Processing of atmospheric organic matter by California radiation fogs

Considerable effort has been put into characterizing the ionic composition of fogs and clouds over the past twenty-five years. Recently it has become evident that clouds and fogs often contain large concentrations of organic material as well. Here we report findings from a series of studies examining the organic composition of radiation fogs in central California. Organic compounds in these fogs comprise a major fraction of total solute mass, with total organic carbon sometimes reaching levels of several tens of mg/L. This organic matter is comprised of a wide variety of compounds, ranging from low molecular weight organic acids to high molecular weight compounds with molecular masses approaching several hundred to a thousand g/mole. The most abundant individual compounds are typically formic acid, acetic acid, and formaldehyde. High concentrations are also observed of some dicarboxylic acids (e.g., oxalate) and dicarbonyls (e.g., glyoxal and methylglyoxal) and of levoglucosan, an anhydrosugar characteristically emitted by biomass combustion. Many other compounds have been identified in fog water by GC/MS, including long chain n-alkanoic acids, n-alkanes, PAH, and others, although these compounds typically comprise a total of only a few percent of fog TOC. Measurements of fog scavenging of organic and elemental carbon reveal preferential scavenging of organic carbon. Tracking of individual organic compounds utilized as source type markers suggests the fogs differentially scavenge carbonaceous particles from different source types, with more active processing of wood smoke than vehicle exhaust. Observations of high deposition velocities of fog-borne organic carbon, in excess of 1 cm/s, indicate that fogs in the region represent an important mechanism for cleansing the atmosphere of pollution.     

The chemical composition of fogs and intercepted clouds in the United States

Over the past decade, the chemical compositions of fogs and intercepted clouds have been investigated at more than a dozen locations across the United States. Sampling sites have been located in the northeast, southeast, Rocky Mountain, and west coast regions of the US. They include both pristine and heavily polluted locations. Frontal/orographic clouds (warm and supercooled), intercepted coastal stratiform clouds, and radiation fogs have all been examined. Sample pH values range from below 3 to above 7. Major ions also exhibit a wide concentration range, with clouds at some locations exhibiting high sea salt concentrations, while composition at other locations is dominated by ammonium and sulfate or nitrate.     

Estimation of fog deposition on epiphytic bryophytes in a subtropical montane forest ecosystem in northeastern Taiwan

The fog meteorology, fog chemistry and fog deposition on epiphytic bryophytes were investigated from July 2000 to June 2001 in the Yuanyang Lake forest ecosystem. The elevation of the site ranges from 1650 to 2420 m, at which the high frequency of fog occurrence throughout the year has been thought to be of benefit to the establishment of the primary Taiwan yellow cypress forest [Chamaecyparis obtusa var. formosana (Hayata) Rehder] and to the extensive growth of the epiphytic bryophytes. A weather station including a visibility sensor and an active fog collector was installed for fog meteorological and chemical study. The fog deposition rate on epiphytic bryophytes was estimated by measuring the increase rate in plant weight when exposed to fog. Average fog duration of 4.7 and 11.0 h per day was measured in summer months (June to August) and the rest of the year, respectively. November 2000 was the foggiest month in which the average fog duration reached 14.9 h per day. The ionic composition of fog water revealed that the area was less polluted than expected from literature data. The in situ exposure experiments done with the dominant epiphytic bryophytes showed an average fog deposition rate of 0.63 g H₂O g⁻¹ d. w. h⁻¹, which approximated 0.17 mm h⁻¹ at the stand scale. The nutrient fluxes estimated for February 2001 showed that for all ions, more than 50% of the ecosystem input was through fog deposition. These results demonstrate the importance of epiphytic bryophytes and fog deposition in nutrient cycling of this subtropical montane forest ecosystem. The incorporation of fog study in the long-term ecosystem research projects is necessary in this area.     

南京市紫外线辐射强度的变化及影响因子

利用南京市2005-02—2009-01共4 a的紫外线辐射观测资料,分析了到达地面的紫外线辐射强度的变化特征,并探讨了云、污染物浓度和雾、霾天气等对紫外线辐射强度的影响。结果表明,低云量对紫外线强度的衰减更明显,最大达58.15%,蔽光性云层对紫外线辐射强度的衰减可达71%～80%;紫外线辐射强度与污染物浓度呈负相关,其中与NO2的相关性最好,为-0.39;晴空条件下,严重霾对紫外线辐射强度的衰减率可达20%以上,浓雾对紫外线辐射强度的衰减接近50%。     

近53年辽宁雾的时空分布及成因分析

利用1951～2003年辽宁12个代表站的雾资料,分析了雾的时空分布特征及形成条件。结果表明:辽宁年平均雾日地域分布呈现两高三低的形势。雾日的年际变化曲线较平稳,雾日最多的年份和最少的年份相差17d。沈阳与大连雾日变化相反,大连呈下降趋势,沈阳则在平稳中略有上升。辽宁大雾每个月都可形成,但沿海地区和内陆又有所差异,沿海地区主要出现在5～8月,而内陆地区主要出现在8～11月。雾日的天气形势可分为5～7种类型,其中以倒槽型、锋面气旋型、地形槽型、冷高压前部型最为典型。     

2006年12月南京连续4天浓雾的微物理结构及演变特征

2006年12月24-27日南京地区出现了连续4天的浓雾天气,其中能见度小于50 m的强浓雾持续了40多个小时.利用FM-100型雾滴谱仪,连续观测了雾滴谱、数密度和含水量等微物理参量.结合自动气象站及能见度仪观测资料,分析了这次浓雾过程的微物理特征,并与1996年观测结果进行对比:雾滴的平均含水量和平均直径与1996年观测结果相当,含水量最大值比1996年观测结果大4倍,数密度比10年前小.认为前2个子过程的雾滴数密度、含水量很高,造成了南京奉次大雾能见度长时间低于50 m的恶劣天气.结合边界层探空资料,认为形成这种强浓雾的主要原因足近地层持续存在强盛的水汽平流,具有平流雾的特征.根据雾微物理参量的起伏变化,将浓雾过程分成4个子过稃,分析并比较了4个子过程的雾滴谱分布,总过程的谱分布及4个子过程的谱分布都服从Dcirmendjian分布,谱型都基本呈指数下降,雾滴主要集中存小滴段.最后,对第一个子过程微物理参量的变化特征进行了细致分析.发现这次浓雾是在夜间晴空辐射降温后形成的,午夜最强,日出后随着气温的升高逐渐减弱,反映了辐射雾的口变化特征.另外,还发现雾形成以后,开始变化不大,但随着进一步辐射降温,地面雾团不断产牛,雾爆发性发展.     

Case study of cloud physical and chemical processes in low clouds at Mt. Brocken

Frequency distributions of cloud base height and cloud type of low clouds observed between May and October 1998 at Mt. Brocken (Germany) have been derived from ceilometer measurements and synoptic observations. The summit at 1142 m a.s.l. was about 50% of that time in cloud. During daytime, Stratus clouds were the dominant cloud type (65%), whereas Cumulus clouds amounted to 27% and Stratocumulus clouds to 8%. Evidence was found that the increase of the cloud base height observed at Mt. Brocken continues since the end of the 1980s. An example for a clear anticorrelation between the liquid water content (LWC) of the cloud and the height above cloud base is shown. Other results of this detailed case study of a cloud event on October 8, 1998 concerning phase partitioning of water-soluble inorganic compounds, black carbon (BC) and organic carbon (OC) between the liquid and the interstitial phase will also be presented. The observed ion-specific increase in the solute mass per cubic meter of air with decrease of the distance between sampling position and cloud base was caused mainly by entrainment of air from the below-cloud layer. As expected, for sulfate, ammonia and nitrate, high scavenging coefficients (>0.8) were found. OC exhibits a high scavenging fraction of between 0.4 and 0.7; the value for black carbon (0.2–0.4) implies that soot was possibly to some extent internally mixed in the cloud condensation nuclei (CCN). Simultaneous measurements during a cloud event of HNO₂ and HNO₃ in the gas phase and N(III) and N(V) in the liquid phase were made for the first time.     

Exploring fog as a supplementary water source in Namibia

Namibia is an arid country where many rural and urban centres depend on ephemeral rivers for their water supply. These water sources are, however, limited and display seasonal salinisation. Fog occurs along the coast and extends for some distance inland, and it could be used as a source of drinking water. Data on groundwater salinisation and fog deposition were collected at villages of the indigenous communities and at the Gobabeb Training and Research Centre (GTRC) in the Central Namib Desert. Fog collection experiments were done with Standard Fog Collectors (SFCs) and 1-m² fog collectors made from the Raschel mesh that is used in SFCs from 1996 onwards. The results indicate that fog occurs throughout the year and that it has low major ion concentrations (chemical composition). The period of high fog deposition coincides with that of high groundwater salinity and would suit mixing of the two waters to provide water of good drinking quality to people in these areas. In conclusion, fog is a viable source of water in the Namib and could supplement traditional sources in rural settlements and perhaps also in urban water supply schemes in this region as in other parts of the world where it is used as a source of drinking water.

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Role of organic acids (formic, acetic, pyruvic and oxalic) in the formation of cloud condensation nuclei (CCN): a review

Although it is believed that organic aerosols play a key role in cloud nucleation and make an important contribution to the cloud condensation nuclei (CCN) population, their specific species remain poorly characterized. This paper reviews the current knowledge of organic acids (mainly formic, acetic, pyruvic and oxalic acids). Without specification, organic acids in this paper refer to these four organic acids in the gas and aerosol phases. This paper analyzes the extent to which organic acids act as CCN and compares the physical and chemical properties of organic acids with those of CCN. The results show that aerosol formate and acetate concentrations range from 0.02 to 5.3 nmol m⁻³ and from 0.03 to 12.4 nmol m⁻³, respectively, and that between 34 to 77% of formate and between 21 to 66% of acetate are present in the fine fraction of aerosols. It was found that although most (98–99%) of these volatile organic acids are present in the gas phase, their concentrations in the aerosol particles are sufficient to make them a good candidate for CCN. The results also show that organic acids may make an important contribution to the formation of CCN in some special sources such as vegetation emissions and biomass-burning. Organic acids are expected to contribute significantly to the estimates of indirect (cloud-mediated) forcing due to aerosols.     

The degree of Cl-loss for the particulate matter (PM) and fog water sampled at the same air mass at the Hachimantai mountain range in northern Japan

It is well known that sea-salt aerosols in particulate matter (PM) react with acids such as H₂SO₄ and HNO₃ during transportation and thereby lose chloride ions (Cl-loss). The PM and fog were sampled concurrently at different altitudes in the Hachimantai mountain range, northern Japan. The PM and fog sampled at different altitudes had nearly identical properties for the ion components. However, the PM was in a Cl-depleted state (more than 80% of all samples), but the fog water was not in so Cl-depleted state (less than 29%). As a result, it could be explained that this phenomenon caused because the fog droplets took up the gaseous state HCl other than sea-salt PM. After all Cl^- in the fog water recovered and was rather rich compared with the sea-salt or the PM by the uptake of the gaseous state HCl. Moreover, it was found that for PM_coarse(2.5 < D < 10), 86% of the acid (H₂SO₄ and HNO₃) was consumed for Cl-loss reactions and/or for dissolution of Ca and Mg in soil particles.     

Advective, orographic and radiation fog in the Tarapacá region, Chile

A project in northern Chile was undertaken to determine the origin and behaviour of fog in the coastal and inland locations of the Tarapacá Region. In the Pampa del Tamarugal, 50 km from the sea, conditions exist for the formation of radiation fog. Advective fog has been studied on the coast and orographic fog was observed at a few coastal sites near mountain ranges with elevations above 1000 m. Fog water collected by two standard fog collectors (SFC) for 3 1/2 years showed an average flux of 8.5 l m⁻² day⁻¹ on the coast and 1.1 l m⁻² day⁻¹ inland 12 km from the coastline. On only a few days in 10 months was water collected at the inland site of Pampa del Tamarugal. GOES satellite images are shown to illustrate the pattern of formation of the stratocumuli cloud over the sea, its approach to the coastline, the entrance of fog by corridors through the coastal range and the presence of radiation fog inland. The results are important for the understanding of fog formation and dissipation along the coastal mountain range and for the recognition of potential sites for the installation of fog water collectors, which can be used as a water source in the Atacama Desert. The results also provide vital information for use in the preservation of the unique ecosystems of the most arid desert of the world.     

Pollutant concentrations in fog and low cloud water at selected sites of the Czech Republic

In this paper, the basic composition of fog and low cloud water are presented, resulting from the analyses of water samples from 111 fog/cloud events. The samples were collected at five sites located in various regions of the Czech Republic. Two sampling sites are in mountainous regions and three sites represent various urban areas. The mountain stations are located in two regions of the Czech Republic with different industry types. At all the sites, active fog collectors were employed. In the water samples, the conductivity, acidity (pH), cations (H⁺, Na⁺, K⁺, NH₄⁺, Mg²⁺, Ca²⁺) and anions (F⁻, Cl⁻, NO₃⁻, SO₄²⁻) were determined.A mean pH value of about 4.5 was obtained at mountain sites whereas the measurements in urban areas showed mean pH values from 4.9 to 6.4. The mean conductivity values in the samples from the two mountain stations were 137 and 191.5 μS cm⁻¹. The samples from urban sites showed mean values between 127.7 and 654.4 μS cm⁻¹. The maximum concentration means for the three dominant pollutants (expressed by the ratio mountain sites/urban sites) are 32.9/99.6 mg l⁻¹ for NO₃⁻, 32.5/192.9 mg l⁻¹ for SO₄²⁻ and 18.5/52.7 mg l⁻¹ for NH₄⁺. As expected, we found higher ion concentrations in the northern part of the Czech Republic where larger numbers of lignite-burning power plants, chemical factories and opencast lignite mines are located. A decrease in ion concentrations was observed at higher altitude sites, probably reflecting at least in part higher liquid water contents at these locations.     

Chromophoric Dissolved Organic Matter (CDOM) In Rainwater,Southeastern North Carolina,USA

The abundance and optical characteristics of dissolved organic matter (DOM) were determined in 120 rain samples collected in Wilmington, North Carolina, USA, between February 21, 2002 and August 11, 2003. All rainwater samples contained chromophoric dissolved organic matter (CDOM) as well as fluorescent compounds. The absorbance spectra of CDOM in the samples decreased exponentially with wavelength with little or no measurable absorbance past 550 nm. Fluorescence excitation emission spectra (EEMS) of the precipitation revealed the presence of four major peaks indicating both terrestrial and marine influences. There was a strong positive correlation between total integrated fluorescence and the absorbance coefficient at 300 nm in rainwater samples, suggesting that these optical properties are directly interrelated and that the compounds responsible for absorbance may be the same as those responsible for fluorescence. Air-mass back-trajectory analysis indicated elevated CDOM levels in continentally influenced rainwater relative to marine dominated events implying that anthropogenic and/or terrestrial sources are important contributors to CDOM levels in precipitation. The presence of highly absorbing and fluorescing CDOM in rainwater has significant ramifications in atmospheric chemistry and may play a previously unrecognized role in the wavelength dependent spectral attenuation of solar radiation by atmospheric waters.     

Numerical study of droplet size dependent chemistry in oceanic,wintertime stratus cloud at southern mid-latitudes

Cloud droplet chemistry is modelled for the first 150 m of rise in a wintertime, mid-latitude, marine stratus cloud using observations made at and near the Cape Grim Baseline Station as a source of input parameters. The emphasis in this work was to study the variation in droplet chemistry as a function of both droplet size and nucleus composition, with a particular focus on the way in which oxidation of dissolved sulfur dioxide varied.At 150 m above the condensation level, solute concentration as a function of droplet size was found to increase by as much as 2 to 3 orders of magnitude for only a factor of 2 increase in droplet radius, primarily as a consequence of the 1/r dependence in the droplet growth equation. This type of size dependence exists at all levels in the model cloud, and has a significant influence on oxidation rate of sulfur dioxide in droplets growing on sulfate nuclei, oxidation by ozone being favoured in the smallest droplets, but oxidation by hydrogen peroxide being favoured in the larger droplets. Oxidation by ozone is favoured at all sizes in droplets formed on sea-salt nuclei as a result of the initially high alkalinity of these droplets, and in the cloud overall is calculated to be the more important oxidation pathway. Although based on a simplified chemical scheme, these results suggest that both size-dependent and nucleus-dependent chemistry of cloud droplets may need to be considered explicitly in cloud modelling work.Volume-weighted mean pH values in the range 5 to 6 were predicted from sensitivity studies in which input variables were varied over reasonable ranges, in agreement with two sets of bulk cloud-water pH data obtained by aircraft near Cape Grim.     

Cloud contribution to the daily and annual radiation budget in a mountainous valley

An automated-ventilated radiation station has been set up in a mountainous valley at the Logan Airport in northern Utah, USA, since mid-1995, to evaluate the daily and annual radiation budget components, and develop an algorithm to study cloudiness and its contribution to the daily and annual radiation. This radiation station (composed of pyranometers, pyrgeometers and a net radiometer) provides continuous measurements of downward and upward shortwave, longwave and net radiation throughout the year. The surface temperature and pressure, the 2-m air temperature and humidity, precipitation, and wind at this station were also measured. A heated rain gauge provided precipitation information. Using air temperature and moisture and measured downward longwave (atmospheric) radiation, appropriate formula (among four approaches) was chosen for computation of cloudless-skies atmospheric emissivity. Considering the additional longwave radiation during the cloudy skies coming from the cloud in the waveband which the gaseous emission lacks (from 8–13 μm), an algorithm was developed which provides continuous 20-min cloud information (cloud base height, cloud base temperature, percent of skies covered by cloud, and cloud contribution to the radiation budget) over the area during day and night. On the partly-cloudy day of 3 February, 2003, for instance, cloud contributed 1.34 MJ m^− 2 d^− 1 out of 26.92 MJ m^− 2 d^− 1 to the daily atmospheric radiation. On the overcast day of 18 December, 2003, this contribution was 5.77 MJ m^− 2 d^− 1 out of 29.38 MJ m^− 2 d^− 1. The same contribution for the year 2003 amounted to 402.85 MJ m^− 2 y^− 1 out of 9976.08 MJ m^− 2 y^− 1. Observations (fog which yielded a zero cloud base height and satellite cloud imaging data) throughout the year confirmed the validity of the computed data. The nearby Bowen ratio station provided the downward radiation and net radiation data. If necessary, these data could be substituted for the missing data at the radiation station. While the automated surface observing systems (ASOS) ceilometer at the Logan airport provides only the overhead cloud information, the proposed algorithm provides this information over the valley. The proposed algorithm is a promising approach for evaluation of the cloud base temperature, cloud base height, percent of skies covered by cloud, and cloud contribution to the daily and annual radiation budget at local and regional scales.     

气候模式中云的次网格结构对全球辐射影响的研究

利用一种用于大尺度天气、气候模式的随机云产生器(SCG)和独立气柱近似(ICA)辐射算法,研究了次网格云的水平结构以及垂直重叠结构对全球辐射场的影响.比较了水平非均匀云(IHCLD)和水平均匀云(HCLD)的辐射场差异以及云的最大.随机重叠(MRO)和一般重叠(GenO)的辐射场差异.结果显示,与HCLD相比,IHCLD一方面可增加地面净短波辐射通量,纬向平均最大值(约1W/m~2)和次大值(约0.6 W/m~2)分别位于高纬度低云密集地区和对流旺盛的热带地区;另一方面可增加大气顶的净长波辐射通量,纬向平均最大值(0.3 W/m~2)出现在热带地区.不同的重叠结构对短波和长波辐射收支也有很大的影响.MRO和GenO的短波辐射通量差异在热带辐合带最大.达到30-40W/m~2,在高纬度低云带的纬向平均也可达到5W/m~2左右;长波辐射通量差异具有相似的地区分布,但量值相对较小.不同重叠结构可以造成大气上下层的辐射加热率差异,影响大气热力层结.云的水平和垂直结构对有云区域辐射收支的影响将改变大气热力、动力状况以及水汽条件,从而影响模拟的气候系统的演变.文中采用单向云-辐射计算,排除了与气候系统其他过程复杂的相互作用,从而使其结果具有一定的普适性,可为不同大尺度模式进行次网格云辐射参数化提供参考.     

Soluble organic compounds in fog and cloud droplets: what have we learned over the past few years?

We have recently set up a new procedure for characterising the water soluble organic compounds (WSOC) in fog water, for which information is still rather limited. Fog samples collected during the 1998–1999 fall–winter season in the Po Valley (Italy) were analysed following this procedure, which allows a quantitative determination of three main classes of organic compounds (neutral species, mono- and di-carboxylic acids, polycarboxylic acids), together accounting for ca. 85% of the total WSOC. This procedure also provides information on the main chemical characteristics of these three classes of compounds (functional groups, aliphatic vs. aromatic character, etc.). The enhanced chemical knowledge on fog/cloud chemical composition opens new scenarios as far as chemical and microphysical processes in clouds and fogs are concerned.     

CMIP6云反馈模式比较计划（CFMIP）概况与评述

世界气候研究计划(WCRP)于2003年支持开展云反馈模式比较计划（CFMIP)。目前已经开展到第三阶段（CFMIP-3)。相比前两阶段的试验,CFMIP-3试验设计更加丰富、具体,除增加CMIP6 DECK和Historical试验的观测模拟器（COSP）输出外,还围绕着回答7个云反馈相关的科学问题,设计了Tier-1（必做）和Tier-2（可选）两类试验。CFMIP将气候模拟、观测研究和过程模拟等几个研究方向更紧密地联系在一起,并为理解和模拟云及其辐射反馈的气候贡献提供更深刻的认识和分析手段。     

Temporal characteristics and fog water collection during summer in Tenerife (Canary Islands, Spain)

The study of fog dynamics in the island of Tenerife began in 1993 at six sites. The analysis of the relationship between fog and several meteorological parameters was conducted at the site located at Anaga. Anaga is located at the summit of a mountain range, at an altitude of 842 m and 3.5 km away from the north-western coastline of the island. The study uses hourly data of the three summer months (June, July and August) that were collected over a period of nine years — from 1996 to 2005. The mean summer (June–August) rainfall was found to be 21.2 mm whilst the total volume of fog water collected was 879.9 l m^− 2; the daily average fog water collection was 9.5 l m^− 2 day^− 1, and the hourly average about 0.4 l m^− 2 h^− 1. Although these amounts were recorded with wind speeds of between 8 and 12 m s^− 1, the correlation between water collected and wind speed is not statistically significant. In spite of this, the volume of fog water collected and wind speed showed a very distinct daily behavioural pattern, their frequency and speed reaching their minimum at 12 a.m. and their maximum from 7 p.m. to 8 a.m. GMT. The importance of this research is that it shows that the fog in the Canary Islands occurs more frequently and makes a more significant contribution to the growth of vegetation in the summer (the dry season) than in the winter, when fog accompanies rainfall.     

A one-dimensional Explicit Time-dependent cloud Model (ETM): Description and validation with a three-dimensional cloud resolving model

An algorithm for a one-dimensional Explicit Time-dependent cloud Model (ETM) that takes into account non-hydrostatic pressure, entrainment, cloud microphysics, lateral and vertical eddy mixing processes is developed and tested against a state-of-the-art cloud resolving three dimensional mesoscale model—the Advanced Regional Prediction System (ARPS). The numerical schemes and sub-grid scale processes are rather similar in both ETM and ARPS, although the dimensionality is different.Results show that the ETM is able to simulate the complete lifecycle for a cloud cell, featuring comparable zones of maximum vertical velocity, and overshooting layers on the cloud top. Heat and moisture fluxes within the cloud column of the ETM occur at the same level as ARPS, giving confidence towards adequate formulations in ETM. However, mass flux fields are not in good agreement; there is significant difference in intensity and the altitude where maxima occur. Sensitivity of the ARPS cloud to the amplitude and depth of the initial thermal bubble was examined; the resulting cloud showed sensitivity to both parameters. The maximum vertical velocity decreases with greater amplitude and occurs earlier. This was used as a tuning parameter to ensure similarity in the lifecycle of ETM and ARPS clouds.