Nonlinear optical properties of silver colloidal solution by in situ synthesis technique

The silver colloidal solutions were prepared by in situ synthesis technique in the presence of the Polymethyl Methacrylate, which was polymerized by reversible addition-fragmentation transfer. The UV–VIS spectra and transmission electron microscopy had shown the formation of sphere silver nanoparticles with average size of 10 nm. Nonlinear optical properties as a function of silver concentration were studied using Z-scan technique with 13 ns pulse duration at 532 nm. The optical nonlinearity enhancement was observed by increasing the concentration. The third-order nonlinear susceptibility χ⁽³⁾ was measured to 1.045 × 10⁻¹¹ esu when the concentration was 2.13 mg/ml. Besides, the sample was founded to exhibit a shift from saturable absorption to reverse saturable absorption at higher incident laser energy. The reverse saturable absorption was observed to be responsible for the optical limiting characteristics in our experiments.     

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.     

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.     

Nonlinear optical characteristics of self-assembled films of ZnO

In the present work, we have investigated the nonlinear optical properties of self-assembled films formed from ZnO colloidal spheres by z-scan technique. The sign of the nonlinear component of refractive index of the material remains the same; however, a switching from reverse saturable absorption to saturable absorption has been observed as the material changes from colloid to self-assembled film. These different nonlinear characteristics can be mainly attributed to ZnO defect states and electronic effects when the colloidal solution is transformed into self-assembled monolayers. We investigated the intensity, wavelength and size dependence of saturable and reverse saturable absorption of ZnO self-assembled films and colloids. Values of the imaginary part of third-order susceptibility are calculated for particles of size in the range 20–300 nm at different intensity levels ranging from 40 to 325 MW/cm² within the wavelength range of 450–650 nm. PACS 81.16.Dn; 42.65.-k; 42.65.An; 42.70.-a; 42.70.Nq; 78.20.Ci     

有机材料反饱和吸收特性分析

从能级角度出发,结合入射激光脉宽对粒子吸收方面的影响,用速率方程模拟了各能级粒子数的瞬时变化关系,给出了激光脉宽与能级寿命可比拟时反饱和吸收的动态解,表明粒子在能级上的分布情况。用C60和HITCI(1,1′,3,3,3′,3′hexa methyl lindo tricarbocyanine Iodide)的实验参数理论模拟了激发态吸收截面大于基态吸收截面时透射率随光强的变化关系,用以说明大的上能级吸收截面可以抑制光强过大时引起的饱和吸收,增强材料的非线性光限幅特性。     

有机材料ZnTBP-CA-PhR的非线性吸收和光学限幅性能

报道了一种新型有机材料ZnTBP-CA-PhR的光学非线性吸收特性，此材料在激光作用下，在可见光区域具有反饱和吸收，再反饱和吸收和饱和吸收效应.同时发现该材料优良的光学限幅性能，不仅光限幅的阈值低，而且限幅前光透射呈线性状态没有光学非线性效应.用5能级结构模型及速率方程模拟了饱和及反饱和的实验曲线，分析了非线性吸收等的物理机理.     

Studies on third-order nonlinear optical properties and reverse saturable absorption in polythiophene/poly (methylmethacrylate) composites

We report here the studies on third-order nonlinear optical properties of two novel polythiophene composite films investigated using the Z-scan technique. The measurements were carried out using a Q-switched, frequency doubled Nd:YAG laser producing 7 nanosecond laser pulses at 532 nm. Z-scan results reveal that the composite films exhibit self-defocusing nonlinearity. The real and imaginary parts of the third-order nonlinear optical susceptibility were of the order 10⁻¹² esu. The effective excited-state absorption cross section was found to be larger than the ground state absorption cross section, indicating that the operating nonlinear mechanism is reverse saturable absorption (RSA). The polythiophene composite films also exhibit good optical power limiting of the nanosecond laser pulses. The nonlinear optical parameters are found to increase on increasing the strength of the electron-donor group, indicating the dependence of χ ⁽³⁾ on the electron-donor/acceptor units of polythiophenes.     

Saturable and reverse saturable absorption in aqueous silver nanoparticles at off-resonant wavelength

Silver nano-colloid was prepared by chemical reduction method and its nonlinear absorption properties were investigated by using open aperture z-scan experiment with nanosecond laser pulses operating at 532?nm. Interestingly, a switch over from saturable absorption to reverse saturable absorption was observed when the input intensity is increased from 28.1 to 175.8?MW/cm². The underlying mechanism responsible for the observed switching behaviour is the interplay between ground state plasmon band bleaching and excited state absorption. Theoretical fitting was done by using a model in which nonlinear absorption coefficient as well as saturation intensity are incorporated.     

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.     

Diploe-allowed optical absorption of an exciton in a spherical parabolic quantum dot

A investigation of the linear and nonlinear optical properties of an exciton in a spherical parabolic quantum dot has been performed by using the matrix diagonalization method. The optical absorption coefficients between the ground state (L=0,π=+1) and the first excited state (L=1,π=-1) have been examined based on the computed energies and wave functions. The results are presented as a function of the incident photon energy for the different values of the incident optical intensity and the confinement strength. We found the optical absorption coefficient is strongly affected by the incident optical intensity and the confinement strength.     

Nonlinear intersubband optical absorption in semiparabolic quantum wells

The linear and third-order nonlinear optical absorptions in semiparabolic quantum wells are studied in detail. Analytic formulas for the linear and third-order nonlinear optical absorption coefficients are obtained using the compact density matrix approach. Based on this model, numerical results are presented for typical GaAs/AlGaAs semiparabolic quantum wells. The results show that the factors of the incident optical intensity and the semiparabolic confinement frequency have great influences on the total optical absorption coefficients.     

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.     

Linear and nonlinear intersubband optical absorption in symmetric double semi-parabolic quantum wells

The linear and the nonlinear intersubband optical absorption in the symmetric double semi-parabolic quantum wells are investigated for typical GaAs/AlxGa1−xAs. Energy eigenvalues and eigenfunctions of an electron confined in finite potential double quantum wells are calculated by numerical methods from Schrödinger equation. Optical properties are obtained using the compact density matrix approach. In this work, the effects of the barrier width, the well width and the incident optical intensity on the optical properties of the symmetric double semi-parabolic quantum wells are investigated. Our results show that not only optical incident intensity but also structure parameters such as the barrier and the well width really affect the optical characteristics of these structures.     

Anisotropic nonlinear optical absorption of gold nanorods in a silica matrix

Nanocomposite films consisting of gold nanospheres or gold nanorods embedded in a silica matrix have been prepared using a hybrid deposition technique consisting of plasma-enhanced chemical vapor deposition of SiO₂ and co-sputtering of gold, followed by annealing at 900 °C. Subsequent irradiation with 30 MeV heavy ions (Cu⁵⁺) was used to form gold nanorods. Linear and nonlinear optical properties of this material are closely related with the surface plasmon resonance in the visible. The nonlinear absorption coefficient (α₂@532 nm) for the films containing gold nanospheres was measured by Z-scan and P-scan techniques, and it was found to be isotropic and equal to −4.8 × 10⁻² cm/W. On the contrary, gold nanorods films exhibited two distinct surface plasmon resonance absorption bands giving rise to a strong anisotropic behavior, namely a polarization-dependent linear absorption and saturable absorption. Z-scan and P-scan measurements using various light polarization directions yielded nonlinear absorption coefficient (α₂@532 nm) values varying from −0.9 × 10⁻² cm/W up to −3.0 × 10⁻² cm/W. Linearity of the P-scan method in the context of nanocomposite saturable absorption is also discussed.     

Designing novel chalcone single crystals with ultrafast nonlinear optical responses and large multi-photon absorption coefficients

A chalcone single crystal, 1-(4-chlorophenyl)-3-(4-methoxyphenyl)prop-2-en-1-one that is transparent over the visible to infrared region is introduced as a new potential material to third-order nonlinear optical applications. The crystal exhibits ultrafast optical response (≤90 fs) and large optical nonlinearity in the wavelength range 800–1200 nm. A very large effective two-photon absorption coefficient β_eff exceeding 120 cm/GW can be obtained with this chalcone crystal, at a low intensity threshold of 41 MW/cm². The mechanism of nonlinear absorption at different levels of intensity has been discussed. The crystal shows no damage against the laser pulse intensity as high as 8 GW/cm². We discuss the molecular and crystal designing of chalcones with large and ultrafast optical nonlinearity combined with low optical cut-off (<450 nm).     

Wavelength dependence of nonlinear absorption in a bis-phthalocyanine studied using the Z-scan technique

The wavelength dependence of the nonlinear absorption of a bis-phthalocyanine, Nd(Pc)₂, dissolved in dimethyl formamide was studied in the rising part of the Q-band using the open aperture Z-scan technique, to determine the wavelength region over which the nonlinear absorption changes from reverse saturable absorption to saturable absorption. It was found that the sample could be used as a reverse saturable absorber, and hence as an optical limiter, up to a wavelength of about 604 nm. The imaginary part of the third order susceptibility was also calculated for these wavelengths. Resonant enhancement of the imaginary part of the third order susceptibility was clearly observed. Received: 26 April 2002 / Revised version: 30 June 2002 / Published online: 20 December 2002 RID="*" ID="*"Corresponding author. Fax: +91-484/576-714, E-mail: kpu@cusat.ac.in RID="**" ID="**"Present address: Optical Sciences Center, University of Arizona, Tucson, USA     

Intersubband optical absorption coefficients and refractive index changes in modulation-doped asymmetric double quantum well

The linear and the third-order nonlinear optical absorption coefficients and refractive index changes in a modulation-doped asymmetric double quantum well are studied theoretically. The electron energy levels and the envelope wave functions in this structure are calculated by the Schrödinger and Poisson equations self-consistently in the effective mass approximation. The analytical expressions of optical properties are obtained by using the compact density-matrix approach. In this regard, the linear, nonlinear and total intersubband absorption coefficients and refractive index changes are investigated as a function of right-well width (Lw₂) of asymmetric double quantum well. Our results show that the total absorption coefficients and refractive index changes shift toward higher energies as the right-well width decreases. In addition, the total optical absorption coefficients and refractive index changes is strongly dependent on the incident optical intensity.     

Nonlinear optical absorption studies of an organo-metallic complex by Z-scan technique

An organo-metallic complex, [(CH₃)₄N][Ni(dmit)₂] (dmit²⁻ = (1,3-dithiole-2-thione-4,5-dithiolate), abbreviated as MeNi, is synthesized. The nonlinear optical absorption properties of MeNi dissolved in acetone have been studied using the open-aperture Z-scan technique with 40 ps pulse width at 1064 nm and 1 ns, 15 ns pulse width at 1053 nm, respectively. Strong saturable absorption has been found when the sample solution is irradiated by 40 ps and 1 ns laser pulses. While irradiated with 15 ns laser pulse, a stronger reverse saturable absorption has been found. The nonlinear optical absorption coefficients are −1.03 × 10⁻¹¹ m/W, −1.85 × 10⁻¹¹ m/W and 3.84 × 10⁻¹⁰ m/W, respectively. The mechanism responsible for the difference between the results is analyzed. All the results suggest that this material may be a promising candidate for the application to laser pulse compression in the near-infrared waveband.     

Linear and nonlinear intersubband optical absorption coefficients and refractive index changes in a quantum box with finite confining potential

In this work, both the intersubband optical absorption coefficients and the refractive index changes are calculated exactly in a quantum box. Analytical expressions for the linear and nonlinear intersubband absorption coefficients and refractive index changes are obtained by using the compact-density matrix approach. Numerical results are presented for typical GaAs/Al_xGa_1−x As quantum box system. The linear, third-order nonlinear and total absorption and refractive index changes are investigated as a function of the incident optical intensity and structure parameters such as box-edge length and stoichiometric ratio. Our results show that both the incident optical intensity and the structure parameters have a great effect on the total absorption and refractive index changes.     

Slow light and saturable absorption

Quantitative analysis of slow light experiments utilising coherent population oscillation (CPO) in a range of saturably absorbing media, including ruby and alexandrite, Er³⁺:Y₂SiO₅, bacteriorhodopsin, semiconductor quantum devices and erbium-doped optical fibres, shows that the observations may be more simply interpreted as saturable absorption phenomena. A basic two-level model of a saturable absorber displays all the effects normally associated with slow light, namely phase shift and modulation gain of the transmitted signal, hole burning in the modulation frequency spectrum and power broadening of the spectral hole, each arising from the finite response time of the non-linear absorption. Only where hole-burning in the optical spectrum is observed (using independent pump and probe beams), or pulse delays exceeding the limits set by saturable absorption are obtained, can reasonable confidence be placed in the observation of slow light in such experiments. Superluminal (“fast light”) phenomena in media with reverse saturable absorption (RSA) may be similarly explained. The article is published in the original.