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Optics Express

Optics Express

  • Editor: Michael Duncan
  • Vol. 10, Iss. 21 — Oct. 21, 2002
  • pp: 1173–1178
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Single femtosecond pulse holography using polymethyl methacrylate

Yan Li, Kazuhiro Yamada, Tomohiko Ishizuka, Wataru Watanabe, Kazuyoshi Itoh, and Zhongxiang Zhou  »View Author Affiliations


Optics Express, Vol. 10, Issue 21, pp. 1173-1178 (2002)
http://dx.doi.org/10.1364/OE.10.001173


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Abstract

Holographic gratings have been written on the surface and inside transparent polymethyl methacrylate (PMMA) with individual 130 fs laser pulses at 800 nm. A surface-relief grating is fabricated by ablation and the diffraction efficiency is measured to be about 20%. A volume grating inside PMMA is formed by the change in the refractive index induced by the two-beam interference fringes. Holographic data storage on the surface is realized when one beam carries information. The stored information can be nondestructively reconstructed when the fluence of the read beam is reduced below the threshold.

© 2002 Optical Society of America

1. Introduction

With the rapid development of high-pulse-energy and high-peak-power lasers, particularly at UV wavelengths and in the femtosecond range, interest in laser direct writing of holographic gratings has increased. In order to replicate two-beam interference fringes as a change in its refractive index, absorption, or thickness, a recording material usually needs to be photosensitive or have high absorption at the wavelength of the writing beams. The resulting surface-relief or refractive-index gratings can be applied to diffractive optics, optical communication, holographic data storage, and optical information processing. Because of its high peak power, a femtosecond laser is able to fabricate holographic gratings in transparent materials by two-photon-absorption or multiphoton processes. With multiple femtosecond pulses, holographic gratings have been recorded in doped materials, such as photorefractive polymers sensitized by two-photon absorption [1

1. P. A. Blanche, B. Kippelen, A. Schulzgen, C. Fuentes-Hernandez, G. Ramos-Ortiz, J. F. Wang, E. Hendrickx, N. Peyghambarian, and S. R. Marder, “Photorefractive polymers sensitized by two-photo absorption,” Opt. Lett. 27, 19–21 (2002). [CrossRef]

], optical resin or syrup with a large two-photon cross-section dye [2

2. S. M. Kirkpatrick, J. W. Baur, C. M. Clark, L. R. Denny, D. W. Tomlin, B. R. Reinhardt, R. Kannan, and M. O. Stone, “Holographic recording using two-photo-induced photopolymerization,” Appl. Phys. A 69, 461–464 (1999). [CrossRef]

,3

3. D. J. Pikas, S. M. Kirkpatrick, D. W. Tomlin, L. Natarajan, V. Tondiglia, and T. J. Bunning, “Electrically switchable reflection holograms formed using two-photon photopolymerization,” Appl. Phys. A 74, 767–772 (2002). [CrossRef]

], photopolymeric cubes containing a highly efficient two-photon fluorophore encapsulated in a host epoxy [4

4. C. Diamond, Y. Boiko, and S. Esener, “Two-photon holography in 3-D photopolymer host-guest matrix,” Opt. Express 6, 64–68 (2000), http://www.opticsexpress.org/abstract.cfm?URI=OPEX-6-3-64. [CrossRef] [PubMed]

], and azo-dye-doped bulk PMMA [5

5. J. Si, J. Qiu, J. Zhai, Y. Shen, and K. Hirao, “Photoinduced permanent gratings inside bulk azodye-doped polymers by the coherent field of a femtosecond laser,” Appl. Phys. Lett. 80, 359–361 (2002). [CrossRef]

]. Time-resolved studies show that holography can be induced on the sub-picosecond time scale in barium fluoride [6

6. Th. Schneider and J. Reif, “Influence of an ultrafast transient refractive-index grating on nonlinear optical phenomena,” Phys. Rev. A 65, 023801-1–10 (2002). [CrossRef]

], charge-transfer polymers sensitized with varying concentrations of C60 [7

7. E. S. Manliloff, D. Vacar, D. W. McBranch, H. Wang, B. R. Mattes, J. Gao, and A. J. Heeger, “Ultrafast holography using charge-transfer polymers,” Opt. Comm. 141, 243–246 (1997). [CrossRef]

], and solid-state films of close-packed semiconductor nanocrystals [8

8. B. Kraabel, A. Malko, J. Hollingsworth, and V. I. Klimov, “Ultrafast dynamic holography in nanocrystal solids,” Appl. Phys. Lett. 78, 1814–1816 (2001). [CrossRef]

]. The induced transient gratings are useful for ultrafast optical information processing and the study of surface dynamics. It has been shown that permanent gratings are induced on glass when the irradiation intensity is above the damage threshold. Below this threshold, the grating relaxes when the recording beams are blocked [9

9. H. G. de Chatellus and E. Freysz, “Characterization and dynamics of gratings induced in glasses by femtosecond pulses,” Opt. Lett. 27, 1165–1167 (2002). [CrossRef]

]. With individual femtosecond laser pulses, permanent gratings have been encoded on the surface of glasses, crystals, and SiO2 thin films [10–13

10. K. Kawamura, T. Ogawa, N. Sarukura, M. Hirano, and H. Hosono, “Fabrication of surface relief gratings on transparent dielectric materials by two-beam holographic method using infrared femtosecond laser pulses,” Appl. Phys. B: Lasers Opt. 71, 119–121 (2000). [CrossRef]

]. We have recently demonstrated the holographic fabrication of multiple layers of gratings inside soda-lime glass [14

14. Y. Li, W. Watanabe, K. Yamada, T. Shinagawa, K. Itoh, J. Nishii, and Y. Jiang, “Holographic fabrication of multiple layers of grating inside soda-lime glass with femtosecond laser pulses,” Appl. Phys. Lett. 80, 1508–1510 (2002). [CrossRef]

] and holographic data storage on the surface of silica, soda-lime and lead glasses [15

15. Y. Li, W. Watanabe, K. Itoh, and X. Sun, “Holographic data storage on nonphotosensitive glass with a single femtosecond laser pulse,” Appl. Phys. Lett. 81, 1952–1954 (2002). [CrossRef]

].

Compared with inorganic glass materials, PMMA has good properties such as lightness, flexibility, and easy formability. In this paper we present experimental results of single femtosecond pulse holography in a commercial PMMA sheet (Shinkolite-A, Mitsubishi Rayon). The sample is almost completely transparent for the laser wavelength employed in our experiments. Both relief gratings on the surface and refractive-index gratings inside PMMA have been written. The application to holographic data storage is also demonstrated.

2. Relief gratings on the surface

The experiments were carried out in air at room temperature. The setup was similar to that described in Ref.14. A Ti:sapphire femtosecond laser system with regenerative amplification (Spitfire, Spectra-Physics) generates a 130 fs pulse centered at 800 nm. The pulse is split into two beams that are focused by two identical lenses of 500 mm focal length and then symmetrically incident on the sample at an angle θ of ∼17° to the normal. When the setup is adjusted to give a perfect spatial and temporal overlap of the two beams, we can observe a high contrast interference pattern with the aid of an optical microscope. The clearest fringe pattern lies in a plane that is through the two overlapping focal points and normal to the perpendicular bisector of the two recording beams, which will be referred to as the recording plane in the following of this paper.

Both relief gratings on the surface and refractive index gratings inside PMMA can be induced with only one femtosecond pulse. When we record a surface-relief grating, we move the sample so that the recording plane is on the front surface of the sample. After exposure, the bright interference fringes induce surface ablation when the fluence is above the threshold. Figure 1 shows a typical grating encoded on a PMMA sheet with thickness of 1 mm. This optical microscope image was taken under the illumination of a halogen lamp across the sample. The incident energy of each beam was ∼80 μJ or the total energy was ∼160 μJ. The grating size was ∼50 μm.

Fig.1. Optical microscope image of a surface-relief grating on PMMA written with pulse energy of each beam of ∼80 μJ.
Fig.2. (Top) AFM image of the grating structure and (bottom) the cross-sectional profile.

The grating profile was analyzed by an atomic force microscope (AFM). Figure 2 shows an AFM image of the central portion of a grating written under the same conditions. A cross-sectional profile is demonstrated at the bottom. The grating period d is ∼1.5 μm. It can be easily changed by varying the angle θ according to the formula d = λ/2sinθ, where λ, is wavelength of the writing beam. The groove depth is ∼ 300 nm. Because the grating is formed through the multiphoton process with a material-dependent threshold, the profile of the grating is not sinusoidal. Additionally, the profile changes with the incident energy of the recording beam. The higher the pulse energy, the deeper the grooves and the sharper the ridges between grooves. The grating size will correspondingly become larger. However, when the pulse energy of each beam is over 100 μJ, visible distortion appears in the central part where the intensity is much higher. The thin ridges between the deep grooves cannot stand alone and tend to topple.

The diffraction efficiency of the first order was measured to be ∼20% while the diffraction efficiency of the second order was less than 1%. When we wrote a grating, we used a single pulse. On the other hand, when we read the grating by either recording beam, we irradiated the grating with multiple pulses at a repetition rate of 1kHz. When the power of the read beam was below 8 mW or the pulse energy was below 8μJ, the surface-relief grating cannot be erased.

Fig.3. (a) A refractive index grating inside PMMA. The pulse energy of each recording beam was ∼80 μJ. (b) The diffraction pattern. The zero-order beam was attenuated by a 10% neutral density filter.

3. Refractive-index gratings inside PMMA

In our experiments, the pulse energy of each beam should be above 50 μJ to ablate a surface relief grating. However, if the pulse energy of each beam is over 100 μJ, distortion will appear as mentioned above. When only one recording beam is used, ablation will not happen if the pulse energy is lower than 180 μJ. Therefore, when the recording plane is deep inside the sample and the pulse energy of each recording beam is between 60 and 100 μJ, no surface ablation will occur because neither beam can cause surface damage. Nevertheless the intensities of bright interference fringes inside the sample are high enough to induce densification, resulting in the change in refractive index. Then, a refractive index grating is consequently written inside PMMA. Due to the threshold, the grating is localized within the focal volume and multiple layers of grating can be recorded inside PMMA with tight focusing as done in soda-lime glass [14

14. Y. Li, W. Watanabe, K. Yamada, T. Shinagawa, K. Itoh, J. Nishii, and Y. Jiang, “Holographic fabrication of multiple layers of grating inside soda-lime glass with femtosecond laser pulses,” Appl. Phys. Lett. 80, 1508–1510 (2002). [CrossRef]

].

Figure 3 presents the readout image of a grating formed by a single femtosecond pulse when the recording plane was at a depth of ∼200 μm. The pulse energy of each beam was ∼80 μJ. Unlike a surface relief grating, the recorded grating inside PMMA cannot be readout from the normal direction. But we can observe a weak image of the grating when the halogen lamp illuminated at Bragg angle. When we read the grating by either recording beam, we can obtain a clear image as shown in Fig. 3(a) which was taken through a 50× objective focusing onto the recording plane. These suggested that the recorded grating was a volume grating. From the top and side views, we estimated the thickness of the grating to be about 100 μm. The diffraction pattern is given in Fig. 3(b) in which the zero-order beam was attenuated by a 10% neutral density filter. The diffraction efficiency of the first order was about 0.8%. With the model of a sinusoidal volume phase grating, the maximum refractive-index change was calculated to be ∼2×10-4 using Kogelnik’s coupled wave theory.

4. Holographic data storage on PMMA

This setup can be easily adapted for holographic data storage [15

15. Y. Li, W. Watanabe, K. Itoh, and X. Sun, “Holographic data storage on nonphotosensitive glass with a single femtosecond laser pulse,” Appl. Phys. Lett. 81, 1952–1954 (2002). [CrossRef]

]. In the following we present the experimental results of the recording and reconstruction of a data image. One beam is used as the reference beam and focused using a 500 mm focal-length lens. The other beam is changed into the object beam. It is expanded by a Galileo telescope and modulated by a data mask. An aperture with a diameter of ∼15 mm is placed in front of the mask to ensure a uniform illumination. Then the data-bearing object beam is focused onto the sample surface by a lens of 50 mm focal length. The data mask, which consists of 9 spots in 3×3 array at a spacing of ∼3 mm as shown in Fig. 4(a), is placed in the front focal plane. After exposure to the interference fringes of the reference and object beams, a Fourier transformed hologram is recorded. Only one pulse was used to write a hologram. The stored information can be reconstructed by the reference beam. An example of the recorded holograms is presented in Fig. 4(b). The energies of the reference beam and object beam are both ∼80 μJ per pulse. The energy of the object beam is measured after the aperture in front of the data mask. The reconstructed data image is shown in Fig. 4(c). The recorded holograms cannot be erased during reconstruction when the power of the reference beam is reduced below the ablation threshold.

Fig.4. Holographic data storage on the surface of PMMA. (a) A data mask. (b) The corresponding hologram recorded with the pulse energy of each beam of ∼80 μJ. (c) The reconstruction image of the data mask.

5. Conclusion

In conclusion, both relief gratings on the surface and refractive index gratings inside PMMA have been written by the two-beam interference of individual 130 fs laser pulses at 800 nm. A surface-relief grating is fabricated by ablation. The higher the incident pulse energy, the larger the grating size and the deeper the groove depth. The diffraction efficiency of the first order can reach 20%. When one beam carries information, holographic data storage on the surface can be realized. A volume grating inside PMMA is formed by the change in the refractive index. Due to the threshold, the grating is localized within the focal volume and multiple layers of gratings can be recorded inside PMMA with tight focusing.

Acknowledgement

The authors are grateful to Hong-Bo Sun of Department of Applied Physics, Graduate School of Engineering, Osaka University, for useful discussion and technical help.

References and Links

1.

P. A. Blanche, B. Kippelen, A. Schulzgen, C. Fuentes-Hernandez, G. Ramos-Ortiz, J. F. Wang, E. Hendrickx, N. Peyghambarian, and S. R. Marder, “Photorefractive polymers sensitized by two-photo absorption,” Opt. Lett. 27, 19–21 (2002). [CrossRef]

2.

S. M. Kirkpatrick, J. W. Baur, C. M. Clark, L. R. Denny, D. W. Tomlin, B. R. Reinhardt, R. Kannan, and M. O. Stone, “Holographic recording using two-photo-induced photopolymerization,” Appl. Phys. A 69, 461–464 (1999). [CrossRef]

3.

D. J. Pikas, S. M. Kirkpatrick, D. W. Tomlin, L. Natarajan, V. Tondiglia, and T. J. Bunning, “Electrically switchable reflection holograms formed using two-photon photopolymerization,” Appl. Phys. A 74, 767–772 (2002). [CrossRef]

4.

C. Diamond, Y. Boiko, and S. Esener, “Two-photon holography in 3-D photopolymer host-guest matrix,” Opt. Express 6, 64–68 (2000), http://www.opticsexpress.org/abstract.cfm?URI=OPEX-6-3-64. [CrossRef] [PubMed]

5.

J. Si, J. Qiu, J. Zhai, Y. Shen, and K. Hirao, “Photoinduced permanent gratings inside bulk azodye-doped polymers by the coherent field of a femtosecond laser,” Appl. Phys. Lett. 80, 359–361 (2002). [CrossRef]

6.

Th. Schneider and J. Reif, “Influence of an ultrafast transient refractive-index grating on nonlinear optical phenomena,” Phys. Rev. A 65, 023801-1–10 (2002). [CrossRef]

7.

E. S. Manliloff, D. Vacar, D. W. McBranch, H. Wang, B. R. Mattes, J. Gao, and A. J. Heeger, “Ultrafast holography using charge-transfer polymers,” Opt. Comm. 141, 243–246 (1997). [CrossRef]

8.

B. Kraabel, A. Malko, J. Hollingsworth, and V. I. Klimov, “Ultrafast dynamic holography in nanocrystal solids,” Appl. Phys. Lett. 78, 1814–1816 (2001). [CrossRef]

9.

H. G. de Chatellus and E. Freysz, “Characterization and dynamics of gratings induced in glasses by femtosecond pulses,” Opt. Lett. 27, 1165–1167 (2002). [CrossRef]

10.

K. Kawamura, T. Ogawa, N. Sarukura, M. Hirano, and H. Hosono, “Fabrication of surface relief gratings on transparent dielectric materials by two-beam holographic method using infrared femtosecond laser pulses,” Appl. Phys. B: Lasers Opt. 71, 119–121 (2000). [CrossRef]

11.

K. Kawamura, N. Sarukura, M. Hirano, and H. Hosono, “Holographic encoding of permanent gratings embedded in diamond by two beam interference of a single femtosecond near-infrared laser pulse,” Jpn. J. Appl. Phys. Part 2 , 39, L767–L769 (2000). [CrossRef]

12.

K. Kawamura, N. Sarukura, M. Hirano, and H. Hosono, “Holographic encoding of fine-pitched micrograting structures in amorphous SiO2 thin films on silicon by a single femtosecond laser pulse,” Appl. Phys. Lett. 78, 1038–1040 (2001). [CrossRef]

13.

K. Kawamura, N. Sarukura, M. Hirano, N. Ito, and H. Hosono, “Periodic nanostructure array in crossed holographic gratings on silica glass by two interfered infrared-femtosecond laser pulses,” Appl. Phys. Lett. 79, 1228–1130 (2001). [CrossRef]

14.

Y. Li, W. Watanabe, K. Yamada, T. Shinagawa, K. Itoh, J. Nishii, and Y. Jiang, “Holographic fabrication of multiple layers of grating inside soda-lime glass with femtosecond laser pulses,” Appl. Phys. Lett. 80, 1508–1510 (2002). [CrossRef]

15.

Y. Li, W. Watanabe, K. Itoh, and X. Sun, “Holographic data storage on nonphotosensitive glass with a single femtosecond laser pulse,” Appl. Phys. Lett. 81, 1952–1954 (2002). [CrossRef]

OCIS Codes
(090.0090) Holography : Holography
(160.4890) Materials : Organic materials
(320.2250) Ultrafast optics : Femtosecond phenomena

ToC Category:
Research Papers

History
Original Manuscript: July 30, 2002
Revised Manuscript: October 11, 2002
Published: October 21, 2002

Citation
Yan Li, Kazuhiro Yamada, Tomohiko Ishizuka, Wataru Watanabe, Kazuyoshi Itoh, and Zhongxiang Zhou, "Single femtosecond pulse holography using polymethyl methacrylate," Opt. Express 10, 1173-1178 (2002)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-10-21-1173


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References

  1. P. A. Blanche, B. Kippelen, A. Schulzgen, C. Fuentes-Hernandez, G. Ramos-Ortiz, J. F. Wang, E. Hendrickx, N. Peyghambarian and S. R. Marder, �??Photorefractive polymers sensitized by two-photo absorption,�?? Opt. Lett. 27, 19-21 (2002). [CrossRef]
  2. S. M. Kirkpatrick, J.W. Baur, C. M. Clark, L. R. Denny, D.W. Tomlin, B. R. Reinhardt, R. Kannan and M. O. Stone, �??Holographic recording using two-photo-induced photopolymerization,�?? Appl. Phys. A 69, 461-464 (1999). [CrossRef]
  3. D. J. Pikas, S. M. Kirkpatrick, D. W. Tomlin, L. Natarajan, V. Tondiglia and T. J. Bunning, �??Electrically switchable reflection holograms formed using two-photon photopolymerization,�?? Appl. Phys. A 74, 767-772 (2002). [CrossRef]
  4. C. Diamond, Y. Boiko and S. Esener, �??Two-photon holography in 3-D photopolymer host-guest matrix,�?? Opt. Express 6, 64-68 (2000), <a href="http://www.opticsexpress.org/abstract.cfm?URI=OPEX-6-3-64">http://www.opticsexpress.org/abstract.cfm?URI=OPEX-6-3-64</a>. [CrossRef] [PubMed]
  5. J. Si, J. Qiu, J. Zhai, Y. Shen and K. Hirao, �??Photoinduced permanent gratings inside bulk azodye-doped polymers by the coherent field of a femtosecond laser,�?? Appl. Phys. Lett. 80, 359-361 (2002). [CrossRef]
  6. Th. Schneider and J. Reif, �??Influence of an ultrafast transient refractive-index grating on nonlinear optical phenomena,�?? Phys. Rev. A 65, 023801-1-10 (2002). [CrossRef]
  7. E. S.Manliloff, D. Vacar, D. W. McBranch, H.Wang, B. R. Mattes, J. Gao and A. J. Heeger, �??Ultrafast holography using charge-transfer polymers,�?? Opt. Commun. 141, 243-246 (1997). [CrossRef]
  8. B. Kraabel, A. Malko, J. Hollingsworth and V. I. Klimov, �??Ultrafast dynamic holography in nanocrystal solids,�?? Appl. Phys. Lett. 78, 1814-1816 (2001). [CrossRef]
  9. H. G. de Chatellus and E. Freysz, �??Characterization and dynamics of gratings induced in glasses by femtosecond pulses,�?? Opt. Lett. 27, 1165-1167 (2002). [CrossRef]
  10. K. Kawamura, T. Ogawa, N. Sarukura, M. Hirano and H. Hosono, �??Fabrication of surface relief gratings on transparent dielectric materials by two-beam holographic method using infrared femtosecond laser pulses,�?? Appl. Phys. B: Lasers Opt. 71, 119-121 (2000). [CrossRef]
  11. K. Kawamura, N. Sarukura, M. Hirano and H. Hosono, �??Holographic encoding of permanent gratings embedded in diamond by two beam interference of a single femtosecond near-infrared laser pulse,�?? Jpn. J. Appl. Phys. Part 2, 39, L767-L769 (2000). [CrossRef]
  12. K. Kawamura, N. Sarukura, M. Hirano and H. Hosono, �??Holographic encoding of fine-pitched micrograting structures in amorphous SiO2 thin films on silicon by a single femtosecond laser pulse,�?? Appl. Phys. Lett. 78, 1038-1040 (2001). [CrossRef]
  13. K. Kawamura, N. Sarukura, M. Hirano, N. Ito and H. Hosono, �??Periodic nanostructure array in crossed holographic gratings on silica glass by two interfered infrared-femtosecond laser pulses,�?? Appl. Phys. Lett. 79, 1228-1130 (2001). [CrossRef]
  14. Y. Li,W.Watanabe, K. Yamada, T. Shinagawa, K. Itoh, J. Nishii and Y. Jiang, �??Holographic fabrication of multiple layers of grating inside soda-lime glass with femtosecond laser pulses,�?? Appl. Phys. Lett. 80, 1508-1510 (2002). [CrossRef]
  15. Y. Li, W. Watanabe, K. Itoh and X. Sun, �??Holographic data storage on nonphotosensitive glass with a single femtosecond laser pulse,�?? Appl. Phys. Lett. 81, 1952-1954 (2002). [CrossRef]

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