S. Follonier, Ch. Bosshard, U. Meier, G. Knöpfle, C. Serbutoviez, F. Pan, and P. Günter, "New nonlinear-optical organic crystal: 4-dimethyl-aminobenzaldehyde-4-nitrophenyl-hydrazone," J. Opt. Soc. Am. B 14, 593-601 (1997)
Single crystals of 4-dimethylaminobenzaldehyde-4-nitrophenylhydrazone were grown from solution. We determined their linear-optical (absorption and refractive indices) as well as their nonlinear-optical properties. From the highest nonlinear-optical coefficient pm/V at µm we determine an effective nonlinear-optical coefficient pm/V for phase-matched frequency doubling that is, to the best of our knowledge, the largest reported phase-matchable coefficient. The nonlinear-optical properties are discussed in terms of the crystal structure and the molecular hyperpolarizabilities. In addition, the phase-matching configurations for second-harmonic generation and optic parametric oscillation are derived.
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Selection of Measured Refractive Indices for Various Wavelengths above the Absorption Edgea
λ (nm)
n1
n2
n3
700
2.36
2.31
1.457
740
2.26
2.22
1.456
780
2.22
2.18
1.453
820
2.19
2.16
1.451
875.3
2.15
2.14
1.458
954*
2.12
2.10
1.448
1064
2.08
2.06
1.441
1313
2.03
2.02
1.443
1542*
2.01
2.00
1.455
1907*
2.00
2.00
1.445
Sellmeier Parameters
ωeg (1015
3.586
3.880
13.625
λeg (nm)
525.6
485.8
138.4
γ0ωp2 (1030)
16.06
22.42
161.84
A
1.652
1.376
0.215
Values indicated by asterisks were calculated from the coherence lengths of Maker-fringe measurements. The parameters used to fit the refractive indices with a one-oscillator Sellmeier model are also listed. The Sellmeier parameters obtained for n3 are only approximate because the dispersion of this refractive index is too small to yield precise values for these parameters.
Table 2
Theoretical (Oriented Gas Model) and Experimental Nonlinear-Optical Susceptibilities dij and Coherence Lengths lijc of DANPHa
(ij)
Theory
Experiment
dij (pm/V)
lijc (µm)
dij (pm/V)
lijc (µm)
λ = 1542 nm
11
185
1.75
200 ± 40
1.76 ± 0.2
33
0.1
51
0.3 ± 0.2
–
12
260
1.67
270 ± 50*
–
32
21
0.7
35 ± 10*
–
λ = 1907 nm
11
125
4.0
140 ± 30
4.1 ± 0.4
33
0.1
98
0.2 ± 0.1
79 ± 8
12
178
4.0
160 ± 30*
–
32
15
0.9
17 ± 5*
–
Values indicated by asterisks are the values calculated from Maker-fringe experiments according to Jerphagnon and Kurtz.23 When the coherence length could not be measured, the corresponding value obtained by the Sellmeier curve was used. Note that there is still an uncertainty about the correct values to be used for d11 of quartz: Here we used pm/V. If the suggested value of pm/V (Ref. 24) is used instead, all our results in this table become 25% smaller.
Table 3
Comparison of the Figure of Merit for Type I Phase-Matched Second-Harmonic Generation of Some Inorganic and Organic Single Crystalsa
Note that all values except that for NPP [reference, pm/V] correspond to a reference of pm/V to permit a meaningful comparison. The values indicated by asterisks correspond to noncritical phase matching.
Tables (3)
Table 1
Selection of Measured Refractive Indices for Various Wavelengths above the Absorption Edgea
λ (nm)
n1
n2
n3
700
2.36
2.31
1.457
740
2.26
2.22
1.456
780
2.22
2.18
1.453
820
2.19
2.16
1.451
875.3
2.15
2.14
1.458
954*
2.12
2.10
1.448
1064
2.08
2.06
1.441
1313
2.03
2.02
1.443
1542*
2.01
2.00
1.455
1907*
2.00
2.00
1.445
Sellmeier Parameters
ωeg (1015
3.586
3.880
13.625
λeg (nm)
525.6
485.8
138.4
γ0ωp2 (1030)
16.06
22.42
161.84
A
1.652
1.376
0.215
Values indicated by asterisks were calculated from the coherence lengths of Maker-fringe measurements. The parameters used to fit the refractive indices with a one-oscillator Sellmeier model are also listed. The Sellmeier parameters obtained for n3 are only approximate because the dispersion of this refractive index is too small to yield precise values for these parameters.
Table 2
Theoretical (Oriented Gas Model) and Experimental Nonlinear-Optical Susceptibilities dij and Coherence Lengths lijc of DANPHa
(ij)
Theory
Experiment
dij (pm/V)
lijc (µm)
dij (pm/V)
lijc (µm)
λ = 1542 nm
11
185
1.75
200 ± 40
1.76 ± 0.2
33
0.1
51
0.3 ± 0.2
–
12
260
1.67
270 ± 50*
–
32
21
0.7
35 ± 10*
–
λ = 1907 nm
11
125
4.0
140 ± 30
4.1 ± 0.4
33
0.1
98
0.2 ± 0.1
79 ± 8
12
178
4.0
160 ± 30*
–
32
15
0.9
17 ± 5*
–
Values indicated by asterisks are the values calculated from Maker-fringe experiments according to Jerphagnon and Kurtz.23 When the coherence length could not be measured, the corresponding value obtained by the Sellmeier curve was used. Note that there is still an uncertainty about the correct values to be used for d11 of quartz: Here we used pm/V. If the suggested value of pm/V (Ref. 24) is used instead, all our results in this table become 25% smaller.
Table 3
Comparison of the Figure of Merit for Type I Phase-Matched Second-Harmonic Generation of Some Inorganic and Organic Single Crystalsa
Note that all values except that for NPP [reference, pm/V] correspond to a reference of pm/V to permit a meaningful comparison. The values indicated by asterisks correspond to noncritical phase matching.