Atmospheric Aerosol and Cloud Condensation Nuclei Formation: A Possible Influence of Cosmic Rays?

A physical mechanism which may have a potential to connect climate with cosmic rays (CR) involves aerosol particle formation by CR generated atmospheric ions followed by new particle growth. Only grown particles can scatter sunlight efficiently and can eventually act as cloud condensation nuclei (CCN) and thereby may influence climate. Moreover grown particles live longer as they are less rapidly scavenged by pre-existing larger particles. The present paper discusses aerosol particle formation and growth in the light of new measurements recently made by our MPIK Heidelberg group. Emphasis is placed upon the upper troposphere where very low temperatures tend to facilitate new particle formation by nucleation. The new measurements include: laboratory measurements of cluster ions, aircraft measurements of ambient atmospheric ions, and atmospheric measurements of the powerful nucleating gas H₂SO₄ and its precursor SO₂. The discussion also addresses model simulations of aerosol formation and growth. It is concluded that in the upper troposphere new aerosol formation by CR generated ions is a frequent process with relatively large rates. However new particle formation by homogeneous nucleation (HONU) which is not related to CR also seems to be efficient. The bottleneck in the formation of upper troposphere aerosol particles with sizes sufficiently large to be climate relevant is not nucleation but growth of small particles. Our recent upper troposphere SO₂ measurements suggest that particle growth by gaseous sulphuric acid condensation is at least occasionally efficient. If so CR mediated formation of CCN sized particles should at least occasionally be operative in the upper troposphere.     

Atmospheric Ions and Aerosol Formation

This paper discusses atmospheric ions and their role in aerosol formation. Emphasis is placed upon the upper troposphere where very low temperatures tend to facilitate new particle formation by nucleation. New measurements addressed include: Laboratory measurements of cluster ions, aircraft measurements of ambient atmospheric ions, atmospheric measurements of the powerful nucleating gas H₂SO₄ and its gaseous precursor SO₂. The paper also discusses model simulations of aerosol formation and growth. It is concluded that in the upper troposphere new aerosol formation via ions is a frequent process with relatively large rates. However new particle formation by homogeneous nucleation which does not involve ions also seems to be efficient. The bottleneck in the formation of upper troposphere aerosol particles with sizes sufficiently large to be climate relevant is mostly not nucleation but sufficient growth of new and still very small particles. Our recent upper troposphere SO₂ measurements suggest that particle growth by gaseous sulphuric acid condensation can be efficient in certain circumstances. If so, cosmic ray mediated formation of CCN sized particles should at least occasionally be operative in the upper troposphere.     

In Situ Collection of Refractory Dust in the Upper Stratosphere: The DUSTER Facility

DUSTER (Dust from the Upper Stratosphere Tracking Experiment and Retrieval) is an instrument designed to collect nanometer to micrometer scale solid aerosol particles in the upper stratosphere on board balloons. With three DUSTER flights we have demonstrated that: (1) the instrument’s performance was within the design parameters of environmental specifications (?80 ^°C; 3–10?mbar); (2) inertial impact collection of aerosols ～500?nm to 24 microns on holey-carbon thin films mounted on Transmission Electron Microscope mesh grids was achieved; (3) the design of an active collector exposed to the air flux and an identical collector “blank”, not exposed to the air flux, to monitor possible contamination permits unambiguous identification of collected particles; (4) save storage of collected samples and subsequent retrieval in the laboratory was achieved with no measurable contamination; (5)?reduced sample manipulation allowed the chemical and structural characterization of collected dust particles by Field-emission scanning electron microscopy and energy dispersive X-Ray analyses, and infrared and Raman micro-spectroscopy. The main and most ambitious goal is the collection and characterization of solid aerosol particles smaller than 3 microns of solar system debris that are currently not sampled on a routine basis by other instruments in the upper stratosphere. DUSTER will provide a record of the amount of solid aerosols, their size, shapes and chemical properties in the upper stratosphere, including particles less than 3 microns in size. The DUSTER program identified 25 particles as collected during the 2008 flight with sizes in the range of 0.4 to 24 microns.     

Profiles of Ion and Aerosol Interactions in Planetary Atmospheres

In planetary atmospheres the nature of the aerosols varies, as does the relative importance of different sources of ion production. The nature of the aerosol and ion production is briefly reviewed here for the atmospheres of Venus, Mars, Jupiter and Titan using the concepts established for the terrestrial atmosphere. Interactions between the ions formed and aerosols present cause (1) charge exchange, which can lead to substantial aerosol charge and (2) ion removal. Consequences of (1) are that (a) charged aerosol are more effectively removed by conducting liquid droplets than uncharged aerosol and (b) particle–particle coagulation rates are modified, influencing particle residence times in the relevant atmosphere. Consequences of (2) are that ions are removed in regions with abundant aerosol, which may preclude charge flow in an atmosphere, such as that associated with an atmospheric electrical circuit. In general, charge should be included in microphysical modeling of the properties of planetary aerosols.     

Atmospheric Ion-induced Aerosol Nucleation

Ion-induced nucleation has been suggested to be a potentially important mechanism for atmospheric aerosol formation. Ions are formed in the background atmosphere by galactic cosmic rays. A possible connection between galactic cosmic rays and cloudiness has been However, the predictions of current atmospheric nucleation models are highly uncertain because the models are usually based on the liquid drop model that estimates cluster thermodynamics based on bulk properties (e.g., liquid drop density and surface tension). Sulfuric acid (H₂SO₄) and water are assumed to be the most important nucleating agents in the free troposphere. Measurements of the molecular thermodynamics for the growth and evaporation of cluster ions containing H₂SO₄ and H₂O were performed using a temperature-controlled laminar flow reactor coupled to a linear quadrupole mass spectrometer as well as a temperature-controlled ion trap mass spectrometer. The measurements were complemented by quantum chemical calculations of the cluster ion structures. The analysis yielded a complete set of H₂SO₄ and H₂O binding thermodynamics extending from molecular cluster ions to the bulk, based on experimental thermodynamics for the small clusters. The data were incorporated into a kinetic aerosol model to yield quantitative predictions of the rate of ion-induced nucleation for atmospheric conditions. The model predicts that the negative ion-H₂SO₄-H₂O nucleation mechanism is an efficient source of new particles in the middle and upper troposphere.     

Cloud Formation and the Possible Significance of Charge for Atmospheric Condensation and Ice Nuclei

Cloud formation in the atmosphere is related to the presence of water vapour, cloud condensation nuclei (CCN) and ice nuclei (IN). Ionisation in the atmosphere is caused by a variety of sources, but the contribution from cosmic rays is always present and is modulated by the solar cycle. Methods of investigating the variability in ionisation are described. The mechanisms proposed by which (1) ionisation could influence cloud formation, and (2) by which changes to the CCN and IN could occur are discussed. Direct formation of sulphate CN is conceivable in atmospheric air by radioactivity, and charging of molecular clusters leads to greater collisions rates than for neutral clusters. Modification of the ice nucleation efficiency of aerosol could also have atmospheric effects through latent heat release. However in both cases definitive atmospheric experimental work is lacking and therefore any link between solar variability and clouds remains unproven.     

Cosmic Rays,Clouds, and Climate

A correlation between a global average of low cloud cover and the flux of cosmic rays incident in the atmosphere has been observed during the last solar cycle. The ionising potential of Earth bound cosmic rays are modulated by the state of the heliosphere, while clouds play an important role in the Earth's radiation budget through trapping outgoing radiation and reflecting incoming radiation. If a physical link between these two features can be established, it would provide a mechanism linking solar activity and Earth's climate. Recent satellite observations have further revealed a correlation between cosmic ray flux and low cloud top temperature. The temperature of a cloud depends on the radiation properties determined by its droplet distribution. Low clouds are warm (>273K) and therefore consist of liquid water droplets. At typical atmospheric supersaturations (1%) a liquid cloud drop will only form in the presence of an aerosol, which acts as a condensation site. The droplet distribution of a cloud will then depend on the number of aerosols activated as cloud condensation nuclei (CCN) and the level of super saturation. Based on observational evidence it is argued that a mechanism to explain the cosmic ray-cloud link might be found through the role of atmospheric ionisation in aerosol production and/or growth. Observations of local aerosol increases in low cloud due to ship exhaust indicate that a small perturbation in atmospheric aerosol can have a major impact on low cloud radiative properties. Thus, a moderate influence on atmospheric aerosol distributions from cosmic ray ionisation would have a strong influence on the Earth's radiation budget. Historical evidence over the past 1000 years indicates that changes in climate have occurred in accord with variability in cosmic ray intensities. Such changes are in agreement with the sign of cloud radiative forcing associated with cosmic ray variability as estimated from satellite observations.     

Aerosols on the Giant Planets and Titan

On the giant planets and Titan, like on the terrestrial planets, aerosols play an important part in the physico-chemistry of the upper atmosphere (P ≤ 0.5 bar). Above all, aerosols significantly affect radiative transfer processes, mainly through light scattering, thus influencing the atmospheric energy budget and dynamics. Because there is usually significant coupling between atmospheric circulation and haze production, aerosols may constitute useful tracers of atmospheric dynamics.More generally, since their production is directly linked to some kind of energy deposition, their study may also provide clues to external sources of energy as well as their variability. Finally, aerosols indirectly influence other processes such as cloud formation and disequilibrium chemistry, by acting either as condensation nuclei or as reaction sites for surface chemistry. Here, I present a review of observational and modeling results based on remote sensing data, and also some insights derived from laboratory simulations. Despite our knowledge of the effects of aerosols in outer planetary atmospheres, however, relatively little is understood about the pathways which produce them, either endogenously (as end-products of gas-phase photochemical or shock reactions) or exogenously (as residues of meteroid ablation).     

Solar Influence on Earth's Climate

An increasing number of studies indicate that variations in solar activity have had a significant influence on Earth's climate. However, the mechanisms responsible for a solar influence are still not known. One possibility is that atmospheric transparency is influenced by changing cloud properties via cosmic ray ionisation (the latter being modulated by solar activity). Support for this idea is found from satellite observations of cloud cover. Such data have revealed a striking correlation between the intensity of galactic cosmic rays (GCR) and low liquid clouds (<3.2 km). GCR are responsible for nearly all ionisation in the atmosphere below 35 km. One mechanism could involve ion-induced formation of aerosol particles (diameter range, 0.001–1.0 μm) that can act as cloud condensation nuclei (CCN). A systematic variation in the properties of CCN will affect the cloud droplet distribution and thereby influence the radiative properties of clouds. If the GCR-Cloud link is confirmed variations in galactic cosmic ray flux, caused by changes in solar activity and the space environment, could influence Earth's radiation budget. This revised version was published online in August 2006 with corrections to the Cover Date.     

Satellite Observations of Natural and Anthropogenic Aerosol Effects on Clouds and Climate

Anthropogenic aerosols affect the climate system and the hydrological cycle. The net effect of aerosols is to cool the climate system, directly by reflecting sunlight to space, and indirectly by increasing the brightness and cover of clouds that in turn also reflect more sunlight to space. The uncertainty in the aerosol effect on climate is 5 times greater than that of the greenhouse gases. The reason for this is the short aerosol lifetime and chemical complexity, that makes it difficult to represent the global aerosol budget from surface or aircraft measurements. Satellites provide daily global information about the aerosol content, generating large statistics with excellent regional and global representation of the aerosol column concentration, and differentiating fine from coarse aerosol. Here we use observations performed with the MODIS instrument onboard the Terra and Aqua satellites to differentiate natural from anthropogenic aerosols, and to measure the aerosol effect on cloud properties and on the reflectivity of sunlight.     

Impact of Solar Activity on Stratospheric Ozone and NO2 Observed by Gomos/Envisat

Energetic proton precipitation occurring during solar events can increase the production of odd nitrogen in the upper stratosphere and mesosphere. A very intense solar proton event (SPE) occurred on 28 October 2003. Its impact on the composition of the middle atmosphere was observed in details due to the availability of several space instruments. Here we present GOMOS observations of a strong NO₂increase and a related ozone decrease in the upper stratosphere at north polar latitude. The perturbation of the chemical composition of the stratosphere was observed until the middle of December 2003. A strong NO₂ increase was also observed in the south polar vortex in June-July 2003. It is tentatively attributed to the effect of an SPE with protons of moderate energy occurring on 29 May 2003. If this hypothesis is confirmed, it will imply that the global effect of SPEs on the composition of the stratosphere is underestimated when only strong energy SPEs are considered.     

Ions in the Terrestrial Atmosphere and Other Solar System Atmospheres

Charged molecular clusters, traditionally called small ions, carry electric currents in atmospheres. Charged airborne particles, or aerosol ions, play an important role in generation and evolution of atmospheric aerosols. Growth of ions depends on the trace gas content, which is highly variable in the time and space. Even at sub-ppb concentrations, electrically active organic compounds (e.g. pyridine derivatives) can affect the ion composition and size. The size and mobility are closely related, although the form of the relationship varies depending on the critical diameter, which, at 273 K, is about 1.6 nm. For ions smaller than this the separation of quantum levels exceeds the average thermal energy, allowing use of a molecular aggregate model for the size-mobility relation. For larger ions the size-mobility relation approaches the Stokes-Cunningham-Millikan law. The lifetime of a cluster ion in the terrestrial lower atmosphere is about one minute, determined by the balance between ion production rate, ion-ion recombination, and ion-aerosol attachment.     

Theory of formation of the ionosphere

Current knowledge about the solar radiation and absorption and ionization cross sections of atmospheric gases is reviewed. Next the main observed features of ionospheric layers are summarized. Using CIRA 1965 model atmospheres the heights of the peak of the ionization rate are calculated for a number of solar emission lines and it is made clear which of these lines are responsible for the formation of E and F1 layers. The mechanism of electron removal in the F and upper E regions as well as in the lower regions is considered, and the mechanism of formation and some behaviours of each ionospheric layer is discussed. In particular, the equatorial F2 layer is briefly considered. Discrepancies are pointed out between the values of the recombination coefficient and the rate constant for ion-atom interchange reaction obtained from ionospheric observations and from laboratory experiments. Inconsistency of the values of the intensity of solar radiation measured by rocket techniques and inferred from ionospheric considerations is also noted. Some evidence is presented suggesting that corpuscular radiation may be responsible for part of the ionization in the ionosphere even in temperate latitudes.     

飞机最优巡航条件的确定

续航性能是飞机的主要战术技术指标之一。从飞机巡航段航程的基本公式出发，利用导数求极值的性质，推导出确定飞机巡航爬升和平流层内最佳巡航条件的方程，证明了最优巡航马赫数出现在飞机阻力增加区段，最优巡航高度存在于飞机阻力最小处。最后以某型飞机的巡航爬升条件和平流层平飞最优马赫数和高度的确定作为算例，说明用此方法确定飞机巡航条件，将使飞机获得最大航程。     

电荷作用对均质-非均质凝结流动的影响

基于Fletcher成核理论及均质-非均质凝结双流体模型,讨论了电荷作用对凝结流动的影响,结果表明:有无电荷影响时,成核率计算公式精度均较高,流场参数的计算结果与实验结果吻合良好,相对误差不超过5%,表明所建的均质-非均质凝结双流体模型具有较高精度.不带电时,加入颗粒半径为5nm颗粒前后流场过冷度差别较小,加入颗粒半径分别为8nm和10nm颗粒后过冷度峰值虽分别降低2K和7K,但均导致自发凝结向下游迁移.当颗粒带电荷量为Q=1e,加入颗粒半径为5nm颗粒情况下对减小成核自由能障、增加非均质成核率的作用最为明显,这一作用在颗粒半径为8nm时较弱,颗粒半径为10nm情况下最弱.当带电量增加至Q=3e时,加入颗粒半径分别为5nm和8nm颗粒情况下峰值过冷度与均质凝结相比分别下降10K和6K,且较明显地抑制了自发凝结发生.      

A Possible Transfer Mechanism for the 11-Year Solar Cycle to the Lower Stratosphere

Observational evidence of the 11-year solar cycle (SC) modulation of stratosphere temperatures and winds from the ERA-40 dataset is reviewed, with emphasis on the Northern winter hemisphere. A frequency modulation of sudden warming events is noted, with warmings occurring earlier in solar minimum periods than in solar maximum periods. The observed interaction between the influence of the SC and the quasi biennial oscillation (QBO) on the frequency of sudden warmings is noted as a possible clue for understanding their mechanism of influence. A possible transfer route for the 11-year solar cycle from the equatorial stratopause region to the lowest part of the stratosphere is proposed, via an influence on sudden warming events and the associated induced meridional circulation. SC and QBO composites of zonal wind anomalies show anomalous wind distributions in the subtropical upper stratosphere in early winter. Mechanistic model experiments are reviewed that demonstrate a sensitivity of sudden warmings to small wind anomalies in this region. Various diagnostics from these experiments are shown, including EP fluxes and their divergence and also the synoptic evolution of the polar vortex, in order to understand the mechanism of the influence. Some recent GCM experiments to investigate the SC/QBO interaction are also described. They simulate reasonably well the observed SC/QBO interaction of sudden warming events and appear to support the hypothesis that tropical/subtropical upper stratospheric wind anomalies are an important influence on the timing of sudden warmings.     

Dust Evolution in Protoplanetary Discs and the Formation of Planetesimals

After 25 years of laboratory research on protoplanetary dust agglomeration, a consistent picture of the various processes that involve colliding dust aggregates has emerged. Besides sticking, bouncing and fragmentation, other effects, like, e.g., erosion or mass transfer, have now been extensively studied. Coagulation simulations consistently show that \(\upmu\mbox{m}\)-sized dust grains can grow to mm- to cm-sized aggregates before they encounter the bouncing barrier, whereas sub-\(\upmu\mbox{m}\)-sized water-ice particles can directly grow to planetesimal sizes. For siliceous materials, other processes have to be responsible for turning the dust aggregates into planetesimals. In this article, these processes are discussed, the physical properties of the emerging dusty or icy planetesimals are presented and compared to empirical evidence from within and without the Solar System. In conclusion, the formation of planetesimals by a gravitational collapse of dust “pebbles” seems the most likely.     

Recent Space Data

This paper summarises the workshop session on recent space data. Most presentations addressed the intense solar storm in October–November 2003. Large perturbations of atmospheric trace gas concentrations, notably NO₂ and HNO₃, were found over extended areas around the magnetic poles in the mesosphere and stratosphere, extending over many weeks in the stratosphere. The impact on total ozone seems to be very limited although some more subtle investigations are still to be done. Several new space instruments with many innovative data products have been introduced. Very good coverage in vertically resolved observations of many chemical species is reached for stratospheric chemistry and dynamics research. Data have already been used to improve stratospheric models. Data continuity is an issue. However, the greatest concern is the lack of any suitable future space instrumentation for tropospheric research (air quality and climate forcing/carbon cycle) as well as UTLS problems (climate/chemistry interaction, stratosphere/troposphere exchange).     

Energy Deposition in Planetary Atmospheres by Charged Particles and Solar Photons

We discuss here the energy deposition of solar FUV, EUV and X-ray photons, energetic auroral particles, and pickup ions. Photons and the photoelectrons that they produce may interact with thermospheric neutral species producing dissociation, ionization, excitation, and heating. The interaction of X-rays or keV electrons with atmospheric neutrals may produce core-ionized species, which may decay by the production of characteristic X-rays or Auger electrons. Energetic particles may precipitate into the atmosphere, and their collisions with atmospheric particles also produce ionization, excitation, and heating, and auroral emissions. Auroral energetic particles, like photoelectrons, interact with the atmospheric species through discrete collisions that produce ionization, excitation, and heating of the ambient electron population. Auroral particles are, however, not restricted to the sunlit regions. They originate outside the atmosphere and are more energetic than photoelectrons, especially at magnetized planets. The spectroscopic analysis of auroral emissions is discussed here, along with its relevance to precipitating particle diagnostics. Atmospheres can also be modified by the energy deposited by the incident pickup ions with energies of eV’s to MeV’s; these particles may be of solar wind origin, or from a magnetospheric plasma. When the modeling of the energy deposition of the plasma is calculated, the subsequent modeling of the atmospheric processes, such as chemistry, emission, and the fate of hot recoil particles produced is roughly independent of the exciting radiation. However, calculating the spatial distribution of the energy deposition versus depth into the atmosphere produced by an incident plasma is much more complex than is the calculation of the solar excitation profile. Here, the nature of the energy deposition processes by the incident plasma are described as is the fate of the hot recoil particles produced by exothermic chemistry and by knock-on collisions by the incident ions.     

镍基高温合金铸件的晶粒组织控制──铸造工艺参数的影响

以ＩＮ７３８ＬＣ合金为例,研究了镍基高温合金在各种铸造工艺条件下的晶粒组织。结果表明,降低合金液均匀化处理温度可以明显细化冷凝后基体的晶粒。在浇注温度、铸型预热温度以及合金液均匀化处理温度等铸造工艺参数中,后者对晶粒尺寸的影响大于前两者。