Implementation of HONO into the chemistry-climate model CHASER (V4.0): roles in tropospheric chemistry

Abstract. Nitrous acid (HONO) is an important atmospheric gas given its contribution to the cycles of NOx and HOx, but its role in global atmospheric photochemistry is not fully understood. This study, for the first time, implemented three pathways of HONO formation in the chemistry-climate model CHASER (MIROC-ESM) to explore three physical phenomena: gas-phase kinetic reactions (GRs), direct emission (EM), and heterogeneous reactions on cloud/aerosol particles (HRs). We evaluated the simulations by the atmospheric measurements from the OMI (Ozone Monitoring Instrument), EANET (Acid Deposition Monitoring Network in eastern Asia) / EMEP (European Monitoring and Evaluation Programme) ground-based stationary observations, observations from the ship R/V Mirai, and aircraft-based measurements by ATom1 (atmospheric tomography) and EMeRGe-Asia-2018 (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global scales). We showed that the inclusion of the HONO chemistry in the modeling process reduces the model bias against the measurements for PM2.5, NO3−/HNO3, NO2, OH, O3, and CO, especially in the lower troposphere and the North Pacific (NP) region. We found that the retrieved global abundance of tropospheric HONO was 1.4 TgN. Of the three source pathways, HRs and EM contributed 63 % and 26 % to the net HONO production, respectively. We also observed that, reactions on the aerosol surfaces contributed larger amounts of HONO (51 %) than those on the cloud surfaces (12 %). The model exhibited significant negative biases for daytime HONO in the Asian off-coast region, compared with the airborne measurements by EMeRGe-Asia-2018, indicating the existence of unknown daytime HONO sources. Strengthening of aerosol uptake of NO2 near-surface and in the middle troposphere, cloud uptake, and direct HONO emission are all potential yet-unknown HONO sources. We also found that the simulated HONO abundance and its impact on NOx-O3 chemistry are sensitive to the yield of the heterogeneous conversion of NO2 to HONO (vs. HNO3). Inclusion of HONO reduces global tropospheric NOx (NO + NO2) levels by 20.4 %, thereby weakening the tropospheric oxidizing capacity, which in turn, increases CH4 lifetime (13 %) and CO abundance (8 %). HRs on the surfaces of cloud particles, which have been neglected in previous modeling studies, are the main drivers of these impacts. This effect is particularly salient for the substantial reductions of levels of OH (40–67 %) and O3 (30–45 %) in the NP region during summer given the significant reduction of NOx level (50–95 %). In contrast, HRs on aerosol surfaces in China (Beijing) enhance OH and O3 winter mean levels by 600–1700 % and 10–33 %, respectively, with regards to their minima in winter. Overall, our findings suggest that a global model that does not consider HONO heterogeneous mechanisms (especially HRs on cloud particle surfaces) may erroneously predict the effect of HONO in remote areas and polluted regions.

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

Geoscientific Model Development ◽

10.5194/gmd-14-3813-2021 ◽

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).

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Effects of heterogeneous reactions on global tropospheric chemistry

10.5194/gmd-2020-335 ◽

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).

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Seasonal Prediction Skill of Northern Extratropical Surface Temperature Driven by the Stratosphere

Journal of Climate ◽

10.1175/jcli-d-16-0475.1 ◽

2017 ◽

Vol 30 (12) ◽

pp. 4463-4475 ◽

Cited By ~ 26

Author(s):

Liwei Jia ◽

Xiaosong Yang ◽

Gabriel Vecchi ◽

Richard Gudgel ◽

Thomas Delworth ◽

...

Keyword(s):

Climate Model ◽

Lower Troposphere ◽

Polar Vortex ◽

Seasonal Prediction ◽

The Arctic ◽

Northern Eurasia ◽

Stratospheric Polar Vortex ◽

Near Surface ◽

Predictive Skill

This study explores the role of the stratosphere as a source of seasonal predictability of surface climate over Northern Hemisphere extratropics both in the observations and climate model predictions. A suite of numerical experiments, including climate simulations and retrospective forecasts, are set up to isolate the role of the stratosphere in seasonal predictive skill of extratropical near-surface land temperature. It is shown that most of the lead-0-month spring predictive skill of land temperature over extratropics, particularly over northern Eurasia, stems from stratospheric initialization. It is further revealed that this predictive skill of extratropical land temperature arises from skillful prediction of the Arctic Oscillation (AO). The dynamical connection between the stratosphere and troposphere is also demonstrated by the significant correlation between the stratospheric polar vortex and sea level pressure anomalies, as well as the migration of the stratospheric zonal wind anomalies to the lower troposphere.

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Characterization of ozone profiles derived from Aura TES and OMI Radiances

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-27589-2012 ◽

2012 ◽

Vol 12 (10) ◽

pp. 27589-27636 ◽

Cited By ~ 5

Author(s):

D. Fu ◽

J. R. Worden ◽

X. Liu ◽

S. S. Kulawik ◽

K. W. Bowman ◽

...

Keyword(s):

Degrees Of Freedom ◽

Surface Ozone ◽

Lower Troposphere ◽

Vertical Resolution ◽

Ozone Monitoring Instrument ◽

Near Surface ◽

Upper Troposphere ◽

Ozone Profile ◽

Mean Square Difference

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Climate of the Greenland ice sheet using a high-resolution climate model – Part 1: Evaluation

The Cryosphere Discussions ◽

10.5194/tcd-4-561-2010 ◽

2010 ◽

Vol 4 (2) ◽

pp. 561-602 ◽

Cited By ~ 8

Author(s):

J. Ettema ◽

M. R. van den Broeke ◽

E. van Meijgaard ◽

W. J. van de Berg ◽

J. E. Box ◽

...

Keyword(s):

Surface Energy ◽

Climate Model ◽

Ice Sheet ◽

Greenland Ice Sheet ◽

Specific Humidity ◽

Katabatic Wind ◽

Turbulent Heat ◽

Atmospheric Measurements ◽

Near Surface ◽

Downward Longwave Radiation

Abstract. A simulation of 51 years (1957–2008) has been performed over Greenland using the regional atmospheric climate model RACMO2 at a horizontal grid spacing of 11 km forced by ECMWF analysis products. To better represent processes affecting ice sheet surface mass balance, such as melt water refreezing and penetration, an additional snow/ice surface module has been developed and implemented into the surface parameterisation of RACMO2v1. The temporal evolution and climatology of the model is evaluated with in situ coastal and ice sheet atmospheric measurements of near-surface variables and surface energy balance components. The bias for the near-surface air temperature (0.9 °C), specific humidity (0.1 g kg−1), wind speed (0.3 m s−1) as well as for radiative (2.5 W m−2 for net radiation) and turbulent heat fluxes shows that the model is in good accordance with available observations. The modeled surface energy budget underestimates the downward longwave radiation and overestimates the sensible heat flux. Due to their compensating effect, the averaged 2 m temperature bias is less than −0.9°C. The katabatic wind circulation is well captured by the model.

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Reassessing Statistical Downscaling Techniques for Their Robust Application under Climate Change Conditions

Journal of Climate ◽

10.1175/jcli-d-11-00687.1 ◽

2013 ◽

Vol 26 (1) ◽

pp. 171-188 ◽

Cited By ~ 78

Author(s):

J. M. Gutiérrez ◽

D. San-Martín ◽

S. Brands ◽

R. Manzanas ◽

S. Herrera

Keyword(s):

Climate Change ◽

Statistical Downscaling ◽

Climate Model ◽

Global Climate ◽

Global Climate Model ◽

Lower Troposphere ◽

Temperature Inversion ◽

Max Planck ◽

Near Surface ◽

Climate Conditions

Abstract The performance of statistical downscaling (SD) techniques is critically reassessed with respect to their robust applicability in climate change studies. To this end, in addition to standard accuracy measures and distributional similarity scores, the authors estimate the robustness of the methods under warming climate conditions working with anomalous warm historical periods. This validation framework is applied to intercompare the performances of 12 different SD methods (from the analog, weather typing, and regression families) for downscaling minimum and maximum temperatures in Spain. First, a calibration of these methods is performed in terms of both geographical domains and predictor sets; the results are highly dependent on the latter, with optimum predictor sets including near-surface temperature data (in particular 2-m temperature), which appropriately discriminate cold episodes related to temperature inversion in the lower troposphere. Although regression methods perform best in terms of correlation, analog and weather generator approaches are more appropriate for reproducing the observed distributions, especially in case of wintertime minimum temperature. However, the latter two families significantly underestimate the temperature anomalies of the warm periods considered in this work. This underestimation is found to be critical when considering the warming signal in the late twenty-first century as given by a global climate model [the ECHAM5–Max Planck Institute (MPI) model]. In this case, the different downscaling methods provide warming values with differences in the range of 1°C, in agreement with the robustness significance values. Therefore, the proposed test is a promising technique for detecting lack of robustness in statistical downscaling methods applied in climate change studies.

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Characterization of ozone profiles derived from Aura TES and OMI radiances

Atmospheric Chemistry and Physics ◽

10.5194/acp-13-3445-2013 ◽

2013 ◽

Vol 13 (6) ◽

pp. 3445-3462 ◽

Cited By ~ 49

Author(s):

D. Fu ◽

J. R. Worden ◽

X. Liu ◽

S. S. Kulawik ◽

K. W. Bowman ◽

...

Keyword(s):

Degrees Of Freedom ◽

Surface Ozone ◽

A Priori ◽

Lower Troposphere ◽

Vertical Resolution ◽

Ozone Monitoring Instrument ◽

Near Surface ◽

Production Code ◽

Ozone Profile

Abstract. We present satellite based ozone profile estimates derived by combining radiances measured at thermal infrared (TIR) wavelengths from the Aura Tropospheric Emission Spectrometer (TES) and ultraviolet (UV) wavelengths measured by the Aura Ozone Monitoring Instrument (OMI). The advantage of using these combined wavelengths and instruments for sounding ozone over either instrument alone is improved sensitivity near the surface as well as the capability to consistently resolve the lower troposphere, upper troposphere, and lower stratosphere for scenes with varying geophysical states. For example, the vertical resolution of ozone estimates from either TES or OMI varies strongly by surface albedo and temperature. Typically, TES provides 1.6 degrees of freedom for signal (DOFS) and OMI provides less than 1 DOFS in the troposphere. The combination provides 2 DOFS in the troposphere with approximately 0.4 DOFS for near surface ozone (surface to 700 hPa). We evaluated these new ozone profile estimates with ozonesonde measurements and found that calculated errors for the joint TES and OMI ozone profile estimates are in reasonable agreement with actual errors as derived by the root-mean-square (RMS) difference between the ozonesondes and the joint TES/OMI ozone estimates. We also used a common a priori profile in the retrievals in order to evaluate the capability of different retrieval approaches on capturing near-surface ozone variability. We found that the vertical resolution of the joint TES/OMI ozone profile estimates shows significant improvements on quantifying variations in near-surface ozone with RMS differences of 49.9% and correlation coefficient of R = 0.58 for the TES/OMI near-surface estimates as compared to 67.2% RMS difference and R = 0.33 for TES and 115.8% RMS difference and R = 0.09 for OMI. This comparison removes the impacts of using the climatological a priori in the retrievals. However, it results in artificially large sonde/retrieval differences. The TES/OMI ozone profiles from the production code of joint retrievals will use climatological a priori and therefore will have more realistic ozone estimates than those from using a common a priori volume mixing ratio profile.

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Representativeness of the IAGOS airborne measurements in the lower troposphere

Elem Sci Anth ◽

10.1525/elementa.280 ◽

2018 ◽

Vol 6 ◽

Cited By ~ 6

Author(s):

H. Petetin ◽

M. Jeoffrion ◽

B. Sauvage ◽

G. Athier ◽

R. Blot ◽

...

Keyword(s):

Air Quality ◽

Lower Troposphere ◽

Monitoring Network ◽

Ratio Distribution ◽

Airborne Measurements ◽

Mixing Ratios ◽

The Difference ◽

The Vertical Distribution ◽

Local Emissions

In the framework of the In Service Aircraft for Global Observing System (IAGOS) program, airborne in-situ O3 and CO measurements are performed routinely using in-service aircraft, providing vertical profiles from the surface to about 10–12 km. Due to the specificity of IAGOS measurements (measurements around busy international airports), uncertainties exist on their representativeness in the lower troposphere as they may be impacted by emissions related to airport activities and/or other aircraft. In this study, we thus investigate how the IAGOS measurements in the lower troposphere compare with nearby surface stations (from the local Air Quality monitoring network (AQN)) and more distant regional surface stations (from the Global Atmospheric Watch (GAW) network). The study focuses on Frankfurt but some results at other European airports (Vienna, Paris) are also discussed. Results indicate that the IAGOS observations close to the surface do not appear to be strongly impacted by local emissions related to airport activities. In terms of mixing ratio distribution, seasonal variations and trends, the CO and O3 mixing ratios measured by IAGOS in the first few hundred metres above the surface have similar characteristics to the mixing ratios measured at surrounding urban background stations. Higher in altitude, both the difference with data from the local AQN and the consistency with the GAW regional stations are higher, which indicates a larger representativeness of the IAGOS data. Despite few quantitative differences with Frankfurt, consistent results are obtained in the two other cities Vienna and Paris. Based on 11 years of data (2002–2012), this study thus demonstrates that IAGOS observations in the lowest troposphere can be used as a complement to surface stations to study the air quality in/around the agglomeration, providing important information on the vertical distribution of pollution.

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Observation of ozone enhancement in the lower troposphere over East Asia from a space-borne ultraviolet spectrometer

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-15-2013-2015 ◽

2015 ◽

Vol 15 (2) ◽

pp. 2013-2054 ◽

Cited By ~ 3

Author(s):

S. Hayashida ◽

X. Liu ◽

A. Ono ◽

K. Yang ◽

K. Chance

Keyword(s):

Eastern China ◽

Lower Troposphere ◽

Spatial And Temporal Variation ◽

Ozone Monitoring Instrument ◽

Airborne Measurements ◽

Model Studies ◽

Earth Observing System ◽

Ozone Distribution ◽

Crop Residue Burning ◽

Ultraviolet Spectrometer

Abstract. We report observations from space using ultraviolet (UV) radiance for significant enhancement of ozone in the lower troposphere over Central and Eastern China (CEC). The recent retrieval products of the Ozone Monitoring Instrument (OMI) onboard the Earth Observing System (EOS)/Aura satellite revealed the spatial and temporal variation of ozone distributions in multiple layers in the troposphere. We compared the OMI-derived ozone over Beijing with airborne measurements by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. The correlation between OMI and MOZAIC ozone in the lower troposphere was reasonable, which assured the reliability of OMI ozone retrievals in the lower troposphere under enhanced ozone conditions. The ozone enhancement was clearly observed over CEC, with Shandong Province as its center, and most notable in June in any given year. Similar seasonal variations were observed throughout the nine-year OMI measurement period of 2005 to 2013. The ozone enhancement in June was associated with the enhancement of carbon monoxide (CO) and hotspots, which is consistent with previous studies of in-situ measurements such those made by the MTX2006 campaign. A considerable part of this ozone enhancement could be attributed to the emissions of ozone precursors from open crop residue burning (OCRB) after the winter wheat harvest, in addition to emissions from industrial activities and automobiles. The ozone distribution presented in this study is also consistent with some model studies that apply emissions from OCRB. The lower tropospheric ozone distribution is first shown from OMI retrieval in this study, and the results will be useful in clarifying any unknown factors that influence ozone distribution by comparison with model simulations.

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Observation of ozone enhancement in the lower troposphere over East Asia from a space-borne ultraviolet spectrometer

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-9865-2015 ◽

2015 ◽

Vol 15 (17) ◽

pp. 9865-9881 ◽

Cited By ~ 14

Author(s):

S. Hayashida ◽

X. Liu ◽

A. Ono ◽

K. Yang ◽

K. Chance

Keyword(s):

Eastern China ◽

Lower Troposphere ◽

Spatial And Temporal Variation ◽

Ozone Monitoring Instrument ◽

Airborne Measurements ◽

Model Studies ◽

Earth Observing System ◽

Ozone Distribution ◽

Crop Residue Burning ◽

Ultraviolet Spectrometer

Abstract. We report observations from space using ultraviolet (UV) radiance for significant enhancement of ozone in the lower troposphere over central and eastern China (CEC). The recent retrieval products of the Ozone Monitoring Instrument (OMI) onboard the Earth Observing System (EOS) Aura satellite revealed the spatial and temporal variation of ozone distributions in multiple layers in the troposphere. We compared the OMI-derived ozone over Beijing with airborne measurements by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. The correlation between OMI and MOZAIC ozone in the lower troposphere was reasonable, which assured the reliability of OMI ozone retrievals in the lower troposphere under enhanced ozone conditions. The ozone enhancement was clearly observed over CEC, with Shandong Province as its center, and was most notable in June in any given year. Similar seasonal variations were observed throughout the 9-year OMI measurement period of 2005 to 2013. A considerable part of this ozone enhancement could be attributed to the emissions of ozone precursors from industrial activities and automobiles, and possibly from open crop residue burning (OCRB) after the winter wheat harvest. The ozone distribution presented in this study is also consistent with some model studies. The lower tropospheric ozone distribution is first shown from OMI retrieval in this study, and the results will be useful in clarifying any unknown factors that influence ozone distribution by comparison with model simulations.

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