Effects of Molding Conditions on Transcription Molding of Microscale Prism Patterns Using Ultra-High-Speed Injection Molding

H. Yokoi Center for Collaborative Research, The University of Tokyo, Meguro-ku, Tokyo 153-8505, Japan X. Han, T. Takahashi, W.K. Kim Institute of Industrial Science, The University of Tokyo, Meguro-ku, Tokyo 153-8505, Japan

In this study, we performed a series of molding tests to investigate the potential of microscale transcription of polymer by ultra-high-speed injection molding (UHSIM). During the tests, the injection speed was varied up to a maximum of 995 mm/s. Polymethyl methacrylate was molded under various injection molding conditions, including cavity vacuum pumping process, so as to replicate an electroformed nickel stamper exhibiting Vgrooves with a pitch of 50 m. Surface congurations of molded samples were observed and measured using a laser scanning microscope. The transcription ratio (TR) is dened as the ratio of the depths of V-grooves in both the molded samples and the stamper. An excellent average TR of 0.97 was performed when molding at an injection rate of 800 cm3/s (injection speed of 995 mm/s), mold temperature of 80C, and holding pressure of 120 MPa. In addition, the effect of vacuum on transcription molding was investigated in detail; the result proved that vacuum is an important factor in the enhancement of transcription delity. The strong inuence of injection rate on the TR indicates the applicability of UHSIM to the eld of transcription molding of polymers. POLYM. ENG.
SCI., 46:1140 1146, 2006. 2006 Society of Plastics Engineers

INTRODUCTION Over the past few years, the transcription of micro- or nanostructures of polymers has been conducted extensively, with increasing applications of polymer materials in IT and biotechnologies. Mainly, two manufacturing processes are commonly employed to replicate the microstructures of polymers, one is hot embossing and the other is injection molding [1]. Hot embossing is a molding process in which master structures are replicated by compressing a plastic plate between a stamper and a cavity plate, after heating the

Correspondence to: H. Yokoi; e-mail: hiyokoi@iis.u-tokyo.ac.jp DOI 10.1002/pen.20519 Published online in Wiley InterScience (www.interscience.wiley. com). 2006 Society of Plastics Engineers

system above the glass transition temperature (Tg). The embossed part is removed after the mold unit cools below the Tg value of the molding material. This process is suitable for both replication and demolding; thus, it is frequently applied to high-aspect-ratio microstructures (HARMs) and nanoscale structures. However, its main drawback is long cycle time [13]. On the other hand, the cycle time of injection molding is relatively short; hence, it is widely used for the mass replication of microstructures for polymer applications, such as CDs, DVDs, and light-guide panels for LCDs. Electroformed nickel plates are often used to develop stampers with ne structures. Some studies have investigated transcription by injection molding using different micro- or nanostructures [4 14]. It is reported that mold temperature is the most important processing parameter that affects transcription molding. At mold temperatures near or above the Tg value of molding material, even HARMs can be completely replicated [9]. However, higher mold temperatures increase the cycle time, thereby, increasing the cost of mass production. To enhance the transcription quality by injection molding, it is preferable to use a polymer with high owability as the molding material. The melt temperature is an effective factor in the transcription process; however, an increase in melt temperature can degrade resin materials. Furthermore, the effect of gas on microtranscription is important [9, 13], but it has not yet been proved experimentally. The most effective approach to improve transcription molding is to delay the formation of a solidied skin layer during injection molding. Accordingly, an increase in the injection rate could be very effective in achieving high transcription quality. During the past 3 decades, Japanese machinery manufacturers have developed a new type injection molding machine, termed ultra-high-speed injection molding (UHSIM) machine, to produce thin-walled plastic products and achieve high cycle molding. The injection speed of UHSIM machine can be increased up to a maxi-

POLYMER ENGINEERING AND SCIENCE2006

FIG. 2. Cavity shape and set up locations of pressure and temperature sensors.

FIG. 1.

Experimental mold with three-plate structure.

mum of 1000 2000 mm/s. UHSIM is being applied extensively to advanced industrial elds [15, 16]. Thus far, however, only a few papers have reported studies on transcription by UHSIM [1721]. Our research goal is to investigate the following: (1) the efciency of UHSIM in transcription molding, (2) the effect of location on transcription ratio (TR) over a replicated surface (150 50 mm2), and (3) the effect of gas on the transcription process. In this study, we used sensors for cavity pressure, gas pressure, and infrared temperature to investigate the fundamental effects of processing parameters on the transcription process. EXPERIMENTAL Experimental Equipments and Setup The UHSIM machine FN4000 9HTN, developed by Nissei Plastic Industrial Co., was used to conduct this experiment. The injection speed of this machine can be increased up to 1000 mm/s; the screw diameter is 32 mm. It provides a clamping force of 1700 kN. The structure of the injection mold used in this study comprises three plates, as shown in Fig. 1. The sensor and gate blocks were inserted in the movable side, and the electroformed nickel stamper was installed in the middle plate. Figure 2 shows the cavity conguration and locations of the sensors for infrared temperature and cavity pressure. In this study, a prism pattern, exhibiting V-grooves with a pitch of 50 m and a right angle, was adopted to fabricate the stamper. In the stamper, the V-grooves were arranged perpendicular to the direction of melt ow. The cavity size
DOI 10.1002/pen

was 150.0 50.0 mm2, with a thickness of 2.0 mm. Two infrared temperature sensors SKB 3453 (Vanzetti) were installed at locations T1 and T3 to measure the melt temperature during molding. Three pressure sensors 6157BA (Kistler Japan Co.,) were installed at locations P1, P2, and P3 in the same cavity, as shown in Fig. 2. A vacuum pumping system shown in Fig. 3 was linked to the cavity through a gas vent (depth of 0.03 mm), which was located at the end of cavity. An O-ring was installed around the cavity on the parting surface of the movable side, to seal the cavity during vacuum pumping, as shown in Fig. 1b. By using this system, we investigated the effect of vacuum on the transcription process. The time for vacuum pumping was set as 9.1 s; it includes 1.1 s required for prevacuuming the cavity and 8 s for lling and holding pressure stages. Furthermore, a gas pressure sensor AP-44 (Keyence Co.) was installed in the vacuum pumping pipe to measure the change in gas pressure. Polymethyl methacrylate (PMMA/ DS200E) was used as the molding material; it is a special low-viscosity material fabricated for CD or DVD molding. Its deection temperature under load (DTUL) is 90C in ASTM D 648, under a load of 1.82 MPa; this value is lower than the DTUL of general purpose PMMA, which is 102C. In addition, molding experiment was performed with a cycle time of 2 min, which includes 8 s of injection and holding stages and 40 s for the cooling stage, and the residual time is for mold operation, demolding, and taking molded part. Table 1 lists the detailed injection molding conditions for this experiment.

FIG. 3.

Vacuum pumping system.

POLYMER ENGINEERING AND SCIENCE2006

1141

TABLE 1.

Molding material and conditions. PMMA/DS200E (MFR 21.0 g/10 min) Mitsubishi Rayon Co. 250 70/80 100/200/400/600/800 (124.4/248.8/497.6/ 746.4/995.2) 100/120 2.0

Resin Melt temperature (C) Mold temperature (C) Injection rate (injection speed) [cm3/s (mm/s)] Holding pressure (MPa) Cavity thickness (mm)

Evaluation Method for Transcription Quality The surface conguration of the molded samples was observed using a laser scanning microscope (LSM) (1HD200, Lasertec Co.). The TR was measured for evaluating the transcription delity of the samples, as shown in Fig. 4a. The TR is dened as the ratio of depths of Vgrooves both in the molded samples and the stamper. In addition, the distribution of TRs over an entire replicated surface was investigated to evaluate the transcription delity. We measured 28 points over half the molded surface of each samples at regular intervals; the TR distribution map is shown in Fig. 4b. On the basis of the aforementioned data, we discussed the relationship between transcription molding and the inuential factors in this study. RESULTS AND DISCUSSION Transcription Molding in UHSIM First, the effect of injection rate on the transcription delity was investigated by varying it from 100 to 800 cm3/s (injection speed was varied from 124 to 995 mm/s). Figure 5 shows two LSM images of the replicated surface of samples molded at the injection rates of 100 and 800 cm3/s. In both images, the proles of the bottom areas are identical; this implies that the peak area of a V-groove of the stamper was effectively replicated. On the other hand, the groove peak of the sample molded at 800 cm3/s is considerably sharper than that of the sample molded at 100 cm3/s. This apparent difference proves that a high injection speed is very effective in improving the transcription. To calculate the TRs, the groove heights of samples molded by varying the injection rate, the holding pressure, the mold temperature, etc. were measured using LSM. Figure 6 shows the relationships between the average TRs and the molding factors, for the case in which molding was performed without vacuum pumping. It is evident that the average TR tends to increase with the injection rate. For example, a high TR of 0.97 was obtained at an injection rate of 800 cm3/s, holding pressure of 120 MPa, and mold temperature of 80C. All curves shown in Fig. 6 prove that the injection rate is very effective in achieving a high TR.
1142 POLYMER ENGINEERING AND SCIENCE2006

The melt velocity V1 from P1 to P2 was calculated from the response time interval between the pressure sensors P1 and P2. Similarly, the velocity V2 from P2 to P3 was calculated. The mean melt ow velocity calculated from these data is shown Fig. 7. In this gure, the maximum melt ow velocity in UHSIM can become greater than 6 m/s, and the cavity with dimensions of 150.0 50.0 2.0 mm3 can be lled in only 25 ms. Such a short lling time is certainly important for improving the transcription in UHSIM, by restraining the formation of a solidied skin layer during the cavity lling process. Figure 8 shows the maximum temperature of resin in the cavity during injection molding. It was measured by the two infrared temperature sensors installed at T1 and T3; T1 is located near the gate and T3 is near the end of the cavity. These data indicate that the temperature of the owing resin melt in UHSIM changes because of the high response time of the temperature sensors. In comparison with the temperature during molding at 100 cm3/s, the temperature during molding at 800 cm3/s increased up to 70C. This apparent temperate change evidently indicates that shear heating occurred in the owing resin melt due to the extremely high melt ow velocity, as mentioned earlier. It was reported that the temperature increases up to 95C by shear heating when the melt is passed through a narrow gate during UHSIM [22]. In this experiment, we used a three-plate mold with a fan-gate; hence, several narrow areas existed that easily caused shear heating when the resin melt owed through them. In addition to the short lling time, the increase in melt temperature due to shear heating causes a decrease in the viscosity of the resin melt; this restrains the formation of the skin layer during molding. In other words, when molding is performed at a lower injection rate, the transcription process during the lling and holding pressure stages is impeded by the quick formation and development of the skin layer. These results indicate that a short lling time and temperature increase due to shear heating are important for

FIG. 4.

Evaluation method for transcription quality.

DOI 10.1002/pen

FIG. 5.

LSMs of replicated surfaces (holding pressure, 100 MPa; mold temperature, 80C).

increasing the transcription delity during molding at ultrahigh-speeds. Furthermore, Fig. 6 shows the change in TR as a function of the injection rate when molding was performed at different holding pressures and mold temperatures. As shown in this gure, the TR increases with the mold temperature and holding pressure. This suggests that mold temperature and holding pressure are very important factors that inuence the transcription delity in injection molding at ultra-highspeeds. The effect of mold temperature is more evident when molding is performed at a lower injection rate. This may indicate that the transcription during the packing stage is more important at lower injection rates than at higher injection rates. On the other hand, the increase in holding pressure promotes the compensatory lling of melt into the cavity, thereby forcing the skin layer to ll into the Vgrooves due to creep deformation and prevent the later recovery of the replicated structure. Effect of Vacuum on Transcription Molding In some cases, venting systems are placed in molds to remove any gases or trapped air. An air trap is formed inside

the mold cavity when air fails to escape from the mold vents. Entrapped air causes voids and bubbles in a molded part, short shot (incomplete ll), or surface defects, such as blemishes or burn marks. In transcription molding, gas may be easily trapped within a groove area, and it may impede further lling of melt into the groove. Moreover, gas plays a more important role in injection molding at high speeds, because of the short lling time. It is reported that gas pressure increases rapidly in UHSIM [23, 24]. Accordingly, we repeated the experiments described earlier with vacuum pumping. Figure 9 shows the relationship between the injection rates and the average TR when molding was performed by creating a vacuum in the cavity. The results were similar to those of molding performed without vacuum pumping (with a conventional gas vent), as shown in Fig. 4. However, the average TR obtained with vacuum pumping is higher than that obtained without it. When molding was performed at an injection rate greater than 400 cm3/s, the effect of injection rate became more evident and the TRs came close to 1.0. For example, when molding was performed at a mold temperature of 70C, holding pressure of 100 MPa, and injection rate of 600 cm3/s, the TRs

FIG. 6. Relationships between TR and injection rate, for molding at different mold temperatures and holding pressures without vacuum pumping.

FIG. 7. Relationship between ow front velocity and injection rate, when molding was performed at a mold temperature of 70C and with vacuum pumping.

DOI 10.1002/pen

POLYMER ENGINEERING AND SCIENCE2006

1143

FIG. 8. Relationship between injection rate and melt temperature (mold temperature, 80C; holding pressure, 100 MPa).

obtained with and without vacuum pumping were 0.95 and 0.92, respectively. This result proves that vacuum is important for microscale transcription. TRs Over Entire Replicated Surface In many applications such as the manufacturing of CDs/ DVDs and light-guide panels, it is essential to replicate microstructures uniformly over the entire surface of a molded sample. Therefore, it is important to investigate the factors that inuence the distribution of TRs over a replicated surface and determine a mechanism to achieve highlevel transcription. In this study, the distribution of TRs over an entire replicated surface under various molding conditions was evaluated and investigated quantitatively. Figure 10 shows the TR distribution in samples prepared by injection molding, with and without vacuum pumping, at injection rates of 100, 400, and 800 cm3/s. At higher injection rates, the TRs increase considerably and distribute more evenly. On the other hand, as the injection rate increases the melt temperature increases, and the difference between the temperatures at the end of the cavity and the gate reduces, as shown in Fig. 8. Based on these temperature changes in the resin melt with the TR distribution, it is assumed that the high value and uniform distribution of melt temperature are the main factors that contribute to a higher and uniform TR
FIG. 10. Overall distribution of TR inside cavity area (holding pressure, 100 MPa; mold temperature, 80C; without vacuum pumping).

distribution in transcription molding using the UHSIM machine. Figure 11 shows the results of molding performed with vacuum pumping. In this case, the uniformity of TR distribution improved in comparison with that shown in Fig. 10;

FIG. 9. Relationships between TR and injection rate for molding at the same conditions as shown in Fig. 6, with vacuum pumping.

FIG. 11. Overall distribution of TR inside cavity area (holding pressure, 100 MPa; mold temperature, 80C; with vacuum pumping).

1144

POLYMER ENGINEERING AND SCIENCE2006

DOI 10.1002/pen

FIG. 12. Effect of vacuum stop timing on the distribution of TR (injection rate, 600 cm3/s; holding pressure, 100 MPa; mold temperature, 70C).

it became more signicant with an increase in the injection rate. Moreover, as shown in Fig. 11a and 11b, the TRs at the central area of the cavity are slightly larger than those at the two sides in samples molded at lower injection rate of 100 and 400 cm3/s. However, when samples were molded at a high injection rate of 800 cm3/s, the TRs at the central area became signicantly larger than those at the two sides. In Fig. 11b and 11c, dotted lines indicate the proles of the ow fronts of two short-shot samples, molded at the injection rates of 400 and 800 cm3/s, respectively. The melt ow fronts of samples molded at different injection rates exhibit different shapes. Comparing these proles with the TR distribution maps shown in Fig. 11, it can be seen that the area where the melt precedes shows higher TR values, mainly due to the residual gas in the cavity. This indicates that the injection rate inuences the distribution of TRs over the replicated surface by changing the melt ow pattern. Effect of Gas Pressure on Transcription Molding Since the gas in the cavity evidently impedes the transcription, as proved earlier, changes in gas pressure during UHSIM should be investigated in detail. The interior of the cavity is the most suitable area for measuring the gas pressure. However, because no gas pressure sensor can withstand the melt at a high pressure above 100 MPa, we investigated the change in gas pressure in the pipe that connects the gas vent to the vacuum pumping system. In this experiment, the vacuum valve was opened 1.1 s before the start of screw injection. To investigate the change in gas pressure and TR distribution of molded samples, the end of times of vacuum pumping were set to (a) 0.05 s before the start of injection, and (b) 0.15 s after the start of injection,
DOI 10.1002/pen

respectively. In case (a), after the cavity was vacuumpumped sufciently for 1.05 s, the vacuum valve was closed just before the start of injection. However, gas generated from the melt during cavity lling could not escape, because the vent was closed by the vacuum valve. Figure 12 shows the behaviors of injection pressure and gas pressure and the TR distribution map for different vacuum pumping times, when molding was performed at an injection rate of 600 cm3/s. In this gure, the gas pressure is indicated by gauge pressure and the atmospheric pressure is considered as 0 kPa. In both cases, shown in Fig. 12, the gas pressure in the pipe increased, as shown by c. However, the gas pressure decreased rapidly in case (b) at the end of the molding process, while it was maintained in case (a) without any reduction. Moreover, the TRs at the end of the cavity reduced in case (a), while a uniform and high-value TR distribution was achieved in case (b) over the entire replicated surface. This is apparently due to the gas generated from the resin melt during the lling stage. In case (a), the gas that was either generated or present initially was compressed during injection molding, because it could not escape. It is assumed that the compressed gas remained in the V-groove area, as the melt ows over the grooves and lled them; it impeded any further lling of melt into the grooves. However, in case (b), the vacuum valve was kept open until the end of the lling stage. This resulted in a considerable increase in the TRs over the entire replicated area, although a lower gas pressure in cavity was maintained in the cavity during the injection molding process. The aforementioned result proves the efciency of vacuum pumping in transcription molding. It also suggests that the gas vent size should be designed based on the changes in gas volume during UHSIM.
POLYMER ENGINEERING AND SCIENCE2006 1145

CONCLUSIONS To investigate the effects of molding conditions on transcription in UHSIM, PMMA was injection-molded into a cavity with an electroformed Ni stamper exhibiting Vgrooves with a pitch of 50 m. Changes in cavity pressure and melt temperature were investigated and discussed using the evaluation results of transcription quality, based on TR and its distribution over the entire replicated surface (150.0 50.0 mm2). Our experimental results demonstrated that UHSIM is a very effective method for improving the transcription quality; it signicantly enhances both TR and transcription uniformity. Mold temperature and holding pressure are important for transcription molding even in UHSIM. The creation of vacuum in the cavity effectively enhanced the transcription quality of transcription molding. An investigation on the relationship between the change in gas pressure change and the transcription delity indicated that the cavity should be vacuumed continuously until the end of injection, so as to ensure the efciency of vacuum. In addition, the distribution maps of TRs for the replicated samples revealed that the distribution of TR distribution is correlated with the ow pattern, injection speed, and gas vent condition. ACKNOWLEDGMENTS This work was carried out as a subproject of U2001 and U2002 Project held at the Institute of Industrial Science, The University of Tokyo. We thank all participated companies for their support and cooperation.
5. 6. 7. 8. 9. 10.

11. 12. 13. 14. 15. 16. 17. 18.

19.

REFERENCES
1. O. Rotting, W. Ropke, H. Becker, and C. Gartner, Microsyst. Technol., 8, 32 (2002). 2. L.J. Heyderman, H. Schift, C. David, B. Ketterer, M. Auf der Maur, and J. Gobrecht, Microelectron. Eng., 57/58, 375 (2001). 3. Y.J. Juang, L.J. Lee, and K.W. Koelling, Polym. Eng. Sci., 42, 539 (2002). 4. H. Schift, C. David, M. Gabriel, J. Gobrecht, L.J. Heyderman,

20. 21. 22. 23. 24.

W. Kaiser, S. Koppel, and L. Scandella, Microelectron. Eng., 53, 171 (2000). M. Yoshii, H. Kuramoto, and K. Kato, Polym. Eng. Sci., 33, 1251 (1993). M. Yoshii, H. Kuramoto, and K. Kato, Polym. Eng. Sci., 34, 1211 (1994). M. Yoshii, H. Kuramoto, and Y. Ochiai, Polym. Eng. Sci., 38, 1587 (1998). D. Macintyre and S. Thoms, Microelectron. Eng., 41/42, 211 (1998). M.S. Despa, K.W. Kelly, and J.R. Collier, Microsyst. Technol., 6, 60 (1999). K. Monkkonen, J. Hietala, P. Paakkonen, E.J. Paakkonen, T. Kaikuranta, T.T. Pakkanen, and T. Jaaskenlainen, Polym. Eng. Sci., 42, 1600 (2002). L. Yu, C.G. Koh, L.J. Lee, K.W. Koelling, and M.J. Madou, Polym. Eng. Sci., 42, 871 (2002). T. Yasuhara, K. Kato, H. Imamura, and N. Ohtake, Sosei-toKakkou, 43, 492 (2002). Y.C. Su, J. Shah, and L.W. Lin, J. Micromech. Microeng., 14, 415 (2004). N. Gadegaard, S. Moser, and N.B. Larsen, Macromol. Mater. Eng., 288, 76 (2003). H. Yokoi, J. JSAE, 56, 89 (2002). H. Yokoi, Plastics Age Encyclopedia, Shinpo Hen, Volume Date 2005, 112 (2004). H. Yokoi, T. Takahashi, W.K. Kim, and A. Segawa, in JSPE Autumn Conference02, 185 (2002). X. Han, H. Yokoi, T. Takahashi, and W.K. Kim, in PPS-19 Annual Meeting, Melbourne, Australia (2003). CD-ROM No. 401. X. Han, H. Yokoi, and T. Takahashi, in PPS-2004 Asia/ Australia Meeting, Gyeongju, Korea (2004). CD-ROM No. 30-O-G2 08. O. Murakami and A. Yuuki, in JSPP Symposia04, 147 (2004). L. Yu, G. Xu, L.J. Lee, and K.W. Koelling, in PPS-20 Annual Meeting, Akron, Ohio (2004). CD-ROM No. 207. H. Yokoi, W.K. Kim, and Y. Murata, in PPS-19 Annual Meeting, Melbourne, Australia (2003). CD-ROM No. 277. S. Hasegawa, W.K. Kim, and H. Yokoi, Seisan-Kenkyu, 55, 506 (2003). H. Yokoi, S. Hasegawa, and W.K. Kim. Die & Mold Tech., 18, 118 (2003).

1146

POLYMER ENGINEERING AND SCIENCE2006

DOI 10.1002/pen