Retrieval of aerosol physical and chemical properties from mid-infrared extinction spectra

We report several results that validate the accuracy of a retrieval method for the determination of a number of aerosol particle properties from their mid infrared (600-6000 cm⁻¹) extinction spectra. These properties include the number density, chemical composition, phase, size distribution, and to some extent, shape. The approach is based on information obtained in laboratory studies of micron-sized particles using the aerosol flow tube (AFT) technique. We report here experiments in which our method is used to measure a variety of aerosols including SiO₂ micro-spheres as well as solid NaCl, (NH₄)₂SO₄, ice and liquid water particles. The uncertainties in the retrieved aerosol properties associated with the particle shapes (spheres, spheroids, cylinders, hexagonal and rectangular prisms) as well as the effect of variations in the spectral range were evaluated. To assess the accuracy of the retrieved size distributions and particle shapes, the properties calculated from infrared spectra were compared with corresponding properties determined using alternative methods. We used scanning electron microscopy (SEM) for solid (NH₄)₂SO₄ and NaCl aerosols and direct particle imaging with an optical microscope assembly for liquid water aerosols. On the basis of the validation results, we discuss the boundaries of applicability of the most popular spectral model, single scattering by spherical, homogeneous aerosol particles.     

Use of elemental size distributions in identifying particle formation modes

The chemical composition of particles generated during pulverized coal combustion is the consequence of their formation processes. This work aims to use the size resolved elemental composition of coal-derived particles to identify their formation modes. A size-classified bituminous coal is burnt in a laboratory drop tube furnace at 1150, 1250, and 1350 °C, respectively. The elemental composition of the size-segregated particles from coal combustion is analyzed and the total mass fraction size distributions of Si and Al are obtained. Three particle formation modes are observed in these distribution profiles. The coarse mode has the highest value of the total mass fraction of Si and Al while the ultrafine mode has the lowest one. The total mass fraction of Si and Al in these two modes is nearly independent of particle size. It is believed that the coarse mode is formed by the mineral coalescence mechanism and the ultrafine mode by the vaporization–condensation mechanism. The difference in the total mass fraction of Si and Al between the central mode and the other two indicates that the central mode is formed by different mechanisms. Based on the observation that the total mass fraction of Si and Al in this mode increases with increasing particle size, heterogeneous condensation of vaporized species on existing fine residual ash particles is proposed to account for the formation of these particles. The study of the elemental composition of the three modes represented in five categories verifies the proposed formation mechanisms for them to some extent.     

Reconstitution of apomyoglobin with bile pigments

Summary Apomyoglobin was reconstituted with bile pigments of the verdinoid, 2,3-dihydroverdinoid, pterobilinoid, and violinoid type. Absorption and circular dichroism data as well as formation constants of the complexes were measured. From these results it was concluded that chromophore binding and induced chirality of these pigments are mainly governed by a lipophilic region opposite to the propionic side chain(s) and the asymmetric position of the hydrogen bonding acceptors of the propionic acid side chain(s) at the entrance of the protein pocket.Dedicated to Prof. Dr. A. Eschenmoser on occasion of his 65th birthday     

Nucleation of atmospheric aerosol particles

A significant fraction of the total number of particles present in the atmosphere is formed originally by nucleation from the gas phase. Binary nucleation of sulphuric acid and water, ternary nucleation of sulphuric acid, water and ammonia and ion-induced nucleation are thought to be the most important aerosol nucleation processes in the atmosphere. Within the last two decades, instrumentation to observe and characterize nucleation has improved greatly and numerous observations of nucleation have been made including quantification of the nucleation rate, characterization of the growth process and first chemical characterizations of the freshly formed particles. Nucleation has been observed at many different places in the atmosphere: in the boundary layer, in the free troposphere, in remote locations, in coastal areas, in boreal forests as well as urban areas and pollution plumes. In most cases gaseous sulphuric acid is assumed to be the key precursor gas. After nucleation, other supersaturated substances, especially low vapour pressure organics often take part in the subsequent aerosol growth. Iodine oxides seem to be responsible for nucleation observed in some coastal areas.Recent advances in modelling allow for a kinetic treatment of the nucleation process based on measured thermochemical data for the cluster formation. Considerable improvement over the classical nucleation treatment is expected from this approach.A detailed understanding of atmospheric aerosol nucleation processes is needed as the freshly formed particles directly influence the number concentration and size distribution of the atmospheric aerosol. The formation of clouds and precipitation is affected and influences on climate are anticipated. Anthropogenic emissions influence atmospheric aerosol nucleation processes considerably.Despite the comprehensive research efforts, substantial inconsistencies remain and conflicting results of laboratory studies, model studies as well as atmospheric observations persist. Several key questions about the predictability of atmospheric nucleation in general, about the substances, that take part in nucleation and subsequent growth and about the size and composition of the critical cluster, have not been resolved so far. To cite this article: J. Curtius, C. R. Physique 7 (2006).     

Portable,Ambient PM2.5 Sensor for Human and/or Animal Exposure Studies

A field-portable device for logging PM_2.5 mass concentration data has been developed. The device combines the Arduino microprocessor with an SD card, a Sharp DN7C3CA006 optical dust monitor, and 10,000-mAh battery. The dust sensor uses a virtual impactor to size select particles <2.5 microns prior to illuminating the selected fraction with an LED. The LED is triggered by a circuit controlled with the Arduino. Nephelometric detection at 120° referenced to incidence is used. The voltage signal reported by the dust sensor is converted to PM_2.5 mass through calibration onboard the Arduino. Data points can be saved to the SD card as rapidly as 0.3?s, although averaging signals over 60?s produced more optimal detection limits. For a 60?s average, the PM_2.5 mass limit of detection was 9?µg?m^?3, indicating that the sensor will be useful for monitoring human exposure to fine particles. Portable exposure monitoring has been demonstrated with the sensing platform as several individuals carried the device with them during daily activities in Lubbock, TX and Atlanta, GA. For this group of test subjects, values of PM_2.5 exposure varied from 0 to 1000?µg?m^?3 during the sampling periods. It was observed that, by far, the highest levels of PM_2.5 occur during periods of cooking, or being near cooking operations. Other periods of high PM_2.5 occurred during ground transportation, use of personal care products, vacuuming, and visiting restrooms. When hourly personal exposure data were correlated with hourly average PM_2.5 for outdoor air for the Atlanta data set, a very weak correlation was found (R²?=?0.026). Only two out of eight sampling periods did the personal monitoring estimate of exposure agree with that predicted by outdoor monitoring to within 15%. Personal exposure was often affected by circumstantial, short-term, high exposure events that are difficult to model or predict effectively. The short-term exposure events generally cause true exposure to be higher than that predicted by using outdoor ambient PM_2.5 to generate estimates. This finding complicates interpretation of epidemiological studies that find links between ambient outdoor PM_2.5 levels and human health, while it buttresses the case for using personal ambient monitors.     

中国红层的分布及地质环境特征

根据我国红层的分布特征及形成背景 ,将我国红层划分为西南地区红层、西北地区红层、中南、东南地区红层和其他地区 (西藏及华北的部分地区 )红层。重点研究了以川滇红层为代表的西南地区红层和以甘肃红层为代表的西北地区红层 ,研究了各个区域红层的地质构造特征、地形地貌特征、气候环境特征等工程地质环境特征 ,根据工程地质环境特征 ,将研究区域的红层划分为四川盆地红层、西昌—滇中红层、滇西红层和甘肃红层.     

Determination of organic compounds from wood combustion aerosol nanoparticles by different gas chromatographic systems and by aerosol mass spectrometry

Organic compounds in atmospheric nanoparticles have an effect on human health and the climate. The determination of these particles is challenged by the difficulty of sampling, the complexity of sample composition, and the trace-level concentrations of the compounds. Meeting the challenge requires the development of sophisticated sampling systems for size-resolved particles and the optimization of sensitive, accurate and simple analytical techniques and methods. A new sampling system is proposed where particles are charged with a bipolar charger and size-segregated with a differential mobility analyzer. This system was successfully used to sample particles from wood pyrolysis with particle sizes 30–100 nm. Particles were analyzed by four techniques: comprehensive two-dimensional gas chromatography–time-of-flight mass spectrometry, gas chromatography–time-of-flight mass spectrometry, gas chromatography–quadrupole mass spectrometry, and aerosol mass spectrometry (aerosol MS). In the chromatographic techniques, particles were collected on a filter and analyzed off-line after sample preparation, whereas in the aerosol MS, particle analysis was performed directly from the particle source. Target compounds of the samples were polyaromatic hydrocarbons and n-alkanes. The analytical techniques were compared and their advantages and disadvantages were evaluated. The sampling system operated well and target compounds were identified in low concentrations.     

Cloud and aerosol contributions to variation in shortwave surface irradiance over East Asia in July during 2001 and 2007

It is important to clarify the contributions of clouds and aerosols to the variation of surface shortwave irradiance (S) for climatological studies. This study examined the contributions of clouds and aerosols to the variation in S over East Asia (75-135°E, 20-55°N) in July during 2001 and 2007 using the index of potential radiative forcing (PRF) to characterize the temporal and geographical variations. After confirming the validity of PRF for multiyear analyses, we performed several temporal analyses of clouds and aerosols over the whole research domain. Changes in the geographical distribution, contribution histograms, and averaged values were studied. In agreement with previous studies that treated single-year cases, we confirmed that the magnitudes of the temporal changes in S variations due to clouds and aerosols were highly variable geographically. As for domain-averaged S variations, we did not observe defined trends for the research period. It was also found that the temporal variation between one parameter and its S variation was negatively correlated, from the point analyses at two locations. Based on these results, we concluded that PRF is a promising tool for research into long-term S variations. This kind of information will be quite valuable as basic data for use in climate modeling.     

Comparison of CALIPSO and ground-based lidar profiles over Chung-Li, Taiwan

We report the first inter-comparison of vertical profiles of aerosols and clouds derived from space (CALIPSO) and ground based lidar over Chung-Li, Taiwan. Results show that inter-comparison is closer in case of aerosols than clouds. The strength/shortcoming of the comparison has been also discussed. An iterative calculation to retrieve extinction-to-backscatter ratio (lidar ratio) by using sun-photometer and CALIPSO data is also documented. By using the mentioned method, a mean lidar ratio of 23.5±8.2 sr was found. The derived lidar ratios are lower than former studies. The possible reasons for the difference have been discussed in this paper. The discussed methodology will be helpful to reduce the uncertainty of optical parameters derived from lidar data especially near the surface where the atmosphere is inhomogeneous.