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04 Jan 2021
04 Jan 2021
Abstract. Which published papers have transformed our understanding of the chemical processes in the troposphere, and shaped the field of atmospheric chemistry? By way of expert solicitation and interactive peer-review, this paper explores the influence of the ideas in peer-reviewed articles based on the input from our community of atmospheric scientists. We explore how these papers have shaped the development of the field of atmospheric chemistry, and identify the major landmarks in the field of atmospheric chemistry through the lens of those papers' impact on science, legislation and environmental events. We also explore the ways in which one can identify the papers that have most impacted the field and discuss the advantages and disadvantages of the various approaches.
Paul S. Monks et al.
Status: open (until 01 Mar 2021)
Dear authors
thank you for gathering this corpus of founding articles to understand the construction, evolution and fundamental discoveries of this discipline that is the chemistry of the atmosphere. This article will remain a reference and an entry point for the new generation of researchers, as well as for the older generation to understand its field and progress.
As indicated at the end of the article, I would like to provide additional information. It seems to me that Lovelock's article (1) and his discovery of DMS (thanks to his invention of the ECD detector (2) which also allowed the first measurements of CFCs) as the reduced sulfur compound emitted by themarine biota(and not H2S as thought previously) would have its place in this article. This article also advances the idea that the MSA resulting from the oxidation of DMS is a probable source of aerosols. It is on the basis of this article that the CLAW hypothesis was born. This article deserves to be mentioned.
In the same vein, I think Patterson's paper on the increase of lead in the air (3) (actually in snow) as well as its decrease since the elimination of lead in gasoline (4) would be worth mentioning. With the elimination of CFCs, this is the other major victory of atmospheric chemistry research over environmental policy.
With regards
1- Lovelock, J. E., Maggs, R. J., and Rasmussen, R. A.: Atmospheric Dimethyl Sulphide and the Natural Sulphur Cycle, Nature, 237, 452-453, 10.1038/237452a0, 1972.
2- Lovelock, J. E., SR Lipsky,Electron Affinity Spectroscopy-A New Method for the Identification of Functional Groups in Chemical Compounds Separated by Gas Chromatography -Journal of the American Chemical, 82, 431, 1960.
3-Murozumi, M., Chow, T. J., and Patterson, C. (2003): Chemical concentrations of pollutant lead aerosols, terrestrial dusts and sea salts in Greenland and Antarctic snow strata, Geochim. Cosmochim. Acta, 33, 1247-1294, https://doi.org/10.1016/0016-7037(69)90045-3, 1969.
4-Boutron, C. F., Görlach, U., Candelone, J.-P., Bolshov, M. A., and Delmas, R. J.: Decrease in anthropogenic lead, cadmium and zinc in Greenland snows since the late 1960s, Nature, 353, 153-156, 10.1038/353153a0, 1991.
Page 35, Section 2.17 - "A step-change in this area was made with the paper “Estimating 929 ground-level PM2.5 using aerosol optical depth determined from satellite remote sensing” by van Donkelaar et al. (2006) which was the first description of the derivation of surface PM2.5 from satellite AOD, and which has been extensively used to estimate the global impact of particulate matter (both PM2.5 and PM10) on health"
It appears that the above assessment is not correct.
The first paper showing quantitative PM2.5 estimation using satellite AOD was published in 2003 as 'Wang, J., and S. A. Christopher, Intercomparison between satellite-derived aerosol optical thickness and PM2.5 mass: Implications for air quality studies, Geophys. Res. Lett., 30(21), 2095, doi:10.1029/2003GL018174, 2003'
introduced a simple statistical method to estimate PM2.5 using satellite data, later on, the following paper by Liu et al., (2004)
"Liu, Y., Park, R. J., Jacob, D. J., Li, Q., Kilaru, V., and Sarnat, J. A. (2004), Mapping annual mean ground‐level PM2.5 concentrations using Multiangle Imaging Spectroradiometer aerosol optical thickness over the contiguous United States, J. Geophys. Res., 109, D22206, doi:."
first introduced the model scaling approach, which was later adopted by van Donkelaar et al. (2006) and resulted in global estimates of PM2.5 at annual mean levels.
Over the last two decades, there have been several hundreds of papers published in assessing the satellite-derived AODs to estimate surface particulate matter air quality.
I want to congratulate the authors for putting together this interesting overview based on a series of suggestions from the science community.
In the spirit of collaboration that the authors ask for, I have a few comments.
Thanks for this excellent overview of atmopheric chemistry research. It made really interesting reading.
I have a suggestion to make about section 2.13 on biogenic VOCs. Please see the linked document.
Dear Paul, Ravi et al.,
Thank you for the considerable effort in putting this history together – to one active in the field since the late 1970s (when the curve in Fig 1 kicks off), it is an enjoyable read, and a trip down memory lane.
Inevitably, having solicited them, you will get lots of suggestions for things that you have left out or rated less important than judged by others. Already there are several… So I will add mine, for your consideration. Two areas in my view deserve their own explicit subsection of section 2. Some aspects are already mentioned in passing in several places, but my judgement would be that they deserved their own explicit subsection.
This is a wonderful paper that will provide many future generations of atmospheric scientists some perspective on how the field developed and its current status. The limitations and approach taken are clearly stated and their emphasis on integrating all aspects of the field, ambient measurements, lab studies and modeling, is terrific.
This reviewer has just a few suggestions and minor typo's etc.
Minor typos, grammar etc:
3.Line 178: "pollutions"
This is an excellent and broad perspective on tropospheric chemistry. As such it will certainly become a valuable reference and resource. As already pointed out by Nick Hewitt, it was actually Sanadze who first reported substantial isoprene emissions from plants in Russia (1957). Rasmussen independently found similar results in the US. I highly recommend the review article by Sharkey and Monson on 60 years of isoprene research. (Isoprene research – 60 years later, the biology is still enigmatic, doi: 10.1111/pce.12930, 2017). Further it is mentioned that "recent interest in deposition reemerged", but that physio-chemical parameters are lacking. Physio – chemical parameters for most gases (e.g. HLC, vapor pressure, reactivity etc.) are very well established and an important reason why the ‘Wesely scheme’ works quite well for classic air pollutants over many surface types. I would argue that the complication stems more from a range of oxygenated VOC that can exhibit bi-directional exchange above vegetation (e.g. doi: 10.1126/science.1192534, doi: 10.1126/science.1235053). Moreover it was recently demonstrated that plants can also "reprocess" OVOCs, produced during atmospheric oxidation, through enzymatic reactions (doi: 10.1038/s43247-020-00041-2 ). The concept of bi-directional exchange is not included in the theoretical framework of emission and deposition models as there is little need for most gases. Yet, it is somewhat overlooked when discussing the fate of reactive organic carbon as many oxygenated volatile species can reside in this no-man’s land.
Paul S. Monks et al.
Paul S. Monks et al.
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