Recent Studies on the Fabrication of Multilayer Films by Magnetron Sputtering and Their Irradiation Behaviors

Round 1

Reviewer 1 Report

The article submitted for review entitled “A review on the fabrication of multilayer films by magnetron sputtering and their irradiation behaviors” presents a detailed review of magnetron deposition parameters and their impact on the deposition of multilayer thin films. The paper presents special cases for the effects of substrate temperature, deposition rate, deposition bias, and target-substrate distance. In the third chapter, the paper discusses the case of multilayer deposition by using Ag/V multilayer as an example, and describes the effect of the deposition mechanism on the internal structure of the multilayer. As a conclusion to this chapter the authors discus coherency between layers of various multilayer films. In the fourth chapter, the authors discuss diffusion or miscibility of different metals in a multi-layered film submitted to irradiation by energetic particles.

The article is very well written, the effect of different deposition parameters and factors is clearly presented and discussed with a clear focus on irradiation phenomena which can play an important role in deposition of multi-layered thin films.

The review article is relevant to the scientific community as it addresses the issues occurring during deposition of multi-layered thin films with a special focus on deposition compatibility due to deposition mechanisms as well as diffusion occurring due to irradiation.

Comments for author File: Comments.pdf

Author Response

Point 1: The article submitted for review entitled “A review on the fabrication of multilayer films by magnetron sputtering and their irradiation behaviors” presents a detailed review of magnetron deposition parameters and their impact on the deposition of multilayer thin films. The paper presents special cases for the effects of substrate temperature, deposition rate, deposition bias, and target-substrate distance. In the third chapter, the paper discusses the case of multilayer deposition by using Ag/V multilayer as an example, and describes the effect of the deposition mechanism on the internal structure of the multilayer. As a conclusion to this chapter the authors discus coherency between layers of various multilayer films. In the fourth chapter, the authors discuss diffusion or miscibility of different metals in a multi-layered film submitted to irradiation by energetic particles.

The article is very well written, the effect of different deposition parameters and factors is clearly presented and discussed with a clear focus on irradiation phenomena which can play an important role in deposition of multi-layered thin films.

The review article is relevant to the scientific community as it addresses the issues occurring during deposition of multi-layered thin films with a special focus on deposition compatibility due to deposition mechanisms as well as diffusion occurring due to irradiation.

Response 1: We sincerely appreciate the reviewer for the careful review and positive comments on our manuscript. All the comments serve very well in improving the thoroughness of the paper.

Author Response File: Author Response.pdf

Reviewer 2 Report

This mini-review considers the effect of different deposition parameters, such as temperature, deposition rate, bias, target-substrate distance and layer thickness, on the microstructure, morphology and irradiation behavior of the multilayer films obtained by magnetron sputtering.

The problem addressed in this paper has been studied all over the world for more than 70 years, but this review is mainly focused on the recent contributions of the Chinese authors in this area (more than half of the papers cited), despite the large amount of the other works being omitted. For a more comprehensive review the authors should consider the papers written by the German, French, Soviet / Russian and other specialist during the last decades and discuss their own results within the context of the worldwide development of this problem. In this case this paper will become more interesting for the readership of Coatings.

The main disadvantage of this paper is a sloppy reference list with numerous incomplete and incorrect bibliographic data, careless and not uniform description of the literature sources cited, which make it impossible to establish whether the citation is reasonable and prevent the reviewer from checking the amount of self-citations. Hence, the reference list must be completely revised and expanded.

The English language of the manuscript is rather poor, so a serious proofreading is strongly recommended to avoid grammatical and stylistic mistakes.

After the above improvements this paper can be reconsidered for publication in Coatings.

Author Response

This mini-review considers the effect of different deposition parameters, such as temperature, deposition rate, bias, target-substrate distance and layer thickness, on the microstructure, morphology and irradiation behavior of the multilayer films obtained by magnetron sputtering.

Point 1: The problem addressed in this paper has been studied all over the world for more than 70 years, but this review is mainly focused on the recent contributions of the Chinese authors in this area (more than half of the papers cited), despite the large amount of the other works being omitted. For a more comprehensive review the authors should consider the papers written by the German, French, Soviet / Russian and other specialist during the last decades and discuss their own results within the context of the worldwide development of this problem. In this case this paper will become more interesting for the readership of Coatings.

Response 1: We very much appreciate the reviewer’s careful review and good suggestions. We have searched on Google Scholar with “magnetron sputtering” and “multilayer films” as keywords. Only nine results have been found from 1900 to 1950. Meanwhile, there are about 120 results from 1950 to 1980, in which only less than 1/5 of them investigated the effect of deposition parameters. However, it rises dozens of times in last ten years than before 1980. Therefore, in the present manuscript, we put our focus on the recent studies. We apologize for the confusion, and we have changed the manuscript title into “Recent studies on the fabrication of multilayer films by magnetron sputtering and their irradiation behaviors”.

In addition, we also found that nearly half of the recent studies were done by the Chinese authors in this area. Taking the articles published in 2021 as an example, we have carefully checked through Google Scholar, and among the first 500 results, the Chinese authors have contributed 223 related papers. Clearly, the Chinese authors definitely play significant roles in this area during the recent years. We have added some reference as following:

9. Ham, B.;  Junkaew, A.;  Arroyave, R.;  Chen, J.;  Wang, H.;  Wang, P.;  Majewski, J.;  Park, J.;  Zhou, H. C.;  Arvapally, R. K.;  Kaipa, U.;  Omary, M. A.;  Zhang, X. Y.;  Ren, Y.; Zhang, X., Hydrogen sorption in orthorhombic Mg hydride at ultra-low temperature. International Journal of Hydrogen Energy 2013,38(20), 8328-8341.
10. Webb, J. B.;  Lockwood, D.; Gnezdilov, V. J. J. o. c. g., Magnetron sputter epitaxy and characterization of InSb/In1− xAlxSb strained layer superlattices. 1994,137(3-4), 405-414.
11. Phythian, W. J.;  Stoller, R. E.;  Foreman, A. J. E.;  Calder, A. F.; Bacon, D. J., A comparison of displacement cascades in copper and iron by molecular dynamics and its application to microstructural evolution. Journal of Nuclear Materials 1995,223(3), 245-261.

Point 2: The main disadvantage of this paper is a sloppy reference list with numerous incomplete and incorrect bibliographic data, careless and not uniform description of the literature sources cited, which make it impossible to establish whether the citation is reasonable and prevent the reviewer from checking the amount of self-citations. Hence, the reference list must be completely revised and expanded.

Response 2: We sincerely apologize for the confusion. We have revised the citation thoroughly to avoid any mistakes.

Point 3: The English language of the manuscript is rather poor, so a serious proofreading is strongly recommended to avoid grammatical and stylistic mistakes.

Response 3: We appreciate the reviewer for the comment, the text has been completely checked for correct use of grammar and common technical terms. The detailed revisions are highlighted in Red in the revised manuscript.

Author Response File: Author Response.pdf

Reviewer 3 Report

The paper “A review on the fabrication of multilayer films by magnetron sputtering and their irradiation behaviors”, by Jinyang Ni, Jin Li, Jie Jian, Jianchao He, Hongsheng Chen, Xuesong Leng, Xiangli Liu, highlights the importance of magnetron sputtering in the frame of thin films deposition. The information is clear, and respects the manuscript template.

     The manuscript can be Accepted for publication with minor corrections. My comments are bellow.

1. Introduction: although it’s a review type manuscript, the introduction section should be more detailed, etc. The Introduction section it’s the state of the art of the manuscript, in this line, the authors are asked to improve this section.
2. Table 2: here it seems that table 2 is a picture, because it’s blurry; please insert a table style.
3. Figure 3: in graphs a, b and c- please increase the size of the text (peaks, graph lines names, etc); it’s too small.

Author Response

The paper “A review on the fabrication of multilayer films by magnetron sputtering and their irradiation behaviors”, by Jinyang Ni, Jin Li, Jie Jian, Jianchao He, Hongsheng Chen, Xuesong Leng, Xiangli Liu, highlights the importance of magnetron sputtering in the frame of thin films deposition. The information is clear, and respects the manuscript template.

     The manuscript can be Accepted for publication with minor corrections. My comments are bellow.

Point 1: Introduction: although it’s a review type manuscript, the introduction section should be more detailed, etc. The Introduction section it’s the state of the art of the manuscript, in this line, the authors are asked to improve this section.

Response 1: We appreciate the reviewer’s great comments and have revised the introduction as suggested. The major revisions are highlighted in Red in the revised manuscript:

Due to their unique structures with high-density interfaces, multilayer films have many advanced properties. For example, they are able to maintain high mechanical stability in extreme environments, such as severe tribological conditions with high temperature [1] and energetic particle irradiation [2-4]. W. L. Chen et al. described the high hardness and low friction coefficient of CrAlN/TiAlSiN multilayer films [1]. E. G. Fu et al. demonstrated that Cu/V interfaces effectively reduced the concentration of radiation-induced point defects [5]. In addition, multilayer films have been widely studied for various functional applications, such as hydrogen fuel cells [6, 7] and magnetic data storage [8, 9]. P. Chen et al. posited that Mg/MmM5 multilayer films have good prospects for the application of hydrogen fuel cells because of their synergetic effects [7]. A. M. et al. concluded that multilayer films, such as Co/Pt and Fe/Pt, have beneficial properties for magnetic data storage [9]. This review primarily focuses on multilayer films with metallic systems, whose irradiation behaviors are studied extensively.

Among numerous preparation methods, magnetron sputtering provides multiple advantages, including controllable properties, high efficiency, and favorable substrate–film bonding strength; as a result, the benefits of this method are widely exploited in the fabrication of multilayer films [10-13]. For instance, individual layer thickness, one of the most important parameters in determining the properties of multilayer films, can be readily adjusted during the sputtering process [14, 15]. Moreover, this method is also suitable for preparing alloy films and compounds with different compositions [16]. During the sputtering process, multiple parameters play important roles in the microstructure evolution of multilayer films, such as the deposition temperature, rate, and bias and the target–substrate distance. The influences of some parameters have been extensively studied, such as the deposition temperature and bias, whereas other parameters, such as the deposition rate, are not well understood [17-22].

Meanwhile, the individual layer thickness also exerts great impacts on the microstructure change of multilayer films, such as the flatness of interfaces, defect density, and coherency [23-26]. When the total thickness of the multilayer films is constant, the thinner the individual layer thickness, the higher the interface density, which may significantly affect many properties of films including the irradiation tolerance. During irradiation, a large population of point defects and larger defect clusters, such as dislocation networks and voids, are introduced into materials under the bombardment of energetic particles [27-32]. Such significant microstructure damages can cause swelling, hardening, embrittlement, and other problems in materials which significantly shorten their service life [33, 34]. The irradiation stability of a material can be strengthened through introducing defect sinks, such as grain boundaries (GBs) [35-38], twin boundaries (TBs) [39-45], free surface[46-52], which facilitate the recombination of irradiation-induced defects and defect clusters. It is well known that interfaces may also act as effective defect sinks [53]. and therefore, multilayer films with high-density layer interfaces are considered as irradiation-resistant materials and have been widely investigated [54-60]. Besides, multilayer films also have good mechanical properties, such as ductility, yield strength, hardness, etc., which can also be manipulated by changing the parameters during the fabrication process [61, 62].

In this review, we summarize the relationships between the preparation parameters and the microstructure evolution of multilayer films. In addition, the influences of individual layer thickness on the microstructure and irradiation behavior of multilayer films are discussed. We integrate extensive research efforts in relevant fields with the goal of providing researchers with a guide to develop advanced multilayer metal films with beneficial properties in the future.

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Point 2: Table 2: here it seems that table 2 is a picture, because it’s blurry; please insert a table style.

Response 2: Following the reviewer’s comment, we have changed Table 2 into a table style. Besides, we have also changed Table 1 and Table 3 to improve the clarity.

Table 1. The FWHM and interplanar spacing data obtained from the XRD curves of MgB₂/Mo multilayer films prepared at different temperatures [27].

Table 2. The average FWHM and SNR of the main peaks obtained from XRD curves of Cu/Nb multilayer films deposited at different temperatures and Cu deposition rates [2].

Table 3. The crystallite size of HA/Ag multilayer films prepared at different substrate temperatures and target–substrate distances [21].

Point 3: Figure 3: in graphs a, b and c- please increase the size of the text (peaks, graph lines names, etc); it’s too small.

Response 3: We apologize for the small font size. We have made revisions accordingly.

Figure 3. XRD patterns of (a-c) CrN/MoN [53] and (d-h) CrAlYN/CrN [23] multilayer films deposited at a series of biases, showing the change in film texture caused by changing deposition bias.

Author Response File: Author Response.pdf