The Impact of Primary Marine Aerosol on Atmospheric Chemistry Radiation and Climate

2011 ◽  
Author(s):  
Michael Smither Long
Keyword(s):  
Atmospheric Chemistry ◽  
Marine Aerosol ◽  
The Impact

scholarly journals Application of random forest regression to the calculation of gas-phase chemistry within the GEOS-Chem chemistry model v10

2019 ◽  
Vol 12 (3) ◽  
pp. 1209-1225 ◽  
Author(s):  
Christoph A. Keller ◽  
Mat J. Evans
Keyword(s):  
Machine Learning ◽  
Random Forest ◽  
Gas Phase ◽  
Atmospheric Chemistry ◽  
Random Forest Regression ◽  
Data Set ◽  
Gas Phase Chemistry ◽  
Chemical Conditions ◽  
Phase Chemistry ◽  
The Impact

Abstract. Atmospheric chemistry models are a central tool to study the impact of chemical constituents on the environment, vegetation and human health. These models are numerically intense, and previous attempts to reduce the numerical cost of chemistry solvers have not delivered transformative change. We show here the potential of a machine learning (in this case random forest regression) replacement for the gas-phase chemistry in atmospheric chemistry transport models. Our training data consist of 1 month (July 2013) of output of chemical conditions together with the model physical state, produced from the GEOS-Chem chemistry model v10. From this data set we train random forest regression models to predict the concentration of each transported species after the integrator, based on the physical and chemical conditions before the integrator. The choice of prediction type has a strong impact on the skill of the regression model. We find best results from predicting the change in concentration for long-lived species and the absolute concentration for short-lived species. We also find improvements from a simple implementation of chemical families (NOx = NO + NO2). We then implement the trained random forest predictors back into GEOS-Chem to replace the numerical integrator. The machine-learning-driven GEOS-Chem model compares well to the standard simulation. For ozone (O3), errors from using the random forests (compared to the reference simulation) grow slowly and after 5 days the normalized mean bias (NMB), root mean square error (RMSE) and R2 are 4.2 %, 35 % and 0.9, respectively; after 30 days the errors increase to 13 %, 67 % and 0.75, respectively. The biases become largest in remote areas such as the tropical Pacific where errors in the chemistry can accumulate with little balancing influence from emissions or deposition. Over polluted regions the model error is less than 10 % and has significant fidelity in following the time series of the full model. Modelled NOx shows similar features, with the most significant errors occurring in remote locations far from recent emissions. For other species such as inorganic bromine species and short-lived nitrogen species, errors become large, with NMB, RMSE and R2 reaching >2100 % >400 % and <0.1, respectively. This proof-of-concept implementation takes 1.8 times more time than the direct integration of the differential equations, but optimization and software engineering should allow substantial increases in speed. We discuss potential improvements in the implementation, some of its advantages from both a software and hardware perspective, its limitations, and its applicability to operational air quality activities.

scholarly journals Analysis of actinic flux profiles measured from an ozonesonde balloon

2015 ◽  
Vol 15 (8) ◽  
pp. 4131-4144 ◽  
Author(s):  
P. Wang ◽  
M. Allaart ◽  
W. H. Knap ◽  
P. Stammes
Keyword(s):  
Atmospheric Chemistry ◽  
Low Cost ◽  
Green Light ◽  
Single Layer ◽  
Radiative Transfer Model ◽  
Cloud Base ◽  
Transfer Model ◽  
Actinic Flux ◽  
Clear Sky ◽  
The Impact

Abstract. A green light sensor has been developed at KNMI to measure actinic flux profiles using an ozonesonde balloon. In total, 63 launches with ascending and descending profiles were performed between 2006 and 2010. The measured uncalibrated actinic flux profiles are analysed using the Doubling–Adding KNMI (DAK) radiative transfer model. Values of the cloud optical thickness (COT) along the flight track were taken from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) Cloud Physical Properties (CPP) product. The impact of clouds on the actinic flux profile is evaluated on the basis of the cloud modification factor (CMF) at the cloud top and cloud base, which is the ratio between the actinic fluxes for cloudy and clear-sky scenes. The impact of clouds on the actinic flux is clearly detected: the largest enhancement occurs at the cloud top due to multiple scattering. The actinic flux decreases almost linearly from cloud top to cloud base. Above the cloud top the actinic flux also increases compared to clear-sky scenes. We find that clouds can increase the actinic flux to 2.3 times the clear-sky value at cloud top and decrease it to about 0.05 at cloud base. The relationship between CMF and COT agrees well with DAK simulations, except for a few outliers. Good agreement is found between the DAK-simulated actinic flux profiles and the observations for single-layer clouds in fully overcast scenes. The instrument is suitable for operational balloon measurements because of its simplicity and low cost. It is worth further developing the instrument and launching it together with atmospheric chemistry composition sensors.

scholarly journals Multi-model study of mercury dispersion in the atmosphere: Vertical distribution of mercury species

2016 ◽  
Author(s):  
Johannes Bieser ◽  
Franz Slemr ◽  
Jesse Ambrose ◽  
Carl Brenninkmeijer ◽  
Steve Brooks ◽  
...  
Keyword(s):  
Vertical Distribution ◽  
Atmospheric Chemistry ◽  
Lower Troposphere ◽  
Elemental Mercury ◽  
Mercury Species ◽  
Substantial Impact ◽  
Model Studies ◽  
Model Study ◽  
The Impact ◽  
The Vertical Distribution

Abstract. Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model inter-comparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground based observations of mercury concentration and deposition, here we investigate the vertical distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on inter-continental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including inter-hemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury (RM) patterns depending on altitude. High RM concentrations in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parametrizations in the chemistry transport models also proved to have a substantial impact on model results.

scholarly journals Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans
Keyword(s):  
Rate Constant ◽  
Atmospheric Chemistry ◽  
Rate Constants ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Photolysis Rates ◽  
The Impact ◽  
Chemical Rate

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.

scholarly journals Atmospheric Mercury Concentrations observed at ground-based monitoring sites globally distributed in the framework of the GMOS network

2016 ◽  
Author(s):  
Francesca Sprovieri ◽  
Nicola Pirrone ◽  
Mariantonia Bencardino ◽  
Francesco D’Amore ◽  
Francesco Carbone ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Ad Hoc ◽  
Temporal Trends ◽  
Global Scale ◽  
Atmospheric Mercury ◽  
Global Network ◽  
Observation System ◽  
Large Network ◽  
Deposition Processes ◽  
The Impact

Abstract. Long-term monitoring data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) project was funded by the European Commission (www.gmos.eu), and started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad-hoc periodic oceanographic cruises and measurement flights in the lower and upper troposphere, as well as in the lower stratosphere. To date more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide in the framework of the GMOS project (2010–2015), analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted in this paper include a clear gradient of Hg concentrations between the Northern and Southern Hemisphere, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both.

scholarly journals Case studies of the impact of orbital sampling on stratospheric trend detection and derivation of tropical vertical velocities: solar occultation vs. limb emission sounding

2016 ◽  
Vol 16 (18) ◽  
pp. 11521-11534 ◽  
Author(s):  
Luis F. Millán ◽  
Nathaniel J. Livesey ◽  
Michelle L. Santee ◽  
Jessica L. Neu ◽  
Gloria L. Manney ◽  
...  
Keyword(s):  
Case Studies ◽  
Atmospheric Chemistry ◽  
Stratospheric Ozone ◽  
Sampling Bias ◽  
Nonuniform Sampling ◽  
Trend Detection ◽  
Trace Gas ◽  
Uniform Sampling ◽  
Solar Occultation ◽  
The Impact

Abstract. This study investigates the representativeness of two types of orbital sampling applied to stratospheric temperature and trace gas fields. Model fields are sampled using real sampling patterns from the Aura Microwave Limb Sounder (MLS), the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The MLS sampling acts as a proxy for a dense uniform sampling pattern typical of limb emission sounders, while HALOE and ACE-FTS represent coarse nonuniform sampling patterns characteristic of solar occultation instruments. First, this study revisits the impact of sampling patterns in terms of the sampling bias, as previous studies have done. Then, it quantifies the impact of different sampling patterns on the estimation of trends and their associated detectability. In general, we find that coarse nonuniform sampling patterns may introduce non-negligible errors in the inferred magnitude of temperature and trace gas trends and necessitate considerably longer records for their definitive detection. Lastly, we explore the impact of these sampling patterns on tropical vertical velocities derived from stratospheric water vapor measurements. We find that coarse nonuniform sampling may lead to a biased depiction of the tropical vertical velocities and, hence, to a biased estimation of the impact of the mechanisms that modulate these velocities. These case studies suggest that dense uniform sampling such as that available from limb emission sounders provides much greater fidelity in detecting signals of stratospheric change (for example, fingerprints of greenhouse gas warming and stratospheric ozone recovery) than coarse nonuniform sampling such as that of solar occultation instruments.

scholarly journals Sensitivity of modeled atmospheric nitrogen species to variations in sea salt emissions in the North and Baltic Sea regions

2015 ◽  
Vol 15 (20) ◽  
pp. 29705-29745
Author(s):  
D. Neumann ◽  
V. Matthias ◽  
J. Bieser ◽  
A. Aulinger ◽  
M. Quante
Keyword(s):  
Baltic Sea ◽  
Atmospheric Chemistry ◽  
Surf Zone ◽  
Fine Particles ◽  
Measurement Data ◽  
Monitoring And Evaluation ◽  
Sea Salt ◽  
The North ◽  
A Minor ◽  
The Impact

Abstract. Coarse sea salt particles are emitted ubiquitously from the oceans' surfaces by wave breaking and bubble bursting processes. These particles impact atmospheric chemistry by affecting condensation of gas-phase species and nucleation of new fine particles, particularly in regions with high air pollution. In this study, atmospheric particle concentrations are modeled for the North and Baltic Sea regions, Northwestern Europe, using the Community Multiscale Air Quality (CMAQ) modeling system and evaluated against European Monitoring and Evaluation Programme (EMEP) measurement data. As model extension, sea salt emissions are scaled by water salinity because of low salinity in large parts of the Baltic Sea and in certain river estuaries. The resulting improvement in predicted sea salt concentrations is assessed. The contribution of surf zone emissions is separately considered. Additionally, the impact of sea salt particles on atmospheric nitrate, ammonium and sulfate concentrations is evaluated. The comparisons show that sea salt concentrations are commonly overestimated at coastal stations and partly underestimated when going inland. The introduced salinity scaling improves predicted Baltic Sea sea salt concentrations considerably. Dates of measured peak concentrations are appropriately reproduced by the model. The impact of surf zone emissions is negligible in both seas. Nevertheless, they might be relevant because surf zone emissions were cut at an upper threshold in this study. Deactivating sea salt leads to a minor increase of NH4+ and NO3- and a minor decrease of SO42- concentrations. However, the overall effect is very low and lower than the deviation from measurements. Size resolved measurements of Na+, NH4+, NO3-, and SO42- are needed for a more detailed analysis on the impact of sea salt particles.

scholarly journals Model – TCCON comparisons of column-averaged methane with a focus on the stratosphere

2016 ◽  
Author(s):  
Andreas Ostler ◽  
Ralf Sussmann ◽  
Prabir K. Patra ◽  
Sander Houweling ◽  
Marko De Bruine ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Meteorological Data ◽  
Michelson Interferometer ◽  
Total Carbon ◽  
Data Sets ◽  
Transport Models ◽  
Improved Model ◽  
The Impact ◽  
Chemistry Experiment

Abstract. The distribution of methane (CH4) in the stratosphere can be a major driver of spatial variability in the dry-air column-averaged CH4 mixing ratio (XCH4), which is being measured increasingly for the assessment of CH4 surface emissions. Chemistry-transport models (CTMs) therefore need to simulate the tropospheric and stratospheric fractional columns of XCH4 accurately for estimating surface emissions from XCH4. Simulations from three CTMs are tested against XCH4 observations from the Total Carbon Column Network (TCCON). We analyze how the model-TCCON agreement in XCH4 depends on the model representation of stratospheric CH4 distributions. Model equivalents of TCCON XCH4 are computed with stratospheric CH4 fields from both the model simulations and from satellite-based CH4 distributions from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and MIPAS CH4 fields adjusted to ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. In comparison to simulated model fields we find an improved model-TCCON XCH4 agreement for all models with MIPAS-based stratospheric CH4 fields. For the Atmospheric Chemistry Transport Model (ACTM) the average XCH4 bias is significantly reduced from 38.1 ppb to 13.7 ppb, whereas small improvements are found for the models TM5 (Transport Model, version 5; from 8.7 ppb to 4.3 ppb), and LMDz (Laboratoire de Météorologie Dynamique model with Zooming capability; from 6.8 ppb to 4.3 ppb), respectively. MIPAS stratospheric CH4 fields adjusted to ACE-FTS reduce the average XCH4 bias for ACTM (3.3 ppb), but increase the average XCH4 bias for TM5 (10.8 ppb) and LMDz (20.0 ppb). These findings imply that the range of satellite-based stratospheric CH4 is insufficient to resolve a possible stratospheric contribution to differences in total column CH4 between TCCON and TM5 or LMDz. Applying transport diagnostics to the models indicates that model-to-model differences in the simulation of stratospheric transport, notably the age of stratospheric air, can largely explain the inter-model spread in stratospheric CH4 and, hence, its contribution to XCH4. This implies that there is a need to better understand the impact of individual model transport components (e.g., physical parameterization, meteorological data sets, model horizontal/vertical resolution) on modeled stratospheric CH4.

scholarly journals Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: results from the EFEU campaign

2007 ◽  
Vol 7 (4) ◽  
pp. 12657-12686 ◽  
Author(s):  
K. Hungershöfer ◽  
K. Zeromskiene ◽  
Y. Iinuma ◽  
G. Helas ◽  
J. Trentmann ◽  
...  
Keyword(s):  
Optical Properties ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Absorption Efficiency ◽  
Max Planck ◽  
Fresh Biomass ◽  
Biomass Burning Aerosol ◽  
Smoke Chamber ◽  
The Impact ◽  
Mass Absorption Efficiency

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the 'Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere' (EFEU) project. Using the measured size distributions as well as mass scattering and absorption efficiencies, Mie calculations provided mean effective refractive indices of 1.60−0.010i and 1.56−0.010i (λ=0.55 μm) for smoke particles emitted from the combustion of savanna grass and an African hardwood (musasa), respectively. The relatively low imaginary parts suggest that the light-absorbing carbon of the investigated fresh biomass burning aerosol is only partly graphitized, resulting in strongly scattering and less absorbing particles. While the observed variability in mass scattering efficiencies was consistent with changes in particle size, the changes in the mass absorption efficiency can only be explained, if the chemical composition of the particles varies with combustion conditions.

scholarly journals New Results on the Composition of the Outer Planets and Titan

2005 ◽  
Vol 13 ◽  
pp. 891-893
Author(s):  
Thierry Fouchet
Keyword(s):  
Solar System ◽  
Atmospheric Chemistry ◽  
Recent Progress ◽  
Giant Planets ◽  
Atmospheric Composition ◽  
Solar System Formation ◽  
Outer Planets ◽  
System Formation ◽  
The Impact

AbstractIn this brief summary, I present recent progress on our knowledge of the Giant Planets and Titan atmospheric composition, as well as the impact of this progress on our understanding of Solar System formation, and atmospheric chemistry.

Sign in / Sign up

Export Citation Format

Share Document