Strong nonlinear optical refractive effect of self-assembled multilayer films containing tetrasulfonated iron phthalocyanine

Multilayer films containing anionic iron phthalocyanine tetrasulfonate (FePcTsNa₄) and cationic poly(diallydimethyl ammonium chloride) were prepared using electrostatic self-assembled layer-by-layer technique. The growth of the film was monitored by ultraviolet-visible absorption spectroscopy, and the morphology of the film was characterized by atomic force microscopy. Polarized visible spectra showed that macrocycles of FePcTsNa₄ in the film presented a flat orientation relative to the plane of the solid substrates. The third-order nonlinear optical properties of the film were studied by using Z-scan technique with laser duration of 21 ps at the wavelength of 532 nm. The FePcTsNa₄/PDDA film exhibited strong self-focusing effect with n₂ value of 4.13 × 10⁻¹⁵ m²/W, which is 4 orders larger than that of FePcTsNa₄ aqueous solution.     

Detection of higher nonlinear harmonics of volume photorefractive gratings in reflection geometry

A comprehensive technique has been used to detect diffraction from the second and the third nonlinear spatial harmonic components, along with the fundamental harmonic of volume photorefractive gratings recorded in a channel waveguide in a LiNbO₃ substrate. For the first time to our knowledge, efficient diffraction from the higher spatial harmonic components of a photorefractive grating has been detected in reflection geometry. The dependence of a Bragg wavelength shift on the order of nonlinearity is also reported.     

Strong optical limiting property of a ball-type supramolecular zinc-phthalocyanine in polymer-phthalocyanine composite film

The nonlinear absorption and optical limiting (OL) performance of a supramolecular hexa-phthalocyaninato-hexazinc (II) with hexylthio substituents in solution and in the solid-state have been described using the open-aperture Z-scan technique. The measurements were performed using collimated 4 ns pulses generated from a frequency-doubled Nd:YAG laser at 532 nm wavelength. The results indicated that OL performance of the investigated compound in the polymeric film is much better compared to properties in solution. With the excellent combination of OL parameters the investigated compound in the solid-state is a candidate for the use as optical limiter.     

Effects of metallization and bromination on nonlinear optical properties of diphenylporphyrins

Nonlinear refraction and nonlinear absorption of diphenylporphyrins with bromination and metallization were studied by Z-scan technique in nanosecond and picosecond regimes. Results show that both metallization and bromination of diphenylporphyrins can cause the regular change of magnitude and sign of nonlinear absorption. The transition between saturable absorption and reverse saturable absorption happens as bromine increases and metal ion changes. The effect of bromination on nonlinear refraction is small, the change of nonlinear refraction is mainly attributed to the metallization. Influences of photophysical parameters on nonlinear absorption and nonlinear refraction have been elucidated using five-level models.     

Influence of the central metal atom on the nonlinear optical properties of MPcs solutions and thin films

Third order nonlinear optical susceptibility (χ^〈3〉) of metallophthalocyanines (MPcs, where M = Co, Cu, Zn, Mg) thin films and solutions was investigated by standard backward degenerate four wave mixing (DFWM) method at 532 nm. Third harmonic generation (THG) measurement at 1064 nm performed on MPcs thin films is also discussed. MPcs thin films were grown by conventional thermal evaporation in high vacuum and solution were dissolved in tetrahydrofuran (THF), in which the studied materials are soluble. In the case of microscopic nonlinearity, we calculated the second order hyperpolarizability (γ) for MPcs solutions. We found that the χ^〈3〉 and the γ values are affected by the nature of the central metal atom. We also found that the value is larger than that measured via THG experiment. The variation in χ^〈3〉 values occurs due to the different resonance contributions.     

Investigation of nonlinear optical properties of organic dye by Z-scan technique using He-Ne laser

The third-order nonlinear optical properties of Basic Green 1 dye were measured by the Z-scan technique and measurements were carried out at different concentrations and several incident intensities. The results showed that the Basic Green 1 dye exhibited large nonlinear refractive coefficient () and nonlinear absorption coefficient () at the wavelength 632.8 nm of He-Ne. The negative sign of the nonlinear refractive index n₂ indicates that this material exhibits self-defocusing optical nonlinearity. These results show that Basic Green 1 dye has potential applications in nonlinear optics.     

Ultra fast third-order non-linear response of amino-triazole donor-acceptor derivatives by optical Kerr effect

We report the study of the temporal dependence of the non-linear optical response of novel organic materials in solution. The experimental results of the optical Kerr gate using 70 fs pulses show a quasi-instantaneous response for three derivatives of an amino-triazole donor-acceptor system. The non-linearity of the compounds is identified as arising from the electronic contribution to the third-order non-linear susceptibility. The non-linear parameters of each sample were obtained using the optical Kerr response of CS₂ as reference.     

Spatial-temporal frequency band of optical parametric amplifier

The spatial-temporal frequency band of optical parametric amplifier for collinear as well as for noncollinear phase-matching is analyzed taking into account angular dispersion of amplified pulsed beam. The simple formulae are derived which make possible determination of the largest frequency bands of parametric amplifiers in noncollinear geometry. It has been demonstrated that a shape of the spatial-temporal frequency band of optical parametric amplifier essentially depends on pump and signal wavelengths, and certain angular dispersion as well as proper beamwidth of signal pulse enable amplification of ultrashort pulses with duration of a few femtoseconds.     

Experimental studies of the second-order nonlinear optical response of a novel class of tricyanovinylated thiophene compounds

We measured the second-order nonlinear optical response of a novel class of tricyanovinylated thiophene compounds using electric-field-induced second-harmonic generation. Very large second-order nonlinearity was observed for these compounds. The results indicate that the combination of the tricyanovinyl acceptor and the thiophene conjugating moiety offers excellent molecular second-order optical nonlinearity.     

Generation of tunable infrared radiation in rubidium titanyl phosphate crystal for the optical measurement of number density, absorption cross-section of methane gas

Tunable near-infrared radiation has been generated in a rubidium titany1 phosphate (RTP) crystal by employing non-collinear difference-frequency mixing (DFM) technique. The input radiation sources are Nd:YAG laser radiation and its second harmonic pumped dye laser radiation. For the generation of 2.0 radiation, the maximum value of the conversion efficiency (quantum) obtained in the process is 49% from the dye (0.6945 μm) to the infrared (2.0 μm) radiation in the 7.9-mm-long crystal. The generated tunable mid-infrared radiation has been used to measure the number density, absorption cross-section and minimum detectable concentration of methane gas in its 2ν₃ band in a multi-pass cell at 30.075 Torr pressure. The number density and column density of the methane molecules are found to be 1.068×10¹⁸ cm⁻³ and 3.02×10²¹ cm⁻², respectively, whereas the minimum still-detectable concentration at 1.658 μm wavelength is estimated to be 4.523×10¹⁷/cm³.     

Dispersion of second-order nonlinear optical coefficient

A simple, approximate relation between the dispersion of the second-order nonlinear optical (SNLO) coefficient and first-order susceptibility has been derived using the well-known results of density-matrix calculation of quantum-mechanical theory. A new tensor of SNLO coefficient has been defined, which retains symmetries when the input beams are in the spectral range of transparency while the generated beam can also be in the spectral range of absorption. The validity of the relation has been checked for three ferroelectric crystals, KTP, LiNbO₃ and KNbO₃, which are transparent in the visible and near infrared, and for two semiconductors, GaP and GaAs, which absorb in the visible. Contrary to Miller’s law, the presented relation is in good agreement with measurements. Received: 8 February 2001 / Revised version: 2 July 2001 / Published online: 10 October 2001     

High sensitive measurements of absorption coefficient and optical nonlinearities

Accurate knowledge of absorption coefficient of a sample is a prerequisite for measuring the third-order optical nonlinearity of materials, which can be a serious limitation for unknown samples. We introduce a method, which measures both the absorption coefficient and the third-order optical nonlinearity of materials with high sensitivity in a single experimental arrangement. We use a dual-beam pump-probe experiment and conventional single-beam z-scan under different conditions to achieve this goal with communication relevant wavelength. We also demonstrate a counterintuitive coupling of the non-interacting probe-beam with the pump-beam in pump-probe z-scan experiment.     

Nonlinear refraction in photo-induced anisotropic states of azo-dye containing materials

The optical anisotropic states in the azo-dye Disperse Red 13 doped poly(methyl methacrylate) polymeric film are induced by polarized light and the nonlinear refractive index in these states are studied by the Z-scan technique. It is found that the n₂ of the sample can be controlled by changing both the polarization direction and the intensity of the 514 nm light. Photo-induced isomerization and reorientation of azo chromophores in polymer matrices are used to explain the results.     

Z-Scan studies of KYW, KYbW, KGW, and Ba(NO3)2 crystals

We present the studies of nonlinear refraction and nonlinear absorption in promising crystals which are extensively used in Raman lasers or as solid-state laser host materials: Ba(NO₃)₂, KGW, KYW, and KYbW. The single-beam z-scan technique with 1 ps laser pulses at 790 and 395 nm has been applied for the study. Nonlinear refraction-index intensity-coefficients and two-photon absorption coefficients have been determined for the crystals. The considerable enhancement of nonlinear refraction is observed in the crystals at 395 nm.     

Parametric dispersion and amplification in semiconductor plasmas: Effects of carrier heating

Using the hydrodynamic model of a semiconductor plasma, the influence of carrier heating on the parametric dispersion and amplification has been analytically investigated in a doped III-V semiconductor, viz. n-InSb. The origin of the phenomena lies in the effective second-order optical susceptibility (χ_e⁽²⁾) arising due to the induced nonlinear current density of the medium. Using the coupled-mode theory, the threshold value of pump electric field (|E_0T|_para) and parametric gain coefficient (α_para) are obtained via χ_e⁽²⁾. The relevant experiment has not been performed. Proper selection of the doping level not only lowers |E_0T|_para required for the onset of parametric excitation but also enhances α_para. The carrier heating induced by the intense pump modifies the electron collision frequency and hence the nonlinearity of the medium, which in turn further lowers |E_0T|_para and enhances α_para by a factor of ∼10³ and ∼2×10², respectively. The results strongly suggest that the incorporation of carrier heating by the pump in the analysis leads to a better understanding of parametric processes in solids and gaseous plasmas, which can be of great use in the generation of squeezed states.     

(1 + 2)-Dimensional sub-strongly nonlocal spatial optical solitons: Perturbation method

By extending the (1 + 1)-dimensional [(1 + 1)-D] perturbation method suggested by Ouyang et al. [S. Ouyang, Q. Guo, W. Hu, Phys. Rev. E. 74 (2006) 036622] to the (1 + 2)-D case, we obtain a fundamental soliton solution to the (1 + 2)-D nonlocal nonlinear Schrödinger equation (NNLSE) with a Gaussian-type response function for the sub-strongly nonlocal case. Numerical simulations show that the soliton solution obtained in this paper can describe the soliton states in both the sub-strongly nonlocal case and the strongly nonlocal case. It is found that the phase constant and the power of the (1 + 2)-D strongly nonlocal spatial optical soliton with a Gaussian-type response function are both in inverse proportion to the 4th power of its beam width.     

Third order nonlinear optical studies of bromocresol purple in liquid and solid media

The quest for materials exhibiting high nonlinear refraction and absorption are required for photonic device application. In this paper we report a simplified Z-scan technique, to study the optical nonlinearity of the dye bromocresol purple in methanol and ethanol for different concentration and dye doped polymer film at the wavelength 532 nm of Nd:YAG laser. The experimental results show that the investigated organic dye molecule exhibits saturation absorption and negative nonlinearity. The nonlinear absorption co-efficient and the nonlinear refractive index were measured for the dye doped film, and for dye in methanol and ethanol at the concentration of 0.03 mM and 0.05 mM. The measured third order susceptibility was found to be of the order of 10⁻⁶ e.s.u. in both solid and liquid medium. The result shows that the dye has potential applications in nonlinear optics.     

Widely tunable femtosecond fiber optical parametric oscillator

The phase-matching condition in a fiber is discussed. A balance among the different orders of fiber dispersion can be found to achieve a widely tuning modulation instability gain for pumping around the normal dispersion regime. Three coupled nonlinear wave equations are used to simulate the femtosecond fiber optical parametric oscillator. The numerical results show that, through appropriate choice of dispersion, femtosecond pulses with a 180-nm tunable range can be generated when pump wavelength near a fiber’s zero-dispersion wavelength is tuned only 7 nm. Further tuning is limited by the walk-off between the pump and the signal pulses.     

High optical gain using counterpropagating beams in iron and terbium-doped photorefractive lithium niobate

Exceptionally high values of photorefractive gain coefficient of up to 100 cm^-1 have been observed in Fe-doped and Fe/Tb-doped crystals of photorefractive lithium niobate. It is believed that these are the highest observed coefficients of any crystalline photorefractive medium. Accurate measurements of gain coefficient have been possible for the first time by using a specially cut triangular crystal which allows the use of short interaction lengths and the complete elimination of surface reflections by having the beams incident at Brewster’s angle. Experimental results are consistent with a simple model of photorefractive beam coupling up until the onset of noise which is observed to deplete the pump for interaction lengths longer than 1 mm. Received: 28 September 1998 / Revised version: 8 January 1999 / Published online: 31 March 1999