Nonlinear optical properties of push–pull polyenes for electro-optics

M. Stähelin; B. Zysset; M. Ahlheim; S. R. Marder; P. V. Bedworth; C. Runser; M. Barzoukas; A. Fort

doi:10.1364/JOSAB.13.002401

Journal of the Optical Society of America B
Vol. 13,
Issue 11,
pp. 2401-2407
(1996)
•https://doi.org/10.1364/JOSAB.13.002401

Nonlinear optical properties of push–pull polyenes for electro-optics

M. Stähelin, B. Zysset, M. Ahlheim, S. R. Marder, P. V. Bedworth, C. Runser, M. Barzoukas, and A. Fort

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M. Stähelin, B. Zysset, M. Ahlheim, S. R. Marder, P. V. Bedworth, C. Runser, M. Barzoukas, and A. Fort, "Nonlinear optical properties of push–pull polyenes for electro-optics," J. Opt. Soc. Am. B 13, 2401-2407 (1996)

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Abstract

Improved nonlinear organic chromophores of varying conjugation length with either thiobarbituric acid or 3-dicyanomethylene-2,3-dihydrobenzothiophene-1,1-dioxide (FORON^® Blue) acceptors have been synthesized and investigated for their nonlinear optical properties. Very large quadratic hyperpolarizabilities $β (- 2 ω; ω, ω)$ have been found, up to $25,700 \times 10^{- 48}$ esu at $λ = 1.91$ µm. In a guest–host polymer very high electro-optic (EO) coefficients, of up to 55 pm/V, have been determined at $λ = 1.31$ µm with 20-wt % chromophore loading. We find good agreement between molecular parameters evaluated by electric-field-induced second-harmonic generation (EFISH) and the measurements of guest–host solid–solid solutions. The latter method is well suited to the determination of the product of dipole moment μ and hyperpolarizability β quickly and reliably at the wavelength of interest for EO applications without the complications associated with EFISH measurements.

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Guest–Host Polymer (solid solutions of Azo 1̲)					pSMAa Side-Chain Polymer Containing 56 wt % Azo ( $E = 150$ V/µm)
Host	Concentration (wt %)	Poling Field (V/µm)	r₃₃ Measured (pm/V)	r₃₃ Scaled to 56 wt % ( $E = 150$ V/µm) (pm/V)	r₃₃ Measured (pm/V)
pSMA	8.4	95	$1.9 \pm 0.4$	$20 \pm 4$
pSMA	11.3	190	$4.8 \pm 0.6$	$19 \pm 2$	20±1
pc	9.5	100	$2.4 \pm 0.2$	$21 \pm 2$

	Guest–Molecule
	${FB}_{n = 0}$ 6	${FB}_{n = 1}$ 8	${FB}_{n = 2}$		${FB}_{n = 3}$ 12	${TBA}_{n = 0}$ 5	${TBA}_{n = 1}$		${TBA}_{n = 2}$		${TBA}_{n = 3}$
	${FB}_{n = 0}$ 6	${FB}_{n = 1}$ 8	10	13	${FB}_{n = 3}$ 12	${TBA}_{n = 0}$ 5	7a	7b	9a	9b	11a	11b
Concentration (wt %)	10	1.6	9.3	20	0.76	10	7.4	2.9	24	3.2	9.4	2.4
E (V/µm)	71	150	151	150	100	71	97	122	147	95	35	87
r₃₃ (pm/V)	1.0	1.5	21	55	2.8	1.0	3.0	1.2	28	2.5	4.4	2.4

Molecule	Conjugation Length	R	M	EO in Guest–Host Polymers (TBA in PC)				EFISH
Molecule	Conjugation Length	R	M	λ_max (nm)	No. of Samples	r₃₃a Scaled to 10 wt % and $E = 100$ V/µm (pm/V)	$µ β (- ω; ω, 0)$ b Relative to Molecule 7a	μβ(2ω; ω, ω) (10^-48 esu)	λ_max (nm)	$µ β (- ω; ω, 0)$ c Relative to Molecule 7a
5a	$n = 0$	C₂H₅	331	490	2	1.3 ± 0.5	0.28	370c	484	0.22
7a	$n = 1$	C₂H₅	357	570	5	4.4 ± 0.5	(1)	1780d	572	(1)
7b	$n = 1$	C₆H₅	454	575	2	3.3 ± 0.5	0.95	—	—	—
9a	$n = 2$	C₂H₅	384	600	3	8.8 ± 2	2.2	3950c	604	2.1
9b	$n = 2$	C₆H₅	480	610	2	8.3 ± 2	2.6	—	—	—
11a	$n = 3$	C₂H₅	410	610	3	14 ± 2	3.7	9830c	624	5.1
11b	$n = 3$	C₆H₅	506	630	2	12 ± 2	3.9	—	—	—

Molecule	Conjugation Length	M	EO in Guest–Host Polymers (FB in PC)				EFISH
Molecule	Conjugation Length	M	λ_max (nm)	No. of Samples	r₃₃a Scaled to 10 wt % and $E = 100$ V/µm (pm/V)	$µ β (- ω; ω, 0)$ a Relative to Molecule 7a	μβ(2ω; ω, ω)b ( $10^{- 48}$ esu)	λ_max (nm)	$µ β (- ω; ω, 0)$ c Relative to Molecule 7a
6	$n = 0$	361	592	2	1.5 ± 0.5	0.35	1070	585	0.59
8	$n = 1$	387	680	5	6.5 ± 0.5	1.6	3300	672	1.7
10	$n = 2$	414	720	4	14 ± 2	3.7	10 500	732	4.6
13	$n = 2$	497	750	2	18 ± 3	5.7	13 500	772	5.2
12	$n = 3$	440	750	2	38 ± 7	11	25 700	742	11

Guest–Host Polymer (solid solutions of Azo 1̲)					pSMAa Side-Chain Polymer Containing 56 wt % Azo ( $E = 150$ V/µm)
Host	Concentration (wt %)	Poling Field (V/µm)	r₃₃ Measured (pm/V)	r₃₃ Scaled to 56 wt % ( $E = 150$ V/µm) (pm/V)	r₃₃ Measured (pm/V)
pSMA	8.4	95	$1.9 \pm 0.4$	$20 \pm 4$
pSMA	11.3	190	$4.8 \pm 0.6$	$19 \pm 2$	20±1
pc	9.5	100	$2.4 \pm 0.2$	$21 \pm 2$

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