ALBERT

Description: Journal of the American Chemical Society DOI: 10.1021/jacs.5b13220

Description: Langmuir DOI: 10.1021/acs.langmuir.6b03771

Description: Formaldehyde (HCHO), a key aerosol precursor, plays a significant role in atmospheric photo-oxidation pathways. In this study, HCHO column densities were measured using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument at the University of Chinese Academy of Science (UCAS) in Huairou District, Beijing, which is about 50 km away from the city center. Measurements were taken during the period of 1 October 2014 to 31 December 2014, and the Asia-Pacific Economic Cooperation (APEC) summit was organized on 5–11 November. Peak values of HCHO vertical column densities (VCDs) around noon and a good correlation coefficient R2 of 0.73 between HCHO VCDs and surface O3 concentration during noontime indicated that the secondary sources of HCHO through photochemical reactions of volatile organic compounds (VOCs) dominated the HCHO values in the area around UCAS. Dependences of HCHO VCDs on wind fields and backward trajectories were identified and indicated that the HCHO values in the area around UCAS were considerably affected by the transport of pollutants (VOCs) from polluted areas in the south. The effects of control measures on HCHO VCDs during the APEC period were evaluated. During the period of the APEC conference, the average HCHO VCDs were ∼38%±20% and ∼30%±24% lower than that during the pre-APEC and post-APEC periods calculated at the 95 % confidence limit, respectively. This phenomenon could be attributed to both the effects of prevailing northwest wind fields during APEC and strict control measures. We also compared the MAX-DOAS results with the Copernicus Atmosphere Monitoring Service (CAMS) model. The HCHO VCDs of the CAMS model and MAX-DOAS were generally consistent with a correlation coefficient R2 greater than 0.68. The peak values were consistently captured by both data datasets, but the low values were systematically underestimated by the CAMS model. This finding may indicate that the CAMS model can adequately simulate the effects of the transport and the secondary sources of HCHO but underestimates the local primary sources.

Description: Recently, Chinese cities have suffered severe events of haze air pollution, particularly in the North China Plain (NCP). Investigating the temporal and spatial distribution of pollutants, emissions, and pollution transport is necessary to better understand the effect of various sources on air quality. We report on mobile differential optical absorption spectroscopy (mobile DOAS) observations of precursors SO2 and NO2 vertical columns in the NCP in the summer of 2013 (from 11 June to 7 July) in this study. The different temporal and spatial distributions of SO2 and NO2 vertical column density (VCD) over this area are characterized under various wind fields. The results show that transport from the southern NCP strongly affects air quality in Beijing, and the transport route, particularly SO2 transport on the route of Shijiazhuang–Baoding–Beijing, is identified. In addition, the major contributors to SO2 along the route of Shijiazhuang–Baoding–Beijing are elevated sources compared to low area sources for the route of Dezhou–Cangzhou–Tianjin–Beijing; this is found using the interrelated analysis between in situ and mobile DOAS observations during the measurement periods. Furthermore, the discussions on hot spots near the city of JiNan show that average observed width of polluted air mass is 11.83 and 17.23 km associated with air mass diffusion, which is approximately 60 km away from emission sources based on geometrical estimation. Finally, a reasonable agreement exists between the Ozone Monitoring Instrument (OMI) and mobile DOAS observations, with a correlation coefficient (R2) of 0.65 for NO2 VCDs. Both datasets also have a similar spatial pattern. The fitted slope of 0.55 is significantly less than unity, which can reflect the contamination of local sources, and OMI observations are needed to improve the sensitivities to the near-surface emission sources through improvements of the retrieval algorithm or the resolution of satellites.

Description: In this study, the tropospheric NO2 vertical column density (VCD) over an urban site in Guangzhou megacity in China is investigated by means of MAX-DOAS measurements during a campaign from late March 2015 to mid-March 2016. A MAX-DOAS system was deployed at the Guangzhou Institute of Geochemistry of the Chinese Academy of Sciences and operated there for about 1 year, during the spring and summer months. The tropospheric NO2 VCDs retrieved by the MAX-DOAS are presented and compared with space-borne observations from GOME-2/MetOp-A, GOME-2/MetOp-B and OMI/Aura satellite sensors. The comparisons reveal good agreement between satellite and MAX-DOAS observations over Guangzhou, with correlation coefficients ranging between 0.795 for GOME-2B and 0.996 for OMI. However, the tropospheric NO2 loadings are underestimated by the satellite sensors on average by 25.1, 10.3 and 5.7 %, respectively, for OMI, GOME-2A and GOME-2B. Our results indicate that GOME-2B retrievals are closer to those of the MAX-DOAS instrument due to the lower tropospheric NO2 concentrations during the days with valid GOME-2B observations. In addition, the effect of the main coincidence criteria is investigated, namely the cloud fraction (CF), the distance (d) between the satellite pixel center and the ground-based measurement site, as well as the time period within which the MAX-DOAS data are averaged around the satellite overpass time. The effect of CF and time window criteria is more profound on the selection of OMI overpass data, probably due to its smaller pixel size. The available data pairs are reduced to half and about one-third for CF  ≤  0.3 and CF  ≤  0.2, respectively, while, compared to larger CF thresholds, the correlation coefficient is improved to 0.996 from about 0.86, the slope value is very close to unity ( ∼  0.98) and the mean satellite underestimation is reduced to about half (from  ∼  7 to  ∼  3.5  ×  1015 molecules cm−2). On the other hand, the distance criterion affects mostly GOME-2B data selection, because GOME-2B pixels are quite evenly distributed among the different radii used in the sensitivity test. More specifically, the number of collocations is notably reduced when stricter radius limits are applied, the r value is improved from 0.795 (d ≤  50 km) to 0.953 (d ≤  20 km), and the absolute mean bias decreases about 6 times for d ≤  30 km compared to the reference case (d ≤  50 km).

Description: In order to promote the development of the passive DOAS technique the Multi Axis DOAS – Comparison campaign for Aerosols and Trace gases (MAD-CAT) was held at the Max Planck Institute for Chemistry in Mainz, Germany, from June to October 2013. Here, we systematically compare the differential slant column densities (dSCDs) of nitrous acid (HONO) derived from measurements of seven different instruments. We also compare the tropospheric difference of SCDs (delta SCD) of HONO, namely the difference of the SCDs for the non-zenith observations and the zenith observation of the same elevation sequence. Different research groups analysed the spectra from their own instruments using their individual fit software. All the fit errors of HONO dSCDs from the instruments with cooled large-size detectors are mostly in the range of 0.1 to 0.3  ×  1015 molecules cm−2 for an integration time of 1 min. The fit error for the mini MAX-DOAS is around 0.7  ×  1015 molecules cm−2. Although the HONO delta SCDs are normally smaller than 6  ×  1015 molecules cm−2, consistent time series of HONO delta SCDs are retrieved from the measurements of different instruments. Both fits with a sequential Fraunhofer reference spectrum (FRS) and a daily noon FRS lead to similar consistency. Apart from the mini-MAX-DOAS, the systematic absolute differences of HONO delta SCDs between the instruments are smaller than 0.63  ×  1015 molecules cm−2. The correlation coefficients are higher than 0.7 and the slopes of linear regressions deviate from unity by less than 16 % for the elevation angle of 1°. The correlations decrease with an increase in elevation angle. All the participants also analysed synthetic spectra using the same baseline DOAS settings to evaluate the systematic errors of HONO results from their respective fit programs. In general the errors are smaller than 0.3  ×  1015 molecules cm−2, which is about half of the systematic difference between the real measurements.The differences of HONO delta SCDs retrieved in the selected three spectral ranges 335–361, 335–373 and 335–390 nm are considerable (up to 0.57  ×  1015 molecules cm−2) for both real measurements and synthetic spectra. We performed sensitivity studies to quantify the dominant systematic error sources and to find a recommended DOAS setting in the three spectral ranges. The results show that water vapour absorption, temperature and wavelength dependence of O4 absorption, temperature dependence of Ring spectrum, and polynomial and intensity offset correction all together dominate the systematic errors. We recommend a fit range of 335–373 nm for HONO retrievals. In such fit range the overall systematic uncertainty is about 0.87  ×  1015 molecules cm−2, much smaller than those in the other two ranges. The typical random uncertainty is estimated to be about 0.16  ×  1015 molecules cm−2, which is only 25 % of the total systematic uncertainty for most of the instruments in the MAD-CAT campaign. In summary for most of the MAX-DOAS instruments for elevation angle below 5°, half daytime measurements (usually in the morning) of HONO delta SCD can be over the detection limit of 0.2  ×  1015 molecules cm−2 with an uncertainty of  ∼  0.9  ×  1015 molecules cm−2.

Description: We characterize the temporal variation and vertical distribution of nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (HCHO) and aerosol extinction based on long-term multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations from May 2011 to November 2014 in Wuxi, China. A new inversion algorithm (PriAM) is implemented to retrieve profiles of the trace gases (TGs) and aerosol extinction (AE) from the UV spectra of scattered sunlight recorded by the MAX-DOAS instrument. We investigated two important aspects of the retrieval process. We found that the systematic seasonal variation of temperature and pressure (which is regularly observed in Wuxi) can lead to a systematic bias of the retrieved aerosol profiles (e.g. up to 20 % for the AOD) if it is not explicitly considered. In this study we take this effect into account for the first time. We also investigated in detail the reason for the differences of tropospheric vertical column densities derived from either the geometric approximation or by the integration of the retrieved profiles, which were reported by earlier studies. We found that these differences are almost entirely caused by the limitations of the geometric approximation (especially for high aerosol loads). The results retrieved from the MAX-DOAS observations are compared with independent techniques not only under cloud-free sky conditions, but also under various cloud scenarios. Under most cloudy conditions (except fog and optically thick clouds), the trace gas results still show good agreements. In contrast, for the aerosol results, only near-surface AE could be still well retrieved under cloudy situations. After applying a quality control procedure, the MAX-DOAS data are used to characterize the seasonal, diurnal and weekly variations of NO2, SO2, HCHO and aerosols. A regular seasonality of the three trace gases is found, but not for aerosols. Similar annual variations of the profiles of the trace gases appear in different years. Only NO2 shows a significant seasonality of the diurnal variations. Considerable amplitudes of weekly cycles occur for NO2 and SO2, but not for HCHO and aerosols. The TGs and aerosols show good correlations, especially for HCHO in winter. More pronounced wind direction dependencies, especially for the near-surface concentrations, are found for the trace gases than for the aerosols, which implies that the local emissions from nearby industrial areas (including traffic emissions) dominate the local pollution, while long-distance transport might also considerably contribute to the local aerosol levels.

Description: Tropospheric vertical column densities (VCDs) of NO2, SO2 and HCHO derived from the Ozone Monitoring Instrument (OMI) on AURA and the Global Ozone Monitoring Experiment 2 aboard METOP-A (GOME-2A) and METOP-B (GOME-2B) are widely used to characterize the global distributions, trends and dominating sources of these trace gases. They are also useful for the comparison with chemical transport models (CTMs). We use tropospheric VCDs and vertical profiles of NO2, SO2 and HCHO derived from MAX-DOAS measurements from 2011 to 2014 in Wuxi, China, to validate the corresponding products (daily and bi-monthly-averaged data) derived from OMI and GOME-2A/B by different scientific teams. Prior to the comparison, the spatial and temporal coincidence criteria for MAX-DOAS and satellite data are determined by a sensitivity study using different spatial and temporal averaging conditions. Cloud effects on both MAX-DOAS and satellite observations are also investigated. Our results indicate that the discrepancies between satellite and MAX-DOAS results increase with increasing effective cloud fraction and are dominated by the effects of clouds on the satellite products. In comparison with MAX-DOAS, we found a systematic underestimation of all SO2 (40 to 57 %) and HCHO products (about 20 %), and an overestimation of the GOME-2A/B NO2 products (about 30 %), but good consistency with the DOMINO version 2 NO2 product. To better understand the reasons for these differences, we evaluated the a priori profile shapes used in the OMI retrievals (derived from CTM) by comparison with those derived from the MAX-DOAS observations. Significant differences are found for the SO2 and HCHO profile shapes derived from the IMAGES model, whereas on average good agreement is found for the NO2 profile shapes derived from the TM4 model. We also applied the MAX-DOAS profile shapes to the satellite retrievals and found that these modified satellite VCDs agree better with the MAX-DOAS VCDs than the VCDs from the original data sets by up to 10, 47 and 35 % for NO2, SO2 and HCHO, respectively. Furthermore, we investigated the effect of aerosols on the satellite retrievals. For OMI observations of NO2, a systematic underestimation is found for large AOD, which is mainly attributed to effect of the aerosols on the cloud retrieval and the subsequent application of a cloud correction scheme (implicit aerosol correction). In contrast, the effect of aerosols on the clear-sky air mass factor (explicit aerosol correction) has a smaller effect. For SO2 and HCHO observations selected in the same way, no clear aerosol effect is found, probably because for the considered data sets no cloud correction is applied (and also because of the larger scatter). From our findings we conclude that for satellite observations with cloud top pressure (CTP) 〉 900 hPa and effective cloud fraction (eCF) 

Description: We show that the up-scaling of wind turbines from rotor diameters of 15–20 m to presently large rotors of 150–200 m has changed the requirements for the aerodynamic Blade Element Momentum (BEM) models in the aeroelastic codes. This is because the typical scales in the inflow turbulence are now comparable with the rotor diameter of the large turbines. Therefore the spectrum of the incoming turbulence relative to the rotating blade has increased energy content on 1P, 2P, ..., nP and the annular mean induction approach in a classical BEM implementation might no longer be a good approximation for large rotors. We present a complete BEM implementation on a polar grid that models the induction response to the considerable 1P, 2P, ..., nP inflow variations, including models for yawed inflow, dynamic inflow and radial induction. At each time step in an aeroelastic simulation the induction derived from a local BEM approach is updated at all the stationary grid points covering the swept area so the model can be characterized as an engineering actuator disc (AD) solution. The induction at each grid point varies slowly in time due to the dynamic inflow filter but the rotating blade now samples the induction field; as a result the induction seen from the blade is highly unsteady and has a spectrum with distinct 1P, 2P, ..., nP peaks. The load impact mechanism from this unsteady induction is analyzed and it is found that the load impact strongly depends on the turbine design and operating conditions. For operation at low to medium thrust coefficients (conventional turbines at above rated wind speed or low induction turbines in the whole operating range) it is found that the grid BEM gives typically 8–10 % lower 1 Hz fatigue loads than the classical annular mean BEM approach. At high thrust coefficients the grid BEM can give slightly increased fatigue loads. In the paper the implementation of the grid based BEM is described in detail and finally several validation cases are presented.

Description: In this study, the tropospheric NO2 vertical column density (VCD) over an urban site in Guangzhou megacity in China is investigated, by means of MAX-DOAS measurements during a campaign from late March 2015 to mid-March 2016. A MAX-DOAS system was deployed at the Guangzhou Institute of Geochemistry of the Chinese Academy of Sciences and operated there for about one year, during the spring and summer months. The tropospheric NO2 VCDs retrieved by the MAX-DOAS are presented and compared with space-borne observations from GOME-2/MetOp-A, GOME-2/MetOp-B and OMI/Aura satellite sensors. The comparisons reveal good agreement between satellite and MAX-DOAS observations over Guangzhou, with correlation coefficients ranging between 0.76 for GOME-2B and 0.99 for GOME-2A. However, the tropospheric NO2 loadings are underestimated by the satellite sensors on average by 25.1 %, 10.3 % and 5.7 %, respectively for OMI, GOME-2A and GOME-2B. Our results indicate that GOME-2B retrievals are closer to those of the MAX-DOAS instrument due to the lower tropospheric NO2 concentrations during the days with valid GOME-2B observations. In addition, the effect of the main coincidence criteria is investigated, namely the cloud fraction (CF), the distance (d) between the satellite pixel center and the ground-based measurement site, as well as the time period within which the MAX-DOAS data are averaged around the satellite overpass time. The effect of CF and time window criteria is more profound on the selection of OMI overpass data, probably due to its smaller pixel size. The available data pairs are reduced to half and about one third for CF ≤ 0.3 and CF ≤ 0.2, respectively, while, compared to larger CF thresholds, the correlation coefficient is improved to 0.99 from about 0.6, the slope value is almost doubled (~ 0.8) and the mean satellite underestimation is reduced to about half (from ~ 7 to ~ 3.5 × 1015 molecules/cm2). On the other hand, the distance criterion affects mostly GOME-2B data selection, because GOME-2B pixels are quite evenly distributed among the different radii used in the sensitivity test. More specifically, the number of collocations is notably reduced when stricter radius limits are applied, the r value is improved from 0.76 (d ≤ 50 km) to 0.93 (d ≤ 20 km), and the absolute mean bias decreases about 6 times for d ≤ 30 km compared to the reference case (d ≤ 50 km).