scholarly journals Supplementary material to "Insight into the in-cloud formation of oxalate based on in situ measurement by single particle mass spectrometry"

Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Yuxiang Yang ◽  
Yuzhen Fu ◽  
...  
2017 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Yuxiang Yang ◽  
Yuzhen Fu ◽  
...  

Abstract. While ground-based works suggest the significance of in-cloud production (or aqueous formation) to oxalate, direct evidence is rare. With the in situ measurements performed at a remote mountain site (1690 m a.s.l.) in southern China, we first reported the size-resolved mixing state of oxalate in the cloud droplet residual (cloud RES), the cloud interstitial (cloud INT), and ambient (cloud-free) particles by single particle mass spectrometry. The results support the growing evidence that in-cloud aqueous reactions promote the formation of oxalate, with ~ 15 % of the cloud RES and cloud INT particles containing oxalate, in contrast to only ~ 5 % of the cloud-free particles. Furthermore, individual particle analysis provides unique insight into the formation and evolution of oxalate during in-cloud processing. Oxalate was predominantly (> 70 % in number) internally mixed with the aged biomass burning particles, highlighting the impact of biomass burning on the formation of oxalate. In contrast, oxalate was underrepresented in aged elemental carbon particles, although they represented the largest fraction of the detected particles. It can be interpreted by the individual particle mixing state that the aged biomass burning particles contained an abundance of organic components serving as precursors for oxalate. Through the analysis of the relationship between oxalate and organic acid ions (−45[HCO2]−, −59[CH3CO2]−, −71[C2H3CO2]−, −73[C2HO3]−), the results show that in-cloud aqueous reaction dramatically improved the conversion of organic acids to oxalate. The abundance of glyoxylate associated with the aged biomass burning particles is the controlling factor for the in-cloud production of oxalate. Since only limited information on oxalate is available in the free troposphere, the results also provide an important reference for future understanding of the abundance, evolution and climate impacts of oxalate.


2017 ◽  
Vol 17 (22) ◽  
pp. 13891-13901 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Yuxiang Yang ◽  
Yuzhen Fu ◽  
...  

Abstract. While ground-based works suggest the significance of in-cloud production (or aqueous formation) to oxalate, direct evidence is rare. With the in situ measurements performed at a remote mountain site (1690 m above sea level) in southern China, we first reported the size-resolved mixing state of oxalate in the cloud droplet residual (cloud RES), the cloud interstitial (cloud INT), and ambient (cloud-free) particles by single particle mass spectrometry. The results support the growing evidence that in-cloud aqueous reactions promote the formation of oxalate, with  ∼  15 % of the cloud RES and cloud INT particles containing oxalate in contrast to only  ∼  5 % of the cloud-free particles. Furthermore, individual particle analysis provides unique insight into the formation of oxalate during in-cloud processing. Oxalate was predominantly (> 70 % in number) internally mixed with the aged biomass-burning particles, highlighting the impact of biomass burning on the formation of oxalate. In contrast, oxalate was underrepresented in aged elemental carbon particles, although they represented the largest fraction of the detected particles. It can be interpreted by the individual particle mixing state that the aged biomass-burning particles contained an abundance of organic components serving as precursors for oxalate. Through the analysis of the relationship between oxalate and organic acids (−45[HCO2]−, −59[CH3CO2]−, −71[C2H3CO2]−, −73[C2HO3]−), the results show that in-cloud aqueous reactions dramatically improved the conversion of organic acids to oxalate. The abundance of glyoxylate associated with the aged biomass-burning particles is a controlling factor for the in-cloud production of oxalate. Since only limited information on oxalate is available in the free troposphere, the results also provide an important reference for future understanding of the abundance, evolution, and climate impacts of oxalate.


2020 ◽  
Author(s):  
Johannes Passig ◽  
Julian Schade ◽  
Ellen Iva Rosewig ◽  
Robert Irsig ◽  
Thomas Kröger-Badge ◽  
...  

2016 ◽  
Author(s):  
Maria A. Zawadowicz ◽  
Karl D. Froyd ◽  
Daniel M. Murphy ◽  
Daniel J. Cziczo

Abstract. Measurements of primary biological aerosol particles, especially at altitudes relevant to cloud formation, are scarce. Single particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to ambient data collected at Storm Peak Laboratory to show that 0.04–0.3 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol.


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