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Journal of Heat Transfer | Volume 127 | Issue 7 | Research Paper
RESEARCH PAPERS: Micro/Nanoscale Heat Transfer

Damage-Free Low Temperature Pulsed Laser Printing of Gold Nanoinks On Polymers

[+] Author and Article Information
Jaewon Chung1

Laser Thermal Laboratory, Department of Mechanical Engineering, University of California, Berkeley, Berkeley, CA 94720-1740cgrigoro@me.berkeley.edu

Seunghwan Ko

Laser Thermal Laboratory, Department of Mechanical Engineering, University of California, Berkeley, Berkeley, CA 94720-1740

Costas P. Grigoropoulos2

Laser Thermal Laboratory, Department of Mechanical Engineering, University of California, Berkeley, Berkeley, CA 94720-1740

Nicole R. Bieri, Cedric Dockendorf, Dimos Poulikakos

Laboratory of Thermodynamics in Emerging Technologies, Department of Mechanical and Process Engineering, ETH Zurich, CH-8092 Zurich, Switzerland

1

Present address: Department of Mechanical Engineering, Korea University, Seoul, Korea.

2

Corresponding author.

J. Heat Transfer 127(7), 724-732 (Jan 12, 2005) (9 pages) doi:10.1115/1.1924627 History: Received June 09, 2004; Revised January 12, 2005
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Citing Articles

In this study, pulsed laser based curing of a printed nanoink (nanoparticle ink) combined with moderate and controlled substrate heating was investigated to create microconductors at low enough temperatures appropriate for polymeric substrates. The present work relies on (1) the melting temperature depression of nanoparticles smaller than a critical size, (2) DOD (drop on demand) jettability of nanoparticle ink, and (3) control of the heat affected zone induced by pulsed laser heating. In the experiments, gold nanoparticles of 3–7nm diameter dissolved in toluene solvent were used as ink. This nanoink was printed on a polymeric substrate that was heated to evaporate the solvent during or after printing. The overall morphology of the gold microline was determined by the printing process and controlled by changing the substrate temperature during jetting. In addition, the printed line width of about 140μm at the room temperature decreased to 70–80μm when the substrate is heated at 90°C. By employing a microsecond pulsed laser, the nanoparticles were melted and coalesced at low temperature to form a conductive microline which had just 3–4 times higher resistivity than the bulk value without damaging the temperature sensitive polymeric substrate. This gold film also survived after Scotch tape test. These are remarkable results, considering the fact that the melting temperature of bulk gold is 1064°C and the polymeric substrate can be thermally damaged at temperatures as low as 500°C.
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References

1
Sirringhaus, H., and Shimoda, T., 2003, “Inkjet Printing of Functional Materials,” MRS Bull., 28 (11), pp. 802–803.
2
Burns, S. E., Cain, P., Mills, J., Wang, J., and Sirringhaus, H., 2003, “Inkjet Printing of Polymer Thin-Film Transistor Circuits,” MRS Bull., 28 (11), pp. 829–834.
3
Bharathan, J., and Yang, Y., 1998, “Polymer Electroluminescent Devices Processed by Inkjet Printing. I. Polymer Light-Emitting Logo,” Appl. Phys. Lett.  [CrossRef], 72 (21), pp. 2660–2662.
4
Hebner, T. R., Wu, C. C., Marcy, D., Lu, M. H., and Sturm, J. C., 1998, “Ink-Jet Printing of Doped Polymers for Organic Light Emitting Devices,” Appl. Phys. Lett.  [CrossRef], 72 (5), pp. 519–521.
5
Oda, M., Abe, T., Suzuki, T., Saito, N., Iwashige, H., and Kutluk, G., 2002, “Application of Dispersed Nano Particles,” Nanoparticulate Materials Symposium , MRS Symposium Proc., Warrendale, PA, Vol. 704 , pp. 3–10.
6
Brust, M., Walker, M., Bethell, D., Schriffin, D. J., and Whyman, R. J., 1994, “Synthesis of Thiol-Derivatized Gold Nanoparticles in a Two-Phase Liquid-Liquid System,” J. Chem. Soc., Chem. Commun.  [CrossRef], 7 , pp. 801–802.
7
Hostetler, M. J., Wingate, J. E., Zhong, C., Harris, J. E., Vachet, R. W., Clark, M. R., Londono, J. D., Green, S. J., Stokes, J. J., Wignall, G. D., Glish, G. L., Porter, M. D., Evans, N. D., and Murray, R. W., 1998, “Alkanethiolate Gold Cluster Molecules With Core Diameters From 1.5to5.2nm: Core and Monolayer Properties as a Function of Core Size,” Langmuir  [CrossRef], 14 , pp. 17–30.
8
Szczech, J. B., Megaridis, C. M., Gamota, D. R., and Zhang, J., 2002, “Fine-Line Conductor Manufacturing Using Drop-on Demand PZT Printing Technology,” IEEE Transactions on Electronics Packaging Manufacturing, 25 (1), pp. 26–33.
9
Fuller, S. B., Wilhelm, E. J., and Jacobson, J. M., 2002, “Ink-Jet Printed Nanoparticle Microelectromechanical Systems,” J. of MEMS, 11 (1), pp. 54–60.
10
Huang, D., Liao, F., Molesa, S., Redinger, D., and Subramanian, V., 2003, “Plastic-Compatible Low Resistance Printable Gold Nanoparticle Conductors for Flexible Electronics,” J. Electrochem. Soc.  [CrossRef], 150 (7), pp. G412–G417.
11
Bieri, N. R., Chung, J., Haferl, S. E., Poulikakos, D., and Grigoropoulos, C. P., 2003, “Microstructuring by Printing and Laser Curing of Nanoparticle Solutions,” Appl. Phys. Lett.  [CrossRef], 82 (20), pp. 3529–3531.
12
Chung, J., Ko, S., Bieri, N. R., Grigoropoulos, C. P., and Poulikakos, D., 2004, “Conductor Microstructures by Laser Curing of Printed Gold Nanoparticle Ink,” Appl. Phys. Lett.  [CrossRef], 84 (5), pp. 801–803.
13
Chung, J., Ko, S., Bieri, N. R., Grigoropoulos, C. P., and Poulikakos, D., 2003, “Laser Curing of Nanoparticle Suspended Solution,” in Proceedings of the 2003 ASME IMECE , Washington, D.C., November.
14
Buffat, P. A., and Borel, J. P., 1976, “Size Effect on the Melting Temperature of Gold Particles,” Phys. Rev. A  [CrossRef], 13 (6), pp. 2287–2298.
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Dijksman, J. F., 1984, “Hydrodynamics of Small Tubular Pumps,” J. Fluid Mech., 139 , pp. 173–191.
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Bogy, D. B., and Talke, F. E., 1984, “Experimental and Theoretical Study of Wave Propagation Phenomena in Drop-on-Demand Ink Jet Devices,” IBM J. Res. Dev., 28 (3), pp. 314–321.
Upilex-S, Ultra-high heat-resistant polyimide film (50μm thick), UBE industries. The minimum glass transition temperature is 500°C.
17
El-adawi, M. K., Abdel-naby, M. A., and Shalaby, S. A., 1995, “Laser Heating of a Two Layer System With Constant Surface Absorption: An Exact Solution,” Int. J. Heat Mass Transfer  [CrossRef], 38 (5), pp. 947–952.
18
Bicerano, J., 1993, "Prediction of Polymer Properties", Marcel Dekker, New York.

Figures

Grahic Jump Location
+Numerical result when Ts=147°C and Tj=37°C. (a) Velocity profile with stream lines. (b) temperature profile.
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Numerical result when Ts=147°C and Tj=37°C. (a) Velocity profile with stream lines. (b) temperature profile.
Figure 6

Numerical result when Ts=147°C and Tj=37°C. (a) Velocity profile with stream lines. (b) temperature profile.

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+Estimated nozzle temperature (Tn) from experiment and numerical simulation due to substrate heating at Tj=37°C.
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Estimated nozzle temperature (Tn) from experiment and numerical simulation due to substrate heating at Tj=37°C.
Figure 7

Estimated nozzle temperature (Tn) from experiment and numerical simulation due to substrate heating at Tj=37°C.

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+Morphology of printed and cured nanoink on polyimide film. The same voltage waveform in Fig. 2 was used with Vamp=14V. Before AFM (atomic force microscopy) scans, all lines were cured at 200°C to evaporate toluene solvent. (a) Shows the morphology of a single droplet deposition obtained at Ts=25°C. In (b–d), the translation speed and jetting frequency were 2mm∕s and 30Hz, respectively. Therefore, the distance between the droplet centers is 67μm. Ts for (b), (c), and (d) was 25, 50, and 90°C, respectively.
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Morphology of printed and cured nanoink on polyimide film. The same voltage waveform in Fig. 2 was used with Vamp=14V. Before AFM (atomic force microscopy) scans, all lines were cured at 200°C to evaporate toluene solvent. (a) Shows the morphology of a single droplet deposition obtained at Ts=25°C. In (b–d), the translation speed and jetting frequency were 2mm∕s and 30Hz, respectively. Therefore, the distance between the droplet centers is 67μm. Ts for (b), (c), and (d) was 25, 50, and 90°C, respectively.
Figure 8

Morphology of printed and cured nanoink on polyimide film. The same voltage waveform in Fig. 2 was used with Vamp=14V. Before AFM (atomic force microscopy) scans, all lines were cured at 200°C to evaporate toluene solvent. (a) Shows the morphology of a single droplet deposition obtained at Ts=25°C. In (b–d), the translation speed and jetting frequency were 2mm∕s and 30Hz, respectively. Therefore, the distance between the droplet centers is 67μm. Ts for (b), (c), and (d) was 25, 50, and 90°C, respectively.

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+(a) rms (root mean square) roughness and resistance per length of printed lines cured at different temperatures. (b) Cross-sectional profiles of printed lines cured at different temperatures.
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(a) rms (root mean square) roughness and resistance per length of printed lines cured at different temperatures. (b) Cross-sectional profiles of printed lines cured at different temperatures.
Figure 9

(a) rms (root mean square) roughness and resistance per length of printed lines cured at different temperatures. (b) Cross-sectional profiles of printed lines cured at different temperatures.

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+Pulsed laser cured printed line at different scanning gaps, dgap. The same voltage waveform in Fig. 2 was used and Vamp=15V. Nanoink was printed on a polyimide film at room temperature and cured by a substrate heating at 200°C. During laser curing, the film was heated at 200°C using the vacuum chuck in Fig. 1. Laser power, beam waist (1∕e2), frequency and translation speed are 0.85W, 30μm, 100Hz, and 0.5mm∕s, respectively. (a) RL versus scanning gap of laser beam. Inset pictures are reflection images corresponding to cases circled with a dotted line. (b) AFM image before pulsed laser irradiation. (c) AFM image after pulsed laser irradiation at tpulse=10μs and dgap=40μm. (d) AFM image after pulsed laser irradiation at tpulse=20μs and dgap=10μm. rms roughness is 2.7nm.
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Pulsed laser cured printed line at different scanning gaps, dgap. The same voltage waveform in Fig. 2 was used and Vamp=15V. Nanoink was printed on a polyimide film at room temperature and cured by a substrate heating at 200°C. During laser curing, the film was heated at 200°C using the vacuum chuck in Fig. 1. Laser power, beam waist (1∕e2), frequency and translation speed are 0.85W, 30μm, 100Hz, and 0.5mm∕s, respectively. (a) RL versus scanning gap of laser beam. Inset pictures are reflection images corresponding to cases circled with a dotted line. (b) AFM image before pulsed laser irradiation. (c) AFM image after pulsed laser irradiation at tpulse=10μs and dgap=40μm. (d) AFM image after pulsed laser irradiation at tpulse=20μs and dgap=10μm. rms roughness is 2.7nm.
Figure 10

Pulsed laser cured printed line at different scanning gaps, dgap. The same voltage waveform in Fig. 2 was used and Vamp=15V. Nanoink was printed on a polyimide film at room temperature and cured by a substrate heating at 200°C. During laser curing, the film was heated at 200°C using the vacuum chuck in Fig. 1. Laser power, beam waist (1∕e2), frequency and translation speed are 0.85W, 30μm, 100Hz, and 0.5mm∕s, respectively. (a) RL versus scanning gap of laser beam. Inset pictures are reflection images corresponding to cases circled with a dotted line. (b) AFM image before pulsed laser irradiation. (c) AFM image after pulsed laser irradiation at tpulse=10μs and dgap=40μm. (d) AFM image after pulsed laser irradiation at tpulse=20μs and dgap=10μm. rms roughness is 2.7nm.

Grahic Jump Location
+Pulsed laser cured printed line at different laser pulse durations. Printed lines in Fig. 1 were used. During laser curing, the polyimide film was heated at 200°C using the vacuum chuck in Fig. 1. Laser power, beam waist (1∕e2), frequency, translation speed and scanning gap are 0.85W, 30μm, 100Hz, 0.5mm∕s, and 10μm, respectively. Inset pictures in (a) are reflection images corresponding to cases circled with dotted line. (b) and (c) are AFM images of the areas circled with a white line in (a).
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Pulsed laser cured printed line at different laser pulse durations. Printed lines in Fig. 1 were used. During laser curing, the polyimide film was heated at 200°C using the vacuum chuck in Fig. 1. Laser power, beam waist (1∕e2), frequency, translation speed and scanning gap are 0.85W, 30μm, 100Hz, 0.5mm∕s, and 10μm, respectively. Inset pictures in (a) are reflection images corresponding to cases circled with dotted line. (b) and (c) are AFM images of the areas circled with a white line in (a).
Figure 11

Pulsed laser cured printed line at different laser pulse durations. Printed lines in Fig. 1 were used. During laser curing, the polyimide film was heated at 200°C using the vacuum chuck in Fig. 1. Laser power, beam waist (1∕e2), frequency, translation speed and scanning gap are 0.85W, 30μm, 100Hz, 0.5mm∕s, and 10μm, respectively. Inset pictures in (a) are reflection images corresponding to cases circled with dotted line. (b) and (c) are AFM images of the areas circled with a white line in (a).

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+Transient temperature profiles in depth with 40μs heating time
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Transient temperature profiles in depth with 40μs heating time
Figure 12

Transient temperature profiles in depth with 40μs heating time

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+Schematic of nanoink printing and curing system
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Schematic of nanoink printing and curing system
Figure 1

Schematic of nanoink printing and curing system

Grahic Jump Location
+Bipolar voltage waveform applied to piezoelectric actuator
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Bipolar voltage waveform applied to piezoelectric actuator
Figure 2

Bipolar voltage waveform applied to piezoelectric actuator

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+Configuration of jet head and aluminum heating block. The nozzle to substrate distance was 1.2mm and in addition to Tj and Ts, the temperature at the aluminum heating block and the fluid temperature at the reservoir were measured to use as boundary conditions for numerical simulations. This configuration was used for numerical simulations.
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Configuration of jet head and aluminum heating block. The nozzle to substrate distance was 1.2mm and in addition to Tj and Ts, the temperature at the aluminum heating block and the fluid temperature at the reservoir were measured to use as boundary conditions for numerical simulations. This configuration was used for numerical simulations.
Figure 3

Configuration of jet head and aluminum heating block. The nozzle to substrate distance was 1.2mm and in addition to Tj and Ts, the temperature at the aluminum heating block and the fluid temperature at the reservoir were measured to use as boundary conditions for numerical simulations. This configuration was used for numerical simulations.

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+(a) Variation of droplet velocity at 1mm from the nozzle in response to changing voltage amplitude and temperature of jetting head and substrate. Gap distance between the substrate and nozzle is 1.2mm. Ts and Tj represent the temperature of the substrate and the jetting head. When only Ts is changed, Tj is set to 37°C. However, Tj increases to 41°C when Ts⩾107°C. Note that the nozzle temperature (Tn) is approximately equal to Tj when Ts=Tj, and that Tn is higher than Tj when Ts>Tj due to heat conduction from the substrate. Images (b), (c), (d) are obtained by multiple 2μs exposures with a 98μs delay when Ts=107°C and Tj=41°C.
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(a) Variation of droplet velocity at 1mm from the nozzle in response to changing voltage amplitude and temperature of jetting head and substrate. Gap distance between the substrate and nozzle is 1.2mm. Ts and Tj represent the temperature of the substrate and the jetting head. When only Ts is changed, Tj is set to 37°C. However, Tj increases to 41°C when Ts⩾107°C. Note that the nozzle temperature (Tn) is approximately equal to Tj when Ts=Tj, and that Tn is higher than Tj when Ts>Tj due to heat conduction from the substrate. Images (b), (c), (d) are obtained by multiple 2μs exposures with a 98μs delay when Ts=107°C and Tj=41°C.
Figure 4

(a) Variation of droplet velocity at 1mm from the nozzle in response to changing voltage amplitude and temperature of jetting head and substrate. Gap distance between the substrate and nozzle is 1.2mm. Ts and Tj represent the temperature of the substrate and the jetting head. When only Ts is changed, Tj is set to 37°C. However, Tj increases to 41°C when Ts⩾107°C. Note that the nozzle temperature (Tn) is approximately equal to Tj when Ts=Tj, and that Tn is higher than Tj when Ts>Tj due to heat conduction from the substrate. Images (b), (c), (d) are obtained by multiple 2μs exposures with a 98μs delay when Ts=107°C and Tj=41°C.

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+Variation of droplet velocity at 1mm from the nozzle changing dwell time, td [(B) in Fig. 2]. Ts changes and Tj is set to 37°C. Inset picture corresponds to the case for Ts=107°C and Vamp=13V and similar satellite droplet was observed at the dwell time of 30μs at different substrate temperatures and voltages.
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Variation of droplet velocity at 1mm from the nozzle changing dwell time, td [(B) in Fig. 2]. Ts changes and Tj is set to 37°C. Inset picture corresponds to the case for Ts=107°C and Vamp=13V and similar satellite droplet was observed at the dwell time of 30μs at different substrate temperatures and voltages.
Figure 5

Variation of droplet velocity at 1mm from the nozzle changing dwell time, td [(B) in Fig. 2]. Ts changes and Tj is set to 37°C. Inset picture corresponds to the case for Ts=107°C and Vamp=13V and similar satellite droplet was observed at the dwell time of 30μs at different substrate temperatures and voltages.

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