the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Interpreting Summertime Hourly Variation of NO2 Columns with Implications for Geostationary Satellite Applications
Abstract. Accurate representation of the hourly variation of the NO2 column-to-surface relationship is needed to interpret geostationary constellation observations of tropospheric NO2 columns. Prior work has revealed inconsistency in the hourly variation in NO2 columns and surface concentrations. In this study, we use the high-performance configuration of the GEOS-Chem model (GCHP) to interpret the daytime hourly variation in NO2 total columns and surface concentrations during summer. We use summer-time Pandora sun photometers and aircraft measurements during the Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field campaign over Maryland, Texas, and Colorado as well as 50 sites (31: contiguous USA, 10: Europe, 9: Asia) from the Pandonia Global Network (PGN). We correct the Pandora columns for 1) hourly variation in the column effective temperature driven by the fractional boundary layer contribution to the total column, and 2) change in local solar time along the line-of-sight of the Pandora instrument. The corrected Pandora observations are increased by about 5–6 × 1014 molecules cm-2 at 9 AM and 6 PM across all Pandora sites. We conduct fine resolution (~12 km) simulations over the contiguous US, Europe, and East Asia using the stretched grid capability of GCHP. We also examine the effect of planetary boundary layer height (PBLH) corrections on the total columns. We first evaluate the GCHP simulated absolute NO2 concentration with Pandora and aircraft observations. We find that fine resolution simulations at 12 km compared with moderate resolution ~55 km reduce the Normalized Bias (NB) versus Pandora total columns (19 % to 10 %) and versus aircraft measurements (25 % to 13 %) over Maryland, Texas, and Colorado. Fine resolution simulations at 12 km compared with moderate resolution at 55 km reduce the NB versus Pandora total columns over the eastern US (17 % to 9 %), western US (22 % to 14 %), Europe (24 % to 15 %), and Asia (29 % to 21 %). We next use the 12 km simulation to examine the hourly variation in the NO2 column and surface concentrations. We explain the weaker hourly variation in NO2 columns than at the surface as a function of 1) hourly variation in the column effective temperature, 2) hourly variation in the local solar time along the Pandora line-of-sight and 3) the integral of weakly connected layers; with the lowest 500 m exhibiting greater NO2 concentrations in morning and evening than midday, while the residual column above 500 m dominates the total column with weaker variability.
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Notice on discussion status
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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Preprint
(2260 KB)
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
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- Final revised paper
Journal article(s) based on this preprint
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2024-1401', Anonymous Referee #1, 29 May 2024
The study investigates the diurnal variation of the NO2 column-to-surface-concentration relationships using observations and corresponding model simulations from three DISCOVER-AQ campaigns and worldwide Pandora NO2 total column measurements. The authors correct the Pandora measurements by considering biases in effective temperature and local solar timing along the line-of-sight used in Pandora retrieval. Regarding model simulations, the manuscript compares two simulations with different horizontal resolutions (12 vs. 55 km) to evaluate the impact of horizontal resolution on model performance in reproducing observed NO2 surface concentrations and columns. The authors demonstrate that NO2 above 500 m has weak temporal variability but dominates total NO2 columns, dampening the variation of total NO2 columns, although NO2 below 500 m shows apparent diurnal variation. The results are interesting and useful to the community. However, I have two major concerns about the quality of the manuscript.
Major comments:
1 Section 3.5 is entirely based on model results. However, Figures 4 and 5 show that the model simulation results differ from the Pandora measurements in the diurnal variations of NO2 total columns even if the Pandora measurements have been slightly corrected. Are you assuming the model is correct? If so, can you explain why Pandora shows weaker diurnal variations than model results? According to the model results, even if NO2 below 500 m contributes less than 50% to total NO2 columns, we should still observe apparent diurnal variations in NO2 columns (Figures 4 and 5). Why doesn’t it occur in Pandora measurements? On the other hand, if you assume Pandora is correct, how can Section 3.5 convince the community, considering that it is based on model results different from observations?
2 Mostly, I can understand what the authors want to say. However, I suggest further improvement of the language of the manuscript. Please find below for further details.
Minor comments:
Line 22: “campaign” to “campaigns”
Line 24: “Pandora columns” to “Pandora NO2 columns”? In addition, do you refer to vertical columns or slant columns? Please use accurate terms.
Line 25-26: Please rewrite the second part of the sentence. I understand what you want to say, but the sentence needs to be clarified.
Line 26: Again, what are the Pandora observations? NO2 vertical columns? Tropospheric or total?
Line 31: “versus” to “against” and delete the second “versus”.
Line 37: “at the surface” to “NO2 surface concentrations”?
Line 39: What do you mean by the integral of weakly connected layers? The sentence following it? Please rewrite the sentence which is too long.
Line 48: Add “spatial” before “gaps”.
Figure A1 (Line 670): Add the period of the DISCOVER-AQ Colorado campaign.
Line 136-137: Please rewrite the sentence.
Lines 145-147: Doesn’t it depend on the accuracy of the stratospheric NO2 vertical columns?
Line 161: Write down the full name of VOC at its first appearance.
Line 200-202: Please rewrite the sentence and explain Equation (1).
Line 209: Add a period after “photometer”.
Figure 2. The observational lines are messed up. Does different coloring make the figures clearer?
Line 236: How did you calculate normalized biases?
Line 241: What do you mean by left panel?
Lines 254-256: Please explain it.
Equation 2: Why did you multiply 0.2? How did you determine this value?
Lines 278-282: I wonder whether comparing the total NO2 columns in the left panel to partial NO2 columns between 300 m and 4 km in the right panel is correct, although it seems the NO2 columns between 300 m and 4 km dominate the NO2 total columns. In addition, is the left panel of Figure 4 for DISCOVER-AQ Pandora or PGN Pandora?
Line 282-287: I think you have applied the correction to the corrected Pandora NO2 total columns. If so, how much does it affect the NO2 total columns?
Line 348-349: Please rewrite this sentence.
Line 397: Does the PBLH modification increase NBs?
Line 403: Add “total” before “NO2”?
Line 408: “versus” to “against”.
Citation: https://doi.org/10.5194/egusphere-2024-1401-RC1 -
AC1: 'Reply on RC1', Deepangsu Chatterjee, 09 Aug 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1401/egusphere-2024-1401-AC1-supplement.pdf
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AC1: 'Reply on RC1', Deepangsu Chatterjee, 09 Aug 2024
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RC2: 'Comment on egusphere-2024-1401', Anonymous Referee #2, 09 Jul 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1401/egusphere-2024-1401-RC2-supplement.pdf
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AC2: 'Reply on RC2', Deepangsu Chatterjee, 09 Aug 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1401/egusphere-2024-1401-AC2-supplement.pdf
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AC2: 'Reply on RC2', Deepangsu Chatterjee, 09 Aug 2024
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2024-1401', Anonymous Referee #1, 29 May 2024
The study investigates the diurnal variation of the NO2 column-to-surface-concentration relationships using observations and corresponding model simulations from three DISCOVER-AQ campaigns and worldwide Pandora NO2 total column measurements. The authors correct the Pandora measurements by considering biases in effective temperature and local solar timing along the line-of-sight used in Pandora retrieval. Regarding model simulations, the manuscript compares two simulations with different horizontal resolutions (12 vs. 55 km) to evaluate the impact of horizontal resolution on model performance in reproducing observed NO2 surface concentrations and columns. The authors demonstrate that NO2 above 500 m has weak temporal variability but dominates total NO2 columns, dampening the variation of total NO2 columns, although NO2 below 500 m shows apparent diurnal variation. The results are interesting and useful to the community. However, I have two major concerns about the quality of the manuscript.
Major comments:
1 Section 3.5 is entirely based on model results. However, Figures 4 and 5 show that the model simulation results differ from the Pandora measurements in the diurnal variations of NO2 total columns even if the Pandora measurements have been slightly corrected. Are you assuming the model is correct? If so, can you explain why Pandora shows weaker diurnal variations than model results? According to the model results, even if NO2 below 500 m contributes less than 50% to total NO2 columns, we should still observe apparent diurnal variations in NO2 columns (Figures 4 and 5). Why doesn’t it occur in Pandora measurements? On the other hand, if you assume Pandora is correct, how can Section 3.5 convince the community, considering that it is based on model results different from observations?
2 Mostly, I can understand what the authors want to say. However, I suggest further improvement of the language of the manuscript. Please find below for further details.
Minor comments:
Line 22: “campaign” to “campaigns”
Line 24: “Pandora columns” to “Pandora NO2 columns”? In addition, do you refer to vertical columns or slant columns? Please use accurate terms.
Line 25-26: Please rewrite the second part of the sentence. I understand what you want to say, but the sentence needs to be clarified.
Line 26: Again, what are the Pandora observations? NO2 vertical columns? Tropospheric or total?
Line 31: “versus” to “against” and delete the second “versus”.
Line 37: “at the surface” to “NO2 surface concentrations”?
Line 39: What do you mean by the integral of weakly connected layers? The sentence following it? Please rewrite the sentence which is too long.
Line 48: Add “spatial” before “gaps”.
Figure A1 (Line 670): Add the period of the DISCOVER-AQ Colorado campaign.
Line 136-137: Please rewrite the sentence.
Lines 145-147: Doesn’t it depend on the accuracy of the stratospheric NO2 vertical columns?
Line 161: Write down the full name of VOC at its first appearance.
Line 200-202: Please rewrite the sentence and explain Equation (1).
Line 209: Add a period after “photometer”.
Figure 2. The observational lines are messed up. Does different coloring make the figures clearer?
Line 236: How did you calculate normalized biases?
Line 241: What do you mean by left panel?
Lines 254-256: Please explain it.
Equation 2: Why did you multiply 0.2? How did you determine this value?
Lines 278-282: I wonder whether comparing the total NO2 columns in the left panel to partial NO2 columns between 300 m and 4 km in the right panel is correct, although it seems the NO2 columns between 300 m and 4 km dominate the NO2 total columns. In addition, is the left panel of Figure 4 for DISCOVER-AQ Pandora or PGN Pandora?
Line 282-287: I think you have applied the correction to the corrected Pandora NO2 total columns. If so, how much does it affect the NO2 total columns?
Line 348-349: Please rewrite this sentence.
Line 397: Does the PBLH modification increase NBs?
Line 403: Add “total” before “NO2”?
Line 408: “versus” to “against”.
Citation: https://doi.org/10.5194/egusphere-2024-1401-RC1 -
AC1: 'Reply on RC1', Deepangsu Chatterjee, 09 Aug 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1401/egusphere-2024-1401-AC1-supplement.pdf
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AC1: 'Reply on RC1', Deepangsu Chatterjee, 09 Aug 2024
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RC2: 'Comment on egusphere-2024-1401', Anonymous Referee #2, 09 Jul 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1401/egusphere-2024-1401-RC2-supplement.pdf
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AC2: 'Reply on RC2', Deepangsu Chatterjee, 09 Aug 2024
The comment was uploaded in the form of a supplement: https://egusphere.copernicus.org/preprints/2024/egusphere-2024-1401/egusphere-2024-1401-AC2-supplement.pdf
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AC2: 'Reply on RC2', Deepangsu Chatterjee, 09 Aug 2024
Peer review completion
Journal article(s) based on this preprint
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Deepangsu Chatterjee
Randall V. Martin
Dandan Zhang
Haihui Zhu
Daven K. Henze
James H. Crawford
Ronald C. Cohen
Lok N. Lamsal
Alexander M. Cede
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(2260 KB) - Metadata XML