A Comprehensive Review of the Fundamentals, Progress, and Applications of the LIBS Method in Analysis of Plants: Quantitative and Qualitative Analysis

Round 1

Reviewer 1 Report (Previous Reviewer 2)

Comments and Suggestions for Authors

The authors have substantially rewritten the manuscript, but the quality is still average at best. They clearly put a lot of work into the assembly, and processed many references. Unfortunately the organization of the manuscript is still unclear, confusing and lacks focus. It reads poorly. The responses provided to my comments do not contain any rebuttal, explanation or details, the authors basically just responded "okay, we will correct it" and then did some corrections, by almost always missing the point (but clearly putting in a lot of work). The "experimental" part is still very lengthy, not really discussing anything and not useful for most readers; it could be omitted. The calibration section could also be reduced to a table. Please note that a plant LIBS analysis review should have an application-oriented focus, considering who will read the paper.  

Author Response

Reviewer 1

Unfortunately the organization of the manuscript is still unclear, confusing and lacks focus. It reads poorly. The "experimental" part is still very lengthy, not really discussing anything and not useful for most readers; it could be omitted. The calibration section could also be reduced to a table. Please note that a plant LIBS analysis review should have an application-oriented focus, considering who will read the paper.  

We have deeply revised the manuscript, also according to the suggestions of the other reviewers. For improving the readability of the review, the number of chapters has been reduced. We divided the review in three parts: the first part describes the experimental setup and the effects of the experimental parameters in LIBS analysis of plants; the second part describes several applications of LIBS in plant analysis, while the third part is devoted to the discussion of the methods proposed for improving the LIBS signal and the quantitative analysis, as well as the future perspectives of the technique. We hope that in the present form the manuscript will be considered suitable for publication.

Reviewer 2 Report (New Reviewer)

Comments and Suggestions for Authors

Overall, the manuscript gives a clear and useful review of LIBS applications in plant and agricultural product analysis. It covers a wide range of literature and recent developments, and the structure makes it easy to follow. I believe it can be accepted after some improvements. The following comments are meant to help make the text clearer, more consistent, and scientifically stronger. Since these are mainly editorial and style corrections, my recommendation is minor revision.

• The manuscript uses inconsistent and non-standard reference grouping such as [5][6][7] and [19][20]. These should be merged into standard grouped formats like [5-7] for consecutive references and [19, 20] for non-consecutive ones. This issue appears multiple times and should be corrected throughout the manuscript. In addition, it needs to be corrected throughout the tables and figure captions for consistency.
• The transition from LIBS fundamentals (lines 31-46) to plant nutrient discussion (lines 47-56) is abrupt; a bridging sentence explaining why nutrient analysis is relevant to LIBS would improve cohesion.
• Some phrases are awkward or grammatically incorrect, e.g., “depending on environmental conditions, some of them (non-essential) elements…” should be replaced with “depending on environmental conditions, some non-essential elements…”; “water absorption, inhibiting growth, and nutrient” should be intended as “water absorption, inhibiting nutrient uptake, and growth…”.
• The phrase “to the authors’ best knowledge” (line 68) is acceptable, but consider supporting it with a more concrete statement about the gap in literature to strengthen the novelty claim.
• Lines 71–80 contain a very long sentence listing all applications; consider splitting into multiple sentences.
• The opening sentence lists multiple laser types (Nd:YAG, ArF excimer, CO₂, Ti:Sapphire) but does not explain why some are more suited than others for plant analysis. Adding a brief rationale would make it more informative.
• Sometimes “femtosecond lasers” is written fully, sometimes “fs lasers” or “fs-LIBS”; pick one style and keep it consistent across the manuscript.
• Units are missing for laser parameters (e.g., pulse duration in fs or ns for Nd:YAG, repetition rates) which are important for reproducibility.
• “less performant” is non-standard phrasing in scientific writing; “lower performance” or “less sensitive” would be clearer.
• The description of Figure 1 is clear, but it repeats “as shown in Figure…” twice in consecutive sentences; could be streamlined.
• Suggest stating explicitly that the spatial resolution of 2 μm was achieved via motorized stage movement (not just “resolution of 2 μm”), to clarify.
• Figure 1 panels are labeled A-D in the text, but the caption doesn’t explain the experimental conditions for each panel (e.g., why 3rd, 4th, and 5th days are shown for silver and copper).
• The color bar in C and D is mentioned but not described in the caption beyond “decreasing content.” Consider adding actual scale units if available.
• The caption in Fig. 2 is long and mixes apparatus description with spectral results. Consider splitting into two sentences or subparts (instrumentation vs. spectra).
• “Soluble salt metals signal” is unclear. Needs clarification or rephrasing (for example: “signal from soluble salt-associated metals”).
• The Galiová et al. and Abdul Jabbar et al. paragraphs repeat what is visible in figures without adding much interpretation; could instead briefly focus on significance, limitations, or how LIBS compares to other techniques.
• The phrase “more enhanced” (line 173) is redundant. Simply “enhanced” is sufficient.
• There are inconsistent laser parameter notations (sometimes “Nd:YAG laser, 1,064 nm” vs. “Nd:YAG, 1064 nm”); this should be standardized.
• Multiple analyte lists are written without consistent separators (sometimes commas only, sometimes commas plus spaces inconsistently).
• Phrases like “recently published an interesting study” (line 160) are too informal for a scientific review; better: “recently reported a study.”
• Avoid subjective descriptors (“interesting,” “remarkable”) unless supported with specific reasoning.
• The table shows CTC and SR values but does not specify units (are these percentages, g/kg, mg/g?).
• Abbreviations CTC and SR are expanded in the text, but the table caption should also include their definitions for stand-alone clarity.
• The sentence in lines 199–200 “for the elemental determinations of the various sections of plant samples” is unnecessarily wordy. Could be simplified to “for elemental analysis of different plant parts.”
• In the Bossu et al. [51] study, correlations between rare metals and air pollution are mentioned, but no statistical or methodological details are given. A review should at least mention the type of correlation analysis or main trends. In addition, the Pouzar et al. [111] and Carvalho et al. [36] studies are briefly summarized but lack context on why LIBS was chosen over other methods in those cases.
• Avoid subjective adjectives (“highly beneficial,” “safe antibacterial and anticancer drugs”) unless directly supported by quantitative evidence in the cited studies.
• “Could be a viable tool” (line 263) is more appropriate for a discussion/conclusion, not the results summary in a review section.
• For Figure 6, it would be helpful to explain the context of the Cd calibration curve (sample preparation, method of spiking Cd).
• Overloaded with detail; better split into separate subfigure descriptions for clarity.
• Units for crater diameters and concentrations are given, but methods for determining these concentrations are not mentioned.
• In line 404, the sentence begins with “…with minimal preparation. laser-induced breakdown spectroscopy…”. The second sentence should start with a capital letter (“Laser-induced…”). This is likely a typographical error.
• Sometimes “LIBS technique” is used, other times “LIBS method” or just “LIBS.” Pick one term and use it consistently.
• Species names should always be italicized.
• The sentence “…with their stability in suspension influencing absorption” (line 1001-1002) is dangling and would read better if linked directly to the observed results.
• The results for Navarro et al. [230] mention that QDs were “…primarily located on the exterior surfaces”. This could benefit from a brief note on how this was confirmed (e.g., microscopy, spectroscopy).
• Use a consistent term for nanoparticles. Sometimes “Ag nanoparticles,” sometimes “silver nanoparticles,” sometimes “AgNPs.”
• Likewise, use either “nano-enhanced LIBS” or “NELIBS” consistently, not both interchangeably without definition.
• In lines 1250-1253 and 1274-1276, the conclusions emphasize the simplicity and potential of LIBS but omit discussion of its known limitations (matrix effects, detection limits, calibration challenges). Including such limitations would make the assessment more balanced.
• In lines 1555-1561, Jabbar et al.’s findings are summarized clearly, but again, the “exponential decrease” in electron number density with distance is mentioned without giving the decay constant or percentage drop. Providing this quantitative detail would improve the scientific rigor.
• In lines 1720–1723, the suggestion to explore 3D elemental imaging, nanoparticle-enhanced LIBS, and micro-LIBS is good, but there is no reference to prior feasibility studies or pilot results. Briefly citing key works that have demonstrated early success in these methods would strengthen the argument.
• As a final note, I would like to say that I was truly sorry to read about your loss, Dr. Rezaei. The way you dedicated this work to your mother is a beautiful way to remember her.

Author Response

Reviewer 2

• The manuscript uses inconsistent and non-standard reference grouping such as [5][6][7] and [19][20]. These should be merged into standard grouped formats like [5-7] for consecutive references and [19, 20] for non-consecutive ones. This issue appears multiple times and should be corrected throughout the manuscript. In addition, it needs to be corrected throughout the tables and figure captions for consistency.

We apologize for the non-standard reference grouping. We have corrected the issue in the revised manuscript.

• The transition from LIBS fundamentals (lines 31-46) to plant nutrient discussion (lines 47-56) is abrupt; a bridging sentence explaining why nutrient analysis is relevant to LIBS would improve cohesion.

We thank the reviewer for their suggestion. We have added a sentence between lines 46 and 47.

• Some phrases are awkward or grammatically incorrect, e.g., “depending on environmental conditions, some of them (non-essential) elements…” should be replaced with “depending on environmental conditions, some non-essential elements…”; “water absorption, inhibiting growth, and nutrient” should be intended as “water absorption, inhibiting nutrient uptake, and growth…”.

We have reformulated the sentences according to the reviewer’s suggestions.

• The phrase “to the authors’ best knowledge” (line 68) is acceptable, but consider supporting it with a more concrete statement about the gap in literature to strengthen the novelty claim.

We have reformulated the sentence to evidence the lack of recent reviews dealing with all the aspects of LIBS analysis of plants.

• Lines 71–80 contain a very long sentence listing all applications; consider splitting into multiple sentences.

Following the kind suggestion of the reviewer, we have split the long sentence into two parts.

• The opening sentence lists multiple laser types (Nd:YAG, ArF excimer, CO₂, Ti:Sapphire) but does not explain why some are more suited than others for plant analysis. Adding a brief rationale would make it more informative.

We have rearranged the paragraph to make clear that excimer lasers are used for short-wavelength laser-ablation, while Ti:Sapphire lasers are used for femtosecond LIBS.

• Sometimes “femtosecond lasers” is written fully, sometimes “fs lasers” or “fs-LIBS”; pick one style and keep it consistent across the manuscript.

We have changed all the occurrences of fs (except in ‘fs-LIBS’ and when it is used as measurement unit) in ‘femtosecond’.

• Units are missing for laser parameters (e.g., pulse duration in fs or ns for Nd:YAG, repetition rates) which are important for reproducibility.

We have simplified the table of laser parameters, showing only the wavelength(s) and the pulse duration ranges. Other information that were not available for all the papers and not particularly relevant for the discussion were removed.

• “less performant” is non-standard phrasing in scientific writing; “lower performance” or “less sensitive” would be clearer.

We have substituted ‘less performant’ with ‘lower spectral resolution and sensitivity’

• The description of Figure 1 is clear, but it repeats “as shown in Figure…” twice in consecutive sentences; could be streamlined.

We thank the reviewer for their patience. We made the sentence more readable by removing the repetition.

• Suggest stating explicitly that the spatial resolution of 2 μm was achieved via motorized stage movement (not just “resolution of 2 μm”), to clarify.

Done.

• Figure 1 panels are labeled A-D in the text, but the caption doesn’t explain the experimental conditions for each panel (e.g., why 3rd, 4th, and 5th days are shown for silver and copper).

We have mentioned in the text and the caption that the accumulation was measured a few days after the treatment.

• The color bar in C and D is mentioned but not described in the caption beyond “decreasing content.” Consider adding actual scale units if available.

The figure was taken from ref. [71], the quantitative scale was not available.

• The caption in Fig. 2 is long and mixes apparatus description with spectral results. Consider splitting into two sentences or subparts (instrumentation vs. spectra).

Done.

• “Soluble salt metals signal” is unclear. Needs clarification or rephrasing (for example: “signal from soluble salt-associated metals”).

We thank the reviewer for pointing out the error. We corrected it in “soluble metal salts”.

• The Galiová et al. and Abdul Jabbar et al. paragraphs repeat what is visible in figures without adding much interpretation; could instead briefly focus on significance, limitations, or how LIBS compares to other techniques.

We have evidenced the main points which make these two papers particularly notable.

• The phrase “more enhanced” (line 173) is redundant. Simply “enhanced” is sufficient.

Done.

• There are inconsistent laser parameter notations (sometimes “Nd:YAG laser, 1,064 nm” vs. “Nd:YAG, 1064 nm”); this should be standardized.

We standardized the notation, using ‘Nd:YAG, 1064 nm’

• Multiple analyte lists are written without consistent separators (sometimes commas only, sometimes commas plus spaces inconsistently).

We have tried to locate and correct all the incongruences.

• Phrases like “recently published an interesting study” (line 160) are too informal for a scientific review; better: “recently reported a study.”

Done.

• Avoid subjective descriptors (“interesting,” “remarkable”) unless supported with specific reasoning.

Done.

• The table shows CTC and SR values but does not specify units (are these percentages, g/kg, mg/g?). Abbreviations CTC and SR are expanded in the text, but the table caption should also include their definitions for stand-alone clarity.

We apologize, the units (%) were added in the previous revision but, for some reason, they did not show in the revised one. We added acronyms definitions and units in the figure captions.

• The sentence in lines 199–200 “for the elemental determinations of the various sections of plant samples” is unnecessarily wordy. Could be simplified to “for elemental analysis of different plant parts.”

Done.

• In the Bossu et al. [51] study, correlations between rare metals and air pollution are mentioned, but no statistical or methodological details are given. A review should at least mention the type of correlation analysis or main trends.

We have added a summary description of the method used by Bossu et al. for qualitatively estimating the level of pollution of the sites where the leaves were collected.

• In addition, the Pouzar et al. [111] and Carvalho et al. [36] studies are briefly summarized but lack context on why LIBS was chosen over other methods in those cases.

We have added some information on the motivation that moved the authors to use LIBS in plant analysis (developing a fast and cheap alternative to conventional analytical methods in the case of Pouzar et al., exploting the complementary nature of LIBS and XRF in the case of Carvalho et al.).

• Avoid subjective adjectives (“highly beneficial,” “safe antibacterial and anticancer drugs”) unless directly supported by quantitative evidence in the cited studies.

Done.

• “Could be a viable tool” (line 263) is more appropriate for a discussion/conclusion, not the results summary in a review section.

We have reformulated the sentence in a way that should be more appropriate to the context (“The authors suggested…”).

• For Figure 6, it would be helpful to explain the context of the Cd calibration curve (sample preparation, method of spiking Cd).

We have added some additional information on the way the Cd calibration curve was built.

• Overloaded with detail; better split into separate subfigure descriptions for clarity.

We have tried simplified the figure for easier reading.

• Units for crater diameters and concentrations are given, but methods for determining these concentrations are not mentioned.

We added information about the technique used for determining Fe concentration in the leaves.

• In line 404, the sentence begins with “…with minimal preparation. laser-induced breakdown spectroscopy…”. The second sentence should start with a capital letter (“Laser-induced…”). This is likely a typographical error.

We thank the reviewer for pointing out the error. We corrected it in the revised manuscript.

• Sometimes “LIBS technique” is used, other times “LIBS method” or just “LIBS.” Pick one term and use it consistently.

For consistency, we used ‘LIBS’ throughout the manuscript.

• Species names should always be italicized.

Done.

• The sentence “…with their stability in suspension influencing absorption” (line 1001-1002) is dangling and would read better if linked directly to the observed results.

We have slightly modified the sentence to make clear that the authors observed a correlation between the quantity of QDs absorbed and their stability in suspension.

• The results for Navarro et al. [230] mention that QDs were “…primarily located on the exterior surfaces”. This could benefit from a brief note on how this was confirmed (e.g., microscopy, spectroscopy).

We mentioned that the surface absorption was confirmed by fluorescence microscopy.

• Use a consistent term for nanoparticles. Sometimes “Ag nanoparticles,” sometimes “silver nanoparticles,” sometimes “AgNPs.”
• Likewise, use either “nano-enhanced LIBS” or “NELIBS” consistently, not both interchangeably without definition.

To be consistent, we used throughout the manuscript ‘Ag nanoparticles’ and ‘NELIBS’.

• In lines 1250-1253 and 1274-1276, the conclusions emphasize the simplicity and potential of LIBS but omit discussion of its known limitations (matrix effects, detection limits, calibration challenges). Including such limitations would make the assessment more balanced.

In the revised version of the manuscript we added, at the end of the subsection devoted to the discussion of advantages and disadvantages of LIBS, a paragraph in which the issues related to self-absorption, matrix effect, etc. are explicitly mentioned.

• In lines 1555-1561, Jabbar et al.’s findings are summarized clearly, but again, the “exponential decrease” in electron number density with distance is mentioned without giving the decay constant or percentage drop. Providing this quantitative detail would improve the scientific rigor.

We have added quantitative detail on the decay length of the electron number density.

• In lines 1720–1723, the suggestion to explore 3D elemental imaging, nanoparticle-enhanced LIBS, and micro-LIBS is good, but there is no reference to prior feasibility studies or pilot results. Briefly citing key works that have demonstrated early success in these methods would strengthen the argument.

We thank the reviewer for the suggestion. We have added some prior references to these applications.

Reviewer 3 Report (New Reviewer)

Comments and Suggestions for Authors

The manuscript currently reads more like a long compilation of individual research articles rather than a critical and coherent review. The emphasis is too much on listing past studies, while the synthesis of knowledge, challenges, and perspectives is lacking. The structure of the paper needs to be reconsidered to provide a logical flow that guides the reader through instrumentation, sample preparation, significance of LIBS in plant analysis, and data analysis strategies.

In the Abstract, the first sentence should begin with “This review” instead of “This research”. The abstract should better emphasize the scope of the review, highlight key challenges, and state the intended contribution of this paper.

Much of the text is dedicated to enumerating existing studies without integrating them into a coherent narrative. The authors should identify the most significant contributions, compare methodologies, and explain the implications for the field. A critical analysis that highlights gaps, challenges, and opportunities will make the review more useful.

Section 2.2 (Optics) is extremely brief and provides little useful information. It would be better to categorize LIBS setups relevant to plant analysis (e.g., benchtop, portable, imaging/mapping, standoff) rather than repeating general textbook information.

Section 2.3 (Spectrometers) currently mixes general descriptions with case-by-case examples. It should instead provide a structured overview of spectrometer types used in LIBS for plant studies, with tables summarizing applications.

Acronyms should be spelled out at first use, and their use should be consistent throughout the manuscript. The current draft does not follow this practice systematically.

The overall sectioning does not follow a logical order. For example, Significance of LIBS in Plant Analysis (Section 3) appears too early and does not match the content, which is mostly a list of studies. Sample preparation section should follow the LIBS instrumentation section.

The role of chemometrics is crucial for LIBS, but this topic is underdeveloped. A separate subsection should be dedicated to statistical and machine learning approaches, with examples of how they enhance classification and quantitative analysis in plant studies. At present, the section is too brief and insufficient.

Section 14 should logically follow the instrumentation section, not appear near the end of the manuscript. The content needs to be reorganized for coherence.

The manuscript has the potential to make a useful contribution, but in its current form it is not yet suitable for publication. I strongly recommend major revision with a substantial restructuring of sections, reduction of redundant literature listing, and greater focus on critical evaluation and future perspectives.

Author Response

Reviewer 3

The manuscript currently reads more like a long compilation of individual research articles rather than a critical and coherent review. The emphasis is too much on listing past studies, while the synthesis of knowledge, challenges, and perspectives is lacking. The structure of the paper needs to be reconsidered to provide a logical flow that guides the reader through instrumentation, sample preparation, significance of LIBS in plant analysis, and data analysis strategies.

The overall sectioning does not follow a logical order. For example, Significance of LIBS in Plant Analysis (Section 3) appears too early and does not match the content, which is mostly a list of studies. Sample preparation section should follow the LIBS instrumentation section.
The role of chemometrics is crucial for LIBS, but this topic is underdeveloped. A separate subsection should be dedicated to statistical and machine learning approaches, with examples of how they enhance classification and quantitative analysis in plant studies. At present, the section is too brief and insufficient. Section 14 should logically follow the instrumentation section, not appear near the end of the manuscript. The content needs to be reorganized for coherence.

Much of the text is dedicated to enumerating existing studies without integrating them into a coherent narrative. The authors should identify the most significant contributions, compare methodologies, and explain the implications for the field. A critical analysis that highlights gaps, challenges, and opportunities will make the review more useful.

Section 2.2 (Optics) is extremely brief and provides little useful information. It would be better to categorize LIBS setups relevant to plant analysis (e.g., benchtop, portable, imaging/mapping, standoff) rather than repeating general textbook information

Section 2.3 (Spectrometers) currently mixes general descriptions with case-by-case examples. It should instead provide a structured overview of spectrometer types used in LIBS for plant studies, with tables summarizing applications.

Much of the text is dedicated to enumerating existing studies without integrating them into a coherent narrative. The authors should identify the most significant contributions, compare methodologies, and explain the implications for the field. A critical analysis that highlights gaps, challenges, and opportunities will make the review more useful.

The manuscript has the potential to make a useful contribution, but in its current form it is not yet suitable for publication. I strongly recommend major revision with a substantial restructuring of sections, reduction of redundant literature listing, and greater focus on critical evaluation and future perspectives.

 

We have deeply revised the manuscript structure, also according to the suggestions of the other reviewers. For improving the readability of the review the number of chapters has been reduced; the first part now describes the experimental setup and the effects of the experimental parameters in LIBS analysis of plants; the second part describes several applications of LIBS in plant analysis, while the third part is devoted to the discussion of the methods proposed for improving the LIBS signal and the quantitative analysis (with special emphasis on chemometrics), as well as the future perspectives of the technique. In the revised manuscript, about 1/3 of the text is now devoted to critically discussing the applications of LIBS to plant analysis through comparison of LIBS results with the ones of other assessed analytical methods, discussion of the advantages and disadvantages of LIBS, presentation of innovative methods for improving the LIBS signal and its analysis, as well as future perspectives of the technique. We hope that in the present form the manuscript will be considered suitable for publication.

Round 2

Reviewer 3 Report (New Reviewer)

Comments and Suggestions for Authors

The authors have not provided point-by-point responses to my comments but instead offered only a general statement regarding the revised manuscript. As a result, it is difficult to ascertain whether my concerns have been adequately addressed and whether the manuscript has been substantially improved in light of the review. Nevertheless, given that the revised version appears to include considerably more content than the previous submission, I believe the manuscript may be considered publishable as a compilation of relevant works in the field.

This manuscript is a resubmission of an earlier submission. The following is a list of the peer review reports and author responses from that submission.

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

The paper resembles a research part of a diploma thesis rather than a scientific review. No technical information is provided. The informations are only cited, but very briefly, without putting in context.  No causalities are established, there are just citations without a point or conclusion. There's not much point in reporting that this person measured some elements in tobacco leaves and another person measured some elements in spinach leaves and some person used this type of nanoparticle...

Graphs and images as they are taken from different sources have different formatting, are blurred and some even deformed.

There are statements, without explanation e.g. 89-90 However, ultraviolet (UV) laser irradiation, particularly with the fourth harmonic, can be  advantageous in minimizing matrix effects and improving measurement precision. - such an announcement should be supported by a citation or explanation.

123-124 "Alternatively, compact spectrometers based on  Czerny–Turner optics and CCD detectors, though less performant, are especially attractive due to their portability, flexibility, and lower cost." Overly simplistic and untrue, on the contrary, the larger the more accurate and the resolution can be good. For example, a Shamrock 750 with a 1200 l/mm grating has a resolution of 0.06 nm is 900 mm large and weighs 35 kg without camera... McPherson Model 2062 (resolution 0.005 nm  for 1200l/mm) measures 2 metres and it costs a lot.

Table 1: it is of no indicative value to cite only Czerny-Turner or Echelle. At least the resolution of the grating used and the focal length must be stated...

294-297 - formatting problem

Author Response

Please find the attachment.

Author Response File: Author Response.pdf

Reviewer 2 Report

Comments and Suggestions for Authors

In recent years, LIBS has become a valuable tool for in-field and industrial measurements. The analysis of plants is one such field in which many new results were published using LIBS. Thus, in spite of the several already existing good reviews on the topic, it makes sense to revisit and overview this field of applications from time to time. The present review undertook this task.

Overall, the manuscript is written well, and provides detailed and carefully collected, useful data on recent literature results. It will be a valuable source of reference for analysts, biologists, agricultural researchers, etc. working in this area. I recommend it for publication; I only have a few minor comments with regard to some issues that need to be dealt with (minor revision). Please find my comments below.

1. The title could be worded better. Vegetables are all plants, more precisely the edible part of plants. Therefore I suggest that the authors formulate a more approriate title.
2. The abstract starts as “This research”. Please change it to “This review”, since it is not original research, but indeed a review.
3. In reviews, it is customary to orient the viewer in terms of the focus of the paper or the coverage in terms of range of years (e.g. last 5-10 years, etc.). This information is missing from the introduction. Please add and enforce.
4. The focus of some sections of the review is not always consistent. For example, the last five paragraphs of section 2.1. on spectrometers discusses papers and includes illustrations with little cohesion to the section. This part of the text feels like it was partly meant for the introduction. Please check. Also in this part, signal enhancement approaches are also mentioned (e.g. Fig 3 and related text), when in actuality they may be more useful in a different (separate) section. At the same time, many of the studies mentioned in section 13 are actually not combining LIBS data with that of other methods, they just include LIBS data side by side with other data. Please correct the text or the title of the section.
5. While soil composition clearly is related to plant composition, but discussing many papers that directly focus on soil LIBS analysis seems to be unjustified. Under the present title, it would be best to focus on plant analytical papers. Please remove these text parts.
6. The topics selected to be emphasized as sections give a mixed feeling. Sometimes they are technically oriented (these parts are not very detailed), others are focusing on signal formation and calibration (not characteristic to plants at all), whereas others are assorted topics related to plant elemental analysis for various purposes (where LIBS is only a tool, but rarely brings novelty, however this is actually the part which would interest biologists, agricultural, or medical people the most). All this is also not in full harmony with the title of the review. Please consider changing the title or reducing the the number sections.  
7. Many recent publications in the LIBS plant mapping field are unfortunately missing from the list of references. I have the impression that the coverage only includes papers that have LIBS in their title. In understand that this is a problem that is not easy to correct, but at least do a more detailed search and you will see that there are far more papers…
8. Many typos, smaller linquistic problems, misuse of smaller case/upper case occur in the text. It would be beneficial to have the text and formatting checked again.

Author Response

Please find the attachment.

Author Response File: Author Response.pdf

Reviewer 3 Report

Comments and Suggestions for Authors

This study comprehensively reviews recent advancements and innovative applications of LIBS for the analysis of mineral and trace element distributions in plant and vegetable matrices. While demonstrating significant potential for rapid elemental characterization, several problems need to be addressed.
(1). Some formatting in the article needs to be corrected. For example, the captions (A), (B), and (C) in Figure 1 are in capital letters while the other captions are in lowercase. The labels (a), (b), and (c) in Figure 2 should be unified, and some parts of the highlights in Figure 7 should also be adjusted.
(2). Some of reference citation are formatted incorrectly. For example, the years and pages information of the reference 71 “Krizkova, S.; Ryant, P.; Krystofova, O.; Adam, V.; Galiova, M.; Beklova, M.; Babula, P.; Kaiser, J.; Novotny, K.; Novotny, J.; et al. Multi-Instrumental Analysis of Tissues of Sunflower Plants Treated with Silver(I) Ions – Plants as Bioindicators of Environmental Pollution. Sensors 2008, Vol. 8, Pages 445-463 2008, 8, 445–463, doi:10.3390/S8010445.” appears twice.
(3). The terms used in the article should be consistent throughout. For instance, "support vector machines (SVM)", "principal component analysis (PCA)" and other similar terms appear multiple times in the article. Only the first occurrence needs to use the given complete spelling; there is no need to repeat it.
(4). There is no introduction to the content of Figure 7 in the paper.
(5). The literature review should not merely be a simple listing of the literature. It should incorporate some of one's own opinions and summary statements. Most of the chapters in the article end with references to the literature. However, there is no summary of the content and key points for this section.
(6). Table 2 presents an overview of different sections of plant samples analyzed using the LIBS method under various laser conditions. However, there still have some results have no expression in tdelay and tint. And, the author should add the result such as limit of detection (LOD) and explain the influence of these parameters for LIBS analysis performance in detail.
(7). Table 3 lacks information on concentration units such as % or ppm.
(8). Repetition of citing the content of the literature. For example, line 335 and line 359, the two paragraph have similar content and are excerpted from the same document. The author should choose one and check in entire text.
(9). Figure 5 is suspended within the paragraph. Figure 5 is between Line 384 and line 385.
(10). Except LIBS's advantages over traditional methods, the disadvantages of LIBS should be also emphasized in Table 8 to comprehensively evaluate the effectiveness of LIBS technology.
(11). A proper review article requires more than sequential literature listing - it demands critical evaluation and integrative synthesis. The manuscript's current structure, where most sections conclude with references rather than analytical summaries, fails to: (1) highlight conceptual connections, (2) identify knowledge gaps, or (3) provide authoritative perspectives on the field's development

Author Response

Please find the attachment.

Author Response File: Author Response.pdf