Electrooptical Chromophores for Nonlinear Optical and Photorefractive Applications

Guanidyl and phosphoraniminyl substituents: New electron donors in second-order nonlinear optical chromophores

Highly transparent and birefringent chromophores for organic photorefractive materials

Abstract A series of chromophores for application in organic photorefractive (PR) materials is investigated by electro-optical absorption measurements (EOAM). This experimental technique yields information on the transition dipole moment μ ag , the ground-state dipole moment μ g , and the change of the dipole moment upon optical excitation Δ μ within the intense charge transfer (CT) band of the dyes. It is shown that the results of the EOAM experiment allow us to estimate the PR figures-of-merits (FOMs) of the chromophores by either perturbational two-level equations or Kramers–Kronig transformation. In particular, chromophores based on the heterocyclic dihydropyran and dihydropyridine grou…

Dipolar NLO-phores with large off-diagonal components of the second-order polarizability tensor

Intramolecular charge transfer in elongated donor-acceptor conjugated polyenes

Abstract Intramolecular charge transfer (ICT) has been investigated by electro-optical absorption measurements for two series of donor-acceptor polyenes of increasing length. Each molecule undergoes an increase in dipole moment upon photoexcitation. The experimental results indicate that lengthening the polyenic chain linking the donor and acceptor end groups results in a bathochromic shift of the ICT absorption band and induces marked increases of both excited state and transition dipoles, whereas the ground-state dipole is relatively unaffected. As a result, marked photoinduced changes in the dipole moment (up to 33 D) were obtained with the longest molecules (up to 27 A) leading to highl…

Intramolecular charge transfer and enhanced quadratic optical non-linearities in push pull polyenes

Abstract Push-pull polyenes, which have an electron-donating group (D) and an electron-withdrawing group (A) grafted on opposite ends of a conjugated polyenic chain, are of particular interest as model compounds for long-distance intramolecular charge transfer (ICT), as well as potent non-linear optical chromophores. Several series of push-pull polyenes of increasing length, combining aromatic donor moieties and various acceptor groups, have been prepared and studied. Their linear and non-linear optical properties have been investigated by performing electro-optical absorption measurements (FOAM) and electric-field-induced second-harmonic generation (EFISH) experiments in solution. Each mol…

Enhanced nonlinear optical properties and thermal stability of donor-acceptor substituted oligothiophenes

Abstract Linear and nonlinear optical properties of a series of novel donor-acceptor substituted α-oligothiophenes were investigated by means of electrooptical absorption measurements (EOAM) and electric field induced second harmonic generation (EFISH). The second-order polarizabilities β(−2ω; ω, ω) were related to dipole changes Δμ ag and transition dipoles μ ag associated with low-lying charge-transfer (CT) excitations by using the perturbational two-level approximation. Systematic variation of the donor and acceptor groups led to compounds with exceptional nonlinearity and thermal stability. Too strong donor/acceptor pairs, however, yielded structures in the charge-resonance (CR) limit w…

Nondipolar Structures With Threefold Symmetry For Nonlinear Optics

Deviations from Kleinman symmetry of the second-order polarizability tensor in molecules with low-lying perpendicular electronic bands

Abstract 4-Nitroaniline (pNA) and 3,5-dinitro-aniline (3,5-DNA) were studied by electric field induced second harmonic generation (EFISH) and electrooptical absorption measurements (EOAM) in dioxane solution at T = 298 K. The measurements were carried out for two polarization conditions, the electric field vector of the linearly polarized incident light being parallel or perpendicular to the static electric field. The second-order polarizability tensor of pNA is confirmed to be Kleinman symmetric, while a strong deviation from index permutation symmetry is observed for 3,5-DNA. The latter is quantitatively interpreted by contributions of a low-lying electronic band with transition dipole pe…

Design and Optimization of Chromophores for Liquid Crystal and Photorefractive Applications

ABSTRACTOrganic chromophores have been exploited for a wide range of discrete optical and electronic functions as well as a growing number of combined opto-electronic functions. We are pursuing development of organic and polymer materials for a range of applications that require properties including liquid crystallinity, second order optical nonlinearity, photorefractivity and, more recently, special nonlinear optical behavior involving molecular chirality.