Spatiotemporal characterization of PM2.5, O3, and trace gases associated with East Asian continental outflows via drone sounding.

East Asian continental outflows with PM2.5, O3, and other species may determine the baseline conditions and affect the air quality in downwind areas via long-range transport (LRT). To gain insight into the impact and spatiotemporal characteristics of airborne pollutants in East Asian continental outflows, a versatile multicopter drone sounding platform was used to simultaneously observe PM2.5, O3, CO2, and meteorological variables (temperature, specific humidity, pressure, and wind vector) above the northern tip of Taiwan, Cape Fuiguei, which often encounters continental outflows during winter monsoon periods. By coordinating hourly high-spatial-resolution profiles provided by drone soundings, WRF/CMAQ model air quality predictions, HYSPLIT-simulated backward trajectories, and MERRA-2 reanalysis data, we analyzed two prominent phenomena of airborne pollutants in continental outflows to better understand their physical/chemical characteristics. First, we found that pollutants were well mixed within a sounding height of 500 m when continental outflows passed through and completely enveloped Cape Fuiguei. Eddies induced by significant fluctuations in wind speeds coupled with minimal temperature inversion and LRT facilitated vertical mixing, possibly resulting in high homogeneity of pollutants within the outflow layer. Second, the drone soundings indicated exceptionally high O3 concentrations (70-100 ppbv) but relatively low concentrations of PM2.5 (10-20 µg/m3), CO2 (420-425 ppmv), and VOCs in some air masses. The low levels of PM2.5, CO2, and VOCs ruled out photochemistry as the cause of the formation of high-level O3. Further coordination of spatiotemporal data with air mass trajectories and O3 cross sections provided by MERRA-2 suggested that the high O3 concentrations could be attributed to stratospheric intrusion and advection via continental outflows. High-level O3 concentrations persisted in the lower troposphere, even reaching the surface, suggesting that stratospheric intrusion O3 may be involved in the rising trend in O3 concentrations in parts of East Asia in recent years in addition to surface photochemical factors.

SRS conversion efficiency assessment of a single cell Raman gas mixture for DIAL ozone lidar.

A single Raman cell configuration useful for DIAL ozone lidar is designed and optimized. The conversion efficiency and flexibility of using a single Raman cell filled with a mixture of high pressure Raman active gases hydrogen (H 2) and methane (C H 4) have been examined and reported. The stimulated Raman scattering (SRS) conversion efficiency of Raman active gases with different total cell pressures and the volume mixing ratio excited with a focused, frequency quadrupled Nd:YAG laser with a maximum pulse energy of 25 mJ and a pulse duration of 10 ns at 100 Hz repetition rate are examined in detail. The gas combination of H 2:C H 4 emits a coaxial beam of two wavelengths, 288.4 nm (C H 4) and 299.1 nm (H 2), with a maximum total conversion efficiency of about 45%. The optimum volume mixing ratio for generating the required wavelength pair with almost equal energies is found to be 2:1 (H 2:C H 4) at a total cell pressure of 18 bar. The contribution of cascade Raman scattering (CRS) and four-wave mixing (FWM) to the higher order Stokes lines is examined. The laser attenuation due to soot formation under various mixing ratios in the cell is also presented.

Effects of boundary layer variations on physicochemical characteristics of aerosols in mid-low-altitude regions.

Variations in the height of the boundary layer have a critical impact on the vertical transport of near-surface aerosols. Variations can affect the interactions between aerosols and clouds/fog by altering the scattering and absorption of solar radiation, significantly changing radiative forcing, convective precipitation, and regional climate. In this study, we simultaneously monitored air pollution and meteorological factors in a flat urban area (YunTech site, 50 m asl) and its peripheral mountainous region (MeiShan site, 980 m asl), analyzed the characteristics of pollutants under different atmospheric conditions, and explored the differences in the chemical reaction mechanisms of aerosols at various altitudes, aiming to clarify the evolution of the boundary layer in urban and suburban areas and its impact on the transport of pollutants. The results show that even without anthropogenic emissions, urban ground-level pollutants could be transported to peripheral mountainous areas through boundary layer height variations and local circulations, such as mountain-valley breezes. The PM2.5 concentration was higher at the urban site (average 31.14 ± 14.82µgm-3) and could be transported aloft by valley winds, leading to the gradual accumulation of daytime PM2.5 with an afternoon peak at the mountain site. Moreover, the nitrogen oxidation rate (NOR = [NO3-]/[NO3-] + [NO2]) exhibited clear site variations, the mountain site (average 0.41 ± 0.20) was higher than the urban site (average 0.19 ± 0.07), likely due to the atmospheric environment with thick clouds/fog and strong oxidation capacity in the mountain area. Our study has verified that aerosol characteristics, origins, formation pathways and transport mechanisms at the two measurement sites are significantly different under different conditions, which provides a theoretical basis for future air pollution prevention and regional climate research.

Integrated ground and vertical measurement techniques to characterize overhead atmosphere: Case studies of local versus transboundary pollution.

Much attention has been found to the long-range transport (LRT) of air pollutants and their adverse effects on downwind air qualities resulting from the Chinese haze, which frequently occurs in association with winter monsoon. This study integrates ground-based measurements, unmanned aerial vehicles (UAVs), and model simulations to characterize the meteorological, chemical, and particulate matter (PM) properties comprehensively for the events that were LRT or local pollution (LP) dominated in northern Taiwan during the wintertime of 2017. During the two types of episodes, various approaches were made to investigate the vertical mixing conditions and PM properties with UAV flights. A confined and PM accumulated feature near ground level with a temperature inversion was found during the LP event. In contrast, a vertically homogeneous atmospheric structure with strong winds was suggested during the LRT event. Independent measurements of criteria air pollutants, meteorological variables, volatile organic compounds (VOCs), and micropulse lidar (MPL) made at the ground level were closely supported by the vertical measurements. When synchronizing all these observational and numerical tools in a three-dimensional manner, the characterization of air masses and possible origins of pollution, such as LP vs. LRT, has now become more versatile and capable of gaining a complete picture of atmospheric conditions that define air quality.

A study of the vertical homogeneity of trace gases in East Asian continental outflow.

East Asian continental outflows containing with pollutants may deteriorate air quality in the downwind region via long-range transport (LRT). In particular, cold fronts with high wind speeds generally promote the LRT of air pollutants to further downwind areas, including Taiwan. To gain an insightful understanding of the characteristics and vertical homogeneity of trace gases in East Asian continental outflows, as well as their relation with atmospheric meteorological conditions, whole air samples were collected above a cape at the northern tip of the island of Taiwan during frontal passages. Aerial samples were collected at multiple altitudes from the surface to a maximum height of 700 m with a multicopter sounding platform carrying a robotic whole air sampling device. Simultaneously, aerial meteorological variables of temperature and wind vector from near the surface to a maximum height of 1000 m were also measured during the whole air sampling periods. An array of 106 volatile organic compounds (VOCs) as well as CO, CO2, and CH4 were analyzed to characterize the air composition and vertical homogeneity of trace gases. The results revealed rather homogeneous vertical distributions of most VOCs, CO, CO2, and CH4 in the frontal passages, indicating well-mixed conditions of trace gases in the East Asian continental outflows. The strong wind shear and minimal temperature inversion associated with the frontal passage likely induced turbulence and increased vertical mixing. Furthermore, higher levels of species characteristic of the East Asian continent were observed from the surface up to hundreds of meters above the cape, revealing a strong inflow of polluted air masses from the East Asian continent brought by cold frontal passages.

Determination of the vertical profile of aerosol chemical species in the microscale urban environment.

This study developed a lightweight air composition measuring equipment (ACME) mounted in unmanned aerial vehicles (UAVs) to measure the vertical distribution characteristics of PM2.5 chemical species in the micro-scale urban environment for the first time. 212 samples collected from 0 to 350 m above ground level were analyzed for water-soluble ions. The concentrations of most ions on the above ground level were higher than that on the ground surface during the sampling period. The measurements of the total ion concentrations were approximately 54 to 26% of the PM2.5 mass concentrations on the ground surface. The concentrations of NH4+ and NO3- decreased with increases in the height from the ground, which may be related to the influence of the vehicle emissions and human activities. NO2- and SO42- both had a peak concentration on the higher vertical altitude at night in the sea-land wind system. In the southern wind system, the emissions of sea salts, dust, and stationary pollution, might be transported by the regional prevailing airflow from the southern coastal area, were the major pollutant sources above the boundary layer. The vertical distribution of ionic concentrations and wind field provided information concerning changes in pollutant transport and source regions that affect the local air quality. The ACME mounted in UAVs is the feasible and convenient method to fast understand the vertical distributions of aerosol chemical species. It provides important information about the accumulation and diffusion effects by the boundary layer variation to aerosol characteristics, which is difficulty observed from the conventional ground-based measurements. In future, this technology is the useful application for investigating the pollutant species emitted from the smokestack and the sudden pollution accident.

Evaluating the Height of Biomass Burning Smoke Aerosols Retrieved from Synergistic Use of Multiple Satellite Sensors over Southeast Asia.

This study evaluates the height of biomass burning smoke aerosols retrieved from a combined use of Visible Infrared Imaging Radiometer Suite (VIIRS), Ozone Mapping and Profiler Suite (OMPS), and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) observations. The retrieved heights are compared against spaceborne and ground-based lidar measurements during the peak biomass burning season (March and April) over Southeast Asia from 2013 to 2015. Based on the comparison against CALIOP, a quality assurance (QA) procedure is developed. It is found that 74% (81-84%) of the retrieved heights fall within 1 km of CALIOP observations for unfiltered (QA-filtered) data, with root-mean-square error (RMSE) of 1.1 km (0.8-1.0 km). Eliminating the requirement for CALIOP observations from the retrieval process significantly increases the temporal coverage with only a slight decrease in the retrieval accuracy; for best QA data, 64% of data fall within 1 km of CALIOP observations with RMSE of 1.1 km. When compared with Micro-Pulse Lidar Network (MPLNET) measurements deployed at Doi Ang Khang, Thailand, the retrieved heights show RMSE of 1.7 km (1.1 km) for unfiltered (QA-filtered) data for the complete algorithm, and 0.9 km (0.8 km) for the simplified algorithm.

The real-time method of assessing the contribution of individual sources on visibility degradation in Taichung.

Visibility degradation caused by air pollution has become a serious environmental problem in megacities in Northeast Asia. In general, aerosol chemical compositions are measured by a conventional method of time integrated filter sampling for off-line analysis, which cannot represent temporal and spatial variations in the real atmosphere. The in situ air composition measuring equipment, OCEC carbon aerosol analyzer and a long-path visibility transmissometer-3 were used to collect hourly measurements of the soluble ions, organic/elemental carbon, and ambient visibility, respectively. During the observation, two types of weather conditions were identified: transport and stagnant. Because PM2.5 was identified as the predominant species of light extinction, the sources of PM2.5 were determined and investigated using a positive matrix factorization (PMF) analysis. The PMF outputs characterized the six main emission sources (marine/crustal aerosols, secondary nitrate, secondary sulfate, direct vehicle exhaust, coal/incinerator combustion, and local sewage emission) and reconstructed the PM2.5 mass concentrations of each pollutant source in two weather conditions. In addition, the light extinction (bext) was reconstructed using a multivariate linear regression analysis with hourly-reconstructed PM2.5 mass concentrations to determine the contributions of each source to bext. The primary results showed that the extinction coefficient was proportional to the PM2.5 with high value in stagnant weather conditions. The secondary sulfate was the most abundant source of bext contribution during the sampling period. In addition, the bext contributions of direct vehicle exhaust and coal/incinerator combustion significantly increased in the stagnant weather condition. According to the results of hourly measurements, this work further emphasized that the sources of direct vehicle exhaust and coal/incinerator combustion in PM2.5 were the important sources of visibility degradation in the stagnant weather conditions, which suggests that the pollutants derived from direct vehicle exhaust and coal/incinerator combustion should be controlled first to improve visibility in Taichung.

Case study of the Asian dust and pollutant event in spring 2006: source, transport, and contribution to Taiwan.

Surface measurements and a regional dust model were used to analyze the source, transport, and contribution of a dust event transporting with aerosol pollutant over Taiwan from 16 to 19 March, 2006. During the event, the hourly aerosol concentrations reached close to 400 µg m(-3) in northern Taiwan, and approximately 300 µg m(-3) in other areas of the island. Trajectory and regional dust models show that the dust event originated in eastern Mongolia and northern China, and the dust layer can descend from 2 to 3 km in the source area to below 1.5 km over Taiwan. On the other hand, model results show that pollution was transported near the surface from coastal China to Taiwan. During this dust event, polluted aerosol was first observed over northern Taiwan right after a frontal passage, and the concentration was strongly enhanced following the passage of the light rainfall 12h later. The descent of dusty air from the free troposphere lagged the arrival of polluted air by 7h, and was partially mixed with polluted aerosol when the transport decelerated over Taiwan. During the event, dust particles accounted for up to 60% of observed particulate matter less than 10 µm (PM10) over Taiwan, but decreased to less than 35% for particulate matter less than 2.5 µm (PM2.5) over most areas of the island. On the other hand, the long-range transport of non-dust aerosols, mainly anthropogenic pollutants, accounted for close to 30% of observed PM10 concentration in northern and western Taiwan prior to dust arrival, and the contribution of PM2.5 increased to close to 40% over the same areas. Local emission of aerosols accounted for less than 25% of PM10 concentrations in northern Taiwan, but was about 60% for PM2.5 in central and southern Taiwan because these areas are less influenced by long-range transport.

Source identifications of PM10 aerosols depending on hourly measurements of soluble components characterization among different events in Taipei Basin during spring season of 2004.

Continuous measurements of hourly PM10 soluble ions were performed by the in situ IC technology in order to assess the impact of Asian outflows on local air quality. The intensive aerosol observation was carried in Taipei from 11 February 22:00 to 7 April 19:00, 2004. Concentrations of the water-soluble ions (Cl(-), NO(-)(2), NO(-)(3), SO(2-)(4), Na(+), NH(+)(4), K(+), and Ca(2+)) were measured in a total of 3,300 samples. The characteristics of air pollutant events in Taipei Basin were classified as frontal dust, dust, northeast monsoon, south wind and sea/land breeze according to the hourly meteorology and air pollutant concentrations. Factor analysis was conducted based on hourly data for 13 variables to find the group of variables with similar behavior. According to the source characteristics of high loading species, the possible sources of PM10 aerosols in each group were identified. Three to four factors were identified for each event. The total variances of frontal dust, dust, northeast trade, south wind, and sea/land breeze events were explained about 85%, 86%, 76%, 77%, and 80%, respectively, indicating that the identified factors were satisfactory.

Lidar ratio and depolarization ratio for cirrus clouds.

We report on studies of the lidar and the depolarization ratios for cirrus clouds. The optical depth and effective lidar ratio are derived from the transmission of clouds, which is determined by comparing the backscattering signals at the cloud base and cloud top. The lidar signals were fitted to a background atmospheric density profile outside the cloud region to warrant the linear response of the return signals with the scattering media. An average lidar ratio, 29 +/- 12 sr, has been found for all clouds measured in 1999 and 2000. The height and temperature dependences ofthe lidar ratio, the optical depth, and the depolarization ratio were investigated and compared with results of LITE and PROBE. Cirrus clouds detected near the tropopause are usually optically thin and mostly subvisual. Clouds with the largest optical depths were found near 12 km with a temperature of approximately -55 degrees C. The multiple-scattering effect is considered for clouds with high optical depths, and this effect lowers the lidar ratios compared with a single-scattering condition. Lidar ratios are in the 20-40 range for clouds at heights of 12.5-15 km and are smaller than approximately 30 in height above 15 km. Clouds are usually optically thin for temperatures below approximately -65 degrees C, and in this region the optical depth tends to decrease with height. The depolarization ratio is found to increase with a height at 11-15 km and smaller than 0.3 above 16 km. The variation in the depolarization ratio with the lidar ratio was also reported. The lidar and depolarization ratios were discussed in terms of the types of hexagonal ice crystals.