Atmospheric Chemistry and Physics

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ISSN / EISSN : 1680-7316 / 1680-7324
Current Publisher: Copernicus GmbH (10.5194)
Total articles ≅ 21,566
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Rui Li, Yilong Zhao, , , , Chunying Wang
Atmospheric Chemistry and Physics, Volume 21, pp 8677-8692; doi:10.5194/acp-21-8677-2021

Abstract:
The rapid response to the COVID-19 pandemic led to unprecedented decreases in economic activities, thereby reducing the pollutant emissions. A random forest (RF) model was applied to determine the respective contributions of meteorology and anthropogenic emissions to the changes in air quality. The result suggested that the strict lockdown measures significantly decreased primary components such as Cr (−67 %) and Fe (−61 %) in PM2.5 (p<0.01), whereas the higher relative humidity (RH) and NH3 level and the lower air temperature (T) remarkably enhanced the production of secondary aerosol, including SO42- (29 %), NO3- (29 %), and NH4+ (21 %) (p<0.05). The positive matrix factorization (PMF) result suggested that the contribution ratios of secondary formation (SF), industrial process (IP), biomass burning (BB), coal combustion (CC), and road dust (RD) changed from 36 %, 27 %, 21 %, 12 %, and 4 % before the COVID-19 outbreak to 44 %, 20 %, 20 %, 9 %, and 7 %, respectively. The rapid increase in the contribution ratio derived from SF to PM2.5 implied that the intermittent haze events during the COVID-19 period were characterized by secondary aerosol pollution, which was mainly contributed by the unfavorable meteorological conditions and high NH3 level.
Zhe Jiang, , , , Yifang Zhu, , Xin Lu, , , , et al.
Atmospheric Chemistry and Physics, Volume 21, pp 8693-8708; doi:10.5194/acp-21-8693-2021

Abstract:
In response to the coronavirus disease of 2019 (COVID-19), California issued statewide stay-at-home orders, bringing about abrupt and dramatic reductions in air pollutant emissions. This crisis offers us an unprecedented opportunity to evaluate the effectiveness of emission reductions in terms of air quality. Here we use the Weather Research and Forecasting model with Chemistry (WRF-Chem) in combination with surface observations to study the impact of the COVID-19 lockdown measures on air quality in southern California. Based on activity level statistics and satellite observations, we estimate the sectoral emission changes during the lockdown. Due to the reduced emissions, the population-weighted concentrations of fine particulate matter (PM2.5) decrease by 15 % in southern California. The emission reductions contribute 68 % of the PM2.5 concentration decrease before and after the lockdown, while meteorology variations contribute the remaining 32 %. Among all chemical compositions, the PM2.5 concentration decrease due to emission reductions is dominated by nitrate and primary components. For O3 concentrations, the emission reductions cause a decrease in rural areas but an increase in urban areas; the increase can be offset by a 70 % emission reduction in anthropogenic volatile organic compounds (VOCs). These findings suggest that a strengthened control on primary PM2.5 emissions and a well-balanced control on nitrogen oxides and VOC emissions are needed to effectively and sustainably alleviate PM2.5 and O3 pollution in southern California.
, , Keiichi Sato, , Junichi Kurokawa, Jiani Tan, Kan Huang, , Xuemei Wang, , et al.
Atmospheric Chemistry and Physics, Volume 21, pp 8709-8734; doi:10.5194/acp-21-8709-2021

Abstract:
Asia has attracted research attention because it has the highest anthropogenic emissions in the world, and the Model Inter-Comparison Study for Asia (MICS-Asia) phase III was carried out to foster our understanding of the status of air quality over Asia. This study analyzed wet deposition in southeast Asian countries (Myanmar, Thailand, Lao People's Democratic Republic (PDR), Cambodia, Vietnam, the Philippines, Malaysia, and Indonesia) with the aim of providing insights into the seasonal variation of wet deposition. Southeast Asia was not fully considered in MICS-Asia phase II due to a lack of observational data; however, the analysis period of MICS-Asia III, namely the year 2010, is covered by ground observations of the Acid Deposition Monitoring Network in East Asia (EANET), and the coordinated simulation domain was extended to cover these observation sites. The analyzed species are wet depositions of S (sulfate aerosol, sulfur dioxide (SO2), and sulfuric acid (H2SO4)), N (nitrate aerosol, nitrogen monoxide (NO), nitrogen dioxide (NO2), and nitric acid (HNO3)), and A (ammonium aerosol and ammonia (NH3)). The wet deposition simulated with seven models driven by a unified meteorological model in MICS-Asia III was used with the ensemble approach, which effectively modulates the differences in performance among models. By comparison with EANET observations, although the seven models generally captured the wet depositions of S, N, and A, there were difficulties capturing these in some cases. Considering the model performance for ambient aerosol concentrations over southeast Asia, this failure of models is considered to be related to the difficulty in capturing the precipitation in southeast Asia, especially during the dry and wet seasons. Generally, meteorological fields overestimate the precipitation during the dry season, which leads to the overestimation of wet deposition during this season. To overcome this, a precipitation-adjusted approach that scaled the modeled precipitation to the observed value was applied, and it was demonstrated that the model performance was improved. Satellite measurements were also used to adjust for precipitation data, which adequately accounted for the spatiotemporal precipitation patterns, especially in the dry season. As the statistical scores were mostly improved by this adjustment, the estimation of wet deposition with precipitation adjustment was considered to be superior. To utilize satellite measurements, the spatial distribution of wet deposition was revised. Based on this revision, it was found that Vietnam, Malaysia, and Indonesia were upward corrected, and Myanmar, Thailand, Lao PDR, Cambodia, and the Philippines were downward-corrected; these corrections were up to ±40 %. The improved accuracy of precipitation amount was key to estimating wet deposition in this study. These results suggest that the precipitation-adjusted approach has the potential to obtain accurate estimates of wet deposition through the fusion of models and observations.
Joshua Baptiste, Connor Williamson, John Fox, Anthony J. Stace, Muhammad Hassan, Stefanie Braun, Benjamin Stamm, ,
Atmospheric Chemistry and Physics, Volume 21, pp 8735-8745; doi:10.5194/acp-21-8735-2021

Abstract:
Agglomeration of charged ice and dust particles in the mesosphere and lower thermosphere is studied using a classical electrostatic approach, which is extended to capture the induced polarisation of surface charge. Collision outcomes are predicted whilst varying the particle size, charge, dielectric constant, relative kinetic energy, collision geometry and the coefficient of restitution. In addition to Coulomb forces acting on particles of opposite charge, instances of attraction between particles of the same sign of charge are discussed. These attractive forces are governed by the polarisation of surface charge and can be strong at very small separation distances. In the mesosphere and lower thermosphere, these interactions could also contribute to the formation of stable aggregates and contamination of ice particles through collisions with meteoric smoke particles.
, Ping Wang, Piet Stammes
Atmospheric Chemistry and Physics, Volume 21, pp 8593-8614; doi:10.5194/acp-21-8593-2021

Abstract:
During a solar eclipse the solar irradiance reaching the top of the atmosphere (TOA) is reduced in the Moon shadow. The solar irradiance is commonly measured by Earth observation satellites before the start of the solar eclipse and is not corrected for this reduction, which results in a decrease in the computed TOA reflectances. Consequently, air quality products that are derived from TOA reflectance spectra, such as the ultraviolet (UV) absorbing aerosol index (AAI), are distorted or undefined in the shadow of the Moon. The availability of air quality satellite data in the penumbral and antumbral shadow during solar eclipses, however, is of particular interest to users studying the atmospheric response to solar eclipses. Given the time and location of a point on the Earth's surface, we explain how to compute the obscuration during a solar eclipse, taking into account wavelength-dependent solar limb darkening. With the calculated obscuration fractions, we restore the TOA reflectances and the AAI in the penumbral shadow during the annular solar eclipses on 26 December 2019 and 21 June 2020 measured by the TROPOMI/S5P instrument. We compare the calculated obscuration to the estimated obscuration using an uneclipsed orbit. In the corrected products, the signature of the Moon shadow disappeared, but only if wavelength-dependent solar limb darkening is taken into account. We find that the Moon shadow anomaly in the uncorrected AAI is caused by a reduction of the measured reflectance at 380 nm, rather than a colour change of the measured light. We restore common AAI features such as the sunglint and desert dust, and we confirm the restored AAI feature on 21 June 2020 at the Taklamakan Desert by measurements of the GOME-2C satellite instrument on the same day but outside the Moon shadow. No indication of local absorbing aerosol changes caused by the eclipses was found. We conclude that the correction method of this paper can be used to detect real AAI rising phenomena during a solar eclipse and has the potential to restore any other product that is derived from TOA reflectance spectra. This would resolve the solar eclipse anomalies in satellite air quality measurements in the penumbra and antumbra and would allow for studying the effect of the eclipse obscuration on the composition of the Earth's atmosphere from space.
Atmospheric Chemistry and Physics, Volume 21, pp 8615-8635; doi:10.5194/acp-21-8615-2021

Abstract:
A known adverse side effect of stratospheric aerosol modification (SAM) is the alteration of the quasi-biennial oscillation (QBO), which is caused by the stratospheric heating associated with an artificial aerosol layer. Multiple studies found the QBO to slow down or even completely vanish for point-like injections of SO2 at the Equator. The cause for this was found to be a modification of the thermal wind balance and a stronger tropical upwelling. For other injection strategies, different responses of the QBO have been observed. A theory which is able to explain those differences in a comprehensive manner has not yet been presented. This is further complicated by the fact that the simulated QBO response is highly sensitive to the used model even under identical boundary conditions. Therefore, within this study we investigate the response of the QBO to SAM for three different injection strategies (point-like injection at the Equator, point-like injection at 30∘ N and 30∘ S simultaneously, and areal injection into a 60∘ wide belt along the Equator). Our simulations confirm that the QBO response significantly depends on the injection location. Based on the thermal wind balance, we demonstrate that this dependency is explained by differences in the meridional structure of the aerosol-induced stratospheric warming, i.e., the location and meridional extension of the maximum warming. Additionally, we also tested two different injection species (SO2 and H2SO4). The QBO response is qualitatively similar for both investigated injection species. Comparing the results to corresponding results of a second model, we further demonstrate the generality of our theory as well as the importance of an interactive treatment of stratospheric ozone for the simulated QBO response.
, Kirsten N. Fossum, Jurgita Ovadnevaite, Chunshui Lin, , , Darius Ceburnis
Atmospheric Chemistry and Physics, Volume 21, pp 8655-8675; doi:10.5194/acp-21-8655-2021

Abstract:
We present an aerosol cloud condensation nuclei (CCN) closure study over the north-east Atlantic Ocean using six approximating methods. The CCN number concentrations (NCCN) were measured at four discrete supersaturations (SSs; 0.25 %, 0.5 %, 0.75 % and 1.0 %). Concurrently, aerosol number size distribution, sub-saturation hygroscopic growth factor and bulk PM1 chemical composition were obtained at matching time resolution and after a careful data validation exercise. Method A used a constant bulk hygroscopicity parameter κ of 0.3; method B used bulk PM1 chemical composition measured by an aerosol mass spectrometer (AMS); method C utilised a single growth factor (GF) size (165 nm) measured by a humidified tandem differential mobility analyser (HTDMA); method D utilised size-dependent GFs measured at 35, 50, 75, 110 and 165 nm; method E divided the aerosol population into three hygroscopicity modes (near-hydrophobic, more-hygroscopic and sea-salt modes), and the total CCN number in each mode was cumulatively added up; method F used the full-size-scale GF probability density function (GF–PDF) in the most complex approach. The studied periods included high-biological-activity and low-biological-activity seasons in clean marine and polluted continental air masses to represent and discuss the most contrasting aerosol populations. Overall, a good agreement was found between estimated and measured NCCN with linear regression slopes ranging from 0.64 to 1.6. The temporal variability was captured very well, with Pearson's R value ranging from 0.76 to 0.98 depending on the method and air mass type. We further compared the results of using different methods to quantify the impact of size-dependent hygroscopicity and mixing state and found that ignoring size-dependent hygroscopicity induced overestimation of NCCN by up to 12 %, and ignoring a mixing state induced overestimation of NCCN by up to 15 %. The error induced by assuming an internal mixing in highly polluted cases was largely eliminated by dividing the full GF–PDF into three conventional hygroscopic modes, while assuming an internal mixing in clean marine aerosol did not induce significant error.
Na Zhao, , , , , , Daven Henze, Tom Kucsera, , Mian Chin, et al.
Atmospheric Chemistry and Physics, Volume 21, pp 8637-8654; doi:10.5194/acp-21-8637-2021

Abstract:
Black carbon (BC) emissions play an important role in regional climate change in the Arctic. It is necessary to pay attention to the impact of long-range transport from regions outside the Arctic as BC emissions from local sources in the Arctic were relatively small. The task force Hemispheric Transport of Air Pollution Phase 2 (HTAP2) set up a series of simulation scenarios to investigate the response of BC in a given region to different source regions. This study investigated the responses of Arctic BC concentrations and surface temperature to 20 % anthropogenic emission reductions from six regions in 2010 within the framework of HTAP2 based on ensemble modeling results. Emission reductions from East Asia (EAS) had the most (monthly contributions: 0.2–1.5 ng m−3) significant impact on the Arctic near-surface BC concentrations, while the monthly contributions from Europe (EUR), Middle East (MDE), North America (NAM), Russia–Belarus–Ukraine (RBU), and South Asia (SAS) were 0.2–1.0, 0.001–0.01, 0.1–0.3, 0.1–0.7, and 0.0–0.2 ng m−3, respectively. The responses of the vertical profiles of the Arctic BC to the six regions were found to be different due to multiple transport pathways. Emission reductions from NAM, RBU, EUR, and EAS mainly influenced the BC concentrations in the low troposphere of the Arctic, while most of the BC in the upper troposphere of the Arctic derived from SAS. The response of the Arctic BC to emission reductions in six source regions became less significant with the increase in the latitude. The benefit of BC emission reductions in terms of slowing down surface warming in the Arctic was evaluated by using absolute regional temperature change potential (ARTP). Compared to the response of global temperature to BC emission reductions, the response of Arctic temperature was substantially more sensitive, highlighting the need for curbing global BC emissions.
Atmospheric Chemistry and Physics, Volume 21, pp 8511-8530; doi:10.5194/acp-21-8511-2021

Abstract:
Despite Australian dust's critical role in the regional climate and surrounding marine ecosystems, the controlling factors of the spatiotemporal variations of Australian dust are not fully understood. Here we assess the connections between observed spatiotemporal variations of Australian dust with key modes of large-scale climate variability, namely the El Niño–Southern Oscillation (ENSO) and Madden–Julian Oscillation (MJO). Multiple dust observations from the Aerosol Robotic Network (AERONET), weather stations, and satellite instruments, namely the Moderate Resolution Imaging Spectroradiometer (MODIS) and Multi-angle Imaging SpectroRadiometer (MISR), are examined. The assessed multiple dust observations consistently identify the natural and agricultural dust hotspots in Australia, including the Lake Eyre basin, Lake Torrens basin, Lake Frome basin, Simpson Desert, Barwon–Darling basin, Riverina, Barkly Tableland, and the lee side of the Great Dividing Range, as well as a country-wide, austral spring-to-summer peak in dust activity. Our regression analysis of observed dust optical depth (DOD) upon an ocean Niño index confirms previous model-based findings on the enhanced dust activity in southern and eastern Australia during the subsequent austral spring and summer dust season following the strengthening of austral wintertime El Niño. Our analysis further indicates the modulation of the ENSO–dust relationship with the MJO phases. During sequential MJO phases, the dust-active center moves from west to east, associated with the eastward propagation of MJO, with the maximum enhancement in dust activity at about 120, 130, and 140∘ E, corresponding to MJO phases 1–2, 3–4, and 5–6, respectively. MJO phases 3–6 are favorable for enhanced ENSO modulation of dust activity, especially the occurrence of extreme dust events, in southeastern Australia, currently hypothesized to be attributed to the interaction between MJO-induced anomalies in convection and wind and ENSO-induced anomalies in soil moisture and vegetation.
, Arlyn Andrews, , , , , , Steven Wofsy, John M. Henderson, James T. Randerson
Atmospheric Chemistry and Physics, Volume 21, pp 8557-8574; doi:10.5194/acp-21-8557-2021

Abstract:
Recent increases in boreal forest burned area, which have been linked with climate warming, highlight the need to better understand the composition of wildfire emissions and their atmospheric impacts. Here we quantified emission factors for CO and CH4 from a massive regional fire complex in interior Alaska during the summer of 2015 using continuous high-resolution trace gas observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CRV) tower in Fox, Alaska. Averaged over the 2015 fire season, the mean CO / CO2 emission ratio was 0.142 ± 0.051, and the mean CO emission factor was 127 ± 40 g kg−1 dry biomass burned. The CO / CO2 emission ratio was about 39 % higher than the mean of previous estimates derived from aircraft sampling of wildfires from boreal North America. The mean CH4 / CO2 emission ratio was 0.010 ± 0.004, and the CH4 emission factor was 5.3 ± 1.8 g kg−1 dry biomass burned, which are consistent with the mean of previous reports. CO and CH4 emission ratios varied in synchrony, with higher CH4 emission factors observed during periods with lower modified combustion efficiency (MCE). By coupling a fire emissions inventory with an atmospheric model, we identified at least 34 individual fires that contributed to trace gas variations measured at the CRV tower, representing a sample size that is nearly the same as the total number of boreal fires measured in all previous field campaigns. The model also indicated that typical mean transit times between trace gas emission within a fire perimeter and tower measurement were 1–3 d, indicating that the time series sampled combustion across day and night burning phases. The high CO emission ratio estimates reported here provide evidence for a prominent role of smoldering combustion and illustrate the importance of continuously sampling fires across time-varying environmental conditions that are representative of a fire season.
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