ALBERT

Description: Carbon–nitrogen (C–N) interactions regulate N availability for plant growth and for emissions of nitrous oxide (N2O) and the uptake of carbon dioxide. Future projections of these terrestrial greenhouse gas fluxes are strikingly divergent, leading to major uncertainties in projected global warming. Here we analyse the large increase in terrestrial N2O emissions over the past 21 000 years as reconstructed from ice-core isotopic data and presented in part 1 of this study. Remarkably, the increase occurred in two steps, each realized over decades and within a maximum of 2 centuries, at the onsets of the major deglacial Northern Hemisphere warming events. The data suggest a highly dynamic and responsive global N cycle. The increase may be explained by an increase in the flux of reactive N entering and leaving ecosystems or by an increase in N2O yield per unit N converted. We applied the LPX-Bern dynamic global vegetation model in deglacial simulations forced with Earth system model climate data to investigate N2O emission patterns, mechanisms, and C–N coupling. The N2O emission changes are mainly attributed to changes in temperature and precipitation and the loss of land due to sea-level rise. LPX-Bern simulates a deglacial increase in N2O emissions but underestimates the reconstructed increase by 47 %. Assuming time-independent N sources in the model to mimic progressive N limitation of plant growth results in a decrease in N2O emissions in contrast to the reconstruction. Our results appear consistent with suggestions of (a) biological controls on ecosystem N acquisition and (b) flexibility in the coupling of the C and N cycles during periods of rapid environmental change. A dominant uncertainty in the explanation of the reconstructed N2O emissions is the poorly known N2O yield per N lost through gaseous pathways and its sensitivity to soil conditions. The deglacial N2O record provides a constraint for future studies.

Description: A total of 252 emission plumes of ships operating in the Mediterranean Sea and around the Arabian Peninsula were investigated using a comprehensive dataset of gas- and submicron-particle-phase properties measured during the 2-month shipborne AQABA (Air Quality and Climate Change in the Arabian Basin) field campaign in summer 2017. The post-measurement identification of the corresponding ship emission events in the measured data included the determination of the plume sources (up to 38 km away) as well as the plume ages (up to 115 min) and was based on commercially available historical records of the Automatic Identification System. The dispersion lifetime of chemically inert CO2 in the ship emission plumes was determined as 70±15 min, resulting in levels indistinguishable from the marine background after 260±60 min. Emission factors (EFs) as quantities that are independent of plume dilution were calculated and used for the investigation of influences on ship emission plumes caused by ship characteristics and the combustion process as well as by atmospheric processes during the early stage of exhaust release and during plume ageing. Combustion efficiency and therefore emission factors of black carbon and NOx were identified to depend mostly on the vessel speed and gross tonnage. Moreover, larger ships, associated with higher engine power, were found to use fuel with higher sulfur content and have higher gas-phase SO2, particulate sulfate, particulate organics, and particulate matter EFs. Despite the independence of EFs of dilution, a significant influence of the ambient wind speed on the particle number and mass EFs was observed that can be traced back to enhanced particle coagulation in the case of slower dilution and suppressed vapour condensation on particles in the case of faster dilution of the emission plume. Atmospheric reactions and processes in ship emission plumes were investigated that include NOx and O3 chemistry, gas-to-particle conversion of NOx and SO2, and the neutralisation of acids in the particle phase through the uptake of ambient gas-phase ammonia, the latter two of which cause the inorganic particulate content to increase and the organic fraction to decrease with increasing plume age. The results allow for us to describe the influences on (or processes in) ship emission plumes quantitatively by parameterisations, which could be used for further refinement of atmospheric models, and to identify which of these processes are the most important ones.

Description: Partitioning uncertainty in projections of future climate change into contributions from internal variability, model response uncertainty and emissions scenarios has historically relied on making assumptions about forced changes in the mean and variability. With the advent of multiple single-model initial-condition large ensembles (SMILEs), these assumptions can be scrutinized, as they allow a more robust separation between sources of uncertainty. Here, the framework from Hawkins and Sutton (2009) for uncertainty partitioning is revisited for temperature and precipitation projections using seven SMILEs and the Coupled Model Intercomparison Project CMIP5 and CMIP6 archives. The original approach is shown to work well at global scales (potential method bias 

Description: Black carbon (BC) or soot is a constituent of particulate matter (PM) which is relevant for negative human health and climate effects, and despite the lack of direct legal limits, it is recognised as an important atmospheric pollutant to monitor, understand, and control. Aethalometers are instruments which continuously monitor BC by measuring absorption at a number of distinct wavelengths. If collocated elemental carbon (EC) observations are used to transform these values into BC mass, by convention, the result is named equivalent black carbon (EBC). BC emitted by different combustion processes has different optical absorption characteristics, and this can be used to apportion EBC mass into traffic (EBCTR) and woodburning (EBCWB) components with a data processing technique known as the aethalometer model. The aethalometer model was applied to six EBC monitoring sites across Switzerland (using data between 2008 and 2018) and was evaluated by investigating diurnal cycles, model coefficients, and ambient temperature dependence of the two EBC components. For one monitoring site, San Vittore, the aethalometer model failed to produce plausible outputs. The reason for this failure was likely due to a high load of freshly emitted wood smoke during the winter which should be thought of as a third distinct emission source. After model evaluation, the trend analysis indicated that EBCTR concentrations at the remaining five locations significantly decreased between 2008 and 2018. EBCWB also demonstrated significant decreases in most monitoring locations but not at a monitoring site south of the Alps with a high PM load sourced from biomass burning. Ratios of EBC and particulate matter with a diameter of less than 2.5 µm (PM2.5) suggested that EBC contributes 6 %–14 % of the PM2.5 mass in Switzerland. The aethalometer model is a useful data analysis procedure but can fail under certain conditions; thus, careful evaluation is required to ensure the method is robust and suitable in other locations.

Description: Shortwave (SW) fluxes estimated from broadband radiometry rely on empirically gathered and hemispherically resolved fields of outgoing top-of-atmosphere (TOA) radiances. This study aims to provide more accurate and precise fields of TOA SW radiances reflected from clouds over ocean by introducing a novel semiphysical model predicting radiances per narrow sun-observer geometry. This model was statistically trained using CERES-measured radiances paired with MODIS-retrieved cloud parameters as well as reanalysis-based geophysical parameters. By using radiative transfer approximations as a framework to ingest the above parameters, the new approach incorporates cloud-top effective radius and above-cloud water vapor in addition to traditionally used cloud optical depth, cloud fraction, cloud phase, and surface wind speed. A two-stream cloud albedo – serving to statistically incorporate cloud optical thickness and cloud-top effective radius – and Cox–Munk ocean reflectance were used to describe an albedo over each CERES footprint. Effective-radius-dependent asymmetry parameters were obtained empirically and separately for each viewing-illumination geometry. A simple equation of radiative transfer, with this albedo and attenuating above-cloud water vapor as inputs, was used in its log-linear form to allow for statistical optimization. We identified the two-stream functional form that minimized radiance residuals calculated against CERES observations and outperformed the state-of-the-art approach for most observer geometries outside the sun-glint and solar zenith angles between 20 and 70∘, reducing the median SD of radiance residuals per solar geometry by up to 13.2 % for liquid clouds, 1.9 % for ice clouds, and 35.8 % for footprints containing both cloud phases. Geometries affected by sun glint (constituting between 10 % and 1 % of the discretized upward hemisphere for solar zenith angles of 20 and 70∘, respectively), however, often showed weaker performance when handled with the new approach and had increased residuals by as much as 60 % compared to the state-of-the-art approach. Overall, uncertainties were reduced for liquid-phase and mixed-phase footprints by 5.76 % and 10.81 %, respectively, while uncertainties for ice-phase footprints increased by 0.34 %. Tested for a variety of scenes, we further demonstrated the plausibility of scene-wise predicted radiance fields. This new approach may prove useful when employed in angular distribution models and may result in improved flux estimates, in particular dealing with clouds characterized by small or large droplet/crystal sizes.

Description: Monitoring of CO2 degassing in seismoactive areas allows the study of correlations of gas release and seismic activity. Reliable continuous monitoring of the gas flow rate in rough field conditions requires robust methods capable of measuring gas flow at different types of gas outlets such as wet mofettes, mineral springs, and boreholes. In this paper we focus on the methods and results of the long-term monitoring of CO2 degassing in the West Bohemia/Vogtland region in central Europe, which is typified by the occurrence of earthquake swarms and discharge of carbon dioxide of magmatic origin. Besides direct flow measurement using flowmeters, we introduce a novel indirect technique based on quantifying the gas bubble contents in a water column, which is capable of functioning in severe environmental conditions. The method calculates the mean bubble fraction in a water–gas mixture from the pressure difference along a fixed depth interval in a water column. Laboratory tests indicate the nonlinear dependence of the bubble fraction on the flow rate, which is confirmed by empirical models found in the chemical and nuclear engineering literature. Application of the method in a pilot borehole shows a high correlation between the bubble fraction and measured gas flow rate. This was specifically the case for two coseismic anomalies in 2008 and 2014, when the flow rate rose during a seismic swarm to a multitude of the preseismic level for several months and was followed by a long-term flow rate decline. However, three more seismic swarms occurring in the same fault zone were not associated with any significant CO2 flow anomaly. We surmise that this could be related to the slightly farther distance of the hypocenters of these swarms compared to the two ones which caused the coseismic CO2 flow rise. Further long-term CO2-flow monitoring is required to verify the mutual influence of CO2 degassing and seismic activity in the area.

Description: Strongly enhanced tropospheric ozone (O3) mixing ratios have been reported in the Arabian Basin, a region with intense solar radiation and high concentrations of O3 precursors such as nitrogen oxides (NOx) and volatile organic compounds (VOCs). To analyze photochemical O3 production in the marine boundary layer (MBL) around the Arabian Peninsula, we use shipborne observations of NO, NO2, O3, OH, HO2, HCHO, the actinic flux, water vapor, pressure and temperature obtained during the summer 2017 Air Quality and Climate in the Arabian Basin (AQABA) campaign, and we compare them to simulation results from the ECHAM-MESSy Atmospheric Chemistry (EMAC) general circulation model. Net O3 production rates (NOPRs) were greatest over both the Gulf of Oman and the northern Red Sea (16 ppbv d−1) and over the Arabian Gulf (32 ppbv d−1). The NOPR over the Mediterranean, the southern Red Sea and the Arabian Sea did not significantly deviate from zero; however, the results for the Arabian Sea indicated weak net O3 production of 5 ppbv d−1 as well as net O3 destruction over the Mediterranean and the southern Red Sea with values of −1 and −4 ppbv d−1, respectively. Constrained by HCHO∕NO2 ratios, our photochemistry calculations show that net O3 production in the MBL around the Arabian Peninsula mostly occurs in NOx-limited regimes with a significant share of O3 production occurring in the transition regime between NOx limitation and VOC limitation over the Mediterranean and more significantly over the northern Red Sea and Oman Gulf.

Description: In the present-day atmosphere, sulfuric acid is the most important vapour for aerosol particle formation and initial growth. However, the growth rates of nanoparticles (

Description: Highly oxygenated organic molecules (HOMs) contribute substantially to the formation and growth of atmospheric aerosol particles, which affect air quality, human health and Earth's climate. HOMs are formed by rapid, gas-phase autoxidation of volatile organic compounds (VOCs) such as α-pinene, the most abundant monoterpene in the atmosphere. Due to their abundance and low volatility, HOMs can play an important role in new-particle formation (NPF) and the early growth of atmospheric aerosols, even without any further assistance of other low-volatility compounds such as sulfuric acid. Both the autoxidation reaction forming HOMs and their NPF rates are expected to be strongly dependent on temperature. However, experimental data on both effects are limited. Dedicated experiments were performed at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN to address this question. In this study, we show that a decrease in temperature (from +25 to −50 ∘C) results in a reduced HOM yield and reduced oxidation state of the products, whereas the NPF rates (J1.7 nm) increase substantially. Measurements with two different chemical ionization mass spectrometers (using nitrate and protonated water as reagent ion, respectively) provide the molecular composition of the gaseous oxidation products, and a two-dimensional volatility basis set (2D VBS) model provides their volatility distribution. The HOM yield decreases with temperature from 6.2 % at 25 ∘C to 0.7 % at −50 ∘C. However, there is a strong reduction of the saturation vapor pressure of each oxidation state as the temperature is reduced. Overall, the reduction in volatility with temperature leads to an increase in the nucleation rates by up to 3 orders of magnitude at −50 ∘C compared with 25 ∘C. In addition, the enhancement of the nucleation rates by ions decreases with decreasing temperature, since the neutral molecular clusters have increased stability against evaporation. The resulting data quantify how the interplay between the temperature-dependent oxidation pathways and the associated vapor pressures affect biogenic NPF at the molecular level. Our measurements, therefore, improve our understanding of pure biogenic NPF for a wide range of tropospheric temperatures and precursor concentrations.

Description: The required reliability of wind turbine gearboxes increases the requirements for large gear measurements. Extensive measurements to reliably assess the geometry of large gears in the single micrometer range are necessary. Due to an individually fixed measuring volume, standard methods like coordinate and gear measuring instruments reach their limits for large gears with diameters 〉 1 m. Therefore, a scalable optical measurement approach consisting of a single sensor in combination with a rotary table for multi-distance measurements with subsequent model-based evaluation of shape parameters of gears is presented. The scalable measurement approach is to be extended to a multisensory system in further work. As a fundamental shape parameter the mean base circle radius using the example of spur gears is determined. The base circle radius is used due to the geometric relationship to further shape parameters for example to the profile slope deviation. The theoretically achievable measurement uncertainty of the mean base circle radius due to sensor noise is estimated to less than 5 µm (k=2) for a small and a large gear, which verifies the scalability of the sensor system. In order to show a general proof of principle, two series of optical measurements on a gear with a diameter of 0.105 m are performed and referenced with a tactile measurement. As a result, random errors of 1.2 µm for k=2 are determined. The remaining systematic deviations to the reference value amount to 4.3 and 1.6 µm, respectively. Hence, the total measurement uncertainty is currently limited by systematic effects, and the defined aim of a total uncertainty of less than 5 µm (k=2) is narrowly missed by 1.5 µm. The random errors of 1.2 µm (k=2) show, however, that an adequate measurement precision is achieved and that the multi-distance measurement approach has the potential to reach the aimed measurement uncertainty with appropriate strategies to compensate for the systematic influences. The experimental and theoretical results prove the principle applicability of the proposed single sensor multi-distance approach for the precise inspection of gears.