Abstract

Directly written by a ultra-short femto-second laser pulse, we report the phase separation and pattern formation induced by polymerization in a liquid-crystal-monomer mixture. By varying the scanning speed of optical fields along a line, pattern transitions of photon-induced polymer structures are illustrated in shapes of double-humped, single-humped, and broken stripes. The experimental data collected by optical microscopic images are in a good agreement with numerical simulations based on a modified set of coupled 2 + 1 dimensional diffusion equations. The demonstration in this work provides a step for controlling phase separation morphologies as well as transferring patterns in polymer-dispersed liquid crystals.

© 2011 OSA

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2010 (3)

2009 (5)

P. Rathi and T. Kyu, “Theory and computation of photopolymerization-induced phase transition and morphology development in blends of crystalline polymer and photoreactive monomer,” Phys. Rev. E79, 031802 (2009).
[CrossRef]

C.-C. Jeng, Y. Y. Lin, R.-C. Hong, and R.-K. Lee, “Optical pattern transitions from modulation to transverse instabilities in photorefractive crystals,” Phys. Rev. Lett.102, 253905 (2009).
[CrossRef]

H. Tanaka, “Formation of network and cellular structures by viscoelastic phase separation,” Adv. Mater.21, 1872–1880 (2009).
[CrossRef]

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

Y. Y. Lin, R.-K. Lee, and Yu. S. Kivshar, “Transverse instability of TM solitons and nonlinear surface plasmons,” Opt. Lett.34, 2982–2984 (2009).
[CrossRef] [PubMed]

2008 (4)

C. H. Lee, H. Yoshida, Y. Miura, A. Fujii, and M. Ozaki, “Local liquid crystal alignment on patterned micro-grating structures photofabricated by two photon excitation direct laser writing,” Appl. Phys. Lett.93, 173509 (2008).
[CrossRef]

Y. Y. Lin, R.-K. Lee, and Yu. S. Kivshar, “Soliton transverse instabilities in nonlocal nonlinear media,” J. Opt. Soc. Am. B25, 576–581 (2008).
[CrossRef]

S. Moynihan, P. Lovera, D. O’Carroll, D. Iacopino, and G. Redmond, “Alignment and dynamic manipulation of conjugated polymer nanowires in nematic crystal hosts,” Adv. Mater.20, 2497–2502 (2008).
[CrossRef]

H. Ren, S. T. Wu, and Y. H. Lin, “In situ observation of fringing-field-induced phase separation in a liquid-crystal-monomer mixture,” Phys. Rev. Lett.100, 117801 (2008).
[CrossRef] [PubMed]

2007 (1)

2006 (1)

N. Gheorghiu, J. L. West, A. V. Glushchenko, and M. Mitrokhin, “Patterned field induced polymer walls for smectic A bistable flexible displays,” App. Phys. Lett.88, 263511 (2006).
[CrossRef]

2005 (1)

S. Matsuo, S. Juodkazis, and H. Misawa, “Femtosecond laser microfabrication of periodic structures using a microlens array,” Phys. Rev. A80, 683–685 (2005).

2002 (1)

H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nat. Mater.1, 64–68 (2002).
[CrossRef]

2000 (3)

R. Sigel, G. Fytas, N. Vainos, S. Pispas, and N. Hadjichristidis, “Pattern formation in homogeneous polymer solutions induced by a continuous-wave visible laser,” Science297, 67–69 (2000).
[CrossRef]

Yu. S. Kivshar and D. E. Pelinovsky, “Self-focusing and transverse instabilities of solitary waves,” Phys. Rep.331, 117–195 (2000).
[CrossRef]

C. C. Bowley and G. P. Crawford, “Diffusion kinetics of formation of holographic polymer-dispersed liquid crystal display materials,” Appl. Phys. Lett.76, 2235–2237 (2000).
[CrossRef]

1996 (1)

1993 (1)

J. Y. Kim, C. H. Cho, P. Palffy-Muhoray, M. Mustafa, and T. Kyu, “Polymerization-induced phase separation in a liquid-crystal-polymer mixture,” Phys. Rev. Lett.71, 2232–2235 (1993).
[CrossRef] [PubMed]

1833 (1)

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Baek, J. W.

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Bowley, C. C.

C. C. Bowley and G. P. Crawford, “Diffusion kinetics of formation of holographic polymer-dispersed liquid crystal display materials,” Appl. Phys. Lett.76, 2235–2237 (2000).
[CrossRef]

Bruendel, M.

Buyuktanir, E. A.

E. A. Buyuktanir, M. W. Frey, and J. L. West, “Self-assembled, optically responsive nematic liquid crystal/polymer core-shell fibers: Formation and characterization,” Polymer51, 4823–4830 (2010).
[CrossRef]

Challa, S. R.

Chen, J.

Chien, L.-C.

Cho, C. H.

J. Y. Kim, C. H. Cho, P. Palffy-Muhoray, M. Mustafa, and T. Kyu, “Polymerization-induced phase separation in a liquid-crystal-polymer mixture,” Phys. Rev. Lett.71, 2232–2235 (1993).
[CrossRef] [PubMed]

Crawford, G. P.

C. C. Bowley and G. P. Crawford, “Diffusion kinetics of formation of holographic polymer-dispersed liquid crystal display materials,” Appl. Phys. Lett.76, 2235–2237 (2000).
[CrossRef]

Frey, M. W.

E. A. Buyuktanir, M. W. Frey, and J. L. West, “Self-assembled, optically responsive nematic liquid crystal/polymer core-shell fibers: Formation and characterization,” Polymer51, 4823–4830 (2010).
[CrossRef]

Fujii, A.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

C. H. Lee, H. Yoshida, Y. Miura, A. Fujii, and M. Ozaki, “Local liquid crystal alignment on patterned micro-grating structures photofabricated by two photon excitation direct laser writing,” Appl. Phys. Lett.93, 173509 (2008).
[CrossRef]

Fytas, G.

R. Sigel, G. Fytas, N. Vainos, S. Pispas, and N. Hadjichristidis, “Pattern formation in homogeneous polymer solutions induced by a continuous-wave visible laser,” Science297, 67–69 (2000).
[CrossRef]

Gennes, P. G. D.

P. G. D. Gennes and J. Prost, The Physics of Liquid Crystals (Oxford University Press, 1995).

Gheorghiu, N.

N. Gheorghiu, J. L. West, A. V. Glushchenko, and M. Mitrokhin, “Patterned field induced polymer walls for smectic A bistable flexible displays,” App. Phys. Lett.88, 263511 (2006).
[CrossRef]

Glushchenko, A. V.

N. Gheorghiu, J. L. West, A. V. Glushchenko, and M. Mitrokhin, “Patterned field induced polymer walls for smectic A bistable flexible displays,” App. Phys. Lett.88, 263511 (2006).
[CrossRef]

Hadjichristidis, N.

R. Sigel, G. Fytas, N. Vainos, S. Pispas, and N. Hadjichristidis, “Pattern formation in homogeneous polymer solutions induced by a continuous-wave visible laser,” Science297, 67–69 (2000).
[CrossRef]

Henzi, P.

Hisakado, Y.

H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nat. Mater.1, 64–68 (2002).
[CrossRef]

Hong, R.-C.

C.-C. Jeng, Y. Y. Lin, R.-C. Hong, and R.-K. Lee, “Optical pattern transitions from modulation to transverse instabilities in photorefractive crystals,” Phys. Rev. Lett.102, 253905 (2009).
[CrossRef]

Huang, Y.

Iacopino, D.

S. Moynihan, P. Lovera, D. O’Carroll, D. Iacopino, and G. Redmond, “Alignment and dynamic manipulation of conjugated polymer nanowires in nematic crystal hosts,” Adv. Mater.20, 2497–2502 (2008).
[CrossRef]

Ichihashi, Y.

Ihm, D. W.

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Jeng, C.-C.

C.-C. Jeng, Y. Y. Lin, R.-C. Hong, and R.-K. Lee, “Optical pattern transitions from modulation to transverse instabilities in photorefractive crystals,” Phys. Rev. Lett.102, 253905 (2009).
[CrossRef]

Juodkazis, S.

S. Matsuo, S. Juodkazis, and H. Misawa, “Femtosecond laser microfabrication of periodic structures using a microlens array,” Phys. Rev. A80, 683–685 (2005).

Kajiyama, T.

H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nat. Mater.1, 64–68 (2002).
[CrossRef]

Kikuchi, H.

H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nat. Mater.1, 64–68 (2002).
[CrossRef]

Kim, J. Y.

J. Y. Kim, C. H. Cho, P. Palffy-Muhoray, M. Mustafa, and T. Kyu, “Polymerization-induced phase separation in a liquid-crystal-polymer mixture,” Phys. Rev. Lett.71, 2232–2235 (1993).
[CrossRef] [PubMed]

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Kim, T. W.

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Kivshar, Yu. S.

Koenig, J. L.

Kyu, T.

P. Rathi and T. Kyu, “Theory and computation of photopolymerization-induced phase transition and morphology development in blends of crystalline polymer and photoreactive monomer,” Phys. Rev. E79, 031802 (2009).
[CrossRef]

J. Y. Kim, C. H. Cho, P. Palffy-Muhoray, M. Mustafa, and T. Kyu, “Polymerization-induced phase separation in a liquid-crystal-polymer mixture,” Phys. Rev. Lett.71, 2232–2235 (1993).
[CrossRef] [PubMed]

Lee, C. H.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

C. H. Lee, H. Yoshida, Y. Miura, A. Fujii, and M. Ozaki, “Local liquid crystal alignment on patterned micro-grating structures photofabricated by two photon excitation direct laser writing,” Appl. Phys. Lett.93, 173509 (2008).
[CrossRef]

Lee, R.-K.

Lin, Y. H.

H. Ren, S. T. Wu, and Y. H. Lin, “In situ observation of fringing-field-induced phase separation in a liquid-crystal-monomer mixture,” Phys. Rev. Lett.100, 117801 (2008).
[CrossRef] [PubMed]

Lin, Y. Y.

Lovera, P.

S. Moynihan, P. Lovera, D. O’Carroll, D. Iacopino, and G. Redmond, “Alignment and dynamic manipulation of conjugated polymer nanowires in nematic crystal hosts,” Adv. Mater.20, 2497–2502 (2008).
[CrossRef]

Lu, S.-Y.

Matsuo, S.

S. Matsuo, S. Juodkazis, and H. Misawa, “Femtosecond laser microfabrication of periodic structures using a microlens array,” Phys. Rev. A80, 683–685 (2005).

Misawa, H.

S. Matsuo, S. Juodkazis, and H. Misawa, “Femtosecond laser microfabrication of periodic structures using a microlens array,” Phys. Rev. A80, 683–685 (2005).

Mitrokhin, M.

N. Gheorghiu, J. L. West, A. V. Glushchenko, and M. Mitrokhin, “Patterned field induced polymer walls for smectic A bistable flexible displays,” App. Phys. Lett.88, 263511 (2006).
[CrossRef]

Miura, Y.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

C. H. Lee, H. Yoshida, Y. Miura, A. Fujii, and M. Ozaki, “Local liquid crystal alignment on patterned micro-grating structures photofabricated by two photon excitation direct laser writing,” Appl. Phys. Lett.93, 173509 (2008).
[CrossRef]

Miyake, Y.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

Mohr, J.

Moynihan, S.

S. Moynihan, P. Lovera, D. O’Carroll, D. Iacopino, and G. Redmond, “Alignment and dynamic manipulation of conjugated polymer nanowires in nematic crystal hosts,” Adv. Mater.20, 2497–2502 (2008).
[CrossRef]

Mustafa, M.

J. Y. Kim, C. H. Cho, P. Palffy-Muhoray, M. Mustafa, and T. Kyu, “Polymerization-induced phase separation in a liquid-crystal-polymer mixture,” Phys. Rev. Lett.71, 2232–2235 (1993).
[CrossRef] [PubMed]

Ni, Z.

O’Carroll, D.

S. Moynihan, P. Lovera, D. O’Carroll, D. Iacopino, and G. Redmond, “Alignment and dynamic manipulation of conjugated polymer nanowires in nematic crystal hosts,” Adv. Mater.20, 2497–2502 (2008).
[CrossRef]

Ozaki, M.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

C. H. Lee, H. Yoshida, Y. Miura, A. Fujii, and M. Ozaki, “Local liquid crystal alignment on patterned micro-grating structures photofabricated by two photon excitation direct laser writing,” Appl. Phys. Lett.93, 173509 (2008).
[CrossRef]

Palffy-Muhoray, P.

J. Y. Kim, C. H. Cho, P. Palffy-Muhoray, M. Mustafa, and T. Kyu, “Polymerization-induced phase separation in a liquid-crystal-polymer mixture,” Phys. Rev. Lett.71, 2232–2235 (1993).
[CrossRef] [PubMed]

Park, S. C.

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Pelinovsky, D. E.

Yu. S. Kivshar and D. E. Pelinovsky, “Self-focusing and transverse instabilities of solitary waves,” Phys. Rep.331, 117–195 (2000).
[CrossRef]

Pispas, S.

R. Sigel, G. Fytas, N. Vainos, S. Pispas, and N. Hadjichristidis, “Pattern formation in homogeneous polymer solutions induced by a continuous-wave visible laser,” Science297, 67–69 (2000).
[CrossRef]

Prost, J.

P. G. D. Gennes and J. Prost, The Physics of Liquid Crystals (Oxford University Press, 1995).

Rabus, D. G.

Rathi, P.

P. Rathi and T. Kyu, “Theory and computation of photopolymerization-induced phase transition and morphology development in blends of crystalline polymer and photoreactive monomer,” Phys. Rev. E79, 031802 (2009).
[CrossRef]

Redmond, G.

S. Moynihan, P. Lovera, D. O’Carroll, D. Iacopino, and G. Redmond, “Alignment and dynamic manipulation of conjugated polymer nanowires in nematic crystal hosts,” Adv. Mater.20, 2497–2502 (2008).
[CrossRef]

Ren, H.

H. Ren, S. T. Wu, and Y. H. Lin, “In situ observation of fringing-field-induced phase separation in a liquid-crystal-monomer mixture,” Phys. Rev. Lett.100, 117801 (2008).
[CrossRef] [PubMed]

Satoshi, F.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

Shimizu, Y.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

Sigel, R.

R. Sigel, G. Fytas, N. Vainos, S. Pispas, and N. Hadjichristidis, “Pattern formation in homogeneous polymer solutions induced by a continuous-wave visible laser,” Science297, 67–69 (2000).
[CrossRef]

Song, E. A.

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Tanaka, H.

H. Tanaka, “Formation of network and cellular structures by viscoelastic phase separation,” Adv. Mater.21, 1872–1880 (2009).
[CrossRef]

Tokuoka, K.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

Vainos, N.

R. Sigel, G. Fytas, N. Vainos, S. Pispas, and N. Hadjichristidis, “Pattern formation in homogeneous polymer solutions induced by a continuous-wave visible laser,” Science297, 67–69 (2000).
[CrossRef]

Wang, Q.

Wang, S-Q.

West, J. L.

E. A. Buyuktanir, M. W. Frey, and J. L. West, “Self-assembled, optically responsive nematic liquid crystal/polymer core-shell fibers: Formation and characterization,” Polymer51, 4823–4830 (2010).
[CrossRef]

N. Gheorghiu, J. L. West, A. V. Glushchenko, and M. Mitrokhin, “Patterned field induced polymer walls for smectic A bistable flexible displays,” App. Phys. Lett.88, 263511 (2006).
[CrossRef]

Woo, H. Y.

J. Y. Kim, H. Y. Woo, J. W. Baek, T. W. Kim, E. A. Song, S. C. Park, and D. W. Ihm, “Polymer-dispersed liquid crystal devices using highly conducting polymers as electrodes,” Appl. Phys. Lett.92, 183301 (2008).

Wu, S. T.

H. Ren, S. T. Wu, and Y. H. Lin, “In situ observation of fringing-field-induced phase separation in a liquid-crystal-monomer mixture,” Phys. Rev. Lett.100, 117801 (2008).
[CrossRef] [PubMed]

D. K. Yang and S. T. Wu, Fundamental of Liquid Crystal Devices (Wiley, 2006).
[CrossRef]

Yang, D. K.

D. K. Yang and S. T. Wu, Fundamental of Liquid Crystal Devices (Wiley, 2006).
[CrossRef]

Yang, H.

H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nat. Mater.1, 64–68 (2002).
[CrossRef]

Yokota, M.

H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nat. Mater.1, 64–68 (2002).
[CrossRef]

Yoshida, H.

K. Tokuoka, H. Yoshida, Y. Miyake, C. H. Lee, Y. Miura, S. Yusuke, F. Satoshi, A. Fujii, Y. Shimizu, and M. Ozaki, “Planar alignment of columnar liquid crystals in microgroove structures,” Mol. Cryst. Liq. Cryst.510, 126–133 (2009).
[CrossRef]

C. H. Lee, H. Yoshida, Y. Miura, A. Fujii, and M. Ozaki, “Local liquid crystal alignment on patterned micro-grating structures photofabricated by two photon excitation direct laser writing,” Appl. Phys. Lett.93, 173509 (2008).
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Figures (3)

Fig. 1
Fig. 1

Illustration of our experimental setup, where a frequency-doubled Ti:sapphire laser is focused on the sample mixed with liquid crystals (LC) and monomer molecules. A half-wave plate (HWP) is used to rotate the polarization of writing pulses. The translational stage is used to control the scanning rate of our focused beam.

Fig. 2
Fig. 2

Optical microscopic images of our liquid-crystal-monomer mixture, taken after the laser writing at the scanning speeds of (a) 0.1 and (b) 3mm/sec, respectively. The corresponding scanning electron microscope (SEM) images, taken after washing out the liquid crystal molecules for the samples, are shown in (c) and (d), respectively. The close-up SEM images in higher resolutions are shown in (e) and (f), respectively.

Fig. 3
Fig. 3

Optical microscopic images of a pattern transition in photo-induced polymerization processes by a laser pulse writing at different scanning speeds of (a) 0.1, (b) 0.5, (c) 2, and (d) 3mm/sec, respectively. Dark regions represents the polymer structures, while bright region corresponds to the liquid crystal rich area. Simulation results based on a modified diffusion model for the concentration of polymer molecules are demonstrated in (e–h) for different scanning parameters: f = (e) 0.001, (f) 0.01, (g) 1, and (h) 5, respectively. The insets shown in (e–h) correspond to the transverse profile of polymer molecules along the x-axis, at a fixed position y = 0. Other parameters used in simulations are D0 = 1, K0 = 6, α = 0.7, and A0 = 1.

Equations (3)

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ϕ m t = [ D ( x , y , t ) ϕ m ( x , y , t ) ] F ( x , y , t ) ϕ m ( x , y , t ) ,
ϕ p t = F ( x , y , t ) ϕ m ( x , y , t ) ,
F ( x , y , t ) = K 0 exp [ α ϕ p ( x , y , t ) ] I ( x , y ) ,

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