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Which published papers have transformed our understanding of the chemical processes in the troposphere, and shaped the field of atmospheric chemistry? 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.
Which published papers have transformed our understanding of the chemical processes in the...
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https://doi.org/10.5194/acp-2020-1266
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-1266
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
04 Jan 2021
04 Jan 2021
Review status: this preprint is currently under review for the journal ACP.
Opinion: Papers that shaped Tropospheric Chemistry
- 1School of Chemistry, University of Leicester, University Rd., Leicester, LE1 7RH, UK
- 2Colorado State University, Fort Collins, Colorado, USA
- 3Institute for Advanced Sustainability Studies, Berlinerstrasse 130, 14467 Potsdam, Germany
- 1School of Chemistry, University of Leicester, University Rd., Leicester, LE1 7RH, UK
- 2Colorado State University, Fort Collins, Colorado, USA
- 3Institute for Advanced Sustainability Studies, Berlinerstrasse 130, 14467 Potsdam, Germany
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.
How to cite. Monks, P. S., Ravishankara, A. R., von Schneidemesser, E., and Sommariva, R.: Opinion: Papers that shaped Tropospheric Chemistry, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2020-1266, in review, 2021.
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Paul S. Monks et al.
Status: open (until 01 Mar 2021)
Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor
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CC1: 'Comment on acp-2020-1266', Joel Savarino, 05 Jan 2021
reply
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.
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CC2: 'Comment on acp-2020-1266', Pawan Gupta, 05 Jan 2021
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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.
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CC3: 'Comment on acp-2020-1266', Viney Aneja, 05 Jan 2021
reply
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2020-1266/acp-2020-1266-CC3-supplement.pdf
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CC4: 'Comment on acp-2020-1266', Sandro Fuzzi, 07 Jan 2021
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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.
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CC5: 'Comment on acp-2020-1266', Sandro Fuzzi, 08 Jan 2021
reply
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CC6: 'Comment on acp-2020-1266', Sandro Fuzzi, 08 Jan 2021
reply
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2020-1266/acp-2020-1266-CC6-supplement.pdf
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CC7: 'Comment on acp-2020-1266', Nick Hewitt, 14 Jan 2021
reply
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.
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CC8: 'Comment on acp-2020-1266', David Griffith, 15 Jan 2021
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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.
- Measurement techniques. We might divide up the whole topic into two sub topics – the chemistry itself, and the methods used to probe it. Many advances in our understanding of atmospheric chemistry have come from stepwise advances in measurement (and modelling) capabilities. There are already explicit sections for kinetics, models, meteorology and transport and satellite measurements, but nothing explicitly for chemical measurement techniques. The success of the high impact journal AMT speaks for the importance. Examples of discoveries that might be included in this area might be (but are not limited to):
- The ECD detector (Lovelock), which enabled the detection of halocarbons
- PTR-MS – already mentioned in 2.12 in the VOC context
- OH measurements – LIF etc.
- The chemiluminescence technique for NO and NOx
- Dobson method for O3 (admittedly stratospheric)
- Satellite retrievals – satellite global mapping of composition has been a real revolution.
- Greenhouse and climate-relevant gases (and aerosols). Given the current state and importance of climate change science and policy, a separate section on greenhouse and other climate-relevant species seems to me to be very desirable. There are some mentions throughout, eg to Keeling and to long term monitoring networks like ALE/AGAGE. GAW, NOAA, ICOS, but it would be valuable to bring them together into their own section. Also the techniques that enable reliable and accurate long term records to be maintained – NDIR, optical in situ and remote sensing techniques, isotopic methods, and satellite measurements (again).
- Measurement techniques. We might divide up the whole topic into two sub topics – the chemistry itself, and the methods used to probe it. Many advances in our understanding of atmospheric chemistry have come from stepwise advances in measurement (and modelling) capabilities. There are already explicit sections for kinetics, models, meteorology and transport and satellite measurements, but nothing explicitly for chemical measurement techniques. The success of the high impact journal AMT speaks for the importance. Examples of discoveries that might be included in this area might be (but are not limited to):
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RC1: 'Comment on acp-2020-1266', Anonymous Referee #1, 18 Jan 2021
reply
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.
- Line 34: Suggest adding at least one other review from the health community re: human health impacts, e.g. by Landrigan et al in Lancet, 2018. The introduction says it is only treating papers 2010 and earlier but cites a 2015 Lelieveld paper for health effects so I assume later papers than 2010 are being cited for background?
- Throughout, the word "aerosols" is used to denote "particles". Historically, the engineers who developed much of this area and the instrumentation have defined aerosols as particles and the gas in which they are suspended (e.g. see Hinds book). This would be a good place to exhibit consistency and use "aerosol particles" throughout, or just "particles" if that is what they mean.
- Line 360: As the authors indicate in the introduction, the fundamental work on which significant advances are made often ends up not being cited as the field develops. The laser ionization MS technique I think originated with Sinha, Rev. Sci. Instrum. (1984), followed by papers coauthored with Friedlander. It might be appropriate to include one of these references along with Prather and Murphy.
- Line 367: I would add for clarity at the end of the sentence on this line "that assumed low viscosity, liquid-like particles where exchange with the gas phase is fast".
- Line 445: They state that the "distinction between heterogenous and multiphase chemistry is not always clear". This would be a good place to define these terms.
- Lines 453-469: These two paragraphs mix multiphase and heterogenous chemistry in a somewhat random order. I think they are using "heterogeneous" to mean reactions at surfaces and "multiphase" to mean reactions involving the uptake of gases into (and reaction in) the liquid phase. It would be good to define the terms first and then separate out the examples they give into the two bins.
- Line 455-459: This cites the work of Akimoto et al on the photoenhancement of HONO formation but it seems some discussion of the dark formation of HONO should come first. The Pitts et al, Int. J. Chem. Kin. (1984) might be the first discussion of this in chambers. Finlayson-Pitts et al, PCCP (2003) is a review of the area to that point.
- Lines 571-573: It reads as if Sillman (1999) was the first to put together ozone isopleths but this goes back into the 1950's or 60's, probably Haagen-Smit and Fox (1954). It would be good to cite the origins here as it is so important to our understanding even today.
- Lines 685-692: Shroeder and Urone (EST, 1974) were probably the first to suggest sea salt reactions as a photochemical source of chlorine atoms. It could be cited here and on line 704. A review by Cicerone in Rev. Geophys. Space Phys. (1981) would be a good review too.
- Line 846: It seems odd to state that emission inventories were pioneered in the 1990's. Surely they were being developed long before that, at least in California?
- Lines 925-927: Satellites have been really useful for tracking dust events but it seems that either here or in another section a reference to the seminal studies on dust transport of Prospero et al in the 1970's should be included.
- Line 988: "by now phased out the ozone-depleting gases". I think this is overly optimistic to say this, given recent measurements showing there seem to be emissions from Asia that were not expected. Maybe "are now phasing out ozone-depleting gases"...
- Table 1 seems quite Euro-centric, for example not including some of the big smog events in the U.S. and the passage of the Clean Air Act etc.
- Table 2 is in two parts. It was not clear to this reviewer how they differ from each other in what they are supposed to illustrate.
- Table 3 seems out of context. It is very detailed on NOx but similar detail is not given for other species. I suggest omitting this.
- Appendix 1 data go to 2020. Since the focus of the article is 2010 and prior years, some comment in the captions might be appropriate.
Minor typos, grammar etc:
- Line 34: impacts.
- Line 35: "latterly links to their climate" is very awkward. Maybe replace "latterly links to their climate" with "and climate"
3.Line 178: "pollutions"
- Line 626: "any" should be "many"?
- Line 824: "..most cited paper"
- Line 885: Should "The study" be omitted so the sentence starts: "Moody et al (1998) ..."
- Line 900: Spelling error "emmited"
- The formatting of the references (no space between etc) makes them very hard to read but I suppose that will get straightened out in the final document.
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CC9: 'Comment on Emission and Deposition', Thomas Karl, 21 Jan 2021
reply
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.
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Which published papers have transformed our understanding of the chemical processes in the troposphere, and shaped the field of atmospheric chemistry? 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.
Which published papers have transformed our understanding of the chemical processes in the...
Atmospheric Chemistry and Physics
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