Representing improved tropospheric ozone distribution by including lightning NOx emissions in CHIMERE

Ghosh, Sanhita; Cholakian, Arineh; Mailler, Sylvain; Menut, Laurent

doi:https://doi.org/10.5194/egusphere-2024-3087

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https://doi.org/10.5194/egusphere-2024-3087

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05 Nov 2024

| 05 Nov 2024

Representing improved tropospheric ozone distribution by including lightning NOx emissions in CHIMERE

Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut

Abstract. Estimating nitrogen oxide emissions from lightning (LNOx) in models is highly uncertain, affecting the accuracy of atmospheric composition and air quality assessments. Still, it is essential to include the emissions in model to increase the realism in representing the model outcomes. LNOx emissions have recently been incorporated into the updated version of the CHIMERE model (v2023r2). In the present study, we evaluate the present state of modelling the lightning flashes and the LNOx emissions, using a classical scheme based on cloud top height (CTH) and the model CHIMERE. We asses the impact of LNOx on tropospheric ozone (O₃) concentration over the northern hemisphere (NH) through a detailed evaluation of simulated tropospheric O₃. The total NO emission from lightning is estimated as 8.82 Tg N yr⁻¹ over the NH. There is an overall increase in O₃ concentration due to inclusion of LNOx. The increase is highest in the mid to upper troposphere, specifically over the tropics. The comparison of the simulated O₃ to measurements shows that the inclusion of LNOx emissions substantially improves the tropospheric O₃ distribution, reducing bias significantly. This is particularly true for the free troposphere over the tropical region. The LNOx emissions hence critically influence the O₃ concentration as well as the concentration of hydroxyl radicals (OH). There are 15 % and 40 % increases, respectively, in O₃ and OH burden as observed due to the inclusion of LNOx in model, which further impact the atmospheric lifetime of trace gas methane (CH₄) by reducing it by 24 %.

Received: 02 Oct 2024 – Discussion started: 05 Nov 2024

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Journal article(s) based on this preprint

26 Jun 2025

Representing improved tropospheric ozone distribution over the Northern Hemisphere by including lightning NO_x emissions in CHIMERE

Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut

Atmos. Chem. Phys., 25, 6273–6297, https://doi.org/10.5194/acp-25-6273-2025,https://doi.org/10.5194/acp-25-6273-2025, 2025

Short summary

Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2024-3087', Anonymous Referee #1, 19 Nov 2024

Summary:
The authors implement a cloud-height based flash rate scheme into the regional model CHIMERE and then evaluate the impact of lightning-NOx production on ambient ozone and NO2 concentrations, ozone profiles, the tropospheric OH burden, and the methane lifetime.
The magnitude of the lightning-NOx source is biased high, which has implications for the LNOx increment, OH burden, and CH4 lifetime. Thus, I think the authors need to re-run the simulation with a lower LNOx source, and then spend more time evaluating the lightning parameterization. As the LNOx scheme is not new, it would help if they modify it to better simulate the seasonal cycle. Thus, I would suggest rejecting the manuscript – at least for now.
Main Comments:
The evaluation of the flash rate scheme needs to be enhanced.
L8 & L202: 8.82 Tg N yr-1 is too high of a production rate for just the Northern Hemisphere. It is consistent with ~15 Tg N yr-1 for the globe, a value that is well outside of the typically cited 2-8 Tg N yr-1 range. You need to justify why you chose that value or choose a lower value.
L119: I don’t understand why the flash rate you obtain is so high given that you’ve scaled it to match a satellite product. What satellite data are you comparing to? What is the estimated flash rate of the satellite-based observation? What is the Northern Hemisphere flash rate after applying the scaling factor?
L210: You note that the model does not capture the seasonality of flash rates. Could you compare the monthly model flashes for 0 to 35 N with OTD/LIS climatology. It would also be interesting to compare the flash rates with the diel OTD/LIS climatology. Is this a problem with the model’s cloud top heights or with the scheme itself?
L125: Typically, the “land-based” parameterization is used for grid boxes near land as well, i.e. continental convection extends a few grid boxes downwind of land.
L132: Could you give values of Hf for 0, 30, and 60 N.
L135: What is the ratio of CG to IC flashes that you obtain over the NH with this parameterization?
L140: Include a plot showing the percent of CG and IC LNOx emissions input into each 1-km layer for land and water over the tropics and midlatitudes.
L187: By what metric is the flash rate in agreement with the ISS-LIS data set? How was the ISS-LIS May-August “climatology” obtained? What years were used? Was there a correction for viewing time? Was there a correction for detection efficiency? How many total flashes are there during May-August (and the year) for ISS-LIS and the model. How do the flash totals compare to the OTD/LIS climatology for this period.
L189: Yes, putting too many flashes in the tropics is a fairly well known bias of cloud-height based schemes. Do you have any suggestions as to how this bias could be reduced while still retaining the cloud-height scheme?
You need to add comparisons with OMI/TROPOMI and SHADOZ.
L214: The impact of lightning-NOx on atmospheric composition is larger in the mid- and upper-troposphere than it is at the surface, yet you begin with a surface comparison. I would suggest saving that comparison for last.
You compare with surface concentrations and profiles. You should also compare model NO2 with satellite-retrieved columns from OMI (January-December 2018) or TROPOMI (April – December 2018).
The SHADOZ ozonesondes are a wonderful source of profile information and should be compared to. Despite the acronym, there are a number of Northern Hemisphere sites.
It should be more revealing to calculate biases as a function of season as opposed to annually.
You need to improve the model simulation. This will add value to the comparison with observations.
L315-320: CH4 lifetime of 4.89 years is considerably less than range of 7-14. Obviously, your large LNOx source is contributing to this low bias in lifetime.
You need to be careful with generalized statements.
There are numerous reasons why a model may have a high-or-low bias in ozone at the surface. The magnitude of the LNOx source plays only a small role here.
Stratosphere-troposphere exchange is poorly resolved in this model due to its low model top. This may make comparison with mid- and high-latitude ozone profiles problematic.
Minor Comments:
L24: The range you cite here (8 to 4000 moles NO / flash) is for individual flashes. Estimates of the mean production per flash are usually between 125 and 500 moles per flash.
L73: Is 998 hPa the mean surface pressure?
L74: A 200 hPa top layer is when evaluating O3 profiles. What is the pressure of the model top? Clearly, this model was designed for tropospheric chemistry.
L160 and L201: Is this a climatological flash data set from ISS-LIS? If so, what years does it cover?
L192: Are you saying that the modeled tropopause height is too high in the tropics? If yes, please show.
L200: Why are you comparing May-August flash rates with the annual mean?
L207: You need to be clear here. 8.8 Tg N yr-1 for the NH is consistent with ~15 Tg N yr-1 for the globe, a value that is well outside of the 2-8 range but below 25.
L214: Why do you think emissions are underestimated?
L265: Do any of these studies give the NH burden? Or do they just list the total burden?
L269: Are you comparing to climatological ozone sondes or ozone sondes from 2018? You should consider comparing to individual SHADOZ sondes as several of the sites are located in NH.
L279: Stratosphere-troposphere exchange is one cause for the very low biases you are seeing in the extratropics and at high latitudes.
Grammatical Comments:
L19: such as lightning --- such as lightning and soil-NOx emissions
L24: 4000 mol NO per flash --- 4000 mol NO per individual flash
L25: suggest a value of 250 --- suggest a mean value of 250
L42: most frequently used CTH scheme --- the frequently used CTH scheme
L75: for chemical mechanisms --- for the chemical mechanism
L91: deep convection fluxes --- deep convective fluxes
L160: … but ISS-LIS only sees a small subset of total flashes …
L197: inconsistancies --- inconsistencies.
L223: represents a spatial variation --- varies spatially
L225: rest part of NH --- rest of the NH
L233: 10-25 ppbv enhancement of annual mean surface ozone due to lightning –
Figure 3d: 500-200 hPa or 500-300 hPa. Caption is not consistent with figure.

Citation: https://doi.org/10.5194/egusphere-2024-3087-RC1
- AC1: 'Reply on RC1', Sanhita Ghosh, 04 Dec 2024
  
  We sincerely thank the Referee for the constructive feedback and valuable suggestions, which have greatly enhanced the quality of our study.
  We are currently revising the manuscript and have addressed all the points raised by the Referee in detail. With improved configurations for advection, emissions, and boundary conditions, we are confident that these improvements will resolve most of the shortcomings identified. A revised version of the manuscript, along with a point-by-point response to the Referee's comments, will be submitted as soon as we have all the reviews.
  We greatly appreciate the Referee's insights and look forward to receiving further feedback on the revised manuscript.
  
  Citation: https://doi.org/10.5194/egusphere-2024-3087-AC1
RC2: 'Comment on egusphere-2024-3087', Anonymous Referee #2, 19 Dec 2024

I share the concerns of the reviewer who posted a comment on Nov. 19th, so I will not repeat them here.
One additional major concern: The scientific content of the paper is very low; it is not clear to me what new insights were found as a result of this analysis relative to what is already in the scientific literature. Therefore, I recommend that the authors consider publishing their manuscript in Geoscientific Model Development (https://www.geoscientific-model-development.net/) instead of ACP. GMD is meant for description papers of significant model development.

Citation: https://doi.org/10.5194/egusphere-2024-3087-RC2

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2024-3087', Anonymous Referee #1, 19 Nov 2024

Summary:
The authors implement a cloud-height based flash rate scheme into the regional model CHIMERE and then evaluate the impact of lightning-NOx production on ambient ozone and NO2 concentrations, ozone profiles, the tropospheric OH burden, and the methane lifetime.
The magnitude of the lightning-NOx source is biased high, which has implications for the LNOx increment, OH burden, and CH4 lifetime. Thus, I think the authors need to re-run the simulation with a lower LNOx source, and then spend more time evaluating the lightning parameterization. As the LNOx scheme is not new, it would help if they modify it to better simulate the seasonal cycle. Thus, I would suggest rejecting the manuscript – at least for now.
Main Comments:
The evaluation of the flash rate scheme needs to be enhanced.
L8 & L202: 8.82 Tg N yr-1 is too high of a production rate for just the Northern Hemisphere. It is consistent with ~15 Tg N yr-1 for the globe, a value that is well outside of the typically cited 2-8 Tg N yr-1 range. You need to justify why you chose that value or choose a lower value.
L119: I don’t understand why the flash rate you obtain is so high given that you’ve scaled it to match a satellite product. What satellite data are you comparing to? What is the estimated flash rate of the satellite-based observation? What is the Northern Hemisphere flash rate after applying the scaling factor?
L210: You note that the model does not capture the seasonality of flash rates. Could you compare the monthly model flashes for 0 to 35 N with OTD/LIS climatology. It would also be interesting to compare the flash rates with the diel OTD/LIS climatology. Is this a problem with the model’s cloud top heights or with the scheme itself?
L125: Typically, the “land-based” parameterization is used for grid boxes near land as well, i.e. continental convection extends a few grid boxes downwind of land.
L132: Could you give values of Hf for 0, 30, and 60 N.
L135: What is the ratio of CG to IC flashes that you obtain over the NH with this parameterization?
L140: Include a plot showing the percent of CG and IC LNOx emissions input into each 1-km layer for land and water over the tropics and midlatitudes.
L187: By what metric is the flash rate in agreement with the ISS-LIS data set? How was the ISS-LIS May-August “climatology” obtained? What years were used? Was there a correction for viewing time? Was there a correction for detection efficiency? How many total flashes are there during May-August (and the year) for ISS-LIS and the model. How do the flash totals compare to the OTD/LIS climatology for this period.
L189: Yes, putting too many flashes in the tropics is a fairly well known bias of cloud-height based schemes. Do you have any suggestions as to how this bias could be reduced while still retaining the cloud-height scheme?
You need to add comparisons with OMI/TROPOMI and SHADOZ.
L214: The impact of lightning-NOx on atmospheric composition is larger in the mid- and upper-troposphere than it is at the surface, yet you begin with a surface comparison. I would suggest saving that comparison for last.
You compare with surface concentrations and profiles. You should also compare model NO2 with satellite-retrieved columns from OMI (January-December 2018) or TROPOMI (April – December 2018).
The SHADOZ ozonesondes are a wonderful source of profile information and should be compared to. Despite the acronym, there are a number of Northern Hemisphere sites.
It should be more revealing to calculate biases as a function of season as opposed to annually.
You need to improve the model simulation. This will add value to the comparison with observations.
L315-320: CH4 lifetime of 4.89 years is considerably less than range of 7-14. Obviously, your large LNOx source is contributing to this low bias in lifetime.
You need to be careful with generalized statements.
There are numerous reasons why a model may have a high-or-low bias in ozone at the surface. The magnitude of the LNOx source plays only a small role here.
Stratosphere-troposphere exchange is poorly resolved in this model due to its low model top. This may make comparison with mid- and high-latitude ozone profiles problematic.
Minor Comments:
L24: The range you cite here (8 to 4000 moles NO / flash) is for individual flashes. Estimates of the mean production per flash are usually between 125 and 500 moles per flash.
L73: Is 998 hPa the mean surface pressure?
L74: A 200 hPa top layer is when evaluating O3 profiles. What is the pressure of the model top? Clearly, this model was designed for tropospheric chemistry.
L160 and L201: Is this a climatological flash data set from ISS-LIS? If so, what years does it cover?
L192: Are you saying that the modeled tropopause height is too high in the tropics? If yes, please show.
L200: Why are you comparing May-August flash rates with the annual mean?
L207: You need to be clear here. 8.8 Tg N yr-1 for the NH is consistent with ~15 Tg N yr-1 for the globe, a value that is well outside of the 2-8 range but below 25.
L214: Why do you think emissions are underestimated?
L265: Do any of these studies give the NH burden? Or do they just list the total burden?
L269: Are you comparing to climatological ozone sondes or ozone sondes from 2018? You should consider comparing to individual SHADOZ sondes as several of the sites are located in NH.
L279: Stratosphere-troposphere exchange is one cause for the very low biases you are seeing in the extratropics and at high latitudes.
Grammatical Comments:
L19: such as lightning --- such as lightning and soil-NOx emissions
L24: 4000 mol NO per flash --- 4000 mol NO per individual flash
L25: suggest a value of 250 --- suggest a mean value of 250
L42: most frequently used CTH scheme --- the frequently used CTH scheme
L75: for chemical mechanisms --- for the chemical mechanism
L91: deep convection fluxes --- deep convective fluxes
L160: … but ISS-LIS only sees a small subset of total flashes …
L197: inconsistancies --- inconsistencies.
L223: represents a spatial variation --- varies spatially
L225: rest part of NH --- rest of the NH
L233: 10-25 ppbv enhancement of annual mean surface ozone due to lightning –
Figure 3d: 500-200 hPa or 500-300 hPa. Caption is not consistent with figure.

Citation: https://doi.org/10.5194/egusphere-2024-3087-RC1
- AC1: 'Reply on RC1', Sanhita Ghosh, 04 Dec 2024
  
  We sincerely thank the Referee for the constructive feedback and valuable suggestions, which have greatly enhanced the quality of our study.
  We are currently revising the manuscript and have addressed all the points raised by the Referee in detail. With improved configurations for advection, emissions, and boundary conditions, we are confident that these improvements will resolve most of the shortcomings identified. A revised version of the manuscript, along with a point-by-point response to the Referee's comments, will be submitted as soon as we have all the reviews.
  We greatly appreciate the Referee's insights and look forward to receiving further feedback on the revised manuscript.
  
  Citation: https://doi.org/10.5194/egusphere-2024-3087-AC1
RC2: 'Comment on egusphere-2024-3087', Anonymous Referee #2, 19 Dec 2024

I share the concerns of the reviewer who posted a comment on Nov. 19th, so I will not repeat them here.
One additional major concern: The scientific content of the paper is very low; it is not clear to me what new insights were found as a result of this analysis relative to what is already in the scientific literature. Therefore, I recommend that the authors consider publishing their manuscript in Geoscientific Model Development (https://www.geoscientific-model-development.net/) instead of ACP. GMD is meant for description papers of significant model development.

Citation: https://doi.org/10.5194/egusphere-2024-3087-RC2

Peer review completion

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

AR by Sanhita Ghosh on behalf of the Authors (09 Feb 2025) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (10 Feb 2025) by Bryan N. Duncan

RR by Anonymous Referee #1 (19 Feb 2025)

Suggestions for revision or reasons for rejection

Ghosh et al. Representing improved tropospheric ozone distribution by including lightning NOx emissions in CHIMERE.

Summary:
The authors implement a cloud-height based flash rate scheme and an ice-flux based scheme into the regional model CHIMERE and then evaluate the impact of lightning-NOx production on ozone profiles, the tropospheric OH burden, the methane lifetime, and ambient ozone and NO2 concentrations. This version of the paper is much improved but remains unpublishable until the authors explain how the addition of LNOx leads to a decrease in NO2 columns over much of the domain.

Major Comments:
L281: Be specific as to what is improved in this simulation over water versus the original PR92. My hunch is that you obtained a better ocean-simulation because the ratio of a/b you use is smaller than that used in PR92, thus after scaling a higher fraction of flashes are over water lessening the low-bias others have observed with PR92 over water. – Do you agree?

L289-296: I don’t follow your rationale here. Are you saying that more realistic midlatitude flash rates could be produced if cloud heights were allowed to extend above the tropopause? Shouldn’t cloud heights be limited by the tropopause? Yes, overshooting storms exist and do transport trace gases into the stratosphere but aren’t anvils typically limited by the tropopause. Perhaps the heights of tropical storms are too high.

Figure 5: Your scale does not include negatives or is there room for negatives in the point of the arrow? I’m surprised that O3 from LNOx-ICEFLUX exceeds ozone from LNOX-CTH everywhere given the similarity in their total flash rates. Please double check your calculations and also verify that the legend matches what is plotted.

L475-479: I don’t understand how the inclusion of LNOx can lead to a decrease in column NO2 over most of your non-tropical domain. This seems wrong. Please double check your calculations. How do the changes vary seasonally? Do you see increases during the spring and summer? Yes, you can see local decreases especially in the boundary layer over polluted regions but total columns must increase.

Minor Comments:
L88: 20 vertical levels is quite coarse and a 200 hPa model top Is very low.

L125-130: As equation (2) is not used, to avoid confusion, this section could be shorted with the equation removed

L156-157: Why is this distinction made? Why is it important that flashes above the freezing level are considered IC and flashes below it CG?

L170: “Beta” = IC/CG = “formula”

L201-202: Justify why you also include NO2 emissions from lightning.

L260-262 and L341-344: Do you also divide by 5 in the tables? Assuming yes, introduce the factor of 5 in section 2.2.2. Move discussion in 341-344 2.2.2 too. You do apply scaling factors to LNOx-CTH but before the model was run.

L274: where in the United States are you referring to?

L288: “explaining the effectiveness of ICEFLUX scheme over CTH, in capturing flashes over the midlatitudes”. Yes, the mean flash rates from the ICEFLUX scheme appear to be more realistic in the midlatitudes. However, the error statistics you show in Table 3 still favor the CTH scheme. Why is that? Is there a metric for which the ICEFLUX scheme does better in the midlatitudes?

Table 2: Add rows showing corresponding values for ISS-LIS and LIS/OTD.

L304-308: The accuracy of the lightning data is also lower at high latitudes. As the data sets contain fewer years. Also, what fraction of flashes does ISS-LIS capture? Does it only view a given area for a few minutes each day? Data are also lower quality over the oceans due to sampling limitations.

L330: Are these correlations temporal or spatial? Based on the context and values, it appears they are temporal – correlations between monthly average flash rates for each latitude band?

L348: You hint at factors of 2-3 magnitudes but only show factors varying by factors of 2-4. Rephrase or give more details.

L350: Given the 4.9th power of cloud height variation, varying the minimum depth would have little effect.

L354: I’m not sure why you use “but” here. How did Finney determine “better”?

L378: Remind the reader how you determined the vertical partitioning of LNOx emissions. Do these plots sum the contributions from IC and CG flashes? Do you assume only IC flashes for some altitudes and only CG for others etc.
L385: What previous studies are you referring to and are you certain they are plotting mass and not mixing ratio.

L393: “evenly distributed over an altitude range”. This information should be given earlier in the text.

L417-420: Midlatitude and polar region changes vary greatly by season. Thus, it is not surprising that annual mean changes are relatively small. What percent changes are seen in the late spring/summer.

L438: Your model top may be too low to adequately resolve cross-tropopause transport.

L485: What is causing that unobserved peak?

L486: Higher uncertainty in OMI observations relative to what?

L553: How do you determine the CH4 lifetime, i.e., what CH4 distribution do you assume. Yes, a CH4 lifetime of 4.5-4.8 years is quite short and yes your OH must have a considerable high-bias. Your mean concentrations of ~15 x 10^5 are approximately 50% greater than the canonical value of 10 x 10^5 and as you note higher than the multi-model mean of 11 x 10^5.

Grammatical Comments:
L29: uncertainties  uncertainty

L98-99: and fire emissions are taken  and fire emissions and are taken

L193: have reported  used

L200: is close to  are close to

L218: Flash rate  Flash data

L245: observation data  observations

Table 3: parenthesis  parentheses

L296: showed  shown

L335: specially while  especially when

L405: maximum  maximum ozone

L410: even higher increase

L547: usually effected  usually affected

L596: which have  which

Hide

ED: Reconsider after major revisions (19 Feb 2025) by Bryan N. Duncan

AR by Sanhita Ghosh on behalf of the Authors (14 Mar 2025) Author's response Author's tracked changes Manuscript

ED: Referee Nomination & Report Request started (14 Mar 2025) by Bryan N. Duncan

RR by Anonymous Referee #1 (25 Mar 2025)

ED: Publish subject to minor revisions (review by editor) (25 Mar 2025) by Bryan N. Duncan

AR by Sanhita Ghosh on behalf of the Authors (31 Mar 2025) Author's response Author's tracked changes Manuscript

ED: Publish as is (01 Apr 2025) by Bryan N. Duncan

AR by Sanhita Ghosh on behalf of the Authors (04 Apr 2025) Manuscript

Journal article(s) based on this preprint

26 Jun 2025

Representing improved tropospheric ozone distribution over the Northern Hemisphere by including lightning NO_x emissions in CHIMERE

Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut

Atmos. Chem. Phys., 25, 6273–6297, https://doi.org/10.5194/acp-25-6273-2025,https://doi.org/10.5194/acp-25-6273-2025, 2025

Short summary

Sanhita Ghosh, Arineh Cholakian, Sylvain Mailler, and Laurent Menut

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In the study, we estimate the emissions of nitrogen oxides from lightning (LNOx) over the northern hemisphere and study its impact on tropospheric ozone (O₃). We evaluate the present state of modelling the lightning, using a classical parametrization scheme and the model CHIMERE. The comparison of the simulated O₃ to measurements shows that the inclusion of LNOx emissions remarkably improves the tropospheric O₃ distribution, reducing the bias significantly, particularly in the free troposphere.


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