scholarly journals The first evaluation of formaldehyde column observations by improved Pandora spectrometers during the KORUS-AQ field study

2018 ◽  
Vol 11 (9) ◽  
pp. 4943-4961 ◽  
Author(s):  
Elena Spinei ◽  
Andrew Whitehill ◽  
Alan Fried ◽  
Martin Tiefengraber ◽  
Travis N. Knepp ◽  
...  

Abstract. 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 m a.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; 160 m a.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 (0–5 km). 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 0.22 DU (Dobson units; R2=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±0.02 DU; and R2=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.

2018 ◽  
Author(s):  
Elena Spinei ◽  
Andrew Whitehill ◽  
Alan Fried ◽  
Martin Tiefengraber ◽  
Travis N. Knepp ◽  
...  

Abstract. The KORUS-AQ field study 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 (latitude: 37.5232° N, longitude: 127.1260° E, 26 m a.s.l.) and at a nearby rural site downwind of the city at the Mount Taehwa Research Forest site (latitude: 37.3123° N, longitude: 127.3106° E, 160 m a.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 (0–5 km). Diurnal variation in HCHO total column densities followed the same pattern at both sites, with the minimum daily values typically observed between 6:00–7:00 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 versus aircraft integrated in-situ data showed that Pandora values were larger by 16 % (intercept = 0.22 DU, R2 =  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 ± 0.02 DU and R2 of 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.


2017 ◽  
Vol 10 (10) ◽  
pp. 3963-3983 ◽  
Author(s):  
Travis N. Knepp ◽  
James J. Szykman ◽  
Russell Long ◽  
Rachelle M. Duvall ◽  
Jonathan Krug ◽  
...  

Abstract. 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 midday) than lidar-derived mixed-layer heights. We show that averaging the retrieved MLH to 1 h resolution (an appropriate timescale for a priori data model initialization) significantly improved the correlation between differing instruments and differing algorithms.


2021 ◽  
Vol 14 (2) ◽  
pp. 905-921
Author(s):  
Shoma Yamanouchi ◽  
Camille Viatte ◽  
Kimberly Strong ◽  
Erik Lutsch ◽  
Dylan B. A. Jones ◽  
...  

Abstract. Ammonia (NH3) is a major source of nitrates in the atmosphere and a major source of fine particulate matter. As such, there have been increasing efforts to measure the atmospheric abundance of NH3 and its spatial and temporal variability. In this study, long-term measurements of NH3 derived from multiscale datasets are examined. These NH3 datasets include 16 years of total column measurements using Fourier transform infrared (FTIR) spectroscopy, 3 years of surface in situ measurements, and 10 years of total column measurements from the Infrared Atmospheric Sounding Interferometer (IASI). The datasets were used to quantify NH3 temporal variability over Toronto, Canada. The multiscale datasets were also compared to assess the representativeness of the FTIR measurements. All three time series showed positive trends in NH3 over Toronto: 3.34 ± 0.89 %/yr from 2002 to 2018 in the FTIR columns, 8.88 ± 5.08 %/yr from 2013 to 2017 in the surface in situ data, and 8.38 ± 1.54 %/yr from 2008 to 2018 in the IASI columns. To assess the representative scale of the FTIR NH3 columns, correlations between the datasets were examined. The best correlation between FTIR and IASI was obtained with coincidence criteria of ≤25 km and ≤20 min, with r=0.73 and a slope of 1.14 ± 0.06. Additionally, FTIR column and in situ measurements were standardized and correlated. Comparison of 24 d averages and monthly averages resulted in correlation coefficients of r=0.72 and r=0.75, respectively, although correlation without averaging to reduce high-frequency variability led to a poorer correlation, with r=0.39. The GEOS-Chem model, run at 2∘ × 2.5∘ resolution, was compared to FTIR and IASI to assess model performance and investigate the correlation of observational data and model output, both with local column measurements (FTIR) and measurements on a regional scale (IASI). Comparisons on a regional scale (a domain spanning 35 to 53∘ N and 93.75 to 63.75∘ W) resulted in r=0.57 and thus a coefficient of determination, which is indicative of the predictive capacity of the model, of r2=0.33, but comparing a single model grid point against the FTIR resulted in a poorer correlation, with r2=0.13, indicating that a finer spatial resolution is needed for modeling NH3.


2017 ◽  
Vol 17 (6) ◽  
pp. 3891-3903 ◽  
Author(s):  
Rui Wang ◽  
Xiaobin Xu ◽  
Shihui Jia ◽  
Ruisheng Ma ◽  
Liang Ran ◽  
...  

Abstract. The North China Plain (NCP) has become one of the most polluted regions in China, with the rapidly increasing economic growth in the past decades. High concentrations of ambient O3 and aerosol have been observed at urban as well as rural sites in the NCP. Most of the in situ observations of air pollutants have been conducted near the ground so that current knowledge about the vertical distributions of tropospheric O3 and aerosol over the NCP region is still limited. In this study, vertical profiles of O3 and size-resolved aerosol concentrations below 2.5 km were measured in summer 2014 over a rural site in the NCP, using an unmanned aerial vehicle (UAV) equipped with miniature analyzers. In addition, vertical profiles of aerosol scattering property in the lower troposphere and vertical profiles of O3 below 1 km were also observed at the site using a lidar and tethered balloon, respectively. The depths of the mixed layer and residual layer were determined according to the vertical gradients of lidar particle extinction and aerosol number concentration. Average O3 and size-resolved aerosol number concentration in both the mixed and residual layer were obtained from the data observed in seven UAV flights. The results show that during most of the flights the O3 levels above the top of mixed layer were higher than those below. Such a positive gradient in the vertical distribution of O3 makes the residual layer an important source of O3 in the mixed layer, particularly during the morning when the top of mixed layer is rapidly elevated. In contrast to O3, aerosol number concentration was normally higher in the mixed layer than in the residual layer, particularly in the early morning. Aerosol particles were overwhelmingly distributed in the size range  <  1 µm, showing slight differences between the mixed and residual layers. Our measurements confirm that the lower troposphere over the rural area of the NCP is largely impacted by anthropogenic pollutants locally emitted or transported from urban areas. Compared with the historic O3 vertical profiles over Beijing from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC), a strong increase in O3 can be found at all heights below 2.5 km in the decade from 2004 to 2014, with the largest enhancement of about 41.6 ppb. This indicates that the lower troposphere over the northern part of the NCP has experienced rapidly worsening photochemical pollution. This worsening trend in photochemical pollution deserves more attention in the future.


2019 ◽  
Vol 12 (5) ◽  
pp. 2139-2153 ◽  
Author(s):  
Hendrik Wouters ◽  
Irina Y. Petrova ◽  
Chiel C. van Heerwaarden ◽  
Jordi Vilà-Guerau de Arellano ◽  
Adriaan J. Teuling ◽  
...  

Abstract. The coupling between soil, vegetation and atmosphere is thought to be crucial in the development and intensification of weather extremes, especially meteorological droughts, heat waves and severe storms. Therefore, understanding the evolution of the atmospheric boundary layer (ABL) and the role of land–atmosphere feedbacks is necessary for earlier warnings, better climate projection and timely societal adaptation. However, this understanding is hampered by the difficulties of attributing cause–effect relationships from complex coupled models and the irregular space–time distribution of in situ observations of the land–atmosphere system. As such, there is a need for simple deterministic appraisals that systematically discriminate land–atmosphere interactions from observed weather phenomena over large domains and climatological time spans. Here, we present a new interactive data platform to study the behavior of the ABL and land–atmosphere interactions based on worldwide weather balloon soundings and an ABL model. This software tool – referred to as CLASS4GL (http://class4gl.eu, last access: 27 May 2018) – is developed with the objectives of (a) mining appropriate global observational data from ∼15 million weather balloon soundings since 1981 and combining them with satellite and reanalysis data and (b) constraining and initializing a numerical model of the daytime evolution of the ABL that serves as a tool to interpret these observations mechanistically and deterministically. As a result, it fully automizes extensive global model experiments to assess the effects of land and atmospheric conditions on the ABL evolution as observed in different climate regions around the world. The suitability of the set of observations, model formulations and global parameters employed by CLASS4GL is extensively validated. In most cases, the framework is able to realistically reproduce the observed daytime response of the mixed-layer height, potential temperature and specific humidity from the balloon soundings. In this extensive global validation exercise, a bias of 10.1 m h−1, −0.036 K h−1 and 0.06 g kg−1 h−1 is found for the morning-to-afternoon evolution of the mixed-layer height, potential temperature and specific humidity. The virtual tool is in continuous development and aims to foster a better process understanding of the drivers of the ABL evolution and their global distribution, particularly during the onset and amplification of weather extremes. Finally, it can also be used to scrutinize the representation of land–atmosphere feedbacks and ABL dynamics in Earth system models, numerical weather prediction models, atmospheric reanalysis and satellite retrievals, with the ultimate goal of improving local climate projections, providing earlier warning of extreme weather and fostering a more effective development of climate adaptation strategies. The tool can be easily downloaded via http://class4gl.eu (last access: 27 May 2018) and is open source.


2021 ◽  
Author(s):  
Mikhail Yu. Arshinov ◽  
Boris Belan ◽  
Denis Davydov ◽  
Artem Kozlov ◽  
Alexandr Fofonov

&lt;p&gt;The Arctic is warming much faster than other regions of the globe. In 2020, temperature anomalies in the Russian Arctic reached unprecedented high levels. The atmospheric composition in this key region still remains insufficiently studied that makes difficult predicting future climate change.&lt;/p&gt;&lt;p&gt;In September 2020, an extensive aircraft campaign was conducted to document the tropospheric composition over the Russian Arctic. The Optik Tu-134 research aircraft was equipped with instruments to carry out in-situ measurements of trace gases and aerosols, as well as with a lidar for profiling of aerosol backscatter. The aircraft flew over a vast area from Arkhangelsk to Anadyr. Six measurement flights with changing altitudes from 0.2 to 9.0 m were conducted over the waters of the Barents, Kara, Laptev, East Siberian, Chukchi, and Bering Seas. The weather was unusually warm for this period of the year, surface air temperatures were above 0&amp;#176;C through the campaign.&lt;/p&gt;&lt;p&gt;Here, we present the results of in-situ measurements of the vertical distribution of aerosol number concentrations in a wide range of sizes. A modified diffusional particle sizer (DPS) consisted of the Novosibirsk-type eight-stage screen diffusion battery connected to the TSI condensation particle counter Model 3756 was used to determine the number size distribution of particles between 0.003 mm and 0.2 mm (20 size bins). Distribution of particles in the size range from 0.25 &amp;#181;m to 32 &amp;#181;m (31 size bins) was measured by means of the Grimm aerosol spectrometer Model 1.109.&lt;/p&gt;&lt;p&gt;The flights over Barents and Kara Seas were predominantly performed under clear sky or partly cloudy weather conditions. Number size distributions were wide representing particles of almost all aerosol fractions. When flying in the upper troposphere with a constant altitude over these seas, some cases of enhanced concentrations of nucleation and Aitken mode particles comparable to ones in the lower troposphere were recorded, suggesting in situ new particle formation was likely to be taking place via gas-to-particle conversion aloft.&lt;/p&gt;&lt;p&gt;East of the Kara Sea, flights were conducted under mostly cloudy conditions resulting in a lower median aerosol number concentration and narrower size distributions.&lt;/p&gt;&lt;p&gt;This work was supported by the Russian Foundation for Basic Research (Grant No. 19-05-50024).&lt;/p&gt;


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