scholarly journals Evaluating Secondary Inorganic Aerosols in 3-Dimensions

2016 ◽  
Author(s):  
Keren Mezuman ◽  
Susanne E. Bauer ◽  
Kostas Tsigaridis
Keyword(s):  
Nitric Acid ◽  
Climate Model ◽  
Model Performance ◽  
Heterogeneous Reactions ◽  
Surface Measurement ◽  
3 Dimensional ◽  
The Matrix ◽  
The Usa ◽  
Dimensional Distribution ◽  
Surface Measurements

Abstract. The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the 3-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e. sulfate, ammonium and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000–2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model, influenced by strong stratosphere-troposphere exchange. Heterogeneous reactions on dust surfaces is an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3/NH4+ partitioning which affects the HNO3/NO3− partitioning.

scholarly journals Evaluating secondary inorganic aerosols in three dimensions

2016 ◽  
Vol 16 (16) ◽  
pp. 10651-10669 ◽  
Author(s):  
Keren Mezuman ◽  
Susanne E. Bauer ◽  
Kostas Tsigaridis
Keyword(s):  
Nitric Acid ◽  
Climate Model ◽  
Three Dimensional ◽  
Model Performance ◽  
Heterogeneous Reactions ◽  
Three Dimensions ◽  
Surface Measurement ◽  
The Matrix ◽  
The Usa ◽  
Dimensional Distribution

Abstract. The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the three-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e., sulfate, ammonium, and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000 to 2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model. Heterogeneous reactions on dust surfaces are an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3 ∕ NH4+ partitioning which affects the HNO3 ∕ NO3− partitioning.

scholarly journals Effects of heterogeneous reactions on tropospheric chemistry: a global simulation with the chemistry–climate model CHASER V4.0

2021 ◽  
Vol 14 (6) ◽  
pp. 3813-3841
Author(s):  
Phuc T. M. Ha ◽  
Ryoki Matsuda ◽  
Yugo Kanaya ◽  
Fumikazu Taketani ◽  
Kengo Sudo
Keyword(s):  
Climate Model ◽  
Model Simulation ◽  
Model Performance ◽  
Lower Troposphere ◽  
Heterogeneous Reactions ◽  
Tropospheric Chemistry ◽  
Small Contribution ◽  
Modeling Framework ◽  
Positive Tendency ◽  
Global Mean

Abstract. This study uses a chemistry–climate model CHASER (MIROC) to explore the roles of heterogeneous reactions (HRs) in global tropospheric chemistry. Three distinct HRs of N2O5, HO2, and RO2 are considered for surfaces of aerosols and cloud particles. The model simulation is verified with EANET and EMEP stationary observations; R/V Mirai ship-based data; ATom1 aircraft measurements; satellite observations by OMI, ISCCP, and CALIPSO-GOCCP; and reanalysis data JRA55. The heterogeneous chemistry facilitates improvement of model performance with respect to observations for NO2, OH, CO, and O3, especially in the lower troposphere. The calculated effects of heterogeneous reactions cause marked changes in global abundances of O3 (−2.96 %), NOx (−2.19 %), CO (+3.28 %), and global mean CH4 lifetime (+5.91 %). These global effects were contributed mostly by N2O5 uptake onto aerosols in the middle troposphere. At the surface, HO2 uptake gives the largest contributions, with a particularly significant effect in the North Pacific region (−24 % O3, +68 % NOx, +8 % CO, and −70 % OH), mainly attributable to its uptake onto clouds. The RO2 reaction has a small contribution, but its global mean negative effects on O3 and CO are not negligible. In general, the uptakes onto ice crystals and cloud droplets that occur mainly by HO2 and RO2 radicals cause smaller global effects than the aerosol-uptake effects by N2O5 radicals (+1.34 % CH4 lifetime, +1.71 % NOx, −0.56 % O3, +0.63 % CO abundances). Nonlinear responses of tropospheric O3, NOx, and OH to the N2O5 and HO2 uptakes are found in the same modeling framework of this study (R>0.93). Although all HRs showed negative tendencies for OH and O3 levels, the effects of HR(HO2) on the tropospheric abundance of O3 showed a small increment with an increasing loss rate. However, this positive tendency turns to reduction at higher rates (>5 times). Our results demonstrate that the HRs affect not only polluted areas but also remote areas such as the mid-latitude sea boundary layer and upper troposphere. Furthermore, HR(HO2) can bring challenges to pollution reduction efforts because it causes opposite effects between NOx (increase) and surface O3 (decrease).

scholarly journals Effects of heterogeneous reactions on global tropospheric chemistry

2020 ◽  
Author(s):  
Phuc T. M. Ha ◽  
Fumikazu Taketani ◽  
Yugo Kanaya ◽  
Ryoki Matsuda ◽  
Kengo Sudo
Keyword(s):  
Climate Model ◽  
Model Simulation ◽  
Model Performance ◽  
Lower Troposphere ◽  
Reanalysis Data ◽  
Heterogeneous Reactions ◽  
Tropospheric Chemistry ◽  
Small Contribution ◽  
Positive Tendency ◽  
Global Mean

Abstract. This study uses a chemistry-climate model CHASER (MIROC) to explore the roles of heterogeneous reactions (HRs) in global tropospheric chemistry. Three distinct HRs of N2O5, HO2, and RO2 are considered for surfaces of aerosols and cloud particles. The model simulation is verified with EANET and EMEP stationary observations, R/V MIRAI ship-based data, ATOM1 aircraft measurements, satellite observations by OMI, ISCCP, and CALIPSO-GOCCP, and reanalysis data JRA55. The heterogeneous chemistry facilitates improvement of model performance with respect to observations for NO2, OH, CO, and O3, especially in the lower troposphere. The calculated effects of heterogeneous reactions cause marked changes in global abundances of O3 (−3 %), NOx (−2.2 %), CO (+3.3 %), and global mean CH4 lifetime (+5.9 %). These global effects were contributed mostly by N2O5 uptake onto aerosols in the middle troposphere. At the surface, HO2 uptake gives the largest contributions, with a particularly significant effect in the North Pacific region (−24% O3, +68 % NOx, +8 % CO, and −70 % OH), mainly attributable to its uptake onto clouds. The RO2 reaction has a small contribution, but its global-mean negative effect on O3 is not negligible. In general, the uptakes onto ice crystals and cloud droplets that occur mainly by HO2 and RO2 radicals cause smaller global effects than the aerosol-uptake effects by N2O5 radicals (+1.34 % CH4 lifetime, +1.71 % NOx, −0.56 % O3, +0.63 % CO abundances). Nonlinear responses of tropospheric O3, NOx, and OH to the N2O5 and HO2 uptakes are found in the same modelling framework of this study (R > 0.93). Although all HRs showed negative tendencies for OH and O3 levels, the effects of HR(HO2) on the tropospheric abundance of O3 showed a small increment with an increasing loss rate. However, this positive tendency turns to reduction at higher rates (> 5 times). Our results demonstrate that the HRs affect not only polluted areas but also remote areas such as the mid-latitude sea boundary layer and upper troposphere. Furthermore, HR(HO2) can bring challenges to pollution reduction efforts because it causes opposite effects between NOx (increase) and surface O3 (decrease).

3-Dimensional immunolabeling and in situ hybridization detection using fluorescence photooxidation and intermediate-voltage Electron Microscopy

1994 ◽  
Vol 52 ◽  
pp. 164-165
Author(s):  
Thomas J. Deerinck ◽  
Maryann E. Martone ◽  
Varda Lev-Ram ◽  
David P. L. Green ◽  
Roger Y. Tsien ◽  
...  
Keyword(s):  
Laser Scanning ◽  
Reactive Oxygen ◽  
Confocal Laser Scanning Microscope ◽  
Fluorescent Dye ◽  
Confocal Laser ◽  
3 Dimensional ◽  
Voltage Electron ◽  
Dimensional Distribution ◽  
Electron Microscopes ◽  
New Generation

The confocal laser scanning microscope has become a powerful tool in the study of the 3-dimensional distribution of proteins and specific nucleic acid sequences in cells and tissues. This is also proving to be true for a new generation of high contrast intermediate voltage electron microscopes (IVEM). Until recently, the number of labeling techniques that could be employed to allow examination of the same sample with both confocal and IVEM was rather limited. One method that can be used to take full advantage of these two technologies is fluorescence photooxidation. Specimens are labeled by a fluorescent dye and viewed with confocal microscopy followed by fluorescence photooxidation of diaminobenzidine (DAB). In this technique, a fluorescent dye is used to photooxidize DAB into an osmiophilic reaction product that can be subsequently visualized with the electron microscope. The precise reaction mechanism by which the photooxidation occurs is not known but evidence suggests that the radiationless transfer of energy from the excited-state dye molecule undergoing the phenomenon of intersystem crossing leads to the formation of reactive oxygen species such as singlet oxygen. It is this reactive oxygen that is likely crucial in the photooxidation of DAB.

scholarly journals Improved tropospheric and stratospheric sulfur cycle in the aerosol–chemistry–climate model SOCOL-AERv2

2019 ◽  
Vol 12 (9) ◽  
pp. 3863-3887 ◽  
Author(s):  
Aryeh Feinberg ◽  
Timofei Sukhodolov ◽  
Bei-Ping Luo ◽  
Eugene Rozanov ◽  
Lenny H. E. Winkel ◽  
...  
Keyword(s):  
Climate Model ◽  
Model Performance ◽  
Stratospheric Aerosol ◽  
Sulfur Cycle ◽  
Sulfate Aerosol ◽  
Tropospheric Chemistry ◽  
Sulfur Deposition ◽  
Aerosol Chemistry ◽  
Deposition Fluxes ◽  
Aerosol Model

Abstract. SOCOL-AERv1 was developed as an aerosol–chemistry–climate model to study the stratospheric sulfur cycle and its influence on climate and the ozone layer. It includes a sectional aerosol model that tracks the sulfate particle size distribution in 40 size bins, between 0.39 nm and 3.2 µm. Sheng et al. (2015) showed that SOCOL-AERv1 successfully matched observable quantities related to stratospheric aerosol. In the meantime, SOCOL-AER has undergone significant improvements and more observational datasets have become available. In producing SOCOL-AERv2 we have implemented several updates to the model: adding interactive deposition schemes, improving the sulfate mass and particle number conservation, and expanding the tropospheric chemistry scheme. We compare the two versions of the model with background stratospheric sulfate aerosol observations, stratospheric aerosol evolution after Pinatubo, and ground-based sulfur deposition networks. SOCOL-AERv2 shows similar levels of agreement as SOCOL-AERv1 with satellite-measured extinctions and in situ optical particle counter (OPC) balloon flights. The volcanically quiescent total stratospheric aerosol burden simulated in SOCOL-AERv2 has increased from 109 Gg of sulfur (S) to 160 Gg S, matching the newly available satellite estimate of 165 Gg S. However, SOCOL-AERv2 simulates too high cross-tropopause transport of tropospheric SO2 and/or sulfate aerosol, leading to an overestimation of lower stratospheric aerosol. Due to the current lack of upper tropospheric SO2 measurements and the neglect of organic aerosol in the model, the lower stratospheric bias of SOCOL-AERv2 was not further improved. Model performance under volcanically perturbed conditions has also undergone some changes, resulting in a slightly shorter volcanic aerosol lifetime after the Pinatubo eruption. With the improved deposition schemes of SOCOL-AERv2, simulated sulfur wet deposition fluxes are within a factor of 2 of measured deposition fluxes at 78 % of the measurement stations globally, an agreement which is on par with previous model intercomparison studies. Because of these improvements, SOCOL-AERv2 will be better suited to studying changes in atmospheric sulfur deposition due to variations in climate and emissions.

Observed and Projected Frontal Activities in East Asia

2021 ◽  
pp. 1-46
Author(s):  
Chia-Chi Wang ◽  
Huang-Hsiung Hsu ◽  
Ying-Ting Chen
Keyword(s):  
East Asia ◽  
Climate Model ◽  
Southern China ◽  
Model Performance ◽  
Moisture Flux ◽  
Central China ◽  
Cmip5 Models ◽  
The South ◽  
Front Detection ◽  
Local Moisture

AbstractAn objective front detection method is applied to ERA5, CMIP5 historical, and RCP8.5 simulations to evaluate climate model performance in simulating front frequency and understand future projections of seasonal front activities. The study area is East Asia for two natural seasons, defined as winter (December 2nd –February 14th) and spring (February 15th –May 15th), in accordance with regional circulation and precipitation patterns. Seasonal means of atmospheric circulation and thermal structures are analyzed to understand possible factors responsible for future front changes.The front location and frequency in CMIP5 historical simulations are captured reasonably. Frontal precipitation accounts for more than 30% of total precipitation over subtropical regions. Projections suggest that winter fronts will decrease over East Asia, especially over southern China. Frontal precipitation is projected to decrease for 10-30%. Front frequency increases in the South China Sea and tropical western Pacific because of more tropical moisture supply, which enhances local moisture contrasts. During spring, southern China and Taiwan will experience fewer fronts and less frontal precipitation while central China, Korea, and Japan may experience more fronts and more frontal precipitation due to moisture flux from the south that enhances 𝜽𝒘 gradients.Consensus among CMIP5 models in front frequency tendency is evaluated. The models exhibit relatively high consensus in the decreasing trend over polar and subtropical frontal zone in winter and over southern China and Taiwan in spring that may prolong the dry season. Spring front activities are crucial for water resource and risk management in the southern China and Taiwan.

scholarly journals Nitrate formation from heterogeneous uptake of dinitrogen pentoxide during a severe winter haze in southern China

2018 ◽  
Author(s):  
Hui Yun ◽  
Weihao Wang ◽  
Tao Wang ◽  
Men Xia ◽  
Chuan Yu ◽  
...  
Keyword(s):  
Nitric Acid ◽  
Time Resolution ◽  
Southern China ◽  
Fine Particulate Matter ◽  
Measurement Data ◽  
Heterogeneous Reactions ◽  
Chemical Mechanism ◽  
Rural Site ◽  
Phase Reaction ◽  
Dinitrogen Pentoxide

Abstract. Nitrate (NO3−) has become a major component of fine particulate matter (PM2.5) during hazy days in China. However, the role of the heterogeneous reactions of dinitrogen pentoxide (N2O5) in nitrate formation is not well constrained. In January 2017, a severe haze event occurred in the Pearl River Delta (PRD) of southern China during which high levels of PM2.5 (~ 400 μg m−3) and O3 (~ 160 ppbv) were observed at a semi-rural site (Heshan) in the western PRD. Nitrate concentrations were up to 108 μg m−3 (1 h time resolution), and the contribution of nitrate to PM2.5 reached nearly 40 %. Concurrent increases in NO3− and ClNO2 (with a maximum value of 8.3 ppbv in 1 min time resolution) were observed in the first several hours after sunset, indicating an intense N2O5 heterogeneous uptake on aerosols. The formation potential of NO3− via N2O5 heterogeneous reactions was estimated to be 39.7 to 77.3 μg m−3 in the early hours (3 to 6 h) after sunset based on the measurement data, which could completely explain the measured increase in the NO3− concentration during the same time period. Daytime production of nitric acid from the gas-phase reaction of OH + NO2 was calculated with a chemical box model built using the Master Chemical Mechanism (MCM v3.3.1) and constrained by the measurement data. The integrated nocturnal nitrate formed via N2O5 chemistry was comparable to or even higher than the nitric acid formed during the daytime. This study confirms that N2O5 heterogeneous chemistry was a significant source of aerosol nitrate during hazy days in southern China.

scholarly journals The global 3-D distribution of tropospheric aerosols as characterized by CALIOP

2013 ◽  
Vol 13 (6) ◽  
pp. 3345-3361 ◽  
Author(s):  
D. M. Winker ◽  
J. L. Tackett ◽  
B. J. Getzewich ◽  
Z. Liu ◽  
M. A. Vaughan ◽  
...  
Keyword(s):  
Lower Troposphere ◽  
Aerosol Extinction ◽  
Transport Pathways ◽  
3 Dimensional ◽  
Clear Sky ◽  
Tropospheric Aerosol ◽  
Vertical Distributions ◽  
Dimensional Distribution ◽  
Level 3 ◽  
Sky Conditions

Abstract. The CALIOP lidar, carried on the CALIPSO satellite, has been acquiring global atmospheric profiles since June 2006. This dataset now offers the opportunity to characterize the global 3-D distribution of aerosol as well as seasonal and interannual variations, and confront aerosol models with observations in a way that has not been possible before. With that goal in mind, a monthly global gridded dataset of daytime and nighttime aerosol extinction profiles has been constructed, available as a Level 3 aerosol product. Averaged aerosol profiles for cloud-free and all-sky conditions are reported separately. This 6-yr dataset characterizes the global 3-dimensional distribution of tropospheric aerosol. Vertical distributions are seen to vary with season, as both source strengths and transport mechanisms vary. In most regions, clear-sky and all-sky mean aerosol profiles are found to be quite similar, implying a lack of correlation between high semi-transparent cloud and aerosol in the lower troposphere. An initial evaluation of the accuracy of the aerosol extinction profiles is presented. Detection limitations and the representivity of aerosol profiles in the upper troposphere are of particular concern. While results are preliminary, we present evidence that the monthly-mean CALIOP aerosol profiles provide quantitative characterization of elevated aerosol layers in major transport pathways. Aerosol extinction in the free troposphere in clean conditions, where the true aerosol extinction is typically 0.001 km−1 or less, is generally underestimated, however. The work described here forms an initial global 3-D aerosol climatology which we plan to extend and improve over time.

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