full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban si...full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.展开更多
Simulation results of the WDM6 scheme and the Thompson scheme,both of which are commonly-used double-moment bulkmicrophysics schemes,are compared within theWeather Research and Forecasting model.The purpose of the com...Simulation results of the WDM6 scheme and the Thompson scheme,both of which are commonly-used double-moment bulkmicrophysics schemes,are compared within theWeather Research and Forecasting model.The purpose of the comparison is to study the difference in the aspects of the warm-rain hydrometeor number concentrations,the droplet size distributions,and the budgets of the rain mixing ratio and number concentration.It is found that the WDM6 scheme overestimates the ratio and the amount of large precipitation,and underestimates those of small precipitation,compared to the Thompson scheme.The cloud number concentration(CNC)predicted in the WDM6 scheme is one to three orders ofmagnitude smaller than that of the Thompson scheme,which is set to the specific valueof CNC.The cloud droplet spectra of the WDM6 scheme are broader.The WDM6 scheme produces a larger rain number concentration and smaller mass mean diameter of raindrops under the influence of both warm and cold rain processes—specifically,autoconversion and melting of snow and graupel.The WDM6 scheme produces a larger autoconversion rate and smaller total melting rate of snow and graupel than the Thompson scheme in the rain mixing ratio budget.The sign of the difference in the rain-cloud collection varieswith region,and the rain-cloud collection process together with evaporation of rain have a major influence on the sign of the surface precipitation difference between the two schemes.展开更多
基金supported by the National Natural Science Foundation of China[grant numbers 42275120 and 42075111]the National Key Research and Development Program[grant number 2023YFC3706101]。
文摘full understanding of the sources of atmospheric nitrous acid(HONO)in the polluted urban atmosphere re-mains a challenge.In this study,ambient HONO and relevant species were measured during January 2019 at an urban site in Beijing,China,and a budget analysis of HONO was conducted using a box model combined with field observations.Large nighttime“missing sources”of HONO were identified on heavily polluted days based on traditional sources,which had a significant correlation with the relative humidity,ammonia(NH_(3)),and aerosol surface area,and the promotional effect of NH_(3)for nitrogen dioxide(NO_(2))uptake on the wet aerosol surface was discussed.Then,an updated parameterization scheme for quantifying the enhanced heterogeneous reactions of NO_(2)on aerosol surfaces is proposed,and the missing nighttime sources of HONO could be substantially com-pensated after the new scheme was incorporated.Further evaluation on the contributions of HONO to hydroxyl radicals was conducted,and the authors found that the photolysis of HONO played a dominant role in the primary OH production on the polluted days(78%-90%).The study reveals great potential of an NH3-enhanced uptake coefficient of NO_(2)on the aerosol surface in the nocturnal HONO budget,and highlights the significance of HONO in the strong atmospheric oxidation capability during episodes with a heavily polluted atmosphere.
基金sponsored by the National Natural Science Foundation of China [grant number 41530427]
文摘Simulation results of the WDM6 scheme and the Thompson scheme,both of which are commonly-used double-moment bulkmicrophysics schemes,are compared within theWeather Research and Forecasting model.The purpose of the comparison is to study the difference in the aspects of the warm-rain hydrometeor number concentrations,the droplet size distributions,and the budgets of the rain mixing ratio and number concentration.It is found that the WDM6 scheme overestimates the ratio and the amount of large precipitation,and underestimates those of small precipitation,compared to the Thompson scheme.The cloud number concentration(CNC)predicted in the WDM6 scheme is one to three orders ofmagnitude smaller than that of the Thompson scheme,which is set to the specific valueof CNC.The cloud droplet spectra of the WDM6 scheme are broader.The WDM6 scheme produces a larger rain number concentration and smaller mass mean diameter of raindrops under the influence of both warm and cold rain processes—specifically,autoconversion and melting of snow and graupel.The WDM6 scheme produces a larger autoconversion rate and smaller total melting rate of snow and graupel than the Thompson scheme in the rain mixing ratio budget.The sign of the difference in the rain-cloud collection varieswith region,and the rain-cloud collection process together with evaporation of rain have a major influence on the sign of the surface precipitation difference between the two schemes.
