Aerosol polarized phase function and single-scattering albedo retrieved from ground-based measurements

Aerosol optical parameters, polarized phase function and single-scattering albdeo, have been retrieved from ground-based sun photometer measurements in Beijing 2003. The measured aerosol optical thickness varies from 0.12 to 0.77 with an average value of 0.39. The measured Ångström coefficient ranges from 0.75 to 1.47 with an average value of 1.21. The retrieved single-scattering albedo at 870 nm is within the 0.76–0.94 range and the average value is 0.85, suggests there are considerable aerosol absorptions in Beijing. The maximum value of retrieved polarized phase function at 870 nm ranges from 0.068 to 0.225 with an average value of 0.16, and it illustrates good correlations with the Ångström coefficient, i.e. the relative size of aerosol particles. Analyses of measurements and theoretical calculations show the polarized phase function is sensitive to aerosol size distribution and complex refractive index, especially the imaginary part of the refractive index which denotes aerosol light absorbing effects. These results suggest that the polarized phase function is an effective and unique aerosol optical parameter and is able to improve the retrieval of aerosol physical properties.     

Interpretation of Mauna Loa atmospheric transmission relative to aerosols,using photometric precipitable water amouts

Precipitable water measurements made coincident in time and space with direct broadband solar irradiance measurements are used in conjunction with an atmospheric transmission model to derive a parameter whose major dependence is on total aerosol extinction. Irradiance measurements are used to calculate an atmospheric transmission factor (ATF) that is independent of the instrument calibration and the extraterrestrial solar constant. The dependency of the ATF on precipitable water is determined using LOWTRAN5, an atmospheric transmission model with high spectral resolution. Precipitable water measurements are then used to adjust the measured ATF to correspond to an ATF value obtained for a constant precipitable water amount. The remaining variability in the adjusted ATF is due mostly to aerosol extinction. The technique is applied to a 6-year period (1978–1983) for clear-sky mornings at Mauna Loa, Hawaii (MLO). MLO ATF aerosol residuals are compared with independently measured monochromatic aerosol optical depth. Results show that the ATF aerosol residual is nearly equal to the 500 nm aerosol optical depth prior to the eruption of E1 Chichon, at which time a nonlinear time-dependent relationship between the two quantities is evident. ATF aerosol residuals reflect the spectrally integrated aerosol influence on transmission and, therefore, could indicate better than monochromatic optical depth the radiation balance perturbations due to aerosols. The 6-year precipitable water record for MLO, determined from a dual-channel sunphotometer, has a mean value of 0.3 cm. An annual cycle in precipitable water is evident, as is a 4-month 5-standard-deviation drought from December 1982 through March 1983.     

火山气溶胶的辐射影响

本文应用辐射传输计算研究了火山气溶胶,特别是大的火山爆发后短时期及火山周围地区内的火山气溶胶,对到达地面的向下的总的太阳辐射通量、行星反照率及大气加热率的可能影响.     

天津城区春节期间大气气溶胶污染特征 和数浓度分布

利用天津城区2009-2014年春节期间大气气溶胶观测资料和相关气象资料,重点分析2013和2014年春节期间气溶胶污染特征,探求燃放烟花爆竹以及气象条件对春节期间大气气溶胶的影响。结果表明,受燃放烟花爆竹影响,春节期间PM_(2.5)质量浓度最高值均发生在除夕夜间;持续雾霾天气条件下燃放烟花爆竹,造成2013年除夕夜间PM_(2.5)质量浓度峰值达到1240μg·m～(-3),是近年来最严重的一次;2014年春节期间烟花爆竹燃放量有所减少,加之空气扩散条件较为有利,PM_(2.5)质量浓度显著低于2013年;不同天气条件下,气溶胶数浓度谱分布特征存在明显差异,燃放烟花爆竹期间气溶胶数浓度水平与严重雾-霾天气相当。     

On the formation and growth of atmospheric nanoparticles

In this paper we summarize recent experimental, theoretical and observational results on the formation and growth of atmospheric nanoparticles. During the last years significant progress has occurred to explain atmospheric nucleation and initial steps of the growth. Due to climatic and health effects of fine and ultrafine particles the formation and growth of new aerosol particles is of growing interest. The question “How and under which conditions does the formation of new atmospheric aerosol particles take place?” has exercised the minds of scientists since the time of John Aitken, who in the late 1880s built the first apparatus to measure the number of dust and fog particles. However, only during the last 15–20 years has the measurement technology developed to such a level that size distributions of nanometer-size particles and concentrations of gases participating in particle formation can be measured in the atmosphere. Also from a theoretical point of view atmospheric nucleation mechanisms have not been resolved: several mechanisms such as ion-induced (or ion mediated) nucleation, ternary and kinetic (barrier-less) nucleation have been suggested. In the most recent theory, the activation of existing neutral and/or ion clusters has been suggested.     

The Global Distribution of Secondary Particulate Matter in a 3-D Lagrangian Chemistry Transport Model

A global 3-D Lagrangian chemistry-transport model STOCHEM is used to describe the tropospheric distributions of four components of the secondary atmospheric aerosol: nitrate, sulphate, ammonium and organic compounds. The model describes the detailed chemistry of the formation of the acid precursors from the oxidation of SO₂, DMS, NO_x, NH₃ and terpenes and their uptake into the aerosol. Model results are compared in some detail with the available surface observations. Comparisons are made between the global budgets and burdens found in other modelling studies. The global distributions of the total mass of secondary aerosols have been estimated for the pre-industrial, present day and 2030 emissions and large changes have been estimated in the mass fractions of the different secondary aerosol components.     

Products and Mechanism of the Gas Phase Reaction of Ozone with β-Pinene

Gas phase ozonolysis of -pinene was performedin a 570 l static reactor at 730 Torr and 296 K insynthetic air and the products were analysed by acombination of gas phase FTIR spectroscopy, HPLC andIC analyses of gas phase and aerosol samples,respectively. The reaction mechanism was investigatedby adding HCHO, HCOOH and H₂O as Criegeeintermediate scavenger and cyclohexane as OH radicalscavenger. Main identified products (yields inparentheses) in the presence of cyclohexane as OHradical scavenger were HCHO (0.65 ± 0.04),nopinone (0.16 ± 0.04), 3-hydroxy-nopinone (0.15± 0.05), CO₂ (0.20 ± 0.04), CO (0.030± 0.002), HCOOH (0.020 ± 0.002), the secondaryozonide of -pinene (0.16 ± 0.05), andcis-pinic acid (0.02 ± 0.01). The decompositionof the primary ozonide was found to yieldpredominantly the excited C₉-Criegee intermediateand HCHO (0.84 ± 0.04) and to a minor extent theexcited CH₂OO intermediate and nopinone (0.16± 0.04). Roughly 40% of the excitedC₉-Criegee intermediate becomes stabilised andcould be shown to react with HCHO, HCOOH and H₂O. The atmospherically important reaction of thestabilised C₉-Criegee intermediate with H₂Owas found to result in a nopinone increase of (0.35± 0.05) and in the formation of H₂O₂(0.24 ± 0.03). Based on the observed products,the unimolecular decomposition/isomerisationchannels of the C₉-Criegee intermediate arediscussed in terms of the hydroperoxide and esterchannels. Subsequent reactions of the nopinonylradical, formed in the hydroperoxide channel, lead tomajor products like 3-hydroxy-nopinone but also tominor products like cis-pinic acid. A mechanismfor the formation of this dicarboxylic acid isproposed and its possible role in aerosol formationprocesses discussed.     

Simulation of the Direct Radiative Effect of Mineral Dust and Sea Salt Aerosols in a Doubled Carbon Dioxide Climate

The authors examine the equilibrium climatic response to the direct radiative effect(DRE)of mineral dust and sea salt aerosols in a doubled-CO2climate with two-way coupling of aerosol-climate interactions.In response to the drier and windier conditions,dust emissions increase by 26%in the Sahara Desert and by 18%on the global scale relative to present day.Sea salt emissions increase in high latitudes(60°)but decrease in middle latitudes(30°–60°)of both hemispheres due to the poleward shift of westerlies,leading to a 3%decrease in global emissions.The burdens of dust and sea salt increase by 31%and 7%respectively,because reductions in rainfall over the tropical oceans increase the lifetime of particles in the warmer climate.The higher aerosol loading in the doubled-CO2climate reinforces aerosol DRE by0.2 W m 2,leading to an additional cooling of 0.1°C at the surface compared with the climatic effects of aerosols in present day.The additional cooling from changes in natural aerosols compensates for up to 15%of the regional warming induced by doubled CO2.     

Aerosol spectra and new particle formation observed in various seasons in Nanjing

The aerosol number spectrum and gas pollutants were measured and the new particle formation （NPF） events were discussed in Nanjing. The results showed that the size distributions of aerosol number concen- trations exhibited distinct seasonal variations, implying the relations of particle sizes and their sources and sinks. The number concentrations of particles in the nuclei mode （10-30 nm）, Aitken mode （30-100 nm）, accumulation mode （100 -1000 nm） and coarse mode （〉1μm） varied in the order of summer 〉 spring 〉 autumn, summer 〉 autumn 〉 spring, autumn 〉 summer 〉 spring, and spring 〉 autumn 〉summer, re- spectively. The diurnal variation of total aerosol number concentrations showed three peaks in all observed periods, which corresponded to two rush hours and the photochemistry period at noon. In general, the NPF in summer occurred under the conditions of east winds and dominant air masses originating from marine areas with high relative humidity （50%-70%） and strong solar radiations （400 -700 W m-2）. In spring, the NPF were generally accompanied by low relative humidity （14%-30%） and strong solar radiations （400-600 W m-2）. The new particle growth rates （GR） were higher in the summertime in the range of 10- 16 nm h-1. In spring, the GR were 6.8-8.3 nm h-1. Under polluted air conditions, NPF events were seldom captured in autumn in Nanjing. During NPF periods, positive correlations between 10- 30 nm particles and 03 were detected, particularly in spring, indicating that NPF can be attributed to photochemical reactions.     

气态SO_2转化及其数值模型研究

本文基于对室外烟雾箱实验,探讨了SO_2的转化机制及影响SO_2转化的因素,由此并借助于烟团模型,建立了SO_2转化和硫酸盐气溶胶细粒子生成的数值模型,用于估算从排放源排入大气的SO_2浓度及其转化成硫酸盐细粒子的浓度以及它们的空间分布,与实测结果相比,两者有较好的一致性.同时指出,由于大气中细粒子(粒径小于1μm)可通过人体呼吸进入并沉积在肺泡中而对健康有不利影响,从而说明研究大气中细粒子污染的迫切性.