Abstract

The electro-optic and dielectric properties of organic–inorganic 2-amino-5-nitropyridium dihydrogen phosphate crystals were measured near room temperature at a wavelength of 632.8 nm and as a function of an electric-field frequency that varied from 1 kHz to 40 MHz. The frequency dispersion of the electro-optic coefficients and their comparison with the second-harmonic generation coefficients showed that the largest part of the electro-optic properties is electronic in origin (whereas the piezo-optic contribution is small). Results reveal a large anisotropy of the ionic and electronic contributions that is related to the contributions of the organic molecule to nonlinear polarizability.

© 2000 Optical Society of America

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  1. D. S. Chemla and J. Zyss, eds., Nonlinear Optical Properties of Organic Molecules and Crystals (Academic, Orlando, Fla., 1987).
  2. P. Günter, ed., Electrooptic and Photorefractive Materials (Springer-Verlag, Berlin, 1987).
  3. J. Pécaut and R. Masse, “Structure of bis(2-amino-5-nitropyridinium) dichromate as a step towards the design of efficient organic–inorganic non-linear optical crystals,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 277–282 (1993).
    [CrossRef]
  4. Z. Kotler, R. Hierle, D. Josse, J. Zyss, and R. Masse, “Quadratic nonlinear-optical properties of a new transparent and highly efficient organic-inorganic crystal: 2-amino-5-nitropyridium-dihydrogen phosphate (2A5NPDP),” J. Opt. Soc. Am. B 9, 534–547 (1992); S. Khodja, D. Josse, and J. Zyss, “Near-infrared optical parametric oscillation in an organomineral crystal,” J. Opt. Soc. Am. B 15, 751–758 (1998).
    [CrossRef]
  5. J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
    [CrossRef]
  6. M. Sigelles and R. Hierle, “Determination of the electrooptic coefficients of 3-methyl 4-nitropyridine 1-oxyde by an interferometric phase modulation technique,” J. Appl. Phys. 52, 4199–4204 (1981).
    [CrossRef]
  7. J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).
  8. A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
    [CrossRef]
  9. J. Zaccaro, M. Bagieu-Beucher, J. Espeso, and A. Ibanez, “Structural characterization and crystal growth of the 2 amino-5-nitropyridinium-dihydrogenophosphate/arsenate hybrid solid solution,” J. Cryst. Growth 186, 224–232 (1998); J. Zaccaro, B. Capelle, and A. Ibanez, “Crystal growth of hybrid nonlinear optical materials: 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate,” J. Cryst. Growth 180, 229–237 (1997).
    [CrossRef]
  10. R. Masse and J. Zyss, “A new approach in the design of polar crystals for quadratic nonlinear optics exemplified by the synthesis of 2-amino-5-nitropyridium-dihydrogen monophosphate (2A5NPDP),” Mol. Eng. 1, 141–152 (1991); J. Pecaut, Y. Lefur, and R. Masse, “Crystal engineering and structural investigations of the 2-amino-5-nitropyridinium salts C5H6N3O2+⋅HSO4 and C5H6N3O2+⋅H2AsO4−1,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 535–541 (1993).
    [CrossRef]
  11. R. Morita and P. V. Vidakovic, “Angle and temperature tuning of phase-matched second-harmonic generation in N-(4-nitrophenyl)-N-methylaminoacetonitrile,” Appl. Phys. Lett. 61, 2854–2856 (1992).
    [CrossRef]
  12. M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
    [CrossRef]
  13. J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
    [CrossRef]

1999 (1)

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

1998 (1)

J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
[CrossRef]

1997 (2)

J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).

A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
[CrossRef]

1993 (1)

J. Pécaut and R. Masse, “Structure of bis(2-amino-5-nitropyridinium) dichromate as a step towards the design of efficient organic–inorganic non-linear optical crystals,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 277–282 (1993).
[CrossRef]

1992 (1)

R. Morita and P. V. Vidakovic, “Angle and temperature tuning of phase-matched second-harmonic generation in N-(4-nitrophenyl)-N-methylaminoacetonitrile,” Appl. Phys. Lett. 61, 2854–2856 (1992).
[CrossRef]

1989 (1)

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

1981 (1)

M. Sigelles and R. Hierle, “Determination of the electrooptic coefficients of 3-methyl 4-nitropyridine 1-oxyde by an interferometric phase modulation technique,” J. Appl. Phys. 52, 4199–4204 (1981).
[CrossRef]

Abdi, F.

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

Aillerie, M.

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

Alexakis, G.

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

Boulanger, B.

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

Brehat, F.

J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).

Carabatos-Nedelec, C.

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

Feve, J. P.

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

Fontana, M. D.

J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
[CrossRef]

J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

Hierle, R.

M. Sigelles and R. Hierle, “Determination of the electrooptic coefficients of 3-methyl 4-nitropyridine 1-oxyde by an interferometric phase modulation technique,” J. Appl. Phys. 52, 4199–4204 (1981).
[CrossRef]

Ibanez, A.

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
[CrossRef]

A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
[CrossRef]

Levy, J. P.

A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
[CrossRef]

Marnier, G.

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

Masse, R.

J. Pécaut and R. Masse, “Structure of bis(2-amino-5-nitropyridinium) dichromate as a step towards the design of efficient organic–inorganic non-linear optical crystals,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 277–282 (1993).
[CrossRef]

Morita, R.

R. Morita and P. V. Vidakovic, “Angle and temperature tuning of phase-matched second-harmonic generation in N-(4-nitrophenyl)-N-methylaminoacetonitrile,” Appl. Phys. Lett. 61, 2854–2856 (1992).
[CrossRef]

Mouget, C.

A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
[CrossRef]

Pécaut, J.

J. Pécaut and R. Masse, “Structure of bis(2-amino-5-nitropyridinium) dichromate as a step towards the design of efficient organic–inorganic non-linear optical crystals,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 277–282 (1993).
[CrossRef]

Prieur, E.

A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
[CrossRef]

Rousseau, I.

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

Salvestrini, J. P.

J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
[CrossRef]

J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).

Sigelles, M.

M. Sigelles and R. Hierle, “Determination of the electrooptic coefficients of 3-methyl 4-nitropyridine 1-oxyde by an interferometric phase modulation technique,” J. Appl. Phys. 52, 4199–4204 (1981).
[CrossRef]

Theofanous, N.

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

Vidakovic, P. V.

R. Morita and P. V. Vidakovic, “Angle and temperature tuning of phase-matched second-harmonic generation in N-(4-nitrophenyl)-N-methylaminoacetonitrile,” Appl. Phys. Lett. 61, 2854–2856 (1992).
[CrossRef]

Wyncke, B.

J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).

Zaccaro, J.

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
[CrossRef]

Acta Crystallogr., Sect. B: Struct. Sci. (1)

J. Pécaut and R. Masse, “Structure of bis(2-amino-5-nitropyridinium) dichromate as a step towards the design of efficient organic–inorganic non-linear optical crystals,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 277–282 (1993).
[CrossRef]

Appl. Phys. B (1)

J. P. Salvestrini, J. Zaccaro, A. Ibanez, and M. D. Fontana, “Investigation of electrooptic modulation from organic-inorganic crystals,” Appl. Phys. B 67, 761–763 (1998).
[CrossRef]

Appl. Phys. Lett. (1)

R. Morita and P. V. Vidakovic, “Angle and temperature tuning of phase-matched second-harmonic generation in N-(4-nitrophenyl)-N-methylaminoacetonitrile,” Appl. Phys. Lett. 61, 2854–2856 (1992).
[CrossRef]

IEEE J. Quantum Electron. (1)

J. P. Feve, B. Boulanger, I. Rousseau, G. Marnier, J. Zaccaro, and A. Ibanez, “Second-harmonic generation properties of 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate organic–inorganic crystals,” IEEE J. Quantum Electron. 35, 66–71 (1999).
[CrossRef]

J. Appl. Phys. (2)

M. Sigelles and R. Hierle, “Determination of the electrooptic coefficients of 3-methyl 4-nitropyridine 1-oxyde by an interferometric phase modulation technique,” J. Appl. Phys. 52, 4199–4204 (1981).
[CrossRef]

M. Aillerie, M. D. Fontana, F. Abdi, C. Carabatos-Nedelec, N. Theofanous, and G. Alexakis, “Influence of the temperature-dependent spontaneous birefringence in the electro-optic measurements of LiNbO3,” J. Appl. Phys. 65, 2406–2408 (1989).
[CrossRef]

J. Solid State Chem. (1)

A. Ibanez, J. P. Levy, C. Mouget, and E. Prieur, “Crystal growth of a promising nonlinear optical material: 2-amino-5-nitropyridinium-chloride,” J. Solid State Chem. 129, 22–29 (1997).
[CrossRef]

Nonlinear Opt. (1)

J. P. Salvestrini, M. D. Fontana, B. Wyncke, and F. Brehat, “Comparative measurements of the frequency dependence of electrooptical and dielectric coefficients in inorganic crystals,” Nonlinear Opt. 17, 271–280 (1997).

Other (5)

J. Zaccaro, M. Bagieu-Beucher, J. Espeso, and A. Ibanez, “Structural characterization and crystal growth of the 2 amino-5-nitropyridinium-dihydrogenophosphate/arsenate hybrid solid solution,” J. Cryst. Growth 186, 224–232 (1998); J. Zaccaro, B. Capelle, and A. Ibanez, “Crystal growth of hybrid nonlinear optical materials: 2-amino-5-nitropyridinium-dihydrogenoarsenate and dihydrogenophosphate,” J. Cryst. Growth 180, 229–237 (1997).
[CrossRef]

R. Masse and J. Zyss, “A new approach in the design of polar crystals for quadratic nonlinear optics exemplified by the synthesis of 2-amino-5-nitropyridium-dihydrogen monophosphate (2A5NPDP),” Mol. Eng. 1, 141–152 (1991); J. Pecaut, Y. Lefur, and R. Masse, “Crystal engineering and structural investigations of the 2-amino-5-nitropyridinium salts C5H6N3O2+⋅HSO4 and C5H6N3O2+⋅H2AsO4−1,” Acta Crystallogr., Sect. B: Struct. Sci. 49, 535–541 (1993).
[CrossRef]

Z. Kotler, R. Hierle, D. Josse, J. Zyss, and R. Masse, “Quadratic nonlinear-optical properties of a new transparent and highly efficient organic-inorganic crystal: 2-amino-5-nitropyridium-dihydrogen phosphate (2A5NPDP),” J. Opt. Soc. Am. B 9, 534–547 (1992); S. Khodja, D. Josse, and J. Zyss, “Near-infrared optical parametric oscillation in an organomineral crystal,” J. Opt. Soc. Am. B 15, 751–758 (1998).
[CrossRef]

D. S. Chemla and J. Zyss, eds., Nonlinear Optical Properties of Organic Molecules and Crystals (Academic, Orlando, Fla., 1987).

P. Günter, ed., Electrooptic and Photorefractive Materials (Springer-Verlag, Berlin, 1987).

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Figures (4)

Fig. 1
Fig. 1

Chemical structure of the organic–inorganic 2A5NPDP crystal. The arrows indicate the mineral plane (H2PO4-).

Fig. 2
Fig. 2

Frequency dispersion of dielectric permittivities 11, 22, and 33 of 2A5NPDP.

Fig. 3
Fig. 3

Frequency dispersion of electro-optic coefficient ra of 2A5NPDP.

Fig. 4
Fig. 4

Time response of electro-optic coefficient ra in 2A5NPDP.

Tables (2)

Tables Icon

Table 1 Refractive Indices nij at λ=632.8 nm.a Dielectric Permittivities ij and Electro-Optic Coefficients rijk of 2A5NPDP at a Frequency of 1 kHzb

Tables Icon

Table 2 Measured Values of rijkTrijkS Calculated Values of rijke [from Eq. (2)], and Measured Values of dijk for 2A5NPDPa

Equations (17)

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

rijke(Ω; Ω; 0)=-2χijk(2)(Ω; Ω; 0)ni2(Ω)nj2(Ω).
rijke(Ω; Ω; 0)=-4dijk(2ω;ω;ω)ni2(Ω)nj2(Ω)WijkFijk,
Wijk=[ω02-(2ω)2]i(ω02-ω2)j(ω02-ω2)k(ω02-Ω2)i(ω02-Ω2)jω0k2,
Fijk=fΩ,ifΩ,jf0,kf2ω,ifω,jfω,k.
rijkT=rijks+pijmnDmnk,
rijkT=rijkpo+rijki+rijke,
Δn23(E)=-n23raE32,
Δn13(E)=-n13rbE32,Δn12(E)=-n13rcE32,
ra=r23-(n33/n23)r33,rb=r13-(n33/n13)r33,
rc=r13-(n23/n13)r23.
Δn13(E)=-n233r42E22,n23=2n22n32n22+n321/2.
Δn23(E)=-n133r51E12,n13=2n12n32n12+n321/2.
Γ(E)=2πLλΔn(E),
r=λdmπLn3V,
Δδ=2Δ(nijL)=2L(-(½)nij3rijk+[nij-1]Dijk)Ek,
Cm=λ2Vπ/2,
rijk=-enij3LVCmΔV+2 (nij-1)nij3Dijk.

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