scholarly journals A new approach for retrieving the UV–vis optical properties of ambient aerosols

2016 ◽  
Vol 9 (8) ◽  
pp. 3477-3490 ◽  
Author(s):  
Nir Bluvshtein ◽  
J. Michel Flores ◽  
Lior Segev ◽  
Yinon Rudich

Abstract. Atmospheric aerosols play an important part in the Earth's energy budget by scattering and absorbing incoming solar and outgoing terrestrial radiation. To quantify the effective radiative forcing due to aerosol–radiation interactions, researchers must obtain a detailed understanding of the spectrally dependent intensive and extensive optical properties of different aerosol types. Our new approach retrieves the optical coefficients and the single-scattering albedo of the total aerosol population over 300 to 650 nm wavelength, using extinction measurements from a broadband cavity-enhanced spectrometer at 315 to 345 nm and 390 to 420 nm, extinction and absorption measurements at 404 nm from a photoacoustic cell coupled to a cavity ring-down spectrometer, and scattering measurements from a three-wavelength integrating nephelometer. By combining these measurements with aerosol size distribution data, we retrieved the time- and wavelength-dependent effective complex refractive index of the aerosols. Retrieval simulations and laboratory measurements of brown carbon proxies showed low absolute errors and good agreement with expected and reported values. Finally, we implemented this new broadband method to achieve continuous spectral- and time-dependent monitoring of ambient aerosol population, including, for the first time, extinction measurements using cavity-enhanced spectrometry in the 315 to 345 nm UV range, in which significant light absorption may occur.

2016 ◽  
Author(s):  
Nir Bluvshtein ◽  
J. Michel Flores ◽  
Lior Segev ◽  
Yinon Rudich

Abstract. Atmospheric aerosols play an important part in the Earth's energy budget by scattering and absorbing incoming solar and outgoing terrestrial radiation. To quantify the effective radiative forcing due to aerosol–radiation interactions, researchers must obtain a detailed understanding of the spectrally dependent intensive and extensive optical properties of different aerosol types. Our new approach obtains the optical coefficients and the single scattering albedo of the total aerosol population over 300–650 nm wavelength, using a broadband cavity-enhanced spectrometer (extinction), a photoacoustic cell coupled to a cavity ring down spectrometer (extinction and absorption), and a nephelometer (scattering). Combining these coefficients with aerosol size distribution data, we retrieved the time- and wavelength-dependent effective complex refractive index of the aerosols. Retrieval simulations and laboratory measurements of brown carbon proxies showed low absolute errors and good agreement with expected and reported values. Finally, we utilized our new broadband method to achieve continuous spectral and time-dependent monitoring of an ambient polydisperse aerosols population, including, for the first time, extinction measurements using cavity enhanced spectrometry in the 315 to 345 nm UV range, in which significant light absorption may occur.


2019 ◽  
Vol 29 (2) ◽  
Author(s):  
Joseph A. Adesina ◽  
Stuart J. Piketh ◽  
Paola Formenti ◽  
Gillian Maggs-Kölling ◽  
Brent N. Holben ◽  
...  

Atmospheric aerosols contribute significantly to the uncertainty in radiative forcing effects that influence the climate and pose a significant health risk to humans.   The climatic implications of aerosols are dependent on many variables, including aerosol size, shape, chemical composition, and position in the atmospheric column. The radiative impact of aerosols transported over the west coast of southern Africa has been found, in particular, to be complicated by the aforementioned aerosol properties.  This study investigated the columnar optical properties of aerosols over Gobabeb, Namibia (23.56oS, 15.04oE, 400 m asl) using sunphotometer data between December 2014 and November 2015. Aerosol mean optical depth AOD500 had its maximum and minimum values in 2015 August (0.37±0.30) and June (0.06±0.02), respectively. The Angström parameter was mostly above unity during the study period and indicated the prevalence of fine particles for the most part of the year with maximum and minimum values observed in August 2015 (1.44±0.19) and December 2014 (0.57±0.19), respectively. The columnar water vapor was highest in January (2.62±0.79) and lowest in June (0.76±0.27). The volume size distribution showed the fine particles having a mean radius of about 0.16 μm and the coarse mode had variation in sizes with a radius ranging between 3 μm and 7 μm. The single scattering albedo at visible wavelengths ranged between 0.87 and 0.88. The phase function was high at small angles but minimum at about 140o in all seasons. The radiative forcing showed a heating effect in all seasons with maximum and minimum in winter (9.41 Wm-2) and autumn (3.64 Wm-2), respectively. Intercomparison of the sunphotometer data with the Moderate Resolution Imaging Spectroradiometer (MODIS) showed that the satellite sensor overestimates the aerosol loading compared to the ground-based sunphotometer measurements. Both sets of observations were better correlated during the spring and winter seasons than for summer and autumn.


2019 ◽  
Vol 19 (17) ◽  
pp. 11363-11382 ◽  
Author(s):  
Krista Luoma ◽  
Aki Virkkula ◽  
Pasi Aalto ◽  
Tuukka Petäjä ◽  
Markku Kulmala

Abstract. Aerosol optical properties (AOPs) describe the ability of aerosols to scatter and absorb radiation at different wavelengths. Since aerosol particles interact with the sun's radiation, they impact the climate. Our study focuses on the long-term trends and seasonal variations of different AOPs measured at a rural boreal forest site in northern Europe. To explain the observed variations in the AOPs, we also analyzed changes in the aerosol size distribution. AOPs of particles smaller than 10 µm (PM10) and 1 µm (PM1) have been measured at SMEAR II, in southern Finland, since 2006 and 2010, respectively. For PM10 particles, the median values of the scattering and absorption coefficients, single-scattering albedo, and backscatter fraction at λ=550 nm were 9.8 Mm−1, 1.3 Mm−1, 0.88, and 0.14. The median values of scattering and absorption Ångström exponents at the wavelength ranges 450–700 and 370–950 nm were 1.88 and 0.99, respectively. We found statistically significant trends for the PM10 scattering and absorption coefficients, single-scattering albedo, and backscatter fraction, and the slopes of these trends were −0.32 Mm−1, −0.086 Mm−1, 2.2×10-3, and 1.3×10-3 per year. The tendency for the extensive AOPs to decrease correlated well with the decrease in aerosol number and volume concentrations. The tendency for the backscattering fraction and single-scattering albedo to increase indicates that the aerosol size distribution consists of fewer larger particles and that aerosols absorb less light than at the beginning of the measurements. The trends of the single-scattering albedo and backscattering fraction influenced the aerosol radiative forcing efficiency, indicating that the aerosol particles are scattering the radiation more effectively back into space.


2018 ◽  
Vol 10 (4) ◽  
pp. 518 ◽  
Author(s):  
Kai Qin ◽  
Luyao Wang ◽  
Jian Xu ◽  
Husi Letu ◽  
Kefei Zhang ◽  
...  

Aerosol haze pollution has had a significant impact on both global climate and the regional air quality of Eastern China, which has a high proportion of high level pollution days. Statistical analyses of aerosol optical properties and direct radiative forcing at two AERONET sites (Beijing and Xuzhou) were conducted from 2013 to 2016. Results indicate: (1) Haze pollution days accounted for 26% and 20% of days from 2013 to 2016 in Beijing and Xuzhou, respectively, with the highest proportions in winter; (2) The averaged aerosol optical depth (AOD) at 550 nm on haze days were about 3.7 and 1.6 times greater than those on clean days in Beijing and Xuzhou, respectively. At both sites, the maximum AOD occurred in summer; (3) Hazes were dominated by fine particles at both sites. However, as compared to Xuzhou, Beijing had larger coarse mode AOD and higher percentage of small α. This data, together with an analysis of size distribution, suggests that the hazes in Beijing were more susceptible to coarse dust particles than Xuzhou; (4) During hazes in Beijing, the single scattering albedo (SSA) is significantly higher when compared to clean conditions (0.874 vs. 0.843 in SSA440 nm), an increase much less evident in Xuzhou. The most noticeable differences in both SSA and the imaginary part of the complex refractive index between Beijing and Xuzhou were found in winter; (5) In Beijing, the haze radiative forcing produced an averaged cooling effect of −113.6 ± 63.7 W/m2 at the surface, whereas the averaged heating effect of 77.5 ± 49.7 W/m2 within the atmosphere was at least twice as strong as clean days. In Xuzhou, such a radiative forcing effect appeared to be much smaller and the difference between haze and clean days was insignificant. Derived from long-term observation, these findings are more significant for the improvement of our understanding of haze formation in China and the assessment of its impacts on radiative forcing of climate change than previous short-term case studies.


Atmosphere ◽  
2020 ◽  
Vol 11 (6) ◽  
pp. 655
Author(s):  
Dapeng Zhao ◽  
Yan Yin ◽  
Min Zhang ◽  
Honglei Wang ◽  
Chunsong Lu ◽  
...  

To study the optical properties of background atmospheric aerosols in East China, we carried out observations of the physical, chemical and optical properties of atmospheric aerosols at the summit of Mount Tai (Mt. Tai, 1533.7 m above sea level) from 13 May to 25 June 2017. The results show that the average scattering coefficient ( σ sca , 550 ) at 550 nm of the aerosols at the summit of Mt. Tai is 40.3 Mm−1, and the average absorption coefficient ( σ abs , 550 ) at 550 nm is 16.0 Mm−1. The complex refractive index of aerosols is a key parameter for aerosol retrieval and modeling. There are few studies on the equivalent complex refractive index of aerosol in the Taishan area. We calculated the aerosol equivalent complex refractive index using the observed aerosol scattering coefficients, absorption coefficients and particle size distribution data, providing more data support for future modeling in this region. The real part (n) of the complex refractive index at 550 nm of aerosol ranges from 1.31 to 1.98 (mostly under 1.50), with an average value of 1.38, while the imaginary part (k) ranges from 0.014 to 0.251 (less than 0.10 for over 95% samples), with an average value of 0.040. The analysis of the n and k of the aerosol average complex refractive index shows that the scattering properties of the aerosols at the summit of Mt. Tai are relatively weak and the absorption properties are relatively strong when compared with those of other kinds of aerosols. The k of the aerosol complex refractive index at the summit of Mt. Tai has strong correlations with the wind speed, temperature, as revealed by the correlation analysis.


2015 ◽  
Vol 15 (22) ◽  
pp. 33675-33730
Author(s):  
X. Xu ◽  
W. Zhao ◽  
Q. Zhang ◽  
S. Wang ◽  
B. Fang ◽  
...  

Abstract. The optical properties and chemical composition of PM1.0 (particulate with an aerodynamic diameter of less than 1.0 μm) particles in a suburban environment (Huairou) near the mega-city Beijing were measured during the HOPE-J3A (Haze Observation Project Especially for Jing-Jin-Ji Area) field campaign. The campaign covered the period November 2014 to January 2015 during the winter coal heating season. The average and standard deviations for the extinction, scattering, absorption coefficients, and the aerosol single scattering albedo (SSA) at λ = 470 nm during the measurement period were 201 ± 240, 164 ± 202, 37 ± 43 Mm-1, and 0.80 ± 0.08, respectively. The mean mass scattering (MSE) and absorption (MAE) efficiencies were 4.77 ± 0.01 and 0.87 ± 0.03 m2g-1, respectively. Highly time-resolved air pollution episodes clearly show the dramatic evolution of the PM1.0 size distribution, extensive optical properties (extinction, scattering, and absorption coefficients) and intensive optical properties (single scattering albedo and complex refractive index) during haze formation, development and decline. Time periods were classified into three different pollution levels (clear, slightly polluted, and polluted) for further analysis. It was found that: (1) The diurnal patterns of the aerosol extinction, scattering, absorption coefficients, and SSA differed for the three pollution classes. (2) The real and imaginary part of complex refractive index (CRI) increased, while the SSA decreased from clear to polluted days. (3) The relative contributions of organic and inorganic species to observed aerosol composition changed significantly from clear to polluted days: the organic mass fraction decreased (50 to 43 %) while the proportion of sulfates, nitrates, and ammonium increased strongly (34 to 44 %). (4) The fractional contribution of chemical components to extinction coefficients was calculated by using the modified IMPROVE algorithm. Organic mass was the largest contributor (58 %) to the total extinction of PM1.0. When the air quality deteriorated, the change of the relative contribution of sulfate aerosol to the total extinction was small, but the contribution of nitrate aerosol increased significantly (from 17 % on clear days to 23 % on polluted days). (5) The observed mass scattering efficiencies increased consistently with the pollution extent, however, the observed mass absorption efficiencies increased consistently with increasing mass concentration in slightly pollution conditions, but decreased under polluted conditions.


2019 ◽  
Vol 19 (14) ◽  
pp. 9181-9208 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.


2021 ◽  
Vol 21 (17) ◽  
pp. 12989-13010
Author(s):  
Baseerat Romshoo ◽  
Thomas Müller ◽  
Sascha Pfeifer ◽  
Jorge Saturno ◽  
Andreas Nowak ◽  
...  

Abstract. The formation of black carbon fractal aggregates (BCFAs) from combustion and subsequent ageing involves several stages resulting in modifications of particle size, morphology, and composition over time. To understand and quantify how each of these modifications influences the BC radiative forcing, the optical properties of BCFAs are modelled. Owing to the high computational time involved in numerical modelling, there are some gaps in terms of data coverage and knowledge regarding how optical properties of coated BCFAs vary over the range of different factors (size, shape, and composition). This investigation bridged those gaps by following a state-of-the-art description scheme of BCFAs based on morphology, composition, and wavelength. The BCFA optical properties were investigated as a function of the radius of the primary particle (ao), fractal dimension (Df), fraction of organics (forganics), wavelength (λ), and mobility diameter (Dmob). The optical properties are calculated using the multiple-sphere T-matrix (MSTM) method. For the first time, the modelled optical properties of BC are expressed in terms of mobility diameter (Dmob), making the results more relevant and relatable for ambient and laboratory BC studies. Amongst size, morphology, and composition, all the optical properties showed the highest variability with changing size. The cross sections varied from 0.0001 to 0.1 µm2 for BCFA Dmob ranging from 24 to 810 nm. It has been shown that MACBC and single-scattering albedo (SSA) are sensitive to morphology, especially for larger particles with Dmob > 100 nm. Therefore, while using the simplified core–shell representation of BC in global models, the influence of morphology on radiative forcing estimations might not be adequately considered. The Ångström absorption exponent (AAE) varied from 1.06 up to 3.6 and increased with the fraction of organics (forganics). Measurement results of AAE ≫ 1 are often misinterpreted as biomass burning aerosol, it was observed that the AAE of purely black carbon particles can be ≫ 1 in the case of larger BC particles. The values of the absorption enhancement factor (Eλ) via coating were found to be between 1.01 and 3.28 in the visible spectrum. The Eλ was derived from Mie calculations for coated volume equivalent spheres and from MSTM for coated BCFAs. Mie-calculated enhancement factors were found to be larger by a factor of 1.1 to 1.5 than their corresponding values calculated from the MSTM method. It is shown that radiative forcings are highly sensitive to modifications in morphology and composition. The black carbon radiative forcing ΔFTOA (W m−2) decreases up to 61 % as the BCFA becomes more compact, indicating that global model calculations should account for changes in morphology. A decrease of more than 50 % in ΔFTOA was observed as the organic content of the particle increased up to 90 %. The changes in the ageing factors (composition and morphology) in tandem result in an overall decrease in the ΔFTOA. A parameterization scheme for optical properties of BC fractal aggregates was developed, which is applicable for modelling, ambient, and laboratory-based BC studies. The parameterization scheme for the cross sections (extinction, absorption, and scattering), single-scattering albedo (SSA), and asymmetry parameter (g) of pure and coated BCFAs as a function of Dmob were derived from tabulated results of the MSTM method. Spanning an extensive parameter space, the developed parameterization scheme showed promisingly high accuracy up to 98 % for the cross sections, 97 % for single-scattering albedos (SSAs), and 82 % for the asymmetry parameter (g).


2019 ◽  
Author(s):  
Zhe Jiang ◽  
Minzheng Duan ◽  
Huizheng Che ◽  
Wenxing Zhang ◽  
Teruyuki Nakajima ◽  
...  

Abstract. This study analyzed the aerosol optical properties derived by SKYRAD.pack versions 5.0 and 4.2 using the radiometer measurements over Qionghai and Yucheng in China, two new sites of the sky radiometer network (SKYNET). The volume size distribution retrieved by V5.0 presented bimodal patterns with a 0.1–0.2 μm fine particle mode and a 5–6 μm coarse particle mode both over Qionghai and Yucheng. The differences of the volume size distributions between the two versions were very large for the coarse mode with a radius of over 5 μm. The mean values of single scattering albedo (SSA) at 500 nm retrieved from V5.0 were approximately 0.02 lower, but 0.03 higher than those from V4.2 in Qionghai and Yucheng, respectively. The average imaginary part of the complex refractive index (mi) retrieved from V5.0 at all wavelengths was systemically higher than those by V4.2 over Qionghai. Moreover, the differences between the real parts of the complex refractive index (mr) obtained using the two versions were within 4.25 % both at Yucheng and Qionghai. The seasonal variability of the aerosol properties over Qionghai and Yucheng were investigated based on SKYRAD.pack V5.0. The seasonal average SSA during the winter was larger than those in other seasons in Yucheng, while the lowest SSA values occurred in winter over Qionghai. Meanwhile, the mr showed a minimum in winter over both sites. The results can provide validation data in China for SKYNET to continue improving the data-processing and inversion method. The results provide valuable references for continued improvement of the retrieval algorithms of SKYNET and other aerosol observational networks.


2016 ◽  
Author(s):  
B. L. Zhuang ◽  
T. J. Wang ◽  
J. Liu ◽  
S. Li ◽  
M. Xie ◽  
...  

Abstract. Observational studies of aerosol optical properties are useful to reducing uncertainties in estimating aerosol radiative forcing and forecasting visibility. In this study, the observed near-surface aerosol optical properties in urban Nanjing are analyzed from Mar 2014 to Feb 2016. Results show that near-surface urban aerosols in Nanjing are mainly from local emissions and the regions around. They have lower loadings but are more scattering than in most cities in China. The annual mean aerosol extinction coefficient (EC), single scattering albedo (SSA) and asymmetry parameter (ASP) at 550 nm are 381.96 Mm−1, 0.9 and 0.57, respectively. The aerosol absorption coefficient (AAC) is about one order of magnitude smaller than its scattering coefficient (SC). However, the absorbing aerosol has larger Ångström exponent (AAE) value, 1.58 at 470/660 nm, about 0.2 larger than the scattering aerosols' (SAE). All the aerosol optical properties followed a near unimodal pattern, the ranges around their averages accounting for more than 60 % of the total samplings. Additionally, they have substantial seasonality and diurnal variations. High levels of SC and AAC all appear in winter due to higher aerosol and trace gas emissions. AAE (ASP) is the smallest (largest) in summer because of high relative humidity (RH) which also causes considerably larger SC and smaller SAE, although intensive gas-to-particle transformation could produce a large number of finer scattering aerosols in this season. Seasonality of EC is different from the columnar aerosol optical depth. Larger AACs appear at the rush hours of the day while SC and Bsp only peak in the early morning. Aerosols are fresher at daytime than at nighttime, leading to their larger AE and smaller ASP. Different temporal variations between AAC and SC cause the aerosols more absorbing (smaller SSA) in autumn and around rush hours. ASP has a good quasi-LogNormal growth trend with increasing SC when RH is below 60 %. The correlation between AAC and SC at the site is close but a little smaller than that in suburban Nanjing in spring. Atmospheric visibility decreases exponentially with increasing EC or SC, more sharply in spring and summer. It could be further deteriorated with increasing SSA and ASP.


Sign in / Sign up

Export Citation Format

Share Document