Heterogeneous chemistry in the atmosphere of Mars

Hydrogen radicals are produced in the martian atmosphere by the photolysis of water vapour and subsequently initiate catalytic cycles that recycle carbon dioxide from its photolysis product carbon monoxide. These processes provide a qualitative explanation for the stability of the atmosphere of Mars, which contains 95 per cent carbon dioxide. Balancing carbon dioxide production and loss based on our current understanding of the gas-phase chemistry in the martian atmosphere has, however, proven to be difficult. Interactions between gaseous chemical species and ice cloud particles have been shown to be key factors in the loss of polar ozone observed in the Earth's stratosphere, and may significantly perturb the chemistry of the Earth's upper troposphere. Water-ice clouds are also commonly observed in the atmosphere of Mars and it has been suggested previously that heterogeneous chemistry could have an important impact on the composition of the martian atmosphere. Here we use a state-of-the-art general circulation model together with new observations of the martian ozone layer to show that model simulations that include chemical reactions occurring on ice clouds lead to much improved quantitative agreement with observed martian ozone levels in comparison with model simulations based on gas-phase chemistry alone. Ozone is readily destroyed by hydrogen radicals and is therefore a sensitive tracer of the chemistry that regulates the atmosphere of Mars. Our results suggest that heterogeneous chemistry on ice clouds plays an important role in controlling the stability and composition of the martian atmosphere.     

Water activity as the determinant for homogeneous ice nucleation in aqueous solutions

The unique properties of water in the supercooled (metastable) state are not fully understood. In particular, the effects of solutes and mechanical pressure on the kinetics of the liquid-to-solid phase transition of supercooled water and aqueous solutions to ice have remained unresolved. Here we show from experimental data that the homogeneous nucleation of ice from supercooled aqueous solutions is independent of the nature of the solute, but depends only on the water activity of the solution--that is, the ratio between the water vapour pressures of the solution and of pure water under the same conditions. In addition, we show that the presence of solutes and the application of pressure have a very similar effect on ice nucleation. We present a thermodynamic theory for homogeneous ice nucleation, which expresses the nucleation rate coefficient as a function of water activity and pressure. Recent observations from clouds containing ice are in good agreement with our theory and our results should help to overcome one of the main weaknesses of numerical models of the atmosphere, the formulation of cloud processes.     

Direct detection of variable tropospheric clouds near Titan's south pole

Atmospheric conditions on Saturn's largest satellite, Titan, allow the possibility that it could possess a methane condensation and precipitation cycle with many similarities to Earth's hydrological cycle. Detailed imaging studies of Titan have hitherto shown no direct evidence for tropospheric condensation clouds, although there has been indirect spectroscopic evidence for transient clouds. Here we report images and spectra of Titan that show clearly transient clouds, concentrated near the south pole, which is currently near the point of maximum solar heating. The discovery of these clouds demonstrates the existence of condensation and localized moist convection in Titan's atmosphere. Their location suggests that methane cloud formation is controlled seasonally by small variations in surface temperature, and that the clouds will move from the south to the north pole on a 15-year timescale.     

Proximate humid and dry regions in Jupiter's atmosphere indicate complex local meteorology

Models of Jupiter's formation and structure predict that its atmosphere is enriched in oxygen, relative to the Sun, and that consequently water clouds should be present globally near the 5-bar pressure level. Past attempts to confirm these predictions have led to contradictory results; in particular, the Galileo probe revealed a very dry atmosphere at the entry site, with no significant clouds at depths exceeding the 2-bar level. Although the entry site was known to be relatively cloud-free, the contrast between the observed local dryness and the expected global wetness was surprising. Here we analyse near-infrared (around 5 microm) observations of Jupiter, a spectral region that can reveal the water vapour abundance and vertical cloud structure in the troposphere. We find that humid and extremely dry regions exist in close proximity, and that some humid regions are spatially correlated with bright convective clouds extending from the deep water clouds to the visible atmosphere.     

Deep convective clouds with sustained supercooled liquid water down to -37.5 degrees C

In cirrus and orographic wave clouds, highly supercooled water has been observed in small quantities (less than 0.15 g m(-3)). This high degree of supercooling was attributed to the small droplet size and the lack of ice nuclei at the heights of these clouds. For deep convective clouds, which have much larger droplets near their tops and which take in aerosols from near the ground, no such measurements have hitherto been reported. However, satellite data suggest that highly supercooled water (down to -38 degrees C) frequently occurs in vigorous continental convective storms. Here we report in situ measurements in deep convective clouds from an aircraft, showing that most of the condensed water remains liquid down to -37.5 degrees C. The droplets reach a median volume diameter of 17 microm and amount to 1.8 gm(-3), one order of magnitude more than previously reported. At slightly colder temperatures only ice was found, suggesting homogeneous freezing. Because of the poor knowledge of mixed-phase cloud processes, the simulation of clouds using numerical models is difficult at present. Our observations will help to understand these cloud processes, such as rainfall, hail, and cloud electrification, together with their implications for the climate system.     

A modeling study of relation between cloud amount and SST over western tropical pacific cloudy regions during TOGA COARE

The relationship between cloud amount and sea surface temperature (SST) over western tropical Pacific cloudy regions during TOGA COARE is investigated based on hourly grid simulation data from a two-dimensional coupled ocean-cloud resolving atmosphere model. The model is forced by the large-scale vertical velocity and zonal wind observed and derived from TOGA COARE for a 50-day period. The cloud amount becomes smaller when the ocean surface gets warmer, which is similar to previous relations obtained from observational analyses. As SST increases, the atmospheric temperature increases whereas the surface sensible heat flux decreases. The atmospheric water vapor is not sensitive to SST whereas the surface evaporation flux decreases as SST increases. These indicate that the oceanic effects do not play an important role in determining atmospheric heat and water vapor budgets. The cold atmosphere produces a larger amount of ice clouds that cover a larger area than the warm atmosphere does. The large amounts of ice clouds lead to cooling of the ocean surface through reflecting large amount of solar radiation back to the space. Thus, the negative correlation between the cloud amount and SST only accounts for the important atmospheric effects on the ocean.     

飞机电热除冰的研究进展与展望

 飞机在结冰气象条件下容易发生结冰现象,冰的存在会破坏飞机气动特性,影响飞行安全,严重结冰可导致机毁人亡,故必须及时将冰移除。电热除冰是目前最常考虑的除冰方式之一,本文系统介绍了电热除冰装置及其工作原理。首先,主要围绕除冰过程的传热特性、冰层力学特性和冰脊的形成,详细阐述了国内外电热除冰研究的发展。然后,针对国内外研究存在的一些问题,提出了几点对电热除冰研究的粗略想法,电热除冰数值计算方法和模拟技术研究、热力耦合特性对冰层融化和力学特性的影响研究、冰脱落准则和运动规律研究是未来研究需要重视的方向。     

Evidence for a link between global lightning activity and upper tropospheric water vapour

Tropospheric water vapour is a key element of the Earth's climate, which has direct effects as a greenhouse gas, as well as indirect effects through interaction with clouds, aerosols and tropospheric chemistry. Small changes in upper-tropospheric water vapour have a much larger impact on the greenhouse effect than small changes in water vapour in the lower atmosphere, but whether this impact is a positive or negative feedback remains uncertain. The main challenge in addressing this question is the difficulty in monitoring upper-tropospheric water vapour globally over long timescales. Here I show that upper-tropospheric water-vapour variability and global lightning activity are closely linked, suggesting that upper-tropospheric water-vapour changes can be inferred from records of global lightning activity, readily obtained from observations at a single location on the Earth's surface. This correlation reflects the fact that continental deep-convective thunderstorms transport large amounts of water vapour into the upper troposphere and thereby dominate the variations of global upper-tropospheric water vapour while producing most of the lightning on Earth. As global lightning induces Schumann resonances, an electromagnetic phenomenon in the atmosphere that can be observed easily at low cost, monitoring of these resonances might provide a convenient method for tracking upper-tropospheric water-vapour variability and hence contribute to a better understanding of the processes affecting climate change.     

Meteorology: dusty ice clouds over Alaska

Particles lofted into the atmosphere by desert dust storms can disperse widely and affect climate directly through aerosol scattering and absorption. They can also affect it indirectly by changing the scattering properties of clouds and, because desert dusts are particularly active ice-forming agents, by affecting the formation and thermodynamic phase of clouds. Here I show that dust storms that occurred in Asia early in 2004 created unusual ice clouds over Alaska at temperatures far warmer than those expected for normal cirrus-cloud formation.     

The impact of humidity above stratiform clouds on indirect aerosol climate forcing

Some of the global warming from anthropogenic greenhouse gases is offset by increased reflection of solar radiation by clouds with smaller droplets that form in air polluted with aerosol particles that serve as cloud condensation nuclei. The resulting cooling tendency, termed the indirect aerosol forcing, is thought to be comparable in magnitude to the forcing by anthropogenic CO2, but it is difficult to estimate because the physical processes that determine global aerosol and cloud populations are poorly understood. Smaller cloud droplets not only reflect sunlight more effectively, but also inhibit precipitation, which is expected to result in increased cloud water. Such an increase in cloud water would result in even more reflective clouds, further increasing the indirect forcing. Marine boundary-layer clouds polluted by aerosol particles, however, are not generally observed to hold more water. Here we simulate stratocumulus clouds with a fluid dynamics model that includes detailed treatments of cloud microphysics and radiative transfer. Our simulations show that the response of cloud water to suppression of precipitation from increased droplet concentrations is determined by a competition between moistening from decreased surface precipitation and drying from increased entrainment of overlying air. Only when the overlying air is humid or droplet concentrations are very low does sufficient precipitation reach the surface to allow cloud water to increase with droplet concentrations. Otherwise, the response of cloud water to aerosol-induced suppression of precipitation is dominated by enhanced entrainment of overlying dry air. In this scenario, cloud water is reduced as droplet concentrations increase, which diminishes the indirect climate forcing.     

冰与混凝土坝坡间的冻结强度模拟试验

根据实际水库观测冰盖与护坡的冻结情况，在实验室内进行模拟水库冰盖与护坡局部断面的冻结试验．采用冰与混凝土板间的冻结，进行一次冻结、多次冻结、冰晶冻结、雪冰冻结等模式．分析出冰压力与冻结力的关系；在不同温度下测得各种冻结情况中的冻结强度，给出冻结强度随着温度变化的规律和数值．其结果为寒区平原水库坝坡抵抗冰推力破坏提供了设计参数．     

Detection of stratospheric ozone intrusions by windprofiler radars

Stratospheric ozone attenuates harmful ultraviolet radiation and protects the Earth's biosphere. Ozone is also of fundamental importance for the chemistry of the lowermost part of the atmosphere, the troposphere. At ground level, ozone is an important by-product of anthropogenic pollution, damaging forests and crops, and negatively affecting human health. Ozone is critical to the chemical and thermal balance of the troposphere because, via the formation of hydroxyl radicals, it controls the capacity of tropospheric air to oxidize and remove other pollutants. Moreover, ozone is an important greenhouse gas, particularly in the upper troposphere. Although photochemistry in the lower troposphere is the major source of tropospheric ozone, the stratosphere-troposphere transport of ozone is important to the overall climatology, budget and long-term trends of tropospheric ozone. Stratospheric intrusion events, however, are still poorly understood. Here we introduce the use of modern windprofiler radars to assist in such transport investigations. By hourly monitoring the radar-derived tropopause height in combination with a series of frequent ozonesonde balloon launches, we find numerous intrusions of ozone from the stratosphere into the troposphere in southeastern Canada. On some occasions, ozone is dispersed at altitudes of two to four kilometres, but on other occasions it reaches the ground, where it can dominate the ozone density variability. We observe rapid changes in radar tropopause height immediately preceding these intrusion events. Such changes therefore serve as a valuable diagnostic for the occurrence of ozone intrusion events. Our studies emphasize the impact that stratospheric ozone can have on tropospheric ozone, and show that windprofiler data can be used to infer the possibility of ozone intrusions, as well as better represent tropopause motions in association with stratosphere-troposphere transport.     

Biosignatures as revealed by spectropolarimetry of Earthshine

Low-resolution intensity spectra of Earth's atmosphere obtained from space reveal strong signatures of life ('biosignatures'), such as molecular oxygen and methane with abundances far from chemical equilibrium, as well as the presence of a 'red edge' (a sharp increase of albedo for wavelengths longer than 700?nm) caused by surface vegetation. Light passing through the atmosphere is strongly linearly polarized by scattering (from air molecules, aerosols and cloud particles) and by reflection (from oceans and land). Spectropolarimetric observations of local patches of Earth's sky light from the ground contain signatures of oxygen, ozone and water, and are used to characterize the properties of clouds and aerosols. When applied to exoplanets, ground-based spectropolarimetry can better constrain properties of atmospheres and surfaces than can standard intensity spectroscopy. Here we report disk-integrated linear polarization spectra of Earthshine, which is sunlight that has been first reflected by Earth and then reflected back to Earth by the Moon. The observations allow us to determine the fractional contribution of clouds and ocean surface, and are sensitive to visible areas of vegetation as small as 10 per cent. They represent a benchmark for the diagnostics of the atmospheric composition, mean cloud height and surfaces of exoplanets.     

The test freezing temperature of C2―C6 dicarboxylic acid: The important indicator for ice nucleation processes

The importance of organic compounds as significant constituents of atmospheric aerosols, and cloud condensation nuclei （CCN）, as well as players influencing the tropospheric oxidation and atmospheric energy budget, have been increasingly recognized. Low molecular weight dicarboxylic acids （LMW-DCAs） are significant identified portions of atmospheric condensed matter including aerosols, fog and clouds. Besides the photochemical transformation of DCA, the implication of organic matter in ice nucleation processes has been considered. In this study, we investigated the freezing temperature of pure and mixed （C2-C6） DCA solutions in ultra-pure water and tap water solution droplets using a freezing nucleus counter at different pH, and in different water ionic conditions. The mean freezing temperature of different mixture of LMW-DCA in ultra-pure and tap water solution droplets ranged from -24.1±2.8 to -21.3±3.9℃ and -10.2±2.2 to -9.5±2.2℃, respectively. The mean freezing temperature of the control （ultra-pure and tap） water droplets （-22.6±3.5℃, 11.2±2.4℃） was also measured. The results, and their implications in atmospheric chemistry and physics of the atmosphere will be discussed.     

过冷水雾相变传播及温度场的实验研究

实验表明在过冷水雾相变传播过程中伴随有脉冲型单峰形式的温度上升,相变传播速率约为1．2cm/s,温度的波形和峰值以及相变的传播速度与过冷水雾的初始温度基本无关,据此对过冷水雾冰晶机制作了探讨。     

Contribution of cloud condensate to surface rainfall process

Contribution of cloud condensate to surface rainfall processes is investigated in a life span of tropical convection based on hourly data from a two-dimensional cloud resolving simulation. The model is forced by the large-scale vertical velocity, zonal wind and horizontal advections obtained from tropical ocean global atmosphere coupled ocean-atmosphere response experiment (TOGA COARE). The results show that during the genesis, development, and decay of tropical convection, calculations with water vapor overestimate surface rain rate, and cloud condensate plays an important role in correcting overestimation in surface rain rates. The analysis is carried out in deep convective clouds and anvil clouds during the development of tropical convection. The surface rain rates calculated with water vapor in deep convective clouds and anvil clouds have similar magnitudes, the large surface rain rate appears in deep convective clouds due to the consumption of water hydrometeors whereas the small surface rain rate occurs in anvil clouds because of the gain of ice hydrometeors. Further analysis of the grid data shows that the surface rain rates calculated with water vapor and with cloud condensate are negatively correlated with the correlation coefficient of -0.85, and the surface rain rate calculated with cloud condensate is mainly contributed to the water hydrometeors in the tropical deep convective regime.     

Dusty cloud radiative forcing derived from satellite data for middle latitude regions of East Asia

The dusty cloud radiative forcing over the middle latitude regions of East Asia was estimated by using the 2-year (July 2002?June 2004) data of collocated clouds and the Earth’s radiant energy system (CERES) scanner and moderate resolution imaging spectroradiometer (MODIS) from Aqua Edition 1B SSF (single scanner footprint). The dusty cloud is defined as the cloud in dust storm environment or dust contaminated clouds. For clouds growing in the presence of dust, the instantaneous short-wave (SW) forcing at the top of the atmosphere (TOA) is about -275.7 W/m² for cloud over dust (COD) region. The clouds developing in no-dust cloud (CLD) regions yield the most negative short-wave (SW) forcing (-311.0 W/m²), which is about 12.8% stronger than those in COD regions. For long-wave (LW) radiative forcing, the no-dust cloud (CLD) is around 102.8 W/m², which is 20% less than the LW forcing from COD regions. The instantaneous TOA net radiative forcing for the CLD region is about -208.2 W/m², which is 42.1% larger than the values of COD regions. The existence of dust aerosols under clouds significantly reduces the cooling effect of clouds.     

Polar methane accumulation and rainstorms on Titan from simulations of the methane cycle

Titan has a methane cycle akin to Earth's water cycle. It has lakes in polar regions, preferentially in the north; dry low latitudes with fluvial features and occasional rainstorms; and tropospheric clouds mainly (so far) in southern middle latitudes and polar regions. Previous models have explained the low-latitude dryness as a result of atmospheric methane transport into middle and high latitudes. Hitherto, no model has explained why lakes are found only in polar regions and preferentially in the north; how low-latitude rainstorms arise; or why clouds cluster in southern middle and high latitudes. Here we report simulations with a three-dimensional atmospheric model coupled to a dynamic surface reservoir of methane. We find that methane is cold-trapped and accumulates in polar regions, preferentially in the north because the northern summer, at aphelion, is longer and has greater net precipitation than the southern summer. The net precipitation in polar regions is balanced in the annual mean by slow along-surface methane transport towards mid-latitudes, and subsequent evaporation. In low latitudes, rare but intense storms occur around the equinoxes, producing enough precipitation to carve surface features. Tropospheric clouds form primarily in middle and high latitudes of the summer hemisphere, which until recently has been the southern hemisphere. We predict that in the northern polar region, prominent clouds will form within about two (Earth) years and lake levels will rise over the next fifteen years.     

An amorphous solid state of biogenic secondary organic aerosol particles

Secondary organic aerosol (SOA) particles are formed in the atmosphere from condensable oxidation products of anthropogenic and biogenic volatile organic compounds (VOCs). On a global scale, biogenic VOCs account for about 90% of VOC emissions and of SOA formation (90?billion kilograms of carbon per year). SOA particles can scatter radiation and act as cloud condensation or ice nuclei, and thereby influence the Earth's radiation balance and climate. They consist of a myriad of different compounds with varying physicochemical properties, and little information is available on the phase state of SOA particles. Gas-particle partitioning models usually assume that SOA particles are liquid, but here we present experimental evidence that they can be solid under ambient conditions. We investigated biogenic SOA particles formed from oxidation products of VOCs in plant chamber experiments and in boreal forests within a few hours after atmospheric nucleation events. On the basis of observed particle bouncing in an aerosol impactor and of electron microscopy we conclude that biogenic SOA particles can adopt an amorphous solid-most probably glassy-state. This amorphous solid state should provoke a rethinking of SOA processes because it may influence the partitioning of semi-volatile compounds, reduce the rate of heterogeneous chemical reactions, affect the particles' ability to accommodate water and act as cloud condensation or ice nuclei, and change the atmospheric lifetime of the particles. Thus, the results of this study challenge traditional views of the kinetics and thermodynamics of SOA formation and transformation in the atmosphere and their implications for air quality and climate.     

Isotopic evidence for Mesoarchaean anoxia and changing atmospheric sulphur chemistry

The evolution of the Earth's atmosphere is marked by a transition from an early atmosphere with very low oxygen content to one with an oxygen content within a few per cent of the present atmospheric level. Placing time constraints on this transition is of interest because it identifies the time when oxidative weathering became efficient, when ocean chemistry was transformed by delivery of oxygen and sulphate, and when a large part of Earth's ecology changed from anaerobic to aerobic. The observation of non-mass-dependent sulphur isotope ratios in sedimentary rocks more than approximately 2.45 billion years (2.45 Gyr) old and the disappearance of this signal in younger sediments is taken as one of the strongest lines of evidence for the transition from an anoxic to an oxic atmosphere around 2.45 Gyr ago. Detailed examination of the sulphur isotope record before 2.45 Gyr ago also reveals early and late periods of large amplitude non-mass-dependent signals bracketing an intervening period when the signal was attenuated. Until recently, this record has been too sparse to allow interpretation, but collection of new data has prompted some workers to argue that the Mesoarchaean interval (3.2-2.8 Gyr ago) lacks a non-mass-dependent signal, and records the effects of earlier and possibly permanent oxygenation of the Earth's atmosphere. Here we focus on the Mesoarchaean interval, and demonstrate preservation of a non-mass-dependent signal that differs from that of preceding and following periods in the Archaean. Our findings point to the persistence of an anoxic early atmosphere, and identify variability within the isotope record that suggests changes in pre-2.45-Gyr-ago atmospheric pathways for non-mass-dependent chemistry and in the ultraviolet transparency of an evolving early atmosphere.