Fabrication of AlN/Cu composite structure via laser metallization assisted direct bonding technology

doi:10.21203/rs.3.rs-2998710/v1

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Fabrication of AlN/Cu composite structure via laser metallization assisted direct bonding technology

https://doi.org/10.21203/rs.3.rs-2998710/v1

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In this work, an innovative and cost-effect method was proposed to fabricate AlN/Cu composite structure. The AlN ceramic was metallized by nanosecond laser irradiation without consuming extra materials. The metallurgical combination between AlN ceramic and Cu was successfully achieved based on the Al-Cu eutectic reaction at a relatively low temperature of 620 ℃. Under the laser irradiation, the AlN ceramic was thermal decomposed to form Al laeyer and microgroove. As the laser power increased, more Al was produced on the the ceramic surface and the micgroove became deeper. The microstructure, mechanical and heat transfer properties of the AlN/Cu joints were investigated. The maximum shear strength of the joint was 11.25MPa when the laser power was 56 W, and the maximum thermal conductivity was 162 W/(m·K) when the laser power was 42 W. The approach of laser-induced direct metallization of ceramics in this work provides a novel strategy for the integration of ceramics/metals composite structures.

AlN ceramic

Composite structure

Laser metallization

Bonding

As a key device in electronic power systems, insulated gate bipolar transistor (IGBT) modules were extensively applied in electric traction inverters, high voltage direct current transmission, aviation power and other critical electronic power systems requiring high safety[1]. With the IGBT modules developing in the direction of miniaturization and high integration, the power density increases sharply, which results in high heat flux and makes the thermal management more complicated[2]. It is reported that about 60% of electronic failures is due to thermal stress and the probability of failure doubles for every 10 ℃ increase in junction temperature[3, 4]. A heat dissipation substrate fabrication by integrating ceramic and copper (Cu) can transfer the heat flux from the die to the heat sink and avoid the failure of devices[5]. As a promising material for heat dissipation substrates, AlN ceramic contains the low coefficient of thermal expansion (CTE 4.5 × 10^− 6 ℃⁻¹) and high thermal conductivity (W/(m·K) in theory), which meets the thermal dissipation requirement of IGBT modules[6, 7]. Therefore, it is of practical significance to fabricate AlN/Cu composite substrate.

Up to now, various methods have been adopted to fabricate AlN/Cu composite structures, such as direct bonding copper (DBC), active metal brazing (AMB), thick film printed copper (TPC), direct plating copper (DPC)[8–12]. The DBC technology was first proposed by Burgess in 1973[13], which was based on the Cu-O eutectic liquid phase forming at 1065 ℃ to achieve the combination of AlN ceramic and Cu[14]. This structure has high current carry capacity, excellent thermal conductivity, and high electrical isolation, widely used in high-power electronic systems[8]. However, the oxygen voids in the interface were inevitable during the production, which had harmful effects on the joints' reliability[15, 16]. The AMB method was fabricated to enhance the joints' reliability by adding active elements in the brazing filler alloy[17, 18]. As for nitride ceramics, Ti was the most commonly used element. Under this circumstance, the brittle and hard phases with low thermal conductivity generated at the interface is detrimental to the heat transfer performance of the joints[9, 19]. The TPC technology adopted the screen printed technology to produce conductive patterns in the ceramic surface without an need for extra etching process. However, the printed paste contained the glass phase was supposed to adversely affect thermal conductivity[20]. In addition, the voids were inevitable in the Cu layer due to the sintering process, which was also a disadvantage[21]. Besides these methods, the DPC substrates were widely applied as heat dissipation substrate due to theirs high metal pattern precision, excellent thermal performance, and low manufacturing temperature[11, 22]. Nevertheless, the Cu layer was easy to delaminated at a relatively high temperature due to the weak bonding strength of van der Waals forces[22]. Therefore, it is necessary to develop a new fabricating methods to produce reliable AlN/Cu composite substrates .

As a high precision and convenient process method, laser surface metallization has recently been widely used to modify ceramics surface[23–27]. The chemical composition of the AlN ceramic surface was altered by laser irradiation[28, 29]. Under the irradiation of laser, the following decomposition reaction (1)[25] would occur on the surface of AlN ceramic.

AlN→Al + N₂

(1)

The N₂ escaped into the environment, while the Al metal remained on the ceramic surface. Therefore, the ceramic surface can be metallized without adding extra materials, which is conducive to subsequent combination with Cu. In our previous work[30, 31], pre-treatment by laser metallization of ceramic has been demonstrated to achieve the bonding of AlN ceramic and Cu. Nonetheless, the process still needs to be improved to obtain better performance.

In this work, the surface microstructure and chemical composition evolution of AlN ceramics irradidated at different power were investigated. Furthermore, the effect of laser power on the mechanical property and heat transfer property of AlN/Cu joints was presented.

2.1 Materials

In this work, the commercial available AlN ceramic (purity ≥ 95%, size in 5 × 5 ×3 mm³ for shear strength test and 10 × 10 × 1.5 mm³ for heat transfer property test) and Cu (T2) were supplied by Fujian Huaqing Electronic Material Technology Co., Ltd and Foshan Guang Long Copper Industry Co., Ltd, respectly. Figure 1 exhibits the surface morphology and chemical components of the pristine AlN ceramics. The shape of AlN particels on the ceramic surface was invisible. The AlN ceramic was synthesised by AlN matrix phase and Y₂O₃ additive by solid sintering as the result of the formation of AlN and YAlO₃ phases. The Cu plate was cut into 10 × 10 × 2 mm³ for shear strength test and 10 × 10 × 0.5 mm³ for heat transfer property measuring by wire cut electric discharge machine. Before the experiments, all the samples were grounded by silicon carbide papers (800#, 1000#, 2000#) and polished by 2.5 µm diamond suspensions. After that, the samples were ultrasonic cleaned in the acetone solution for 10 min.

2.2 Laser metallization and bonding processes

The laser metallization assisted direct AlN ceramic/Cu bonding process was shown in Fig. 2. First, the surface laser metallization of AlN ceramic was performed in the K9 glass box under argon atmosphere. The argon was input at a gas flow rate of 20 sccm and vented through the air outlet. The whole laser metallization treatment was under the protection of inert gases. The AlN ceramics were irradiated by nanosecond pulse fiber laser (SP-070 P-A-ER-Z-B-Y, HAN’S LASER, China) with a wave length of 1065nm and a spot diameter of 30 µm. The laser pulses frequency and scanning speed were fixed at 200 kHz and 250 mm/s, respectively. To make sure the entire ceramic surface was irradiated by laser beam, the scanning routine of the laser beam was designed as parallel lines with an interval of 30 µm. During the metallization process, various powers of 28 W, 42 W, 56 W, and 70 W were exerted.

Then, the as-treated AlN ceramics and Cu plates were put in the vacuum brazing furnace immediately. The vacuum brazing was carried out with a vacuum under 5 × 10^− 3Pa. An axial pressure of 15 MPa was applied during the whole brazing process. The samples were first heated to 620 ℃ at a rate of 10 ℃/min and held for 30 min. Then, the temperature was cooled down to 200 at a rate of 5 ℃/min and finally cooled down to room temperature naturally.

2.3 Characterization and properties measurement

The surface morphology and chemical composition of laser irradiated AlN ceramic were characterized by super depth optical microscopy (OM, DSX510, OLYMOUS), scanning electron microscopy (SEM, MERLIN COMPACT, ZEISS) and grazing incidence X-ray diffraction (GIXRD, Rigaku Dmax-2500) with an incident andgel of 1°. The microstructure evolution and interfacial phase of AlN/Cu joints were verified by SEM and transmission electron microscopy (TEM). The shear strength of the AlN/Cu joints was measured by a universal testing machine (Instron 5976) with a loading rate of 0.5 mm/min. The thermal diffusivity of the joints was measured by the laser flash analysis system (NETZSCH, LFA 447) and the thermal conductivity K were calculated according to Eq. (2):

K = ρ × α × C_p

(2)

where ρ, α, and C_p are the density, thermal diffusivity, and specific heat of the joint, respectively.

3.1 Evolution of surface chemical composition and structure of AlN ceramics

To confirm the metallization effect of laser irradiation on the surface of AlN ceramic, the GIXRD patterns of AlN ceramic surface after different power laser irradiation are shown in Fig. 3. The results showed that the diffraction peaks of aluminum were detected on the ceramic surface except for the diffraction peaks of AlN matrix. And the intensity of the diffraction peak of aluminum enhanced with the increase of laser power, which indicated the amount of surface aluminum production increased with the increase of laser power. The result of the XRD pattern confirmed that the AlN ceramic was thermal decomposed to form Al layer and metalized under laser irradiation.

The surface morphologies of laser-metallized AlN ceramics with different processing power levels are exhibited in Fig. 4. Microgroove structures were observed on the ceramic surface due to the solidification of the material after melting. With the increase of laser power, the depth of the micro-groove structure on the ceramic surface increases. When the power was 28 W, the recast layer formed by the melting of the material did not cover the entire ceramic surface, and the shape of the ceramic particles was exposed between the two laser scanning routes, as shown in Fig. 4 (a2). With the increase of laser power, a convex structure was formed between the two laser scanning routes, and the rows of convexes constituted the microgroove structure on the ceramic surface. Besides, the circular splash particles were observed on the convex surface, and the number of splash particles increased with the increase of laser power.

Since the intensity of the laser spot is not uniformly distributed, it is Gaussian distributed. The intensity gradually decreases from the center to the edge of speckle[32]. Therefore, when the laser power was 28 W, the energy density of the spot edge was not enough to make the AlN ceramics thermolysis. Thus, the shape of ceramic particles remained between the two adjacent laser scanning paths. With the increase of laser power, the intensity of the edge of the laser spot was also enough to make the AlN ceramics undergo thermal decomposition to form the aluminum layer. While the intensity of laser spot center was higher than that of edge, part of the material was melted and vaporized forming the gas phase recoil force and pushing the liquid phase to the sides[33, 34]. After re-solidification, the parallel aligned microgrooves were fabricated along the laser scanning direction. In addition, the splash particles were visible as the power continue increased, and the number and size were expanded.

The cross-sectional SEM images of AlN ceramic irradiated by different laser powers and corresponding profile curves are shown in Fig. 5 and Fig. 6, respectively. The microgrooves textured by laser irradiation were clearly observed. As the laser power enhanced, the depth of the grooves and the thickness of the recast layers were increased. It was noted that platform regions appeared on the ceramic irradiated at 28 W, as shown in Fig. 5(a) and Fig. 6(a). These were undecomposed regions due to the insufficient power of laser spot edge, which was in accordance with the phenomenon of Fig. 4(a1, a2). As the laser power increased, the platform areas disappeared and were replaced by regular arrangement microgrooves. The cross-sectional profiles maintained a good periodic pattern and no large deviation in the position of the wave crest and trough, as shown in Fig. 6(b, c). When the laser power increased to 70 W, the import laser flux was larger and the energy density was higher, which made the material vaporized and splashed and the profile curve irregular, as shown in Fig. 6(d). Besides, when the laser was higher, the temperature and range of heat-affected zone were higher and larger. Therefore, when the next orbital laser beam was scanned, its heat-affected zone had a re-melting effect on the previous microgrooves[34]. In this case, the solidified recast layer was re-melt and distributed, resulting in a change of the profile shape.

The average depth of microgrooves on the as-metallized AlN ceramic surfaces is shown in Fig. 7(a). The structure depth of microgrooves tended to increase and then decrease with the increase of laser power. As the laser power enhanced, the energy input increased and the laser ablation effect became stronger[24, 35]. As a result, the severe ablation made the microgroove deeper. However, as the laser power further increased to 70 W, the structure depth of microgroove turned to decline slightly. This could be resulted by the re-melting effect, which caused the microgroove to re-melt and become shallower due to the wider heat-effect zone. The surface roughness of AlN ceramics irradiated at various power is shown in Fig. 7(b). The surface roughness increased monotonically with increasing of laser power, which was different with the trend of structure depth. On the one hand, the deeper microgrooves contributed to increase the surface roughness; on the other hand, the splashed particles also played an important role in the surface roughness. Both the two conditions made the AlN ceramic irradiated at 70 W achieved the highest surface roughness.

3.2 Interfacial microstructure and properties of AlN/Cu joints

The typical interfacial microstructure and element distribution map of laser-metallized AlN/Cu joint are shown in Fig. 8, and the chemical composition of each spot in Fig. 8 (a) is listed in Table 1. Due to the laser metallization induced microstructure evolution, the joint was exhibited a wave-like structure, where the Cu and ceramic were interlaced. A band-like gray phase was detected in the interface. According to the elements distribution map shown in Fig. 8(c, d), this band-like phase mainly contained elements of Al and Cu. As shown in Table 1, spot A contained 32.45% Al, 45.44% Cu, 8.47%N, and 13.64% O, and spot B contained 41.65% Al, 32.33% Cu, 8.58% N, and 17.4%O, which indicated some Al-Cu compounds formed during the brazing process. The spot C was a Cu-rich phase and confirmed to be Cu(s, s). Therefore, the typical microstructure of laser-metallized AlN/Cu joint was AlN/Al-Cu IMCs + Cu(s,s)/Cu.

Table 1

EDS results of the chemical composition at each spot in Fig. 8(a) (at.%).
Spots	Al	Cu	N	O
A	32.45	45.44	8.47	13.64
B	41.65	32.33	8.58	17.44
C	18.21	76.04	3.51	2.24

To further determine the interfacial phase, TEM analysis was performed and the results were displayed in Fig. 9. The interface was well joined without holes or other defects, as shown in Fig. 9(a). The inset in Fig. 9(a) indicated that the lower left phase was AlN. Figure 9(b) shows the HRTEM of the region A in Fig. 9(a), and its corresponding Fast Fourier transform (FFT) pattern is shown in Fig. 9(c). The results showed that the interfacial phase in region A was Al₄Cu₉, where the atoms were ordered along the (010) crystal plane with a crystal plane spacing of 0.882 nm. The above results were consistent with our previous conclusions[30, 31] that laser-induced metallized AlN ceramic and Cu achieved metallurgical bonding through Cu-Al eutectic reaction. It is worth noting that this method can realize the joining between ceramic and Cu without additional brazing filler alloy.

The interfacial microstructures of AlN/Cu joints under various laser powers were investigated, as shown in Fig. 10. When the laser power was 28 W, the laser input flux was too little to make the AlN ceramic fully thermal decomposed to produce a sufficient amount of Al. Therefore, the insufficient Cu-Al eutectic reaction resulted in microcracks and unbonded areas at the interface between the ceramic and Cu, as shown in Fig. 10(a2). With the increase of laser power, the generation of Al increased and the sufficient Al-Cu eutectic reaction was able to form an abundant amount of liquid phase, which formed a complete and defect-free joint interface after cooling. It was worth noting that the interfacial striped Al-Cu compounds gradually widened with increasing power. In addition, the interfacial microgroove depth also increased with increasing laser power. However, when the power was increased to 70 W, overlarge laser input flux resulted in vast splash and re-melt effect, causing the depth of microgroove decline.

The shear strength of AlN/Cu joints under various laser powers is shown in Fig. 11. It was found that the shear strength of AlN/Cu joints tended to increase and then decrease with increasing laser power, and the maximum value of 11.25 MPa was obtained when the power was 56 W. When the laser power was 28 W, the AlN/Cu joints obtained a weak combination and poor shear strength, as shown in Fig. 10(a). After the laser power was increased to 42 W or higher, the laser beam was sufficient to produce sufficient Al from the thermal decomposition of AlN ceramics. The flawless interfaces and stronger combination of AlN/Cu joints were obtained. Besides, a mechanical interlocking effect of the interface was formed, which also contributed to the strength improvement. However, when the power was further increased to 70W, the depth of the microgroove structure and the joint strength was slightly reduced.

Figure 12 exhibits the fracture morphologies of ceramic side of AlN/Cu joints being irradiated at different laser powers. It was found that the fracture surface showed microgroove structures, which was consistent with interfacial structure. Under the effect of shear force, the recast layer was peeled off, exposed the inner ceramic matrix, and the degree of peeling off was different for samples irradiated with different powers. With the increase of laser power, the peeled area was gradually increased. As mentioned in Fig. 10, when the laser input power was low, the AlN ceramic obtained a poor combination with Cu, and cracks mainly propagated along the interface. When the laser power was intense, the bonding strength of completely metallized ceramics and Cu increased. The interface bonding strength exceeded the strength of the ceramic convex structure in some areas, and the crack propagated through the ceramic convex structure. In this case, more internal ceramic particles were exposed on the fracture surfaces.

The thermal diffusivity and thermal conductivity of AlN/Cu joints fabricated with various laser powers are displayed in Fig. 13. The heat transfer properties of the joints increasing first and then decreasing with the increasing laser power, which showed a similar trend of shear strength. When the laser power reached 42 W, the optimal thermal diffusion coefficient and thermal conductivity of the joint were obtained, which were 59.46 mm²/s and 162.19 W/(m·k), respectively. The flawless interfaces contributed to excellent heat transfer properties. When the laser power was 28 W, the joint got a poor joining, which led to weak heat transfer properties. When the laser power increased to 42 W or higher, the heat transfer properties of joints became better due to the flawless interfaces. However, when the laser power was increased from 42 W to 70 W, the heat transfer properties went slightly worse. As previous studies report, the Al-Cu IMCs generally have low thermal conductivity (31–37 W/(m·k)), which is supposed to deteriorate the total thermal conductivity of the joint[36]. Furthermore, the increase of the thickness of Al-Cu IMCs will act as heat transfer barrier and lead to worse thermal performance[37, 38]. Therefore, as the laser power was increased from 42 W to 70 W, the number of Al₄Cu₉ increased and the heat transfer properties of joints weakened.

In this work, the AlN ceramic was metallized by laser-induced thermal decomposition and directly brazed to Cu without adding extra brazing filler alloy. The main conclusions can be listed as follows:

(1) The AlN ceramics irradiated by laser were thermally decomposed to form microgroove structures and Al layers. With the increase of laser power, the surface roughness of AlN was monotonous increased. The maximum average depth was obtained when the laser power was 56W. When the laser power was further increased to 70 W, the depth was reduced due to a large number of vaporization and splash.

(2) The as-metallized AlN ceramics were successfully joined to Cu based on the Al-Cu eutectic reaction. The TEM results confirmed the existence of Al₄Cu₉ at the interface.

(3) When the laser power was 56 W, the AlN/Cu joints obtained the best shear strength of 11.25 MPa. When the laser power was 42 W, the joints reached the optimal thermal diffusivity and thermal conductivity, which were 59.46 mm²/s and 162.19 W/(m·k), respectively.

The method presented in this work provides a novel thought for the fabrication of ceramic/metal composites.

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Author contribution

Yanyu Song: conceptualization, methodology and revise; Naibin Chen and Haitao Zhu: experiment, data analysis, and writing; Ningning Wang, Jingming Fei, and Qi An: assisting in experiment and testing; Duo Liu: supervision and resources; Caiwang Tan and Xiaoguo Song: review and editing.

Funding

The project is supported by National Natural Science Foundation of China (grant Nos. 52275318 and 52175307), the Taishan Scholars Foundation of Shandong Province (NO. tsqn201812128) and China Academy of Space Technology Innovation Foundation (CAST2022).

Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Fabrication of AlN/Cu composite structure via laser metallization assisted direct bonding technology

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Abstract

Figures

1. Introduction

2. Experimental materials and methods

2.1 Materials

2.2 Laser metallization and bonding processes

2.3 Characterization and properties measurement

3. Results and disscusion

3.1 Evolution of surface chemical composition and structure of AlN ceramics

3.2 Interfacial microstructure and properties of AlN/Cu joints

4. Conclusions

Declarations

References

Additional Declarations

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