Abstract

We report a technique to encode grayscale digital images in thin films composed of copolymers containing coumarins. A nonlinear microscopy setup was implemented and two nonlinear optical processes were used to store and read information. A third-order process (two-photon absorption) was used to photoinduce a controlled dimer-to-monomer ratio within a defined tiny volume in the material, which corresponds to each recorded bit of data. Moreover, a second-order process (second-harmonic generation) was used to read the stored information, which has been found to be highly dependent upon the monomer-to-dimer ratio.

© 2013 Optical Society of America

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  1. S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
    [CrossRef]
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    [CrossRef]
  3. T. Watanabe and M. Watanabe, Opt. Express 19, 24147 (2011).
    [CrossRef]
  4. Y.-C. Jeong, B. Jung, D. Ahn, and J.-K. Park, Opt. Express 18, 25008 (2010).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  8. J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  13. P. Zijlstra, J. W. M. Chon, and M. Gu, Nature 459, 410 (2009).
    [CrossRef]
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    [CrossRef]
  15. F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
    [CrossRef]
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    [CrossRef]
  17. Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
    [CrossRef]

2013 (2)

Y. Yamashita, M. Kuwabara, K. Torii, and H. Yoshida, Opt. Express 21, 3133 (2013).
[CrossRef]

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

2012 (1)

G. M. Church, Y. Gao, and S. Kosuri, Science 337, 1628 (2012).
[CrossRef]

2011 (3)

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

T. Watanabe and M. Watanabe, Opt. Express 19, 24147 (2011).
[CrossRef]

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

2010 (2)

Y.-C. Jeong, B. Jung, D. Ahn, and J.-K. Park, Opt. Express 18, 25008 (2010).
[CrossRef]

K. Iliopoulos, O. Krupka, D. Gindre, and M. Sallé, J. Am. Chem. Soc. 132, 14343 (2010).
[CrossRef]

2009 (2)

P. Zijlstra, J. W. M. Chon, and M. Gu, Nature 459, 410 (2009).
[CrossRef]

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

2008 (1)

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

2007 (2)

2006 (2)

D. Gindre, A. Boeglin, A. Fort, L. Mager, and K. D. Dorkenoo, Opt. Express 14, 9896 (2006).
[CrossRef]

C. C. Corredor, Z.-L. Huang, and K. D. Belfield, Adv. Mater. 18, 2910 (2006).
[CrossRef]

2000 (1)

S. Kawata and Y. Kawata, Chem. Rev. 100, 1777 (2000).
[CrossRef]

1994 (1)

J. F. Heanue, M. C. Bashaw, and L. Hesselink, Science 265, 749 (1994).
[CrossRef]

Ahn, D.

Barsella, A.

Bashaw, M. C.

J. F. Heanue, M. C. Bashaw, and L. Hesselink, Science 265, 749 (1994).
[CrossRef]

Belfield, K. D.

C. C. Corredor, Z.-L. Huang, and K. D. Belfield, Adv. Mater. 18, 2910 (2006).
[CrossRef]

Boeglin, A.

Castagna, R.

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

Champigny, E.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

Chernyak, L.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Chon, J. W. M.

P. Zijlstra, J. W. M. Chon, and M. Gu, Nature 459, 410 (2009).
[CrossRef]

Chu, S.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Church, G. M.

G. M. Church, Y. Gao, and S. Kosuri, Science 337, 1628 (2012).
[CrossRef]

Corredor, C. C.

C. C. Corredor, Z.-L. Huang, and K. D. Belfield, Adv. Mater. 18, 2910 (2006).
[CrossRef]

Crégut, O.

Criante, L.

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

Dorkenoo, K. D.

Essaïdi, Z.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

Fort, A.

Gao, Y.

G. M. Church, Y. Gao, and S. Kosuri, Science 337, 1628 (2012).
[CrossRef]

Gindre, D.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

K. Iliopoulos, O. Krupka, D. Gindre, and M. Sallé, J. Am. Chem. Soc. 132, 14343 (2010).
[CrossRef]

D. Gindre, I. Ka, A. Boeglin, A. Fort, and K. D. Dorkenoo, Appl. Phys. Lett. 90, 094103 (2007).
[CrossRef]

D. Gindre, A. Boeglin, G. Taupier, O. Crégut, J.-P. Vola, A. Barsella, L. Mager, A. Fort, and K. D. Dorkenoo, J. Opt. Soc. Am. B 24, 532 (2007).
[CrossRef]

D. Gindre, A. Boeglin, A. Fort, L. Mager, and K. D. Dorkenoo, Opt. Express 14, 9896 (2006).
[CrossRef]

Gu, M.

P. Zijlstra, J. W. M. Chon, and M. Gu, Nature 459, 410 (2009).
[CrossRef]

Heanue, J. F.

J. F. Heanue, M. C. Bashaw, and L. Hesselink, Science 265, 749 (1994).
[CrossRef]

Hesselink, L.

J. F. Heanue, M. C. Bashaw, and L. Hesselink, Science 265, 749 (1994).
[CrossRef]

Huang, Z.-L.

C. C. Corredor, Z.-L. Huang, and K. D. Belfield, Adv. Mater. 18, 2910 (2006).
[CrossRef]

Iliopoulos, K.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

K. Iliopoulos, O. Krupka, D. Gindre, and M. Sallé, J. Am. Chem. Soc. 132, 14343 (2010).
[CrossRef]

Jeong, Y.-C.

Jiang, G.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Jiang, L.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Johnson, J. R.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Jung, B.

Ka, I.

D. Gindre, I. Ka, A. Boeglin, A. Fort, and K. D. Dorkenoo, Appl. Phys. Lett. 90, 094103 (2007).
[CrossRef]

Kawata, S.

S. Kawata and Y. Kawata, Chem. Rev. 100, 1777 (2000).
[CrossRef]

Kawata, Y.

S. Kawata and Y. Kawata, Chem. Rev. 100, 1777 (2000).
[CrossRef]

Kong, J.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Kosuri, S.

G. M. Church, Y. Gao, and S. Kosuri, Science 337, 1628 (2012).
[CrossRef]

Krupka, O.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

K. Iliopoulos, O. Krupka, D. Gindre, and M. Sallé, J. Am. Chem. Soc. 132, 14343 (2010).
[CrossRef]

Kuwabara, M.

Li, F.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Li, L.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Li, Y.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Lin, Y.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Liu, J.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Lott, J.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Lucchetta, D. E.

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

Mager, L.

Park, J.-K.

Ren, J.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Ryan, C.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Sahraoui, B.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

Sallé, M.

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

K. Iliopoulos, O. Krupka, D. Gindre, and M. Sallé, J. Am. Chem. Soc. 132, 14343 (2010).
[CrossRef]

Schiraldi, D. A.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Shan, J.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Simoni, F.

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

Singer, K. D.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Song, Y.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Tang, H.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Taupier, G.

Torii, K.

Valle, B.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Vita, F.

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

Vola, J.-P.

Wang, G.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Watanabe, M.

Watanabe, T.

Weder, C.

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Xia, A.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Yamashita, Y.

Yoshida, H.

Zhao, J.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Zhou, W.

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Zhu, D.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Zhuang, J.

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Zijlstra, P.

P. Zijlstra, J. W. M. Chon, and M. Gu, Nature 459, 410 (2009).
[CrossRef]

Adv. Mater. (3)

R. Castagna, F. Vita, D. E. Lucchetta, L. Criante, and F. Simoni, Adv. Mater. 21, 589 (2009).
[CrossRef]

C. C. Corredor, Z.-L. Huang, and K. D. Belfield, Adv. Mater. 18, 2910 (2006).
[CrossRef]

J. Lott, C. Ryan, B. Valle, J. R. Johnson, D. A. Schiraldi, J. Shan, K. D. Singer, and C. Weder, Adv. Mater. 23, 2425 (2011).
[CrossRef]

Appl. Phys. Lett. (1)

D. Gindre, I. Ka, A. Boeglin, A. Fort, and K. D. Dorkenoo, Appl. Phys. Lett. 90, 094103 (2007).
[CrossRef]

Chem. Mater. (1)

F. Li, J. Zhuang, G. Jiang, H. Tang, A. Xia, L. Jiang, Y. Song, Y. Li, and D. Zhu, Chem. Mater. 20, 1194 (2008).
[CrossRef]

Chem. Rev. (1)

S. Kawata and Y. Kawata, Chem. Rev. 100, 1777 (2000).
[CrossRef]

J. Am. Chem. Soc. (1)

K. Iliopoulos, O. Krupka, D. Gindre, and M. Sallé, J. Am. Chem. Soc. 132, 14343 (2010).
[CrossRef]

J. Opt. Soc. Am. B (1)

Nat. Nanotechnol. (1)

S. Chu, G. Wang, W. Zhou, Y. Lin, L. Chernyak, J. Zhao, J. Kong, L. Li, J. Ren, and J. Liu, Nat. Nanotechnol. 6, 506 (2011).
[CrossRef]

Nature (1)

P. Zijlstra, J. W. M. Chon, and M. Gu, Nature 459, 410 (2009).
[CrossRef]

Opt. Express (4)

Opt. Mater. (1)

Z. Essaïdi, O. Krupka, K. Iliopoulos, E. Champigny, B. Sahraoui, M. Sallé, and D. Gindre, Opt. Mater. 35, 576 (2013).
[CrossRef]

Science (2)

G. M. Church, Y. Gao, and S. Kosuri, Science 337, 1628 (2012).
[CrossRef]

J. F. Heanue, M. C. Bashaw, and L. Hesselink, Science 265, 749 (1994).
[CrossRef]

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Figures (4)

Fig. 1.
Fig. 1.

(a) Molecular structure of the initial coumarin/copolymer (schematized by the orange ellipse in the yellow circle) and the photo-cross-linked state of the coumarin/copolymer (blue ellipse in the soft blue circle) obtained by ultraviolet irradiation. (b) Principle of analogic level storage. The oriented state of the copolymer (2) was induced from the initial disordered state (1) by using the corona poling technique. The laser is then focalized on a small area of the film. At a high power of the laser or long-time exposure (3), all molecules in the voxel become cross-linked (4). At a lower power or a lower exposure time (3), only a part of the molecules becomes dimerized (4).

Fig. 2.
Fig. 2.

(a) Optical setup. P, polarizer; BS, beam splitter; M, mirrors; TS, telescope; F1, long-pass filter; OB, microscope objective; S, sample; L, collection lens; F2, short-pass filter; CCD, charge-coupled device camera. (b) Definition of the plane of the sample. The orthonormal coordinate system xyz is defined by the translation stages, and A1, A2, and A3 are three points on the thin film, which permit defining the plane equation (u,v) of the sample.

Fig. 3.
Fig. 3.

(a) Reference image (upper part) and SHG image (lower part) used for calibration. (b) Normalized SHG intensity as a function of the exposure time during the writing process.

Fig. 4.
Fig. 4.

(a) Normalized SHG image obtained after a scan of the initial area. (b) Reference image. (c) Normalized SHG image obtained by scanning the area after the recording. (d) Reference image (CNRS logo). (e) SHG image of the CNRS logo. (f) Zoom of an area in the SHG image.

Equations (1)

Equations on this page are rendered with MathJax. Learn more.

u⃗=A1A2A1A2;v⃗=A1A3u⃗(A1A3·u⃗)A1A3u⃗(A1A3·u⃗).

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