scholarly journals Observations on aerosol optical properties and scavenging during cloud events

2020 ◽  
Author(s):  
Antti Ruuskanen ◽  
Sami Romakkaniemi ◽  
Harri Kokkola ◽  
Antti Arola ◽  
Santtu Mikkonen ◽  
...  

Abstract. Long term statistics of atmospheric aerosol and especially cloud scavenging were studied at the Puijo measurement station in Kuopio, Finland, during October 2010–November 2014. Aerosol size distributions, scattering coefficients at three different wavelengths (450 nm, 550 nm, and 700 nm), and absorption coefficient at wavelength 637 nm were measured with a special inlet system to sample interstitial and total aerosol in clouds. On average, accumulation mode particle concentration was found to be temperature dependent with lowest average concentrations of 200 cm−3 around 0 °C increasing to more than 800 cm−3 for temperatures higher than 20 °C. From the in-cloud measurements, both scattering and absorbing material scavenging efficiencies were observed to have slightly increasing temperature dependence. At 0 °C the efficiencies of scattering and absorbing matter were 0.85 and 0.55 with slopes of 0.005 °C−1 and 0.003 °C−1, respectively. Additionally, scavenging efficiencies were studied as a function of the diameter at which half of the particles are activated into cloud droplets. This analysis indicated that the is a higher fraction of absorbing material, typically black carbon, in smaller sizes so that at least 20–30 % of interstitial particles within clouds consist of absorbing material. In addition, the PM1-inlet revealed that approximately 20 % of absorbing material was observed to reside in particles with ambient diameter larger than ~ 1 µm at relative humidity below 90 %. Similarly, 40 % of scattering material was seen to be in particles larger than 1 µm. Altogether, this dataset provides information on size dependent aerosol composition that can be applied in evaluating how well large-scale aerosol models reproduce aerosol composition, especially with respect to scavenging in stratus clouds.

2021 ◽  
Vol 21 (3) ◽  
pp. 1683-1695
Author(s):  
Antti Ruuskanen ◽  
Sami Romakkaniemi ◽  
Harri Kokkola ◽  
Antti Arola ◽  
Santtu Mikkonen ◽  
...  

Abstract. Long-term statistics of atmospheric aerosol and especially cloud scavenging were studied at the Puijo measurement station in Kuopio, Finland, during October 2010–November 2014. Aerosol size distributions, scattering coefficients at three different wavelengths (450, 550, and 700 nm), and absorption coefficient at wavelength 637 nm were measured with a special inlet system to sample interstitial and total aerosol in clouds. On average, accumulation mode particle concentration was found to be correlated with temperature with the lowest average concentrations of 200 cm−3 around 0 ∘C increasing to 800 cm−3 at 20 ∘C. The scavenging efficiencies of both scattering and absorbing material were observed to have a slightly positive temperature correlation in in-cloud measurements. At 0 ∘C, the scavenging efficiencies of scattering and absorbing material were 0.85 and 0.55 with slopes of 0.005 and 0.003 ∘C−1, respectively. Scavenging efficiencies were also studied as a function of the diameter at which half of the particles are activated into cloud droplets. This analysis indicated that there is a higher fraction of absorbing material, typically black carbon, in smaller sizes so that at least 20 %–30 % of interstitial particles within clouds consist of absorbing material. In addition, the PM1 inlet revealed that approximately 20 % of absorbing material was observed to reside in particles with ambient diameter larger than ∼ 1 µm at relative humidity below 90 %. Similarly, 40 % of scattering material was seen to be in particles larger than 1 µm. Altogether, this dataset provides information on the size-dependent aerosol composition and in-cloud scavenging of different types of aerosol. The dataset can be useful in evaluating how well the size-dependent aerosol composition is simulated in global aerosol models and how well these models capture the in-cloud scavenging of different types of aerosol in stratus clouds.


2013 ◽  
Vol 26 (21) ◽  
pp. 8378-8391 ◽  
Author(s):  
Yi Zhang ◽  
Rucong Yu ◽  
Jian Li ◽  
Weihua Yuan ◽  
Minghua Zhang

Abstract Given the large discrepancies that exist in climate models for shortwave cloud forcing over eastern China (EC), the dynamic (vertical motion and horizontal circulation) and thermodynamic (stability) relations of stratus clouds and the associated cloud radiative forcing in the cold season are examined. Unlike the stratus clouds over the southeastern Pacific Ocean (as a representative of marine boundary stratus), where thermodynamic forcing plays a primary role, the stratus clouds over EC are affected by both dynamic and thermodynamic factors. The Tibetan Plateau (TP)-forced low-level large-scale lifting and high stability over EC favor the accumulation of abundant saturated moist air, which contributes to the formation of stratus clouds. The TP slows down the westerly overflow through a frictional effect, resulting in midlevel divergence, and forces the low-level surrounding flows, resulting in convergence. Both midlevel divergence and low-level convergence sustain a rising motion and vertical water vapor transport over EC. The surface cold air is advected from the Siberian high by the surrounding northerly flow, causing low-level cooling. The cooling effect is enhanced by the blocking of the YunGui Plateau. The southwesterly wind carrying warm, moist air from the east Bay of Bengal is uplifted by the HengDuan Mountains via topographical forcing; the midtropospheric westerly flow further advects the warm air downstream of the TP, moistening and warming the middle troposphere on the lee side of the TP. The low-level cooling and midlevel warming together increase the stability. The favorable dynamic and thermodynamic large-scale environment allows for the formation of stratus clouds over EC during the cold season.


2018 ◽  
Vol 4 (4) ◽  
Author(s):  
Qiang Zhao ◽  
Yang Li ◽  
Zheng Zhang ◽  
Xiaoping Ouyang

The sputtering of graphite due to the bombardment of hydrogen isotopes is crucial to successfully using graphite in the fusion environment. In this work, we use molecular dynamics to simulate the sputtering using the large-scale atomic/molecular massively parallel simulator (lammps). The calculation results show that the peak values of the sputtering yield are between 25 eV and 50 eV. When the incident energy is greater than the energy corresponding to the peak value, a lower carbon sputtering yield is obtained. The temperature that is most likely to sputter is approximately 800 K for hydrogen, deuterium, and tritium. Below the 800 K, the sputtering yields increase with temperature. By contrast, above the 800 K, the yields decrease with increasing temperature. Under the same temperature and incident energy, the sputtering rate of tritium is greater than that of deuterium, which in turn is greater than that of hydrogen. When the incident energy is 25 eV, the sputtering yield at 300 K increases below an incident angle at 30 deg and remains steady after that.


2018 ◽  
Author(s):  
Franz Slemr ◽  
Andreas Weigelt ◽  
Ralf Ebinghaus ◽  
Johannes Bieser ◽  
Carl A. M. Brenninkmeijer ◽  
...  

Abstract. Mercury was measured onboard the IAGOS-CARIBIC passenger aircraft since May 2005 until February 2016 during nearly monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa, and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Elevated upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Using speciation experiments, we show that nearly identical TM and gaseous elementary mercury (GEM) concentrations exist at and below the tropopause. Above the thermal tropopause GEM concentrations are almost always smaller than those of TM and the TM – GEM (i.e. Hg2+) difference increases up to ~ 40 % of TM at ~ 2 km and more above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72 ± 37 and 74 ± 27 yr for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation, and cloud scavenging processes.


2010 ◽  
Vol 10 (13) ◽  
pp. 6435-6459 ◽  
Author(s):  
N. D. Gordon ◽  
J. R. Norris

Abstract. Clouds play an important role in the climate system by reducing the amount of shortwave radiation reaching the surface and the amount of longwave radiation escaping to space. Accurate simulation of clouds in computer models remains elusive, however, pointing to a lack of understanding of the connection between large-scale dynamics and cloud properties. This study uses a k-means clustering algorithm to group 21 years of satellite cloud data over midlatitude oceans into seven clusters, and demonstrates that the cloud clusters are associated with distinct large-scale dynamical conditions. Three clusters correspond to low-level cloud regimes with different cloud fraction and cumuliform or stratiform characteristics, but all occur under large-scale descent and a relatively dry free troposphere. Three clusters correspond to vertically extensive cloud regimes with tops in the middle or upper troposphere, and they differ according to the strength of large-scale ascent and enhancement of tropospheric temperature and humidity. The final cluster is associated with a lower troposphere that is dry and an upper troposphere that is moist and experiencing weak ascent and horizontal moist advection. Since the present balance of reflection of shortwave and absorption of longwave radiation by clouds could change as the atmosphere warms from increasing anthropogenic greenhouse gases, we must also better understand how increasing temperature modifies cloud and radiative properties. We therefore undertake an observational analysis of how midlatitude oceanic clouds change with temperature when dynamical processes are held constant (i.e., partial derivative with respect to temperature). For each of the seven cloud regimes, we examine the difference in cloud and radiative properties between warm and cold subsets. To avoid misinterpreting a cloud response to large-scale dynamical forcing as a cloud response to temperature, we require horizontal and vertical temperature advection in the warm and cold subsets to have near-median values in three layers of the troposphere. Across all of the seven clusters, we find that cloud fraction is smaller and cloud optical thickness is mostly larger for the warm subset. Cloud-top pressure is higher for the three low-level cloud regimes and lower for the cirrus regime. The net upwelling radiation flux at the top of the atmosphere is larger for the warm subset in every cluster except cirrus, and larger when averaged over all clusters. This implies that the direct response of midlatitude oceanic clouds to increasing temperature acts as a negative feedback on the climate system. Note that the cloud response to atmospheric dynamical changes produced by global warming, which we do not consider in this study, may differ, and the total cloud feedback may be positive.


2017 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Xinhui Bi ◽  
Duohong Chen ◽  
...  

Abstract. In the present study, a ground-based counterflow virtual impactor (GCVI) was used to sample cloud droplet residual (cloud RES) particles, while a parallel PM2.5 inlet was used to sample cloud-free or cloud interstitial (cloud INT) particles. The mixing state of black carbon (BC)-containing particles in a size range of 0.1–1.6 µm and the mass concentrations of BC in the cloud-free, RES and INT particles were investigated using a single particle aerosol mass spectrometer (SPAMS) and two aethalometers, respectively, at a mountain site (1690 m a.s.l.) in southern China. The measured BC-containing particles were internally mixed extensively with sulfate, and were activated into cloud droplets to the same extent as all the measured particles. The results indicate the preferential activation of larger particles and/or that the production of secondary compositions shifts the BC-containing particles towards larger sizes. BC-containing particles with an abundance of both sulfate and organics were activated less than those with sulfate but limited organics, implying the importance of the mixing state on the incorporation of BC-containing particles into cloud droplets. The mass scavenging efficiency of BC with an average of 33 % was similar for different cloud events independent of the air mass. This is the first time that both the mixing state and cloud scavenging of BC in China have been reported. Since limited information on BC-containing particles in the free troposphere is available, the results also provide an important reference for the representation of BC concentrations, properties, and climate impacts in modeling studies.


2004 ◽  
Vol 4 (3) ◽  
pp. 715-728 ◽  
Author(s):  
A. Marinoni ◽  
P. Laj ◽  
K. Sellegri ◽  
G. Mailhot

Abstract. The chemical composition of cloud water was investigated during the winter-spring months of 2001 and 2002 at the Puy de Dôme station (1465 m above sea level, 45°46′22′′ N, 2°57′43′′ E) in an effort to characterize clouds in the continental free troposphere. Cloud droplets were sampled with single-stage cloud collectors (cut-off diameter approximately 7 µm) and analyzed for inorganic and organic ions, as well as total dissolved organic carbon. Results show a very large variability in chemical composition and total solute concentration of cloud droplets, ranging from a few mg l-1 to more than 150 mg l-1. Samplings can be classified in three different categories with respect to their total ionic content and relative chemical composition: background continental (BG, total solute content lower than 18 mg l-1), anthropogenic continental (ANT, total solute content from 18 to 50 mg l-1), and special events (SpE, total solute content higher than 50 mg l-1). The relative chemical composition shows an increase in anthropogenic-derived species (NO3-, SO42- and NH4+) from BG to SpE, and a decrease in dissolved organic compounds (ionic and non-ionic) that are associated with the anthropogenic character of air masses. We observed a high contribution of solute in cloud water derived from the dissolution of gas phase species in all cloud events. This was evident from large solute fractions of nitrate, ammonium and mono-carboxylic acids in cloud water, relative to their abundance in the aerosol phase. The comparison between droplet and aerosol composition clearly shows the limited ability of organic aerosols to act as cloud condensation nuclei. The strong contribution of gas-phase species limits the establishment of direct relationships between cloud water solute concentration and LWC that are expected from nucleation scavenging.


2005 ◽  
Vol 5 (4) ◽  
pp. 879-885 ◽  
Author(s):  
S. Romakkaniemi ◽  
H. Kokkola ◽  
A. Laaksonen

Abstract. In this paper we present a parameterization of the nitric acid effect on cloud droplet formation. The new parameterization is intended to be used in large scale models in order to obtain regional and global estimates of the effect of nitric acid on cloud drop concentrations and the radiative balance. The parameterization is based on numerical air parcel model simulations and can be applied for unimodal and bimodal lognormal aerosol particle size distributions in a large variety of different conditions. In addition to the aerosol particle distribution and gas-phase HNO3 concentration, the parameterization requires temperature, total pressure, updraft velocity, and the number concentration of cloud droplets formed at zero nitric acid concentration, as input parameters. The parameterization is also suitable for describing the effect of hydrochloric acid on the cloud drop concentrations, and in practice, the HNO3 and HCl concentrations can be summed up to yield the total effect. The comparison between the parameterization and the results from numerical air parcel model simulations show good consistency.


2018 ◽  
Vol 18 (13) ◽  
pp. 9823-9830 ◽  
Author(s):  
Leah A. Curry ◽  
William G. Tsui ◽  
V. Faye McNeill

Abstract. We present updated recommendations for the reactive uptake coefficients for glyoxal and methylglyoxal uptake to aqueous aerosol particles and cloud droplets. The particle and droplet types considered were based on definitions in GEOS-Chem v11, but the approach is general. Liquid maritime and continental cloud droplets were considered. Aerosol types include sea salt (fine and coarse), with varying relative humidity and particle size, and sulfate/nitrate/ammonium as a function of relative humidity and particle composition. We take into account salting effects, aerosol thermodynamics, mass transfer, and irreversible reaction of the organic species with OH in the aqueous phase. The new recommended values for the reactive uptake coefficients in most cases are lower than those currently used in large-scale models, such as GEOS-Chem. We expect application of these parameterizations will result in improved representation of aqueous secondary organic aerosol formation in atmospheric chemistry models.


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