Nucleation processes and aerosol chemistry

As the result of many observable optical phenomena, the occasional existence of upper atmospheric aerosols has been known since the beginning of the Century. Nevertheless, it is only during the last two decades that their persistent nature and extent of global distribution have become recognized. This review is addressed to the chemistry of upper atmospheric aerosols with particular attention to the chemical reactions and nucleation mechanisms responsible for their formation.Considering the stratosphere, it is now generally agreed that sulfate, mainly in the form of sulfuric acid, represents the single most abundant constituent of stratospheric aerosols. There is now strong evidence that these aerosols are formed in situ from sulfur bearing gases oxidized by free radicals. The various nucleation processes of atmospheric importance are reviewed, and it is shown that heteromolecular nucleation processes are almost certainly responsible for new particle formation in the stratosphere.The nature, and even existence, of aerosol layers above the stratosphere is less certain. The influx of extraterrestrial materials into the Earth atmosphere is estimated to be in the order of 50 to 500 tons per day. Considerations are given to the possible mechanisms which convert these materials to aerosol size particles. Although these particles provide one possible explanation for the appeareance of noctilucent clouds, nucleation about ions, most probably H₃O⁺ hydrates, is a strong contender as a more plausible formation mechanism. Considerable attention is given to this important atmospheric process, where it is shown that chemical forces contribute to the stability of the prenucleation clusters and the overall height of the energy barrier to nucleation. Finally, the role of aerosols in the sodium and other cycles of trace upper atmospheric constituents, is discussed.This research was performed under the auspices of the U.S. Atomic Energy Commission and partially financed by the Department of Transportation and the National Science Foundation under interagency agreements.     

Stratospheric dust and its relationship to the meteoric influx

A review of measurements sensitive to dust in the stratosphere is presented with special emphasis on the data obtained during the last 10 years. The measurements made by indirect techniques such as light scattering tend to show more stratospheric dust than the measurements obtained by direct sampling techniques, although this interpretation is somewhat complicated by the injection of dust from the Bali eruption in 1963. The discrepancy is interpreted as indicating that the stratospheric dust smaller than a few microns diameter is volital. Recent direct experimental evidence of the author supports this conclusion.The size distribution of stratospheric dust is presented as a composite of the results of several observers. A natural break in the distribution at a size of about 5 diameter is interpreted as indicating that the smaller dust is terrestrial in origin, while the larger dust is meteoric in origin. Other evidence is presented to support this conclusion. A comparison with particle flux measurements at 100 km and higher indicates that the meteoric component of the stratospheric dust is ablation products rather than single particles that have survived entry into the atmosphere. It is also argued that the small particles accounting for the high flux as measured by rocket and satellite microphone techniques are not present in the stratosphere.     

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.     

The Descent Imager/Spectral Radiometer (DISR) Experiment on the Huygens Entry Probe of Titan

The payload of the Huygens Probe into the atmosphere of Titan includes the Descent Imager/Spectral Radiometer (DISR). This instrument includes an integrated package of several optical instruments built around a silicon charge coupled device (CCD) detector, a pair of linear InGaAs array detectors, and several individual silicon detectors. Fiber optics are used extensively to feed these detectors with light collected from three frame imagers, an upward and downward-looking visible spectrometer, an upward and downward looking near-infrared spectrometer, upward and downward looking violet phtotometers, a four-channel solar aerole camera, and a sun sensor that determines the azimuth and zenith angle of the sun and measures the flux in the direct solar beam at 940 nm. An onboard optical calibration system uses a small lamp and fiber optics to track the relative sensitivity of the different optical instruments relative to each other during the seven year cruise to Titan. A 20 watt lamp and collimator are used to provide spectrally continuous illumination of the surface during the last 100 m of the descent for measurements of the reflection spectrum of the surface. The instrument contains software and hardware data compressors to permit measurements of upward and downward direct and diffuse solar flux between 350 and 1700 nm in some 330 spectral bands at approximately 2 km vertical resolution from an alititude of 160 km to the surface. The solar aureole camera measures the brightness of a 6° wide strip of the sky from 25 to 75° zenith angle near and opposite the azimuth of the sun in two passbands near 500 and 935 nm using vertical and horizontal polarizers in each spectral channel at a similar vertical resolution. The downward-looking spectrometers provide the reflection spectrum of the surface at a total of some 600 locations between 850 and 1700 nm and at more than 3000 locations between 480 and 960 nm. Some 500 individual images of the surface are expected which can be assembled into about a dozen panoramic mosaics covering nadir angles from 6° to 96° at all azimuths. The spatial resolution of the images varies from 300 m at 160 km altitude to some 20 cm in the last frames. The scientific objectives of the experiment fall into four areas including (1) measurement of the solar heating profile for studies of the thermal balance of Titan; (2) imaging and spectral reflection measurements of the surface for studies of the composition, topography, and physical processes which form the surface as well as for direct measurements of the wind profile during the descent; (3) measurements of the brightness and degree of linear polarization of scattered sunlight including the solar aureole together with measurements of the extinction optical depth of the aerosols as a function of wavelength and altitude to study the size, shape, vertical distribution, optical properties, sources and sinks of aerosols in Titan's atmosphere; and (4) measurements of the spectrum of downward solar flux to study the composition of the atmosphere, especially the mixing ratio profile of methane throughout the descent. We briefly outline the methods by which the flight instrument was calibrated for absolute response, relative spectral response, and field of view over a very wide temperature range. We also give several examples of data collected in the Earth's atmosphere using a spare instrument including images obtained from a helicopter flight program, reflection spectra of various types of terrain, solar aureole measurements including the determination of aerosol size, and measurements of the downward flux of violet, visible, and near infrared sunlight. The extinction optical depths measured as a function of wavelength are compared to models of the Earth's atmosphere and are divided into contributions from molecular scattering, aerosol extinction, and molecular absorption. The test observations during simulated descents with mountain and rooftop venues in the Earth's atmosphere are very important for driving out problems in the calibration and interpretion of the observations to permit rapid analysis of the observations after Titan entry. This revised version was published online in August 2006 with corrections to the Cover Date.     

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.     

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.     

MIDAS – The Micro-Imaging Dust Analysis System for the Rosetta Mission

The International Rosetta Mission is set for a rendezvous with Comet 67 P/Churyumov-Gerasimenko in 2014. On its 10 year journey to the comet, the spacecraft will also perform a fly-by of the two asteroids Stein and Lutetia in 2008 and 2010, respectively. The mission goal is to study the origin of comets, the relationship between cometary and interstellar material and its implications with regard to the origin of the Solar System. Measurements will be performed that shed light into the development of cometary activity and the processes in the surface layer of the nucleus and the inner coma. The Micro-Imaging Dust Analysis System (MIDAS) instrument is an essential element of Rosetta’s scientific payload. It will provide 3D images and statistical parameters of pristine cometary particles in the nm-μm range from Comet 67P/Churyumov-Gerasimenko. According to cometary dust models and experience gained from the Giotto and Vega missions to 1P/Halley, there appears to be an abundance of particles in this size range, which also covers the building blocks of pristine interplanetary dust particles. The dust collector of MIDAS will point at the comet and collect particles drifting outwards from the nucleus surface. MIDAS is based on an Atomic Force Microscope (AFM), a type of scanning microprobe able to image small structures in 3D. AFM images provide morphological and statistical information on the dust population, including texture, shape, size and flux. Although the AFM uses proven laboratory technology, MIDAS is its first such application in space. This paper describes the scientific objectives and background, the technical implementation and the capabilities of MIDAS as they stand after the commissioning of the flight instrument, and the implications for cometary measurements.     

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.     

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.     

Signature of the 11-Year Cycle in the Upper Atmosphere

In the last 45 years I have studied the thermal structure of the atmosphere from the thermosphere down to the stratosphere, and found evidence of its variability in relationship with the change of solar irradiation during the 11-year solar cycle. I would review, in the light of recent model results, the measurements which I had made since the 1960s and which, for some of them, did not find any explanation at the time of their publication. The data were obtained by two different techniques, rockets and lidars and correspond to different regions of the atmosphere from the upper thermosphere to the stratosphere. The expectation was until recently that the atmosphere should be warmed by an increase of solar flux in the course of the solar cycle due to the increase of UV flux. It has been shown to be the case in the tropical stratosphere and at all latitudes in the upper thermosphere. But, at high and mid latitudes and at other altitudes, the reverse situation was found to exist and, until recently, this cooling observed in parts of the atmosphere with increasing solar flux had never been simulated by models. In addition to reviewing our own data, the paper will present recent results using other dataset which support our observations. It is only recently that we succeeded with a model able to tune the forcing by planetary waves at the tropopause level and thus reproduce such behaviour.     

The Infrared Space Observatory (ISO)

The Infrared Space Observatory (ISO), a fully approved and funded project of ESA, will operate at wavelengths from 3–200 microns. The satellite essentially consists of a large cryostat containing about 2300 litres of superfluid helium to maintain the telescope (primary mirror diameter of 60 cm) and the scientific instruments at temperatures between 2K and 8K. A pointing accuracy of a few arc seconds is provided by a three-axis-stabilisation system. ISO's instrument complement consists of four instruments, namely: an imaging photo-polarimeter (3–200 microns), a camera (3–17 microns), a short wavelength spectrometer (3–45 microns) and a long wavelength spectrometer (45–180 microns). ISO's scheduled launch date is May 1993 and it will be operational for at least 18 months. In keeping with ISO's role as an observatory, two-thirds of its observing time will be made available to the general astronomical community via several Calls for Observing Proposals.     

The Galileo Dust Detector

The Galileo Dust Detector is intended to provide direct observations of dust grains with masses between 10^-19 and 10^-9 kg in interplanetary space and in the Jovian system, to investigate their physical and dynamical properties as functions of the distances to the Sun, to Jupiter and to its satellites, to study its interaction with the Galilean satellites and the Jovian magnetosphere. Surface phenomena of the satellites (like albedo variations), which might be effects of meteoroid impacts will be compared with the dust environment. Electric charges of particulate matter in the magnetosphere and its consequences will be studied; e.g., the effects of the magnetic field on the trajectories of dust particles and fragmentation of particles due to electrostatic disruption. The investigation is performed with an instrument that measures the mass, speed, flight direction and electric charge of individual dust particles. It is a multicoincidence detector with a mass sensitivity 10⁶ times higher than that of previous in-situ experiments which measured dust in the outer solar system. The instrument weighs 4.2 kg, consumes 2.4 W, and has a normal data transmission rate of 24 bits s^-1 in nominal spacecraft tracking mode. On December 29, 1989 the instrument was switched-on. After the instrument had been configured to flight conditions cruise science data collection started immediately. In the period to May 18, 1990 at least 168 dust impacts have been recorded. For 81 of these dust grains masses and impact speeds have been determined. First flux values are given.     

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.     

Aerosol-Cloud Interactions Control of Earth Radiation and Latent Heat Release Budgets

Aircraft observations and model simulations show that cloud development is strongly modulated by the impact of cloud-aerosol interactions on precipitation forming processes. New insights into the mechanisms by which aerosols dominate the cloud cover of marine shallow clouds suggest that feedbacks between the cloud microstructure and cloud dynamics through precipitation processes play a major role in determining when a solid cloud cover will break up into a field of trade wind cumulus. Cloud-aerosol interactions dominate not only the dynamics of marine shallow clouds, but also the lifetime and the vertical disposition of latent heat of deep convective clouds over ocean and even more strongly over land. Recent coincident satellite measurements of aerosols and cloud properties quantify the aerosol effects on cloud cover and radiative forcing on regional and global scales. The shapes of the satellite retrieved relations between aerosols and cloud properties are consistent with the suggested ways by which aerosols affect clouds via precipitation processes, particularly by affecting the intensity of the cloud vertical air motions and its vertical development.     

平流层螺旋桨多工况等离子体增效控制方案研究

基于S1223翼型建立了平流层螺旋桨3维模型,在螺旋桨上下表面设置等离子体激励器,设计了5种螺旋桨工况下的等离子体控制方案,采用唯象学等离子体体积力模型进行数值仿真,研究了5种工况下不同等离子体控制方案对螺旋桨拉力和效率的影响。结果表明,设计工况下不宜开启等离子体激励器,采用交流激励时等离子体对高转速前进工况下的螺旋桨控制效果不明显,低速重载工况和滑翔工况下螺旋桨拉力和效率增加,低转速抗风工况下螺旋桨拉力大。采用等离子体流动控制技术提高平流层螺旋桨性能是可行的,需要进一步开展大量研究以优化等离子体激励器的布置方案和控制方案,提高等离子体控制效果,以满足低速临近空间飞行器对推进系统的需求。     

Huygens Probe Aerosol Collector Pyrolyser Experiment

ACP's main objective is the chemical analysis of the aerosols in Titan's atmosphere. For this purpose, it will sample the aerosols during descent and prepare the collected matter (by evaporation, pyrolysis and gas products transfer) for analysis by the Huygens Gas Chromatograph Mass Spectrometer (GCMS). A sampling system is required for sampling the aerosols in the 135'32 km and 22'17 km altitude regions of Titan's atmosphere. A pump unit is used to force the gas flow through a filter. In its sampling position, the filter front face extends a few mm beyond the inlet tube. The oven is a pyrolysis furnace where a heating element can heat the filter and hence the sampled aerosols to 250 °C or 600 °C. The oven contains the filter, which has a thimble-like shape (height 28 mm). For transferring effluent gas and pyrolysis products to GCMS, the carrier gas is a labeled nitrogen ¹⁵N₂, to avoid unwanted secondary reactions with Titan's atmospheric nitrogen. Aeraulic tests under cold temperature conditions were conducted by using a cold gas test system developed by ONERA. The objective of the test was to demonstrate the functional ability of the instrument during the descent of the probe and to understand its thermal behavior, that is to test the performance of all its components, pump unit and mechanisms. In order to validate ACP's scientific performance, pyrolysis tests were conducted at LISA on solid phase material synthesized from experimental simulation. The chromatogram obtained by GCMS analysis shows many organic compounds. Some GC peaks appear clearly from the total mass spectra, with specific ions well identified thanks to the very high sensitivity of the mass spectrometer. The program selected for calibrating the flight model is directly linked to the GCMS calibration plan. In order not to pollute the two flight models with products of solid samples such as tholins, we excluded any direct pyrolysis tests through the ACP oven during the first phase of the calibration. Post probe descent simulation of flight results are planned, using the much representative GCMS and ACP spare models. This revised version was published online in August 2006 with corrections to the Cover Date.     

NEPE高能推进剂凝相燃烧产物的特性分析

通过改进固体推进剂凝相燃烧产物收集装置,在降低系统复杂程度的同时实现了对工作压强的稳定控制。对NEPE高能推进剂在三种工作压强下产生的凝相产物进行了收集,采用粒度分析仪、扫描电镜、X射线能谱仪和X射线衍射仪对获得的凝相燃烧产物进行了深入分析。结果表明,对于NEPE高能推进剂,工作压强对峰值粒度的影响不大,各压强下的平均峰值粒度均在1μm至2μm之间;大部分粒子呈规则球形,少数大粒子会发生形状改变;铝粒子在燃烧室中一般不会全部被氧化成Al2O3。     

Stratosphere NO y Species Measured by MIPAS and GOMOS Onboard ENVISAT During 2002–2010: Influence of Plasma Processes onto the Observed Distribution and Variability

We present observations of stratosphere NO _y species from 2002 to 2010 taken by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and by the Global Ozone Monitoring by Occultation of Stars (GOMOS) instruments on board ENVISAT. We jointly used observations of MIPAS NO₂, HNO₃, N₂O₅, ClONO₂ and N₂O, and GOMOS NO₂ and NO₃. MIPAS results are part of the MIPAS2D database retrieved adopting a full 2D tomographic approach. We describe the mean distribution and variability of NO _y species in the stratosphere, identifying changes induced by plasma processes. Beside enhancements due to sporadic solar proton events, we show that winter polar NO₂ has an almost linear relationship with the geomagnetic activity index Ap down to about 10?hPa. This indicates a dominant role of energetic precipitating particles in the production of upper atmosphere NO _y . The correlation has clear signatures extending to mid latitudes. Partitioning of the NO _y reservoir species are also traced, with HNO₃ and N₂O₅ showing a correlation with Ap extending to lower altitude within the polar regions. We found no large signatures of an impact of thunderstorm-induced plasma processes onto monthly means of NO _y species in the stratosphere.     

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).     

Isotopic Signatures of Presolar Materials in Interplanetary Dust

Interplanetary dust particles collected in the stratosphere frequently exhibit enrichments in deuterium (D) and ¹⁵N relative to terrestrial materials. These effects are most likely due to the preservation of presolar interstellar materials. While the elevated D/H ratios probably resulted from mass fractionation during chemical reactions at very low < 100 K temperatures, the origin of the N isotopic anomalies remains unresolved. The bulk of the N-bearing material may have obtained its isotopic signatures from low temperature chemistry, but a nucleosynthetic origin is also possible. This revised version was published online in August 2006 with corrections to the Cover Date.