Resonant third-order hyperpolarizabilities of large organic molecules

C. Maloney; W. Blau

doi:10.1364/JOSAB.4.001035

Journal of the Optical Society of America B
Vol. 4,
Issue 6,
pp. 1035-1039
(1987)
•https://doi.org/10.1364/JOSAB.4.001035

Resonant third-order hyperpolarizabilities of large organic molecules

C. Maloney and W. Blau

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C. Maloney and W. Blau, "Resonant third-order hyperpolarizabilities of large organic molecules," J. Opt. Soc. Am. B 4, 1035-1039 (1987)

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Abstract

Resonant degenerate four-wave mixing in a number of infrared-absorbing dyes was studied with 160-psec pulses at 1.064 μm. Hyperpolarizabilities in the range of 10⁻⁴⁴ to 10⁻⁴² V⁻² m⁵ were observed. A theoretical model based on a two-band system is developed that explains the results and permits the prediction of hyperpolarizabilities from the linear spectroscopic properties.

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Dye	T	n	R	$χ_{x y y x}^{(3)} (m^{2} / V^{2})$	L_L⁴	N₀ (m⁻³)	γ_xyyx (V⁻² m⁵)
β-Carotene	1.0	1.3	<0.0010	<0.2 ×IO⁻²⁰	0.726	2 × 10²³	<1 × 10⁻⁴⁴
Nigrosine	0.38	1.33	0.0056	2.62 × 10⁻²⁰	0.726	4,2 × 10²³	7.2 × 10⁻⁴⁴
DTTC	1.0	1.3	0.0054	0.8 × 10⁻²⁰	0.726	2.5 × 10²³	4.9 × 10⁻⁴⁴
DNTPC	0.94	1.3	0.0074	1.02 × 10⁻²⁰	0.726	4.3 × 10²²	3.27 × 10⁻⁴³
BDN	0.53	1.49	0.011	1.7 × 10⁻²⁰	1.23	1.6 × 10²²	8.6 × 10⁻⁴³
A9860	0.65	1.45	0.023	1.75 × 10⁻²⁰	1.1	5.8 × 10²¹	2.7 × 10⁻⁴²
IR5	0.55	1.45	0.021	2.13 × 10⁻²⁰	1.1	1 × 10²²	1.9 × 10⁻⁴²
S501	0.67	1.55	0.27	1.25 × 10⁻¹⁹	1.65	5 × 10²¹	1.27 × 10⁻⁴²

Dye	ω (sec⁻¹)	Δω (sec⁻¹)	τ_rad (nsec)	τ_f (fsec)	T₂ (fsec)	ϕ_f	γ_xyyx (V⁻² m⁵)
Nigrosine	3.34 × 10¹⁵	1.57 × 10¹⁵	3	–	40	1.0 × 10⁻⁴	3.25 × 10⁻⁴⁴
DTTC	2.5 × 10¹⁵	7.34 × 10¹⁴	12	2000	18.7	1.67 × 10⁻¹	9.5 × 10⁻⁴³
DNTPC	1.89 × 10¹⁵	1.2 × 10¹⁴	54	–	7.6	1.0 × 10⁻⁴	1.16 × 10⁻⁴³
BDN	1.81 × 10¹⁵	0.41 × 10¹⁴	56	5600	14.8	1.0 × 10⁻¹	2.7 × 10⁻⁴³
A9860	1.76 × 10¹⁵	–	28	7.0	18.1	2.5 × 10⁻⁴	4.9 × 10⁻⁴²
IR5	1.73 × 10¹⁵	–	37	2.7	18.5	7.3 × 10⁻⁵	1.26 × 10⁻⁴²
S501	1.26 × 10¹⁵	–	90	17	15.3	1.89 × 10⁻⁴	2.56 × 10⁻⁴²

Dye	T	n	R	$χ_{x y y x}^{(3)} (m^{2} / V^{2})$	L_L⁴	N₀ (m⁻³)	γ_xyyx (V⁻² m⁵)
β-Carotene	1.0	1.3	<0.0010	<0.2 ×IO⁻²⁰	0.726	2 × 10²³	<1 × 10⁻⁴⁴
Nigrosine	0.38	1.33	0.0056	2.62 × 10⁻²⁰	0.726	4,2 × 10²³	7.2 × 10⁻⁴⁴
DTTC	1.0	1.3	0.0054	0.8 × 10⁻²⁰	0.726	2.5 × 10²³	4.9 × 10⁻⁴⁴
DNTPC	0.94	1.3	0.0074	1.02 × 10⁻²⁰	0.726	4.3 × 10²²	3.27 × 10⁻⁴³
BDN	0.53	1.49	0.011	1.7 × 10⁻²⁰	1.23	1.6 × 10²²	8.6 × 10⁻⁴³
A9860	0.65	1.45	0.023	1.75 × 10⁻²⁰	1.1	5.8 × 10²¹	2.7 × 10⁻⁴²
IR5	0.55	1.45	0.021	2.13 × 10⁻²⁰	1.1	1 × 10²²	1.9 × 10⁻⁴²
S501	0.67	1.55	0.27	1.25 × 10⁻¹⁹	1.65	5 × 10²¹	1.27 × 10⁻⁴²

Dye	ω (sec⁻¹)	Δω (sec⁻¹)	τ_rad (nsec)	τ_f (fsec)	T₂ (fsec)	ϕ_f	γ_xyyx (V⁻² m⁵)
Nigrosine	3.34 × 10¹⁵	1.57 × 10¹⁵	3	–	40	1.0 × 10⁻⁴	3.25 × 10⁻⁴⁴
DTTC	2.5 × 10¹⁵	7.34 × 10¹⁴	12	2000	18.7	1.67 × 10⁻¹	9.5 × 10⁻⁴³
DNTPC	1.89 × 10¹⁵	1.2 × 10¹⁴	54	–	7.6	1.0 × 10⁻⁴	1.16 × 10⁻⁴³
BDN	1.81 × 10¹⁵	0.41 × 10¹⁴	56	5600	14.8	1.0 × 10⁻¹	2.7 × 10⁻⁴³
A9860	1.76 × 10¹⁵	–	28	7.0	18.1	2.5 × 10⁻⁴	4.9 × 10⁻⁴²
IR5	1.73 × 10¹⁵	–	37	2.7	18.5	7.3 × 10⁻⁵	1.26 × 10⁻⁴²
S501	1.26 × 10¹⁵	–	90	17	15.3	1.89 × 10⁻⁴	2.56 × 10⁻⁴²

Abstract

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Equations (17)

Journal of the Optical Society of America B