the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement Report: Wintertime new particle formation in the rural area of the North China Plain – influencing factors and possible formation mechanism
Juan Hong
Min Tang
Qiaoqiao Wang
Nan Ma
Shaowen Zhu
Shaobin Zhang
Xihao Pan
Linhong Xie
Uwe Kuhn
Jiangchuan Tao
Yao He
Wanyun Xu
Runlong Cai
Yaqing Zhou
Zhibin Wang
Guangsheng Zhou
Yafang Cheng
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- Final revised paper (published on 22 May 2023)
- Supplement to the final revised paper
- Preprint (discussion started on 15 Dec 2022)
- Supplement to the preprint
Interactive discussion
Status: closed
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RC1: 'Comment on acp-2022-784', Anonymous Referee #1, 10 Feb 2023
The measurement report "Wintertime new particle formation in the rural area of North China Plain" by Hong et al. presents measurements of particle size distribution at a rural measurement site, Gucheng, located at the North China Plain (NCP). The measurements were carried out between November and December 2018. With their measurements down to sub 3 nm particles, they aim to gain a better understanding of the new particle formation mechanisms in the rural area of the NCP and compare the results to studies in nearby urban environment.The study shows deficiencies regarding citations, phrasing and data transparency, which have to be addressed.
General comments:
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The authors refer to size bins of the PSM in nm size with 2 digit precision (e.g. line 1471.34-1.39 nm) and further refer to J rates and GR for 1.34 nm particles. I would suggest to round this number, as other studies show, that there is e.g. an uncertainty of 0.1 nm for the calibration of the PSM (Kangasluoma et al., 2015) and also other particle instruments, such as CPCs have an uncertainty for the cut-off size of 0.2 nm (e.g. stated in Dada et al., 2020). I am not sure the PSM can distinguish the sizes down to 0.01 nm difference in diameter.
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In section 2.2.3 the authors mention measurements with an ACSM, however I did not find any data shown from this instrument in this measurement report. Was the data used for the study? If so, could it support the NPF mechanism assumptions of the study?
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Do I interpret this correctly from Fig. 2 that there are NPF events at the GC site almost every day, but they seem to be transported? And on certain days, such as the example in Fig. 3, there is NPF in the range of 1.3-3.7 nm and further a growth is visible in the larger particles, measured by SMPS? Could the authors be more precise regarding the NPF event classification? In Fig. 2 it seems like most events are transported events, since there are barely any paritcles below approx. 18 nm.
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The authors mention several measurements of tracehouse gases, the proxy of sulfuric acid and ACSM data, however only show a fraction or mean of it. I would suggest to add those measurements in the time series plot of figure 2 or potentially in the supplementary, so that the reader gets a clearer idea of the behaviour of the various parameters.
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Figure 5 is not mentioned anywhere in the text. Please include or remove the figure if irrelevant for the study.
Specific remarks:
Line 41: "This implies that H2SO4-amine nucleation..." What is meant by "This"?, the fact that both locations show NPF at the same time? Did the air mass origin from the urban site? Please rephrase to be more clear.Line 42-46: This sentence sounds ambigous; the CS and CoagS are factors that potentially limit the nucleation, as they act as a sink, while H2SO4 is a precursor. Those are two different things, affecting NPF from different angles. Please rephrase the sentence to correct this statement.Line 61: "H2SO4 are the key precursors": Sulfuric acid is one of the key precursors but not the only one as stated here. Other examples are iodic acid (He et al., 2021, Sipilä et al., 2016) or highly oxygenated organic molecules (Kirkby et al., 2016).Line 70-71: please cite original publications describing the NAIS rather than publications including the instrumentation only in the methods section (Mirme & Mirme, 2013)Line 71: same as above, include citations which actually describe the instrument when introducing them (Jokinen et al., 2012)Line 143: see above, please include original description of the PSM as citation (Vanhanen et al., 2011)Line 153: Typo in the name of the instrument: Thermo Fisher AnalysersFigure 2: I would suggest to change the y-axis limit and label of the PNSD (panel d) to 10 nm as stated in the text and figure captionFigure 3: the y-label should show that it is a H2SO4 proxy concentrationLine 255-257: Please rephrase the sentence, the meaning is unclear.Line 267: "clearly proved" (correct would be: clearly proven) sounds too certain. I would be more cautious with the statement and suggest something like "is indicated by"Line 268: I suggest to add the information here, that it is an SA proxy concentrationLine 267-269: I suggest to add the SA proxy concentration in Fig. 2 so that the reader can see the daily variation, and to support the mean SA concentration mentioned here at GC measurement site.Line 269-270: please add a citation for the Hyytiälä, Shanghai and Nanjing SA concentrationLine 287 -288: add citations for the GR at Hyytiälä, Jungfraujoch, Beijing and PingyuanLine 325-329: What is the meaning of this sentence? Was the I-APi-TOF deployed at GC measurement site? It was not mentioned in the methods, only a ACSM. Please clarify.Line 349: here you mention the concentration of VOCs. In the method section I could not find any information regarding VOC measurements. Please clarify.Line 367-370: The sentence is very confusing, please rephrase.Line 375: Add citation for SO2 at BeijingLine 376-377: add citation for SO2 at HyytiäläLine 377-379: This statement is quite daring, as it might also be that other precursors were simply not abundant to initiate NPF. As previously mentioned (line 370), the NPF mechanism at the measurement site is probably a mixture of several precursors.Line 385-387: Please add a citation for this statementLine 387-390: It is not clear to me, how this is differnt. It was stated that the H2SO4 concentration is mainly depending on the solar radiation, thus the concentration of H2SO4 as precursor is determining (among probably other precursors) whether there is NPF or not. Now it is stated that this is different from other countries where the "intensity" (I assume this means concentration) determines the NPF occurence. Please clarify.Figure 6: Is the diurnal variation calculated for all NPF and non-NPF days? I suggest to mention how many days are included in the mean calculation to be more transparent with the overview and how much one can interpret from these figures.Line 409-410: A brief comment: Generally lower temperatures favour nucleation, also citations from the previously mentioned CLOUD experiments regarding RH and temperature could be included here.Line 419: I would add to the sentence "that involve, among others, O3 oxidation", as also OH, NO3 are oxidants involved in forming HOM.Line 420: When referring to "these oxygenated organic compounds", they should be elaborated on more thoroughly and a citation should be included.Language remarks:
Line 41 "... might be a regional phenomena" phenomenonLine 58 "CCNs" CCNLine 172: "being mainly for PSM data": a word is missing hereLine 185: "fresh formed" freshly formedLine 239: "dramatic" rather use something like "rapid"Line 254: "formation rate [...] was based" should be plural: rates [...] were basedLine 265: "could be the more abundance" the higher abundanceLine 312: "during a much longer time" for a longer period of timeLine 315: "might be a regional phenomena" phenomenonLine 319: "our results deviates" deviateLine 333: "on the other side" on the other handLine 335: "dominating one varies" varryingLine 381: "Taking both" a word is missingLine 384: remove "reaching to the Earth"Line 390: I believe the citation should be Kulmala, the mistake repeats in the reference listLine 419: "that involving O3 oxidation" that involve O3Line 439: "high formation rate" ratesLine 448-449: this sentence lacks a word or punctuation markSupplementary material:
Figure S1: The figure caption states that the left panel is showing formation rate as a function of SA concentration, however the label shows SA*DIACIDS and the concentration is given in 10^17 - 10^18 range. It is not clear what is meant here, is it a multiplication product or clusters, and how is this concentration retrieved? It seems extremely high.Figure S2: "square dots" should be denoted as squares, otherwise it is contradictoryCitation: https://doi.org/10.5194/acp-2022-784-RC1 -
AC1: 'Reply on RC1', Juan Hong, 12 Apr 2023
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2022-784/acp-2022-784-AC1-supplement.pdf
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RC2: 'Comment on acp-2022-784', Anonymous Referee #2, 26 Mar 2023
Hong et al. presents a measurement report on wintertime new particle formation (NPF) in the rural area of North China Plain, exploring its influencing factors and possible formation mechanism. While NPF in urban cities of China are relatively well investigated, measurements in the rural areas are rather not enough to understand its underlying mechanisms. This manuscript is of great interest to readers of general aerosol formation, particularly in the NPF research. However, the following issues/concerns need to be addressed before it can be accepted for publication in the journal.
- The sulfuric acid (SA) concentration in this study was calculated according to proxy proposed by Petaja et al. (2009). However, Lu et al. (2019) proposed a better proxy for estimating SA concentration in urban Beijing. It would be beneficial to compare both proxies for their performance since Petaja et al.’s proxy is based on measurements in boreal environments while Lu et al’s one might be more applicable to the current study.
- This study measured only particle number size distribution and no potential nucleating precursors (e.g., sulfuric acid, amines, carboxylic acids) were measured. A SA-DMA mechanism was proposed based on the similarity of correlations of the particle formation rate with sulfuric acid concentration for this study and for the Cloud studies. It seems that proposing such a mechanism based solely on this similarity does not make any sense, providing no any measured DMA concentration in this area. In addition, how can the authors ensure the base is DMA rather than any other amines?
- The exclusion of SA-acid mechanism was based on Figure S1 which show a bad correlation between J and SA*diacids. However, the rationale needs to be validated since concentrations of both SA and diacids varied in the correlation plot, leading to violation of thermodynamic roles. This approach is not convincing.
- The authors conclude that the controlling factor for NPF is the condensational sink which is based on qualitative comparison of CS characteristics between the measurement site and urban Beijing. However, some quantitative representations are needed to make sure the CS indeed is the most important factor for determining the occurrence of NPF at the site.
- Below are rather minor:
- There are lots of typos, ill-sentences through the manuscript which need to be corrected.
- L39, at an urban site
- L61 and throughout the text, H2SO4 needs subscript for 2 and 4. There are lots of such typos in the text for H2SO4 and other molecular formula
- L61, sulfuric acid molecules, follow a plural form
- L67, newly form
- L73-74, I don’t think the chemical composition of 1-3 nm particles has been speciated thus far.
- L80, important contributors to atmospheric nucleation
- L84, formation
- L137-138, I think 3080 include DMA inside
- L188&198, where, ???
- L203, particles in new mode? What does this mean?
- L207, discussion
- L208, section 3.1.
- L215, at the current site
- L222 & others, lower than, not “compared to”
- L226, what are they referred to?
- L253&others, “Note that” is simple than “It has to be noted that”
- L256-257, it is hard to understand this sentence
- L262, formation rates vs those
- L266, in those polluted atmospheres
- L288-289, that clause is ambiguous here
Reference
Lu, Y., Yan, C., Fu, Y., Chen, Y., Liu, Y., Yang, G., et al. (2019). A proxy for atmospheric daytime gaseous sulfuric acid concentration in urban Beijing. Atmospheric Chemistry and Physics, 19(3), 1971–1983. https://doi.org/10.5194/acp-19-1971-2019
Citation: https://doi.org/10.5194/acp-2022-784-RC2 -
AC2: 'Reply on RC2', Juan Hong, 12 Apr 2023
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2022-784/acp-2022-784-AC2-supplement.pdf