-
This paper introduces a definition of sand/dust storm process as a new standard and idea of sand/dust storm (SDS) groups a number of SDS-events in Northeast Asia. Based on the meteorological data from WMO/GOS network, 2456 Chinese surface stations and NCEP-NCAR reanalysis, the sand/dust storm processes in Northeast Asia in spring 2000–2006 are investigated. And the evolutions of anomalies of general circulation in the troposphere are analyzed by comparing the spring having most and least occurrences of SDS in year 2006 and 2003. Associated with the noticeably increased occurrence of SDS processes in spring 2006, the anomalies in 3-D structure of general circulation especially in the mid-and high latitudes of the Northen Hemisphere (NH) are revealed. The transition period from the winter of 2005 to spring 2006 has witnessed a fast-developed high center over the circumpolar vortex area in the upper troposphere, which pushes the polar vortex more southwards to mid-latitudes with a more extensive area over the east NH. In spring 2006, there are the significant circulation anomalies in the middle troposphere from the Baikal Lake to northern China with a stronger southward wind anomaly over Northeast Asia. Compared with a normal year, stronger meridional wind with a southward wind anomaly also in the lower troposphere prevail over the arid and semiarid regions in Mongolia and northern China during spring 2006. The positive anomalies of surface high pressure registered an abnormal high of 4–10 hPa in the Tamil Peninsular make a stronger cold air source for the repeated cold air outbreak across the desert areas in spring 2006 resulting in the most frequent SDS seasons in the last 10 years in Northeast Asia.
-
An ensemble of space-borne and ground-based instruments has been used to evaluate the quality of the version 2.2 temperature retrievals from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The agreement of ACE-FTS temperatures with other sensors is typically better than 2 K in the stratosphere and upper troposphere and 5 K in the lower mesosphere. There is evidence of a systematic high bias (roughly 3–6 K) in the ACE-FTS temperatures in the mesosphere, and a possible systematic low bias (roughly 2 K) in ACE-FTS temperatures near 23 km. Some ACE-FTS temperature profiles exhibit unphysical oscillations, a problem fixed in preliminary comparisons with temperatures derived using the next version of the ACE-FTS retrieval software. Though these relatively large oscillations in temperature can be on the order of 10 K in the mesosphere, retrieved volume mixing ratio profiles typically vary by less than a percent or so. Statistical comparisons suggest these oscillations occur in about 10% of the retrieved profiles. Analysis from a set of coincident lidar measurements suggests that the random error in ACE-FTS version 2.2 temperatures has a lower limit of about ±2 K.
-
Mid-infrared solar absorption spectra recorded by a state-of-the-art ground-based FTIR system have the potential to provide precise total O<sub>3</sub> amounts. The currently best-performing retrieval approaches use a combination of small and broad spectral O<sub>3</sub> windows between 780 and 1015 cm<sup>−1</sup>. We show that for these approaches the uncertainties of the temperature profile are by far the major error sources. We demonstrate that a joint optimal estimation of temperature and O<sub>3</sub> profiles widely eliminates this error. The improvements are documented by an extensive theoretical error estimation. Our results suggest that mid-infrared FTIR measurements can provide total O<sub>3</sub> amounts with a precision of around 1 DU, placing this method among the most precise ground-based O<sub>3</sub> monitoring techniques. We recapitulate the requirements on the instrumental hardware and on the retrieval that are needed to achieve this high precision.
-
The Michelson Interferometer for Passive Atmospheric Sounding onboard ENVISAT (MIPAS-E) offers the opportunity to detect and spectrally resolve many atmospheric minor constituents affecting atmospheric chemistry. In this paper, we describe an algorithm produced to retrieve HCFC–22 profiles from MIPAS-E measurements made in 2003 and present results from this scheme between 300 and 50 mb. By comparison with ATMOS (AT–3) version 3 data, we find a mean Northern Hemisphere mid-latitude (20–50° N) HCFC–22 growth rate between 1994 and 2003 of 5.4±0.7 pptv/yr in the lower stratosphere (LS) and a mean LS Southern Hemisphere growth rate (60–80° S) of 6.0±0.7 pptv/yr in the same period. We test the feasibility of using a global data set to estimate the chemical lifetime of HCFC–22 in the LS and we derive this for two regions: 20–50° N (246±38 years) and 60–80° S (274±34 years). From these data we note a global LS lifetime of 260±25 years, significantly longer than previous estimates.
-
Statistical analyses of data from ground-based sun photometer stations in Central Europe are presented. All stations are part of the Aerosol Robotic Network (AERONET), and only data of the highest data quality level 2.0 has been applied. The averages by weekday of Aerosol Optical Thickness (AOT) at a wavelength of 440 nm of 12 of the 14 stations in the investigation area show a weekly periodicity with lowest values on Sunday and Monday, but greatest values from Wednesday until Saturday, that is significant at least on a 90% level. The stations in Germany and in Greater Paris show weekly cycles with ranges of about 20% on average. In Northern Italy and Switzerland this range is about 10% on average. By applying several checks, we exclude that the weekly cycles were caused by a maintenance effect or by different retrieval conditions as a consequence of a weekly cycle in cloud cover. The corresponding weekly cycle of anthropogenic gaseous and particulate emissions leads us to the conclusion of the anthropogenic origin of the weekly AOT cycle. Since these AOT patterns are derived from the reduction of the direct sun radiation by the columnar atmospheric aerosol, this result represents strong evidence for an anthropogenic direct aerosol effect on shortwave radiation. Furthermore, this study makes a first contribution to the understanding and explanation of recently observed weekly periodicities in meteorological variables as temperature in Germany.
-
Biogenic aerosol formation is likely to contribute significantly to the global aerosol load. In recent years, new-particle formation has been observed in various ecosystems around the world but hardly any measurements have taken place in the terrestrial Southern Hemisphere. Here, we report the first results of atmospheric ion and charged particle concentrations as well as of new-particle formation in a Eucalypt forest in Tumbarumba, South-East Australia, from July 2005 to October 2006. The measurements were carried out with an Air Ion Spectrometer (AIS) with a size range from 0.34 to 40 nm. The Eucalypt forest was a very strong source of new aerosol particles. Daytime aerosol formation took place on 52% of days with acceptable data, which is 2–3 times as often as in the Nordic boreal zone. Average growth rates for negative/positive 1.5–3 nm particles during these formation events were 2.89/2.68 nmh<sup>−1</sup>, respectively; for 3-7 nm particles 4.26/4.03, and for 7–20 nm particles 8.90/7.58 nmh<sup>−1</sup>, respectively. The growth rates for large ions were highest when the air was coming from the native forest which suggests that the Eucalypts were a strong source of condensable vapours. Average concentrations of cluster ions (0.34–1.8 nm) were 2400/1700 cm<sup>−3</sup> for negative/positive ions, very high compared to most other measurements around the world. One reason behind these high concentrations could be the strong radon efflux from the soils around the Tumbarumba field site. Furthermore, comparison between night-time and daytime concentrations supported the view that cluster ions are produced close to the surface within the boundary layer also at night but that large ions are mostly produced in daytime. Finally, a previously unreported phenomenon, nocturnal aerosol formation, appeared in 32% of the analysed nights but was clustered almost entirely within six months from summer to autumn in 2006. From January to May, nocturnal formation was 2.5 times as frequent as daytime formation. Therefore, it appears that in summer and autumn, nocturnal production was the major mechanism for aerosol formation in Tumbarumba.
-
The interaction of mineral dust with N<sub>2</sub>O<sub>5</sub> was investigated using both airborne mineral aerosol (using an aerosol flow reactor with variable relative humidity) and bulk samples (using a Knudsen reactor at zero humidity). Both authentic (Saharan, SDCV) and synthetic dust samples (Arizona test dust, ATD and calcite, CaCO<sub>3</sub>) were used to derive reactive uptake coefficients (γ). The aerosol experiments (Saharan dust only) indicated efficient uptake, with e.g. a value of γ(SDCV)=(1.3±0.2)×10<sup>−2</sup> obtained at zero relative humidity. The values of γ obtained for bulk substrates in the Knudsen reactor studies are upper limits due to assumptions of available surface area, but were in reasonable agreement with the AFT measurements, with: γ(SDCV)=(3.7±1.2)×10<sup>−2</sup>, γ(ATD)=(2.2±0.8)×10<sup>−2</sup> and γ(CaCO<sub>3</sub>=(5±2)×10<sup>−2</sup>. The errors quoted are statistical only. The results are compared to literature values and assessed in terms of their impact on atmospheric N<sub>2</sub>O<sub>5</sub>.
-
Levels of PM<sub>10</sub>, PM<sub>2.5</sub> and PM<sub>1</sub> and chemical speciation of PM<sub>10</sub> and PM<sub>2.5</sub> were measured during the MILAGRO campaign (1st to 31st March 2006, but extended in some cases until 6th April) at four urban, one suburban, two rural background and two rural sites, with different degree of industrial influence, in the Mexico City Metropolitan Area (MCMA) and adjacent regions. PM<sub>10</sub> and PM<sub>2.5</sub> daily levels varied between 50–56μg/m<sup>3</sup> and 24–46μg/m<sup>3</sup> at the urban sites, 22–35μg/m<sup>3</sup> and 13–25μg/m<sup>3</sup> at the rural sites, and 75μg/m<sup>3</sup> and 31μg/m<sup>3</sup> at the industrial hotspot, lower than those recorded at some Asian mega-cities and similar to those recorded at other Latin American cities. At the urban sites, hourly PM<sub>2.5</sub> and PM<sub>1</sub> concentrations showed a marked impact of road traffic emissions (at rush hours), with levels of coarse PM remaining elevated during daytime. At the suburban and rural sites different PM daily patterns were registered according to the influence of the pollution plume from MCMA, and also of local soil resuspension. <br><br> The speciation studies showed that mineral matter accounted for 25–27% of bulk PM<sub>10</sub> at the urban sites and a higher proportion (up to 43%) at the suburban and rural sites. This pattern is repeated in PM<sub>2.5</sub>, with 15% at urban and 28% at suburban and rural sites. Carbonaceous compounds accounted for a significant proportion at the urban and industrial sites (32–46% in PM<sub>10</sub>, and 51–55% in PM<sub>2.5</sub>), markedly reduced at the suburban and rural sites (16–23% in PM<sub>10</sub>, and 30% in PM<sub>2.5</sub>). The secondary inorganic aerosols accounted for 10–20% of bulk PM<sub>10</sub> at urban, suburban, rural and industrial sites, with a higher proportion (40%) at the industrial background site. A relatively high proportion of nitrate in rural sites was present in the coarse fraction. <br><br> Typically anthropogenic elements (As, Cr, Zn, Cu, Pb, Sn, Sb, Ba, among others) showed considerably high levels at the urban sites; however levels of particulate Hg and crustal trace elements (Rb, Ti, La, Sc, Ga) were generally higher at the suburban site. <br><br> Principal component analysis identified three major common factors: crustal, regional background and road traffic. Moreover, some specific factors were obtained for each site.
-
For high-resolution measurements of temperature fields in the atmospheric boundary layer and the lower free troposphere a scanning eye-safe lidar which deploys the rotational Raman technique at 355 nm was developed. To optimize the filters of the receiver for both high nighttime and daytime performance, detailed simulation studies have been performed. The receiver is fiber-coupled to a sequential setup of multicavity interference filters used under small angles of incidence. Examples of nighttime and daytime measurements with the system which has a total power-aperture-efficiency product of 0.006 W m<sup>2</sup> are presented. Noontime temperature measurements with a temporal resolution of 60 s result in 1-sigma statistical temperature uncertainty of <1 K up to 1 km height and <2 K up to 2 km height. With an integration time of 60 min and a gliding average of 750 m a 1-sigma statistical temperature uncertainty of <1 K up to 14 km height is achieved during night.
-
The long standing issue of sub-grid emission heterogeneity and its influence to upper air concentration is addressed here and a subgrid model proposed. The founding concept of the approach is the assumption that average emission act as source terms of average concentration, emission fluctuations are source for the concentration variance. The model is based on the derivation of the sub-grid contribution of emission and the use of the concentration variance equation to transport it in the atmospheric boundary layer. The model has been implemented in an existing mesoscale model and the results compared with Large-Eddy Simulation data for ad-hoc simulation devised to test specifically the parametrization. The results show an excellent agreement of the models. For the first time a time evolving error bar reproducing the sub-grid scale heterogeneity of the emissions and the way in which it affects the concentration has been shown. The concentration variance is presented as an extra attribute to better define the mean concentrations in a Reynolds-average model. The model has applications from meso to global scale and that go beyond air quality.