GSTDTAP  > 地球科学
DOI10.5194/acp-19-8783-2019
Enhanced ice nucleation activity of coal fly ash aerosol particles initiated by ice-filled pores
Umo, Nsikanabasi Silas1; Wagner, Robert1; Ullrich, Romy1; Kiselev, Alexei1; Saathoff, Harald1; Weidler, Peter G.2; Cziczo, Daniel J.3,4; Leisner, Thomas1; Moehler, Ottmar1
2019-07-10
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2019
卷号19期号:13页码:8783-8800
文章类型Article
语种英语
国家Germany; USA
英文摘要

Ice-nucleating particles (INPs), which are precursors for ice formation in clouds, can alter the microphysical and optical properties of clouds, thereby impacting the cloud lifetimes and hydrological cycles. However, the mechanisms with which these INPs nucleate ice when exposed to different atmospheric conditions are still unclear for some particles. Recently, some INPs with pores or permanent surface defects of regular or irregular geometries have been reported to initiate ice formation at cirrus temperatures via the liquid phase in a two-step process, involving the condensation and freezing of supercooled water inside these pores. This mechanism has therefore been labelled pore condensation and freezing (PCF). The PCF mechanism allows formation and stabilization of ice germs in the particle without the formation of macroscopic ice. Coal fly ash (CFA) aerosol particles are known to nucleate ice in the immersion freezing mode and may play a significant role in cloud formation. In our current ice nucleation experiments with a particular CFA sample (CFA_UK), which we conducted in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) aerosol and cloud simulation chamber at the Karlsruhe Institute of Technology (KIT), Germany, we observed a strong increase (at a threshold relative humidity with respect to ice of 101%-105%) in the ice-active fraction for experiments performed at temperatures just below the homogeneous freezing of pure water. This observed strong increase in the ice-active fraction could be related to the PCF mechanism. To further investigate the potential of CFA particles undergoing the PCF mechanism, we performed a series of temperature-cycling experiments in AIDA. The temperature-cycling experiments involve exposing CFA particles to lower temperatures (down to similar to 228 K), then warming them up to higher temperatures (238-273 K) before investigating their ice nucleation properties. For the first time, we report the enhancement of the ice nucleation activity of the CFA particles for temperatures up to 263 K, from which we conclude that it is most likely due to the PCF mechanism. This indicates that ice germs formed in the CFA particles' pores during cooling remain in the pores during warming and induce ice crystallization as soon as the pre-activated particles experience ice-supersaturated conditions at higher temperatures; hence, these pre-activated particles show an enhancement in their ice-nucleating ability compared with the scenario where the CFA particles are directly probed at higher temperatures without temporary cooling. The enhancement in the ice nucleation ability showed a positive correlation with the specific surface area and porosity of the particles. On the one hand, the PCF mechanism can play a significant role in mixed-phase cloud formation in a case where the CFA particles are injected from higher altitudes and then transported to lower altitudes after being exposed to lower temperatures. On the other hand, the PCF mechanism could be the prevalent nucleation mode for ice formation at cirrus temperatures rather than the previously acclaimed deposition mode.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000474738000006
WOS关键词IMMERSION FREEZING BEHAVIOR ; HETEROGENEOUS NUCLEATION ; CLOUD DROPLETS ; SURFACE-AREA ; MINERAL DUST ; ACTIVATION ; NUCLEI ; PARAMETERIZATION ; CRYSTALLIZATION ; FRAGMENTATION
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/184935
专题地球科学
作者单位1.Karlsruhe Inst Technol, Inst Meteorol & Climate Res Atmospher Aerosol Res, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany;
2.Karlsruhe Inst Technol, Inst Funct Interfaces, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany;
3.MIT, Earth Atmospher & Planetary Sci, Civil & Environm Engn, 77 Massachusetts Ave 54-1324, Cambridge, MA 02139 USA;
4.Purdue Univ, Dept Earth Atmospher & Planetary Sci, 550 Lafayette St, W Lafayette, IN 47907 USA
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Umo, Nsikanabasi Silas,Wagner, Robert,Ullrich, Romy,et al. Enhanced ice nucleation activity of coal fly ash aerosol particles initiated by ice-filled pores[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(13):8783-8800.
APA Umo, Nsikanabasi Silas.,Wagner, Robert.,Ullrich, Romy.,Kiselev, Alexei.,Saathoff, Harald.,...&Moehler, Ottmar.(2019).Enhanced ice nucleation activity of coal fly ash aerosol particles initiated by ice-filled pores.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(13),8783-8800.
MLA Umo, Nsikanabasi Silas,et al."Enhanced ice nucleation activity of coal fly ash aerosol particles initiated by ice-filled pores".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.13(2019):8783-8800.
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