Vertical profiles of NO<sub>2</sub>, SO<sub>2</sub>, HONO, HCHO, CHOCHO and aerosols derived from MAX-DOAS measurements at a rural site in the central western North China Plain and their relation to emission sources and effects of regional transport
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Published:2019-04-24
Issue:8
Volume:19
Page:5417-5449
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Wang YangORCID, Dörner SteffenORCID, Donner SebastianORCID, Böhnke Sebastian, De Smedt IsabelleORCID, Dickerson Russell R.ORCID, Dong Zipeng, He HaoORCID, Li ZhanqingORCID, Li Zhengqiang, Li Donghui, Liu DongORCID, Ren XinrongORCID, Theys Nicolas, Wang YuyingORCID, Wang YangORCID, Wang ZhenzhuORCID, Xu Hua, Xu JiweiORCID, Wagner Thomas
Abstract
Abstract. A multi-axis differential optical absorption spectroscopy (MAX-DOAS)
instrument was deployed in May and June 2016 at a monitoring station
(37.18∘ N, 114.36∘ E) in the suburban area of Xingtai,
which is one of the most polluted cities in the North China Plain (NCP),
during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) experiment and Air chemistry Research In Asia
(ARIAs) joint experiments to derive tropospheric vertical profiles of
NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical
depths derived from MAX-DOAS were found to be consistent with collocated
sun-photometer measurements. Also the derived near-surface aerosol extinction
and HCHO mixing ratio agree well with the coincident visibility meter and in
situ HCHO measurements, with mean HCHO near-surface mixing ratios of ∼3.5 ppb. Underestimations of MAX-DOAS results compared to in situ
measurements of NO2 (∼60 %) and SO2 (∼20 %) are found expectedly due to vertical and horizontal inhomogeneity
of trace gases. Vertical profiles of aerosols and NO2 and SO2
are reasonably consistent with those measured by a collocated Raman lidar and
aircraft spirals over the station. The deviations can be attributed to
differences in sensitivity as a function of altitude and substantial
horizontal gradients of pollutants. Aerosols, HCHO and CHOCHO profiles
typically extended to higher altitudes (with 75 % integrated column
located below ∼1.4 km) than NO2, SO2 and HONO did
(with 75 % integrated column below ∼0.5 km) under polluted
conditions. Lifted layers were systematically observed for all species
(except HONO), indicating accumulation, secondary formation or long-range
transport of the pollutants at higher altitudes. Maximum values routinely
occurred in the morning for NO2, SO2 and HONO but occurred at
around noon for aerosols, HCHO and CHOCHO, mainly dominated by
photochemistry, characteristic upslope–downslope circulation and planetary
boundary layer (PBL) dynamics. Significant day-to-day variations are found
for all species due to the effect of regional transport and changes in
synoptic pattern analysed with the backward propagation approach based on
HYSPLIT trajectories. Low pollution was often observed for air masses from
the north-west (behind cold fronts), and high pollution was observed from the
southern areas such as industrialized Wu'an. The contribution of regional
transport for the pollutants measured at the site during the observation
period was estimated to be about 20 % to 30 % for trace gases and
about 50 % for aerosols. In addition, agricultural burning events
impacted the day-to-day variations in HCHO, CHOCHO and aerosols. It needs to
be noted that although several MAX-DOAS measurements of trace gases and
aerosols in the NCP area have been reported in previous studies, this study
is the first work to derive a comprehensive set of vertical profiles of
NO2, SO2, HONO, HCHO, CHOCHO and aerosols from measurements
of one MAX-DOAS instrument. Also, so far, the validation of MAX-DOAS profile
results by comparison with various surface in situ measurements as well as
profile measurements from lidar and aircraft is scarce. Moreover, the
backward propagation approach for characterizing the contributions of
regional transport of pollutants from different regions was applied to the
MAX-DOAS results of trace gases and aerosols for the first time.
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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