3.1. Manufacturing of a Metal Micro-Mold
In this experiment, copper foils of different thickness were used for LSI. The copper foil was annealed to eliminate its residual stress, rendering it is easier to form. After LSI, the processed part was strengthened; this step greatly increases the strength and is beneficial for repeated use as a mold in hot embossing. In this way, the microstructure of the processed copper mold can be retained in the subsequent hot-embossing process without deformation.
In the experiment, 20 μm, 50 μm, 80 μm and 100 μm copper foils were used to carry out LSI experiments. For samples of different thicknesses, the same initial mold and different laser shock parameters were selected. With the increase in the thickness of the copper foil, we increased the number of laser pulses in order to reach the maximum forming depth. The formed copper foil samples are shown in
Figure 5.
With the increase in the thickness of the copper foil, the forming depth gradually decreased. Compared with the 20 μm copper foil, the difference from the 50 μm and 80 μm copper foil is minimal, and the difference from the 100 μm copper foil is highly apparent. From the profile curve, we can see that the forming depth of the 20 μm copper foil is the greatest, reaching 11.512 μm, while that of the 50 μm copper foil is 10,645 μm, and that of 80 μm copper foil is slightly lower, reaching 8.743 μm. For the 100 μm copper foil, the large number of laser pulses has no effect on the greater deformation of the copper foil. From
Figure 5h, it can be seen that the forming depth is only 3.370 μm, which is far less than the values for the first three copper foils. Moreover, the surface morphology of the profile of the 100 μm copper foil indicates that its forming effect is poor, the forming depth and the surface of the microstructure are uneven, and the edge of the profile shows obvious defects.
As shown in
Figure 6a, for the square-hole initial mold, the 20 μm thick copper foil was selected for LSI.
Because the pressure of a plasma shock wave exceeds the dynamic yield limit of a copper foil, the shocked copper foil flows, thus filling the holes in the initial mold. The back of the copper foil will also be deformed due to flow filling on the front side. For the 50 μm copper foil, as shown in
Figure 6b, the forming process is similar to that of the 20 μm copper foil, but the 50 μm copper foil is thicker, so that the deformation on the back side is smaller than that on the 20 μm copper foil. As shown in
Figure 6c, when the 80 μm copper foil was selected for the LSI experiment, in order to obtain a better microstructure-forming effect, more laser pulses were needed. The shock wave was transmitted through the copper foil, and flow occurred in each part of the shocked area; however, because the copper foil was thick, the flow on the inner and front surfaces was enough to fill in the holes in the initial mold, so that the back side could be kept flat. From the SEM images in
Figure 6, it can be seen that the back side of the 20 μm copper foil has obvious deformation, while the back side of the 80 μm copper foil has no deformation. As shown in
Figure 6d, for the 100 μm copper foil, the shock wave first propagated through the copper foil. In such a case, there will be attenuation when the thickness of the copper foil exceeds the forming limit of the shock wave; the thicker the copper foil is, the worse the micro-structure-forming accuracy is. Therefore, in the process of LSI, although there is no deformation on the back side of the 100 μm copper foil, the side in contact with the initial mold has insufficient liquidity, and the forming depth and forming accuracy are greatly reduced. From the experimental results, it can be concluded that in LSI experiments, in order to obtain complete imprinting shapes, with the increase in the target thickness, the number of laser pulses required must also be increased. If the thickness of the target is small, this will easily lead to formation and completely filled holes in the initial mold during LSI, but because of its small thickness, there will be deformation on the back side; if the thickness of the target is large, the increase in the number of laser pulses will not produce obvious deformation.
Figure 7 shows the overall distribution of stress in the 20 μm copper foil and 80 μm copper foil throughout the whole process of LSI.
Figure 7a shows the stress of the 20 μm copper foil under the action of the 1st laser pulse, the 3rd laser pulse and the 5th laser pulse in the LSI experiments;
Figure 7b shows the stress of the 80 μm copper foil under the action of the 1st laser pulse, the 15th laser pulse and the 25th laser pulse; and
Figure 7a,b shows the stress of the 20 μm copper foil and 80 μm copper foils. Based on the aspect of stress distribution, the process can be divided into two stages. (1) In the copper foil compression stage, after the first laser pulse, although the copper foil is not significantly deformed, a large stress is generated within it. (2) In the copper mold formation stage, as the number of laser pulses increases, the copper foil is gradually formed. With the change in the forming depth, different stress distributions appear in the copper foil, and the low-stress areas gradually disappear. As shown in
Figure 7a, due to the high deformation of the back side of the copper foil, stress concentration occurs on the back surface.
Figure 7b demonstrates that because the copper foil is thick, the back side is not deformed due to superplastic flow; hence, the stress in the overall shock area of the copper foil is more balanced.
As shown in
Figure 8, the 20 μm and 80 μm copper molds were used in the hot-embossing experiment.
For the 20 μm copper mold, because deformation occurs on the back, during the repeated pressurization process, the convex microstructure on the front side will deform due to the lack of support; thus, the strength is low. However, the back of the 80 μm copper mold is flat, and there is no longitudinal deformation under the conditions of the hot-embossing experiment. Therefore, the 80 μm copper mold was finally selected for the hot-embossing experiment.
In order to transfer the microstructure to the surface of the polymer, the metal micro-molds formed via LSI were used in the hot-embossing experiment instead of the initial mold. In order to meet the diversity demand of hot-pressed products, three different microstructure-shaped molds were fabricated through large-scale integrated circuit experiments.
Figure 9 shows a square microstructure mold,
Figure 10a depicts a circular-hole microstructure copper mold labeled as 296, and
Figure 10b represents a grating microstructure mold. In the SEM images, it can be seen that the three types of copper molds have a high forming accuracy.
3.2. Forming Mechanism of a Copper Mold
In order to verify the performance stability of the copper mold under the conditions of hot embossing, an optical profiler was used to measure the forming depth of the copper mold before and after the hot-embossing experiment. The forming depth of PET was also measured. The copper mold was subjected to five hot-embossing experiments. The measurement results are shown in
Figure 11.
Figure 11a shows the comparison curve of the copper mold and the formed PET.
Figure 11b–d, moving from top to bottom, shows the profile curve of the copper mold before the hot-embossing experiment, the copper mold after the hot-embossing experiment and the formed PET, respectively. It can be seen from
Figure 11b that the forming depth of the microstructure of the copper mold before hot embossing is 5.554 μm, while in
Figure 11c, the forming depth of the microstructure after hot embossing is 5.5095 μm, and the rebound level is approximately 0.8%. Therefore, it is proved that the copper mold processed via LSI has a high strength and can withstand the temperature and pressure conditions of hot embossing, as well as the external force perpendicular to the mold microstructure during the demolding process, so as to keep its shape and structural size unchanged. In
Figure 11d, the surface microstructure depth of the formed PET is 5.439 μm, which shows that the copper mold formed via LSI can ensure the free flow and full filling of the PET in the hot-embossing experiment.
In order to observe the mechanical properties of the copper mold in the hot-embossing experimental process, the load–displacement curves of the annealed copper foil and the copper molds before and after the hot-embossing experiment were monitored.
As shown in
Figure 12a, at the same indentation depth, the required indentation load of the annealed copper foil is the smallest, and the required indentation loads of the copper molds before and after the hot-embossing experiment are very close, being larger the value of the annealed copper foil.
Therefore, it can be proved that the mechanical properties of the formed parts are strengthened.
Figure 12b shows the elastic modulus and nano-hardness values of the copper mold before and after hot embossing and the annealed copper foil. The elastic modulus and nano-hardness of the copper mold before and after hot embossing are improved compared with the annealed copper foil. After LSI, the elastic modulus of the copper mold before hot embossing increased from 70.5 to 91.3 GPa, which is an increase of 29.5%. The nano-hardness of the copper mold before hot embossing increased from 1.11 to 1.46 GPa, which is an increase of 24.0%. After the hot-embossing experiment, compared with the mold before hot embossing, the elastic modulus decreased to 88 GPa, a decrease of 3.61%, and the nano-hardness decreased to 1.32 GPa, a decrease of 9.58%, but its mechanical properties were still better than those of the annealed copper foil. The improvements in the mechanical properties of the copper mold can mainly be attributed to work hardening from the plastic deformation caused by the laser shock.
Laser shock processing is an effective method for achieving the deformation of metal materials at an ultra-high strain rate. The strain rate is usually as high as 106–107s-1, which is different from that of the traditional processing method [
21]. The shock wave generated by the laser shock can cause the metal to rapidly undergo high plastic deformation, increasing the number of crystal defects in the metal and enhancing its mechanical properties [
22]. On this basis, according to the evolution of the inner structure of the copper foil, the strengthening mechanism of the copper foil was analyzed in an LSI experiment.
In the experiment, the copper foil was annealed to reduce its crystal defects and residual stress. As shown in
Figure 13, a small number of dislocation lines and dislocation tangles can be seen in the TEM image of the annealed copper foil.
The annealed copper foil before laser shock only has a small number of dislocation structures. The copper foil after the laser shock is shown in
Figure 14. A large amount of dislocation cells (DCs), dislocation walls (DWs), dislocation tangles (DTs) and dislocation lines (DLs) are formed in the coarse grains, and these dislocation structures greatly increase the density of the crystal defects.
In the LSI process, the laser acted on the ablative layer to generate a shock wave with an ultra-high peak pressure, which could trigger most of the dislocation sources in the coarse grains in the beginning of the deformation process and caused the rapid plastic deformation of the copper foil. As the plastic deformation increased, the dislocation density increased, and then, the ultra-high peak pressure caused the DCs formed through plastic deformation to crack and multiply, as shown in
Figure 14b,c.
There are two modes of plastic deformation of copper: dislocation slip and deformation twinning. In this experiment, the dislocation structure of the copper increased significantly, and no mechanical crystal caused by plastic deformation was observed. Therefore, dislocation slip is the main deformation mode in the LSI process.
In our previous experiments, the stability of LSI samples at high temperature was verified [
23]. Although the thickness of the copper foil, with respect to the initial mold depth, is larger in this paper, the strengthening mechanism is the same as that in the previous experiment. Therefore, after the hot-embossing experiment, the mechanical properties of the copper mold changed only slightly, which proved that the copper mold formed via LSI can withstand the high temperature and pressure under hot-embossing conditions.
As shown in
Figure 15, in the LSI experiment, the copper foil initially underwent tensile deformation to fill in the holes in the initial mold. After making contact with the bottom of the initial mold, the copper foil was extruded and deformed under the joint action of the laser pulse and the mold.
Another reason for the nano-hardness difference in the microstructure is the strengthening effect of LSI and contact stress. In the plastic deformation stage, the laser shock renders the material at the bottom of the microstructure subject to longitudinal pressure. At the same time, the contact between the copper foil and the bottom of the initial mold caused stress in the microstructure. This deformation process is similar to that in the research conducted by Shen et al. In their experiment, the ratio of the target thickness to the initial mold depth is 0.21 [
24]. The residual stress field formed on the target surface, along with crystal defects such as grain refinement, dislocation and twin (as discussed in the literature [
12]), can effectively improve the comprehensive mechanical properties of the material; thus, the nano-hardness will be significantly improved compared with the annealed copper foil. In the hot-embossing experiment, the pressure and temperature are not sufficient to cause changes in the stress and crystal defects in the microstructure of the copper mold; hence, the mechanical properties remain unchanged.