Chemical composition of nanoparticles from α-pinene nucleation and the influence of isoprene and relative humidity at low temperature
- 1Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- 2Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- 3Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO, 80309-0215, USA
- 4Max Planck Institute for Chemistry, Mainz, 55128, Germany
- 5CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
- 6Leibniz Institute for Tropospheric Research, Leipzig, 04318, Germany
- 7Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein-Leopoldshafen, Germany
- 8Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- 9Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
- 10Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- 11Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
- 12Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
- 13California Air Resources Board, Sacramento, CA 95814, USA
- 14Lebedev Physical Institute, Russian Academy of Sciences, 119991, Moscow, Russia
- 15CERN, 1211 Geneva, Switzerland
- 16Dipartimento di Fisica, Università di Genova and INFN, 16146 Genova, Italy
- 17Department of Atmospheric and Oceanic Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
- 18Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- 19Ionicon Analytik GmbH, 6020 Innsbruck, Austria
- 20Forest Dynamics, Swiss Federal Institute for Forest, Snow and Landscape Research, 8903 Birmensdorf, Switzerland
- 21Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA
- 22Finnish Meteorological Institute, 00560 Helsinki, Finland
- 23Beijing Weather Modification Office, China
- 24IDL, Universidade da Beira Interior, R. Marquês de Ávila e Bolama, Covilhã, 6201-001, Portugal
- 25Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P.R. China
- 26Moscow Institute of Physics and Technology (National Research University), 117303, Moscow, Russia
- 1Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
- 2Institute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, 00014 Helsinki, Finland
- 3Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO, 80309-0215, USA
- 4Max Planck Institute for Chemistry, Mainz, 55128, Germany
- 5CENTRA and FCUL, University of Lisbon, 1749-016 Lisbon, Portugal
- 6Leibniz Institute for Tropospheric Research, Leipzig, 04318, Germany
- 7Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein-Leopoldshafen, Germany
- 8Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
- 9Helsinki Institute of Physics, University of Helsinki, 00014 Helsinki, Finland
- 10Faculty of Physics, University of Vienna, 1090 Vienna, Austria
- 11Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
- 12Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125, USA
- 13California Air Resources Board, Sacramento, CA 95814, USA
- 14Lebedev Physical Institute, Russian Academy of Sciences, 119991, Moscow, Russia
- 15CERN, 1211 Geneva, Switzerland
- 16Dipartimento di Fisica, Università di Genova and INFN, 16146 Genova, Italy
- 17Department of Atmospheric and Oceanic Sciences, University of Colorado Boulder, Boulder, CO 80309, USA
- 18Institute for Ion and Applied Physics, University of Innsbruck, 6020 Innsbruck, Austria
- 19Ionicon Analytik GmbH, 6020 Innsbruck, Austria
- 20Forest Dynamics, Swiss Federal Institute for Forest, Snow and Landscape Research, 8903 Birmensdorf, Switzerland
- 21Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA
- 22Finnish Meteorological Institute, 00560 Helsinki, Finland
- 23Beijing Weather Modification Office, China
- 24IDL, Universidade da Beira Interior, R. Marquês de Ávila e Bolama, Covilhã, 6201-001, Portugal
- 25Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P.R. China
- 26Moscow Institute of Physics and Technology (National Research University), 117303, Moscow, Russia
Abstract. New Particle Formation (NPF) from biogenic organic precursors is an important atmospheric process. One of the major species is α-pinene, which upon oxidation, can form a suite of products covering a wide range of volatilities. A fraction of the oxidation products is termed Highly Oxygenated Organic Molecules (HOM). These play a crucial role for nucleation and the formation of Secondary Organic Aerosol (SOA). However, measuring the composition of newly formed particles is challenging due to their very small mass. Here, we present results on the gas and particle phase chemical composition for a system where α-pinene was oxidized by ozone, and for a mixed system of α-pinene and isoprene, respectively. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber at temperatures between −50 °C and −30 °C and at low and high relative humidity (20 % and 60 to 100 % RH). These conditions were chosen to simulate pure biogenic new particle formation in the upper free troposphere. The particle chemical composition was analyzed by the Thermal Desorption-Differential Mobility Analyzer (TD-DMA) coupled to a nitrate chemical ionization time-of-flight mass spectrometer. This instrument can be used for particle and gas phase measurements using the same ionization and detection scheme. Our measurements revealed the presence of C8-10 monomers and C18-20 dimers as the major compounds in the particles (diameter up to ~ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5-7) and C15 compounds (C15H24O5-10) are detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene might enhance growth at particle sizes larger than 15 nm. Besides the chemical information regarding the HOM formation for the α-pinene (plus isoprene) system, we report on the nucleation rates measured at 1.7 nm and found that the lower J1.7nm values compared with previous studies are very likely due to the higher α-pinene and ozone mixing ratios used in the present study
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Journal article(s) based on this preprint
Lucía Caudillo et al.
Interactive discussion
Status: closed
-
RC1: 'Comment on acp-2021-512', Anonymous Referee #1, 28 Jul 2021
Caudillo and co-authors present and discuss the gas and particle phase composition of pure biogenic nucleation events measured with a nitrate chemical ionization atmospheric pressure interface time of flight mass spectrometer (coupled with a thermal desorption-differential mobility analyzer for the particle phase) in the CLOUD chamber at a range of conditions representing free tropospheric conditions. Specifically, alpha-pinene and a mix of alpha-pinene and isoprene were oxidized at -30 deg C and - 50 deg C, and at 20 % or 60 - 100 % relative humidity. The authors find C8-10 monomers and C18-20 dimers as major compounds, and C5 and C15 compounds contributing to particle growth when isoprene is present in the system. I very much appreciate the systematic analysis. The manuscript is well-written and the experimental results are thoroughly discussed. In my opinion, this is an original and valuable contribution to the field. Therefore, it should be published in ACP after minor revisions.
Specific comments:
In the abstract, the last sentence ("Besides the chemical information...", lines 64-66) was confusing to me. After reading section 3.4.1, I suggest to be more specific in the abstract, e.g. "Compared with previous studies, we found lower nucleation rates measured at 1.7 nm, very likely due to higher alpha-pinene and ozone mixing ratios used in the present study."In section 2.1, there is no information about GCR conditions during the experiments, please add.
In section 2.2, please add some more information about the heating procedure of the filament. Is the temperature slowly ramped up, or do you apply high temperature directly to instantaneously vaporize the sample? This is also relevant for the discussion of potential thermal decomposition of molecules in section 3.2.2.
Regarding the non-size selective mode of operation of the TD-DMA, it would be helpful to get an idea about the contribution of freshly nucleated particles vs. grown particles to the sampled mass. From the measured particle size distributions and the PSM and CPC total number concentrations, could you calculate a rough estimate of the volume/mass fraction of particles < 15 nm in the samples collected in the periods shown in Figure 1 as shaded areas? Please add this information to Table 1.
In Figure 3f, to me it is not obvious that specifically C4-5 and C13-16 compounds are enhanced as stated in lines 237/238. Please clarify.
In section 3.3, looking at Figures 5 and S4 I agree with the statement that mainly LVOC and ELVOC compounds were detected in the particle phase, however, the ULVOC compounds appear to be a minor fraction.
Section 3.4.2: Regarding the discussion of isoprene suppression of new particle formation, please consider adding a reference to Lee et al. (2016), doi:10.1002/2016JD024844.
In Figures 6 and 8, please explain the meaning of "1α run-to-run uncertainty".
Technical comments:
lines 225, 301, 322 : Make sure that there is no line break between sign and number in "- 30" and "- 50".
line 226: "While the gas..." is not a full sentence.
Section 3.2, first paragraph: When presenting and discussing Figure 2, add a reference to supplementary material Figures S1 and S2 for other systems.
line 248: "While GR..." is not a full sentence.
line 285: Change "autooxidation" to "autoxidation" to be consistent throughout the manuscript.
lines 204, 312, 336, 375: Here, "new particle formation rate" is used, while J_1.7nm is introduced as "nucleation rate" in the manuscript. For consistency, I recommend using "nucleation rate" throughout the manuscript.
In Figures 6 and 8: "GRC" should read "GCR" in the figure legend. Also, in the last sentence of the figure caption, remove "and" before "is not shown".-
AC1: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-512/acp-2021-512-AC1-supplement.pdf
-
AC1: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
-
RC2: 'Review of Caudillo et al.', Anonymous Referee #2, 11 Aug 2021
General comments
Caudillo et al. present chamber measurements of new-particle formation from α-pinene (AP) oxidation products at low temperatures, and study the effects of added isoprene (IP) and increased relative humidity (RH). The main focus is on the chemical composition of gas-phase species and (non-size-resolved) ultrafine particles, determined with a nitrate chemical ionization mass spectrometer and a thermal desorption-differential mobility analyzer, and in addition also nucleation rates are reported. Isoprene is observed to affect the chemical composition through an increase in e.g. C5 and C15 compounds, and to suppress new-particle formation as also reported in other studies.
Simultaneous measurements of gas- and particle-phase composition are essential for improving the understanding of biogenic secondary aerosol formation. The manuscript is generally well written and the results are clearly presented. I can recommend the work to be published in ACP after the authors have addressed the following comments:
Specific comments
1. Regarding the discussion on the effects of isoprene on the elemental composition, especially C5 and C15 compounds are stated to be increased in intensity. This seems clearer in the case of gas phase, whereas for particle phase the effects seem more diverse and e.g. Figure 3 shows similar increases in the signal intensity for various compounds with carbon content of up to ca. C18, C19. I cannot clearly distinguish a stronger increase specifically at C15 in Figs. 3 or S1; can this be further clarified?
2. It may not be obvious that higher particle growth rates (GR) at larger particle sizes are due to isoprene (Section 3.2.1, last paragraph: “Reaching the same mass with a lower number of particles for the experiment with isoprene (αIP-30,20) compared to α-30,20, means that the growth rates at larger sizes (> 15 nm) are higher in the presence of isoprene”).
Particle GRs can generally be higher at lower particle number concentrations, as the amount of available condensable vapor per particle is higher. Can it be concluded that the enhanced growth at larger sizes is specifically related to isoprene, and not to such dynamic effects?
3. Effect of RH (Section 3.2.2): the particle mass concentration is observed to increase at elevated RH at otherwise similar conditions. However, Fig. S3 shows that the α-pinene level is somewhat higher for the experiments with higher RH. Can the higher AP level contribute to the increased particle mass?
Also, the RH range of 60-100% for the high-RH experiments is rather broad. What is the reasoning for lumping together these different RH values, and is it possible that the RH effects vary within this 60-100% range?
4. Similarly to the RH experiments, it seems that the AP level during the particle formation event and sample collection of the isoprene experiment is not exactly similar to the experiments without IP; it seems to be lower for the AP-IP set-up (Figure 1, third row). Can this affect the AP vs. AP-IP comparison?
5. Section 3.3: It would be helpful to list the actual fractions of the different VBS bins instead of only stating that the particle-phase species are mainly LVOC, ELVOC and ULVOC (it also seems that ULVOC is only a minor fraction). This could be a table with the bin fractions given for the different experiments.
6. The O3 level of 100 ppbv seems rather high. How does it compare with typical tropospheric values? This is relevant considering the discussion on the effects of mixing ratios on the composition and nucleation of HOM (Section 3.4.1).
7. On P5L149-150, it is stated that particle evaporation before analysis should not be substantial; can this be assessed in a quantitative manner? Are there other uncertainty sources such as different charging efficiencies or transmission of the compounds?
I also agree with Referee #1 that an assessment of the relative contributions of the smallest and the larger particles to the particle-phase mass samples would be very useful.
8. P11L350: The meaning of “GCR conditions” is not explained; please clarify.
Technical corrections
P6L174: The particle formation rate is said to be defined as the flux of particles of a certain size as a function of time, but presumably the reported rates are not actually time-dependent; “as a function of time” should thus be removed, for clarity.
P6L202: It may be more appropriate to write “this is in line with the results of Kiendler-Scharr et al….” instead of “this confirms the results of …”
P7L226-227: Please reformulate the expression “the gas and particle of α-pinene” and similar occurrences.
P8L245: Please change “nSEMS” to “nSMPS” (?).
P8L254: Change “growth at higher sizes” to “growth at larger sizes”.
P9L268: The term “mass distribution” (here referring to particle mass size distribution?) may be a bit misleading as it might be confused with elemental composition or volatility distribution; please reformulate.
Figure 2 and similar plots: also the particle-phase fractions should preferably be written as positive instead of negative numbers (even if they are presented on the “negative” axis).
Caption of Figure 2: For clarity, “each system” could be changed to “each system and phase”.
Caption of Figure 3 and similar occurrences: the expression “mass defect plots of gas and particle phase and the intensity difference between them” is misleading; this sounds like the intensity difference between the gas and particle phases instead of the difference between the experiments. Please reformulate.
Legend of Figure 6 and similar occurrences: Please change “GRC” to “GCR”.
Caption of Figure 8 and similar occurrences: Please change “galactic comic rays” to “galactic cosmic rays”. :-)
Caption of Figure S4: Please state that this is Figure 5 in linear scale.
Figure S5: Why are the orange shades triangle-shaped?
Caption of Figure S6: Please explain the meaning of “overflow bin” and why the values of the first bin are both negative and positive.
-
AC2: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-512/acp-2021-512-AC2-supplement.pdf
-
AC2: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
Peer review completion


Interactive discussion
Status: closed
-
RC1: 'Comment on acp-2021-512', Anonymous Referee #1, 28 Jul 2021
Caudillo and co-authors present and discuss the gas and particle phase composition of pure biogenic nucleation events measured with a nitrate chemical ionization atmospheric pressure interface time of flight mass spectrometer (coupled with a thermal desorption-differential mobility analyzer for the particle phase) in the CLOUD chamber at a range of conditions representing free tropospheric conditions. Specifically, alpha-pinene and a mix of alpha-pinene and isoprene were oxidized at -30 deg C and - 50 deg C, and at 20 % or 60 - 100 % relative humidity. The authors find C8-10 monomers and C18-20 dimers as major compounds, and C5 and C15 compounds contributing to particle growth when isoprene is present in the system. I very much appreciate the systematic analysis. The manuscript is well-written and the experimental results are thoroughly discussed. In my opinion, this is an original and valuable contribution to the field. Therefore, it should be published in ACP after minor revisions.
Specific comments:
In the abstract, the last sentence ("Besides the chemical information...", lines 64-66) was confusing to me. After reading section 3.4.1, I suggest to be more specific in the abstract, e.g. "Compared with previous studies, we found lower nucleation rates measured at 1.7 nm, very likely due to higher alpha-pinene and ozone mixing ratios used in the present study."In section 2.1, there is no information about GCR conditions during the experiments, please add.
In section 2.2, please add some more information about the heating procedure of the filament. Is the temperature slowly ramped up, or do you apply high temperature directly to instantaneously vaporize the sample? This is also relevant for the discussion of potential thermal decomposition of molecules in section 3.2.2.
Regarding the non-size selective mode of operation of the TD-DMA, it would be helpful to get an idea about the contribution of freshly nucleated particles vs. grown particles to the sampled mass. From the measured particle size distributions and the PSM and CPC total number concentrations, could you calculate a rough estimate of the volume/mass fraction of particles < 15 nm in the samples collected in the periods shown in Figure 1 as shaded areas? Please add this information to Table 1.
In Figure 3f, to me it is not obvious that specifically C4-5 and C13-16 compounds are enhanced as stated in lines 237/238. Please clarify.
In section 3.3, looking at Figures 5 and S4 I agree with the statement that mainly LVOC and ELVOC compounds were detected in the particle phase, however, the ULVOC compounds appear to be a minor fraction.
Section 3.4.2: Regarding the discussion of isoprene suppression of new particle formation, please consider adding a reference to Lee et al. (2016), doi:10.1002/2016JD024844.
In Figures 6 and 8, please explain the meaning of "1α run-to-run uncertainty".
Technical comments:
lines 225, 301, 322 : Make sure that there is no line break between sign and number in "- 30" and "- 50".
line 226: "While the gas..." is not a full sentence.
Section 3.2, first paragraph: When presenting and discussing Figure 2, add a reference to supplementary material Figures S1 and S2 for other systems.
line 248: "While GR..." is not a full sentence.
line 285: Change "autooxidation" to "autoxidation" to be consistent throughout the manuscript.
lines 204, 312, 336, 375: Here, "new particle formation rate" is used, while J_1.7nm is introduced as "nucleation rate" in the manuscript. For consistency, I recommend using "nucleation rate" throughout the manuscript.
In Figures 6 and 8: "GRC" should read "GCR" in the figure legend. Also, in the last sentence of the figure caption, remove "and" before "is not shown".-
AC1: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-512/acp-2021-512-AC1-supplement.pdf
-
AC1: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
-
RC2: 'Review of Caudillo et al.', Anonymous Referee #2, 11 Aug 2021
General comments
Caudillo et al. present chamber measurements of new-particle formation from α-pinene (AP) oxidation products at low temperatures, and study the effects of added isoprene (IP) and increased relative humidity (RH). The main focus is on the chemical composition of gas-phase species and (non-size-resolved) ultrafine particles, determined with a nitrate chemical ionization mass spectrometer and a thermal desorption-differential mobility analyzer, and in addition also nucleation rates are reported. Isoprene is observed to affect the chemical composition through an increase in e.g. C5 and C15 compounds, and to suppress new-particle formation as also reported in other studies.
Simultaneous measurements of gas- and particle-phase composition are essential for improving the understanding of biogenic secondary aerosol formation. The manuscript is generally well written and the results are clearly presented. I can recommend the work to be published in ACP after the authors have addressed the following comments:
Specific comments
1. Regarding the discussion on the effects of isoprene on the elemental composition, especially C5 and C15 compounds are stated to be increased in intensity. This seems clearer in the case of gas phase, whereas for particle phase the effects seem more diverse and e.g. Figure 3 shows similar increases in the signal intensity for various compounds with carbon content of up to ca. C18, C19. I cannot clearly distinguish a stronger increase specifically at C15 in Figs. 3 or S1; can this be further clarified?
2. It may not be obvious that higher particle growth rates (GR) at larger particle sizes are due to isoprene (Section 3.2.1, last paragraph: “Reaching the same mass with a lower number of particles for the experiment with isoprene (αIP-30,20) compared to α-30,20, means that the growth rates at larger sizes (> 15 nm) are higher in the presence of isoprene”).
Particle GRs can generally be higher at lower particle number concentrations, as the amount of available condensable vapor per particle is higher. Can it be concluded that the enhanced growth at larger sizes is specifically related to isoprene, and not to such dynamic effects?
3. Effect of RH (Section 3.2.2): the particle mass concentration is observed to increase at elevated RH at otherwise similar conditions. However, Fig. S3 shows that the α-pinene level is somewhat higher for the experiments with higher RH. Can the higher AP level contribute to the increased particle mass?
Also, the RH range of 60-100% for the high-RH experiments is rather broad. What is the reasoning for lumping together these different RH values, and is it possible that the RH effects vary within this 60-100% range?
4. Similarly to the RH experiments, it seems that the AP level during the particle formation event and sample collection of the isoprene experiment is not exactly similar to the experiments without IP; it seems to be lower for the AP-IP set-up (Figure 1, third row). Can this affect the AP vs. AP-IP comparison?
5. Section 3.3: It would be helpful to list the actual fractions of the different VBS bins instead of only stating that the particle-phase species are mainly LVOC, ELVOC and ULVOC (it also seems that ULVOC is only a minor fraction). This could be a table with the bin fractions given for the different experiments.
6. The O3 level of 100 ppbv seems rather high. How does it compare with typical tropospheric values? This is relevant considering the discussion on the effects of mixing ratios on the composition and nucleation of HOM (Section 3.4.1).
7. On P5L149-150, it is stated that particle evaporation before analysis should not be substantial; can this be assessed in a quantitative manner? Are there other uncertainty sources such as different charging efficiencies or transmission of the compounds?
I also agree with Referee #1 that an assessment of the relative contributions of the smallest and the larger particles to the particle-phase mass samples would be very useful.
8. P11L350: The meaning of “GCR conditions” is not explained; please clarify.
Technical corrections
P6L174: The particle formation rate is said to be defined as the flux of particles of a certain size as a function of time, but presumably the reported rates are not actually time-dependent; “as a function of time” should thus be removed, for clarity.
P6L202: It may be more appropriate to write “this is in line with the results of Kiendler-Scharr et al….” instead of “this confirms the results of …”
P7L226-227: Please reformulate the expression “the gas and particle of α-pinene” and similar occurrences.
P8L245: Please change “nSEMS” to “nSMPS” (?).
P8L254: Change “growth at higher sizes” to “growth at larger sizes”.
P9L268: The term “mass distribution” (here referring to particle mass size distribution?) may be a bit misleading as it might be confused with elemental composition or volatility distribution; please reformulate.
Figure 2 and similar plots: also the particle-phase fractions should preferably be written as positive instead of negative numbers (even if they are presented on the “negative” axis).
Caption of Figure 2: For clarity, “each system” could be changed to “each system and phase”.
Caption of Figure 3 and similar occurrences: the expression “mass defect plots of gas and particle phase and the intensity difference between them” is misleading; this sounds like the intensity difference between the gas and particle phases instead of the difference between the experiments. Please reformulate.
Legend of Figure 6 and similar occurrences: Please change “GRC” to “GCR”.
Caption of Figure 8 and similar occurrences: Please change “galactic comic rays” to “galactic cosmic rays”. :-)
Caption of Figure S4: Please state that this is Figure 5 in linear scale.
Figure S5: Why are the orange shades triangle-shaped?
Caption of Figure S6: Please explain the meaning of “overflow bin” and why the values of the first bin are both negative and positive.
-
AC2: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
The comment was uploaded in the form of a supplement: https://acp.copernicus.org/preprints/acp-2021-512/acp-2021-512-AC2-supplement.pdf
-
AC2: 'Interactive discussion_Response to both referees_Caudillo et al', Lucía Caudillo Murillo, 27 Sep 2021
Peer review completion


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Lucía Caudillo et al.
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