Abstract

A new type of organic molecule, calix[4]arene, is applied in a second-harmonic-generating waveguide device for the first time. Linear optical properties of the calix[4]arene waveguiding film have been measured with the prism-coupling method. The molecules in the film are oriented by a corona-poling technique. With a Maker-fringe experiment, the induced d33 and d31 at λ = 1064 nm are determined at 8.6 and 2.0 pm/V, respectively. The calix[4]arene thin film has been applied to a Čerenkov-type device that generates second-harmonic light radiating into the glass substrate. The highest efficiency obtained is 0.23% for a fundamental wavelength of 820 nm by the use of fundamental power densities of 100 MW/cm2 in the waveguide and a device length of 6 mm. A coupled-mode theory has been developed that can properly explain the experimentally observed second-harmonic-generating efficiency and the angle of radiation into the substrate. Two methods for the enhancement of device efficiency are proposed, both based on theoretical calculations with the coupled-mode theory. An enhancement of 2 orders of magnitude is feasible.

© 1995 Optical Society of America

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1993

K. Clays, N. J. Armstrong, and T. L. Penner, "Blue and green Čerenkov-type second-harmonic generation in a polymeric Langmuir–Blodgett waveguide," J. Opt. Soc. Am. B 10, 886–893 (1993).
[CrossRef]

G. J. T. Heesink, A. G. T. Ruiter, N. F. van Hulst, and B. Bölger, "Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering," Phys. Rev. Lett. 71, 999–1002 (1993).
[CrossRef] [PubMed]

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

1992

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

1991

G. L. J. A. Rikken, C. J. E. Seppen, S. Nijhuis, and E. W. Meijer, "Poled polymers for frequency doubling of diode lasers," Appl. Phys. Lett. 58, 435–437 (1991).
[CrossRef]

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

H. Tamada, "Coupled-mode analysis of second harmonic generation in the form of Cerenkov radiation from a planar optical waveguide," IEEE J. Quantum Electron. 27, 502–508 (1991).
[CrossRef]

1990

1989

J. R. Li and H. J. Wintle, "Unipolar corona space charge in wire-plane geometry: a first principles numerical computation," J. Appl. Phys. 65, 4617–4624 (1989).
[CrossRef]

1985

J. Zyss, "Nonlinear organic materials for integrated optics: a review," J. Mol. Electron. 1, 25–45 (1985).

1984

D. J. Williams, "Organische polymere und nichtpolymere Materialien mit guten nichtlinearen optische eigenschaften," Angew. Chem. 96, 637–651 (1984).
[CrossRef]

1974

B. Chen, C. L. Tang, and J. M. Telle, "CW harmonic generation in the uv using a thin-film waveguide on a nonlinear substrate," Appl. Phys. Lett. 25, 495–498 (1974).
[CrossRef]

1970

P. K. Tien, R. Ulrich, and R. J. Martin, "Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide," Appl. Phys. Lett. 17, 447–450 (1970).
[CrossRef]

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

R. Ulrich, "Theory of the prism-film coupler by plane-wave analysis," J. Opt. Soc. Am. 60, 1337–1350 (1970).
[CrossRef]

1969

P. K. Tien, R. Ulrich, and R. J. Martin, "Modes of propagating light waves in thin deposited semiconductor films," Appl. Phys. Lett. 14, 291–294 (1969).
[CrossRef]

Aizawa, R.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Armstrong, N. J.

Beck, B.

Bjorklund, G. C.

Bölger, B.

G. J. T. Heesink, A. G. T. Ruiter, N. F. van Hulst, and B. Bölger, "Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering," Phys. Rev. Lett. 71, 999–1002 (1993).
[CrossRef] [PubMed]

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

O. F. J. Noordman, N. F. van Hulst, and B. Bölger, "Cerenkov second-harmonic radiation from organic calix[4]arenes thin films," in Conference on Lasers and Electro-Optics Europe (Optical Society of America, Washington, D.C., 1994), paper CWL6, pp. 274–275.
[CrossRef]

Burland, D. M.

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

Chen, B.

B. Chen, C. L. Tang, and J. M. Telle, "CW harmonic generation in the uv using a thin-film waveguide on a nonlinear substrate," Appl. Phys. Lett. 25, 495–498 (1974).
[CrossRef]

Clays, K.

K. Clays, N. J. Armstrong, and T. L. Penner, "Blue and green Čerenkov-type second-harmonic generation in a polymeric Langmuir–Blodgett waveguide," J. Opt. Soc. Am. B 10, 886–893 (1993).
[CrossRef]

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

Derhaeg, L.

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Engbersen, J. F.

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Hashizume, N.

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

Hayden, L. M.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Heesink, G. J. T.

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

G. J. T. Heesink, A. G. T. Ruiter, N. F. van Hulst, and B. Bölger, "Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering," Phys. Rev. Lett. 71, 999–1002 (1993).
[CrossRef] [PubMed]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Henry, R. A.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Hoover, J. M.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Hulst, N. F. van

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

G. J. T. Heesink, A. G. T. Ruiter, N. F. van Hulst, and B. Bölger, "Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering," Phys. Rev. Lett. 71, 999–1002 (1993).
[CrossRef] [PubMed]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

O. F. J. Noordman, N. F. van Hulst, and B. Bölger, "Cerenkov second-harmonic radiation from organic calix[4]arenes thin films," in Conference on Lasers and Electro-Optics Europe (Optical Society of America, Washington, D.C., 1994), paper CWL6, pp. 274–275.
[CrossRef]

Ito, R.

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

Jerphagnon, J.

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

Jurich, M. C.

Kelderman, E.

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Kinoshita, T.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Klaasse, P. T. A.

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

Koike, Y.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Kondo, T.

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

Kunioka, S.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Kurtz, S. K.

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

Li, J. R.

J. R. Li and H. J. Wintle, "Unipolar corona space charge in wire-plane geometry: a first principles numerical computation," J. Appl. Phys. 65, 4617–4624 (1989).
[CrossRef]

Lindsay, G. A.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Martin, R. J.

P. K. Tien, R. Ulrich, and R. J. Martin, "Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide," Appl. Phys. Lett. 17, 447–450 (1970).
[CrossRef]

P. K. Tien, R. Ulrich, and R. J. Martin, "Modes of propagating light waves in thin deposited semiconductor films," Appl. Phys. Lett. 14, 291–294 (1969).
[CrossRef]

Meijer, E. W.

G. L. J. A. Rikken, C. J. E. Seppen, S. Nijhuis, and E. W. Meijer, "Poled polymers for frequency doubling of diode lasers," Appl. Phys. Lett. 58, 435–437 (1991).
[CrossRef]

Miller, R. D.

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

Nijhuis, S.

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

G. L. J. A. Rikken, C. J. E. Seppen, S. Nijhuis, and E. W. Meijer, "Poled polymers for frequency doubling of diode lasers," Appl. Phys. Lett. 58, 435–437 (1991).
[CrossRef]

Nonaka, Y.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Noordman, O. F. J.

O. F. J. Noordman, N. F. van Hulst, and B. Bölger, "Cerenkov second-harmonic radiation from organic calix[4]arenes thin films," in Conference on Lasers and Electro-Optics Europe (Optical Society of America, Washington, D.C., 1994), paper CWL6, pp. 274–275.
[CrossRef]

Ogasawara, N.

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

Onda, T.

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

Ore, F. R.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Page, R. H.

Pasillas, P. L.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Penner, T. L.

Persoons, A.

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Picken, S. J.

Reinhoudt, D. N.

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Reiser, O.

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

Rikken, G. L. J. A.

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

G. L. J. A. Rikken, C. J. E. Seppen, S. Nijhuis, and E. W. Meijer, "Poled polymers for frequency doubling of diode lasers," Appl. Phys. Lett. 58, 435–437 (1991).
[CrossRef]

Ruiter, A. G. T.

G. J. T. Heesink, A. G. T. Ruiter, N. F. van Hulst, and B. Bölger, "Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering," Phys. Rev. Lett. 71, 999–1002 (1993).
[CrossRef] [PubMed]

Sasaki, K.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Sauter, G. F.

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

Sen, A.

Seppen, C. J. E.

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

G. L. J. A. Rikken, C. J. E. Seppen, S. Nijhuis, and E. W. Meijer, "Poled polymers for frequency doubling of diode lasers," Appl. Phys. Lett. 58, 435–437 (1991).
[CrossRef]

Staring, E. G. J.

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

Sugihara, O.

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

Swalen, J. D.

Tamada, H.

H. Tamada, "Coupled-mode analysis of second harmonic generation in the form of Cerenkov radiation from a planar optical waveguide," IEEE J. Quantum Electron. 27, 502–508 (1991).
[CrossRef]

Tang, C. L.

B. Chen, C. L. Tang, and J. M. Telle, "CW harmonic generation in the uv using a thin-film waveguide on a nonlinear substrate," Appl. Phys. Lett. 25, 495–498 (1974).
[CrossRef]

Telle, J. M.

B. Chen, C. L. Tang, and J. M. Telle, "CW harmonic generation in the uv using a thin-film waveguide on a nonlinear substrate," Appl. Phys. Lett. 25, 495–498 (1974).
[CrossRef]

Tien, P. K.

P. K. Tien, R. Ulrich, and R. J. Martin, "Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide," Appl. Phys. Lett. 17, 447–450 (1970).
[CrossRef]

P. K. Tien, R. Ulrich, and R. J. Martin, "Modes of propagating light waves in thin deposited semiconductor films," Appl. Phys. Lett. 14, 291–294 (1969).
[CrossRef]

Twieg, R. J.

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

R. H. Page, M. C. Jurich, B. Beck, A. Sen, R. J. Twieg, J. D. Swalen, G. C. Bjorklund, and C. G. Wilson, "Electrochromic and optical waveguide studies of corona-poled electro-optic polymer films," J. Opt. Soc. Am. B 7, 1239–1250 (1990).
[CrossRef]

Ulrich, R.

P. K. Tien, R. Ulrich, and R. J. Martin, "Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide," Appl. Phys. Lett. 17, 447–450 (1970).
[CrossRef]

R. Ulrich, "Theory of the prism-film coupler by plane-wave analysis," J. Opt. Soc. Am. 60, 1337–1350 (1970).
[CrossRef]

P. K. Tien, R. Ulrich, and R. J. Martin, "Modes of propagating light waves in thin deposited semiconductor films," Appl. Phys. Lett. 14, 291–294 (1969).
[CrossRef]

Umegaki, S.

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

Venhuizen, A. H. J.

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

Verbiest, T.

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

Verboom, W.

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

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

Walsh, C. A.

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

Williams, D. J.

D. J. Williams, "Organische polymere und nichtpolymere Materialien mit guten nichtlinearen optische eigenschaften," Angew. Chem. 96, 637–651 (1984).
[CrossRef]

Wilson, C. G.

Wintle, H. J.

J. R. Li and H. J. Wintle, "Unipolar corona space charge in wire-plane geometry: a first principles numerical computation," J. Appl. Phys. 65, 4617–4624 (1989).
[CrossRef]

Zyss, J.

J. Zyss, "Nonlinear organic materials for integrated optics: a review," J. Mol. Electron. 1, 25–45 (1985).

Adv. Mater.

E. Kelderman, G. J. T. Heesink, L. Derhaeg, T. Verbiest, P. T. A. Klaasse, W. Verboom, J. F. Engbersen, N. F. van Hulst, K. Clays, A. Persoons, and D. N. Reinhoudt, "Highly ordered films of neat calix[4]arenes for second order nonlinear optics," Adv. Mater. 5, 925–930 (1993).
[CrossRef]

Angew. Chem.

D. J. Williams, "Organische polymere und nichtpolymere Materialien mit guten nichtlinearen optische eigenschaften," Angew. Chem. 96, 637–651 (1984).
[CrossRef]

Angew. Chem. Int. Ed. Engl.

E. Kelderman, L. Derhaeg, G. J. T. Heesink, W. Verboom, J. F. Engbersen, N. F. van Hulst, A. Persoons, and D. N. Reinhoudt, "NitroCalix[4]arenes as molecules for second-order nonlinear optics," Angew. Chem. Int. Ed. Engl. 31, 1075–1077 (1992).
[CrossRef]

Appl. Phys. Lett.

B. Chen, C. L. Tang, and J. M. Telle, "CW harmonic generation in the uv using a thin-film waveguide on a nonlinear substrate," Appl. Phys. Lett. 25, 495–498 (1974).
[CrossRef]

P. K. Tien, R. Ulrich, and R. J. Martin, "Optical second harmonic generation in form of coherent Cerenkov radiation from a thin-film waveguide," Appl. Phys. Lett. 17, 447–450 (1970).
[CrossRef]

G. L. J. A. Rikken, C. J. E. Seppen, S. Nijhuis, and E. W. Meijer, "Poled polymers for frequency doubling of diode lasers," Appl. Phys. Lett. 58, 435–437 (1991).
[CrossRef]

P. K. Tien, R. Ulrich, and R. J. Martin, "Modes of propagating light waves in thin deposited semiconductor films," Appl. Phys. Lett. 14, 291–294 (1969).
[CrossRef]

G. J. T. Heesink, N. F. van Hulst, B. Bölger, E. Kelderman, J. F. Engbersen, W. Verboom, and D. N. Reinhoudt, "Novel calixarenes in thin films for efficient second harmonic generation," Appl. Phys. Lett. 62, 2015–2017 (1993).
[CrossRef]

IEEE J. Quantum Electron.

H. Tamada, "Coupled-mode analysis of second harmonic generation in the form of Cerenkov radiation from a planar optical waveguide," IEEE J. Quantum Electron. 27, 502–508 (1991).
[CrossRef]

N. Hashizume, T. Kondo, T. Onda, N. Ogasawara, S. Umegaki, and R. Ito, "Theoretical analysis of Cerenkov-type optical second-harmonic generation in slab waveguides," IEEE J. Quantum Electron. 28, 1798–1815 (1992).
[CrossRef]

J. Appl. Phys.

J. R. Li and H. J. Wintle, "Unipolar corona space charge in wire-plane geometry: a first principles numerical computation," J. Appl. Phys. 65, 4617–4624 (1989).
[CrossRef]

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

L. M. Hayden, G. F. Sauter, F. R. Ore, P. L. Pasillas, J. M. Hoover, G. A. Lindsay, and R. A. Henry, "Second-order nonlinear optical measurements in guest-host and side-chain polymers," J. Appl. Phys. 68, 456–465 (1990).
[CrossRef]

D. M. Burland, R. D. Miller, O. Reiser, R. J. Twieg, and C. A. Walsh, "The design, synthesis, and evaluation of chromophores for second harmonic generation in a polymer waveguide," J. Appl. Phys. 71, 410–417 (1992).
[CrossRef]

O. Sugihara, S. Kunioka, Y. Nonaka, R. Aizawa, Y. Koike, T. Kinoshita, and K. Sasaki, "Second harmonic generation by Cerenkov-type phase matching in a poled polymer waveguide," J. Appl. Phys. 70, 7249–7252 (1991).
[CrossRef]

J. Mol. Electron.

J. Zyss, "Nonlinear organic materials for integrated optics: a review," J. Mol. Electron. 1, 25–45 (1985).

J. Opt. Soc. Am.

J. Opt. Soc. Am. B

Philips J. Res.

G. L. J. A. Rikken, C. J. E. Seppen, A. H. J. Venhuizen, S. Nijhuis, and E. G. J. Staring, "Frequency doubling of diode lasers with poled polymers," Philips J. Res. 46, 215–230 (1992).

Phys. Rev. Lett.

G. J. T. Heesink, A. G. T. Ruiter, N. F. van Hulst, and B. Bölger, "Determination of hyperpolarizability tensor components by depolarized hyper Rayleigh scattering," Phys. Rev. Lett. 71, 999–1002 (1993).
[CrossRef] [PubMed]

Other

D. S. Chemla and J. Zyss, eds., Nonlinear Optical Properties of Organic Molecules and Crystals (Academic, Orlando, Fla., 1987), Vol. 1, Chap. II-7.

O. F. J. Noordman, N. F. van Hulst, and B. Bölger, "Cerenkov second-harmonic radiation from organic calix[4]arenes thin films," in Conference on Lasers and Electro-Optics Europe (Optical Society of America, Washington, D.C., 1994), paper CWL6, pp. 274–275.
[CrossRef]

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Figures (11)

Fig. 1
Fig. 1

Čerenkov SH-generating scheme with coordinate axes.

Fig. 2
Fig. 2

Field distributions in a Čerenkov device and their influence on the overlap integral.

Fig. 3
Fig. 3

Structure of the tetranitro-tetrapropoxycalix[4]arene.

Fig. 4
Fig. 4

Corona-poling setup.

Fig. 5
Fig. 5

Absorption spectra of 75 wt. % calix[4]arene/PPMA thin film before and after poling at 7 kV at 100 °C for 15 min.

Fig. 6
Fig. 6

Refractive indices of the corona-poled 75 wt. % calix[4]arene/PPMA thin film perpendicular and parallel to the film and the glass substrate.

Fig. 7
Fig. 7

Experimental and theoretical values for the Čerenkov angle and the overlap integral for a 675 ± 10 nm thick, 78 wt. % calix[4]arene/PPMA corona-poled film at λ = 1064 nm.

Fig. 8
Fig. 8

Experimental and theoretical values for the Čerenkov angle and the overlap integral for a 591 ± 10 nm thick, 75 wt. % calix[4]arene/PPMA corona-poled film at λ = 1064 nm.

Fig. 9
Fig. 9

Experimental and theoretical values for the Čerenkov angle and the overlap integral for a 599 ± 10 nm thick, 75 wt. % calix[4]arene/PPMA corona-poled film at λ = 1064 and 820 nm.

Fig. 10
Fig. 10

Influence of the distribution and the sign of the d33 value on the overlap integral.

Fig. 11
Fig. 11

Enhancement of the overlap integral by the bleaching of or the inversion of the sign of the d33 value.

Tables (5)

Tables Icon

Table 1 d33, d31, d33/d31 Ratio, and 〈cos3θ〉 Alignment Parameter Calculated from d33/d31 with the Isotropic Model and Calculated from the Molecular βzzz and d33 for Two Different Corona-Poled 75 wt. % Calix[4]arene/PPMA Thin Films

Tables Icon

Table 2 Sellmeier Coefficients for a Corona-Poled 75 wt. % Calix[4]arene/PPMA Thin Film and Glass Substrate

Tables Icon

Table 3 Experimental Values, Calculated Efficiencies, and Overlap Integrals [From Eq. (16)] for the Čerenkov Experiment on a 675 ± 10 nm thick, 78 wt. % Corona-Poled Calix[4]arene/PPMA Filma

Tables Icon

Table 4 Experimental Values, Calculated Efficiencies, and Overlap Integrals for the Čerenkov Experiment on a 591 ± 10 nm thick, 75 wt. % Corona-Poled Calix[4]arene/PPMA Filma

Tables Icon

Table 5 Experimental Values, Calculated Efficiencies, and Overlap Integrals for the Čerenkov Experiment on a 599 ± 10 nm thick, 75 wt. % Corona-Poled Calix[4]arene/PPMA Filma

Equations (21)

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

P = χ ( 1 ) · E + χ ( 2 ) : E 2 + χ ( 3 ) E 3 + , ,
P ( 2 ω ) = ½ χ ( 2 ) ( - 2 ω ; ω , ω ) : E ( ω ) E ( ω ) = 0 d · E ( ω ) 2 .
d 33 = ½ N β z z z f 2 ω f ω 2 cos 3 ( θ ) ,
d 31 = ½ N β z z z f 2 ω f ω 2 ½ cos ( θ ) sin 2 ( θ ) = ¼ N β z z z f 2 ω f ω 2 [ cos ( θ ) - cos 3 ( θ ) ] ,
f ω = n 2 ( ω ) + 2 3 ,
d 33 d 31 = 2 cos 3 ( θ ) cos ( θ ) - cos 3 ( θ ) ,
cos θ cer = n eff ω n substrate 2 ω ,
× ( × E ν ) = - μ 0 2 t 2 ( ¯ : E ν + P NLO , ν ) , ν = ω , 2 ω ,
E ν ( r , t ) = Re A ν ( x ) E y ν ( z ) exp [ i ( ν t - β ν x ) ] e y             ( TE mode ) , H ν ( r , t ) = Re A ν ( x ) H y ν ( z ) exp [ i ( ν t - β ν x ) ] e y             ( TM mode ) , ν = ω , 2 ω .
H x ω ( z ) = - i μ 0 ω E y ω ( z ) z , H z ω ( z ) = β ω μ 0 ω E y ω ( z )             ( TE mode ) ; E x ω ( z ) = i ω x H y ω ( z ) z , E z ω ( z ) = - β ω ω z H y ω ( z )             ( TM mode ) .
A 2 ω ( x ) x = | A 2 ω ( x ) x | NLO + | A 2 ω ( x ) x | rad ,
| A 2 ω ( x ) x | rad = - A 2 ω ( x ) l d ,
- h 0 2 π / 2 ω ( E × H ) x d t d z = l d 2 - h ( E y 2 ω ) 2 d z = l d μ 0 2 ω β 2 ω             ( TE mode ) , - h ( H y 2 ω ) z d z = l d 2 ω β 2 ω             ( TM mode ) .
| A 2 ω ( x ) x | NLO = A 2 ω , equi l d .
P 2 ω = - - [ A 2 ω ( y , x ) ] 2 d y d x ( A 2 ω , equi ) 2 b L ,
A 2 ω , equi l d E y 2 ω ( z ) = - i 2 μ 0 ω 2 β 2 ω P ind , y ( 2 ω )             ( TE mode ) , A 2 ω , equi l d H y 2 ω ( z ) = i ω P ind , z ( 2 ω ) + ω n z , 2 ω 2 β 2 ω z [ 1 n x , 2 ω 2 P ind , x ( 2 ω ) ]             ( TM mode ) ,
A 2 ω , equi = A ω 2 { i β ω - H y 2 ω ( z ) n z , 2 ω 2 d 32 ( z ) [ E y ω ( z ) ] 2 d z + i μ 0 ω - H y 2 ω ( z ) n x , 2 ω 2 d 12 ( z ) E y ω ( z ) H x ω ( z ) d z + 1 2 i = 1 n - 1 H y 2 ω ( z i ) Δ i , i + 1 ( d 12 1 n x , 2 ω 2 ) [ E y ω ( z i ) ] 2 } .
ω n z , 2 ω 2 β 2 ω z [ 1 n x , 2 ω 2 P ind , x ( 2 ω ) ]
A 2 ω , equi = A ω 2 [ i β ω - H y 2 ω ( z ) n z , 2 ω 2 { d 31 ( z ) [ E x ω ( z ) ] 2 + d 33 ( z ) [ E z ω ( z ) ] 2 + 2 d 35 ( z ) E x ω ( z ) E z ω ( z ) } d z + - H y 2 ω ( z ) n x , 2 ω 2 ( d 11 ( z ) E x ω ( z ) - i ω 0 n x , ω 2 k ω 2 ( z ) H y ω ( z ) + d 13 ( z ) E z ω ( z ) i β ω n x , ω 2 n z , ω 2 E x ω ( z ) + d 15 ( z ) { i β ω n x , ω 2 n z , ω 2 [ E x ω ( z ) ] 2 + - i ω 0 n x , ω 2 k ω 2 ( z ) H y ω ( z ) E z ω ( z ) } ) d z + 1 2 i = 1 n - 1 H y 2 ω ( z i ) Δ i , i + 1 ( 1 n x , 2 ω 2 { d 11 [ E x ω ( z i ) ] 2 + d 13 [ E z ω ( z i ) ] 2 + 2 d 15 E x ω ( z i ) E z ω ( z i ) } ) ] .
P 2 ω = P ω 2 L b ( - i = 1 n - 1 ) 2 .
n 2 ( λ ) = A 2 + B λ 2 λ 2 - λ 0 2 .

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