ALBERT

Description: The climate impact of the seasonality of Biomass Burning emitted Carbonaceous Aerosols (BBCA) is studied using an aerosol-climate model coupled with a slab ocean model in a set of 60-year long simulations, driven by BBCA emission data with and without seasonal variation, respectively. The model run with seasonally varying emission of BBCA leads to an increase in the external mixture of carbonaceous aerosols as well as in the internal mixture of organic carbon and sulfate but a decrease in the internal mixture of black carbon and sulfate relative to those in the run with constant annual BBCA emissions, as a result of different strengths of source/sink processes. The differences in atmospheric direct radiative forcing (DRF) caused by BBCA seasonality are in phase with the differences in column concentrations of the external mixture of carbonaceous aerosols in space and time. In contrast, the differences in all-sky radiative forcing at the top of the atmosphere and at the earth's surface extend beyond the BBCA source regions due to climate feedback through cloud distribution and precipitation. The seasonality of biomass burning emissions uniquely affects the global distributions of convective clouds and precipitation, indicating that these emissions have an impact on atmospheric circulation. In addition, the climate response to the periodic climate forcing of BBCA is not limited to biomass burning seasons but dynamically extends into non-biomass burning seasons as well.

Description: Bi-directional air–surface exchange of ammonia (NH3) has been neglected in many air quality models. In this study, we implement the bi-directional exchange of NH3 in the GEOS-Chem global chemical transport model. We also introduce an updated diurnal variability scheme for NH3 livestock emissions and evaluate the recently developed MASAGE_NH3 bottom up inventory. While updated diurnal variability improves comparison of modeled-to-hourly in situ measurements in the Southeastern US, NH3 concentrations decrease throughout the globe, up to 17 ppb in India and Southeastern China, with corresponding decreases in aerosol nitrate by up to 7 μg m−3. The ammonium (NH4+) soil pool in the bi-directional exchange model largely extends the NH3 lifetime in the atmosphere. Including bi-directional exchange generally increases NH3 gross emissions (7.1%) and surface concentrations (up to 3.9 ppb) throughout the globe in July, except in India and Southeastern China. In April and October, it decreases NH3 gross emissions in the Northern Hemisphere (e.g., 43.6% in April in China) and increases NH3 gross emissions in the Southern Hemisphere. Bi-directional exchange does not largely impact NH4+ wet deposition overall. While bi-directional exchange is fundamentally a better representation of NH3 emissions from fertilizers, emissions from primary sources are still underestimated and thus significant model biases remain when compared to in situ measurements in the US. The adjoint of bi-directional exchange has also been developed for the GEOS-Chem model and is used to investigate the sensitivity of NH3 concentrations with respect to soil pH and fertilizer application rate. This study thus lays the groundwork for future inverse modeling studies to more directly constrain these physical processes rather than tuning bulk uni-directional NH3 emissions.

Description: Particulate solar absorption is a critical factor in determining the value and even sign of the direct radiative forcing of aerosols. The heating to the atmosphere and cooling to the Earth's surface caused by this absorption are hypothesized to have significant climate impacts. We find that anthropogenic aerosols play an important role around the globe in total particulate absorption of solar radiation. The global-average anthropogenic fraction in total aerosol absorbing optical depth exceeds 65% in all seasons. Combining the potentially highest dust absorption with the lowest anthropogenic absorption within our model range, this fraction would still exceed 47% in most seasons except for boreal spring (36%) when dust abundance reaches its peak. Nevertheless, dust aerosol is still a critical absorbing constituent over places including North Africa, the entire tropical Atlantic, and during boreal spring in most part of Eurasian continent. The equality in absorbing solar radiation of dust and anthropogenic aerosols appears to be particularly important over Indian subcontinent and nearby regions as well as North Africa.

Description: The climate impact of the seasonality of Biomass Burning emitted Carbonaceous Aerosols (BBCA) has been studied using an aerosol-climate model coupled with a slab ocean model in a set of 60-year long simulations driven by BBCA emission data with and without seasonal variation, respectively. The model run with seasonally varying emission of BBCA leads to an increase in external mixture of carbonaceous aerosols and a decrease in internal mixtures of carbonaceous aerosols relative to those in the run with constant annual BBCA emissions, resulting from different strengths of source/sink processes. We find that the differences in atmospheric direct radiative forcing (DRF) caused by BBCA seasonality are in phase with the differences in column concentrations of an external mixture of carbonaceous aerosols in space and time; thus, the differences in surface temperature and heat fluxes are limited to the biomass burning source regions. In contrast, the differences in all-sky radiative forcing at the top of the atmosphere and at the earth's surface extend beyond the BBCA source regions due to climate feedback through cloud distribution and precipitation. The seasonality of biomass burning emissions uniquely affects the global distributions of high-level clouds and convective precipitation, which indicate an impact on atmospheric circulation. We especially find that the Inter-Tropical Convergence Zone (ITCZ) shifts northward when the seasonality of BBCA emissions is included in the model, compared to the case otherwise configured. In addition, the climate response to the periodic climate forcing of BBCA is not static in biomass burning seasons but dynamically extends into non-biomass seasons as well. The climate effects in contrasting biomass burning seasons occur in the springtime in northern Tropics with the largest difference in precipitation and mixed aerosol abundance caused by the seasonality of BBCA.

Description: Bidirectional air–surface exchange of ammonia (NH3) has been neglected in many air quality models. In this study, we implement the bidirectional exchange of NH3 in the GEOS-Chem global chemical transport model. We also introduce an updated diurnal variability scheme for NH3 livestock emissions and evaluate the recently developed MASAGE_NH3 bottom-up inventory. While updated diurnal variability improves comparison of modeled-to-hourly in situ measurements in the southeastern USA, NH3 concentrations decrease throughout the globe, up to 17 ppb in India and southeastern China, with corresponding decreases in aerosol nitrate by up to 7 μg m−3. The ammonium (NH4+) soil pool in the bidirectional exchange model largely extends the NH3 lifetime in the atmosphere. Including bidirectional exchange generally increases NH3 gross emissions (7.1 %) and surface concentrations (up to 3.9 ppb) throughout the globe in July, except in India and southeastern China. In April and October, it decreases NH3 gross emissions in the Northern Hemisphere (e.g., 43.6 % in April in China) and increases NH3 gross emissions in the Southern Hemisphere. Bidirectional exchange does not largely impact NH4+ wet deposition overall. While bidirectional exchange is fundamentally a better representation of NH3 emissions from fertilizers, emissions from primary sources are still underestimated and thus significant model biases remain when compared to in situ measurements in the USA. The adjoint of bidirectional exchange has also been developed for the GEOS-Chem model and is used to investigate the sensitivity of NH3 concentrations with respect to soil pH and fertilizer application rate. This study thus lays the groundwork for future inverse modeling studies to more directly constrain these physical processes rather than tuning bulk unidirectional NH3 emissions.

Description: Particulate solar absorption is a critical factor in determining the value and even sign of the direct radiative forcing of aerosols. The heating to the atmosphere and cooling to the Earth's surface caused by this absorption are hypothesized to have significant climate impacts. We find that anthropogenic aerosols play an important role around the globe in total particulate absorption of solar radiation. The global-average anthropogenic fraction in total aerosol absorbing optical depth exceeds 65% in all seasons. Combining the potentially highest dust absorption with the lowest anthropogenic absorption within our model range, this fraction would still exceed 47% in most seasons except for boreal spring (36%) when dust abundance reaches its peak. Nevertheless, dust aerosol is still a critical absorbing constituent over places including North Africa, the entire tropical Atlantic, and during boreal spring in most part of Eurasian continent. The equality in absorbing solar radiation of dust and anthropogenic aerosols appears to be particularly important over Indian subcontinent and nearby regions as well as North Africa.