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Estimation of a trend of an atmospheric state variable is usually performed by fitting a linear regression line to a set of data of this variable sampled at different times. Often these data are irregularly sampled in space and time and clustered in a sense that error correlations among data points cause a similar error of data points sampled at similar times. Since this can affect the estimated trend, we suggest to take the full error covariance matrix of the data into account. Superimposed periodic variations can be jointly fitted in a straightforward manner, even if the shape of the periodic function is not known. Global data sets, particularly satellite data, can form the basis to estimate the error correlations. State-dependent amplitudes of superimposed periodic corrections result in a non-linear optimization problem which is solved iteratively.
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Aerosol properties were studied during an intensive airborne measurement campaign that took place at Rotterdam in Netherlands in May 2008 within the framework of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). The objective of this study is to illustrate seven events of new particle formation (NPF) observed with two Condensation Particle Counters (CPCs) operated on board the ATR-42 research aircraft in airsectors around Rotterdam, and to provide information on the spatial extent of the new particle formation phenomenon based on 1-s resolution measurements of ultra-fine particle (in the size range 3–10 nm diameter, denoted N<sub>3-10</sub> hereafter) concentrations. The results show that particle production occurred under the influence of different air mass origins, at different day times and over the North Sea as well as over the continent. The number concentration of freshly nucleated particles (N<sub>3-10</sub>) varied between 5000 and 100 000 cm<sup>−3</sup> within the boundary layer (BL). Furthermore the vertical extension for all nucleation events observed on the ATR-42 never exceeded the upper limit of the BL. The horizontal extent of N<sub>3-10</sub> could not be delimited due to inflexible flight plans which could not be modified to accommodate real-time results. However, the NPF events were observed over geographically large areas; typically the horizontal extension was about 100 km and larger.
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Systematic changes of the ozone weekend effect are found over broad areas of Japan. These changes are characterized by (1) spatial reversals from a weekend increase in the vicinity of huge precursor source areas to a weekend decrease in the surrounding rural areas, and (2) temporal reversals from a weekend increase under relatively unsuitable meteorological conditions for ozone formation to a weekend decrease under relatively suitable conditions. We developed a simple numerical advection–reaction model to explain the relationship between the duration of advection and the supplied solar energy, which causes the daily maximum ozone concentration to be lower near the precursor source. Ozone isopleth diagrams for individual advection durations (equivalent to the distance from the source) for a wide range of initial precursor conditions show that both VOC-limited and NO<sub>x</sub>-limited regimes exist for each advection duration, but the area of NO<sub>x</sub>-limited regime becomes dominant as the advection duration increases because of the increased exposure of the air mass to solar energy. For given initial VOC and NO<sub>x</sub> concentrations, the area remote from the source becomes a NO<sub>x</sub>-limited regime even if the precursor source area is in the VOC-limited regime. The rate of reduction of weekend emissions of NO<sub>x</sub> is larger than that of VOC, causing a weekend increase in ozone inside an area of VOC-limited regime near the source, but a weekend decrease in remote areas with a NO<sub>x</sub>-limited regime. The boundary between these two ozone formation regimes depends on meteorological conditions: when sunlight intensity and temperature are relatively low, the change from a VOC-limited to a NO<sub>x</sub>-limited regime occurs at a point more remote from the source than when they are relatively high, which causes a prevailing ozone weekend increase over a wide geographical area on days with lower ozone potential. Therefore, observations of ozone weekend changes can be interpreted in light of the theoretical implications of our model; they can be used for determination of ozone formation regimes, which change in different locations and under different meteorological conditions.
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Archived Federal Reference Method (FRM) Teflon filters used by state regulatory agencies for measuring PM<sub>2.5</sub> mass were acquired from 15 sites throughout the southeastern US and analyzed for water-soluble organic carbon (WSOC), water-soluble ions and carbohydrates to investigate biomass burning contributions to fine aerosol mass. Based on over 900 filters that spanned all of 2007, levoglucosan and K<sup>+</sup> were studied in conjunction with MODIS Aqua fire count data to compare their performances as biomass burning tracers. Levoglucosan concentrations exhibited a distinct seasonal variation with large enhancement in winter and spring and a minimum in summer, and were well correlated with fire counts, except in winter when residential wood burning contributions were significant. In contrast, K<sup>+</sup> concentrations had no apparent seasonal trend and poor correlation with fire counts. Levoglucosan and K<sup>+</sup> only correlated well in winter (<i>r</i><sup>2</sup>=0.59) when biomass burning emissions were highest, whereas in other seasons they were not correlated due to the presence of other K<sup>+</sup> sources. Levoglucosan also exhibited larger spatial variability than K<sup>+</sup>. Both species were higher in urban than rural sites (mean 44% higher for levoglucosan and 86% for K<sup>+</sup>). Positive Matrix Factorization (PMF) was applied to analyze PM<sub>2.5</sub> sources and four factors were resolved: biomass burning, refractory material, secondary light absorbing WSOC and secondary sulfate/WSOC. The biomass burning source contributed 13% to PM<sub>2.5</sub> mass annually, 27% in winter, and less than 2% in summer, consistent with other souce apportionment studies based on levoglucosan, but lower in summer compared to studies based on K<sup>+</sup>.
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It is well-known that aerosols affect clouds and that the effect of aerosols on clouds is critical for understanding human-induced climate change. Most climate model studies have focused on the effect of aerosols on warm stratiform clouds (e.g., stratocumulus clouds) for the prediction of climate change. However, systems like the Asian and Indian Monsoon, storm tracks, and the intertropical convergence zone, play important roles in the global hydrological cycle and in the circulation of energy and are driven by thunderstorm-type convective clouds. Here, we show that the different morphologies of these two cloud types lead to different aerosol-cloud interactions. Increasing aerosols are known to suppress the conversion of droplets to rain (i.e., so-called autoconversion). This increases droplets as a source of evaporative cooling, leading to an increased intensity of downdrafts. The acceleration of the intensity of downdrafts is larger in convective clouds due to their larger cloud depths (providing longer paths for downdrafts to follow to the surface) than in stratiform clouds. More accelerated downdrafts intensify the gust front, leading to significantly increased updrafts, condensation and thus the collection of cloud liquid by precipitation, which offsets the suppressed autoconversion. This leads to an enhancement of precipitation with increased aerosols in convective clouds. However, the downdrafts are less accelerated in stratiform clouds due to their smaller cloud depths, and they are not able to induce changes in updrafts as large as those in convective clouds. Thus, the offset is not as effective, and this allows the suppression of precipitation with increased aerosols. Thus aerosols affect these cloud systems differently. The dependence of the effect of aerosols on clouds on the morphology of clouds should be taken into account for a more complete assessment of climate change.
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This study presents an empirical method to estimate the CCN concentration as a function of percent supersaturation. The aerosol optical properties, backscatter fraction and single scatter albedo, function as proxies for the aerosol size and composition in a power law relationship to CCN. This method is tested at four sites with aged aerosol: SGP (Oklahoma, USA), FKB (Black Forest, Germany), HFE (Hefei, China) and GRW (Graciosa, Azores). Each site represents a different aerosol type and thus demonstrates the method robustness and limitations. Good agreement was found between the calculated and measured CCN with slopes between 0.81 and 1.03 and correlation coefficients (<i>r</i><sup>2</sup> values) between 0.59 and 0.67. The fit quality declined at low CCN concentrations.
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It has recently been shown that at high rainfall intensities, small raindrops may fall with much larger velocities than would be expected from their diameters. These were argued to be fragments of recently broken-up larger drops. In this paper we quantify the effect of this phenomenon on raindrop size distribution measurements from a Joss-Waldvogel disdrometer, a 2-D Video Distrometer, and a vertically-pointing Doppler radar. Probability distributions of fall velocities have been parameterized, where the parameters are functions of both rainfall intensity and drop size. These parameterizations have been used to correct Joss-Waldvogel disdrometer measurements for this phenomenon. The effect of these corrections on fitted scaled drop size distributions are apparent but not major. Fitted gamma distributions for three different types of rainfall have been used to simulate drop size measurements. The effect of the high-velocity small drops is shown to be minor. Especially for the purpose of remote sensing of rainfall using radar, microwave links, or optical links, the errors caused by using the slightly different retrieval relations will be masked completely by other error sources.
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A month (4 May to 8 June 2008) of ambient aerosol, air ion and gas phase sampling (Finokalia Aerosol Measurement Experiment 2008, FAME-08) was conducted at Finokalia, on the island of Crete, Greece. The purpose of the study was to characterize the physical and chemical properties of aged aerosol and to investigate new particle formation. Measurements included aerosol and air ion size distributions, size-resolved chemical composition, organic aerosol thermal volatility, water uptake and particle optical properties (light scattering and absorption). Statistical analysis of the aerosol mass concentration variations revealed the absence of diurnal patterns suggesting the lack of strong local sources. Sulfates accounted for approximately half of the particulate matter less than 1 micrometer in diameter (PM<sub>1</sub>) and organics for 28%. The PM<sub>1</sub> organic aerosol fraction was highly oxidized with 80% water soluble. The supermicrometer particles were dominated by crustal components (50%), sea salt (24%) and nitrates (16%). The organic carbon to elemental carbon (OC/EC) ratio correlated with ozone measurements but with a one-day lag. The average OC/EC ratio for the study period was equal to 5.4. For three days air masses from North Africa resulted in a 6-fold increase of particulate matter less than 10 micrometers in diameter (PM<sub>10</sub>) and a decrease of the OC/EC ratio by a factor of 2. Back trajectory analysis, based on FLEXPART footprint plots, identified five source regions (Athens, Greece, Africa, other continental and marine), each of which influenced the PM<sub>1</sub> aerosol composition and properties. Marine air masses had the lowest PM<sub>1</sub> concentrations and air masses from the Balkans, Turkey and Eastern Europe the highest.
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The global observation, assimilation and prediction in numerical models of ice super-saturated (ISS) regions (ISSR) are crucial if the climate impact of aircraft condensation trails (contrails) is to be fully understood, and if, for example, contrail formation is to be avoided through aircraft operational measures. Given their small scales compared to typical atmospheric model grid sizes, statistical representations of the spatial scales of ISSR are required, in both horizontal and vertical dimensions, if global occurrence of ISSR is to be adequately represented in climate models. <br><br> This paper uses radiosonde launches made by the UK Meteorological Office, from the British Isles, Gibraltar, St. Helena and the Falkland Islands between January 2002 and December 2006, to investigate the probabilistic occurrence of ISSR. Each radiosonde profile is divided into 50- and 100-hPa pressure layers, to emulate the coarse vertical resolution of some atmospheric models. Then the high resolution observations contained within each thick pressure layer are used to calculate an average relative humidity and an ISS fraction for each individual thick pressure layer. These relative humidity pressure layer descriptions are then linked through a probability function to produce an s-shaped curve which empirically describes the ISS fraction in any average relative humidity pressure layer. Using this empirical understanding of the s-shaped relationship a mathematical model was developed to represent the ISS fraction within any arbitrary thick pressure layer. Two models were developed to represent both 50- and 100-hPa pressure layers with each reconstructing their respective s-shapes within 8–10% of the empirical curves. These new models can be used, to represent the small scale structures of ISS events, in modelled data where only low vertical resolution is available. This will be useful in understanding, and improving the global distribution, both observed and forecasted, of ice super-saturation.
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The effects of lightning and other meteorological factors on wildfire activity in the North American boreal forest are statistically analyzed during the fire seasons of 2000–2006 through an integration of the following data sets: the MODerate Resolution Imaging Spectroradiometer (MODIS) level 2 fire products, the 3-hourly 32-km gridded meteorological data from North American Regional Reanalysis (NARR), and the lightning data collected by the Canadian Lightning Detection Network (CLDN) and the Alaska Lightning Detection Network (ALDN). Positive anomalies of the 500 hPa geopotential height field, convective available potential energy (CAPE), number of cloud-to-ground lightning strikes, and the number of consecutive dry days are found to be statistically important to the seasonal variation of MODIS fire counts in a large portion of Canada and the entirety of Alaska. Analysis of fire occurrence patterns in the eastern and western boreal forest regions shows that dry (in the absence of precipitation) lightning strikes account for only 20% of the total lightning strikes, but are associated with (and likely cause) 40% of the MODIS observed fire counts in these regions. The chance for ignition increases when a threshold of at least 10 dry strikes per NARR grid box and at least 10 consecutive dry days is reached. Due to the orientation of the large-scale pattern, complex differences in fire and lightning occurrence and variability were also found between the eastern and western sub-regions. Locations with a high percentage of dry strikes commonly experience an increased number of fire counts, but the mean number of fire counts per dry strike is more than 50% higher in western boreal forest sub-region, suggesting a geographic and possible topographic influence. While wet lightning events are found to occur with a large range of CAPE values, a high probability for dry lightning occurs only when 500 hPa geopotential heights are above ~5700 m and CAPE values are near the maximum observed level, underscoring the importance of low-level instability to boreal fire weather forecasts.
