Laboratory and field studies of ice-nucleating particles from open-lot livestock facilities in Texas

Hiranuma, Naruki; Auvermann, Brent W.; Belosi, Franco; Bush, Jack; Cory, Kimberly M.; Georgakopoulos, Dimitrios G.; Höhler, Kristina; Hou, Yidi; Lacher, Larissa; Saathoff, Harald; Santachiara, Gianni; Shen, Xiaoli; Steinke, Isabelle; Ullrich, Romy; Umo, Nsikanabasi S.; Vepuri, Hemanth S. K.; Vogel, Franziska; Möhler, Ottmar

doi:https://doi.org/10.5194/acp-21-14215-2021

Articles | Volume 21, issue 18

https://doi.org/10.5194/acp-21-14215-2021

© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.

https://doi.org/10.5194/acp-21-14215-2021

© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.

Articles | Volume 21, issue 18

Research article

|

24 Sep 2021

Research article |

| 24 Sep 2021

Laboratory and field studies of ice-nucleating particles from open-lot livestock facilities in Texas

Naruki Hiranuma, Brent W. Auvermann, Franco Belosi, Jack Bush, Kimberly M. Cory, Dimitrios G. Georgakopoulos, Kristina Höhler, Yidi Hou, Larissa Lacher, Harald Saathoff, Gianni Santachiara, Xiaoli Shen, Isabelle Steinke, Romy Ullrich, Nsikanabasi S. Umo, Hemanth S. K. Vepuri, Franziska Vogel, and Ottmar Möhler

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Final revised paper (published on 24 Sep 2021)
Supplement to the final revised paper
Preprint (discussion started on 20 Nov 2020)
Supplement to the preprint

Interactive discussion

Status: closed

AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment

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RC1: 'Comments on acp-2020-1042', Anonymous Referee #1, 24 Jan 2021
- AC2: 'Reply on RC1', Naruki Hiranuma, 22 Apr 2021
RC2: 'Review of ‘Feedlot is a unique and constant source of atmospheric ice-nucleating particles’ by Naruki et al.', Anonymous Referee #2, 25 Jan 2021
- AC3: 'Reply on RC2', Naruki Hiranuma, 22 Apr 2021

Peer-review completion

AR: Author's response | RR: Referee report | ED: Editor decision

AR by Naruki Hiranuma on behalf of the Authors (22 Apr 2021) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (22 Apr 2021) by James Allan

RR by Anonymous Referee #3 (23 May 2021)

Suggestions for revision or reasons for rejection

Review of “Ice-nucleating particles from open-lot livestock facilities in Texas” by Hiranuma et al.

General comment:

This is a valuable contribution to the ice nucleation community and it has a good level of novelty. This is the first time that I reviewed this manuscript and given that this was the second round of revisions I was expecting to see a more readable, clean, and concise document. Although the incorporated changes improved the manuscript, it cannot be accepted in its current verison. I invite the authors to take into account the comment by original reviewer #2 “I do not wish to spend a great deal of time going from line to line trying to edit the manuscript for them”.

Major Comments:
The authors wanted to cover too much: i) field (annual trends, seasonal trends, downwind vs, upwind); ii) field vs. lab; iii) lab (heat vs. no heat, super micron vs. sub micron, bulk vs. filter, ); iv) intercomparison between 4 different instruments; and v) a parametrization. Although it is not bad at all to be ambitious and to report several measurements/observations, the authors need to combine the large amount of data into something that is easy to read and to follow.
Given that the samples were found to be heat insensitive, the IN properties are likely coming from the mineral components. Why the mineralogical composition is not reported. In lines 110-112 it is stated “However, our knowledge regarding what particular features of OLLF dust trigger immersion freezing at heterogeneous freezing temperatures (Ts; i.e., size vs. composition) is still lacking”. The authors focused on the size of the particles but in terms of composition the minerals are completely ignored.
This is the second round of revisions and the manuscript still needs to be edited to improve its readability and the language. I was expecting to see a cleaner version.
Lines 367-368 it is mentioned that “These results imply the following: (1) ambient meteorological conditions, as summarized in Table 1, might not be determining factors for nINP for our study sites”. This refers to RH, T and P but not to wind speed, one of the most important meteorological variables to resuspend dust particles. Why is wind speed and wind direction not reported?
Lines 417-418 and Line 524: “For each sample, the spectra nearly overlap each other at T ~ -25 °C, verifying their comparability and complementing features.” and “Upon confirmation of the comparability between field and lab ns,geo values”. Why is this overlap only true at -25C and not at other temperatures? obtaining similar results at this temperature is enough to conclude that the systems are really comparable. Is it not the overlap at -25C suspicious? Why should they be comparable? In the field, aerosol particles are naturally aerosolized and this resuspension from the ground can favor specific aerosol sizes. On the other hand, the aerosolization in the laboratory is mechanical and the particles sizes, and hence, their composition may significantly differ from those found in natural environments.
Lines 438-441: The authors need to show that the composition and particle size distribution of ambient and Laboratory particles are comparable.

Minor Comments:
The Abstract is extremely long. The authors need to shorten it focusing on the main results only.
Similar to the Abstract, several parts in the Results section (and along the manuscript) are repetitive, longer than needed and not very concrete. The manuscript needs to be further edited to improve its readability.
Avoid self citations. From my personal point of view this is excessive.
Move sections 3.3 and 3.4 to SI as they contribute little to the main text.
The use of “T” and “Ts” instead of “temperature” and “temperatures” add too much noise to the manuscript.
Lines 66-67: “(i.e., the freezing propensity of INP immersed in supercooled water)”. Who freezes the INP or the droplet?
Lines 95-96: How about convection?
Line 99: “where a convective cloud and updraft system persists”. What does it mean? that you have such a system 365 days per year?
Lines 115-118: This is not the right place. Please add this text earlier.
Section 2.2. This Section is not easy to follow. It is longer than needed and it has to be rewritten to be more concise and clear.
Lines 154-155: Add the depth and how were they collected?
Line 186: How about wind speed?
Line 345: “Even assuming we evaluate INP up to 2,000 L-1, our INP fraction is 1%. Thus, our ns parameterization is reasonable.” I don’t get the message here.
Line2 354, 374 and 375: “cumulative mass”, “cumulative PM mass”, and “aerosol particle mass”. What does it mean? In methods two different systems to measure PM10 were described. Do the authors refer to PM10?
Lines 363-364: “However, because the measured nINP is low at high T, the CI95% error of nINP,upwind at around -15 °C is relatively large as compared to that at a lower T (Fig. 3a)”. I do not get it.
Line 366: “on local meteorological conditions”. What was the typical wind speed?
Line 367: “short episode of soil dust”. What do the authors mean? Resuspended dust?
Lines 388.389: “This motivates the need for further characterization of our OLLF samples in a controlled-lab setting in order to identify what particulate size population (i.e., supermicron vs. submicron) and other properties trigger their”. This cannot be evaluated in the field? should not just simply change the cut-off of the filter sampling PM1.0 vs. PM10?
Lines 399-410: This belongs to methods. Most of this information is already known from previous experiments in the AIDA, and therefore, their contribution to the manuscript is little and should not be in this section.
Lines 420-421: “the INSEKT results suggest that the bulk TXD01 sample is more active than filter-collected samples”. Is this not expected as the bulk likely contain larger particles?
Lines 424-425: “the lab-derived immersion spectra of both surface materials are reasonably comparable to the minimum – maximum boundaries of our field ns,geo spectra for T > -25 °C”. If it is the same samples analyzed by different setups why should they show the large variability observed on the field samples?
Lines 424-426: WWhile the variability of ns,geo at a single T could vary several orders of magnitude, similar variations are found for both lab and field results, implying the similarity of freezing efficiencies of our lab and field samples”. This is expected for field samples as they are not identical and may have different composition, but in the laboratory, the instruments collected exactly the same samples.
Lines 427-430: “there is a difference in the INP abundance between bulk (< 75 μm-sieved) and aerosolized/filtered-samples for TXD01 (⪅ 6.5 μm; Table 3) presumably due to different properties in particles of these two size subsets (6.5 – 75 μm and ⪅ 6.5 μm) and/or different amount of IN-active soil organic matter”. Again, is this not expected?
Line 431: “be more representative of atmospherically relevant dust”. Based on what? This needs to be clearly discussed.
Line 433: “This comparability suggests that freezing ability is similar for condensation and immersion for our surface samples”. I am not sure if such a strong conclusion can be said from just 2 data points from the DFPC.
Line 569: “Our lab and field measurements-based parameterizations”. It is not clear how the laboratory results were incorporated or used into the parametrizations. As stated in Major point #5 Lab and Field data should not be combined.
Lines 643-544: “Additionally, the observed consistency in the spectral slopes (i.e., Table 5) suggests that lab and field measurements exhibit similar IN ability at examined Ts”. This was true at -25C not for the whole temperature range.
Figure 5: In x-axis is it micro or milligrams? In Table 1 it is reported in micrograms
Figure 7: it does not make sense to have a, b,c,d on each panel. The description of panels d are unclear. What is the concentration reported in red and blue?
Figure 9: Why is it that noise? What is the time resolution? Would it not be better to do at a lower time resolution to avoid the noise?

Technical comments:

Lines 28: what is the meaning of “3 × 10-7 g L-1” .
Lines 48-51: Delete them.
Line 54: delete “chapter 9”.
Line 56: Add other references in addition to Storelvmo (2017)
Line 78: “Agricultural land use is in excess of 50% of total U.S. land use”. Please rewrite it.
Line 87: Add references after “conditions”.
Line 90: Add references after “head”.
Line 101: “we examinedthe”. Fix it.
Line 106: Add references after “materials”.
Line 125: Add references after “definition”.
Line 161: “using an offline freezing technique”. Which one?
Line 171: “those of previously measured”. Fix it.
Line 184: Remove “Fig 5.”
Lines 196-198: “proxies. We chose the AIDA chamber as our study platform because it simulates ice formation in mixed-phase clouds in a controlled setting with respect to both T (± 0.3 °C) and humidity (± 5%; Fahey et al. 2014).” Delete.
Lines 201-203: “experiment. The AIDA has been applied for the analysis of both ambient and lab-generated INPs and has facilitated characterization of many INP species with the IN efficiency uncertainty of ± 39% (Steinke et al., 2020; Ullrich et al., 2017; Niemand et al., 2012; Hoose and Möhler, 2012).” Delete.
Lines 223-225: “Another motivation for using the AIDA facility is its ice-selecting pumped counterflow virtual impactor (IS-PCVI; Hiranuma et al., 2016). As detailed in Supplemental Information (SI) Sect. S1, IS-PCVI separates ICRs from interstitial particles, including cloud droplets, at Ts below -20 °C.” Delete.
Line 225: “evaporation”. Should it be sublimation?
Line 300: “Texas dust”. Delete.
Line 310: “Next, our metagenomics analysis method of total DNA is described”. Delete.
Line 386: “at below -20 °C”. Fix it.
Lines 386-387: “ambient aerosol particle mass concentrations based”. PM10?
Line 389: “in a controlled lab setting”. Delete.
Line 412: “O14, S16, S20”. Add the origin/source of the samples.
Line 472: Add references after “mass”.
Lines 486-487: “properties. All of our single particle analyses were carried out with the following parameters: electron beam accelerating voltages of 15 keV, spot size of 50, and working distance of 10 mm”. This belongs to Methods.
Line 525: “We elected to use the”. Fix it.
Line 529: “typically substantially lower”. Fix it.
Line 580: “atmospherically relevant”. What do the authors mean?
Line 593: “dust samplew”. Fix it.
Table 6. Last column “Spermicron Size”. Fix it.

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RR by Anonymous Referee #4 (24 May 2021)

Suggestions for revision or reasons for rejection

The reviewed manuscript presents IN measurements and particle characteristics from particles emitted from select feedlot sites in the Texas Panhandle. The field measurements are complemented by laboratory measurements and the study benefits from the various analyzed particle characteristics. However, I would strongly suggest the authors to further revise the manuscript for conciseness and thus increasing readability and clarity of most sections, but particularly the methods and results sections.

Some additional comments for the authors:
- Line 214/215: What is the scientific motivation of point (2)?
- Line 218/219: INSEKT covers a different size range than AIDA? If this is the main point for using INSEKT then the authors should mention this here to make it more clear why certain methods are used alongside others. I would recommend to generally revise the methods section for conciseness and thus clarity with a focus on providing the reader with a clear overview of how methods complement each other.
- Method on DNA analysis: does sterilization remove DNA which might interfere with the DNA of interest here?
- Please ensure that acronyms are defined the first time they appear in the manuscript, this will help the reader to better follow along without having to search for definitions. E.g., definition of ICR in line 226 missing.
- Figure 1: OLLF schematic is helpful but not very clear. Would suggest to adapt the shape and relative size of the study areas. Additionally, it is not clear from the map where the boundary between OLLF 2 and 3 is.
- Comment 6. Ln 48 from reviewer 2, would suggest to also clarify in the manuscript
- SI, particularly Figure S3: increase font size and/or image resolution for legibility.
- SI, Table S3: check for significant figures of the values provided in the table and be consistent.

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ED: Reconsider after major revisions (24 May 2021) by James Allan

AR by Naruki Hiranuma on behalf of the Authors (29 Jul 2021) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (02 Aug 2021) by James Allan

RR by Anonymous Referee #4 (14 Aug 2021)

RR by Anonymous Referee #3 (19 Aug 2021)

ED: Publish subject to technical corrections (19 Aug 2021) by James Allan

AR by Naruki Hiranuma on behalf of the Authors (27 Aug 2021) Author's response Manuscript

Post-review adjustments

AA: Author's adjustment | EA: Editor approval

AA by Naruki Hiranuma on behalf of the Authors (22 Sep 2021) Author's adjustment Manuscript

EA: Adjustments approved (22 Sep 2021) by James Allan

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Short summary

We present laboratory and field studies showing that an open-lot livestock facility is a substantial source of atmospheric ice-nucleating particles (INPs). The ambient concentration of INPs from livestock facilities in Texas is very high. It is up to several thousand INPs per liter below –20 °C and may impact regional aerosol–cloud interactions. About 50% of feedlot INPs were supermicron in diameter. No notable amount of known ice-nucleating microorganisms was found in our feedlot samples.