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We analyze present-day and future carbon monoxide (CO) simulations in 26 state-of-the-art atmospheric chemistry models run to study future air quality and climate change. In comparison with near-global satellite observations from the MOPITT instrument and local surface measurements, the models show large underestimates of Northern Hemisphere (NH) extratropical CO, while typically performing reasonably well elsewhere. The results suggest that year-round emissions, probably from fossil fuel burning in east Asia and seasonal biomass burning emissions in south-central Africa, are greatly underestimated in current inventories such as IIASA and EDGAR3.2. Variability among models is large, likely resulting primarily from intermodel differences in representations and emissions of nonmethane volatile organic compounds (NMVOCs) and in hydrologic cycles, which affect OH and soluble hydrocarbon intermediates. Global mean projections of the 2030 CO response to emissions changes are quite robust. Global mean midtropospheric (500 hPa) CO increases by 12.6 ± 3.5 ppbv (16%) for the high-emissions (A2) scenario, by 1.7 ± 1.8 ppbv (2%) for the midrange (CLE) scenario, and decreases by 8.1 ± 2.3 ppbv (11%) for the low-emissions (MFR) scenario. Projected 2030 climate changes decrease global 500 hPa CO by 1.4 ± 1.4 ppbv. Local changes can be much larger. In response to climate change, substantial effects are seen in the tropics, but intermodel variability is quite large. The regional CO responses to emissions changes are robust across models, however. These range from decreases of 10–20 ppbv over much of the industrialized NH for the CLE scenario to CO increases worldwide and year-round under A2, with the largest changes over central Africa (20–30 ppbv), southern Brazil (20–35 ppbv) and south and east Asia (30–70 ppbv). The trajectory of future emissions thus has the potential to profoundly affect air quality over most of the world's populated areas.

Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing "optimistic," "likely," and "pessimistic" options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of -50, 180, and 300 mW m-2, compared to a CO2 forcing over the same time period of 800-1100 mW m-2. These values indicate the importance of air pollution emissions in short- to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%. The ensemble mean year 2000 tropospheric ozone budget indicates chemical production, chemical destruction, dry deposition and stratospheric input fluxes of 5100, 4650, 1000 and 550 Tg(O3) yr-1, respectively. These values are significantly different to the mean budget documented by the Intergovernmental Panel on Climate Change (IPCC) Third Assessment Report (TAR). The mean ozone burden (340 Tg(O3)) is 10% larger than the IPCC TAR estimate, while the mean ozone lifetime (22 days) is 10% shorter. Results from individual models show a correlation between ozone burden and lifetime, and each model's ozone burden and lifetime respond in similar ways across the emissions scenarios. The response to climate change is much less consistent. Models show more variability in the tropics compared to midlatitudes. Some of the most uncertain areas of the models include treatments of deep tropical convection, including lightning NOx production; isoprene emissions from vegetation and isoprene's degradation chemistry; stratosphere-troposphere exchange; biomass burning; and water vapor concentrations. Copyright 2006 by the American Geophysical Union.

The Hamburg Aerosol Module version 2.3 (HAM2.3) from the ECHAM6.3‐HAM2.3 global atmosphere‐aerosol model is coupled to the recently developed icosahedral nonhydrostatic ICON‐A (icon‐aes‐1.3.00) global atmosphere model to yield the new ICON‐A‐HAM2.3 atmosphere‐aerosol model. The ICON‐A and ECHAM6.3 host models use different dynamical cores, parameterizations of vertical mixing due to sub‐grid scale turbulence, and parameter settings for radiation balance tuning. Here, we study the role of the different host models for simulated aerosol optical thickness (AOT) and evaluate impacts of using HAM2.3 and the ECHAM6‐HAM2.3 two‐moment cloud microphysics scheme on several meteorological variables. Sensitivity runs show that a positive AOT bias over the subtropical oceans is remedied in ICON‐A‐HAM2.3 because of a different default setting of a parameter in the moist convection parameterization of the host models. The global mean AOT is biased low compared to MODIS satellite instrument retrievals in ICON‐A‐HAM2.3 and ECHAM6.3‐HAM2.3, but the bias is larger in ICON‐A‐HAM2.3 because negative AOT biases over the Amazon, the African rain forest, and the northern Indian Ocean are no longer compensated by high biases over the sub‐tropical oceans. ICON‐A‐HAM2.3 shows a moderate improvement with respect to AOT observations at AERONET sites. A multivariable bias score combining biases of several meteorological variables into a single number is larger in ICON‐A‐HAM2.3 compared to standard ICON‐A and standard ECHAM6.3. In the tropics, this multivariable bias is of similar magnitude in ICON‐A‐HAM2.3 and in ECHAM6.3‐HAM2.3. In the extra‐tropics, a smaller multivariable bias is found for ICON‐A‐HAM2.3 than for ECHAM6.3‐HAM2.3. Plain Language Summary: Aerosols are tiny particles in the air which are either emitted into the atmosphere directly or formed from precursor gases such as sulfur dioxide. Aerosols reflect and absorb solar radiation and affect the radiative properties of clouds. In order to estimate how changing emissions of aerosol precursor gases and aerosols affect the radiation budget of the atmosphere, aerosol models are coupled to global atmosphere models. Here, an aerosol model that has already been part of a well‐established coupled model is coupled to a recently developed atmosphere model. The reasons for differences between the original and the new model are investigated and simulated aerosol optical thickness is evaluated against observations. The aerosol optical thickness over subtropical oceans is lower in the new model, which is in better agreement with estimates from satellite observations. This better agreement is traced back to a parameter setting in the cloud description part in the new model. However, because cancellation of positive and negative biases is reduced in the new model, the global mean aerosol optical thickness is biased lower the new model. A bias score based on several meteorological variables is lower in the new model because of lower biases in the extra‐tropics. Key Points: The new ICON‐A‐Hamburg Aerosol Module version 2.3 (HAM2.3) global atmosphere‐aerosol model is introducedThe sensitivity of simulated aerosol optical thickness (AOT) to using two different host models but the same aerosol module is investigatedA positive AOT bias over subtropical oceans is remedied in ICON‐A‐HAM2.3 because of a different parameter setting in the host model [ABSTRACT FROM AUTHOR]

Nuclear magnetic relaxation dispersion (NMRD) of the (CH3)(sub 4)N(super +) proton spins is employed for determining the relative motion of a tetramethylammonium (CH3)(sub 4)N(super +) ion with respect to a Gd(super 3+) octoaqua complex, along with the quantum dynamics of the electron spin of the lanthanide. It was seen that the measured proton resonance frequencies range between 10 and 800 megahertz (MHz), whereas a pronounced maximum was observed at around 90 MHz.

Recent advances in the design of fast field cycling (FFC) relaxometers make it now possible to explore the nuclear magnetic relaxation dispersion (NMRD) of semidilute nuclei with short relaxation times. The paramagnetic relaxation rate enhancement of the protons of the tetramethylammonium (CH[sub 3])[sub 4]N[sup +] cation due to the intermolecular magnetic dipolar coupling with the electronic spin S=7/2 of [Gd(D[sub 2]O)[sub 8]][sup 3+] in heavy water has been measured between 10 kHz and 800 MHz by combining FFC and standard relaxation techniques. In order to interpret the complete paramagnetic NMRD profile, particularly in the low field region, two previously neglected features are taken into account: (i) The evolution beyond the Redfield limit of the electronic relaxation of the spin S is obtained from accurate Monte Carlo simulations. (ii) The time fluctuation of the static zero field splitting (ZFS) is attributed not only to the usual global Brownian rotational diffusion of the complex, but also to the rearrangement of the water molecules in the first hydration shell of the Gd[sup 3+] ion via 90° pseudorotations [Th. Kowall et al., J. Phys. Chem. 99, 13078 (1995)]. To calculate the longitudinal electronic relaxation function G[sub ∥](t) of the Gd[sup 3+] ion, its static and transient ZFS parameters in the aqua complex as well as the correlation times of the Brownian rotation and vibrations of this complex are needed. We use the values of these parameters derived from an independent multiple frequency and temperature study of the full electronic paramagnetic resonance spectra of Gd[sup 3+] in light water H[sub 2]O, for magnetic fields where the Redfield limit applies. The predicted NMRD profile is in excellent global agreement with experiment over the whole proton frequency range, especially if the correlation times governing the rotational dynamics of the aqua complex are slightly increased to account for the higher viscosity of D[sub 2]O with respect to H[sub 2]O. © 2003 American Institute of Physics. [ABSTRACT FROM AUTHOR]

The time correlation functions of the electronic spin components of a metal ion without orbital degeneracy in solution are computed. The approach is based on the numerical solution of the time-dependent Schro¨dinger equation for a stochastic perturbing Hamiltonian which is simulated by a Monte Carlo algorithm using discrete time steps. The perturbing Hamiltonian is quite general, including the superposition of both the static mean crystal field contribution in the molecular frame and the usual transient ligand field term. The Hamiltonian of the static crystal field can involve the terms of all orders, which are invariant under the local group of the average geometry of the complex. In the laboratory frame, the random rotation of the complex is the only source of modulation of this Hamiltonian, whereas an additional Ornstein–Uhlenbeck process is needed to describe the time fluctuations of the Hamiltonian of the transient crystal field. A numerical procedure for computing the electronic paramagnetic resonance (EPR) spectra is proposed and discussed. For the [Gd(H[sub 2]O)[sub 8]][sup 3+] octa-aqua ion and the [Gd(DOTA)(H[sub 2]O)][sup -] complex [DOTA=1,4,7,10-tetrakis(carboxymethyl)-1,4,7,10-tetraazacyclo dodecane] in water, the predictions of the Redfield relaxation theory are compared with those of the Monte Carlo approach. The Redfield approximation is shown to be accurate for all temperatures and for electronic resonance frequencies at and above X-band, justifying the previous interpretations of EPR spectra. At lower frequencies the transverse and longitudinal relaxation functions derived from the Redfield approximation display significantly faster decays than the corresponding simulated functions. The practical interest of this simulation approach is underlined. © 2001 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Abstract: We evaluate the new icosahedral nonhydrostatic atmospheric (ICON‐A) general circulation model of the Max Planck Institute for Meteorology that is flexible to be run at grid spacings from a few tens of meters to hundreds of kilometers. A simulation with ICON‐A at a low resolution (160 km) is compared to a not‐tuned fourfold higher‐resolution simulation (40 km). Simulations using the last release of the ECHAM climate model (ECHAM6.3) are also presented at two different resolutions. The ICON‐A simulations provide a compelling representation of the climate and its variability. The climate of the low‐resolution ICON‐A is even slightly better than that of ECHAM6.3. Improvements are obtained in aspects that are sensitive to the representation of orography, including the representation of cloud fields over eastern‐boundary currents, the latitudinal distribution of cloud top heights, and the spatial distribution of convection over the Indian Ocean and the Maritime Continent. Precipitation over land is enhanced, in particular at high‐resolution ICON‐A. The response of precipitation to El Niño sea surface temperature variability is close to observations, particularly over the eastern Indian Ocean. Some parameterization changes lead to improvements, for example, with respect to rain intensities and the representation of equatorial waves, but also imply a warmer troposphere, which we suggest leads to an unrealistic poleward mass shift. Many biases familiar to ECHAM6.3 are also evident in ICON‐A, namely, a too zonal SPCZ, an inadequate representation of north hemispheric blocking, and a relatively poor representation of tropical intraseasonal variability. [ABSTRACT FROM AUTHOR]

Abstract: ICON‐A is the new icosahedral nonhydrostatic (ICON) atmospheric general circulation model in a configuration using the Max Planck Institute physics package, which originates from the ECHAM6 general circulation model, and has been adapted to account for the changed dynamical core framework. The coupling scheme between dynamics and physics employs a sequential updating by dynamics and physics, and a fixed sequence of the physical processes similar to ECHAM6. To allow a meaningful initial comparison between ICON‐A and the established ECHAM6‐LR model, a setup with similar, low resolution in terms of number of grid points and levels is chosen. The ICON‐A model is tuned on the base of the Atmospheric Model Intercomparison Project (AMIP) experiment aiming primarily at a well balanced top‐of atmosphere energy budget to make the model suitable for coupled climate and Earth system modeling. The tuning addresses first the moisture and cloud distribution to achieve the top‐of‐atmosphere energy balance, followed by the tuning of the parameterized dynamic drag aiming at reduced wind errors in the troposphere. The resulting version of ICON‐A has overall biases, which are comparable to those of ECHAM6. Problematic specific biases remain in the vertical distribution of clouds and in the stratospheric circulation, where the winter vortices are too weak. Biases in precipitable water and tropospheric temperature are, however, reduced compared to the ECHAM6. ICON‐A will serve as the basis of further development and as the atmosphere component to the coupled model, ICON‐Earth system model (ESM). [ABSTRACT FROM AUTHOR]

The ECHAM6 atmospheric general circulation model is the atmosphere component of the Max Planck Institute Earth System Model (MPI-ESM) that is used in the Coupled Model Intercomparison Project Phase 5 (CMIP5) simulations. As ECHAM6 has its uppermost layer centered at 0.01 hPa in the upper mesosphere, these simulations offer the opportunity to study the middle atmosphere climate change and its relation to the troposphere on the basis of a very comprehensive set of state-of-the-art model simulations. The goals of this paper are (a) to introduce those new features of ECHAM6 particularly relevant for the middle atmosphere, including external forcing data, and (b) to evaluate the simulated middle atmosphere and describe the simulated response to natural and anthropogenic forcings. New features in ECHAM6 with respect to ECHAM5 include a new short-wave radiation scheme, the option to vary spectral irradiance independent of total solar irradiance, and a latitude-dependent gravity-wave source strength. The description of external forcing data focuses on solar irradiance and ozone. Stratospheric temperature trends simulated with the MPI-ESM for the last decades of the 20th century agree well with observations. The future projections depend strongly on the scenario. Under the high emission scenario RCP8.5, simulated temperatures are locally lower by more than 20 K than preindustrial values. Many of the simulated patterns of the responses to natural forcings as provided by solar variability, volcanic aerosols, and El Niño-Southern Oscillation, largely agree with the observations. [ABSTRACT FROM AUTHOR]

Abstract. This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation. Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker in- cloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher Ångström parameters. Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans in Ångström parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aerosol mass concentrations are very similar to those in the old version. The total aerosol water content in HAM2 is considerably closer to the multi-model average from Phase I of the AeroCom intercomparison project. Model deficiencies that require further efforts in the future include (I) positive biases in AOD over the ocean, (ii) negative biases in AOD and aerosol mass concentration in high-latitude regions, and (iii) negative biases in particle number concentration, especially that of the Aitken mode, in the lower troposphere in heavily polluted regions. [ABSTRACT FROM AUTHOR]

Clouds cool Earth's climate by reflecting 20% of the incoming solar energy, while also trapping part of the outgoing radiation. The effect of human activities on clouds is poorly understood, but the present-day anthropogenic cooling via changes of cloud albedo and lifetime could be of the same order as warming from anthropogenic addition in CO2. Soluble trace gases can increase water condensation to particles, possibly leading to activation of smaller aerosols and more numerous cloud droplets. We have studied the effect of nitric acid on the aerosol indirect effect with the global aerosol-climate model ECHAM5.5-HAM2. Including the nitric acid effect in the model increases cloud droplet number concentrations globally by 7%. The nitric acid contribution to the present-day cloud albedo effect was found to be -0.32 W m-2 and to the total indirect effect -0.46 W m-2. The contribution to the cloud albedo effect is shown to increase to -0.37 W m-2 by the year 2100, if considering only the reductions in available cloud condensation nuclei. Overall, the effect of nitric acid can play a large part in aerosol cooling during the following decades with decreasing SO2 emissions and increasing NOxand greenhouse gases. [ABSTRACT FROM AUTHOR]

The degree of non-linearity in DMS-cloud-climate interactions is assessed using the ECHAM5-HAMMOZ model by taking into account end-to-end aerosol chemistry-cloud microphysics link. The evaluation is made over the Southern oceans in austral summer, a region of minimal anthropogenic influence. In this study, we compare the DMS-derived changes in the aerosol and cloud microphysical properties between a baseline simulation with the ocean DMS emissions from a prescribed climatology, and a scenario where the DMS emissions are doubled. Our results show that doubling the DMS emissions in the current climate results in a non-linear response in atmospheric DMS burden and subsequently, in SO2 and H2SO4 burdens due to inadequate OH oxidation. The aerosol optical depth increases by only ~20% in the 30° S-75° S belt in the SH summer months. This increases the vertically integrated cloud droplet number concentrations (CDNC) by 25 %. Since the vertically integrated liquid water vapor is constant in our model simulations, an increase in CDNC leads to a reduction in cloud droplet radius of 3.4% over the Southern oceans in summer. The equivalent increase in cloud liquid water path is 10.7 %. The above changes in cloud microphysical properties result in a change in global annual mean radiative forcing at the TOA of -1.4Wm-2. The results suggest that the DMS-cloud microphysics link is highly non-linear. This has implications for future studies investigating the DMS-cloud climate feedbacks in a warming world and for studies evaluating geoengineering options to counteract warming by modulating low level marine clouds. [ABSTRACT FROM AUTHOR]

The degree of non-linearity in DMS-cloud-climate interactions is assessed using the ECHAM5-HAMMOZ model by taking into account end-to-end aerosol chemistry-cloud microphysics link. The evaluation is made over the Southern oceans in austral summer, a region of minimal anthropogenic influence. In this study, we compare the DMS-derived changes in the aerosol and cloud microphysical properties between a baseline simulation with the ocean DMS emissions from a prescribed climatology, and a scenario where the DMS emissions are doubled. Our results show that doubling the DMS emissions in the current climate results in a non-linear response in atmospheric DMS burden and subsequently, in SO2 and H2SO4 burdens due to inadequate OH oxidation. The aerosol optical depth increases by only ~20% in the 30° S-75° S belt in the SH summer months. This increases the vertically integrated cloud droplet number concentrations (CDNC) by 25 %. Since the vertically integrated liquid water vapor is constant in our model simulations, an increase in CDNC leads to a reduction in cloud droplet radius of 3.4% over the Southern oceans in summer. The equivalent increase in cloud liquid water path is 10.7 %. The above changes in cloud microphysical properties result in a change in global annual mean radiatve forcing at the TOA of -1.4 W m-2. The results suggest that the DMS-cloud microphysics link is highly non-linear. This has implications for future studies investigating the DMS-cloud climate feedbacks in a warming world and for studies evaluating geoengineering options to counteract warming by modulating low level marine clouds. [ABSTRACT FROM AUTHOR]

A noncontact atomic force microscope (nc-AFM) operating in magnetic fields up to ±7 T and liquid helium temperatures is presented in this article. In many common AFM experiments the cantilever is mounted parallel to the sample surface, while in our system the cantilever is assembled perpendicular to it; the so called pendulum mode of AFM operation. In this mode measurements employing very soft and, therefore, ultrasensitive cantilevers can be performed. The ultrahigh vacuum conditions allow to prepare and transfer cantilevers and samples in a requested manner avoiding surface contamination. We demonstrate the possibility of nc-AFM and Kelvin force probe microscopy imaging in the pendulum mode. Ultrasensitive experiments on small spin ensembles are presented as well. [ABSTRACT FROM AUTHOR]

The contribution of ocean dimethyl sulfide (DMS) emissions to changes in cloud microphysical properties is quantified seasonally and globally for present day climate conditions using an aerosol-chemistry-climate general circulation model, ECHAM5-HAMMOZ, coupled to a cloud microphysics scheme. We evaluate DMS aerosol-cloud-climate linkages over the southern oceans where anthropogenic influence is minimal. The changes in the number of activated particles, cloud droplet number concentration (CDNC), cloud droplet effective radius, cloud cover and the radiative forcing are examined by analyzing two simulations: a baseline simulation with ocean DMS emissions derived from a prescribed climatology and one in which the ocean DMS emissions are switched off. Our simulations show that the model realistically simulates the seasonality in the number of activated particles and CDNC, peaking during Southern Hemisphere (SH) summer coincident with increased phytoplankton blooms and gradually declining with a minimum in SH winter. In comparison to a simulation with no DMS, the CDNC level over the southern oceans is 128% larger in the baseline simulation averaged over the austral summer months. Our results also show an increased number of smaller sized cloud droplets during this period. We estimate a maximum decrease of up to 15-18% in the droplet radius and a mean increase in cloud cover by around 2.5% over the southern oceans during SH summer in the simulation with ocean DMS compared to when the DMS emissions are switched off. The global annual mean top of the atmosphere DMS aerosol all sky radiative forcing is -2.03 W/m², whereas, over the southern oceans during SH summer, the mean DMS aerosol radiative forcing reaches -9.32 W/m². [ABSTRACT FROM AUTHOR]

Nucleation from the gas phase is an important source of aerosol particles in the Earth's atmosphere, contributing to the number of cloud condensation nuclei, which form cloud droplets. We have implemented in the aerosol-climate model ECHAM5-HAM a new scheme for neutral and charged nucleation of sulfuric acid and water based on laboratory data, and nucleation of an organic compound and sulfuric acid using a parametrization of cluster activation based on field measurements. We give details of the implementation, compare results with observations, and investigate the role of the individual aerosol nucleation mechanisms for clouds and the Earth's radiative budget. The results of our simulations are most consistent with observations when neutral and charged nucleation of sulfuric acid proceed throughout the troposphere and nucleation due to cluster activation is limited to the forested boundary layer. The globally averaged annual mean contributions of the individual nucleation processes to total absorbed solar short-wave radiation via the direct, semi-direct, indirect cloud-albedo and cloud-lifetime effects in our simulations are -1.15 W/m2 for charged H2SO4/H2O nucleation, -0.235 W/m2 for cluster activation, and -0.05 W/m2 for neutral H2SO4/H2O nucleation. The overall effect of nucleation is -2.55 W/m2, which exceeds the sum of the individual terms due to feedbacks and interactions in the model. Aerosol nucleation contributes over the oceans with -2.18 W/m2 to total absorbed solar short-wave radiation, compared to -0.37 W/m2 over land. We explain the higher effect of aerosol nucleation on Earth's radiative budget over the oceans with the larger area covered by ocean clouds, due to the larger contrast in albedo between clouds and the ocean surface compared to continents, and the larger susceptibility of pristine clouds owing to the saturation of effects. The large effect of charged nucleation in our simulations is not in contradiction with small effects seen in local measurements: over southern Finland, where cluster activation proceeds efficiently, we find that charged nucleation of sulfuric acid and water contributes on average less than 10% to ultrafine aerosol concentrations, in good agreement with observations [ABSTRACT FROM AUTHOR]

Atmospheric transport of traces gases and aerosols plays an important role in the distribution of air pollutants and radiatively active compounds. For model simulations of chemistry-climate interactions it is important to know how the transport of tracers depends on the geographical resolution of the general circulation model. However, this aspect has been scarcely investigated until now. Here, we analyse tracer transport in the ECHAM5 general circulation model using 6 independent idealized tracers with constant lifetimes, which are released in two different altitudes at the surface and in the stratosphere, respectively. Model resolutions from T21L19 to T106L31 were tested by performing multi-annual simulations with prescribed sea surface temperatures and sea ice fields of the 1990s. The impacts of the tracer lifetime were investigated by varying the globally uniform exponential decay time between 0.5 and 50 months. We also tested the influence of using prescribed meteorological fields (ERA40) instead of climatological sea surface temperature and sea ice fields. Meridional transport of surface tracers decreases in the coarse resolution model due to enhanced vertical mixing, with the exception of the advection into the tropical region, which shows an inconsistent trend between the resolutions. Whereas, the meridional transport of tracers released in the stratosphere was enhanced with higher model resolutions, except in the transport from tropical stratosphere to the Southern Hemisphere, which exhibits an increase trend with increasing model resolution. The idealized tracers exhibit a seasonal cycle, which is modulated by the tracer lifetime. In comparison to the run with prescribed sea surface temperature and sea ice fields, the simulation with prescribed meteorological fields did not exhibit significant change in the meridional transport, except in the exchange of stratospheric tracers between both hemispheres, where it causes about 100% increase. The import of the surface tracers into the stratosphere is increased by up to a factor of 2.5, and the export from the stratosphere into the troposphere was increased by up to 60% when prescribed meteorological fields is used. The ERA40 simulation also showed larger interannual variability (up to 24% compared to 12% in the standard simulations). Using our surface tracers released in either the northern or Southern Hemisphere, respectively, we calculate inter-hemispheric transport times between 11 and 17 months, consistent with values reported in the literature. While this study cannot be used to relate differences in model results to specific changes in transport processes, it nevertheless provides some insight into the characteristics of tracer transport in the widely used ECHAM5 general circulation model. [ABSTRACT FROM AUTHOR]

The contribution of ocean dimethyl sulfide (DMS) emissions to changes in cloud microphysical properties is quantified seasonally and globally for present day climate conditions using an aerosol-chemistry-climate general circulation model, ECHAM5-HAMMOZ, coupled to a cloud microphysics scheme. We evaluate DMS aerosol-cloudclimate linkages over the southern oceans where anthropogenic influence is minimal. The changes in the number of activated particles, cloud droplet number concentration (CDNC), cloud droplet effective radius, cloud cover and the radiative forcing are examined by analyzing two simulations: a baseline simulation with ocean DMS emissions derived from a prescribed climatology and one in which the ocean DMS emissions are switched off. Our simulations show that the model realistically simulates the seasonality in the number of activated particles and CDNC, peaking during Southern Hemisphere (SH) summer coincident with increased phytoplankton blooms and gradually declining with a minimum in SH winter. In comparison to a simulation with no DMS, the CDNC level over the southern oceans is 128% larger in the baseline simulation averaged over the austral summer months. Our results also show an increased number of smaller sized cloud droplets during this period. We estimate a maximum decrease of up to 15-18% in the droplet radius and a mean increase in cloud cover by around 2.5% over the southern oceans during SH summer in the simulation with ocean DMS com pared to when the DMS emissions are switched off. The global annual mean top of the atmosphere DMS aerosol all sky radiative forcing is -2.03W/m², whereas, over the southern oceans during SH summer, the mean DMS aerosol radiative forcing reaches -9.32W/m². [ABSTRACT FROM AUTHOR]

Large volcanic eruptions emit huge amounts of sulfur and fine ash into the stratosphere. These products cause an impact on radiative processes, temperature and wind patterns. In simulations with a General Circulation Model including detailed aerosol microphysics, the relation between the impact of sulfur and fine ash is determined for different eruption strengths and locations, one in the tropics and one in high Northern latitudes. Fine ash with effective radii between 1 μm and 15 μm has a lifetime of several days only. Nevertheless, the strong absorption of shortwave and long-wave radiation causes additional heating and cooling of±20K/day and impacts the evolution of the volcanic cloud. Depending on the location of the volcanic eruption, transport direction changes due to the presence of fine ash, vortices develop and temperature anomalies at ground increase. The results show substantial impact on the local scale but only minor impact on the evolution of sulfate in the stratosphere in the month after the simulated eruptions. [ABSTRACT FROM AUTHOR]

The transport of tracers in the general circulation model ECHAM5 is analysed using 9 independent idealized tracers with constant lifetimes released in different altitude regions of the atmosphere. The source regions were split into the tropics, Northern and Southern Hemisphere. The dependency of tracer transport on model resolution is tested in the resolutions T21L19, T42L19, T42L31, T63L31 and T106L31, by employing tracers with a globally uniform lifetime of 5 months. Each of the experiments uses prescribed sea surface temperatures and sea ice fields of the 1990s. The influence of meteorology and tracer lifetimes were tested by performing additional experiments in the T63L31 resolution, by nudging ECHAM5 towards the European Centre for Medium Range Weather Forecast 40 years re-analysis data (ERA40), and by using tracer lifetimes of 0.5 and 50 months, respectively. The transport of tracers is faster in the finer resolution models and is mostly dependent on the number of vertical levels. We found a decrease in the inter-hemispheric transport of tracers with source region at the sur face or the tropopause in the coarse resolution models due to increasing recirculation within the source region and vertical mixing. However, a coarse model resolution leads to enhanced inter-hemispheric transport in the stratosphere. The use of ERA40 data only slightly affects the inter-hemispheric transport of surface and tropopause tracers, whereas it increases the inter-hemispheric and vertical transport in the stratosphere by up to 100% and by a factor of 2.5, respectively. The inter-hemispheric transport time was deduced from simulations with tracers of infinite lifetime and source regions at the surface in the Northern and Southern Hemisphere. Again, the transport was found to be faster for models with higher vertical resolution. We find inter-hemispheric transport times of about 7 to 9 months which are lower than the values reported in the literature, based for example on 85Kr observations. [ABSTRACT FROM AUTHOR]

We investigate the influence of African biomass burning, biogenic, lightning and anthropogenic emissions on the tropospheric ozone over Africa and globally using a coupled global chemistry climate model. Our model studies indicate that surface ozone concentration may rise by up to 50 ppbv in the burning region during the biomass burning seasons. Biogenic emissions yield between 5-30 ppbv increase in the near surface ozone concentration over tropical Africa. The impact of lightning on surface ozone is negligible, while anthropogenic emissions yield a maximum of 7 ppbv increase in the annual-mean surface ozone concentration over Nigeria, South Africa and Egypt. Our results show that biogenic emissions are the most important African emission source affecting total tropospheric ozone. The influence of each of the African emissions on the global tropospheric ozone burden (TOB) of 384 Tg yields about 9.5 Tg, 19.6 Tg, 9.0 Tg and 4.7 Tg for biomass burning, biogenic, lightning and anthropogenic emissions emitted in Africa respectively. The impact of each of these emission categories on African TOB of 33 Tg is 2.5 Tg, 4.1 Tg, 1.75 Tg and 0.89 Tg respectively, which together represents about 28% of the total TOB calculated over Africa. Our model calculations also suggest that more than 70% of the tropospheric ozone produced by each of the African emissions is found outside the continent, thus exerting a noticeable influence on a large part of the tropical troposphere. Apart from the Atlantic and Indian Ocean, Latin America experiences the largest impact of African emissions, followed by Oceania, the Middle East, Southeast and south-central Asia, northern North America (i.e. the United States and Canada), Europe and north-central Asia, for all the emission categories. [ABSTRACT FROM AUTHOR]

We use 23 atmospheric chemistry transport models to calculate current and future (2030) deposition of reactive nitrogen (NOy, NHx) and sulfate (SOx) to land and ocean surfaces. The models are driven by three emission scenarios: (1) current air quality legislation (CLE); (2) an optimistic case of the maximum emissions reductions currently technologically feasible (MFR); and (3) the contrasting pessimistic IPCC SRES A2 scenario. An extensive evaluation of the present-day deposition using nearly all information on wet deposition available worldwide shows a good agreement with observations in Europe and North America, where 60-70% of the model-calculated wet deposition rates agree to within ±50% with quality-controlled measurements. Models systematically overestimate NHx deposition in South Asia, and underestimate NOy deposition in East Asia. We show that there are substantial differences among models for the removal mechanisms of NOy, NHx, and SOx, leading to ±1 σ variance in total deposition fluxes of about 30% in the anthropogenic emissions regions, and up to a factor of 2 outside. In all cases the mean model constructed from the ensemble calculations is among the best when comparing to measurements. Currently, 36-51% of all NOy, NHx, and SOx is deposited over the ocean, and 50-80% of the fraction of deposition on land falls on natural (nonagricultural) vegetation. Currently, 11% of the world's natural vegetation receives nitrogen deposition in excess of the "critical load" threshold of 1000 mg(N) m-2 yr-1. The regions most affected are the United States (20% of vegetation), western Europe (30%), eastern Europe (80%), South Asia (60%), East Asia (40%), southeast Asia (30%), and Japan (50%). Future deposition fluxes are mainly driven by changes in emissions, and less importantly by changes in atmospheric chemistry and climate. The global fraction of vegetation exposed to nitrogen loads in excess of 1000 mg(N) m-2 yr-1 increases globally to 17% for CLE and 25% for A2. In MFR, the reductions in NOy are offset by further increases for NHx deposition. The regions most affected by exceedingly high nitrogen loads for CLE and A2 are Europe and Asia, but also parts of Africa. [ABSTRACT FROM AUTHOR]

We investigate the relative importance of African biomass burning, biogenic volatile organic compounds (VOC), lightning and anthropogenic emissions to the tropospheric ozone budget over Africa and globally using a coupled global chemistry climate model. Our model studies indicate that the photochemical surface ozone concentration may rise by up to 50 ppbv in the burning region during the biomass burning seasons. Biogenic VOCs contribute between 5-20 ppbv to the near surface ozone concentration over the tropical African region. The impact of lightning on surface ozone is negligible, while anthropogenic emissions contribute a maximum of 10 ppbv to the surface ozone over Nigeria, South-Africa and Egypt. The annual average of the surface and column ozone over Africa shows that biomass burning is the single most important emission source affecting the African region, while biogenic emissions have the highest contribution during the rainy seasons. The contributions of African emissions to global tropospheric ozone burden (TOB) are about 9 Tg, 13 Tg, 8 Tg and 4 Tg for African biomass burning, biogenic VOC, lightning and anthropogenic emissions respectively. These correspond to 2.4%, 3.4%, 2.1% and 1% of the global tropospheric ozone budget respectively. Over Africa itself, the contribution of each of these emission types is only 2.4 Tg, 2.2 Tg, 1.4 Tg and 0.8 Tg respectively. Outside the continent, African biogenic VOC emissions yield the highest contribution to the TOB. Our model calculations suggest that about 70% of the tropospheric ozone produced from emissions in Africa is found outside the continent, thus exerting a noticeable influence on a large part of the tropical troposphere. Latin America experiences the highest impact of African emissions, followed by southeast and south-central Asia, Oceania, and the Middle East for all the emission categories; while Canada, the United States, Russia, Mongolia, China and Europe experience the least impact of African emissions. [ABSTRACT FROM AUTHOR]

One of the intrinsic difficulties for in situ photoemission studies of high T[sub c] oxide films is the surface volatility, especially the oxygen loss. In order to solve this problem, we have constructed a dedicated system for high T[sub c] film surface studies, in particular for ARPES measurements. Here we briefly describe our pulsed laser deposition (PLD) system that is linked to the photoemission chamber at the Synchrotron Radiation Center (SRC) in Wisconsin, and discuss crystallographic and electronic properties measured on epitaxial YBa[sub 2]Cu[sub 3]O[sub 7-δ] (YBCO) and NdBa[sub 2]CuaO[sub 7-δ] (NBCO) films. Resistivity and XRD studies show that the best c axis epitaxial films, with T[sub c] (onset) = 92 K (T[sub co] = 90.5 K), are monophase and single crystalline with crystal coherence up to almost 1 µm. Initial core level photoemission study indicates that, for YBCO on SrTiO[sub 3] (without any buffer layer), the Ba oxide layer tends to be the dominant surface layer. Further experiments are underway to reproducibly detect sharp Fermi edge and perform ARPES study on optimally doped film surfaces. [ABSTRACT FROM AUTHOR]

We describe an efficient biased Monte-Carlo method for calculating the diagrams appearing in the coefficients of the so-called bridge function B=zeta n=2bn rhon n of the integral equation theory of liquids. These diagrams represent multi-dimensional integrals of products of 'bond' functions of the intermolecular distances. The method rests on the generation of independent Markov chains and is well adapted to highly parallel computation. It can be used for systems with any pair potential. The feasibility and efficiency of the method are demonstrated for the second and third order coefficients of the bridge functions of fluids of hard and Lennard-Jones spheres. For these systems there are analytical expressions of the bridge function deduced from computer simulations to which we compare our bridge function approximations which include the second and third order coefficients with h as the bond function. Our new approximations of the bridge function are used in the closure of the Ornstein-Zernike relation. The obtained structural and thermodynamical properties are found in better agreement with the exact simulation data than the hypernetted chain results. [ABSTRACT FROM AUTHOR]

Site-site distribution functions, internal energies, compressibilities, and dielectric constants of liquid acetone and chloroform are computed and compared. The hypernetted chain approximation is used for the molecular Ornstein-Zernike (MOZ) and site-site Ornstein-Zernike (SSOZ) theories. Both solvent molecules are described as sets of interaction sites, which are the centres of Lennard-Jones potentials and which carry partial electric charges. How the approximations inherent in both OZ theories affect the calculated liquid properties is discussed. In contrast to SSOZ theory, MOZ theory yields a correct description of the liquid structure as defined by the site-site distribution functions of simulations. The MOZ results for the dielectric constants are in good agreement with simulation, but both OZ theories slightly underestimate the internal excess energies. In contrast to the SSOZ formalism and to the simulations, the molecular pair distribution of MOZ theory can be computed readily for all two-molecule configurations, allowing a detailed study of the complex relief of this distribution. A search was performed for configurations that are highly probable in the liquid. They can be assigned to a small number of peaks of the molecular distribution function. These peaks have major contributions to the Kirkwood factors, which measure the orientational order in the liquid, and to the electrostatic part of the excess energies. The partitioning of the whole two-molecule configuration space makes it possible to study the details of the site-site distribution functions. For instance, a sharp peak in the oxygen-oxygen distribution in acetone results from many superimposed contributions of acetone-acetone arrangements of low and medium statistical weights, and not from the highly probable arrangements. [ABSTRACT FROM AUTHOR]

A general theory of the electronic relaxation of an S state complexed paramagnetic metal ion (Mn[sup 2+], Gd[sup 3+]) in solution is developed. Contrarily to the usual assumption, the electronic relaxation is not only due to the effects of the transient zero field splitting, but is strongly influenced by the static crystal field effect which is modulated by the random Brownian rotation of the complex. The electron paramagnetic resonance measured linewidths of three Gd[sup 3+] (S=7/2) complexes at various temperatures and fields [D. H. Powell et al. J. Am. Chem. Soc. 118, 9333 (1996)] are well interpreted in the framework of this model and show the contributions of both mechanisms. The fitted crystal field parameters, the correlation times, and the activation energies are in good agreement with their expected values from the underlying processes. Moreover, our interpretation does not require the addition of any field independent contribution to the linewidth like the spin-rotation mechanism. The longitudinal relaxation function is well approximated using a single relaxation time, whereas the transverse relaxation function is a superposition of four decreasing exponentials. © 2000 American Institute of Physics. [ABSTRACT FROM AUTHOR]

In atomic force microscopy cantilevers are used to detect forces caused by interactions between probing tip and sample. The minimum forces which can be detected with commercial sensors are typically in the range of 10[sup -12] N. In the future, the aim will be to construct sensors with improved sensitivities to detect forces in the range of 10[sup -18] N. These sensors could be used for mass spectroscopy or magnetic resonance force microscopy. Achieving this goal requires smaller sensors and increased quality factor Q. In this article we describe a model to characterize the dynamics of cantilevers of each eigenmode. In contrast to previous models, the damping is treated rigorously in the calculations. © 2000 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Background: Nestin, a class VI intermediate filament protein of the cytoskeleton, and CD34, a transmembrane phosphoglycoprotein, are markers of progenitor cells. This study aimed to evaluate their expression and clinical significance in colorectal cancer., Methods: A clinically annotated tissue microarray, including 599 patients with colorectal cancer, was analyzed by immunohistochemistry. Furthermore, nestin and CD34 correlations with HIF-1a and a panel of cytokines and chemokines were assessed using quantitative reverse transcription PCR and The Cancer Genome Atlas dataset., Results: Expression of nestin and CD34 was observed only in the tumor stroma. Patients displaying high expression of nestin and CD34 demonstrated higher rates of T1 and T2 tumors ( p  = .020), lower vascular invasion ( p  < .001) and improved 5-year overall survival (65%; 95% CI = 55-73 vs 45%; 95% CI = 37-53) after adjusting for clinicopathological characteristics (HR: 0.67; 95% CI = 0.46-0.96). A moderate to strong correlation ( r  = 0.37-0.78, p  < .03) of nestin and CD34 was demonstrated for the following markers; HIF-1α, CD4, CD8, FOXP3, IRF1, GATA3, CCL2, CCL3, CXCL12 and CCL21., Conclusions: Combined expression of nestin and CD34 expression is associated with better overall survival possibly by modulating a favorable immune response.

Background: Currently, the two most common bariatric procedures are laparoscopic sleeve gastrectomy (LSG) and laparoscopic Roux-en-Y gastric bypass (LRYGB). Long-term data comparing the two interventions in terms of their effect on body composition and bone mass density (BMD) are scarce., Objective: The aim of this study was to assess body composition and BMD at least 5 years after LSG and LRYGB., Setting: Department of Endocrinology and Nutrition, St. Claraspital Basel and St. Clara Research Ltd., Basel, Switzerland., Methods: Bariatric patients at least 5 years after surgery (LSG or LRYGB) were recruited, and body composition and BMD were measured by means of dual-energy X-ray absorptiometry. Data from body composition before surgery were included in the analysis. Blood samples were taken for determination of plasma calcium, parathyroid hormone, vitamin D3, alkaline phosphatase, and C-terminal telopeptide, and the individual risk for osteoporotic fracture assessed by the Fracture Risk Assessment Tool score was calculated. After surgery, all patients received multivitamins, vitamin D3, and zinc. In addition, LRYGB patients were prescribed calcium., Results: A total of 142 patients were included, 72 LSG and 70 LRYGB, before surgery: median body mass index 43.1, median age 45.5 years, 62.7% females. Follow-up after a median of 6.7 years. For LRYGB, the percentage total weight loss at follow-up was 26.3% and for LSG 24.1% (p = 0.243). LRYGB led to a slightly lower fat percentage in body composition. At follow-up, 45% of both groups had a T score at the femoral neck below -1, indicating osteopenia. No clinically relevant difference in BMD was found between the groups., Conclusions: At 6.7 years after surgery, no difference in body composition and BMD between LRYGB and LSG was found. Deficiencies and bone loss remain an issue after both interventions and should be monitored., (© 2020 The Author(s) Published by S. Karger AG, Basel.)

A new release of the Max Planck Institute for Meteorology Earth System Model version 1.2 (MPI-ESM1.2) is presented. The development focused on correcting errors in and improving the physical processes representation, as well as improving the computational performance, versatility, and overall user friendliness. In addition to new radiation and aerosol parameterizations of the atmosphere, several relatively large, but partly compensating, coding errors in the model's cloud, convection, and turbulence parameterizations were corrected. The representation of land processes was refined by introducing a multilayer soil hydrology scheme, extending the land biogeochemistry to include the nitrogen cycle, replacing the soil and litter decomposition model and improving the representation of wildfires. The ocean biogeochemistry now represents cyanobacteria prognostically in order to capture the response of nitrogen fixation to changing climate conditions and further includes improved detritus settling and numerous other refinements. As something new, in addition to limiting drift and minimizing certain biases, the instrumental record warming was explicitly taken into account during the tuning process. To this end, a very high climate sensitivity of around 7 K caused by low-level clouds in the tropics as found in an intermediate model version was addressed, as it was not deemed possible to match observed warming otherwise. As a result, the model has a climate sensitivity to a doubling of CO 2 over preindustrial conditions of 2.77 K, maintaining the previously identified highly nonlinear global mean response to increasing CO 2 forcing, which nonetheless can be represented by a simple two-layer model., (©2019. The Authors.)