Next Article in Journal
Enhanced Performance of Nickel–Cobalt Oxides as Selective Coatings for Flat-Plate Solar Thermal Collector Applications
Next Article in Special Issue
Microstructure and Wear Resistance of High-Chromium Cast Iron with Multicomponent Carbide Coating via Laser Cladding
Previous Article in Journal
Optimized Strain Response in (Co0.5Nb0.5)4+-Doped 76Bi0.5Na0.5TiO3-24SrTiO3 Relaxors
Previous Article in Special Issue
Effect of Substrate Bias Voltage on Microstructure and Mechanical Properties of Cr-Nb-Ti-Zr-N-O Ceramic Thin Films Produced by Reactive Sputtering
 
 
Search for Articles:
Title / Keyword
Author / Affiliation / Email
Journal
Article Type
 
 
Advanced Search
 
Section
Special Issue
Volume
Issue
Number
Page
 
Journals
Coatings
Volume 13
Issue 8
10.3390/coatings13081328
coatings-logo
Submit to this Journal Review for this Journal Propose a Special Issue
► Article Menu

Article Menu

share Share announcement Help format_quote Cite question_answer Discuss in SciProfiles thumb_up
...
Endorse textsms
...
Comment
first_page
settings
Order Article Reprints
Font Type:
Arial Georgia Verdana
Font Size:
Aa Aa Aa
Line Spacing:
Column Width:
Background:
Article

Determining the Annealing Temperature Dependency of Wetting and Mechanical Features on Fe3Si Films

by
Nattakorn Borwornpornmetee
1,
Chawapon Achirawongwat
1,
Thawichai Traiprom
2,
Bunpot Saekow
3,
Supanit Porntheeraphat
3,
Boonchoat Paosawatyanyong
4,
Tsuyoshi Yoshitake
5 and
Nathaporn Promros
1,*
1
Department of Physics, School of Science, King Mongkut’s Institute of Technology Ladkrabang, Bangkok 10520, Thailand
2
Program of Science for industry, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand
3
Digital Agriculture Technology Research Team, National Electronics and Computer Technology Center, Pathumthani 12120, Thailand
4
Department of Physics, Faculty of Science, Chulalongkorn University, Bangkok 10330, Thailand
5
Department of Advanced Energy Science and Engineering, Kyushu University, Fukuoka 816-8580, Japan
*
Author to whom correspondence should be addressed.
Coatings 2023, 13(8), 1328; https://doi.org/10.3390/coatings13081328
Submission received: 15 June 2023 / Revised: 24 July 2023 / Accepted: 25 July 2023 / Published: 28 July 2023
(This article belongs to the Special Issue Trends in Coatings and Surface Technology)
Browse Figures
Versions Notes

Abstract

:
The impact of thermal annealing under temperature alteration on the wetting and mechanical attributes of Fe3Si films built through facing target sputtering (FTS) is an essential topic for study in order to identify their characteristics under varying temperatures. Consequently, we introduced a thermal annealing process in a vacuum for two hours under varying temperatures of 300, 600, and 900 °C to our Fe3Si films created via FTS. The primary purpose of this current research is to examine the effect of the thermal annealing technique under temperature alteration on the wetting and mechanical traits of Fe3Si films. In this research, Fe3Si films were built onto the Si wafer by FTS and divided for use in thermal annealing under temperature alteration. The structural, morphological, wetting, and mechanical traits of the Fe3Si films under thermal annealing are provided in the present work. Based on our information, this work represents an original study on the change in wetting and mechanical traits of Fe3Si films through thermal annealing under temperature alteration.

1. Introduction

Ferromagnetic silicide (Fe3Si), composed of naturally available materials (Si and Fe), is known to be appealing in the plausible application of spin transistors and self-cleaning surfaces [1,2,3,4]. Prior related studies show that the epitaxial production of Fe3Si films onto 111-oriented Si wafers can be achieved via the usage of facing target sputtering (FTS) [5,6]. The Fe3Si films own the 4.2% misfit of the lattice parameter for Si and three different bcc-like structures (D03, B2, A2) for Fe3Si to exist [5,6]. The Fe3Si films possess a striking magnetic attribute of a small coercive field (7.5 Oe) and a high spin polarization (45%) [7,8,9]. They also own a noticeable thermal stability above an 800 K Curie temperature [7,8,9]. The Fe3Si films own corrosion resistance and a high degree of hardness [10,11,12]. With these promising attributes, Fe3Si is a plausible candidate for ferromagnetic material, self-cleaning surfaces, and hard coatings [1]. The magnetic and structural attributes of Fe3Si films have been explored and reported in prior studies [2,3,4]. Nevertheless, the wettability and mechanical attributes of the Fe3Si films including the influence of an annealing temperature have barely been studied until now.
Upon a review of previous studies, the research team involved in this current work reported the epitaxial production of the Fe3Si film layer onto 111-oriented Si wafers utilizing the FTS appliance [1,2,3,4]. In principle, the FTS appliance has two equally sized circular targets facing each other, placed far from a substrate holder [13,14,15,16]. The advantages of the FTS are that it creates high plasma density, operates under low pressure, suffers little plasma damage, has a smooth surface, and exhibits little stoichiometry change [13,14,15,16]. The influence of temperature heated at the substrate on Fe3Si film growth was formerly studied [3]. At a substrate temperature of 300 °C, the crystallinity of Fe3Si films increased and retained its phase [3]. Xie et al. [17] reported dependency on the annealing temperature of Fe3Si film’s properties. The Fe3Si films are fabricated onto SiO2 by resistive thermal evaporation and annealed at temperatures ranging from 700 to 950 °C. The films initially possessed a crystalline structure of Fe0.9Si1 and then developed into that of the Fe3Si phase after annealing at 850 °C or higher. In comparison, our method of FTS epitaxy could form Fe3Si at room temperature without the need for annealing. Recently, the author reported the employment of argon (Ar) plasma etching by varying the etching power to modify the surface as well as the chemical composition over the surface of Fe3Si films [1]. The hydrophobic behavior of the untreated Fe3Si layer surface was found to turn into a hydrophilic surface through etching at 150 W of power [1]. Nevertheless, the surface property of Fe3Si films needs to be further studied to identify its novel characteristics.
Based on the literature review, thermal annealing plays a primary role in modifying the physical attributes of thin films, such as enhancing the crystallinity, crystallite size, and surface roughness of the films as well as wettability [18,19,20,21]. According to a previous report, Raj et al. annealed the BFO thin films under different annealing times, resulting in the increment of grain size and roughness as the temperature increased [19]. Bazhan et al. reported the influence of different annealing temperatures on the wettability of iron oxide films [20]. An increment in temperature induces the transition of the phase and surface topology of iron oxide films, increasing the contact angle of the film’s surface [20]. Until now, reports on the influence of annealing as an extension of the wettability and mechanical attributes of Fe3Si films created utilizing FTS are extremely scarce.
The influence of temperature in the annealing procedure on the wettability and mechanical attributes of Fe3Si films is an essential topic for study to provide their annealing characteristics under varying temperatures. Thus, the characteristics of the Fe3Si film attributes after annealing in a vacuum for two hours at different annealing temperatures of 300 °C, 600 °C, and 900 °C are revealed in the current study. To the best of the author’s information and knowledge, this current study is the first on the characteristics of wettability and mechanical attributes of Fe3Si films after annealing at different temperatures.

2. Materials and Methods

2.1. Production of Fe3Si Films

The n-type 111-oriented Si wafer (SUMCO Corporation) with a resistivity of 1000–4000 ohm·cm was used as a substrate for producing the Fe3Si film. The oils and organic residues on the Si sample were cleaned utilizing two acetone and methanol solvents obtained from the Fujifilm Wako Pure Chemical Corporation. Next, the native silicon dioxide on the Si sample surface was removed using 1% hydrofluoric acid. Deionized water was then employed to rinse the hydrofluoric acid from the Si sample surface. Finally, nitrogen gas (99.999% purity) obtained from the Iwatani Corporation was used for blow drying the Si wafer. Two equally sized circular Fe3Si alloy targets (99.9% purity) purchased from TOSHIMA Manufacturing Co., Ltd. were used in the sputtering process. A rotary pump (model: CIT-Alcatel 2030C) obtained from Alcatel Japan and a turbo molecular pump (model: TG1003) obtained from Osaka Vacuum were used to vacuumize the FTS chamber for sputtering. For the Fe3Si deposition procedure, the base pressure was achieved with a value below 3 × 10−5 Pascal. A sputtering pressure with a value of 1.33 × 10−1 Pascal was achieved after feeding Ar gas (99.9999% purity) obtained from the Iwatani Corporation into the inside of the FTS chamber. The Ar gas flow rate was 15 sccm. The temperature at the rear of the Si sample was fixed at 300 °C through the temperature controller (model: E5CN) purchased from OMRON. A voltage of 1 kV for the gas discharge process was fixed via a DC power source (model: HD1K-30N) purchased from Micro Denshi. A current of around 1.2 mA was generated during the sputtering process. After sputtering for 24 h, the rate of Fe3Si film production was 0.57 nm/min. The low pressure and low deposition rate during sputtering are the key that allows FTS to precisely coat Fe3Si at low temperatures as reported by our past work, where K. Sakai et. al. were able to epitaxially coat the Fe3Si on FeSi2 with a deposition rate of 0.62 nm/min at an ambient temperature [4]. This precision and energy allow the epitaxy mechanism to occur without the need for external thermal energy [2].

2.2. Post Annealing of Fe3Si Films

After completing the sputtering process, the Fe3Si films were separated into four pieces in the case of non-annealing and annealing at 300 °C, 600 °C, and 900 °C temperatures. In the annealing process, the Fe3Si films were positioned on the inside of the quartz tube. Through the operation of a mechanical pump (Leybold, Bonner, Germany, Trivac D2.5) and a turbomolecular pump (Leybold, TW70 H), the base pressure inside the quartz tube was vacuumized below 3 × 10−6 mbar. The temperature and annealing period were set through the temperature controller (Shimaden, SR53, Tokyo, Japan). The period for annealing under the current study conditions was two hours.

2.3. Investigation of the Properties of Fe3Si Films

An X-ray diffractometer (XRD; Model: Rigaku, TTRAX III, Tokyo, Japan) was utilized to investigate the crystallographic features of the as-produced and annealed Fe3Si films. The measurement was performed in the grazing incidence mode (2θ scan) with a fixed incidence angle of 2°. To confirm the crystallinity, the crystallite size was simulated using JADE software by a function of Scherrer’s equation. A SU 8230 Field Emission Scanning Electron Microscope (FESEM, Hitachi, Tokyo, Japan) and an XE-120 Atomic Force Microscope (AFM, Park Systems, Suwon, Korea) were employed to investigate the morphology and roughness of the as-produced and annealed Fe3Si film surface. The Hitachi S-4700 Scanning Electron Microscope was utilized to study the cross-sectional view of as-produced and annealed Fe3Si films. The Contact Angle OCA 20 appliance (DataPhysics, San Jose, CA, USA) was used to measure the contact angles of the unannealed and annealed Fe3Si film surface. A nanoindenter (model: Ti premier) obtained from Bruker’s Hysitron (Minneapolis, MN, USA) was employed to measure the mechanical attributes of the non-annealing and annealing Fe3Si films.

3. Results and Discussion

3.1. XRD Results of Fe3Si Films

The measured XRD patterns of the Fe3Si films without annealing and under the annealing procedure with fixed temperatures of 300 °C, 600 °C, and 900 °C are shown in Figure 1, while the list of preferred orientation of Fe-Si based materials can be referred in Table 1. In the case of Fe3Si films without annealing, the preferred crystal orientations of Fe3Si (111), Fe3Si (220), Fe3Si (222), Fe3Si (400), and Fe3Si (422) were observed at 28.50°, 44.38°, 56.28°, 64.72°, and 82.06°, respectively [2,3,11]. The strongly preferred orientations of Fe3Si (222) in comparison to the fundamental peaks of Fe3Si (111), Fe3Si (220), Fe3Si (400), and Fe3Si (422) indicate that the film’s structure was predominantly occupied by a B2 structure superlattice [2]. Among homogeneous iron silicide phases of different stoichiometry, Fe3Si is the sole well-ordered phase of the Fe-rich composition. As shown in Figure 2, Fe3Si exists in the bulk phase at room temperature and is stable from there up to the melting point [5]. Hypothetically, Fe3Si with a different order of Si atom arrangement, such as the B2 structure, can also have similar properties to D03. The B2 (= CsCl) phase, where either Fe or Si randomly occupy the C sites and B sites, will replace the D03 phase when the Si concentration is below the threshold [5,6]. In our work, we formed the Fe3Si at room temperature to prevent the inter-diffusion of Fe to Si from thermal energy, resulting in a B2 structure [2]. At an annealing temperature of 300 °C, the obtained preferential orientations were observed to be in the same positions as without annealing. However, an increase in peak intensity was detected after annealing at 300 °C. This is due to the Fe atoms gaining activation energy by annealing, allowing lower surface energy atoms to diffuse to a site in the crystal lattice with favorable energy [18]. Afterward, the crystallites grew in the preferred direction and the crystallinity of the film was improved [18]. After annealing at 600 °C, an intense peak of Si (111) was clearly observed at 28.44°. In contrast, the peak intensity of Fe3Si (111) and Fe3Si (222) disappeared. After gradually providing thermal energy by conventional annealing, the structure implied to undergo a transition into a D03 structure [6]. The peak of the semiconducting phase (β-FeSi2) of β (202)/(220) at 29.12° also appeared [22,23,24,25]. Since Fe has a significantly higher diffusion coefficient than Si, the Fe atoms could diffuse into the Si layer with the application of sufficient diffusion energy [26,27,28]. Therefore, an improvement in the crystallinity of the film along with the phase transition was observed during annealing at 600 °C [26,27,28]. Subsequently, the crystalline orientation shifted further with a higher activation energy from annealing at 900 °C. The β (202)/(220) evolved dramatically, causing a superposition between itself and Si(111). At the same time, several peaks of β (400), β (331), β (422), and β (333) appeared at 34.72, 45.20, 49.80, and 58.90°, respectively [22,29]. When annealing further, the sample at the phase above the ideal Si concentration of the D03 structure can retain the phase from the boundary of 26% at RT to 31% at 1200 °C, even when an absurd phase transition occurs [5]. The FeSi phase will only appear when the Fe and Si atom’s structure themselves in the almost 1:1 composition [5,6]. Meanwhile, the β phase could mainly form when Si concentration is around 67% at temperatures below 950 °C. Also, the β phase could appear with periodic stoichiometry deviations after atomic segregation and diffusion at the Fe3Si surface [5]. According to the estimation, the crystallite size of the Fe3Si films without annealing was 22.69 nm. The estimated values for the crystallite size were improved to 33.97, 34.71, and 37.98 nm under fixed annealing temperatures of 300 °C, 600 °C, and 900 °C, respectively. In contrast to the result reported by Xie et al. [17], the annealing reduces our film’s Fe3Si structure rather than enhances the structure. This should be taken into account that our circumstances are wildly different since our films were B2 structured Fe3Si on Si (111) substrate. The combination of the high diffusion coefficient of Fe in Si combined with the structure defect allows our films to phase shift to compensate for those downsides [30,31]. On the other hand, Xie et al.’s sample was bcc-structured Fe3Si resulting from the 700 °C annealing of the thermally evaporated sample on the SiO2 before turning into fcc-structured Fe3Si by thermal annealing of 950 °C [17]. Si has a high diffusion coefficient against the SiO2, while diffusion rate of Fe against SiO2 is dwarfed by that of Fe against Si [32,33]. Hence, the misaligned Fe-Si structure and stoichiometry of the evaporated films were corrected resulting in enhancement by increasing the temperature rather than a phase shifting through interdiffusion like in our case [34].

3.2. FESEM Results of Fe3Si films

The FESEM images of the surface morphology together with cross sections of Fe3Si films without annealing and annealed under various temperatures are displayed in Figure 3. From the FESEM images in plane view, the Fe3Si films without annealing and annealing at 300 °C exhibited a smooth surface consisting of many tiny uniform crystallites. The tiny crystallites with surface uniformity merged together and became nanocrystalline clusters with an annealing temperature of 600 °C. In addition, a void increment can be observed in the midst of the generated nanocrystalline clusters. At an annealing temperature of 900 °C, many tiny crystallites were completely clustered, leading to many bigger clusters. Xie et al. [17] also report a significant change of surface morphology after annealing, where their Fe3Si films possess an island-like morphology at 700 °C similar to ours at 600 °C. Then, 950 °C turns separated crystallites into clustered, like we observe at 900 °C.
The FESEM cross-sectional images of the Fe3Si films for non-annealing and annealing at a temperature of 300 °C showed a sharp interface between the produced films and the Si wafers. In addition, the unannealed Fe3Si films exhibited a smooth surface which changes slightly after annealing at 300 °C. After annealing at 600 °C and 900 °C, the interface became uneven. A rough surface on the Fe3Si films can be observed due to the creation of several big clustered crystalline structures together with pinholes on the Fe3Si film surface.

3.3. AFM Results of Fe3Si Films

AFM topographic images of the Fe3Si film surface in the case of non-annealing and annealed under temperature values set at 300 °C, 600 °C, and 900 °C are depicted in Figure 4. For non-annealing Fe3Si film, an extremely smooth surface was observed with an estimated root-mean-square (RMS) roughness of 0.588 nm as shown in Table 2. In the case of film fabrication via FTS, the plasma zone was far from the Si wafer on the substrate holder [13,14,15,16]. Thus, the plasma caused very little damage by plasma to the Fe3Si film surface [13,14,15,16]. The temperature of the film surface during film production did not increase. For these reasons, the Fe3Si film surface was quite smooth. After annealing at 300 °C, the RMS roughness increased slightly to 0.743 nm. The RMS roughness increased dramatically to 98.235 and 113.361 nm under annealing temperatures fixed at 600 °C and 900 °C, respectively. Based on the FESEM images, big clusters and pinholes were formed in the case of annealing temperatures set at 600 °C and 900 °C. Thus, the Fe3Si film surfaces after annealing under these temperatures were rougher than those under lower temperatures and non-annealing.

3.4. Contact Angles of Fe3Si Films

In this work, the measurement of the contact angle in the midst of the droplet and the Fe3Si film surface was carried out to determine the wetting behavior of the Fe3Si film surface under annealed and unannealed conditions. Normally, the hydrophilicity can be defined by the acquired contact angle values measured in the range of 10° < θ < 90° [35,36,37]. For hydrophobicity, the measured contact angle values are in the range of 90° < θ < 150° [35,36,37]. Superhydrophilic and superhydrophobic are defined as the values of the contact angle measured in the range of θ < 10° and θ > 150°, respectively [35,36,37].
The contact angles in the midst of the droplet and surface for the as-produced and annealed Fe3Si films are displayed in Figure 5. The contact angles of the Fe3Si film surface without annealing and with annealing at 300 °C were 95.8° and 95.5°, respectively. These contact angle values show that the Fe3Si film surfaces are hydrophobic under these conditions. Several porous regions between the crystallites can be seen on the FESEM image of the unannealed and annealed Fe3Si films at 300 °C. According to the model of Cassie and Baxter, the porous region performs like an air pocket, allowing air to enter the grooves and assist in the buoyancy of the liquid [38,39]. This leads to a higher contact angle value than for a flat surface. A decrement in contact angles was found with annealing under fixed temperatures of 600 °C and 900 °C with values of 80.6° and 77.9°, respectively. This suggests the transition from the Cassie and Baxter model to the Wenzel model for the Fe3Si film surface [40,41]. The spaces in the midst of the nanostructures are filled by water since a water/solid interface is more desirable than an air/solid interface at high annealing temperatures [40,41]. Hence, the droplet bottom possesses conformal contact with the solid surface [40,41]. This can increase the interfacial force between solids and water on the surface, leading to a decrement in the contact angle value. Therefore, the contact angles of annealed films reduced with the significantly increasing roughness are shown in Figure 5e, depicting the correlation between the contact angles and roughness of annealed films. The contact angle values of non-annealing Fe3Si films and annealing at different annealing temperatures were summarized in Table 3.

3.5. Nanoindentation Results of Fe3Si Films

A nanoindentation appliance was used with a Berkovich indenter to assess the average hardness (H) and reduced elastic modulus (Er) values for the surfaces of annealed and unannealed Fe3Si films. The applied indentation load was 3 mN and the fixed maximum depth was 10% of the Fe3Si films’ thickness. Figure 6 demonstrates the applied indentation load versus the depth plot for the Fe3Si films without annealing and through annealing under temperature values of 300 °C, 600 °C, and 900 °C. The values of H and Er of the annealed and unannealed Fe3Si layer surfaces were extracted from the unloading portions of their curve of load–depth [42,43]. The acquired H and Er values for the experimental conditions in this study are displayed in Table 4. The H value of unannealed Fe3Si film was 8.741 GPa. The Fe3Si films exhibited an increment in hardness values of 9.363, 14.543, and 15.341 GPa under fixed annealing temperatures of 300 °C, 600 °C, and 900 °C, respectively. An increase in the annealing temperature can enhance the grain size of the Fe3Si films. This developed grain may affect the nanoindentation mechanism by dislocation through grain boundary sliding [44,45,46]. Hence, the hardness result trending in the same manner as the inverse Hall–Petch effect relies heavily on the grain boundary structure of the testing material [44,45,46]. This sudden change in the film’s morphology may also be linked to inconsistency in the hardness [47]. The Er value of Fe3Si films without annealing was approximately 184.899 GPa. The Er value exhibited the same rising trend as the hardness. In other words, the value of Er increased along with the annealing temperature. The Er values of 204.803, 271.261, and 323.187 GPa were obtained for Fe3Si films annealed at 300 °C, 600 °C, and 900 °C, respectively. The Er tends to follow the crystal orientation of the crystalline materials, aligning with the XRD results in this study [44].

4. Conclusions

This study reveals the results of the thermal annealing process under fixed temperatures of 300 °C, 600 °C, and 900 °C for the modification of wettability, surface morphology, and mechanical attributes of Fe3Si films produced through FTS. According to the XRD measurement, several preferred crystal orientations can be observed for Fe3Si films without annealing and those annealed at 300 °C. Higher crystallinity and several preferred crystal orientations appeared in the 600 °C and 900 °C annealed Fe3Si films. According to the FESEM results, the Fe3Si films without annealing and those annealed under a fixed temperature of 300 °C exhibited a significant number of little uniform nanocrystallites. At an annealing temperature of 600 °C, they merged into little nanocrystalline clusters, huddling to generate large clusters at 900 °C. The acquired AFM images indicate that Fe3Si films without annealing and with an annealing temperature of 300 °C own a very smooth surface, having a small rms roughness which increased dramatically by annealing at temperatures above 300 °C. The average contact angle for the surface of the Fe3Si films without annealing and with annealing exhibited hydrophobic properties. It became hydrophilic after annealing at temperatures above 300 °C. The film hardness of the as-formed Fe3Si was significantly enhanced after annealing above 300 °C. It can therefore be concluded that an annealing temperature above 300 °C significantly alters the structural, morphological, wettability, and mechanical attributes of Fe3Si films.

Author Contributions

Conceptualization, N.P.; methodology, N.B., B.S., S.P. and N.P.; formal analysis, N.B., T.T. and N.P.; investigation, N.B., C.A., T.T. and N.P.; writing—original draft preparation, N.B., T.T. and N.P.; writing—review and editing, N.B., T.T., B.S., S.P., B.P., T.Y. and N.P.; Visualization, N.B., C.A., T.T. and N.P.; Supervision, B.P. and T.Y. All authors have read and agreed to the published version of the manuscript.

Funding

This work is supported by King Mongkut’s Institute of Technology Ladkrabang (grant numbers KDS2022-06). The allowance for carrying out this research was provided by the Academic Research Fund, School of Science, King Mongkut’s Institute of Technology Ladkrabang, with grant numbers 2562-01-05-29, 2562-01-05-44, and 2563-02-05-36.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The data presented in this study are available in this article.

Acknowledgments

This work is supported by King Mongkut’s Institute of Technology Ladkrabang. The authors also express their gratitude for the contribution and cooperation received from Research Unit of Integrated Science for Electronic, Material and Industry (ISEMI), School of Science, King Mongkut’s Institute of Technology Ladkrabang.

Conflicts of Interest

The authors declare no conflict of interest.

References

  1. Borwornpornmetee, N.; Charoenyuenyao, P.; Chaleawpong, R.; Paosawatyanyong, B.; Phatthanakun, R.; Sittimart, P.; Aramaki, K.; Hamasaki, T.; Yoshitake, T.; Promros, N. Physical Properties of Fe3Si Films Coated through Facing Targets Sputtering after Microwave Plasma Treatment. Coatings 2021, 11, 923. [Google Scholar] [CrossRef]
  2. Yoshitake, T.; Nakagauchi, D.; Ogawa, T.; Itakura, M.; Kuwano, N.; Tomokiyo, Y.; Kajiwara, T.; Nagayama, K. Room-Temperature Epitaxial Growth of Ferromagnetic Fe3Si Films on Si(111) by Facing Target Direct-Current Sputtering. Appl. Phys. Lett. 2005, 86, 262505. [Google Scholar] [CrossRef]
  3. Nakagauchi, D.; Yoshitake, T.; Nagayama, K. Fabrication of Ferromagnetic Fe3Si Thin Films by Pulsed Laser Deposition Using an Fe3Si Target. Vacuum 2004, 74, 653–657. [Google Scholar] [CrossRef]
  4. Sakai, K.; Noda, Y.; Tsumagari, D.; Deguchi, H.; Takeda, K.; Yoshitake, T. Temperature-Dependent Interlayer Coupling in Fe3Si/FeSi2 Artificial Lattices. Phys. Status Solidi (A) Appl. Mater. Sci. 2014, 211, 323–328. [Google Scholar] [CrossRef]
  5. Starke, U.; Schardt, J.; Weiss, W.; Meier, W.; Polop, C.; de Andres, P.L.; Heinz, K. Structural and Compositional Reversible Phase Transitions on Low-Index Fe3Si Surfaces. Europhys. Lett. 2001, 56, 822. [Google Scholar] [CrossRef] [Green Version]
  6. Gude, A.; Mehrer, H. Diffusion in the D03-Type Intermetallic Phase Fe3Si. Philos. Mag. A 1997, 76, 1–29. [Google Scholar] [CrossRef]
  7. Sadoh, T.; Takeuchi, H.; Ueda, K.; Kenjo, A.; Miyao, M. Epitaxial Growth of Ferromagnetic Silicide Fe3Si on Si(111) Substrate. Jpn. J. Appl. Phys. 2006, 45, 3598. [Google Scholar] [CrossRef]
  8. Hamaya, K.; Ueda, K.; Kishi, Y.; Ando, Y.; Sadoh, T.; Miyao, M. Epitaxial Ferromagnetic Fe3Si/Si(111) Structures with High-Quality Heterointerfaces. Appl. Phys. Lett. 2008, 93, 132117. [Google Scholar] [CrossRef] [Green Version]
  9. Herfort, J.; Schönherr, H.-P.; Ploog, K.H. Epitaxial Growth of Fe3Si/GaAs(001) Hybrid Structures. Appl. Phys. Lett. 2003, 83, 3912–3914. [Google Scholar] [CrossRef]
  10. Tang, C.; Wen, F.; Chen, H.; Liu, J.; Tao, G.; Xu, N.; Xue, J. Corrosion Characteristics of Fe3Si Intermetallic Coatings Prepared by Molten Salt Infiltration in Sulfuric Acid Solution. J. Alloys Compd. 2019, 778, 972–981. [Google Scholar] [CrossRef]
  11. Chang-bin, T.; Hong-xia, C.; Fu-rong, W.; Ni-jun, X.; Wei, H.; Juan-qin, X. Facile Preparation and Tribological Property of Alloyed Fe3Si Coatings on Stainless Steels Surface by Molten-Salt Infiltration Method. Surf. Coat. Technol. 2020, 397, 126049. [Google Scholar] [CrossRef]
  12. Schneeweiss, O.; Pizúrová, N.; Jirásková, Y.; Žák, T.; Cornut, B. Fe3Si surface coating on SiFe steel. J. Magn. Magn. Mater. 2000, 215, 115–117. [Google Scholar] [CrossRef]
  13. Lee, M.; Park, Y.; Kim, K.; Hong, J. Influence of Sputtering Conditions on the Properties of Aluminum-Doped Zinc Oxide Thin Film Fabricated Using a Facing Target Sputtering System. Thin Solid Film. 2020, 703, 137980. [Google Scholar] [CrossRef]
  14. Tominaga, K.; Ueda, T.; Ao, T.; Kataoka, M.; Mori, I. ITO Films Prepared by Facing Target Sputtering System. Thin Solid Films 1996, 281–282, 194–197. [Google Scholar] [CrossRef]
  15. Hossain, M.F.; Biswas, S.; Takahashi, T.; Kubota, Y.; Fujishima, A. Influence of Direct Current Power on the Photocatalytic Activity of Facing Target Sputtered TiO2 Thin Films. Thin Solid Film. 2008, 517, 1091–1095. [Google Scholar] [CrossRef]
  16. Jeong, J.A.; Shin, H.S.; Choi, K.H.; Kim, H.K. Flexible Al-Doped ZnO Films Grown on PET Substrates Using Linear Facing Target Sputtering for Flexible OLEDs. J. Phys. D Appl. Phys. 2010, 43, 465403. [Google Scholar] [CrossRef]
  17. Xie, J.; Xie, Q.; Ma, R.; Huang, J.; Zhang, C.; Liu, D. Annealing Temperature Dependent Structures and Properties of Ferromagnetic Fe3Si Films Fabricated by Resistive Thermal Evaporation. J. Mater. Sci. Mater. Electron. 2018, 29, 1369–1376. [Google Scholar] [CrossRef]
  18. Ng, Z.-N.; Chan, K.-Y.; Tohsophon, T. Effects of Annealing Temperature on ZnO and AZO Films Prepared by Sol–Gel Technique. Appl. Surf. Sci. 2012, 258, 9604–9609. [Google Scholar] [CrossRef]
  19. Raj, C.A.; Muneeswaran, M.; Jegatheesan, P.; Giridharan, N.V.; Sivakumar, V.J.; Senguttuvan, G. Effect of Annealing Time in the Low-Temperature Growth of BFO Thin Films Spin Coated on Glass Substrates. J. Mater. Sci. Mater. Electron. 2013, 24, 4148–4154. [Google Scholar] [CrossRef]
  20. Bazhan, Z.; Ghodsi, F.E.; Mazloom, J. Effect of Phase Transition Induced by Annealing Temperature on Wettability, Optical and Photocatalytic Properties of Nanostructured Iron Oxide Thin Film. J. Mater. Sci. Mater. Electron. 2018, 29, 11489–11497. [Google Scholar] [CrossRef]
  21. Gojda, F.; Loulakis, M.; Papoutsakis, L.; Tzortzakis, S.; Chrissopoulou, K.; Anastasiadis, S.H. Altering the Surface Properties of Metal Alloys Utilizing Facile and Ecological Methods. Langmuir 2022, 38, 4826–4838. [Google Scholar] [CrossRef]
  22. Terai, Y.; Yoneda, K.; Noda, K.; Miura, N.; Fujiwara, Y. Effect of Residual Impurities on Transport Properties of β-FeSi2 Epitaxial Films Grown by Molecular Beam Epitaxy. J. Appl. Phys. 2012, 112, 13702. [Google Scholar] [CrossRef]
  23. Tode, M.; Takigawa, Y.; Ohmukai, M.; Kurosawa, K.; Muroya, M. Epitaxially Growth of β-FeSi2 Thin Films on Si(100) Substrates from ε-FeSi Targets with ArF Excimer Laser Deposition. J. Phys. Conf. Ser. 2007, 59, 376–379. [Google Scholar] [CrossRef]
  24. Shimura, K.; Katsumata, T.; Yamaguchi, K.; Yamamoto, H.; Hojou, K. The Role of Sputter Etching and Annealing Processes on the Formation of β-FeSi2 Thin Films. Thin Solid Films 2004, 461, 22–27. [Google Scholar] [CrossRef]
  25. Nishikawa, Y.; Hiehata, K.; Nakamura, K. Reduction of Surface Cracks in β-FeSi2 Films by Substrate Heating during RF-Sputtering Deposition. Trans. Mat. Res. Soc. Jpn. 2013, 38, 243–247. [Google Scholar] [CrossRef]
  26. Lakshantha, W.J.; Dhoubhadel, M.S.; Reinert, T.; McDaniel, F.D.; Rout, B. Investigation of Various Phases of Fe–Si Structures Formed in Si by Low Energy Fe Ion Implantation. Nucl. Instrum. Methods Phys. Res. B 2015, 365, 114–119. [Google Scholar] [CrossRef]
  27. Baldwin, N.R.; Ivey, D.G. Iron Slicide Formation in Bulk Iron-Silicon Diffusion Couples. J. Phase Equilibria 1995, 16, 300–307. [Google Scholar] [CrossRef]
  28. Li, M.; Chen, X.; Guan, J.; Wang, J.; Liang, C. Thermally Induced Phase Transition and Magnetic Properties of Fe–FeSi2 with Core–Shell Structure. Phys. Status Solidi (A) 2013, 210, 2710–2715. [Google Scholar] [CrossRef]
  29. Tian, Y.; Bento Montes, A.R.; Vančo, Ľ.; Čaplovičová, M.; Vogrinčič, P.; Šutta, P.; Satrapinskyy, L.; Zeman, M.; Isabella, O. Toward BaSi2/Si Heterojunction Thin-Film Solar Cells: Insights into Heterointerface Investigation, Barium Depletion, and Silicide-Mediated Silicon Crystallization. Adv. Mater. Interfaces 2020, 7, 2000887. [Google Scholar] [CrossRef]
  30. Isobe, T.; Nakashima, H.; Hashimoto, K. Diffusion Coefficient of Interstitial Iron in Silicon. Jpn. J. Appl. Phys. 1989, 28, 1282. [Google Scholar] [CrossRef]
  31. Mehrer, H. Diffusion in Intermetallics. Mater. Trans. JIM 1996, 37, 1259–1280. [Google Scholar] [CrossRef] [Green Version]
  32. Béjina, F.; Jaoul, O. Silicon Self-Diffusion in Quartz and Diopside Measured by Nuclear Micro-Analysis Methods. Phys. Earth Planet. Inter. 1996, 97, 145–162. [Google Scholar] [CrossRef]
  33. Ramappa, D.A.; Henley, W.B. Diffusion of Iron in Silicon Dioxide. J. Electrochem. Soc. 1999, 146, 3773. [Google Scholar] [CrossRef]
  34. Inaba, T.; Saito, Y.; Kominami, H.; Nakanishi, Y.; Murakami, K.; Matsuyama, T.; Tatsuoka, H. Growth of SiOx Nanofibers Using FeSi Substrates with Ga Droplets. Jpn. J. Appl. Phys. 2006, 45, L1320. [Google Scholar] [CrossRef]
  35. Drelich, J.; Chibowski, E.; Meng, D.D.; Terpilowski, K. Hydrophilic and Superhydrophilic Surfaces and Materials. Soft Matter 2011, 7, 9804–9828. [Google Scholar] [CrossRef]
  36. Krasowska, M.; Zawala, J.; Malysa, K. Air at Hydrophobic Surfaces and Kinetics of Three Phase Contact Formation. Adv. Colloid Interface Sci. 2009, 147–148, 155–169. [Google Scholar] [CrossRef]
  37. Mohamed, A.M.A.; Abdullah, A.M.; Younan, N.A. Corrosion Behavior of Superhydrophobic Surfaces: A Review. Arab. J. Chem. 2015, 8, 749–765. [Google Scholar] [CrossRef] [Green Version]
  38. Cassie, A.B.D.; Baxter, S. Wettability of Porous Surfaces. Trans. Faraday Soc. 1944, 40, 546–551. [Google Scholar] [CrossRef]
  39. Lafuma, A.; Quéré, D. Superhydrophobic States. Nat. Mater. 2003, 2, 457–460. [Google Scholar] [CrossRef] [PubMed]
  40. Wenzel, R.N. Surface Roughness and Contact Angle. J. Phys. Colloid Chem. 1949, 53, 1466–1467. [Google Scholar] [CrossRef]
  41. Quéré, D. Wetting and Roughness. Annu. Rev. Mater. Res 2008, 38, 71–99. [Google Scholar] [CrossRef]
  42. Beegan, D.; Chowdhury, S.; Laugier, M.T. Comparison between Nanoindentation and Scratch Test Hardness (Scratch Hardness) Values of Copper Thin Films on Oxidised Silicon Substrates. Surf. Coat. Technol. 2007, 201, 5804–5808. [Google Scholar] [CrossRef]
  43. Fischer-Cripps, A.C. A Review of Analysis Methods for Sub-Micron Indentation Testing. Vacuum 2000, 58, 569–585. [Google Scholar] [CrossRef]
  44. Torrents, A.; Yang, H.; Mohamed, F.A. Effect of Annealing on Hardness and the Modulus of Elasticity in Bulk Nanocrystalline Nickel. Metall. Mater. Trans. A 2010, 41, 621–630. [Google Scholar] [CrossRef] [Green Version]
  45. Swygenhoven, H. Van Grain Boundaries and Dislocations. Science (1979) 2002, 296, 66–67. [Google Scholar] [CrossRef]
  46. Chen, J.; Wang, W.; Qian, L.H.; Lu, K. Critical Shear Stress for Onset of Plasticity in a Nanocrystalline Cu Determined by Using Nanoindentation. Scr. Mater. 2003, 49, 645–650. [Google Scholar] [CrossRef]
  47. Chen, L.; Ahadi, A.; Zhou, J.; Ståhl, J.-E. Modeling Effect of Surface Roughness on Nanoindentation Tests. Procedia CIRP 2013, 8, 334–339. [Google Scholar] [CrossRef] [Green Version]
Coatings 13 01328 g001 550
Figure 1. The measured XRD spectra of non-annealed Fe3Si film along with annealed Fe3Si films at 300 °C, 600 °C, and 900 °C.
Figure 1. The measured XRD spectra of non-annealed Fe3Si film along with annealed Fe3Si films at 300 °C, 600 °C, and 900 °C.
Coatings 13 01328 g001
Coatings 13 01328 g002 550
Figure 2. Phase diagram of Fe-Si material as a function of temperature versus Si atomic concentration.
Figure 2. Phase diagram of Fe-Si material as a function of temperature versus Si atomic concentration.
Coatings 13 01328 g002
Coatings 13 01328 g003a 550Coatings 13 01328 g003b 550
Figure 3. FESEM images of Fe3Si film surfaces (a) without annealing and annealing (b) 300 °C, (c) 600 °C, (d) 900 °C in plane-view. The cross-sectional images of Fe3Si films present in (e) for unannealed films along with (f) for 300 °C annealed films, (g) for 600 °C annealed films, and (h) for 900 °C annealed films.
Figure 3. FESEM images of Fe3Si film surfaces (a) without annealing and annealing (b) 300 °C, (c) 600 °C, (d) 900 °C in plane-view. The cross-sectional images of Fe3Si films present in (e) for unannealed films along with (f) for 300 °C annealed films, (g) for 600 °C annealed films, and (h) for 900 °C annealed films.
Coatings 13 01328 g003aCoatings 13 01328 g003b
Coatings 13 01328 g004 550
Figure 4. AFM topographic images of Fe3Si film surfaces (a) without annealing and annealing (b) 300 °C, (c) 600 °C, and (d) 900 °C.
Figure 4. AFM topographic images of Fe3Si film surfaces (a) without annealing and annealing (b) 300 °C, (c) 600 °C, and (d) 900 °C.
Coatings 13 01328 g004
Coatings 13 01328 g005 550
Figure 5. Image of the contact angle between droplet and Fe3Si film surfaces (a) without post-annealing and after annealing at different temperatures of (b) 300 °C, (c) 600 °C, and (d) 900 °C, while (e) shows the relation between contact angle and rms roughness.
Figure 5. Image of the contact angle between droplet and Fe3Si film surfaces (a) without post-annealing and after annealing at different temperatures of (b) 300 °C, (c) 600 °C, and (d) 900 °C, while (e) shows the relation between contact angle and rms roughness.
Coatings 13 01328 g005
Coatings 13 01328 g006a 550Coatings 13 01328 g006b 550
Figure 6. Comparison between depth and load on non-annealed and annealed Fe3Si films. (a) is non-annealed Fe3Si films; (b) is 300 °C annealed Fe3Si films; (c) is 600 °C annealed Fe3Si films; (d) is 900 °C annealed Fe3Si films.
Figure 6. Comparison between depth and load on non-annealed and annealed Fe3Si films. (a) is non-annealed Fe3Si films; (b) is 300 °C annealed Fe3Si films; (c) is 600 °C annealed Fe3Si films; (d) is 900 °C annealed Fe3Si films.
Coatings 13 01328 g006aCoatings 13 01328 g006b
Table
Table 1. The crystal orientation of non-annealed Fe3Si films along with annealed Fe3Si films at 300 °C, 600 °C, and 900 °C.
Table 1. The crystal orientation of non-annealed Fe3Si films along with annealed Fe3Si films at 300 °C, 600 °C, and 900 °C.
AngleOrientationReference
28.50Fe3Si (111)[8]
29.12β (202)/(220)[19,20,21,22]
34.72β (400)[19]
44.38Fe3Si (220)[8]
45.20β (331)[19]
49.80β (422)[26]
56.28Fe3Si (222)[2]
58.90β (333)[26]
64.72Fe3Si (400)[8]
82.06Fe3Si (422)[8]
Table
Table 2. The values of RMS roughness of Fe3Si films without annealing and through annealing at fixed temperatures of 300 °C, 600 °C, and 900 °C.
Table 2. The values of RMS roughness of Fe3Si films without annealing and through annealing at fixed temperatures of 300 °C, 600 °C, and 900 °C.
Annealing Temperature (°C)RMS Roughness (nm)
Non-annealing0.588
3000.743
60098.235
900113.361
Table
Table 3. Contact angle values of Fe3Si films at different annealing temperatures.
Table 3. Contact angle values of Fe3Si films at different annealing temperatures.
Annealing Temperature (°C)θ CA (°)Wetting State
Non-annealed95.8Hydrophobic
30095.5Hydrophobic
60080.6Hydrophilic
90077.9Hydrophilic
Table
Table 4. H and Er values of Fe3Si films at different annealing temperatures.
Table 4. H and Er values of Fe3Si films at different annealing temperatures.
Annealing Temperature (°C)H (GPa)Er (GPa)
Without annealing8.741 ± 0.111184.899 ± 1.343
3009.363 ± 0.081204.803 ± 1.347
60014.543 ± 0.983271.261 ± 34.495
90015.341 ± 1.777323.187 ± 89.125
Disclaimer/Publisher’s Note: The statements, opinions and data contained in all publications are solely those of the individual author(s) and contributor(s) and not of MDPI and/or the editor(s). MDPI and/or the editor(s) disclaim responsibility for any injury to people or property resulting from any ideas, methods, instructions or products referred to in the content.

Share and Cite

MDPI and ACS Style

Borwornpornmetee, N.; Achirawongwat, C.; Traiprom, T.; Saekow, B.; Porntheeraphat, S.; Paosawatyanyong, B.; Yoshitake, T.; Promros, N. Determining the Annealing Temperature Dependency of Wetting and Mechanical Features on Fe3Si Films. Coatings 2023, 13, 1328. https://doi.org/10.3390/coatings13081328

AMA Style

Borwornpornmetee N, Achirawongwat C, Traiprom T, Saekow B, Porntheeraphat S, Paosawatyanyong B, Yoshitake T, Promros N. Determining the Annealing Temperature Dependency of Wetting and Mechanical Features on Fe3Si Films. Coatings. 2023; 13(8):1328. https://doi.org/10.3390/coatings13081328

Chicago/Turabian Style

Borwornpornmetee, Nattakorn, Chawapon Achirawongwat, Thawichai Traiprom, Bunpot Saekow, Supanit Porntheeraphat, Boonchoat Paosawatyanyong, Tsuyoshi Yoshitake, and Nathaporn Promros. 2023. "Determining the Annealing Temperature Dependency of Wetting and Mechanical Features on Fe3Si Films" Coatings 13, no. 8: 1328. https://doi.org/10.3390/coatings13081328

APA Style

Borwornpornmetee, N., Achirawongwat, C., Traiprom, T., Saekow, B., Porntheeraphat, S., Paosawatyanyong, B., Yoshitake, T., & Promros, N. (2023). Determining the Annealing Temperature Dependency of Wetting and Mechanical Features on Fe3Si Films. Coatings, 13(8), 1328. https://doi.org/10.3390/coatings13081328

Note that from the first issue of 2016, this journal uses article numbers instead of page numbers. See further details here.

Article Metrics

Back to TopTop