 km model simulations, likely reflecting the spatial distribution bias of NO x emissions in the National Emissions Inventory (NEI) 2011.
RESUMO
The Korea-United States Air Quality Study (KORUS-AQ) conducted during May-June 2016 offered the first opportunity to evaluate direct-sun observations of formaldehyde (HCHO) total column densities with improved Pandora spectrometer instruments. The measurements highlighted in this work were conducted both in the Seoul megacity area at the Olympic Park site (37.5232° N, 27.1260° E; 26 ma.s.l.) and at a nearby rural site downwind of the city at the Mount Taehwa research forest site (37.3123° N, 127.3106° E; 160ma.s.l.). Evaluation of these measurements was made possible by concurrent ground-based in situ observations of HCHO at both sites as well as overflight by the NASA DC-8 research aircraft. The flights provided in situ measurements of HCHO to characterize its vertical distribution in the lower troposphere (0-5km). Diurnal variation in HCHO total column densities followed the same pattern at both sites, with the minimum daily values typically observed between 6:00 and 7:00 local time, gradually increasing to a maximum between 13:00 and 17:00 before decreasing into the evening. Pandora vertical column densities were compared with those derived from the DC-8 HCHO in situ measured profiles augmented with in situ surface concentrations below the lowest altitude of the DC-8 in proximity to the ground sites. A comparison between 49 column densities measured by Pandora vs. aircraft-integrated in situ data showed that Pandora values were larger by 16% with a constant offset of 0.22DU (Dobson units; R 2 = 0.68). Pandora HCHO columns were also compared with columns calculated from the surface in situ measurements over Olympic Park by assuming a well-mixed lower atmosphere up to a ceilometer-measured mixed-layer height (MLH) and various assumptions about the small residual HCHO amounts in the free troposphere up to the tropopause. The best comparison (slope = 1.03±0.03; intercept = 0.29±0.02DU; and R 2 = 0.78±0.02) was achieved assuming equal mixing within ceilometer-measured MLH combined with an exponential profile shape. These results suggest that diurnal changes in HCHO surface concentrations can be reasonably estimated from the Pandora total column and information on the mixed-layer height. More work is needed to understand the bias in the intercept and the slope relative to columns derived from the in situ aircraft and surface measurements.
RESUMO
Differing boundary/mixed-layer height measurement methods were assessed in moderately-polluted and clean environments, with a focus on the Vaisala CL51 ceilometer. This intercomparison was performed as part of ongoing measurements at the Chemistry And Physics of the Atmospheric Boundary Layer Experiment (CAPABLE) site in Hampton, Virginia and during the 2014 Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaign that took place in and around Denver, Colorado. We analyzed CL51 data that were collected via two different methods (BLView software, which applied correction factors, and simple terminal emulation logging) to determine the impact of data collection methodology. Further, we evaluated the STRucture of the ATmosphere (STRAT) algorithm as an open-source alternative to BLView (note that the current work presents an evaluation of the BLView and STRAT algorithms and does not intend to act as a validation of either). Filtering criteria were defined according to the change in mixed-layer height (MLH) distributions for each instrument and algorithm and were applied throughout the analysis to remove high-frequency fluctuations from the MLH retrievals. Of primary interest was determining how the different data-collection methodologies and algorithms compare to each other and to radiosonde-derived boundary-layer heights when deployed as part of a larger instrument network. We determined that data-collection methodology is not as important as the processing algorithm and that much of the algorithm differences might be driven by impacts of local meteorology and precipitation events that pose algorithm difficulties. The results of this study show that a common processing algorithm is necessary for LIght Detection And Ranging (LIDAR)-based MLH intercomparisons, and ceilometer-network operation and that sonde-derived boundary layer heights are higher (10-15% at mid-day) than LIDAR-derived mixed-layer heights. We show that averaging the retrieved MLH to 1-hour resolution (an appropriate time scale for a priori data model initialization) significantly improved correlation between differing instruments and differing algorithms.