Measurement report: Hygroscopicity of Size-Selective Aerosol&nbsp;Particles at Heavily Polluted Urban Atmosphere of Delhi:&nbsp;Impacts of Chloride Aerosol&nbsp;

Mandariya, Anil Kumar; Ahlawat, Ajit; Haneef, Mohamad M. V.; Baig, Nisar A.; Patel, Kanan; Apte, Joshua S.; Hildebrandt Ruiz, Lea; Wiedensohler, Alfred; Habib, Gazala

doi:https://doi.org/10.5194/egusphere-2023-577

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https://doi.org/10.5194/egusphere-2023-577

Preprints

07 Jul 2023

| 07 Jul 2023

Measurement report: Hygroscopicity of Size-Selective Aerosol Particles at Heavily Polluted Urban Atmosphere of Delhi: Impacts of Chloride Aerosol

Anil Kumar Mandariya, Ajit Ahlawat, Mohamad M. V. Haneef, Nisar A. Baig, Kanan Patel, Joshua S. Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib

Abstract. Recent studies reveal that wintertime chloride emission in the Delhi region is crucial in governing enhancement to theoretically calculated aerosol hygroscopicity and aerosol-bound liquid water to trigger Delhi's fog episodes. Here, we reported that the high volume fractional contribution of ammonium chloride into aerosol governs the high aerosol hygroscopicity and associated liquid water content based on the experimental data first time in Delhi. The episodically high chlorides bonded with excess ammonia present in Delhi's atmosphere, which could lead to haze and fog formation under high relative humidity in the region. Therefore, our study suggests that controlling the plastic-contained waste, open burning, and e-waste industrial chloride emission could significantly minimize Delhi’s heavily polluted haze/fog events. The high chloride (H-Cl) period was observed significantly (p<0.05) higher hygroscopicity (0.35 ± 0.06) compared to high biomass burning (H-BB) (0.18 ± 0.04), high hydrocarbon-like organic aerosol (H-HOA) (0.17 ± 0.05), and relatively cleaner period (0.27 ± 0.07).

In this study, we present the measurement results of bulk aerosol composition of non-refractory PM1 from ACSM and size-resolved (Nucleation, Aitken, and Accumulated mode particles) hygroscopic growth factor and associated hygroscopicity parameter at 90 % relative humidity (RH) measured using H-TDMA at Delhi Aerosol Supersite (DAS) first time. The hygroscopic parameter (κ_{H-TDMA_ 90%}) was significantly (p<0.05) enhanced with the size of the particles. The observed κ_{H-TDMA_90%} ranged from .00 to 0.11 (0.03 ± 0.02), 0.05 to 0.22 (0.11 ± 0.03), 0.05 to 0.30 (0.14 ± 0.04), 0.05 to 0.41 (0.18 ± 0.06), and 0.05 to 0.56 (0.22 ± 0.07) for 20, 50, 100, 150, and 200 nm aerosol particles, respectively. The Inorganic-to-organic aerosol ratio in aerosol modulated mainly the aerosol hygroscopicity. In addition, the accumulation mode particle's hygroscopicity was regulated potentially by the volume fraction of NH₄Cl and OA in aerosol particles. Interestingly, our results reveal that the daytime flattening pattern of accumulation aerosol particles in diurnal variation is potentially due to counter the effect of increment of (NH₄)₂SO₄ and NH₄NO₃ and decrement of NH₄Cl and OA in aerosol particles.

Received: 26 Mar 2023 – Discussion started: 07 Jul 2023

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22 Mar 2024

Measurement report: Hygroscopicity of size-selected aerosol particles in the heavily polluted urban atmosphere of Delhi: impacts of chloride aerosol

Anil Kumar Mandariya, Ajit Ahlawat, Mohammed Haneef, Nisar Ali Baig, Kanan Patel, Joshua Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib

Atmos. Chem. Phys., 24, 3627–3647, https://doi.org/10.5194/acp-24-3627-2024,https://doi.org/10.5194/acp-24-3627-2024, 2024

Short summary

Anil Kumar Mandariya, Ajit Ahlawat, Mohamad M. V. Haneef, Nisar A. Baig, Kanan Patel, Joshua S. Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2023-577', Anonymous Referee #2, 24 Jul 2023

The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-577/egusphere-2023-577-RC1-supplement.pdf

Citation: https://doi.org/10.5194/egusphere-2023-577-RC1
- AC2: 'Reply on RC1', Gazala Habib, 24 Oct 2023
  
  The authors thank the reviewer for constructive comments. Your suggestion seems very legitimate. As suggested, this comment has been addressed in the revised manuscript. Please see the attached file for the response to referee 1 for the detailed replies against the comments.
  
  Citation: https://doi.org/10.5194/egusphere-2023-577-AC2
RC2:
'Comment on egusphere-2023-577', Anonymous Referee #3, 24 Jul 2023
The manuscript ” Measurement report: Hygroscopicity of Size-Selective Aerosol Particles at Heavily Polluted Urban Atmosphere of Delhi: Impacts of Chloride Aerosol” revealed the wintertime chloride emission in the Delhi region governing the enhancement of aerosol hygroscopicity and aerosol-bound liquid water that trigger Delhi's fog episodes. The manuscript is written well and within the interest of the scientific communities. However, there are many gaps in the quality of presentation and lack of clarity in the manuscript.
Major Comments
The author did not present the schematic of the experimental design. Therefore, it is difficult to understand the different instruments used in the study.

There is a lack of clarity on the classification of different events e.g., H-BB, H-HOA, H-Cl and clean. For example, how was the event classification made based on the aerosol chemical compositions? There is missing information about these events in figure 1 caption. It is recommended that the author should add a table to the text to discuss the event classification explicitly.

The mathematical equations used in the text should be cross verified.

Minor comments
Page 1 and Line 27: Expand HTDMA
Page 1 and Line 33: Expand OA
Page 3 and Line 67: Expand IGP
Page 5 and Line 137: This is a repeated sentence.
Page 6 and Line 159: The equation is not correct.
Page 6 and Line 169: It is not clear the modified ion pairing scheme: what is the difference between SA and AS
Page 8 and Line 195: The author should discuss the source of the gas and meteorological data. At what height the met parameters were measured?
Page 8 and Line 196: The author talked about PNSD. It is not clear how they measured it? Is it from the HTDMA or additionally a size spectrometer was used. A detailed schematic experimental design is needed.
Page 8 and Line 205-207: Reference is missing.
Page 8 and Line 213: It is not clear how the intensity of biomass burning activities was determined.
Page 9 and Line 220: Author should explain the nighttime peak of SO2.
Page 9 and Line 235: It is not clear about MPSS. Is it a separate instrument associated with the experimental design? If so, why was the MPSS data not presented in this study?
Page 9 and Line 240: … average mass concentration 46.5 ±39.6 ug/m3 consistent with 112 ug/m3…. This is not clear.
Page 12: The y- axis of diel Cl plot is not clear.
Page 17 and Line No.398: Author should explain why two linear regressions are drawn in the correlation plot (example Fig. 5a).
Page 18 and Line No.418: Author should provide the ALWC vs mass fraction of AN and AS in the supplement.
Page 19 and Line No 434. The author should clearly mention the dates they consider for a relatively clean period.
Page 22 and Line No 505-507. Is it 39% of BBOA by mass? Figure 8 is not clear. The color coding should be clarified in the plot.
Page 22 and Line No 505-507. The dates and times of the event should be clarified in the figure 1 caption.
Page 23 and Line 535: The x-axis label is missing.
Page 25 and Line 583: However,…time in India…This statement is not true.

Supplements
Page 2 and Line 23: Author should present the time series data of MPSS during the study period.
Page 7 and Line 80: I don’t see any difference in the probability distributions of BBOA, HOA and ACL. The Author should clarify it.
Citation: https://doi.org/10.5194/egusphere-2023-577-RC2
- AC1: 'Reply on RC2', Gazala Habib, 23 Oct 2023
  
  The authors thank the reviewer for constructive comments. Your suggestion seems very legitimate. As suggested, this comment has been addressed in the revised manuscript. Please see the attached file for the response to referee 2 for the detailed replies against the comments.
  
  Citation: https://doi.org/10.5194/egusphere-2023-577-AC1

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2023-577', Anonymous Referee #2, 24 Jul 2023

The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2023/egusphere-2023-577/egusphere-2023-577-RC1-supplement.pdf

Citation: https://doi.org/10.5194/egusphere-2023-577-RC1
- AC2: 'Reply on RC1', Gazala Habib, 24 Oct 2023
  
  The authors thank the reviewer for constructive comments. Your suggestion seems very legitimate. As suggested, this comment has been addressed in the revised manuscript. Please see the attached file for the response to referee 1 for the detailed replies against the comments.
  
  Citation: https://doi.org/10.5194/egusphere-2023-577-AC2
RC2:
'Comment on egusphere-2023-577', Anonymous Referee #3, 24 Jul 2023
The manuscript ” Measurement report: Hygroscopicity of Size-Selective Aerosol Particles at Heavily Polluted Urban Atmosphere of Delhi: Impacts of Chloride Aerosol” revealed the wintertime chloride emission in the Delhi region governing the enhancement of aerosol hygroscopicity and aerosol-bound liquid water that trigger Delhi's fog episodes. The manuscript is written well and within the interest of the scientific communities. However, there are many gaps in the quality of presentation and lack of clarity in the manuscript.
Major Comments
The author did not present the schematic of the experimental design. Therefore, it is difficult to understand the different instruments used in the study.

There is a lack of clarity on the classification of different events e.g., H-BB, H-HOA, H-Cl and clean. For example, how was the event classification made based on the aerosol chemical compositions? There is missing information about these events in figure 1 caption. It is recommended that the author should add a table to the text to discuss the event classification explicitly.

The mathematical equations used in the text should be cross verified.

Minor comments
Page 1 and Line 27: Expand HTDMA
Page 1 and Line 33: Expand OA
Page 3 and Line 67: Expand IGP
Page 5 and Line 137: This is a repeated sentence.
Page 6 and Line 159: The equation is not correct.
Page 6 and Line 169: It is not clear the modified ion pairing scheme: what is the difference between SA and AS
Page 8 and Line 195: The author should discuss the source of the gas and meteorological data. At what height the met parameters were measured?
Page 8 and Line 196: The author talked about PNSD. It is not clear how they measured it? Is it from the HTDMA or additionally a size spectrometer was used. A detailed schematic experimental design is needed.
Page 8 and Line 205-207: Reference is missing.
Page 8 and Line 213: It is not clear how the intensity of biomass burning activities was determined.
Page 9 and Line 220: Author should explain the nighttime peak of SO2.
Page 9 and Line 235: It is not clear about MPSS. Is it a separate instrument associated with the experimental design? If so, why was the MPSS data not presented in this study?
Page 9 and Line 240: … average mass concentration 46.5 ±39.6 ug/m3 consistent with 112 ug/m3…. This is not clear.
Page 12: The y- axis of diel Cl plot is not clear.
Page 17 and Line No.398: Author should explain why two linear regressions are drawn in the correlation plot (example Fig. 5a).
Page 18 and Line No.418: Author should provide the ALWC vs mass fraction of AN and AS in the supplement.
Page 19 and Line No 434. The author should clearly mention the dates they consider for a relatively clean period.
Page 22 and Line No 505-507. Is it 39% of BBOA by mass? Figure 8 is not clear. The color coding should be clarified in the plot.
Page 22 and Line No 505-507. The dates and times of the event should be clarified in the figure 1 caption.
Page 23 and Line 535: The x-axis label is missing.
Page 25 and Line 583: However,…time in India…This statement is not true.

Supplements
Page 2 and Line 23: Author should present the time series data of MPSS during the study period.
Page 7 and Line 80: I don’t see any difference in the probability distributions of BBOA, HOA and ACL. The Author should clarify it.
Citation: https://doi.org/10.5194/egusphere-2023-577-RC2
- AC1: 'Reply on RC2', Gazala Habib, 23 Oct 2023
  
  The authors thank the reviewer for constructive comments. Your suggestion seems very legitimate. As suggested, this comment has been addressed in the revised manuscript. Please see the attached file for the response to referee 2 for the detailed replies against the comments.
  
  Citation: https://doi.org/10.5194/egusphere-2023-577-AC1

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload

AR by Gazala Habib on behalf of the Authors (24 Oct 2023) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (03 Nov 2023) by Luis A. Ladino

RR by Anonymous Referee #3 (08 Nov 2023)

RR by Anonymous Referee #2 (16 Nov 2023)

ED: Publish subject to minor revisions (review by editor) (01 Dec 2023) by Luis A. Ladino

I would like to thank the authors for incorporating the suggestions made by both reviewers; however, there are some important key points that need to be properly addressed before I can accept the manuscript.

Reviewer #2:
1. Fig. 2 caption: I thought the pink boxes indicated the high-CL events. Please double check.
2. Fig. 3d: The wind direction should be averaged arithmetically. Vector averaging should be used to do so. Check the following link for instructions: https://math.stackexchange.com/questions/44621/calculate-average-wind-direction
3. No x-axis label for Fig. 8 in the revised manuscript.

Reviewer #3:
There is a technical error still in the revised version and need to be fixed before publication. The figure 3 (o) left axis is not well adjusted.

Editor:
1. The readability and the grammar of the manuscript need to be deeply improved. It is highly recommended that the manuscript is reviewed by a native English speaker.
2. In the abstract several terms are defined; however, they are only used once. Please only use an abbreviation when a specific term is going to be used several times. For example, there is no need to use the following abbreviations in the abstract: ACSM, DAS, H-TDMA, CCN, and OA.
3. On the other hand, the authors define the same term several times along the manuscript. It is recommended that a term is defined the first time it is used and later on only the abbreviation is used. For example, H-Cl should be defined in L15 and not in L26.
4. Figures S3 and S4 are not called in the main text.
5. Figures S5 and S6 cannot be called before Figures S2, S3, and S4.
L29-30: “Ammonium Chloride” should be “ammonium chloride”
L35: Add a reference after “budgets”
L39: “is crucial to predict the” should be “is crucial to better predict the”
L41: Delete “atmospheric conditions”
L56: It seems that “counter” is misplaced.
L58-61. Improve the grammar.
L62: “Delhi’s atmosphere to understand” should be “Delhi’s atmosphere to better understand”
L64-65: “to severe air quality”. Do the authors mean “to severely poor/low air quality”?
L70-71: Improve the grammar.
L79-80: “hygroscopicity. Hence, it is essential to measure size-resolved aerosol hygroscopicity in Delhi's atmosphere and investigate its role in the context of high chloride”. This is redundant, therefore, I suggest deleting it.
L83-84: H-TDMA was already defined.
L84: Add the model and manufacturer of the MPSS.
L87: “The lab-2 is situated at the height of 15 m a.g.l. and lab-2 is 50 m apart” should be “The lab-2 is situated at the height of 15 m a.g.l. and is 50 m apart”
L99: “for aerosol and sheath respectively” should be “for aerosol flow and sheath flow, respectively.”
L103: “Both the DMAs were”. Fix it.
L110: MPSS was already defined.
L111: “A Detailed description” should be “A detailed description”
L111: “ACSM was” should be “The ACSM was”
L113: “ratio (m/z) m/z 10 to m/z 140” should be “ratio (m/z) 10 to m/z 140.”
Lines 111-118 need to be combined with Lines 165-175 in one single section.
L167: “Patel et al., 2021.” Fix it.
L220-223: RH, T, WD, WS, PNSD, and OA were already defined.
L226. RH and T were already defined.
L243: WS was already defined.
From here on, I stopped checking the grammar, spelling, and punctuation. Please check out the rest of the manuscript.

Hide

AR by Gazala Habib on behalf of the Authors (13 Dec 2023) Author's response Author's tracked changes Manuscript

ED: Publish subject to technical corrections (18 Jan 2024) by Luis A. Ladino

AR by Gazala Habib on behalf of the Authors (18 Jan 2024) Author's response Manuscript

Journal article(s) based on this preprint

22 Mar 2024

Measurement report: Hygroscopicity of size-selected aerosol particles in the heavily polluted urban atmosphere of Delhi: impacts of chloride aerosol

Anil Kumar Mandariya, Ajit Ahlawat, Mohammed Haneef, Nisar Ali Baig, Kanan Patel, Joshua Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib

Atmos. Chem. Phys., 24, 3627–3647, https://doi.org/10.5194/acp-24-3627-2024,https://doi.org/10.5194/acp-24-3627-2024, 2024

Short summary

Anil Kumar Mandariya, Ajit Ahlawat, Mohamad M. V. Haneef, Nisar A. Baig, Kanan Patel, Joshua S. Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib

Supplement

https://doi.org/10.5194/egusphere-2023-577-supplement

Data sets

Measurement report: Hygroscopicity of Size-Selective Aerosol Particles at Heavily Polluted Urban Atmosphere of Delhi: Impacts of Chloride Aerosol Anil Kumar Mandariya, Ajit Ahlawat, Mohamad M. V. Haneef, Nisar A. Baig, Kanan Patel, Joshua S. Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib https://web.iitd.ac.in/~gazala/publications.html

Anil Kumar Mandariya, Ajit Ahlawat, Mohamad M. V. Haneef, Nisar A. Baig, Kanan Patel, Joshua S. Apte, Lea Hildebrandt Ruiz, Alfred Wiedensohler, and Gazala Habib

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Short summary

The current study explored the temporal variation of size-selective particle hygroscopicity in Delhi first time. Here, we reported that the high volume fractional contribution of ammonium chloride into aerosol governs the high aerosol hygroscopicity and associated liquid water content based on the experimental data first time in Delhi. The episodically high ammonium chlorides present in Delhi's atmosphere could lead to haze and fog formation under high relative humidity in the region.

Measurement report: Hygroscopicity of Size-Selective Aerosol Particles at Heavily Polluted Urban Atmosphere of Delhi: Impacts of Chloride Aerosol

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