Acentric nonlinear optical N-benzyl stilbazolium crystals with high environmental stability and enhanced molecular nonlinearity in solid state

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We have developed a new cation core structure, N-benzyl stilbazolium nonlinear optical chromophore with a non-polar benzyl group to achieve acentric molecular ordering in the crystalline state. New N-benzyl stilbazolium crystal, BP3 (N,N-dimethylamino-N'-2,5-dimethylbenzyl-stilbazolium p-toluenesulfonate), exhibits an acentric crystal structure with the monoclinic P2(1) phase with a large macroscopic optical nonlinearity of 540 times the powder second harmonic generation efficiency of urea at the non-resonant wavelength of 1.9 mu m. Compared to conventional rod-shaped N-alkyl stilbazolium crystals, an enhanced hyperpolarizability of the chromophores beta(0) in the solid state can be utilized in bent-shaped N-benzyl stilbazolium crystals. This is attributed to the decreased inter-chromophore interactions due to the larger chromophore-chromophore separation induced by the bulky and bent-shaped N-benzyl group, so-called site-isolation effect. Moreover, by introducing the non-polar dimethylbenzyl group, BP3 crystals show a high environmental stability: they exhibit almost one order of magnitude smaller solubility in water than conventional stilbazolium crystals and also do not form a hydrated centrosymmetric phase even if crystallized in water-containing solvents. We have grown good optical quality crystals large enough for optical characterization. With as-grown BP3 crystals without additional polishing and cutting procedures we have demonstrated THz generation by optical rectification using 180 fs pulses at the pump wavelength of 836 nm.
Publisher
ROYAL SOC CHEMISTRY
Issue Date
2011
Language
English
Article Type
Article
Keywords

CONFIGURATIONALLY LOCKED POLYENE; SINGLE-CRYSTALS; ORGANIC SALTS; WAVE-GUIDES; TOSYLATE; GROWTH; DERIVATIVES; TECHNOLOGY; HYDRATE; DAPSH

Citation

CRYSTENGCOMM, v.13, no.2, pp.444 - 451

ISSN
1466-8033
DOI
10.1039/c0ce00456a
URI
http://hdl.handle.net/10203/98064
Appears in Collection
CH-Journal Papers(저널논문)PH-Journal Papers(저널논문)
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