Recent Advances in the Growth and Characterizations of SILAR-Deposited Thin Films

Round 1

Reviewer 1 Report

Comments for author File: Comments.pdf

Author Response

Please find the author response in attachment. 

Author Response File: Author Response.pdf

Reviewer 2 Report

In this manuscript, the author showed extensive review of the formation of various films via SILAR deposition techniques. Although the author mentioned that the film growth and reaction mechanisms will be highlighted in the review at introduction part, it looks like the main text failed to cover them. Moreover, figures failed to show informative data or scheme in an organized way, for example, just showing FTIR spectrum in Fig 4 not including morphologies, scheme, or etc. all together. Therefore, I hesitate its publication in the journal until the above issues are addressed.

 

Minor comment.

1.     Resolution of figures must be improved

2.     Please give a full name of abbreviations at least once, e.g.,) In line 144 abbreviation EDAX, SILAR in abstract, DDW in Figure 3  

3.     For improved legibility, please express the equations between paragraphs.

Author Response

Comments and Suggestions for Authors

In this manuscript, the author showed extensive review of the formation of various films via SILAR deposition techniques. Although the author mentioned that the film growth and reaction mechanisms will be highlighted in the review at introduction part, it looks like the main text failed to cover them [Thin film formation was explained by using equation (based on literature), and also highlighted specific precursor in the main text]. Moreover, figures failed to show informative data or scheme in an organized way, for example, just showing FTIR spectrum in Fig 4 not including morphologies, scheme, or etc. all together. [The main purpose added figure in this paper to attract readers. This is one of the strategic to increase reader’s interest in reading. For example, figure 1 and 2, the scheme of SILAR-deposited thin films. In figure 3, HRTEM images of Cu₂S prepared by using different complexing agents such as ammonia and hexamethyltetrammine. Readers can easily understand the morphology of the obtained films was strongly depended on the complexing agent. In figure 4, FTIR spectrum of SILAR deposited was presented. In figure 5, FESEM micrographs of PbS films deposited under various precursor concentrations such as 0.1M, 0.15M, 0.2M, 0.25M, and 0.3M. From this figure 5, readers understood the influence of precursor concentration of the morphology of the films. In this work, author cannot put too many figures such as EDX, XRD, XPS, FTIR, UV-visible, SEM and AFM to study the properties of particular metal chalcogenide thin films. Because of too many SILAR-deposited thin films have been reported here (22 metal sulfides, 5 metal tellurides, 13 metal selenides and 25 metal oxides)]. Therefore, I hesitate its publication in the journal until the above issues are addressed.

 

Minor comment.

1. Resolution of figures must be improved.

Clearly figure has been provided in paper.

2. Please give a full name of abbreviations at least once, e.g.,) In line 144 abbreviation EDAX, SILAR in abstract, DDW in Figure 3

Abbreviation was defined at its first mention in the main body of the manuscript.

3. For improved legibility, please express the equations between paragraphs.

In certain cases, the thin film formation was explained by using equations.

Author Response File: Author Response.pdf

Reviewer 3 Report

Type of manuscript: applsci-1823362

Title: Recent Advances in the growth and characterizations of SILAR deposited thin films

Review

 The author of the manuscript presents a review of metal sulfide, metal selenide, metal oxide and metal telluride thin films prepared by SILAR method. The author shows that the number of deposition cycle, rinsing time, immersion time, and the concentration of the precursors affected the crystallinity, grain size, film thickness, surface roughness and shapes of the obtained films. These films could be used in solar cell applications with high power conversion efficiency due to appropriate band gap value, and high absorption co-efficient value.

 In my opinion the manuscript needs major revision.

1.    The review just explains the results on thin layers’ investigations obtained by some physical methods (for example SEM, FTIR etc.) as well the applications announced at the Introduction section, but they are not all confirmed by the presented figures and graphs in the manuscript. Somewhere there is TEM micrograph, somewhere - SEM micrograph or FTIR graph, but somewhere there is not any figure to confirm the statement. For example – line 60 the author says that: “The obtained films showed homogeneous, and polycrystalline with the most intense peak along (100) plane based on the FESEM and XRD analysis” – but the figures with FESEM and XRD analyses are missing. Please, insert the figures and graphs for confirming the results presented in the manuscript.

2.    Please, write the abbreviations, when insert them for the first time in the text (SILAR, TEA, FESEM, etc.)

3.    Figure 3 is very unclear. Please, improve the resolution.

4.    Figure 4 is not mentioned in the text – Line 259. Sometimes the author uses different brackets () or [] to note the figures in the text.

5.    SAED patterns should be indexed when they show polycrystalline structure. The indexing is missing in figure 12b - SAED pattern.

6.    There is a technical mistake in figure 12-SAED patterns. The marker of 500 nm on the SAED patterns (fig.12a and 12b) is not correct and should be removed. The distances [d], measured from SAED patterns are calculated from the reciprocal space and that means the marker could not be 500 nm.

7.    The subtitles should be at the same style. Either the chemical formula, or text – for example – Line 340 “2.16 Iron sulphide films” and Line 347 “2.17 CuInS₂ films”. Line 872 “5.14. Cobalt doped manganese oxide films”, and Line 878 “5.15. Mn-doped CuO films”. Let all titles and subtitles begin with capital letter.

8.    Line 76 – short circuit current

9.    The sentences at Line 67 “Deposition of Ag₂S films onto glass slides in the presence of ammonia [complexing agent] at 40 °C [17].” and Line 73 “In the optical studies, the absorption edge at 620 nm with the band gap of 2.09 eV.” are not clear. I think I miss the verbs.

10.    Line 430 – CoSnS instead CoSS.

 

Author Response

read my answer

Author Response File: Author Response.docx

Reviewer 4 Report

The review has an interest approach, but it should be improved a lot before publishing.

The author should describe abbreviation “SILAR”.

The introduction, should be corrected. The author should provide more literature for every method and type of films. For example, in the following sentence, I suggested only two for specific methods, but the rest used by author literature should be also added: “Several physical method and chemical deposition technique were used for the 31 growth of thin films on substrate. These deposition methods include electro deposition [2], chemical bath deposition [3], sputtering [DOI: 10.1016/J.TSF.2012.11.023], chemical vapor deposition, spray pyrolysis, thermal evaporation [4], vacuum evaporation, flash evaporation, electron beam evaporation, atomic layer epitaxy [DOI: 10.3390/COATINGS10100954], spin coating method [5], pulsed laser deposition method and SILAR technique. “

After introduction, the description of SILAR method should be given and the table with comparison to other methods should be presented.

Quality of Figure 1 should be improved. And using of other figures should be reconsidered.

Some types of films have a detailed description of their properties and even TEM images are shown. But the others are described by a short paragraph. The author should present the examples more evenly.

Author Response

The review has an interest approach, but it should be improved a lot before publishing.

The author should describe abbreviation “SILAR”.

[Abbreviation was defined at its first mention in the main body of the manuscript]

The introduction, should be corrected. The author should provide more literature for every method and type of films. For example, in the following sentence, I suggested only two for specific methods, but the rest used by author literature should be also added: “Several physical method and chemical deposition technique were used for the 31 growth of thin films on substrate. These deposition methods include electro deposition [2], chemical bath deposition [3], sputtering [DOI: 10.1016/J.TSF.2012.11.023], chemical vapor deposition, spray pyrolysis, thermal evaporation [4], vacuum evaporation, flash evaporation, electron beam evaporation, atomic layer epitaxy [DOI: 10.3390/COATINGS10100954], spin coating method [5], pulsed laser deposition method and SILAR technique. “

After introduction, the description of SILAR method should be given and the table with comparison to other methods should be presented.

Table 1: The advantages and disadvantages of various deposition techniques

Deposition method	Benefits	Disadvantages
spray pyrolysis	Low-cost deposition method, high growth rate could be observed	It was very complicated process, and showed very low yield
chemical bath deposition	Cheaper and simple method, deposition process requires substrate and solution in the container	Wastage of solution after deposition process
electron beam evaporation	Multiple thin films can be produced	The non-uniform evaporating rate could be seen due to filament degradation
Electrodeposition method	Cheaper deposition method, and showed high deposition rate	Not suitable for large scale production
Ion beam deposition	Uniform morphology of the obtained films could be seen	Deposition rate was very low, and this method is very expensive
Atomic layer epitaxy	Can synthesis high quality films	High energy waste rate could be observed during the deposition process
Chemical vapour deposition	Can synthesis thick films, under high deposition rate	High temperature is requited during the deposition
molecular beam epitaxy	High purity and epitaxial materials could be produced	Very expensive deposition method
Magnetron sputtering	High adhesion and uniform morphology of the obtained films	Very expensive deposition method and the very low deposition rate
Pulsed laser deposition	Dense and porous morphology could be observed in the obtained samples	Very expensive deposition technique
Spin coating	Very thin, fine and uniform morphology of the obtained sample by using this method	High speed spinning became very difficult when the size of the substrate was increasing
Thermal evaporation	High deposition rate could be seen during the deposition process	Very poor coverage could be observed because of low vacuum

 

 

Quality of Figure 1 should be improved. And using of other figures should be reconsidered.

[The main purpose added figure in this paper to attract readers. This is one of the strategic to increase reader’s interest in reading. For example, figure 1 and 2, the scheme of SILAR-deposited thin films. In figure 3, HRTEM images of Cu₂S prepared by using different complexing agents such as ammonia and hexamethyltetrammine. Readers can easily understand the morphology of the obtained films was strongly depended on the complexing agent. In figure 4, FTIR spectrum of SILAR deposited was presented. In figure 5, FESEM micrographs of PbS films deposited under various precursor concentrations such as 0.1M, 0.15M, 0.2M, 0.25M, and 0.3M. From this figure 5, readers understood the influence of precursor concentration of the morphology of the films.

Some types of films have a detailed description of their properties and even TEM images are shown. But the others are described by a short paragraph. The author should present the examples more evenly.

In this work, author cannot put too many figures such as EDX, XRD, XPS, FTIR, UV-visible, SEM and AFM to study the properties of particular metal chalcogenide thin films. Because of too many SILAR-deposited thin films have been reported here (22 metal sulfides, 5 metal tellurides, 13 metal selenides and 25 metal oxides). Therefore, author presented figure for selected metal chalcogenide films only.

Author Response File: Author Response.pdf

Reviewer 5 Report

 The manuscript gives an overview of deposition conditions for producing thin films by SILAR technique, the kind of deep coating method that enables layer-by-layer film growth. The manuscript does not contain any discussion about the method itself or a comparison of the quality of films obtained by SILAR with those deposited by other methods. However, the presented possibilities of film formation by SILARB method could be useful for the readers.

Before I recommend publishing the manuscript, it would be good to make the changes listed below.

 

  The term “SILAR” is not common and should be explained at the beginning of the manuscript.

Some sentences should be added that explain this method's basic principles of film formation.

 

 

Author Response

Comments and Suggestions for Authors

 The manuscript gives an overview of deposition conditions for producing thin films by SILAR technique, the kind of deep coating method that enables layer-by-layer film growth. The manuscript does not contain any discussion about the method itself or a comparison of the quality of films obtained by SILAR with those deposited by other methods. However, the presented possibilities of film formation by SILARB method could be useful for the readers.

Table 1: The advantages and disadvantages of various deposition techniques

Deposition method	Benefits	Disadvantages
spray pyrolysis	Low-cost deposition method, high growth rate could be observed	It was very complicated process, and showed very low yield
chemical bath deposition	Cheaper and simple method, deposition process requires substrate and solution in the container	Wastage of solution after deposition process
electron beam evaporation	Multiple thin films can be produced	The non-uniform evaporating rate could be seen due to filament degradation
Electrodeposition method	Cheaper deposition method, and showed high deposition rate	Not suitable for large scale production
Ion beam deposition	Uniform morphology of the obtained films could be seen	Deposition rate was very low, and this method is very expensive
Atomic layer epitaxy	Can synthesis high quality films	High energy waste rate could be observed during the deposition process
Chemical vapour deposition	Can synthesis thick films, under high deposition rate	High temperature is requited during the deposition
molecular beam epitaxy	High purity and epitaxial materials could be produced	Very expensive deposition method
Magnetron sputtering	High adhesion and uniform morphology of the obtained films	Very expensive deposition method and the very low deposition rate
Pulsed laser deposition	Dense and porous morphology could be observed in the obtained samples	Very expensive deposition technique
Spin coating	Very thin, fine and uniform morphology of the obtained sample by using this method	High speed spinning became very difficult when the size of the substrate was increasing
Thermal evaporation	High deposition rate could be seen during the deposition process	Very poor coverage could be observed because of low vacuum

 

Before I recommend publishing the manuscript, it would be good to make the changes listed below.

   The term “SILAR” is not common and should be explained at the beginning of the manuscript.

[Abbreviation was defined at its first mention in the main body of the manuscript.]

Some sentences should be added that explain this method's basic principles of film formation.

Generally, background of SILAR deposition technique could be represented by adsorption and reaction of ions (anion and cation from solutions), and also rinsing process (deionized water) to prevent precipitation happened in the solution. SILAR technique consisted of four steps [12], namely adsorption (cation is adsorbed on substrate surface), first rinsing with water (excess adsorbed ions were rinsed away), reaction process (introduce anionic ion into the system) and second rinsing (unreacted species and excess ions were removed). Formation of thin films on substrate could be observed by repeating these cycles [13]. The complexing agent, rinsing time, immersion time, deposition cycles, concentration of the precursor solutions, and the nature of the precursors have been shown to affect the SILAR growth phenomena.

 

 

 

Author Response File: Author Response.docx

Round 2

Reviewer 1 Report

Comments for author File: Comments.pdf

Author Response

see attachment. thanks 

Author Response File: Author Response.pdf

Reviewer 2 Report

The manuscript was modified accordingly thereby I can suggest its publication in the journal. 

Author Response

Thanks, reviewer 

Reviewer 3 Report

Unfortunately I am not satisfied with the answers of my remarks No 5 and 6. 

Author Response

Comments and Suggestions for Authors

Unfortunately I am not satisfied with the answers of my remarks No 5 and 6.

I decided to remove this figure in my paper. It does not affect the paper content after removed this figure.

Reviewer 4 Report

The manucript can be published.

Author Response

Thanks, reviewer