Abstract

Acentric films of 4-[trans-(pyridin-4-ylvinyl)] benzoic acid (PVBA) are grown on amorphous substrates by oblique incidence organic molecular beam deposition. The molecules in the bulk of the films show a preferential noncentrosymmetric in-plane orientation determined by the molecular beam direction. We investigate this symmetry-breaking mechanism by studying the structural and nonlinear optical properties of the films as a function of deposition conditions, with special focus on the molecular beam angle of incidence. The most pronounced preferential orientation of the molecules is found for an incident angle of 50±10 deg relative to the substrate normal.

© 2004 Optical Society of America

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  1. C. Bosshard, K. Sutter, P. Pre⁁tre, J. Hulliger, M. Flörsheimer, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon & Breach, Amsterdam, 1995).
  2. F. Kajzar and J. D. Swalen, Organic Thin Films for Waveguiding Nonlinear Optics (Gordon & Breach, Amsterdam, 1996).
  3. C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
    [CrossRef]
  4. C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
    [CrossRef]
  5. C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
    [CrossRef]
  6. C. Cai, M. Bösch, C. Bosshard, B. Müller, Y. Tao, A. Kündig, J. Weckesser, J. V. Barth, L. Bürgi, O. Jeandupeux, M. Kiy, I. Biaggio, I. Liakatas, K. Kern, and P. Günter, “Self-assembly growth of organic thin films and nanostructures by molecular beam deposition,” in Anisotropic Organic Materials, Approaches to Polar Order, R. Glazer and P. Kaszynski, eds. (American Chemical Society, Washington, D.C., 2002), Chap. 3, pp. 34–49.
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    [CrossRef]
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    [CrossRef]
  9. R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
    [CrossRef]
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    [CrossRef]
  11. J. Jerphagnon and S. Kurtz, “Maker fringes: a detailed comparison of theory and experiment for isotropic and uniaxial crystals,” J. Appl. Phys. 41, 1667–1681 (1970).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]

2000

D. L. Everitt, W. J. Miller, N. L. Abbott, and X. D. Zhu, “Evolution of a preferred orientation of polycrystalline grains in obliquely deposited gold films on an amorphous substrate,” Phys. Rev. B 62, R4833–R4836 (2000).
[CrossRef]

1999

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

1998

K. Robbie, J. C. Sit, and M. J. Brett, “Advanced techniques for glancing angle deposition,” J. Vac. Sci. Technol. B 16, 1115–1122 (1998).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

1997

L. Abelmann and C. Lodder, “Oblique evaporation and surface diffusion,” Thin Solid Films 305, 1–21 (1997).
[CrossRef]

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

1995

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

1990

1970

J. Jerphagnon and S. Kurtz, “Maker fringes: a detailed comparison of theory and experiment for isotropic and uniaxial crystals,” J. Appl. Phys. 41, 1667–1681 (1970).
[CrossRef]

Abbott, N. L.

D. L. Everitt, W. J. Miller, N. L. Abbott, and X. D. Zhu, “Evolution of a preferred orientation of polycrystalline grains in obliquely deposited gold films on an amorphous substrate,” Phys. Rev. B 62, R4833–R4836 (2000).
[CrossRef]

Abelmann, L.

L. Abelmann and C. Lodder, “Oblique evaporation and surface diffusion,” Thin Solid Films 305, 1–21 (1997).
[CrossRef]

Barth, J. V.

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

Biaggio, I.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

Bösch, M.

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Bosshard, C.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Brett, M. J.

K. Robbie, J. C. Sit, and M. J. Brett, “Advanced techniques for glancing angle deposition,” J. Vac. Sci. Technol. B 16, 1115–1122 (1998).
[CrossRef]

Cai, C.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Everitt, D. L.

D. L. Everitt, W. J. Miller, N. L. Abbott, and X. D. Zhu, “Evolution of a preferred orientation of polycrystalline grains in obliquely deposited gold films on an amorphous substrate,” Phys. Rev. B 62, R4833–R4836 (2000).
[CrossRef]

Frankel, C.

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

Gan, Z.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Gehrke, T.

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

Günter, P.

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Jäger, M.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Jerphagnon, J.

J. Jerphagnon and S. Kurtz, “Maker fringes: a detailed comparison of theory and experiment for isotropic and uniaxial crystals,” J. Appl. Phys. 41, 1667–1681 (1970).
[CrossRef]

Kim, Y. D.

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

Kündig, A.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Kurtz, S.

J. Jerphagnon and S. Kurtz, “Maker fringes: a detailed comparison of theory and experiment for isotropic and uniaxial crystals,” J. Appl. Phys. 41, 1667–1681 (1970).
[CrossRef]

Lakhtakia, A.

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

Lee, S.

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

Liakatas, I.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Lodder, C.

L. Abelmann and C. Lodder, “Oblique evaporation and surface diffusion,” Thin Solid Films 305, 1–21 (1997).
[CrossRef]

Messier, R.

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

Miller, W. J.

D. L. Everitt, W. J. Miller, N. L. Abbott, and X. D. Zhu, “Evolution of a preferred orientation of polycrystalline grains in obliquely deposited gold films on an amorphous substrate,” Phys. Rev. B 62, R4833–R4836 (2000).
[CrossRef]

Müller, B.

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

Otano, W.

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

Park, B.

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

Park, G.

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

Picken, S. J.

Robbie, K.

K. Robbie, J. C. Sit, and M. J. Brett, “Advanced techniques for glancing angle deposition,” J. Vac. Sci. Technol. B 16, 1115–1122 (1998).
[CrossRef]

Schwer, H.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

Sit, J. C.

K. Robbie, J. C. Sit, and M. J. Brett, “Advanced techniques for glancing angle deposition,” J. Vac. Sci. Technol. B 16, 1115–1122 (1998).
[CrossRef]

Tao, Y.

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

van der Vorst, C. P. J. M.

Venugopal, V. C.

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

Weckesser, J.

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

Zhu, X. D.

D. L. Everitt, W. J. Miller, N. L. Abbott, and X. D. Zhu, “Evolution of a preferred orientation of polycrystalline grains in obliquely deposited gold films on an amorphous substrate,” Phys. Rev. B 62, R4833–R4836 (2000).
[CrossRef]

Adv. Mater.

C. Cai, M. Bösch, B. Müller, Y. Tao, A. Kündig, C. Bosshard, Z. Gan, I. Biaggio, I. Liakatas, M. Jäger, H. Schwer, and P. Günter, “Oblique incidence organic molecular beam deposition and nonlinear optical properties of organic thin films with a stable in-plane directional order,” Adv. Mater. 11, 745–749 (1999).
[CrossRef]

C. Cai, B. Müller, J. Weckesser, J. V. Barth, Y. Tao, M. Bösch, A. Kündig, C. Bosshard, I. Biaggio, and P. Günter, “Model for in-plane directional ordering of organic thin films by oblique incidence organic molecular beam deposition,” Adv. Mater. 11, 750–754 (1999).
[CrossRef]

J. Am. Chem. Soc.

C. Cai, M. Bösch, Y. Tao, B. Müller, Z. Gan, A. Kündig, C. Bosshard, I. Liakatas, M. Jäger, and P. Günter, “Self-assembly in ultrahigh vacuum: growth of organic thin films with a stable in-plane directional order,” J. Am. Chem. Soc. 120, 8563–8564 (1998).
[CrossRef]

J. Appl. Phys.

J. Jerphagnon and S. Kurtz, “Maker fringes: a detailed comparison of theory and experiment for isotropic and uniaxial crystals,” J. Appl. Phys. 41, 1667–1681 (1970).
[CrossRef]

J. Opt. Soc. Am. B

J. Vac. Sci. Technol. A

R. Messier, T. Gehrke, C. Frankel, V. C. Venugopal, W. Otano, and A. Lakhtakia, “Engineered sculptured nematic thin films,” J. Vac. Sci. Technol. A 15, 2148–2152 (1997).
[CrossRef]

J. Vac. Sci. Technol. B

K. Robbie, J. C. Sit, and M. J. Brett, “Advanced techniques for glancing angle deposition,” J. Vac. Sci. Technol. B 16, 1115–1122 (1998).
[CrossRef]

Opt. Quantum Electron.

S. Lee, B. Park, S. Lee, G. Park, and Y. D. Kim, “Second-harmonic generation in poled films of nonlinear optical polymer composites,” Opt. Quantum Electron. 27, 411–420 (1995).
[CrossRef]

Phys. Rev. B

D. L. Everitt, W. J. Miller, N. L. Abbott, and X. D. Zhu, “Evolution of a preferred orientation of polycrystalline grains in obliquely deposited gold films on an amorphous substrate,” Phys. Rev. B 62, R4833–R4836 (2000).
[CrossRef]

Thin Solid Films

L. Abelmann and C. Lodder, “Oblique evaporation and surface diffusion,” Thin Solid Films 305, 1–21 (1997).
[CrossRef]

Other

C. Cai, M. Bösch, C. Bosshard, B. Müller, Y. Tao, A. Kündig, J. Weckesser, J. V. Barth, L. Bürgi, O. Jeandupeux, M. Kiy, I. Biaggio, I. Liakatas, K. Kern, and P. Günter, “Self-assembly growth of organic thin films and nanostructures by molecular beam deposition,” in Anisotropic Organic Materials, Approaches to Polar Order, R. Glazer and P. Kaszynski, eds. (American Chemical Society, Washington, D.C., 2002), Chap. 3, pp. 34–49.

C. Bosshard, K. Sutter, P. Pre⁁tre, J. Hulliger, M. Flörsheimer, P. Kaatz, and P. Günter, Organic Nonlinear Optical Materials (Gordon & Breach, Amsterdam, 1995).

F. Kajzar and J. D. Swalen, Organic Thin Films for Waveguiding Nonlinear Optics (Gordon & Breach, Amsterdam, 1996).

Y. R. Shen, Principles of Nonlinear Optics (Wiley, New York, 1984).

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Figures (5)

Fig. 1
Fig. 1

(a) Schematic of the oblique incident organic molecular beam deposition with the coordinate system used. γ is the angle of incidence of the molecular beam measured from the substrate normal. (b) Molecular structure of a head-to-tail arrangement of PVBA molecules.

Fig. 2
Fig. 2

Dependence of the nonlinear optical susceptibilities (a) d33 and (b) d31 of thin PVBA films on the angle of incidence of the molecular beam. This is an average of measurements performed on 15 different batches of ten films, each grown at slightly different deposition conditions. Quoted errors are statistical, one standard deviation.

Fig. 3
Fig. 3

Angle dependence of the nonlinear optical coefficient for three different film thicknesses (the thickness used to label the curves in the legend is the one corresponding to a molecular beam angle of incidence of 50 deg). The exact thicknesses of films grown at 90° are also indicated. For angle of incidences larger than 60° and actual film thicknesses larger than 40 nm the relationship between the square root of the SHG signal and the thickness is no longer linear. The inset shows the square root of the SHG intensity for films grown with a molecular beam angle of incidence of 30° as a function of the film thickness. The straight line is the linear least-squares fit to the experimental data.

Fig. 4
Fig. 4

(a) Second-harmonic intensity as a function of the angle of incidence of the fundamental laser beam for a 200-nm PVBA film grown with a molecular beam angle of incidence of 30°. The solid curve is a fit using Eq. (2) with d33 as the only nonzero nonlinear optical coefficient. The dashed curve would be the same function with d33=3d32. (b) Second-harmonic intensity as a function of sample rotation angle. The solid curve is a fit using Eq. (3) with d33=3d31. The dashed curve would be the same function with d33 as the only nonzero nonlinear optical coefficient.

Fig. 5
Fig. 5

Same measurements as for Fig. 4(a) but for films grown with three different molecular beam angle of incidences.

Equations (12)

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I2ω=2ω20c3(ni2ω)2d3i2L2(tA/Fω)4(tS/A2ω)2(Iω)2,
deff(α, β=0)=d33 cos3 α+3d32 cos α sin2 α,
deff(α=0, β)=d33 cos3 β+(d31+2d15)cos β sin2 β=(d33-3d31)cos3 β+3d31 cos β,
d33β333(θ, ψ)=cos2 θβzzz,
d31β311(θ, ψ)=sin2 θ cos θ cos2 ψβzzz,
f=0π sin θdθ02πdψf(θ, ψ)ρ(θ, ψ)0π sin θdθ02πdψρ(θ, ψ),
ρ(θ, ψ)expcos θ EkBT,
d33=E5kBTβzzz,
d31=E15kBTβzzz,
f=0πdθf(θ, ψ)ρ(θ, ψ)0πdθρ(θ, ψ),
d33=3E8kBTβzzz,
d31=E8kBTβzzz,

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