N-(4-nitrophenyl)-N-methylamino-aceto-nitrile: a new organic material for efficient second-harmonic generation in bulk and waveguide configurations. I. Growth, crystal structure, and characterization of organic crystal-cored fibers
P. V. Vidaković, M. Coquillay, and F. Salin, "N-(4-nitrophenyl)-N-methylamino-aceto-nitrile: a new organic material for efficient second-harmonic generation in bulk and waveguide configurations. I. Growth, crystal structure, and characterization of organic crystal-cored fibers," J. Opt. Soc. Am. B 4, 998-1012 (1987)
Second-harmonic generation (SHG) is theoretically investigated in weakly guiding organic crystal-cored fibers (OCCF’s), where the crystal axes are parallel to the corresponding waveguiding ones. The analysis made for all acentric point groups clearly singled out core orientations favorable for efficient SHG (under appropriate phase-matching conditions). The analysis of molecular orientations maximizing the relevant nonlinear (NL) coefficients shows that NL organic materials optimized for efficient SHG in the bulk are also optimized for efficient SHG in OCCF’s. We discuss the growth methods of OCCF’s and present the results obtained when two organic materials, N-(4-nitrophenyl)-(L)-prolinol (NPP) and N-(4-nitrophenyl)-N-methylamino-aceto-nitrile (NPAN), are used. The crystal structure of the new material NPAN as well as related NL properties are presented for the first time to the authors’ knowledge. The nonlinear properties of NPAN are comparable with those of the best phase-matchable organic material, NPP.
P. A. Norman, D. Bloor, J. S. Obhi, S. A. Karaulov, M. B. Hursthouse, P. V. Kolinsky, R. J. Jones, and S. R. Hall J. Opt. Soc. Am. B 4(6) 1013-1017 (1987)
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Molecules are assumed to be 2-D. NL coefficients marked by asterisks are zero for 1-D molecules.
Orientation of crystal axes with respect to waveguide axes.
Table 2
Maximum Values of Relevant Nonlinear Coefficients for Optimized Molecular Orientations in the Crystal Unit Cell for Both 1-D and 2-D Molecules
Orthorhombic
Monoclinic
Triclinic
mm2 p.g.
NL Coefficient
2 p.g.
NL Coefficient
m p.g.
NL Coefficient
1 p.g.
Dimensionality of β
NL Coefficient
0
d11
0
1-D
d11
βxxx
βxxx
2-D
0
d12
0
1-D
d12
βyyy
βxyy
2-D
(0°)
0
d12
0
d12
0
1-D
d12
βyxx
βxyy
βyxx
2-D
(0°)
(0°)
0.385βyyy
d31
βyyy
d22
0
d31
βyyy
1-D
d22
(54.74°; 90°)
(0°)
2-D
f(βijk)
βyyy
βyxx
βyyy
(αmax; ϕmax)
(0°)
(0°)
0.385βyyy
d32
0.385βyyy
d23
0.385
d32
(54.74°; 0°)
(54.74°)
(35.26°)
f(βijk)
0.385βyyy
0.385βyyy
(αmax; ϕmax)
(54.74°)
(35.26°)
βyyy
d33
βyyy
d33
(0°; ∀ ϕ)
(90°)
βyyy
βyyy
(0°; ∀ ϕ)
(90°)
Hexagonal
Tetragonal
m2 p.g.
NL Coefficient
6,6mm p.g.
NL Coefficient
p.g.
NL Coefficient
4mm p.g.
NL Coefficient
p.g.
NL Coefficient
4 P-g.
Dimensionality of β
NL Coefficient
0.25βyyy
d22
0.192βyyy
d31
0
d11
0.192βyyy
d31
0.192βyyy
d31
0.192βyyy
1-D
d31
(90°)
(54.74°)
(54.74°)
(54.74°)
(54.74°)
f(βyxx/βyyy)
f(βyxx/βyyy)
f(βxyy/βxxx)
f(βyxx/βyyy)
f(βyxx/βyyx)
f(βyxx/βyyy)
2-D
α(βyxx/βyyy)
α(βyxx/βyyy)
α(βxyy/βxxx)
βyxx/βyyy)
α(βyxx/βyyy)
α(βyxx/βyyy)
βyyy
d33
0.25βyyy
d22
βyyy
d33
βyyy
1-D
d33
(0°)
(90°)
(0°)
(0°)
βyyy
f(βyxx/βyyy)
βyyy
βyyy
2-D
(0°)
α(βyxx/βyyy)
(0°)
(0°)
Triogonal
32 p.g.
NL Coefficient
3m p.g.
NL Coefficient
3 p.g.
Dimensionality of β
NL Coefficient
025βyyy
d11
O25βyyy
d22
0
1-D
d11
(90°;30°)
(90°; 0°)
f(βijk)
f(βijk)
f(βxyy/βxxx)
1-D
(αmax; ϕmax)
(αmax; ϕmax)
(90°)
0.192βyyy
d31
0.25βyyy
1-D
d22
(54.74°)
(90°)
f(βyxx/βyyy)
f(βyxx/βyyy)
1-D
α(βyxx/βyyy)
(90°)
βyyy
d33
0.192βyyy
1-D
d31
(0°)
(54.74°)
βyyy
f(βyxx/βyyy)
1-D
(0°)
α(βyxx/βyyy)
βyyy
1-D
d33
(0°)
βyyy
1-D
(0°)
Table 3
Linear and Nonlinear Properties of Inorganic and Organic Materials Relevant for Their Use in Device Applications
Molecules are assumed to be 2-D. NL coefficients marked by asterisks are zero for 1-D molecules.
Orientation of crystal axes with respect to waveguide axes.
Table 2
Maximum Values of Relevant Nonlinear Coefficients for Optimized Molecular Orientations in the Crystal Unit Cell for Both 1-D and 2-D Molecules
Orthorhombic
Monoclinic
Triclinic
mm2 p.g.
NL Coefficient
2 p.g.
NL Coefficient
m p.g.
NL Coefficient
1 p.g.
Dimensionality of β
NL Coefficient
0
d11
0
1-D
d11
βxxx
βxxx
2-D
0
d12
0
1-D
d12
βyyy
βxyy
2-D
(0°)
0
d12
0
d12
0
1-D
d12
βyxx
βxyy
βyxx
2-D
(0°)
(0°)
0.385βyyy
d31
βyyy
d22
0
d31
βyyy
1-D
d22
(54.74°; 90°)
(0°)
2-D
f(βijk)
βyyy
βyxx
βyyy
(αmax; ϕmax)
(0°)
(0°)
0.385βyyy
d32
0.385βyyy
d23
0.385
d32
(54.74°; 0°)
(54.74°)
(35.26°)
f(βijk)
0.385βyyy
0.385βyyy
(αmax; ϕmax)
(54.74°)
(35.26°)
βyyy
d33
βyyy
d33
(0°; ∀ ϕ)
(90°)
βyyy
βyyy
(0°; ∀ ϕ)
(90°)
Hexagonal
Tetragonal
m2 p.g.
NL Coefficient
6,6mm p.g.
NL Coefficient
p.g.
NL Coefficient
4mm p.g.
NL Coefficient
p.g.
NL Coefficient
4 P-g.
Dimensionality of β
NL Coefficient
0.25βyyy
d22
0.192βyyy
d31
0
d11
0.192βyyy
d31
0.192βyyy
d31
0.192βyyy
1-D
d31
(90°)
(54.74°)
(54.74°)
(54.74°)
(54.74°)
f(βyxx/βyyy)
f(βyxx/βyyy)
f(βxyy/βxxx)
f(βyxx/βyyy)
f(βyxx/βyyx)
f(βyxx/βyyy)
2-D
α(βyxx/βyyy)
α(βyxx/βyyy)
α(βxyy/βxxx)
βyxx/βyyy)
α(βyxx/βyyy)
α(βyxx/βyyy)
βyyy
d33
0.25βyyy
d22
βyyy
d33
βyyy
1-D
d33
(0°)
(90°)
(0°)
(0°)
βyyy
f(βyxx/βyyy)
βyyy
βyyy
2-D
(0°)
α(βyxx/βyyy)
(0°)
(0°)
Triogonal
32 p.g.
NL Coefficient
3m p.g.
NL Coefficient
3 p.g.
Dimensionality of β
NL Coefficient
025βyyy
d11
O25βyyy
d22
0
1-D
d11
(90°;30°)
(90°; 0°)
f(βijk)
f(βijk)
f(βxyy/βxxx)
1-D
(αmax; ϕmax)
(αmax; ϕmax)
(90°)
0.192βyyy
d31
0.25βyyy
1-D
d22
(54.74°)
(90°)
f(βyxx/βyyy)
f(βyxx/βyyy)
1-D
α(βyxx/βyyy)
(90°)
βyyy
d33
0.192βyyy
1-D
d31
(0°)
(54.74°)
βyyy
f(βyxx/βyyy)
1-D
(0°)
α(βyxx/βyyy)
βyyy
1-D
d33
(0°)
βyyy
1-D
(0°)
Table 3
Linear and Nonlinear Properties of Inorganic and Organic Materials Relevant for Their Use in Device Applications