Simulation of Turbulent Mixing Effects on Essential NOx–O3–Hydrocarbon Photochemistry in Convective Boundary Layer
Round 1
Reviewer 1 Report
Please, try to put ONE word by ONE in your keywords.
Please, what is the originality of your work ? Put a section at the end of your introduction to show us the originality of your work.
Please, define each term in your EQUATIONS.
Please, you have to reduce the number of your figures.
You have to reduce you conclusion
Author Response
Response of Reviewer 1 Comment:
Please, try to put ONE word by ONE in your keywords.
Turbulent; kinetics; Mixing; Segregation; Photochemistry; CBL
Please, what is the originality of your work ? Put a section at the end of your introduction to show us the originality of your work.
In the end of introduction, following sentences are added:
“The present study has an originality to develop the computational turbulent kinetic model (TKM) for expressing nonlinear kinetics and dynamics of chemicals in heterogeneous systems. For validating TKM applicability, model simulations run for essential NOx-O3-RH photochemistry in a convective boundary layer (CBL).” The present study uses the turbulent kinetics model (TKM) [10] .....
Please, define each term in your EQUATIONS.
For understanding, all equations including equations summarized in Table 2(Table 2 is deleted) have been rearranged in text with expression of each term. (refer to Section 2.2)
Please, you have to reduce the number of your figures.
The number of figures are reduced from 9 to 8. Figure 5 becomes Figure 5(a) and Figure 6 becomes Figure 5(b).
You have to reduce you conclusion
Conclusion is reduced and rearranged as below:
The TKM successfully incorporates the “essential” chemical system using a generic hydrocarbon, RH, in conjunction with NOx and O3 for a typical rural agricultural regional atmosphere with RH having the same reactivity with OH as isoprene. The transport scheme in the TKM assures that significant concentration gradients exist only near the upper and lower boundaries of the CBL. Emissions of NO and RH and dry deposition of species cause gradients near the surface. Turbulence represented in the TKM produces significant segregation in the three reaction pairs among eleven reactions NO + O3, NO + HO2, and RH + OH for times up to 200 minutes. As represented in the TKM, turbulence in the CBL allows for build-up of significantly higher concentrations of NO, NO2 and RH, while preventing the increase in O3 concentrations compared to the CKM, in which the reactions proceed with no segregation due to turbulence. The similarity between the CKM results and those of the simple box model (BM) are nearly identical. This provides justification for the application of box model chemistry to represent the behavior of the boundary layer when turbulence effects are not included. However, the present study with the TKM indicates that turbulence effects should not be ignored in the convective boundary layer. Comparisons of the TKM with LES results are difficult because of differences in model structure and parameterizations. The LES gives lower coefficients of segregation for the principal reactions, thus representing a relatively small role of turbulence in affecting reaction rates. The TKM produces results similar to the LES for an increased molecular time scale, or equivalently, a decreased turbulent time scale. The sensitivity analysis, in which several model parameters and boundary conditions were varied, revealed less than linear changes in concentrations of the major species from changes in RH and NO emission rates. Lower emission rates lead to lower segregation effects in the principal reactions involving RH, NO, and NO2. The concentrations of the intermediate radicals OH and HO2 are more sensitive to the variations than the more stable and abundant species. However, changing the chemical mechanism from the “essential chemistry” to CB-4 leads to relatively small changes in species concentrations and reaction segregations. Finally, it would be desirable to have a set of high resolution time-concentration data of the key species in the CBL to provide critical
Reviewer 2 Report
The English is a little bit patchy, as if some sections have been sub-edited and others not.
Some typos:-
- Title: Hydorcarbon?
- Table 4 is missing.
- The SI abbreviation of second is s not sec.
- L155. Surely R9 rather than R6?
- References 3-4 (Vinuesa), 10, 24,33
I can work out which direction the systems evolve in in Figure 8, but it might be helpful to mark the starting ends of the various trajectories.
Section 4.1 could perhaps be a little bit clearer. The 'inert' species calculation is for the same old species but taking account only of their dispersion and not of the chemical reactions between them.
LIkewise in Section 4.3 my understanding is that turbulence should speed up the rate of chemical reaction - after all, if there were no turbulent mixing the rate of chemical reaction (through molecular diffusion) would be extremely slow. Clearly, however, if the timescale for chemical reaction is faster than that for turbulent mixing then the mixing layer will remain inhomogeneous. It seems to me misleading so say that turbulence has a retarding effect: if turbulence was faster, there would be less segregation.
Author Response
Response of Reviewer 2’ comments
The English is a little bit patchy, as if some sections have been sub-edited and others not.
Some typos:-
- Title: Hydorcarbon?
“Hydorcarbon” is modified to “Hydrocarbon.”
- Table 4 is missing.
Table 4 is added and Table 4 is marked to Table 3.
- The SI abbreviation of second is s not sec.
Unit “sec” is changed to “s.”
- L155. Surely R9 rather than R6?
R6 is modified to R9.
- References 3-4 (Vinuesa), 10, 24,33
References 3-4 (Vinuesa) is modified as below:
Molemaker, M. J., Arellano J. V.-G. d. Control of chemical reactions by convective turbulence in the boundary layer, Journal of the Atmospheric Sciences 1998, 55, 568-579.
3. Vinuesa, J.-F., Arellano, J. V.-G. d. Introducing effective reaction rates to account for the inefficient mixing of the convective boundary layer. Atmospheric Environment 2005, 39, 445-461.
4. Fraigneau, Y., Gonzalez, M., Coppalle, A. The influence of turbulence upon the chemical reaction of nitric oxide released from a ground source into ambient ozone, Atmospheric Environment 1996, 30(9), 1467-1480.
“[10], [24], and [33]” in references 10,24, and 33 are removed.
I can work out which direction the systems evolve in in Figure 8, but it might be helpful to mark the starting ends of the various trajectories.
Red circles are added in Figure 8 and “Red circles mark starting points of the various trajectories” is added in the title of Figure 8.
Section 4.1 could perhaps be a little bit clearer. The 'inert' species calculation is for the same old species but taking account only of their dispersion and not of the chemical reactions between them.
According to reviewer’s suggestion, Section 4.1 includes the following sentence:
(The reader is reminded that the term “inert” as used here refers to a model pseudospecies and not to real unreactive substances. The 'inert' species calculation is for the same species but taking account only of their dispersion and not of the chemical reactions between them.)
Likewise in Section 4.3 my understanding is that turbulence should speed up the rate of chemical reaction - after all, if there were no turbulent mixing the rate of chemical reaction (through molecular diffusion) would be extremely slow. Clearly, however, if the timescale for chemical reaction is faster than that for turbulent mixing then the mixing layer will remain inhomogeneous. It seems to me misleading so say that turbulence has a retarding effect: if turbulence was faster, there would be less segregation.
As mentioned in the introduction part, the turbulent mixing effect on the chemical reaction rate can expressed as a function of the intensity of segregation Is (when Is = -1 for the complete segregation between the species in the strong turbulent flow ( ), chemical reaction rate is ignored and if Is = 0 for the perfectly mixed species by the turbulence (), the mean chemical reaction rate is considered. However, when Is > 0 for the enhanced () or Is < 0 lowered reaction rate compared to the perfectly mixed case (), the effective reaction rate is considered effect of segregation intensity Is). Thus, the sentence is changed as below:
“When the chemical reaction timescale is of similar magnitude to or smaller than the turbulence timescale (), segregation of reactants becomes significant (Is > 0 or Is < 0) thus the reaction rate enhances or retards”.
Author Response File: 
Author Response.pdf
Reviewer 3 Report
General comments:
This manuscript introduced a 1-D turbulent kinetics model (TKM) and a set of simplified photochemical reactions to simulate the effects of turbulence on the reaction rates and distribution of important species for ozone chemistry in the CBL. The modeling result has been compared with a box model, a conventional kinetics model, and the LES model (Krol et al., 2000). In addition, this study conducted a series of sensitivity analysis of the 1-D TKM to show the effects of variations in important input parameters to the model results, such as NO and VOC emission rates, turbulent time scale, reaction rate constants, dry deposition velocity, exchange velocity, and initial concentrations of species. The current manuscript closely followed the contents of Krol et al. (2000) with the same simplified ozone photochemistry reactions and the quite similar arrangements of sensitivity studies but with a 1-D TKM simulation. Also, the manuscript heavily refers to the reference that the author published in a Korean scientific journal without English online access (Kim, M.-S., 2017) for the methodology details. The current version of simulation results section is loose with only focusing only on simulation results description but no clear analysis of scientific implications. With the successful implementation of 3D regional air quality model for ozone modeling under much complex boundary layer flow conditions and much detailed photochemistry simulation than this study during at least the last 10-15 years, I cannot see much contribution of this study to the current scientific understanding on this topic. Nevertheless, I feel the manuscript may be publishable under revisions to tide up the English writing and strengthen the section of results discussion section, more importantly, the author needs to point out what the originality of this study and the advantage of using this approach. Please also see my detail comments below.
Specific comments:
Page 1, Line 13. The symbol “Is” for separation intensity is confusing here. Either mention it later (e.g. Line 53) or change the font to Itatic.
Page 1, Line 16. “Kim’s study [10]”, is the right formation for citation in this journal since it first appears in the manuscript. Also, if it possible, I would avoid citing any reference in the abstract section.
Page 1, Line 23. define “LES” as Large Eddy Simulation first.
Page 2, Line 49-50. Consider “slow” to “extremely slow” in order to be consistent with the Dt <<1 notation.
Page 2, Line 55-61. Need to first notice the symbols A and B represent two reactants.
Page 2, Line 74-75. The description is not rigorous here. See the link https://www.epa.gov/ground-level-ozone-pollution/table-historical-ozone-national-ambient-air-quality-standards-naaqs
Page 2, Line 86 and Line 90. CBL in Line 86 has been defined in Line 82. Convective boundary layer in Line 90 can use the abbreviation.
Page 3, Line 94. Define ABL first, also please go through the whole manuscript to make sure all the abbreviations have been defined properly before usage and no need to re-define in the latter when using them. e.g. Line 105, define HC first.
Page 4. Table 1. The sub-notation for b and c is in reverse order, e.g. b should be for J1 and c should be for CB-IV.
Page 6, Line 197. “… and i is the species A and B”, why I see the Eq (2) and (3) the subscript for concentration is l instead of i?
Page 6-7, Table 2. I personally feel odd to see the equations summarized in the form of Table without clarifications of each term in the equations; the equation names are also vague without clarifications, e.g. “CRR”, “VT”, “MGP” … I suggest to move the description of the 1-D TKM model governing equations into supplemental and do NOT use the form of a table with a clear description of each one.
Page 8, Line 261. Where is Table 4?
Page 8. Table 3. I recommend moving the content of Table 3 into supplemental. Also, about the content in Table 3, (1) the reference Jacob and Wofsy (1988) should be [35]. (2) the abbreviation “FA” definition only appeared in the caption of Figure 1. Clarify here before using it.
Page 10, Line 302. Figure 3 has the vertical profile evolutions from 10 to 200 minutes.
Page 10, Line 309-310. You have 64 vertical grids evenly distributed in 1000 m, how you allocate “surface, middle and top layers of the model” for that 64 layers? Also, for Figure 4, the time evolution for each species at SL, ML, and TL is the arithmetic mean of each layer’s concentration at the three groups?
Page 11, Figure 3 and Figure 4. Please revise the caption of the two figures to make it detailed enough for self-explanatory for the key parameters in all the subplots.
Page 12, Line 320-357. Notice that due to the nonlinearity of ozone chemistry, the concentration evolution will be totally different depending on the model initial setting for NOx and VOC concentration (and the OH level).
Page 16, Figure 8. Please adjust the symbol for your plotting. The color symbol for the case “TKM #3” make it looks wired. Also, the title for Figure 8(b), mixed layer or middle layer?
Page 21, Ling 591-594. The numbering is not in order, notice #3 include two references (Molemaker et al., and Vinuesa et al.), please correct.
Page 21, Line 610-612. The Kim et al. reference. (1) please correct the format. (2) is this reference published in Korean and provide English abstract? Need to mark down as “(in Korean)”.
Reference:
Kim, M.-S. Turbulent chemical kinetics model (TKM): A study of turbulent mixing effects on simple NOx-O3 photochemistry in Convective Boundary Layer, J. of Korean Society of Environmental Technology 2017, 611 18(2), 86-102.
Krol, M. C., Molemaker, M. J. Effects of turbulence and heterogeneous emissions on photochemically active species in the convective boundary layer, Journal of Geophysical Research 2000, 105(D5), 6871-6884.
Author Response
Response of Reviewer 3’ Comments
General comments:
This manuscript introduced a 1-D turbulent kinetics model (TKM) and a set of simplified photochemical reactions to simulate the effects of turbulence on the reaction rates and distribution of important species for ozone chemistry in the CBL. The modeling result has been compared with a box model, a conventional kinetics model, and the LES model (Krol et al., 2000). In addition, this study conducted a series of sensitivity analysis of the 1-D TKM to show the effects of variations in important input parameters to the model results, such as NO and VOC emission rates, turbulent time scale, reaction rate constants, dry deposition velocity, exchange velocity, and initial concentrations of species. The current manuscript closely followed the contents of Krol et al. (2000) with the same simplified ozone photochemistry reactions and the quite similar arrangements of sensitivity studies but with a 1-D TKM simulation. Also, the manuscript heavily refers to the reference that the author published in a Korean scientific journal without English online access (Kim, M.-S., 2017) for the methodology details. The current version of simulation results section is loose with only focusing only on simulation results description but no clear analysis of scientific implications. With the successful implementation of 3D regional air quality model for ozone modeling under much complex boundary layer flow conditions and much detailed photochemistry simulation than this study during at least the last 10-15 years, I cannot see much contribution of this study to the current scientific understanding on this topic. Nevertheless, I feel the manuscript may be publishable under revisions to tide up the English writing and strengthen the section of results discussion section, more importantly, the author needs to point out what the originality of this study and the advantage of using this approach. Please also see my detail comments below.
Specific comments:
Page 1, Line 13. The symbol “Is” for separation intensity is confusing here. Either mention it later (e.g. Line 53) or change the font to Itatic.
The symbol “Is” for separation intensity is changed the font to Italic. Is to Is
Page 1, Line 16. “Kim’s study [10]”, is the right formation for citation in this journal since it first appears in the manuscript. Also, if it possible, I would avoid citing any reference in the abstract section.
According to the reviewer’s suggestion, I deleted “Kim’s study [10]” from the sentence as follow:
From “Modeling approach follows Kim’s study [10] for all species except OH with an assumption of photostationary steady state” to “Modeling approach applies for all species except OH with an assumption of photostationary steady state.”
Page 1, Line 23. define “LES” as Large Eddy Simulation first.
“LES simulation” is changed to “Large Eddy simulation (LES).”
Page 2, Line 49-50. Consider “slow” to “extremely slow” in order to be consistent with the Dt <<1 notation.
“Slow” is changed to “extremely slow”.
Page 2, Line 55-61. Need to first notice the symbols A and B represent two reactants.
The sentence is modified to “it can be related to the concentration fluctuation and the mean concentrations and of the reactive species A and B.”
Page 2, Line 74-75. The description is not rigorous here. See the link https://www.epa.gov/ground-level-ozone-pollution/table-historical-ozone-national-ambient-air-quality-standards-naaqs
The description is changed:
In those areas maximum ozone concentrations during the summer exceeded the O3 national ambient air quality standard (NAAQS) of 70 ppb finalized by USEPA in 2015. Ozone studies have led to recognition that realistic representations of turbulent mixing processes are very important for air quality simulation.
Page 2, Line 86 and Line 90. CBL in Line 86 has been defined in Line 82. Convective boundary layer in Line 90 can use the abbreviation.
“Convective boundary layer” in Line 86 and Line 90 is changed to “CBL.”
Page 3, Line 94. Define ABL first, also please go through the whole manuscript to make sure all the abbreviations have been defined properly before usage and no need to re-define in the latter when using them. e.g. Line 105, define HC first.
“ABL” in Line 94 is changed to Atmospheric Boundary Layer (ABL).
NO and HC in Line 105 are changed to Nitric Oxide (NO) and Hydrocarbon (HC or RH).
Page 4. Table 1. The sub-notation for b and c is in reverse order, e.g. b should be for J1 and c should be for CB-IV.
The superscription for b and c is changed to b for J1 and c for CB-IV.
Page 6, Line 197. “… and i is the species A and B”, why I see the Eq (2) and (3) the subscript for concentration is l instead of i?
The subscripts for concentration in Eq(2) and(3) are modified from I to i.
→
→
Page 6-7, Table 2. I personally feel odd to see the equations summarized in the form of Table without clarifications of each term in the equations; the equation names are also vague without clarifications, e.g. “CRR”, “VT”, “MGP” … I suggest to move the description of the 1-D TKM model governing equations into supplemental and do NOT use the form of a table with a clear description of each one.
Table 2 is deleted and the equations are described in text. (refer to section 2.2)
2.2. Model Equations
…
Also, a concept of a local phenomenal extent reaction ξ incorporates both stoichiometry and diffusion effects simultaneously in space and time. To reduce the number of partial differential equations needed to describe the evolution of multimolecular systems in the turbulent (incompletely mixed) field, the stoichiometric relations are combined with the concept of inert surrogate concentrations (see [30-31, 10] for details). Therefore, the mean concentration of the reactive species A and B,, can be calculated using the inert surrogate mean concentration, , and the phenomenal extent of reaction ξ in space and time (): and for two reactants and for product P.
The governing equations of variables in the TKM for inert species, for reactive species, and for phenomenal extent of reaction ξ are time-dependent, nonlinear, and coupled partial differential equations, which are expressed in a fixed Eulerian framework as given below (see [10] for details):
(2)
(3)
(3)’
I II III
where, term I is the local rate of change of the variables, term II is the vertical turbulent flux transport, term III is the source and sink term, and i is the species A and B. The source term in term III is, where E(ppb m s-1) is the emission flux of species A at the surface level Δz, or it is the entrained flux of species B at the top level Δz. The effective reaction rate, (ppb s-1) for sink term in term III, is calculated for the mean phenomenal extents of reaction based on the CSM (see 2.3 for details). In this study, the mean concentration of reactive species is calculated using the inert surrogate mean concentration and the phenomenal extent of reaction instead of using eq (3): for reactants and for products. The governing equations of variables in the TKM are solved by forward finite difference methods (FFDM). For the numerical integration of μi and μj, and , with the current time step m and the next time step m+1, and the time difference Δt between m and m+1. These are summarized in Table 2.
2.3. Model Approaches
The major governing equations solved in the TKM, listed in Table 2, are the same as those described in the previous study [10]. The symbols and subscripts have, in general, the same meanings, but now the subscript i denotes species NO, O3, NO2, RH, HO2, and OH, and subscript j denotes the partner of species i for chemical reactions detailed in Table 1 (e.g., for NO in a reaction, R3, i = NO and j = O3). Similarly, the source, sink, and reaction rate terms are formulated to account for surface sources of NO and RH, dry deposition removal of species, entrainment of species from the free troposphere above the CBL, and the reactions listed in Table 1. The overall effective reaction rate (ppbv s-1) for species i is
(4)
where Rk represents an individual reaction and subscript k denotes reaction number in Table 1 for all reactions of species involving species i. For example, the overall effective reaction rate of the species NO is
(5)
The individual reaction Rk between species i and j is expressed in terms of the segregation coefficient as
or (6)
or
(7)
where is the intensity of segregation for inert species , µi and µj are the mixing parameters, with and with , and is the reaction parameter as below:
or
where D is the molecular diffusivity of species i and j (m2 s-1) [D = Di = Dj], Id is the turbulent dissipative scale length (m), and are the concentration variances of inert species i and j, and is the concentration covariance of inert species i and j.
The concentration variance and concentration covariance of inert species i and j are expressed by eq (8) and (9), respectively.
(8)
(9)
I II III IV
where, term I is the local rate of change, term II is the vertical turbulent flux transport processes, term III is the mean gradient production processes, and term IV is the molecular dissipation of the mean concentration variance and covariance for inert species i and j and of the mean concentration covariance for reactive species i and j [ppb2 s-1] (refer to [10] for details).
Page 8, Line 261. Where is Table 4?
The missing table 4 is added and Table 4 is changed to Table 3 and Table 3 is changed to Table 2 since Table 2 has been deleted.
Table 3. Description of Models for simulating Model Problems: BMch (Photochemical Box Model with chemistry only), BM (Box Model with chemical and physical processes), CKM (Conventional Kinetics Model with mean reaction rate and ACM), and TKM (Turbulent Kinetics Model with concentration fluctuation using conventional extent of reaction and ACM.
Model | BMch | BM | CKM | TKM |
Conditions | All same conditions described in table 2 (no emission source in BMch; only depending upon initial concentrations and photochemistry of species) | |||
Deposition term | No | Concentration in BM | Concentration at lowest model layer (surface layer) | |
Vertical Diffusion term | No | No | Asymmetric Convective Model (ACM): vertical mixing scheme | |
Chemical Kinetics term : for Irreversible Reaction
| Mean reaction rate
| Effective reaction rate Using Concentration Splitting Method (CSM) with segregation coefficient Is,AB in eq(4) | ||
Page 8. Table 3. I recommend moving the content of Table 3 into supplemental. Also, about the content in Table 3, (1) the reference Jacob and Wofsy (1988) should be [35]. (2) the abbreviation “FA” definition only appeared in the caption of Figure 1. Clarify here before using it.
Table 3 is changed to Table 2. In Table 2, two things are changed: (1) the reference “Jacob and Wofsy (1988)” is changed to “[35]” and (2) the abbreviation “FA” is changed to “free atmosphere (FA)”.
Page 10, Line 302. Figure 3 has the vertical profile evolutions from 10 to 200 minutes.
“60” in Line 302 is fixed to “200”
Page 10, Line 309-310. You have 64 vertical grids evenly distributed in 1000 m, how you allocate “surface, middle and top layers of the model” for that 64 layers? Also, for Figure 4, the time evolution for each species at SL, ML, and TL is the arithmetic mean of each layer’s concentration at the three groups?
In Appendix, there is the vertical coordinate system associated with height (z).
The vertical coordinate system is associated with height, z, and it can be defined using Ma, the column mass density of air (kg m-2), as where, is the average air density () and Δz is the difference between the height. Using the hydrostatic relation, , the average air density is related to the height and the pressure or .The air density in the layer can be expressed as . Since the height of each layer can be determined as using for uniform vertical grid space of model layer when the surface height , the boundary layer height , and the veritical grid .
According to the reviewer’s suggestion, title of Figure 4 is modified as below:
Figure 4. Temporal behaviors of the highest concentrations of reactive species for 200 minutes at the surface layer (SL) [z ≤ 100 m], in the middle layer (ML) [100 < z < 900 m], and at the top layer (TL) [z ≥ 900m] of 64 uniform vertical grids in zi = 1000 m. Simulation designed with emission fluxes for reactive species (a) NO and (d) RH and no emission fluxes for other reactive species (b) O3, (c) NO2, (e) HO2, (f) OH, (g) HNO3, and (h) H2O2 at the surface layer, with flux exchanges between CBL and FA for all reactive species, and with no deposition velocity for the end-product species (g) HNO3 and (h) H2O2.
Page 11, Figure 3 and Figure 4. Please revise the caption of the two figures to make it detailed enough for self-explanatory for the key parameters in all the subplots.
The caption of the two figures are revised as below:
Figure 3. Vertical distribution of concentrations for reactive species at 10, 20, 30, 60, 120, and 200 minutes. Simulation designed with emission fluxes for reactive species (a) NO and (d) RH and no emission fluxes for other reactive species (b) O3, (c) NO2, (e) HO2 and (f) OH at the surface layer and with flux exchanges between CBL and FA for all reactive species.
Figure 4. Temporal behaviors of the highest concentrations of reactive species for 200 minutes at the surface layer (SL) [z ≤ 100 m], in the middle layer (ML) [100 < z < 900 m], and at the top layer (TL) [z ≥ 900m] of 64 uniform vertical grids in zi = 1000 m. Simulation designed with emission fluxes for reactive species (a) NO and (d) RH and no emission fluxes for other reactive species (b) O3, (c) NO2, (e) HO2, (f) OH, (g) HNO3, and (h) H2O2 at the surface layer, with flux exchanges between CBL and FA for all reactive species, and with no deposition velocity for the end-product species (g) HNO3 and (h) H2O2.
Page 12, Line 320-357. Notice that due to the nonlinearity of ozone chemistry, the concentration evolution will be totally different depending on the model initial setting for NOx and VOC concentration (and the OH level).
You are right. It depends on the simulation design. Line 320-357 explain only results run for simulation conditions of this study.
Page 16, Figure 8. Please adjust the symbol for your plotting. The color symbol for the case “TKM #3” make it looks wired. Also, the title for Figure 8(b), mixed layer or middle layer?
The title for Figure 8(b) is changed from mixed layer to middle layer. I would like to keep the color symbol for the case “TKM #3”. Red circles are marked for starting points of the various trajectories.
Page 21, Ling 591-594. The numbering is not in order, notice #3 include two references (Molemaker et al., and Vinuesa et al.), please correct.
References 3-4 (Vinuesa) is modified as below:
Molemaker, M. J., Arellano J. V.-G. d. Control of chemical reactions by convective turbulence in the boundary layer, Journal of the Atmospheric Sciences 1998, 55, 568-579.
3. Vinuesa, J.-F., Arellano, J. V.-G. d. Introducing effective reaction rates to account for the inefficient mixing of the convective boundary layer. Atmospheric Environment 2005, 39, 445-461.
4. Fraigneau, Y., Gonzalez, M., Coppalle, A. The influence of turbulence upon the chemical reaction of nitric oxide released from a ground source into ambient ozone, Atmospheric Environment 1996, 30(9), 1467-1480.
Page 21, Line 610-612. The Kim et al. reference. (1) please correct the format. (2) is this reference published in Korean and provide English abstract? Need to mark down as “(in Korean)”.
Reference:
Kim, M.-S. Turbulent chemical kinetics model (TKM): A study of turbulent mixing effects on simple NOx-O3 photochemistry in Convective Boundary Layer, J. of Korean Society of Environmental Technology 2017, 611 18(2), 86-102.
Krol, M. C., Molemaker, M. J. Effects of turbulence and heterogeneous emissions on photochemically active species in the convective boundary layer, Journal of Geophysical Research 2000, 105(D5), 6871-6884.
The format of reference in Line 601-612 is changed and this reference is published in English.
[10] Kim, M.-S. Turbulent chemical kinetics model (TKM): A study of turbulent mixing effects on simple NOx-O3 photochemistry in Convective Boundary Layer, J. of Korean Society of Environmental Technology 2017, 18(2), 86-102.
The missing author’s name in Reference 25 is added:
Krol, M. C., Molemaker, M. J., Arellano, J.V.G.de Effects of turbulence and heterogeneous emissions on photochemically active species in the convective boundary layer, Journal of Geophysical Research 2000, 105(D5), 6871-6884.
Author Response File: Author Response.pdf
