scholarly journals Seasonal cycle, size dependencies, and source analyses of aerosol optical properties at the SMEAR II measurement station in Hyytiälä, Finland

2011 ◽  
Vol 11 (9) ◽  
pp. 4445-4468 ◽  
Author(s):  
A. Virkkula ◽  
J. Backman ◽  
P. P. Aalto ◽  
M. Hulkkonen ◽  
L. Riuttanen ◽  
...  

Abstract. Scattering and absorption were measured at the Station for Measuring Ecosystem–Atmosphere Relations (SMEAR II) station in Hyytiälä, Finland, from October 2006 to May 2009. The average scattering coefficient σSP (λ = 550 nm) 18 Mm−1 was about twice as much as at the Pallas Global Atmosphere Watch (GAW) station in Finnish Lapland. The average absorption coefficient σAP (λ = 550 nm) was 2.1 Mm−1. The seasonal cycles were analyzed from hourly-averaged data classified according to the measurement month. The ratio of the highest to the lowest average σSP and σAP was ~1.8 and ~2.8, respectively. The average single-scattering albedo (ω0) was 0.86 in winter and 0.91 in summer. σSP was highly correlated with the volume concentrations calculated from number size distributions in the size range 0.003–10 μm. Assuming that the particle density was 1.5 g cm−3, the PM10 mass scattering efficiency was 3.1 ± 0.9 g m−2 at λ = 550 nm. Scattering coefficients were also calculated from the number size distributions by using a Mie code and the refractive index of ammonium sulfate. The linear regression yielded σSP(modelled) = 1.046 × σSP(measured) for the data with the low nephelometer sample volume relative humidity (RHNEPH = 30 ± 9 %) and σSP(modelled) = 0.985 × σSP(measured) when RHNEPH = 55 ± 4 %. The effective complex refractive index was obtained by an iterative approach, by matching the measured and the modelled σSPand σAP. The average effective complex refractive index was (1.517 ± 0.057) + (0.019 ± 0.015)i at λ = 550 nm. The iterated imaginary part had a strong seasonal cycle, with smallest values in summer and highest in winter. The contribution of submicron particles to scattering was ~90 %. The Ångström exponent of scattering, σSP, was compared with the following weighted mean diameters: count mean diameter (CMD), surface mean diameter (SMD), scattering mean diameter (ScMD), condensation sink mean diameter (CsMD), and volume mean diameter (VMD). If αSP is to be used for estimating some measure of the size of particles, the best choice would be ScMD, then SMD, and then VMD. In all of these the qualitative relationship is similar: the larger the Ångström exponent, the smaller the weighted mean diameter. Contrary to these, CMD increased with increasing αSP and CsMD did not have any clear relationship with αSP. Source regions were estimated with backtrajectories and trajectory statistics. The geometric mean σSP and σAP associated with the grid cells in Eastern Europe were in the range 20–40 Mm−1 and 4–6 Mm−1, respectively. The respective geometric means of σSP and σAP in the grid cells over Norwegian Sea were in the range 5–10 Mm−1 and <1 Mm−1. The source areas associated with high αSP values were norther than those for σSP and σAP. The trajectory statistical approach and a simple wind sector classification agreed well.

2010 ◽  
Vol 10 (12) ◽  
pp. 29997-30053
Author(s):  
A. Virkkula ◽  
J. Backman ◽  
P. P. Aalto ◽  
M. Hulkkonen ◽  
L. Riuttanen ◽  
...  

Abstract. Scattering and absorption were measured at the SMEAR II station in Hyytiälä, Finland, from October 2006 to May 2009. The average scattering coefficient σSP (λ=550 nm) 18 Mm−1 was about twice as much as at the Pallas GAW station in Finnish Lapland. The average absorption coefficient σAP (λ=550 nm) was 2.1 Mm−1. The seasonal cycles were analyzed from hourly-averaged data classified according to the measurement month. The ratio of the highest to the lowest average σSP and σAP was ~1.8 and ~2.8, respectively. The average single-scattering albedo (ω0) was 0.86 in winter and 0.91 in summer. σSP was highly correlated with the volume concentrations calculated from number size distributions in the size range 0.003–10 μm yielding PM10 mass scattering efficiency of 2.75 ± 0.01 g m−2 at λ=550 nm. Scattering coefficients were also calculated from the number size distributions by using a Mie code and the refractive index of ammonium sulfate. The linear regression yielded σSP(modelled)=1.04×σSP(measured) but there were also large deviations from the regression line: 10% of the σSP(modelled)-to-σSP(measured) ratios, calculated for each hour, were smaller than 0.9 and 10% of them were larger than 1.27. The scattering size distributions were bimodal, with a large submicrometer mode with geometric mean diameters Dg between ~300 and 400 nm and a smaller supermicrometer mode with Dg at ~1.5–1.9 μm. The contribution of submicrometer particles to scattering was ~90%. The Ångström exponent of scattering, αSP, was compared with the following weighted mean diameters: count mean diameter (CMD), surface mean diameter (SMD), scattering mean diameter (ScMD), condensation sink mean diameter (CsMD), and volume mean diameter (VMD). If αSP is to be used for estimating some measure of the size of particles, the best choice would be ScMD, then SMD, and then VMD. In all of these the qualitative relationship is similar: the larger the Ångström exponent, the smaller the weighted mean diameter. Contrary to these, CMD increased with increasing αSP and CsMD did not have any clear relationship with αSP. Source regions were estimated with backtrajectories and trajectory statistics. The geometric mean σSP and σAP associated with the grid cells in Eastern Europe were in the range 20–40 Mm−1 and 4–6 Mm−1, respectively. The respective geometric means of σSP and σAP in the grid cells over Norwegian Sea were in the range 5–10 Mm−1 and <1 Mm−1. The source areas associated with high αSP values were norther than those for σSP and σAP. The trajectory statistical approach and a simple wind sector classification agreed well.


2019 ◽  
Vol 19 (24) ◽  
pp. 15483-15502 ◽  
Author(s):  
Yicheng Shen ◽  
Aki Virkkula ◽  
Aijun Ding ◽  
Krista Luoma ◽  
Helmi Keskinen ◽  
...  

Abstract. The concentration of cloud condensation nuclei (CCN) is an essential parameter affecting aerosol–cloud interactions within warm clouds. Long-term CCN number concentration (NCCN) data are scarce; there are a lot more data on aerosol optical properties (AOPs). It is therefore valuable to derive parameterizations for estimating NCCN from AOP measurements. Such parameterizations have already been made, and in the present work a new parameterization is presented. The relationships between NCCN, AOPs, and size distributions were investigated based on in situ measurement data from six stations in very different environments around the world. The relationships were used for deriving a parameterization that depends on the scattering Ångström exponent (SAE), backscatter fraction (BSF), and total scattering coefficient (σsp) of PM10 particles. The analysis first showed that the dependence of NCCN on supersaturation (SS) can be described by a logarithmic fit in the range SS <1.1 %, without any theoretical reasoning. The relationship between NCCN and AOPs was parameterized as NCCN≈((286±46)SAE ln(SS/(0.093±0.006))(BSF − BSFmin) + (5.2±3.3))σsp, where BSFmin is the minimum BSF, in practice the 1st percentile of BSF data at a site to be analyzed. At the lowest supersaturations of each site (SS ≈0.1 %), the average bias, defined as the ratio of the AOP-derived and measured NCCN, varied from ∼0.7 to ∼1.9 at most sites except at a Himalayan site where the bias was >4. At SS >0.4 % the average bias ranged from ∼0.7 to ∼1.3 at most sites. For the marine-aerosol-dominated site Ascension Island the bias was higher, ∼1.4–1.9. In other words, at SS >0.4 % NCCN was estimated with an average uncertainty of approximately 30 % by using nephelometer data. The biases were mainly due to the biases in the parameterization related to the scattering Ångström exponent (SAE). The squared correlation coefficients between the AOP-derived and measured NCCN varied from ∼0.5 to ∼0.8. To study the physical explanation of the relationships between NCCN and AOPs, lognormal unimodal particle size distributions were generated and NCCN and AOPs were calculated. The simulation showed that the relationships of NCCN and AOPs are affected by the geometric mean diameter and width of the size distribution and the activation diameter. The relationships of NCCN and AOPs were similar to those of the observed ones.


2018 ◽  
Vol 18 (8) ◽  
pp. 5235-5252 ◽  
Author(s):  
Rosalie H. Shepherd ◽  
Martin D. King ◽  
Amelia A. Marks ◽  
Neil Brough ◽  
Andrew D. Ward

Abstract. Optical trapping combined with Mie spectroscopy is a new technique used to record the refractive index of insoluble organic material extracted from atmospheric aerosol samples over a wide wavelength range. The refractive index of the insoluble organic extracts was shown to follow a Cauchy equation between 460 and 700 nm for organic aerosol extracts collected from urban (London) and remote (Antarctica) locations. Cauchy coefficients for the remote sample were for the Austral summer and gave the Cauchy coefficients of A = 1.467 and B = 1000 nm2 with a real refractive index of 1.489 at a wavelength of 589 nm. Cauchy coefficients for the urban samples varied with season, with extracts collected during summer having Cauchy coefficients of A=1.465±0.005 and B=4625±1200 nm2 with a representative real refractive index of 1.478 at a wavelength of 589 nm, whilst samples extracted during autumn had larger Cauchy coefficients of A = 1.505 and B = 600 nm2 with a representative real refractive index of 1.522 at a wavelength of 589 nm. The refractive index of absorbing aerosol was also recorded. The absorption Ångström exponent was determined for woodsmoke and humic acid aerosol extract. Typical values of the Cauchy coefficient for the woodsmoke aerosol extract were A=1.541±0.03 and B=14800±2900 nm2, resulting in a real refractive index of 1.584 ± 0.007 at a wavelength of 589 nm and an absorption Ångström exponent of 8.0. The measured values of refractive index compare well with previous monochromatic or very small wavelength range measurements of refractive index. In general, the real component of the refractive index increases from remote to urban to woodsmoke. A one-dimensional radiative-transfer calculation of the top-of-the-atmosphere albedo was applied to model an atmosphere containing a 3 km thick layer of aerosol comprising pure water, pure insoluble organic aerosol, or an aerosol consisting of an aqueous core with an insoluble organic shell. The calculation demonstrated that the top-of-the-atmosphere albedo increases by 0.01 to 0.04 for pure organic particles relative to water particles of the same size and that the top-of-the-atmosphere albedo increases by 0.03 for aqueous core-shell particles as volume fraction of the shell material increases to 25 %.


2018 ◽  
Vol 18 (9) ◽  
pp. 6259-6273 ◽  
Author(s):  
Chao Liu ◽  
Chul Eddy Chung ◽  
Yan Yin ◽  
Martin Schnaiter

Abstract. The absorption Ångström exponent (AAE) is an important aerosol optical parameter used for aerosol characterization and apportionment studies. The AAE of black carbon (BC) particles is widely accepted to be 1.0, although observational estimates give quite a wide range of 0.6–1.3. With considerable uncertainties related to observations, a numerical study is a powerful method, if not the only one, to provide a better and more accurate understanding on BC AAE. This study calculates BC AAE using realistic particle geometries based on fractal aggregate and an accurate numerical optical model (namely the multiple-sphere T-matrix method), and considers bulk properties of an ensemble of BC particles following lognormal size distributions. At odds with the expectations, BC AAE is not 1.0, even when BC is assumed to have small sizes and a wavelength-independent refractive index. With a wavelength-independent refractive index, the AAE of fresh BC is approximately 1.05 and relatively insensitive to particle size. For BC with geometric mean diameters larger than 0.12 µm, BC AAE becomes smaller when BC particles are aged (compact structures or coated by other non-absorptive materials). For coated BC, we prescribe the coating fraction variation based on a laboratory study, where smaller BC cores are shown to develop larger coating fractions than those of bigger BC cores. For both compact and coated BC, the AAE is highly sensitive to particle size distribution, ranging from approximately 0.8 to even over 1.4 with wavelength-independent refractive index. When the refractive index is allowed to vary with wavelength, a feature with observational backing, the BC AAE may show an even wider range. For different BC morphologies, we derive simple empirical equations on BC AAE based on our numerical results, which can serve as a guide for the response of BC AAE to BC size and refractive index. Due to its complex influences, the effects of BC geometry is better to be discussed at certain BC properties, i.e., known size and refractive index.


2016 ◽  
Author(s):  
I. Veselovskii ◽  
P. Goloub ◽  
T. Podvin ◽  
V. Bovchaliuk ◽  
Y. Derimian ◽  
...  

Abstract. West Africa and the adjacent oceanic regions are very important locations for studying dust properties and their influence on weather and climate. The SHADOW (Study of SaHAran Dust Over West Africa) campaign is performing a multi-scale and multi-laboratory study of aerosol properties and dynamics using a set of in situ and remote sensing instruments at an observation site located at IRD (Institute for Research and Development) Center, Mbour, Senegal (14° N, 17° W). In this paper, we present the results of lidar measurements performed during the first phase of SHADOW which occurred in March-April, 2015. The multiwavelength Mie-Raman lidar acquired 3β + 2α + 1δ measurements during this period. This set of measurements has permitted particle intensive properties such as extinction and backscattering Ångström exponents (BAE) for 355/532 nm wavelengths corresponding lidar ratios and depolarization ratio at 532 nm to be determined. The mean values of dust lidar ratios during the observation period were about 53 sr at both 532 nm and 355 nm, which agrees with the values observed during the SAMUM 1 and SAMUM 2 campaigns held in Morocco and Cape Verde in 2006, 2008. The mean value of particle depolarization ratio at 532 nm was 30 ± 4.5 %, however during strong dust episodes this ratio increased to 35 ± 5 %, which is also in agreement with the results of the SAMUM campaigns. The backscattering Ångström exponent during the dust episodes decreased to ~ −0.7, while the extinction Ångström exponent though being negative, was greater than −0.2. Low values of BAE can likely be explained by an increase in the imaginary part of the dust refractive index at 355 nm compared to 532 nm. The dust extinction and backscattering coefficients at multiple wavelengths were inverted to the particle microphysics using the regularization algorithm and the model of randomly oriented spheroids. The analysis performed has demonstrated that the spectral dependence of the imaginary part of the dust refractive index may significantly influence the inversion results and should be taken into account.


2013 ◽  
Vol 6 (2) ◽  
pp. 3317-3338 ◽  
Author(s):  
A. Bayat ◽  
H. R. Khalesifard ◽  
A. Masoumi

Abstract. Aerosol optical depth, Ångström exponent, single scattering albedo, and polarized phase function have been retrieved from polarized sun-photometer measurements for atmosphere of Zanjan (36.70° N, 48.51° E, and 1800 m a.m.s.l.) from January 2010 to December 2012. The results show that the maximum value of aerosol polarized phase function as well as the polarized phase function retrieved for a specific scattering angle (i.e. 60°), are strongly correlated with the Ångström exponent. The latter one has a meaningful variations respect to the changes in the complex refractive index of the atmospheric aerosols. Furthermore the polarized phase function shows a moderate negative correlation respect to atmospheric aerosol optical depth and single scattering albedo. Therefore the polarized phase function can be regarded as a key parameter to characterize the atmospheric particles.


2018 ◽  
Vol 18 (1) ◽  
pp. 405-425 ◽  
Author(s):  
Huizheng Che ◽  
Bing Qi ◽  
Hujia Zhao ◽  
Xiangao Xia ◽  
Thomas F. Eck ◽  
...  

Abstract. Aerosol pollution in eastern China is an unfortunate consequence of the region's rapid economic and industrial growth. Here, sun photometer measurements from seven sites in the Yangtze River Delta (YRD) from 2011 to 2015 were used to characterize the climatology of aerosol microphysical and optical properties, calculate direct aerosol radiative forcing (DARF) and classify the aerosols based on size and absorption. Bimodal size distributions were found throughout the year, but larger volumes and effective radii of fine-mode particles occurred in June and September due to hygroscopic growth and/or cloud processing. Increases in the fine-mode particles in June and September caused AOD440 nm > 1.00 at most sites, and annual mean AOD440 nm values of 0.71–0.76 were found at the urban sites and 0.68 at the rural site. Unlike northern China, the AOD440 nm was lower in July and August (∼ 0.40–0.60) than in January and February (0.71–0.89) due to particle dispersion associated with subtropical anticyclones in summer. Low volumes and large bandwidths of both fine-mode and coarse-mode aerosol size distributions occurred in July and August because of biomass burning. Single-scattering albedos at 440 nm (SSA440 nm) from 0.91 to 0.94 indicated particles with relatively strong to moderate absorption. Strongly absorbing particles from biomass burning with a significant SSA wavelength dependence were found in July and August at most sites, while coarse particles in March to May were mineral dust. Absorbing aerosols were distributed more or less homogeneously throughout the region with absorption aerosol optical depths at 440 nm ∼ 0.04–0.06, but inter-site differences in the absorption Angström exponent indicate a degree of spatial heterogeneity in particle composition. The annual mean DARF was −93 ± 44 to −79 ± 39 W m−2 at the Earth's surface and ∼ −40 W m−2 at the top of the atmosphere (for the solar zenith angle range of 50 to 80∘) under cloud-free conditions. The fine mode composed a major contribution of the absorbing particles in the classification scheme based on SSA, fine-mode fraction and extinction Angström exponent. This study contributes to our understanding of aerosols and regional climate/air quality, and the results will be useful for validating satellite retrievals and for improving climate models and remote sensing algorithms.


2015 ◽  
Vol 15 (15) ◽  
pp. 20911-20956 ◽  
Author(s):  
G. L. Schuster ◽  
O. Dubovik ◽  
A. Arola ◽  
T. F. Eck ◽  
B. N. Holben

Abstract. Recently, some authors have suggested that the absorption Angstrom exponent (AAE) can be used to deduce the component aerosol absorption optical depths (AAOD) of carbonaceous aerosols in the AERONET database. This "AAE approach" presumes that AAE &amp;ll; 1 for soot carbon, which contrasts the traditional small particle limit of AAE = 1 for soot carbon. Thus, we provide an overview of the AERONET retrieval, and investigate how the microphysics of carbonaceous aerosols can be interpreted in the AERONET AAE product. We find that AAE &amp;ll; 1 in the AERONET database requires large coarse mode fractions and/or imaginary refractive indices that increase with wavelength. Neither of these characteristics are consistent with the current definition of soot carbon, so we explore other possibilities for the cause of AAE &amp;ll; 1. We note that AAE is related to particle size, and that coarse mode particles have a smaller AAE than fine mode particles for a given aerosol mixture of species. We also note that the mineral goethite has an imaginary refractive index that increases with wavelength, is very common in dust regions, and can easily contribute to AAE &amp;ll; 1. We find that AAE &amp;ll; 1 can not be caused by soot carbon, unless soot carbon has an imaginary refractive index that increases with wavelength throughout the visible and near infrared spectrums. Finally, AAE is not a robust parameter for separating carbonaceous absorption from dust aerosol absorption in the AERONET database.


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