We demonstrate capability to structure photo-polymers with sub-wavelength resolution, ∼ 200 – 500 nm, and retrieve three-dimensional (3D) structures using a picosecond laser exposure. This alternative to commonly used ultra-short femtosecond lasers extends accessability of 3D direct write. A popular hybrid sol-gel resist SZ2080 was used for quantitative determination of structuring resolution at 1064 nm and 532 nm wavelengths and for pulses of 8–25 ps duration at the repetition rates of 0.2 – 1 MHz. Systematic study of feature size dependence of 3D suspended nano-rods shows that linear power dependence of photopolymerization on the dose-per-pulse becomes dominant at higher repetition rates (≥ 0.5 MHz) while the two-photon nonlinear absorption is still distinguishable at rates lower than 0.2 MHz and shorter pulses (≤ 8 ps). Thermal accumulation defines polymerization when cooling time of the focal volume is larger than separation between pulses. Photopolymerization and its scaling mechanisms, quality, and fidelity at tight focusing of fs-, ps-, and cw-laser radiation are revealed and explained. 3D scaffolds for biomedicine and microlenses for optical applications are fabricated by the ps-laser direct write.

© 2011 Optical Society of America

1. S. Maruo, O. Nakamura, and S. Kawata, “Three-dimensional microfabrication with two-photon-absorbed photopolymerization,” Opt. Lett. 2, 132–134 (1997). [CrossRef]
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3. M. Farsari and B. N. Chichkov, “Materials processing: two-photon fabrication,” Nat. Photonics 3, 450–452 (2009). [CrossRef]
4. S. Juodkazis, V. Mizeikis, and H. Misawa, “Three-dimensional microfabrication of materials by femtosecond lasers for photonics applications,” J. Appl. Phys. 106, 051101 (2009). [CrossRef]
5. A. Ostendorf and B. N. Chichkov, “Two-photon polymerization: a new approach to micromachining,” Photon. Spectra 40, 72–80 (2006).
6. F. Qi, Y. Li, D. Tan, H. Yang, and Q. Gong, “Polymerized nanotips via two-photon photopolymerization,” Opt. Express 15, 971–976 (2007). [CrossRef] [PubMed]
7. S. Juodkazis, V. Mizeikis, K. K. Seet, M. Miwa, and H. Misawa, “Two-photon lithography of nanorods in SU-8 photoresist,” Nanotechnology 16, 846–849 (2005). [CrossRef]
8. I. Sakellari, A. Gaidukeviciute, A. Giakoumaki, D. Gray, C. Fotakis, M. Farsari, M. Vamvakaki, C. Reinhardt, A. Ovsianikov, and B. N. Chichkov, “Two-photon polymerization of titanium-containing sol-gel composites for three-dimensional structure fabrication,” Appl. Phys., A Mater. Sci. Process. 100, 359–364 (2010). [CrossRef]
9. R. J. Narayan, C. Jin, A. Doraiswamy, I. N. Mihailescu, M. Jelinek, A. Ovsianikov, B. Chichkov, and D. B. Chrisey, “Laser processing of advanced bioceramics,” Adv. Eng. Mater. 7, 1083–1098 (2005). [CrossRef]
10. A. Ovsianikov, M. Malinauskas, S. Schlie, B. Chichkov, S. Gittard, R. Narayan, M. Löbler, K. Sternberg, K.-P. Schmitz, and A. Haverich, “Three-dimensional laser micro- and nano-structuring of acrylated poly(ethylene glycol) materials and evaluation of their cytoxicity for tissue engineering applications,” Acta Biomater. 7, 967–974 (2011). [CrossRef]
11. M. Malinauskas and V. Purlys, A. Žukauskas, G. Bičkauskaitė, T. Gertus, P. Danilevičius, D. Paipulas, M. Rutkauskas, H. Gilbergs, D. Baltriukienė, L. Bukelskis, R. Širmenis, V. Bukelskienė, R. Gadonas, V. Sirvydis, and A. Piskarskas, “Laser two-photon polymerization micro- and nanostructuringover a large area on various substrates,” Proc. SPIE 7715, 77157F–1 (2010).
12. M. Malinauskas, A. Žukauskas, V. Purlys, K. Belazaras, A. Momot, D. Paipulas, R. Gadonas, A. Piskarskas, H. Gilbergs, A. Gaidukevičiūtė, I. Sakellari, M. Farsari, and S. Juodkazis, “Femtosecond laser polymerization of hybrid/integrated micro-optical elements and their characterization,” J. Opt. 12, 124010 (2010). [CrossRef]
13. A. Ovsianikov and A. Gaidukevičiūtė, B. N. Chichkov, M . Oubaha, B. D. MacCraith, I. Sakellari, A. Giakoumaki, D. Gray, M. Vamvakaki, M. Farsari, and C. Fotakis, “Two-photon polymerization of hybrid sol-gel materials for photonics applications,” Laser Chem. 2008, 493059 (2008). [CrossRef]
14. M. Malinauskas and H. Gilbergs, A. Žukauskas, V. Purlys, D. Paipulas, and R. Gadonas, “A femtosecond laser induced two-photon photopolymerization technique for structuring microlenses,” J. Opt. 12, 035204 (2010). [CrossRef]
15. C. Schizas, V. Melissinaki, A. Gaidukevičiūtė, C. Reinhardt, C. Ohrt, V. Dedoussis, B. Chichkov, C. Fotakis, M. Farsari, and D. Karalekas, “On the design and fabrication by two-photon polymerization of a readily assembled micro-valve,” Int. J. Adv. Manuf. Technol. 48, 435–441 (2010). [CrossRef]
16. A. Ovsianikov, A. Doraiswamy, R. Narayan, and B. N. Chichkov, “Two-photon polymerization for fabrication of biomedical devices,” Proc. SPIE 6465, 64650O (2007). [CrossRef]
17. S. Maruo and K. Ikuta, “Three-dimensional microfabrication by use of single-photon-absorbed polymerization,” Appl. Phys. Lett. 76, 2656–2658 (2000). [CrossRef]
18. I. Wang, M. Bouriau, P. L. Baldeck, C. Martineau, and C. Andraud, “Three-dimensional microfabrication by two-photon-initiated polymerization with low-cost microlaser,” Opt. Lett. 27, 1348–1350 (2002). [CrossRef]
19. M. Thiel, J. Fischer, G. von Freymann, and M. Wegener, “Direct laser writing of three-dimensional submicron structures using a continuous-wave laser at 532 nm,” Appl. Phys. Lett. 97, 221102 (2010). [CrossRef]
20. A. Pikulin and N. Bityurin, “Spatial resolution in polymerization of sample features at nanoscale,” Phys. Rev. B 75, 195430 (2009).
21. M. Malinauskas, A. Žukauskas, G. Bičkauskaitė, R. Gadonas, and S. Juodkazis, “Mechanisms of threedimensional structuring of photo-polymers by tightly focussed femtosecond laser pulses,” Opt. Express 18, 10209–10221 (2010). [CrossRef] [PubMed]
22. S. Juodkazis, Y. Nishi, H. Misawa, V. Mizeikis, O. Schecker, R. Waitz, P. Leiderer, and E. Scheer, “Optical transmission and laser structuring of silicon membranes,” Opt. Express 17, 15308–15317 (2009). [CrossRef] [PubMed]
23. A. Marcinkevičius, V. Mizeikis, S. Juodkazis, S. Matsuo, and H. Misawa, “Effect of refractive index-mismatch on laser microfabrication in silica glass,” Appl. Phys., A Mater. Sci. Process. 76, 257–260 (2003). [CrossRef]
24. J. Morikawa, A. Orie, T. Hashimoto, and S. Juodkazis, “Thermal diffusivity in femtosecond-laser-structured micro-volumes of polymers,” Appl. Phys., A Mater. Sci. Process. 98, 551–556 (2009). [CrossRef]
25. M. Beresna, T. Gertus, R. Tomasiunas, H. Misawa, and S. Juodkazis, “Three-dimensional modeling of the heataffected zone in laser machining applications,” Laser Chem. 2008, 976205 (2008). [CrossRef]
26. N. Murazawa, S. Juodkazis, H. Misawa, and K. Kamada, “Two-photon excitation of dye-doped liquid crystal by a cw-laser irradiation,” Mol. Cryst. Liq. Cryst. (Phila. Pa.) 489, 310–319 (2008). [CrossRef]
27. M. P. Hernández-Garay, O. Martínez-Matos, J. G. Izquierdo, M. L. Calvo, P. Vaveliuk, P. Cheben, and L. Banares, “Femtosecond spectral pulse shaping with holographic gratings recorded in photopolymerizable glasses,” Opt. Express 19, 1516–1527 (2011). [CrossRef] [PubMed]
28. S. Nolte, M. Will, J. Burghoff, and A. Tünnermann, “Femtosecond waveguide writing: a new avenue to threedimensional integrated optics,” Appl. Phys., A Mater. Sci. Process. 77, 109–111 (2003). [CrossRef]
29. W. Gawelda, D. Puerto, J. Siegel, A. Ferrer, A. Ruiz de la Cruz, H. Fernandez, and J. Solis, “Ultrafast imaging of transient electronic plasmas produced in conditions of femtosecond waveguide writing in dielectrics,” Appl. Phys. Lett. 93, 121109 (2008). [CrossRef]
30. G. Cheng, K. Mishchik, C. Mauclair, E. Audouard, and R. Stoian, “Ultrafast laser photoinscription of polarization sensitive devices in bulk silica glass,” Opt. Express 17, 9515–9525 (2009). [CrossRef] [PubMed]
31. D. Day and M. Gu, “Microchannel fabrication in PMMA based on localized heating by nanojoule high repetition rate femtosecond pulses,” Opt. Express 13, 5939–5946 (2005). [CrossRef] [PubMed]
32. L. Shah, A. Arai, S. Eaton, and P. Herman, “Waveguide writing in fused silica with a femtosecond fiber laser at 522 nm and 1 MHz repetition rate,” Opt. Express 13, 1999–2006 (2005). [CrossRef] [PubMed]
33. J. Siebenmorgen, K. Petermann, G. Huber, K. Rademaker, S. Nolte, and A. T¨unnermann, “Femtosecond laser written stress-induced Nd:Y3Al5O12(Nd:YAG) channel waveguide laser,” Appl. Phys. B 97, 251–255 (2009). [CrossRef]
34. K. K. Seet, S. Juodkazis, V. Jarutis, and H. Misawa, “Feature-size reduction of photopolymerized structures by femtosecond optical curing of SU-8,” Appl. Phys. Lett. 89, 024106 (2006). [CrossRef]

Acta Biomater.

• A. Ovsianikov, M. Malinauskas, S. Schlie, B. Chichkov, S. Gittard, R. Narayan, M. Löbler, K. Sternberg, K.-P. Schmitz, and A. Haverich, “Three-dimensional laser micro- and nano-structuring of acrylated poly(ethylene glycol) materials and evaluation of their cytoxicity for tissue engineering applications,” Acta Biomater. 7, 967–974 (2011). [CrossRef]

Adv. Eng. Mater.

• R. J. Narayan, C. Jin, A. Doraiswamy, I. N. Mihailescu, M. Jelinek, A. Ovsianikov, B. Chichkov, and D. B. Chrisey, “Laser processing of advanced bioceramics,” Adv. Eng. Mater. 7, 1083–1098 (2005). [CrossRef]

Appl. Phys. B

• J. Siebenmorgen, K. Petermann, G. Huber, K. Rademaker, S. Nolte, and A. T¨unnermann, “Femtosecond laser written stress-induced Nd:Y3Al5O12(Nd:YAG) channel waveguide laser,” Appl. Phys. B 97, 251–255 (2009). [CrossRef]

Appl. Phys. Lett.

• K. K. Seet, S. Juodkazis, V. Jarutis, and H. Misawa, “Feature-size reduction of photopolymerized structures by femtosecond optical curing of SU-8,” Appl. Phys. Lett. 89, 024106 (2006). [CrossRef]
• W. Gawelda, D. Puerto, J. Siegel, A. Ferrer, A. Ruiz de la Cruz, H. Fernandez, and J. Solis, “Ultrafast imaging of transient electronic plasmas produced in conditions of femtosecond waveguide writing in dielectrics,” Appl. Phys. Lett. 93, 121109 (2008). [CrossRef]
• S. Maruo and K. Ikuta, “Three-dimensional microfabrication by use of single-photon-absorbed polymerization,” Appl. Phys. Lett. 76, 2656–2658 (2000). [CrossRef]
• M. Thiel, J. Fischer, G. von Freymann, and M. Wegener, “Direct laser writing of three-dimensional submicron structures using a continuous-wave laser at 532 nm,” Appl. Phys. Lett. 97, 221102 (2010). [CrossRef]

Appl. Phys., A Mater. Sci. Process.

• A. Marcinkevičius, V. Mizeikis, S. Juodkazis, S. Matsuo, and H. Misawa, “Effect of refractive index-mismatch on laser microfabrication in silica glass,” Appl. Phys., A Mater. Sci. Process. 76, 257–260 (2003). [CrossRef]
• J. Morikawa, A. Orie, T. Hashimoto, and S. Juodkazis, “Thermal diffusivity in femtosecond-laser-structured micro-volumes of polymers,” Appl. Phys., A Mater. Sci. Process. 98, 551–556 (2009). [CrossRef]
• I. Sakellari, A. Gaidukeviciute, A. Giakoumaki, D. Gray, C. Fotakis, M. Farsari, M. Vamvakaki, C. Reinhardt, A. Ovsianikov, and B. N. Chichkov, “Two-photon polymerization of titanium-containing sol-gel composites for three-dimensional structure fabrication,” Appl. Phys., A Mater. Sci. Process. 100, 359–364 (2010). [CrossRef]
• S. Nolte, M. Will, J. Burghoff, and A. Tünnermann, “Femtosecond waveguide writing: a new avenue to threedimensional integrated optics,” Appl. Phys., A Mater. Sci. Process. 77, 109–111 (2003). [CrossRef]

Int. J. Adv. Manuf. Technol.

• C. Schizas, V. Melissinaki, A. Gaidukevičiūtė, C. Reinhardt, C. Ohrt, V. Dedoussis, B. Chichkov, C. Fotakis, M. Farsari, and D. Karalekas, “On the design and fabrication by two-photon polymerization of a readily assembled micro-valve,” Int. J. Adv. Manuf. Technol. 48, 435–441 (2010). [CrossRef]

J. Appl. Phys.

• S. Juodkazis, V. Mizeikis, and H. Misawa, “Three-dimensional microfabrication of materials by femtosecond lasers for photonics applications,” J. Appl. Phys. 106, 051101 (2009). [CrossRef]

J. Opt.

• M. Malinauskas and H. Gilbergs, A. Žukauskas, V. Purlys, D. Paipulas, and R. Gadonas, “A femtosecond laser induced two-photon photopolymerization technique for structuring microlenses,” J. Opt. 12, 035204 (2010). [CrossRef]
• M. Malinauskas, A. Žukauskas, V. Purlys, K. Belazaras, A. Momot, D. Paipulas, R. Gadonas, A. Piskarskas, H. Gilbergs, A. Gaidukevičiūtė, I. Sakellari, M. Farsari, and S. Juodkazis, “Femtosecond laser polymerization of hybrid/integrated micro-optical elements and their characterization,” J. Opt. 12, 124010 (2010). [CrossRef]

Laser Chem.

• A. Ovsianikov and A. Gaidukevičiūtė, B. N. Chichkov, M . Oubaha, B. D. MacCraith, I. Sakellari, A. Giakoumaki, D. Gray, M. Vamvakaki, M. Farsari, and C. Fotakis, “Two-photon polymerization of hybrid sol-gel materials for photonics applications,” Laser Chem. 2008, 493059 (2008). [CrossRef]
• M. Beresna, T. Gertus, R. Tomasiunas, H. Misawa, and S. Juodkazis, “Three-dimensional modeling of the heataffected zone in laser machining applications,” Laser Chem. 2008, 976205 (2008). [CrossRef]

Mol. Cryst. Liq. Cryst. (Phila. Pa.)

• N. Murazawa, S. Juodkazis, H. Misawa, and K. Kamada, “Two-photon excitation of dye-doped liquid crystal by a cw-laser irradiation,” Mol. Cryst. Liq. Cryst. (Phila. Pa.) 489, 310–319 (2008). [CrossRef]

Nano Today

• Y. L. Zhang, Q. D. Chen, H. Xia, and H. B. Sun, “Designable 3D nanofabrication by femtosecond laser direct writing,” Nano Today 5, 435–448 (2010). [CrossRef]

Nanotechnology

• S. Juodkazis, V. Mizeikis, K. K. Seet, M. Miwa, and H. Misawa, “Two-photon lithography of nanorods in SU-8 photoresist,” Nanotechnology 16, 846–849 (2005). [CrossRef]

Nat. Photonics

• M. Farsari and B. N. Chichkov, “Materials processing: two-photon fabrication,” Nat. Photonics 3, 450–452 (2009). [CrossRef]

Opt. Express

• F. Qi, Y. Li, D. Tan, H. Yang, and Q. Gong, “Polymerized nanotips via two-photon photopolymerization,” Opt. Express 15, 971–976 (2007). [CrossRef] [PubMed]
• M. P. Hernández-Garay, O. Martínez-Matos, J. G. Izquierdo, M. L. Calvo, P. Vaveliuk, P. Cheben, and L. Banares, “Femtosecond spectral pulse shaping with holographic gratings recorded in photopolymerizable glasses,” Opt. Express 19, 1516–1527 (2011). [CrossRef] [PubMed]
• G. Cheng, K. Mishchik, C. Mauclair, E. Audouard, and R. Stoian, “Ultrafast laser photoinscription of polarization sensitive devices in bulk silica glass,” Opt. Express 17, 9515–9525 (2009). [CrossRef] [PubMed]
• D. Day and M. Gu, “Microchannel fabrication in PMMA based on localized heating by nanojoule high repetition rate femtosecond pulses,” Opt. Express 13, 5939–5946 (2005). [CrossRef] [PubMed]
• L. Shah, A. Arai, S. Eaton, and P. Herman, “Waveguide writing in fused silica with a femtosecond fiber laser at 522 nm and 1 MHz repetition rate,” Opt. Express 13, 1999–2006 (2005). [CrossRef] [PubMed]
• M. Malinauskas, A. Žukauskas, G. Bičkauskaitė, R. Gadonas, and S. Juodkazis, “Mechanisms of threedimensional structuring of photo-polymers by tightly focussed femtosecond laser pulses,” Opt. Express 18, 10209–10221 (2010). [CrossRef] [PubMed]
• S. Juodkazis, Y. Nishi, H. Misawa, V. Mizeikis, O. Schecker, R. Waitz, P. Leiderer, and E. Scheer, “Optical transmission and laser structuring of silicon membranes,” Opt. Express 17, 15308–15317 (2009). [CrossRef] [PubMed]

Opt. Lett.

• I. Wang, M. Bouriau, P. L. Baldeck, C. Martineau, and C. Andraud, “Three-dimensional microfabrication by two-photon-initiated polymerization with low-cost microlaser,” Opt. Lett. 27, 1348–1350 (2002). [CrossRef]
• S. Maruo, O. Nakamura, and S. Kawata, “Three-dimensional microfabrication with two-photon-absorbed photopolymerization,” Opt. Lett. 2, 132–134 (1997). [CrossRef]

Photon. Spectra

• A. Ostendorf and B. N. Chichkov, “Two-photon polymerization: a new approach to micromachining,” Photon. Spectra 40, 72–80 (2006).

Phys. Rev. B

• A. Pikulin and N. Bityurin, “Spatial resolution in polymerization of sample features at nanoscale,” Phys. Rev. B 75, 195430 (2009).

Proc. SPIE

• M. Malinauskas and V. Purlys, A. Žukauskas, G. Bičkauskaitė, T. Gertus, P. Danilevičius, D. Paipulas, M. Rutkauskas, H. Gilbergs, D. Baltriukienė, L. Bukelskis, R. Širmenis, V. Bukelskienė, R. Gadonas, V. Sirvydis, and A. Piskarskas, “Laser two-photon polymerization micro- and nanostructuringover a large area on various substrates,” Proc. SPIE 7715, 77157F–1 (2010).
• A. Ovsianikov, A. Doraiswamy, R. Narayan, and B. N. Chichkov, “Two-photon polymerization for fabrication of biomedical devices,” Proc. SPIE 6465, 64650O (2007). [CrossRef]

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