Real-time detection of highly oxidized organosulfates and BSOA marker compounds during the F-BEACh 2014 field study

Brüggemann, Martin; Poulain, Laurent; Held, Andreas; Stelzer, Torsten; Zuth, Christoph; Richters, Stefanie; Mutzel, Anke; van Pinxteren, Dominik; Iinuma, Yoshiteru; Katkevica, Sarmite; Rabe, René; Herrmann, Hartmut; Hoffmann, Thorsten

doi:https://doi.org/10.5194/acp-17-1453-2017

Articles | Volume 17, issue 2

https://doi.org/10.5194/acp-17-1453-2017

© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

https://doi.org/10.5194/acp-17-1453-2017

© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Articles | Volume 17, issue 2

Research article

|

31 Jan 2017

Research article |

| 31 Jan 2017

Real-time detection of highly oxidized organosulfates and BSOA marker compounds during the F-BEACh 2014 field study

Martin Brüggemann, Laurent Poulain, Andreas Held, Torsten Stelzer, Christoph Zuth, Stefanie Richters, Anke Mutzel, Dominik van Pinxteren, Yoshiteru Iinuma, Sarmite Katkevica, René Rabe, Hartmut Herrmann, and Thorsten Hoffmann

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Final revised paper (published on 31 Jan 2017)
Supplement to the final revised paper
Preprint (discussion started on 28 Jul 2016)
Supplement to the preprint

Interactive discussion

Status: closed

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

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- Supplement

RC1: 'Review of Brüggemann et al.', Anonymous Referee #1, 05 Sep 2016
- AC1: 'Reply to Reviewer 1', Martin Brüggemann, 30 Nov 2016
RC2: 'Review of Brüggemann et al.', Anonymous Referee #2, 06 Sep 2016
- AC2: 'Reply to Reviewer 2', Martin Brüggemann, 30 Nov 2016
RC3: 'Real-time detection of highly oxidized organosulfates and BSOA marker compounds during the F–BEACh 2014 field study', Anonymous Referee #3, 07 Sep 2016
- AC3: 'Reply to Reviewer 3', Martin Brüggemann, 30 Nov 2016

Peer-review completion

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

AR by Martin Brüggemann on behalf of the Authors (30 Nov 2016) Author's response Manuscript

ED: Referee Nomination & Report Request started (04 Dec 2016) by Alexander Laskin

RR by Anonymous Referee #3 (16 Dec 2016)

RR by Anonymous Referee #2 (18 Dec 2016)

Suggestions for revision or reasons for rejection

It is a central part of the peer-review process that colleagues in the field spend time and efforts to comment on your work in order to improve the quality. In return, it is expected that the authors take the comments into account in order to actually improve the quality of the manuscript. Here the authors have addressed some of the issues that the reviewers brought forward, while other questions have not been discussed or answered.

In point 12 the authors must at least try to comment on the central question: Do organosulfates evaporate at 200C?
This is also related to the main question in point 21 below.

In point 14 the authors do not adequately answer my question about their extraction efficiency, but instead add a very general statement on this issue. They must at least discuss this point more thoroughly in their reply.

Point 20: Even though Hallquist et al. has written about organosulfates, it is not clear that the review shows that they are ubiquitous, due to the limited number of studies available back in 2009.

Point 21: The authors " believe that the signals for organosulfates are not affected by such processes in the ionization region". Why was this not investigated using commercially available standards in both the offline and online versions of the instrument? This would normally be a minimum requirement for a new measurement technique.

Point 23: I know the statistical background, but the problem (as brought up by reviewer 3 as well) is that the presentation confuses correlation and causation e.g. when the authors write: "supporting the hypothesis that these compounds reflect major sources of the organic aerosol mass at the site." Furthermore, it should be kept in mind that the explanation of variability is for either variable, i.e. AMS-OM also explains the Aero-FAPA-MS signal. When two distinguished reviewers bring this up, it should be a hint to the authors to write the statements more clearly.

Abstract: In the new version of the abstract the following sentences should be clarified according to the discussion (and to make them easier to read):
"Although volatile organic compound (VOC) measurements exhibited high mixing ratios for monoterpenes, such as α-/β-pinene, especially later-generation monoterpene oxidation products were observed in the particle phase. In particular, compared to concentrations for early-generation oxidation products, such as pinic acid, high concentrations were found for the photooxidation products 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA) and 3-carboxyheptanedioic acid, suggesting that aged aerosol masses were present during the campaign period".

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ED: Reconsider after minor revisions (Editor review) (20 Dec 2016) by Alexander Laskin

AR by Martin Brüggemann on behalf of the Authors (29 Dec 2016) Author's response Manuscript

ED: Publish as is (08 Jan 2017) by Alexander Laskin

AR by Martin Brüggemann on behalf of the Authors (12 Jan 2017)

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Short summary

Using complementary mass spectrometric techniques during a field study in central Europe, characteristic contributors to the organic aerosol mass were identified. Besides common marker compounds for biogenic secondary organic aerosol, highly oxidized sulfur species were detected in the particle phase. High-time-resolution measurements revealed correlations between these organosulfates and particulate sulfate as well as gas-phase peroxyradicals, giving hints to underlying formation mechanisms.