Nonlinear optical characteristics of polymethine dyes

Nonlinear refraction, nonlinear absorption, and saturated absorption of a number of polymethine dyes are studied and their nonlinear optical parameters are measured by the Z-scan method (λ=1064 nm). Simultaneous occurrence of several nonlinear optical processes in the case of excitation of dye solutions by picosecond pulses is analyzed. Saturated absorption of dye solutions is considered in terms of different models.     

Thermally induced nonlinear optical response and optical power limiting of acid blue 40 dye

We report the investigations of thermally induced third-order nonlinear optical and optical limiting characterizations for various concentrations of acid blue 40 dye in N,N-Dimethyl Formamide, studied by employing z-scan technique under cw He–Ne laser irradiation at 633 nm wavelength. The samples exhibited nonlinear absorption and nonlinear refraction under the experimental conditions. For lower concentration, the samples display both saturable absorption (SA) and reverse saturable absorption (RSA); whereas with increase in concentration, RSA behaviour prevails. The estimated values of the effective coefficients of nonlinear absorption β_eff, nonlinear refraction n₂ and third-order nonlinear susceptibility χ⁽³⁾ were found to be of the order of 10^?2 cm/W, 10^?4 esu and 10^?6 esu respectively. Multiple diffraction rings were observed when the samples were exposed to laser beam due to refractive index change and thermal lensing. The effect of concentration and the laser intensity on the self-diffraction ring patterns was studied experimentally. The acid blue 40 dye also exhibited strong optical limiting properties under cw excitation and reverse saturable absorption is found to be the dominant nonlinear optical process leading to the observed nonlinear behaviour.     

Data analysis of z-scan experiment using Fresnel–Kirchoff integral method in colloidal TiO2 nanoparticles

In this study, a precise method to evaluate nonlinear optical absorption and refraction of materials using z-scan method based on Fresnel–Kirchhoff integral method (FK method) has been offered. The real electric field of a Gaussian beam passing through a nonlinear sample having both nonlinear absorption and refraction has been investigated using FK method. Subsequently, the z-scan curves have been studied. This is the first time that FK method has been used for calculating the nonlinear absorption coefficient. Additionally, an appropriate numerical curve-fitting method for calculating the nonlinear optical coefficients based on z-scan method has been suggested. Z-scan curves and nonlinear optical coefficients have been obtained for TiO₂ nanoparticles in CW irradiation regime with the particle size ranges from 70 to 90 nm. This is the first experimental study which uses this analytical numerical method. Finally, all calculated results extracted from this new method have been compared with those of the previous methods.     

Nonlinear optical response of silver and copper nanoparticles in the near-ultraviolet spectral range

The nonlinear optical response of silver and copper nanoparticles synthesized by ion implantation in silica glasses is studied in the near-ultraviolet spectral range at a wavelength of 354.7 nm. The real and imaginary parts of the third-order nonlinear susceptibility χ⁽³⁾ of composite materials are measured. It is shown that the quantity Imχ⁽³⁾ is due to saturated absorption, while Reχ⁽³⁾ is due to the self-defocusing effect in composite materials.     

Third-order optical nonlinearities of α,ω-dithienylpolyenes and oligo(thienylvinylene)

α,ω-Dithienylpolyenes and oligo(thienylvinylene) are interesting third-order nonlinear optical materials for a variety of device applications. To better understand the third-order nonlinear response of these materials, the third-order susceptibilities (χ⁽³⁾) and nonlinear absorption behaviors of two α,ω-dithienylpolyenes with different conjugation length and two oligo(thienylvinylene) with different substituents on the thiophene rings have been studied using degenerate four wave mixing (DFWM) and nonlinear transmission techniques at 532 nm. The χ⁽³⁾ values of 1×10⁻³ mol/l solutions are all of the order of 10⁻¹³ esu. The χ⁽³⁾ values increase with the increase of the linear absorption coefficient. In addition, these compounds exhibit reverse saturable absorption for nanosecond laser pulses. The strength of reverse saturable absorption varies when the conjugation length and substituents change. Moreover, the nonlinear absorption characteristics of these compounds in the picosecond regime differ from those in the nanosecond regime. The different nonlinear absorption behavior is due to the relative contributions from excited singlet–singlet and triplet–triplet absorption. The strong reverse saturable absorption characteristics of two of the compounds suggest that they could be potential candidates for optical limiting applications in the nanosecond regime.     

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.     

Enhanced nonlinear optical responses in metal-glass nanocomposites

The “engineered” nonlinear nanocomposite materials with extremely large values of optical Kerr susceptibility and fast temporal responses that can be precisely tuned to satisfy the requirements of switching applications is of current interest in photonics. Metal quantum-dot composite glasses can exhibit enhanced optical susceptibility, χ⁽³⁾, whose real and imaginary parts are related to the intensity-dependent refractive index and two-photon absorption coefficient, respectively. Classical (dielectric) and quantum confinement effects come into play in the nonlinear optical responses of these nanocomposites. Metal nanocluster-glass composites have been synthesized by 200 keV Cu⁺ and 1.5 MeV Au⁺ ion implantations in fused silica glasses at a dose of 3 × 10¹⁶ ions/cm², followed by thermal annealing in reducing atmosphere to promote cluster growth. UV-Visible spectroscopy has revealed prominent linear absorption bands at characteristic surface plasmon resonance (SPR) frequencies signifying appreciable formation of copper and gold colloids in glass matrices. Third-order optical properties of the composite materials have been studied by Z-Scan and Anti-Resonant Interferometric Nonlinear Spectroscopy (ARINS) measurements. The sign of nonlinear refraction is readily obtained from the Z-Scan signatures. The ARINS technique utilizes the dressing of two unequal-intensity counter-propagating pulsed light beams with differential nonlinear phases, which occur upon traversing the sample if it exhibits nonlinear optical response. This difference in phase manifests itself in the intensity-dependent transmission. The nonlinear refractive index, nonlinear absorption coefficient, the real and imaginary parts of the third-order optical susceptibility have been extracted.     

A study of photolysis of polychlorobiphenyl-containing transformer oil by UV spectroscopy

UV absorption spectra of polychlorobiphenyls in transformer oil have been studied. We have shown that the absorption of the corresponding bands decreases with the growth of the time of irradiation. At t = 40 min, the degree of transformation of Abs is up to 40–66%.     

Study of optical properties in a cubic quantum dot

In this paper, the effect of hydrostatic pressure on both the intersubband optical absorption coefficients and the refractive index changes is studied for typical GaAs/Al _x  Ga_1?x As cubic quantum dot. We use analytical expressions for the linear and third-order nonlinear intersubband absorption coefficients and refractive index changes obtained by the compact-density matrix formalism. The linear, third-order nonlinear, and total intersubband absorption coefficients and refractive index changes are calculated at different pressures as a function of the photon energy with known values of box length (L), the incident optical intensity (I), and Al concentration (x). According to the results obtained from the present work, we have found that the pressure plays an important role in the intersubband optical absorption coefficient and refractive index changes in a cubic quantum dot.     

Effect of nonlinear absorption in estimation of order of nonlinear optical process by fluorescence intensity

We report the effect of nonlinear absorption on the fluorescence signal. Attenuation of the incident beam intensity (I) in the medium due to nonlinear absorption reduces the fluorescence signal. We show that fluorescence signal proportional to I² is not always indicative of two-photon absorption process but such a dependence can be obtained for three or four-photon absorption process due to attenuation of the pump beam by nonlinear absorption. This reduction in the fluorescence signal due to nonlinear absorption is found to be more sensitive in the higher order nonlinear optical processes.     

Third-Order Nonlinear Optical Response near the Plasmon Resonance Band of Cu_(2-x)Se Nanocrystals

The third-order nonlinear optical properties of water-soluble Cu_(2-x)Se nanocrystals are studied in the near infrared range of 700-980 nm using a femtosecond pulsed laser by the Z-scan technique. It is observed that the nonlinear optical response of Cu_(2-x)Se nanocrystals is sensitively dependent on the excitation wavelength and exhibits the enhanced nonlinearity compared with other selenides such as ZnSe and CdSe. The W-shaped Z-scan trace, a mixture of the reversed saturated absorption and saturated absorption, is observed near the plasmon resonance band of Cu_(2-x)Se nanocrystals, which is attributed to the state-filling of free carriers generated by copper vacancies(self-doping effect) of Cu_(2-x)Se nanocrystals as well as the hot carrier thermal effect upon intense femtosecond laser excitation. The large nonlinear optical response and tunable plasmonic band make Cu_(2-x)Se nanocrystals promising materials for applications in ultra-fast all-optical switching devices as well as nonlinear nanosensors.     

Synthesis and optical properties of silver nanoparticles in ORMOCER

Experimental results on synthesis of metal nanoparticles in ORMOCER by ion implantation are presented. Silver ions were implanted into organic/inorganic matrix at an accelerating energy of 30?keV and doses in the range of 0.25?10¹⁷ to 0.75?10¹⁷?ion/cm². The silver ions form metal nanoparticles, which demonstrate surface plasmon absorption at the wavelength of 425?C580?nm. The nonlinear absorption of new composite materials is measured by Z-scan technique using 150?fs laser pulses at 780?nm wavelength. ORMOCER matrix shows two-photon nonlinear absorption, whereas ORMOCER with silver nanoparticles demonstrates saturated absorption. Some optical applications of these composite materials are discussed.     

Measurement of nonlinear properties and optical limiting ability of Rhodamine6G doped silica and polymeric samples

The third order nonlinear optical properties of Rhodamine6G (Rh6G) doped silica and polymeric samples have been investigated using single beam z-scan technique under excitation by the second harmonic of Nd:YAG laser beam (532 nm). The nonlinear refractive index, nonlinear absorption coefficient, real and imaginary parts of third order nonlinear susceptibility in the samples of silica and poly-methylmethacrylate (PMMA) matrices are measured. Thermal contribution to the nonlinear refractive index in case of undoped silica samples has been calculated in order to have better accuracy of the material response contribution to third order nonlinearity. The comparative study of the optical limiting performance of Rh6G doped silica and polymeric samples show that Rh6G doped silica is relatively superior for optical limiting applications.     

Nonlinear properties of polyurethane-urea/multi-wall carbon nanotube composite films

The third-order nonlinear optical properties of polyurethane-urea/multiwalled carbon nanotube composites (PU/MWNT) films with different MWNT concentrations are investigated by the use of the Z-scan technique at a wavelength of 532 nm with a pulse duration of 8 ns. The results reveal that the nonlinear refraction and absorption coefficients are linearly dependent on the MWNT concentration. The negative nonlinear refraction effect is validated from the closed-aperture Z-scan measurements. We find that PU/MWNT films are promising nonlinear optical materials, and the nonlinear coefficients can be controlled.     

Optical properties of impurity-bound polaron in a parabolic quantum dot

The linear and nonlinear optical properties of an electron, which is bounded to a Coulomb impurity in a polar semiconductor quantum dot with parabolic confinement in both two and three dimensions, are studied by using the Landau-Pekar variational method and the compact density-matrix approach. With typical semiconducting GaAs-based materials, the linear, third-order nonlinear, total optical absorption coefficients and refractive indexes have been examined. We find that the all absorption spectra and refractive index changes are strongly affected by the electron-LO-phonon interaction. The results also indicate that the polaron effect increases with decreasing dimensionality of a quantum dot.     

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.     

Ultrafast nonlinear optical response of Ag:BaTiO3 composite films at the near-ultraviolet wavelengths

The ultrafast nonlinear optical response of Ag:BaTiO3 composite films synthesized by pulse laser deposition (PLD) is studied at the near-ultraviolet (400 nm) wavelength. The pulse duration of the laser used in the measurement is 200 fs. The real and imaginary parts of the third-order nonlinear susceptibility x(3) of the composite materials are measured. The composite films indicate self-focusing effect and nonlinear saturation, the values of Rex(3) and Imx(3) are measured to be 3.42 × 10-10 and -1.37 × 10-10 esu respectively, which are much lower than those reported before. It is mainly because that the duration of the laser used in the measurements is too short to induce the hot electron excitation and the thermal effect. The ultrafast nonlinear saturated absorption response of the Ag:BaTiO3 composite films may have potential applications for femtosecond laser mode locking.     

Linear and nonlinear intersubband optical absorption in double triangular quantum wells

The linear and the third-order nonlinear optical absorptions in the asymmetric double triangular quantum wells (DTQWs) are investigated theoretically. The dependence of the optical absorption on the right-well width of the DTQWs is studied, and the influence of the applied electric field on the optical absorption is also taken into account. The analytical expressions of the linear and the nonlinear optical absorption coefficients are obtained by using the compact density-matrix approach and the iterative method. The numerical calculations are presented for the typical GaAs/Al_xGa_1?xAs asymmetric DTQWs. The results show that the linear as well as the nonlinear optical absorption coefficients are not a monotonous function of the right-well width, but have complex relationships with it. Moreover, the calculated results also reveal that applying an electric field to the DTQWs with a thinner right-well can enhance the linear optical absorption but has no prominent influence on the nonlinear optical absorption. In addition, the total optical absorption is strongly dependent on the incident optical intensity.     

I-scan thermal lens experiment in the pulse regime for measuring two-photon absorption coefficient

We present a new pump-probe mode-mismatched thermal lens method for pulse excitation aimed to the measurement of nonlinear absorption coefficient in optical materials. We develop a theoretical model based on the Fresnel diffraction approximation and their predictions are verified experimentally with samples of Rhodamine 6G and Rhodamine B in ethanol solution. The principal advantage of this technique is that it does not require any mechanical movement during measurement. Below we perform the new type of thermal lens experiment in the pulse regime for the measurement of nonlinear absorption coefficient in transparent samples and we demonstrate the validity of theoretical predictions using an alternative method to the classical thermal lens technique.     

A new type of resonances in saturated absorption spectroscopy of 3-level systems

We report the experimental observation of new resonances in saturated absorption spectra of a J = 1 to J = 0 transition of Ne atoms in a static magnetic field. These resonances, which are distinct from the well-known Zeeman and cross-over resonances, result from the modification of stimulated Raman processes by the simultaneous resonant saturation of an optical transition. The light-shifts of the various resonances are also studied.