Steffen Dörner

Bio: Steffen Dörner is an academic researcher from Max Planck Society. The author has contributed to research in topics: Differential optical absorption spectroscopy & Zenith. The author has an hindex of 12, co-authored 47 publications receiving 640 citations.

NO x lifetimes and emissions of cities and power plants in polluted background estimated by satellite observations

Abstract: . We present a new method to quantify NOx emissions and corresponding atmospheric lifetimes from OMI NO2 observations together with ECMWF wind fields without further model input for sources located in a polluted background. NO2 patterns under calm wind conditions are used as proxy for the spatial patterns of NOx emissions, and the effective atmospheric NOx lifetime is determined from the change of spatial patterns measured at larger wind speeds. Emissions are subsequently derived from the NO2 mass above the background, integrated around the source of interest. Lifetimes and emissions are estimated for 17 power plants and 53 cities located in non-mountainous regions across China and the USA. The derived lifetimes for the ozone season (May–September) are 3.8 ± 1.0 h (mean ± standard deviation) with a range of 1.8 to 7.5 h. The derived NOx emissions show generally good agreement with bottom-up inventories for power plants and cities. Regional inventory shows better agreement with top-down estimates for Chinese cities compared to global inventory, most likely due to different downscaling approaches adopted in the two inventories.

Structural uncertainty in air mass factor calculation for NO2 and HCHO satellite retrievals

Abstract: . Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (

Estimating the volcanic emission rate and atmospheric lifetime of SO 2 from space: a case study for Kīlauea volcano, Hawai`i

Abstract: . We present an analysis of SO2 column densities derived from GOME-2 satellite measurements for the Kīlauea volcano (Hawai`i) for 2007–2012. During a period of enhanced degassing activity in March–November 2008, monthly mean SO2 emission rates and effective SO2 lifetimes are determined simultaneously from the observed downwind plume evolution and meteorological wind fields, without further model input. Kīlauea is particularly suited for quantitative investigations from satellite observations owing to the absence of interfering sources, the clearly defined downwind plumes caused by steady trade winds, and generally low cloud fractions. For March–November 2008, the effective SO2 lifetime is 1–2 days, and Kīlauea SO2 emission rates are 9–21 kt day−1, which is about 3 times higher than initially reported from ground-based monitoring systems.

Pinpointing nitrogen oxide emissions from space.

Abstract: Satellite observations of nitrogen dioxide (NO2) provide valuable information on the location and strength of NOx emissions, but spatial resolution is limited by horizontal transport and smearing of temporal averages due to changing wind fields. In this study, we map NOx emissions on high spatial resolution from TROPOMI observations of NO2 combined with wind fields based on the continuity equation. The divergence of horizontal fluxes proves to be highly sensitive for point sources like exhaust stacks. Thus, NOx emissions from individual power plants can be resolved and quantified even on top of considerably high urban pollution from the Saudi Arabian capital city Riyadh. This allows us to catalog NOx emissions from large point sources globally, as demonstrated for South Africa and Germany, with a detection limit of about 0.11 kg/s down to 0.03 kg/s for ideal conditions.

Vertical profiles of NO 2 , SO 2 , HONO, HCHO, CHOCHO and aerosols derived from MAX-DOAS measurements at a rural site in the central western North China Plain and their relation to emission sources and effects of regional transport

Abstract: . A multi-axis differential optical absorption spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18 ∘ N, 114.36 ∘ E) in the suburban area of Xingtai, which is one of the most polluted cities in the North China Plain (NCP), during the Atmosphere-Aerosol-Boundary Layer-Cloud (A 2 BC) experiment and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2 , SO2 , HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with the coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ∼3.5 ppb. Underestimations of MAX-DOAS results compared to in situ measurements of NO2 ( ∼60 %) and SO2 ( ∼20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2 and SO2 are reasonably consistent with those measured by a collocated Raman lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ∼1.4 km) than NO2 , SO2 and HONO did (with 75 % integrated column below ∼0.5 km) under polluted conditions. Lifted layers were systematically observed for all species (except HONO), indicating accumulation, secondary formation or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2 , SO2 and HONO but occurred at around noon for aerosols, HCHO and CHOCHO, mainly dominated by photochemistry, characteristic upslope–downslope circulation and planetary boundary layer (PBL) dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with the backward propagation approach based on HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution was observed from the southern areas such as industrialized Wu'an. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations in HCHO, CHOCHO and aerosols. It needs to be noted that although several MAX-DOAS measurements of trace gases and aerosols in the NCP area have been reported in previous studies, this study is the first work to derive a comprehensive set of vertical profiles of NO2 , SO2 , HONO, HCHO, CHOCHO and aerosols from measurements of one MAX-DOAS instrument. Also, so far, the validation of MAX-DOAS profile results by comparison with various surface in situ measurements as well as profile measurements from lidar and aircraft is scarce. Moreover, the backward propagation approach for characterizing the contributions of regional transport of pollutants from different regions was applied to the MAX-DOAS results of trace gases and aerosols for the first time.

Unexpected air pollution with marked emission reductions during the COVID-19 outbreak in China.

Abstract: The absence of motor vehicle traffic and suspended manufacturing during the coronavirus disease 2019 (COVID-19) pandemic in China enabled assessment of the efficiency of air pollution mitigation. Up to 90% reduction of certain emissions during the city-lockdown period can be identified from satellite and ground-based observations. Unexpectedly, extreme particulate matter levels simultaneously occurred in northern China. Our synergistic observation analyses and model simulations show that anomalously high humidity promoted aerosol heterogeneous chemistry, along with stagnant airflow and uninterrupted emissions from power plants and petrochemical facilities, contributing to severe haze formation. Also, because of nonlinear production chemistry and titration of ozone in winter, reduced nitrogen oxides resulted in ozone enhancement in urban areas, further increasing the atmospheric oxidizing capacity and facilitating secondary aerosol formation.

Multiphase chemistry at the atmosphere-biosphere interface influencing climate and public health in the anthropocene.

Abstract: This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. Review pubs.acs.org/CR Multiphase Chemistry at the Atmosphere−Biosphere Interface Influencing Climate and Public Health in the Anthropocene Ulrich Po schl* and Manabu Shiraiwa* Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany air contaminants (SHCC) and their multiphase chemical interactions at the atmosphere−biosphere interface, including human lungs and skin, plant leaves, cryptogamic covers, soil, and aquatic surfaces. After an overview of different groups of SHCC, we address the chemical interactions of reactive oxygen species and reactive nitrogen species (ROS, RNS), primary biological and secondary organic aerosols (PBA, SOA), as well as carbonaceous combustion aerosols (CCA) including soot, black/elemental carbon, polycyclic aromatic hydrocarbons, and related compounds (PAH, PAC). ROS and RNS interact strongly with other SHCC and are central to both atmospheric and physiological processes and their coupling through the atmosphere−biosphere interface, for example, in the formation and aging of biogenic and combustion aerosols as well as in CONTENTS inflammatory and allergic immune responses triggered by air pollution. Deposition of atmospheric ROS/RNS and aerosols 1. Introduction and Motivation can damage biological tissues, modify surface microbiomes, and 2. Health- and Climate-Relevant Air Contaminants induce oxidative stress through Fenton-like reactions and 2.1. Reactive Oxygen and Nitrogen Species immune responses. The chemical mechanisms and kinetics are 2.2. Primary Biological Aerosols not yet fully elucidated, but the available evidence suggests that 2.3. Secondary Organic Aerosols multiphase processes are crucial for the assessment, prediction, 2.4. Carbonaceous Combustion Aerosols and handling of air quality, climate, and public health. Caution 2.5. Other Air Contaminants Linking Atmospher- should be taken to avoid that human activities shaping the ic and Physiological Chemistry Anthropocene create a hazardous or pathogenic atmosphere 3. Multiphase Chemical Reactions at Specific Bio- overloaded with allergenic, corrosive, toxic, or infectious logical Interfaces contaminants. 3.1. Lung Lining Fluid Multiphase chemistry deals with chemical reactions, trans- 3.2. Human Skin port processes, and transformations between gaseous, liquid, 3.3. Plant Surfaces and Cryptogamic Covers and solid matter. These processes are essential for Earth system 3.4. Soil and Aquatic Surfaces science and climate research as well as for life and health 4. Conclusions and Outlook sciences on molecular and global levels, bridging a wide range Author Information of spatial and temporal scales from below nanometers to Corresponding Authors thousands of kilometers and from less than nanoseconds to Notes years and millennia as illustrated in Figure 1. Biographies From a chemical perspective, life and the metabolism of most Acknowledgments living organisms can be regarded as multiphase processes References involving gases like oxygen and carbon dioxide; liquids like water, blood, lymph, and plant sap; and solid or semisolid substances like bone, tissue, skin, wood, and cellular 1. INTRODUCTION AND MOTIVATION membranes. Even primitive forms of life and metabolic activity Multiphase chemistry plays a vital role in the Earth system, under anaerobic conditions generally involve multiple liquid climate, and health. Chemical reactions, mass transport, and and solid or semisolid phases structured by cells, organelles, and phase transitions between gases, liquids, and solids are essential membranes. 2 On global scales, the biogeochemical cycling of for the interaction and coevolution of life and climate. chemical compounds and elements, which can be regarded as Knowledge of the mechanisms and kinetics of these processes the metabolism of planet Earth, also involves chemical is also required to address societally relevant questions of global reactions, mass transport, and phase transitions within and environmental change and public health in the Anthropocene, that is, in the present era of globally pervasive and steeply Special Issue: 2015 Chemistry in Climate increasing human influence on planet Earth. 1 In this work, we review the current scientific understanding and recent advances Received: September 1, 2014 in the investigation of short-lived health- and climate-relevant Published: April 9, 2015 © 2015 American Chemical Society DOI: 10.1021/cr500487s Chem. Rev. 2015, 115, 4440−4475

High-resolution inventory of technologies, activities, and emissions of coal-fired power plants in China from 1990 to 2010

Abstract: . This paper, which focuses on emissions from China's coal-fired power plants during 1990–2010, is the second in a series of papers that aims to develop a high-resolution emission inventory for China. This is the first time that emissions from China's coal-fired power plants were estimated at unit level for a 20-year period. This inventory is constructed from a unit-based database compiled in this study, named the China coal-fired Power plant Emissions Database (CPED), which includes detailed information on the technologies, activity data, operation situation, emission factors, and locations of individual units and supplements with aggregated data where unit-based information is not available. Between 1990 and 2010, compared to a 479 % growth in coal consumption, emissions from China's coal-fired power plants increased by 56, 335, and 442 % for SO2, NOx, and CO2, respectively, and decreased by 23 and 27 % for PM2.5 and PM10 respectively. Driven by the accelerated economic growth, large power plants were constructed throughout the country after 2000, resulting in a dramatic growth in emissions. The growth trend of emissions has been effectively curbed since 2005 due to strengthened emission control measures including the installation of flue gas desulfurization (FGD) systems and the optimization of the generation fleet mix by promoting large units and decommissioning small ones. Compared to previous emission inventories, CPED significantly improved the spatial resolution and temporal profile of the power plant emission inventory in China by extensive use of underlying data at unit level. The new inventory developed in this study will enable a close examination of temporal and spatial variations of power plant emissions in China and will help to improve the performances of chemical transport models by providing more accurate emission data.

Tropospheric Halogen Chemistry: Sources, Cycling,and Impacts

Abstract: In the past 40 years, atmospheric chemists have come to realize that halogens exert a powerful influence on the chemical composition of the troposphere and through that influence affect the fate of pollutants and may affect climate. Of particular note for climate is that halogen cycles affect methane, ozone, and particles, all of which are powerful climate forcing agents through direct and indirect radiative effects. This influencecomes from the high reactivity of atomic halogen radicals (e.g.,Cl, Br, I) and halogen oxides (e.g., ClO, BrO, IO, and higher oxides), known as reactive halogen species in this review. These reactive halogens are potent oxidizers for organic and inorganic compounds throughout the troposphere.

Stratospheric Aerosol--Observations, Processes, and Impact on Climate

Abstract: Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.