Electro-optic effects in molecular crystals

Ch. Bosshard; K. Sutter; R. Schlesser; P. Günter

doi:10.1364/JOSAB.10.000867

Journal of the Optical Society of America B
Vol. 10,
Issue 5,
pp. 867-885
(1993)
•https://doi.org/10.1364/JOSAB.10.000867

Electro-optic effects in molecular crystals

Ch. Bosshard, K. Sutter, R. Schlesser, and P. Günter

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Ch. Bosshard, K. Sutter, R. Schlesser, and P. Günter, "Electro-optic effects in molecular crystals," J. Opt. Soc. Am. B 10, 867-885 (1993)

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Abstract

The electro-optic properties of 2-cyclooctylamino-5-nitropyridine and 2-(N-prolinol)-5-nitropyridine single crystals have been evaluated. The dependence of the electro-optic coefficients on the optical wavelength and the frequency of the applied electric field was determined. Enhancements of these coefficients near acoustic resonances were observed and are discussed in terms of elasto-optic contributions. We propose a simple expression for estimation of the limiting values of electro-optic and nonlinear-optical coefficients. In addition, the wavelength dependence of the electro-optic figure of merit for organic and inorganic materials is estimated.

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Material	r (pm/V), n	λ_eg = 2πc/ω_eg of Bulk (nm)	Ref.
DAST	r₁₁ (820 nm) = 400	600	2
4′-dimethylamino-N-methyl-4-stilbazolium tosylate	n₁ (820 nm) = 2.19	Assumed: 100 nm below cutoff wave length at 700 nm

SPCD (DMSM)	r₃₃ (632.8 nm) = 430	460	3,4
4′-dimethylamino-N-methyl-4-stilbazolium methylsulfate	n₃³r₃₃ (632.8 nm) = 1300	Estimated from absorption peak at 2.7 eV
	n₃ (632.8 nm) = 1.55
DCNP	r₃₃ (632.8 nm) = 87	531	5
3-(1,1-dicyanoethenyl)-1-phenyl-4,5-dihydro-1H-pyrazole	r₃₃ (632.8 nm) = 2.7	From the fit of the measured values of n³r using Eq. (19)

MNA	r₁₁ (632.8 nm) = 67	414	6,7
2-methyl-4-nitroaniline	n₁ (632.8 nm) = 2.00	From the Sellmeier coefficients of n₁ in Ref. 7

MMONS	r₃₃ (632.8 nm) = 39.9	421	8
3-methyl-4-methoxy-4′-nitrostilbene	n₃ (632.8 nm) = 2.129	From the Sellmeier coefficients n₃

NMBA	r₁₁ (488 nm) = 37.2	353	9
4-nitro-4′-methylbenzylidene aniline	r₁₁(514.5 nm) = 36.4	From the fit of the measured values of n³r using Eq. (19)
	r₁₁ (632.8 nm) = 25.2
	n₁ (488 nm) = 2.283
	n₁ (514.5 nm) = 2.216
	n₁ (632.8 nm) = 2.078
PNP	For r₁₂ and r₂₂ see Table 6 below	404	10
2-(N-prolinol)-5-nitropyridine	n₁ (632.8 nm) = 1.994	From the Sellmeier coefficients of the refractive indices	This work
	n₂ (632.8 nm) = 1.788
DAN	r₃₂ (632.8 nm) = 13	419	11,12
4-(N,N-dimethylamino)-3-acetamidonitrobenzene	n₃ (632.8 nm) = 1.949	From the Sellmeier coefficients of n₃

mNA	r₃₃ (632.8 nm) = 16.7	400	13
meta-nitroaniline	n₃ (632.8 nm) = 1.675	Estimated

COANP	For r₃₃ see Table 6 below	410	14
2-cyclooctylamine-5-nitropyridine	n₃ (632.8 nm) = 1.647	From the Sellmeier coefficients of n₃	This work

POM	r₅₂ (632.8 nm) = 5.2	358	15
3-methyl-4-nitropyridine-1-oxide	n₂ (632.8 nm) = 1.92	From the Sellmeier coefficients of the refractive indices
	n₃ (632.8 nm) = 1.64
Optimized benzene	r (501 nm) = 210	401	This work
(λ_eg (solid state) = 401 nm)	n (501 nm) = 2.2	= λ_eg^solution + 40 nm

Optimized stilbene	r (579 nm) = 1150	479	This work
(λ_eg (solid state) = 479 nm)	n (579 nm) = 2.4	= λ_eg^solution + 60 nm

Material	r (632.8= nm; pm/V)	K₀, K, K′, λ_eg of Bulk	n (632.8 nm)	Ref.
KNbO₃	r₄₂ = 380	From fit through the measured points with	n_b = 2.329	22, 29
		K₄₂ = −1 and λ_eg = 255.2 nm(from Ref. 29)	n_c = 2.169
		K′ = 580 pm/V	From Ref. 29
LiNbO₃	r₃₃ = 32.2	λ_eg = 208 nm (from Sellmeier parameters)	n_e = 2.20	30
		K′ = 46 pm/V (calculated from point)
		K = −1 (arbitrary)
BaTiO₃	r₅₁ = 1640 (at 546 nm)	λ_eg = 215 nm (from Sellmeier parameters)	n_e = 2.37	30
		K = −1 (arbitrary)	n_o = 2.44
		K′ = 815 pm/V	(at 546 nm)

Electro-Optics		Phase-Matched Frequency Doubling

Benzenes	Stilbenes	Benzenes	Stilbenes
A₁ = 1.54 × 10⁻¹⁵	A₁ = 8.73 × 10⁻³⁷	A₁ = 1.38 × 10⁻¹⁵	A₁ = 3.95 × 10⁻³⁹
b₁ = 6.28	b₁ = 14.23	b₁ = 5.59	b₁ = 13.50
A₂ = 1.87 × 10⁻¹⁵	A₂ = 5.47 × 10⁻³⁷	A₃ = 2.55 × 10⁻¹⁵	A₃ = 5.38 × 10⁻³⁹
b₂ = 6.28	b₂ = 14.23	b₃ = 5.59	b₃ = 13.50
		A₄ = 6.61 × 10⁻¹⁵	A₄ = 1.41 × 10⁻³⁸
—	—	b₄ = 5.59	b₄ = 13.50

λ_c (nm)	β_max(−ω,ω,0) (10⁻⁴⁰ m⁴/V)	2λ_c (nm)	β_max(−ω,ω,0) (10⁻⁴⁰ m⁴/V)	r_max (pm/V)	2λ_c (nm)	d_max (pm/V)	$d_{max}^{‖} (pm / V)$
500	170^a_,^b,…,220^c	1000	100^a_,^b,…, 140^a_,^c	140^c,…,210^a_,^b	1000	180^a_,^b,…,190^a_,^c	470^a_,^b,…,490^a_,^c
550	250^b,…, 860^c	1060	110^b,…,270^c	300^b,…,540^c	1060	210^b,…,370^c	540^b,…,980^c
630	590^b,…,6000^c	1300	350^b,…,4300^c	710^b,…,3700^c	1300	650^b,…,5900^c	1700^b…15,400^c

Characteristic	COANP	PNP
Formula	C₁₃H₁₉N₃O₂	C₁₀H₁₃N₃O₃
Molecular mass	249.32	223.23
Density	ρ = 1.24 g/cm³	ρ = 1.42 g/cm³
Melting point	T_m = 72.8°C	T_m = 83°C
Space-group symmetry	Pca2₁(Z = 4)	P2₁(Z = 2)
Point-group symmetry	mm2	2
Unit cell	a = 2.6281(5) nm	a = 0.5182(1) nm
	b = 0.6655(1) nm	b = 1.4964(4) nm
	c = 0.7630(6) nm	c = 0.7045(1) nm
		β = 106.76(1)°
	V = 1.3345(6) nm³	V = 0.5231 nm³

Crystal	d (mm)	L (mm)	w (mm)	d/L	Remark
COANP 1	1.7	1.448	6.97	1.17	Crystal between metal plates
COANP 2	1.66	1.424	6.43	1.17	Crystal between metal plates
COANP 3	1.75	1.428	5.40	1.23	Silver paste electrodes
COANP 4	2	1.35	—	1.48	Silver paste electrodes
COANP 5	1.7	1.448	—	1.17	Silver paste electrodes
COANP 6	6	4.135	—	1.45	Silver paste electrodes
PNP 1	4.2	2.2	—	1.91	Silver paste electrodes
PNP 2	2.7	3.015	6.8	0.90	Silver paste electrodes

Wavelength (nm)	r₁₃ (pm/V)	r₂₃ (pm/V)	r₃₃ (pm/V)	ν_π13 (kV)	ν_π23 (kV)	ν_π33 (kV)
514.5	+6.8 ± l.4^a	+26 ± 4	+28 ± 5	14.8 ± 2.2	2.8 ± 0.4	3.6 ± 0.5
632.8	+3.4 ± 0.5	+13 ± 2	+15 ± 2	40 ± 6	8.6 ± 1.3	9.5 ± 1.3
1064	+0.9 ± 0.5	+6.3 ± 1	+7.7 ± 1.1	270 ± 40	34 ± 5	33 ± 5

Wavelength (nm)	r₁₂ (pm/V)	r₂₂ (pm/V)	ν_π21 (kV)	ν_π22 (kV)
514.5	+20.2 ± 2.4	+28.3 ± 3.4	2.5 ± 0.4	2.8 ± 0.4
632.8	+13.1 ± 1.3	+12.8 ± 1.3	6.2 ± 0.9	8.7 ± 1.3
1064	+8.7± 1.3	+7.6± 1.1	18 ± 3	27 ± 4

Wavelength (nm)	\|n₃³r₃₃ − n₂³r₂₃\|		\|n₃³r₃₃ − n₁³r₁₃\|

	Measured	Calculated	Measured	Calculated
514.5	37 ± 6	38 ± 6	—	98 ± 20
632.8	8.6 ± 1.3	6 ± 20	54 ± 11	52 ± 14

Wavelength (nm)	r₂₃ (pm/V)	r₂₃^e (pm/V)	d₃₂(pm/V)^b	r₃₃ (pm/V)	r₃₃^e (pm/V)	d₃₃ (pm/V)^b
632.8	+13 ± 2	16 ± 4	—	+15 ± 2	9.3 ± 1.5	—
1064	+6.3 ± 1	9 ± 2	43 ± 9	+7.7 ± 1.1	5.1 ± 0.9	19.3 ± 3

Wavelength (nm)	r₁₂ (pm/V)	r₁₂^e (pm/V)	d₂₁(pm/V)^b	r₂₂ (pm/V)	r₂₂^e (pm/V)	d₂₂ (pm/V)^b
632.8	+13.1 ± 1.3	16 ± 2.2	⋯	+13.1 ± 1.3	7.4 ± 1.4	⋯
1064	8.7 ± 1.3	9.4 ± 1.4	68 ± 8	7.6 ± 1.1	4.1 ± 0.6	21.6 ± 4

Wavelength (nm)	f₁₃ (m²/C)	f₂₃ (m²/C)	f₃₃ (m²/C)
514.5	0.63 ± 0.13	+1.84 ± 0.37	+2.00 ± 0.40
632.8	0.24 ± 0.05	+0.92 ± 0.18	+1.06 ± 0.21
1064	0.06 ± 0.01	+0.44 ± 0.09	+0.54 ± 0.11

Crystal Axis	∊^a.	n² (ω ≈ 0)^b
a	2.8 ± 0.5	2.65
b	2.7 ± 0.7	2.87
c	2.6 ± 0.5	2.54

Crystal Axis	∊^a.	n² (ω ≈ 0)^b
a	2.8 ± 0.5	2.65
b	2.7 ± 0.7	2.87
c	2.6 ± 0.5	2.54

Abstract

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Figures (14)

Tables (14)

Equations (38)

Journal of the Optical Society of America B