From the journal Environmental Science: Atmospheres Peer review history

15-Feb-2024

Dear Dr He:

Manuscript ID: EA-ART-01-2024-000013
TITLE: Temperature, humidity, and ionisation effect of iodine oxoacid nucleation

Thank you for your submission to Environmental Science: Atmospheres, published by the Royal Society of Chemistry. I sent your manuscript to reviewers and I have now received their reports which are copied below.

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Reviewer 1

See attached

Reviewer 2

Rörup and co-workers investigated the influence of temperature, humidity, and ionisation on iodine oxoacid nucleation by the combination of measurements from the CLOUD chamber at CERN and simulations with a kinetic model. This study reveals that charged cluster nucleation pathway of iodic acid is unlikely to be enhanced in the upper troposphere by higher ionisation rates. However, the neutral nucleation channel is likely to be the dominant channel in that region. Iodine oxoacid nucleation mechanism remains unaffected by changes in relative humidity from 2% to 80%. Thus, iodine oxoacid nucleation is the dominant nucleation mechanism for iodine nucleation in the marine and polar boundary layer atmosphere. In general, the manuscript is well written and is of broad interest to the readership of Environmental Science: Atmospheres. I can recommend publication in Environmental Science: Atmospheres after the following comments have been addressed.
Specific Comments:
Lines 100-102: “Recent theoretical work utilizing quantum chemical calculations and kinetic simulations further uncovered the critical role of HIO2 in stabilizing HIO3 clusters because HIO2 exhibits strong alkaline-like behavior. The fact that iodine oxidation produces both HIO3 and HIO2 makes its nucleation process autonomous; this differentiates iodine species from the sulphuric acid nucleation, which typically requires additional base molecules such as ammonia and amines to form stable cluster.”
The stabilizing effect of HIO2 on the cluster formation without additional base molecules because of its strong alkaline-like behavior should be further illustrated. The relevant studies [Science, 2023, 382(6676), 1308-1314; Atmospheric Environment, 2024, 318, 120266; Environmental Research Letters, 2024, 19, 014076; Physical Chemistry Chemical Physics, 2023, 25, 16745-16752] also should be referred to illustrate the important role of HIO2 in cluster formation without base molecules.
Lines 109-110: “These factors include atmospheric ionisation rates, humidity, and temperature.”
Please further elaborate the importance of the influence of atmospheric ionization rates and temperature on the particle formation.
Lines 118-119: “Combining those parameters allows us to evaluate how significant the charged cluster formation mechanism is in the upper troposphere.”
What’s the significance of particle formation in the upper troposphere? The necessity to evaluate the significance of charged cluster formation mechanism is in the upper troposphere should be illustrated.
Lines 323-327: “This is likely due to the fact that the neutral iodine oxoacid nucleation dominates the total formation rate at -10°C and the ion-induced channel has only a small contribution. On the contrary, elevating the ionisation rate from 0 to 4.1 ion pairs cm-3 s-1 at +10°C results in an increase of the formation rate at +10°C from 0.04 to 3.5 cm-3 s-1, highlighting the importance of ion-induced nucleation at warmer temperatures.”
Please explain why the neutral iodine oxoacid nucleation dominates the total formation rate at relative low temperature while the ion-induced nucleation is important at warmer temperatures.
Lines 374-377: “It is important to note that increasing the sink from its default value has a more significant impact on overall formation rates compared to decreasing the sink by the same factor at HIO3 < 2×107 cm-3, as the charged cluster formation process is growth-limited.”
Please explain in more detail why the charged cluster formation process is growth-limited.
Lines 510-512: “Figure 6: Formation rates at different relative humidities (below 0.008 to 80%) in the CLOUD chamber under GCR conditions at +10°C against different iodine compounds: A) HIO3, B) HIO2, C) HIO3×HIO2, D) I2O4, E) I2O5 and F) HIO3×HIO2×(I2O4+I2O5).”
How are the concentrations of HIO3, HIO2, I2O4, and I2O5 shown in Figure 6 F respectively determined in the CLOUD chamber?
Technical corrections:
Figure 1: The particle formation rate, J, should be in italic in the Figure 1.
Figure 6: The unit of the concentration of different iodine compounds should be indicated in the title of the abscissa axis.

Review of Rörup et al for Environmental Science: Atmospheres
Title: Temperature, humidity, and ionisation effect of iodine oxoacid nucleation
Dear Prof. Wang,
We value the reviewers' feedback, which has helped enhance our manuscript. Please find below our point-by-point replies to the comments. The Line numbers refer to the revised manuscript showing tracked changes.

Referee 1:
Rorup and the CLOUD consortium study the effect of temperature, humidity and ionization level on iodine oxoacid nucleation. It is found that ion-induced nucleation is little affected by temperature. The ionization level has a limited impact on the nucleation unless HIO3 concentrations reach unrealistically high values. Interestingly, hydration also has a negligible effect on the nucleation mechanism. This is an interesting paper that builds well upon previous studies of iodine oxoacid nucleation. While the work is essentially a null result in the sense that the studied mechanism is unaffected, it still gives valuable insight into the nucleation mechanism of iodine oxyacids.
I am no expert on chamber experiments, but as far as I can see the measurements are carried out impeccably. I only have a few minor comments and can recommend publication after these are taken into account.


Environmental Significance Statement
”Our findings indicate that iodine oxoacid nucleation rates increase with decreasing temperature because of the neutral nucleation channel.”
I do not understand the logic behind this statement. What in the neutral nucleation channel is it that makes the nucleation rate to increase with decreasing temperature? Usually, the nucleation rate increase with decreasing temperature as a result of the evaporation rate of the clusters will decrease. Please rephrase.

The reviewer is correct. The statement has been rephrased.
“Understanding atmospheric new particle formation is of paramount importance, since it is impacting the climate. Particle formation through iodine oxoacid nucleation has rarely been incorporated into global simulations, despite observations at various coastal locations and increasing concentration of iodine, primarily driven by climate change. This study employs chamber measurements and a kinetic model to explore the influence of temperature, ionisation rate, and humidity on iodine oxoacid nucleation. Our findings indicate that ion-induced formation rates of iodine oxoacid are not significantly affected by temperature, but the neutral nucleation rates increase with decreasing temperature. Furthermore, increases in ionisation rates decrease the ion-induced nucleation rate under atmospherically relevant iodic acid concentrations and humidity has no significant effect on iodine oxoacid nucleation.”


Line 227: I assume that “Chapter” should “SecMon” throughout the manuscript.

“Chapter” has been replaced with “Section” throughout the manuscript.


Line 231: JGCR has not been defined here.

The sentence has been adjusted to be clearer.
“At CLOUD we can directly measure JN, JGCR, and JBeam by varying the ionisation setting of the chamber between Neutral, GCR and Beam, as explained in Section 2.1.” (Lines 237-238)


Line 240: “We want to point out that J± is not exactly the same as Jiin since ion-ion recombination might contribute to the enhancement of formation rates due to ions, which cannot be accounted for in the model.”
It is explicitly written in line 262 that ion-ion-recombination parameterization is included?

The ion-ion recombination takes into account the ion loss due to neutralisation, but it does not take into account the neutralised particles. The sentence has been changed for clarification.
“We note that J± differs from Jiin because the model does not account for neutralised particles resulting from ion-ion recombination.” (Lines 246-247)


Section 2.6: Some more detail about the kinetics model is needed. What input is needed and how do you set up the model? Is evaporation completely suppressed in the model? Perhaps a more in-depth description should be added to ESI. In addition, it would be worth discussing the difference between the currently applied model and results obtained in the literature with the Atmospheric Cluster Dynamics Code (ACDC).

The model has not been developed for this paper and the detailed information can be found in He et al (2021)52. Some sentences have been added to answer the questions and make it clearer where further information is found.
“The kinetic model Polar ANd high-altituDe Atmospheric research 520 (PANDA520)1 was used to calculate the formation rate of the charged clusters (J±) for ion-induced iodic acid nucleation. Further information on the model can be found in He et al (2021)52. For this study, the PANDA520 model was simplified to only include the parametrisations that are necessary for this study, which are wall and dilution loss, ion-ion recombination and ion-neutral collision processes. Additionally, we included temperature and pressure dependent parametrisations to investigate the temperature and altitude dependency of the formation rate of charged clusters.
It was previously shown that ion-induced iodic acid nucleation only occurs in the negative ion channel, while the positive ion channel shows no cluster growth16. Therefore, positive clusters are treated as one of the sinks for the negative clusters in the model. Additionally, evaporation rates are not taken into account in the model since He et al (2021)16 concluded that ion-induced nucleation from iodine oxoacids proceeds at the collision limit with negligible cluster evaporation, especially at temperatures below 10°C. Furthermore, the model includes parametrisations for wall and dilution loss, ion-ion recombination and ion-neutral collision.” (Lines 259-272)


Line 317: “This confirms that a lower temperature significantly enhances the neutral iodine oxoacid nucleation, consistent with our previous study.”
It sounds a bit like this is a finding only realized by the current and the previous study by the authors. However, this has been an established fact in the nucleation community for many years (see https://doi.org/10.1021/cr2001756 and https://doi.org/10.1016/j.jaerosci.2020.105621). It is simply a direct consequence of the cluster formation process (ΔS < 0 and ΔH < 0). Please make it transparent that this is known fact.

Those studies have been included in the references.
“This confirms that a lower temperature significantly enhances the neutral iodine oxoacid nucleation, consistent with previous studies16,62,63.” (Line 328)


Line 439: “This good agreement indicates that J± dominates the Jtot (JGCR) under these conditions. This is independently confirmed by the negligible JN measurements in CLOUD under these conditions.”
This is not necessarily true. It could also be a lucky coincidence. Please add the caveat that as the model is not perfect and thereby a match with experiment might be caused by error cancellation.

We agree with the reviewer and have adjusted the logic flow and added the uncertainty statement.
“Our earlier study16has confirmed a negligible JN under these conditions. Thus, this good agreement indicates that J± dominates the Jtot (JGCR). However, due to uncertainties of our experiments and model, we cannot distinguish a Jrec contribution of up to 50 % to Jtot. Therefore, we do not exclude the possibility of a minor contribution from Jrec.” (Lines 458-461)


Line 451: ”… we consider that the agreement is reasonable. The observed particle formation rates in the Arctic Ocean at temperatures from -1°C to -9°C fall mostly between the CLOUD data at +10°C and -10°C, and a little bit above the simulated J±. ”
The authors say that the agreement is reasonable. However, very few datapoints overlap with the model. Why does the -10°C show worse agreement compared to the +10°C, when the measurements are at -1°C to -9°C? Why is the model failing at high HIO3 concentration? Some more discussion on these discrepancies is warranted.

The formation rate for the field data is calculated at 2.5 nm because there were no instruments present that measured lower particle sizes while our data report nucleation rate at 1.7 nm. The nucleation rate at 2.5 nm is expected to be smaller than the nucleation rate at 1.7 nm. We tried to make it clearer.
“We used the data from Baccarini et al. (2020)24 to calculate J2.5 for a subset of reported particle formation events, where particles were present in the smallest size channels of the NAIS so that we could assume that they were formed at or very close to the measurement location (Figure 5, triangle symbols). It was not possible to calculate J1.7 directly, since no instruments that measured this size range were present. Given the uncertainties in the instrumentation, slightly different size range (J2.5 is commonly smaller than J1.7) and method to calculate the formation rates (see Section 2.4), we consider that the agreement is reasonable.” (Line 471-478)
The model is not failing at high HIO3 concentrations but the neutral nucleation becomes the dominant process. This is explained earlier.
“At higher HIO3 concentrations JN increases rapidly, while J± levels off because it is limited by the ion production rate and therefore, JGCR starts to deviate from the model line.” (Line 462-464)


Line 470: “… relative humidity from below 0.008% to 80%, which is equivalent to 0.0007 – 7.5 g m-3 absolute humidity.”
What is the range of the absolute water concentration in molecules cm-3? It will make it a lot easier to judge whether the lowest value is essentially zero or comparable to the other vapours if they are given in the same units.

The absolute water concentration was added.
These experiments were conducted at +10°C and relative humidity from below 0.008% to 80%, which is equivalent to an absolute water molecule concentration of 2.52×1013 - 2.55×1017 cm-3. (Lines 494-495)
 

Referee: 2
Comments to the Author
Rörup and co-workers investigated the influence of temperature, humidity, and ionisation on iodine oxoacid nucleation by the combination of measurements from the CLOUD chamber at CERN and simulations with a kinetic model. This study reveals that charged cluster nucleation pathway of iodic acid is unlikely to be enhanced in the upper troposphere by higher ionisation rates. However, the neutral nucleation channel is likely to be the dominant channel in that region. Iodine oxoacid nucleation mechanism remains unaffected by changes in relative humidity from 2% to 80%. Thus, iodine oxoacid nucleation is the dominant nucleation mechanism for iodine nucleation in the marine and polar boundary layer atmosphere. In general, the manuscript is well written and is of broad interest to the readership of Environmental Science: Atmospheres. I can recommend publication in Environmental Science: Atmospheres after the following comments have been addressed.


Specific Comments:

Lines 100-102: “Recent theoretical work utilizing quantum chemical calculations and kinetic simulations further uncovered the critical role of HIO2 in stabilizing HIO3 clusters because HIO2 exhibits strong alkaline-like behavior. The fact that iodine oxidation produces both HIO3 and HIO2 makes its nucleation process autonomous; this differentiates iodine species from the sulphuric acid nucleation, which typically requires additional base molecules such as ammonia and amines to form stable cluster.”
The stabilizing effect of HIO2 on the cluster formation without additional base molecules because of its strong alkaline-like behavior should be further illustrated. The relevant studies [Science, 2023, 382(6676), 1308-1314; Atmospheric Environment, 2024, 318, 120266; Environmental Research Letters, 2024, 19, 014076; Physical Chemistry Chemical Physics, 2023, 25, 16745-16752] also should be referred to illustrate the important role of HIO2 in cluster formation without base molecules.

The papers mentioned here are talking about the H2SO4-HIO2 nucleation mechanism, and have been added to the manuscript.
“The stabilising effect of HIO2 was also seen with sulphuric acid 21,37,38.” (Lines 107-108)


Lines 109-110: “These factors include atmospheric ionisation rates, humidity, and temperature.”
Please further elaborate the importance of the influence of atmospheric ionization rates and temperature on the particle formation.

A sentence has been added to make it clearer.
The importance of atmospheric ionisation rates lies in their direct influence on particle formation dynamics, particularly in the upper troposphere where charged clusters play a significant role. Similarly, temperature is a crucial parameter affecting nucleation rates, as variations in temperature can significantly impact the stability and reactivity of precursor molecules39. Hence, understanding the precise influence of these factors is paramount for accurately representing them in models. (Lines 111-116)


Lines 118-119: “Combining those parameters allows us to evaluate how significant the charged cluster formation mechanism is in the upper troposphere.”
What’s the significance of particle formation in the upper troposphere? The necessity to evaluate the significance of charged cluster formation mechanism is in the upper troposphere should be illustrated.

The text has been adjusted to show the significance of HIO3 in the upper troposphere.
“Recent measurements of iodine in the upper troposphere suggest the presence of HIO3 in this region40. Combining those parameters allows us to evaluate how significant the charged cluster formation mechanism of iodic acid is in the upper troposphere.” (Lines 125-127)


Lines 323-327: “This is likely due to the fact that the neutral iodine oxoacid nucleation dominates the total formation rate at -10°C and the ion-induced channel has only a small contribution. On the contrary, elevating the ionisation rate from 0 to 4.1 ion pairs cm-3 s-1 at +10°C results in an increase of the formation rate at +10°C from 0.04 to 3.5 cm-3 s-1, highlighting the importance of ion-induced nucleation at warmer temperatures.”
Please explain why the neutral iodine oxoacid nucleation dominates the total formation rate at relative low temperature while the ion-induced nucleation is important at warmer temperatures.

The sentence was changed to make it clearer.
“This is likely due to the fact that ion-induced nucleation of iodic oxoacids is already proceeding at the kinetic limit at +10°C and therefore cannot increase further when the temperature decreases16. On the other hand, the neutral iodine oxoacid nucleation is relatively weak at +10°C and it is significantly enhanced at -10°C. Hence, the neutral iodine oxoacid nucleation dominates the total formation rate at -10°C and the ion-induced channel becomes less significant.” (Lines 333-337)


Lines 374-377: “It is important to note that increasing the sink from its default value has a more significant impact on overall formation rates compared to decreasing the sink by the same factor at HIO3 < 2×107 cm-3, as the charged cluster formation process is growth-limited.”
Please explain in more detail why the charged cluster formation process is growth-limited.

An explanation has been added.
It is important to note that increasing the sink from its default value has a more significant impact on overall formation rates compared to decreasing the sink by the same factor at HIO3 < 2×107 cm 3. This is because the charged cluster formation process is controlled by two major sinks in the atmosphere: ion-ion recombination and coagulation with existing neutral particles. Neither of these processes depends on the concentration of HIO3. Conversely, the charged cluster growth process is dominated by HIO3 condensation. Therefore, at lower HIO3 concentrations, increasing the sink would have a more significant impact on reducing the cluster formation rate. (Lines 388-395)


Lines 510-512: “Figure 6: Formation rates at different relative humidities (below 0.008 to 80%) in the CLOUD chamber under GCR conditions at +10°C against different iodine compounds: A) HIO3, B) HIO2, C) HIO3×HIO2, D) I2O4, E) I2O5 and F) HIO3×HIO2×(I2O4+I2O5).”
How are the concentrations of HIO3, HIO2, I2O4, and I2O5 shown in Figure 6 F respectively determined in the CLOUD chamber?

They are measured with the nitrate-CIMS. A sentence has been added to the figure description.
The iodine species are measured with the nitrate-CIMS. (Line 539)


Technical corrections:

Figure 1: The particle formation rate, J, should be in italic in the Figure 1.

The figure has been adjusted accordingly.


Figure 6: The unit of the concentration of different iodine compounds should be indicated in the title of the abscissa axis.

The figure has been adjusted accordingly.

 
References

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21-Mar-2024

Dear Dr He:

Manuscript ID: EA-ART-01-2024-000013.R1
TITLE: Temperature, humidity, and ionisation effect of iodine oxoacid nucleation

Thank you for submitting your revised manuscript to Environmental Science: Atmospheres. I am pleased to accept your manuscript for publication in its current form.

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