We introduce and evaluate aerosol simulations with the global aerosol–climate model ECHAM6.3–HAM2.3, which is the aerosol component of the fully coupled aerosol–chemistry–climate model ECHAM–HAMMOZ. ...Both the host atmospheric climate model ECHAM6.3 and the aerosol model HAM2.3 were updated from previous versions. The updated version of the HAM aerosol model contains improved parameterizations of aerosol processes such as cloud activation, as well as updated emission fields for anthropogenic aerosol species and modifications in the online computation of sea salt and mineral dust aerosol emissions. Aerosol results from nudged and free-running simulations for the 10-year period 2003 to 2012 are compared to various measurements of aerosol properties. While there are regional deviations between the model and observations, the model performs well overall in terms of aerosol optical thickness, but may underestimate coarse-mode aerosol concentrations to some extent so that the modeled particles are smaller than indicated by the observations. Sulfate aerosol measurements in the US and Europe are reproduced well by the model, while carbonaceous aerosol species are biased low. Both mineral dust and sea salt aerosol concentrations are improved compared to previous versions of ECHAM–HAM. The evaluation of the simulated aerosol distributions serves as a basis for the suitability of the model for simulating aerosol–climate interactions in a changing climate.
The export of organic matter from ocean to atmosphere represents a substantial carbon flux in the Earth system, yet the impact of environmental drivers on this transfer is not fully understood. This ...work presents dissolved and particulate organic carbon (DOC, POC) concentrations, their enrichment factors in the sea surface microlayer (SML), and equivalent measurements in marine aerosol particles across the Atlantic Ocean. DOC concentrations averaged 161 ± 139 µmol L–1 (n = 78) in bulk seawater and 225 ± 175 µmol L–1 (n = 79) in the SML; POC concentrations averaged 13 ± 11 µmol L–1 (n = 80) and 17 ± 10 µmol L–1 (n = 80), respectively. High DOC and POC enrichment factors were observed when samples had low concentrations, and lower enrichments when concentrations were high. The impacts of wind speed and chlorophyll-a levels on concentrations and enrichment of DOC and POC in seawater were insignificant. In ambient submicron marine aerosol particles the concentration of water-soluble organic carbon was approximately 0.2 µg m–3. Water-insoluble organic carbon concentrations varied between 0.01 and 0.9 µg m–3, with highest concentrations observed when chlorophyll-a concentrations were high. Concerted measurements of bulk seawater, the SML and aerosol particles enabled calculation of enrichment factors of organic carbon in submicron marine ambient aerosols, which ranged from 103 to 104 during periods of low chlorophyll-a concentrations and up to 105 when chlorophyll-a levels were high. The results suggest that elevated local biological activity enhances the enrichment of marine-sourced organic carbon on aerosol particles. However, implementation of the results in source functions based on wind speed and chlorophyll-a concentrations underestimated the organic fraction at low biological activity by about 30%. There may be additional atmospheric and oceanic parameters to consider for accurately predicting organic fractions on aerosol particles.
In this paper we systematically analyze the electronic structures of polar and nonpolar wurtzite-InN/GaN quantum dots and their modification due to the quantum-confined Stark effect caused by ...intrinsic fields. This is achieved by combining continuum elasticity theory with an effective-bond orbital model to describe the elastic and single-particle electronic properties in these nitride systems. Based on these results, a many-body treatment is used to determine optical absorption spectra. The efficiency of optical transitions depends on the interplay between the Coulomb interaction and the quantum-confined Stark effect. We introduce an effective confinement potential which represents the electronic structure under the influence of the intrinsic polarization fields and calculate the needed strength of Coulomb interaction to diminish the separation of electrons and holes.
Sea spray aerosol particle is a dominating part of the global aerosol mass load of natural origin. Thus, it strongly influences the atmospheric radiation balance and cloud properties especially over ...the oceans. Uncertainties of the estimated climate impacts by this aerosol type are partly caused by the uncertainties in the particle size dependent emission fluxes of sea spray aerosol particle. We present simulations with a regional aerosol transport model system in two domains, for three months and compared the model results to measurements at four stations using various sea spray aerosol particle source source functions. Despite these limitations we found the results using different source functions are within the range of most model uncertainties. Especially the model's ability to produce realistic wind speeds is crucial. Furthermore, the model results are more affected by a function correcting the emission flux for the effect of the sea surface temperature than by the use of different source functions.
•Effect of SST can be higher than differences between source functions.•Differences between source functions can be smaller than current uncertainties.•Main uncertainty is model performance of surface wind speed.
Nanostructures with open shell transition metal or molecular constituents host often strong electronic correlations and are highly sensitive to atomistic material details. This tutorial review ...discusses method developments and applications of theoretical approaches for the realistic description of the electronic and magnetic properties of nanostructures with correlated electrons. First, the implementation of a flexible interface between density functional theory and a variant of dynamical mean field theory (DMFT) highly suitable for the simulation of complex correlated structures is explained and illustrated. On the DMFT side, this interface is largely based on recent developments of quantum Monte Carlo and exact diagonalization techniques allowing for efficient descriptions of general four fermion Coulomb interactions, reduced symmetries and spin-orbit coupling, which are explained here. With the examples of the Cr (001) surfaces, magnetic adatoms, and molecular systems it is shown how the interplay of Hubbard
U
and Hund’s
J
determines charge and spin fluctuations and how these interactions drive different sorts of correlation effects in nanosystems. Non-local interactions and correlations present a particular challenge for the theory of low dimensional systems. We present our method developments addressing these two challenges, i.e., advancements of the dynamical vertex approximation and a combination of the constrained random phase approximation with continuum medium theories. We demonstrate how non-local interaction and correlation phenomena are controlled not only by dimensionality but also by coupling to the environment which is typically important for determining the physics of nanosystems.
The project MarParCloud (Marine biological production, organic
aerosol Particles and marine Clouds: a process
chain) aims to improve our understanding of the genesis, modification and
impact of ...marine organic matter (OM) from its biological production, to
its export to marine aerosol particles and, finally, to its ability to
act as ice-nucleating particles (INPs) and cloud condensation nuclei (CCN). A
field campaign at the Cape Verde Atmospheric Observatory (CVAO) in the
tropics in September–October 2017 formed the core of this project that was
jointly performed with the project MARSU (MARine atmospheric
Science Unravelled). A suite of chemical,
physical, biological and meteorological techniques was applied, and
comprehensive measurements of bulk water, the sea surface microlayer (SML),
cloud water and ambient aerosol particles collected at a ground-based and a
mountain station took place. Key variables comprised the chemical characterization of the atmospherically
relevant OM components in the ocean and the atmosphere as well as
measurements of INPs and CCN. Moreover, bacterial cell counts, mercury
species and trace gases were analyzed. To interpret the results, the
measurements were accompanied by various auxiliary parameters such as air
mass back-trajectory analysis, vertical atmospheric profile analysis, cloud
observations and pigment measurements in seawater. Additional modeling
studies supported the experimental analysis. During the campaign, the CVAO exhibited marine air masses with low and
partly moderate dust influences. The marine boundary layer was well mixed as
indicated by an almost uniform particle number size distribution within the
boundary layer. Lipid biomarkers were present in the aerosol particles in
typical concentrations of marine background conditions. Accumulation- and
coarse-mode particles served as CCN and were efficiently transferred to the
cloud water. The ascent of ocean-derived compounds, such as sea salt and
sugar-like compounds, to the cloud level, as derived from chemical analysis
and atmospheric transfer modeling results, denotes an influence of marine
emissions on cloud formation. Organic nitrogen compounds (free amino acids)
were enriched by several orders of magnitude in submicron aerosol particles
and in cloud water compared to seawater. However, INP measurements also indicated
a significant contribution of other non-marine sources to the local INP
concentration, as (biologically active) INPs were mainly present in
supermicron aerosol particles that are not suggested to undergo strong
enrichment during ocean–atmosphere transfer. In addition, the number of CCN
at the supersaturation of 0.30 % was about 2.5 times higher during dust
periods compared to marine periods. Lipids, sugar-like compounds, UV-absorbing (UV: ultraviolet) humic-like substances and low-molecular-weight neutral components
were important organic compounds in the seawater, and highly surface-active
lipids were enriched within the SML. The selective enrichment of specific
organic compounds in the SML needs to be studied in further detail and
implemented in an OM source function for emission modeling to better
understand transfer patterns, the mechanisms of marine OM transformation in the
atmosphere and the role of additional sources. In summary, when looking at particulate mass, we see oceanic compounds
transferred to the atmospheric aerosol and to the cloud level, while from a
perspective of particle number concentrations, sea spray aerosol (i.e.,
primary marine aerosol) contributions to both CCN and INPs are rather
limited.
Sea salt aerosol (SSA) is one of the major components of primary aerosols and has significant impact on the formation of secondary inorganic particles mass on a global scale. In this study, the fully ...online coupled WRF-Chem model was utilized to evaluate the SSA emission scheme and its influence on the nitrate simulation in a case study in Europe during 10–20 September 2013. Meteorological conditions near the surface, wind pattern and thermal stratification structure were well reproduced by the model. Nonetheless, the coarse-mode (PM1 − 10) particle mass concentration was substantially overestimated due to the overestimation of SSA and nitrate. Compared to filter measurements at four EMEP stations (coastal stations: Bilthoven, Kollumerwaard and Vredepeel; inland station: Melpitz), the model overestimated SSA concentrations by a factor of 8–20. We found that this overestimation was mainly caused by overestimated SSA emissions over the North Sea during 16–20 September. Over the coastal regions, SSA was injected into the continental free troposphere through an “aloft bridge” (about 500 to 1000 m above the ground), a result of the different thermodynamic properties and planetary boundary layer (PBL) structure between continental and marine regions. The injected SSA was further transported inland and mixed downward to the surface through downdraft and PBL turbulence. This process extended the influence of SSA to a larger downwind region, leading, for example, to an overestimation of SSA at Melpitz, Germany, by a factor of ∼ 20. As a result, the nitrate partitioning fraction (ratio between particulate nitrate and the summation of particulate nitrate and gas-phase nitric acid) increased by about 20 % for the coarse-mode nitrate due to the overestimation of SSA at Melpitz. However, no significant difference in the partitioning fraction for the fine-mode nitrate was found. About 140 % overestimation of the coarse-mode nitrate resulted from the influence of SSA at Melpitz. In contrast, the overestimation of SSA inhibited the nitrate particle formation in the fine mode by about 20 % because of the increased consumption of precursor by coarse-mode nitrate formation.
Hydrogen adatoms and other species covalently bound to graphene act as resonant scattering centers affecting the electronic transport properties and inducing Anderson localization. We show that ...attractive interactions between adatoms on graphene and their diffusion mobility strongly modify the spatial distribution, thus fully eliminating isolated adatoms and increasing the population of larger size adatom aggregates. Such spatial correlation is found to strongly influence the electronic transport properties of disordered graphene. Our scaling analysis shows that such aggregation of adatoms increases conductance by up to several orders of magnitude and results in significant extension of the Anderson localization length in the strong localization regime. We introduce a simple definition of the effective adatom concentration x*, which describes the transport properties of both random and correlated distributions of hydrogen adatoms on graphene across a broad range of concentrations.
Diluted magnetic semiconductors (DMS) like Ga
1−
x
Mn
x
As are described by a realistic tight-binding model (TBM) for the (valence) bands of GaAs, by a Zener (
J
-)term modeling the coupling of the ...localized Mn-spins to the spins of the valence band electrons, and by an additional potential scattering (
V
-) term due to the Mn-impurities. We calculate the effective (Heisenberg) exchange interaction between two Mn-moments mediated by the valence electrons. The influence of the number of bands taken into account (6-band or 8-band TBM) and of the potential (impurity) scattering
V
-term is investigated. We find that for realistic values of the parameters the indirect exchange integrals show a long-range, oscillating (RKKY-like) behavior, if the
V
-term is neglected, probably leading to spin-glass behavior rather than magnetic order. But by including a
V
-term of a realistic magnitude the exchange couplings become short ranged and mainly positive allowing for the possibility of ferromagnetic order. Our results are in good agreement with available results of ab initio treatments.
PDF
