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.     

Comparative analysis of multi-wave mixing and measurements of the higher-order nonlinearities in resonant media

The features of degenerate multi-wave mixing in resonant media (dye solutions) have been studied theoretically and experimentally. It has been demonstrated that thermal nonlinearity due to the induced absorption from the excited level contributes significantly to the efficiency of four-wave mixing, but results in lower efficiency of higher-order interactions. The measurement results obtained for the energy efficiency of four-, six- and eight-wave mixing enable calculations of the third-, fifth- and seventh-order nonlinear optical susceptibilities, respectively. Experimentally, the method proposed for measurements of the higher-order nonlinearities has been realized with the use of the multi-wave mixing at second harmonic λ = 532 nm of monopulse YAG:Nd³⁺ laser radiation in a Rhodamine 6G dye solution. The ratios ∣χ⁽⁵⁾∣/∣χ⁽³⁾∣ and ∣χ⁽⁷⁾∣/∣χ⁽⁵⁾∣ are determined to be of the order of 10⁻⁵ cm³/erg.     

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.     

Femtosecond Z-scan measurement of third-order optical nonlinearities in anatase TiO2 thin films

Anatase phase TiO₂ films have been grown on fused silica substrate by pulsed laser deposition technique at substrate temperature of 750 °C under the oxygen pressure of 5 Pa. From the transmission spectra, the optical band gap and linear refractive index of the TiO₂ films were determined. The third-order optical nonlinearities of the films were measured by Z-scan method using a femtosecond laser (50 fs) at the wavelength of 800 nm. The real and imaginary parts of third-order nonlinear susceptibility χ⁽³⁾ were determined to be −7.1 × 10⁻¹¹esu and −4.42 × 10⁻¹²esu, respectively. The figure of merit, T, defined by T=βλ/n₂, was calculated to be 0.8, which meets the requirement of all-optical switching devices. The results show that the anatase TiO₂ films have great potential applications for nonlinear optical devices.     

Oxygen-deficiency effect on thermal poling of silica-based glasses

Thermal poling has been investigated in silica-based glasses prepared by the sol-gel method. Samples with different OH-content (from 40 ppm to few 10³ ppm), doping (oxygen-vacancies, substitutional Sn, SnO₂ clusters) and post-synthesis treatment (X-ray irradiation) have been heated in vacuum at 280 °C with an applied voltage of 4 kV. Second-order non-linearity has been observed after poling, with χ⁽²⁾ of the order of 0.1 pm/V. The comparison among samples suggests that OH-content is not the only factor responsible for the observed non-linearity.     

Nonlinear optical properties of Cu nanoclusters by ion implantation in silicate glass

Metal nanocluster composite glass prepared by 180 keV Cu ions into silica with dose of 1 × 10¹⁷ ions/cm² has been studied. The microstructural properties of the nanoclusters were analysed by optical absorption spectra and transmission electron microscopy (TEM). Third-order nonlinear optical properties of the nanoclusters were measured at 1064 nm and 532 nm excitations using Z-scan technique. The nonlinear refraction index, nonlinear absorption coefficient, and the real and imaginary parts of the third-order nonlinear susceptibility were deduced. The mechanisms responsible for the nonlinear response were discussed. Absolute third-order nonlinear susceptibility χ⁽³⁾ of this kind of sample was determined to be 2.1 × 10⁻⁷ esu at 532 nm and 1.2 × 10⁻⁷ esu at 1064 nm, respectively.     

Third-order nonlinear optical properties of multiwalled carbon nanotubes modified by CdS nanoparticles

CdS nanoparticles were coated on the side wall of multiwalled carbon nanotubes (MWCNTs) by a wet chemical synthesis approach via noncovalent functionalization of MWCNTs with poly(diallyldimethylammonium chloride) (PDDA). The as-prepared material was characterized by X-ray diffraction (XRD), UV–vis absorption, fluorescence and transmission electron microscopy (TEM). The results indicated that CdS nanoparticles were uniformly coated on the surface of MWCNTs. Third-order optical nonlinearity of the as-prepared material was studied with the Z-scan technique with picosecond laser pulses at 532 nm. The Z-scan curve revealed that CdS nanoparticle-modified MWCNTs exhibited negative nonlinear refraction index and positive absorption coefficient. The real part and imaginary part of the third-order nonlinear susceptibility χ⁽³⁾ were calculated to be −4.9 × 10⁻¹² and 6.8 × 10⁻¹³ esu, respectively.     

Intracavity frequency doubling of an active Q-switched Nd:YAG laser with 2.25 W output power at 473 nm

An active Q-switched diode-end-pumped Nd:YAG laser is reported with 2.9 W output power on the ⁴F_3/2 → ⁴I_9/2 transitions at a pump power of 24 W. With intracavity frequency doubling using a 20-mm-long LBO, a maximum blue output power of 2.25 W is achieved at a repetition rate of 23 kHz. The conversion efficiency from the corresponding Q-switched fundamental output to blue output is 96%. The peak power of the Q-switched blue pulse is up to 610 W with 160 ns pulse width. The fluctuation of the blue output power is less than 4.0% at the maximum output power.     

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.     

Nonlinear optical properties of Au/ZnO nanoparticle arrays

The triangular-shaped Au/ZnO nanoparticle arrays were fabricated on fused quartz substrate using nanosphere lithography. The structural characterization of the Au/ZnO nanoparticle arrays was investigated by atomic force microscopy. The absorption peak due to the surface plasmon resonance of Au particles at the wavelength of about 570 nm was observed. The nonlinear optical properties of the nanoparticle arrays were measured using the z-scan method at a wavelength of 532 nm with pulse duration of 10 ns. The real and imaginary part of third-order nonlinear optical susceptibility, Re χ⁽³⁾ and Im χ⁽³⁾, were determined to be 1.15 × 10⁻⁶ and −5.36 × 10⁻⁷ esu, respectively. The results show that the Au/ZnO nanoparticle arrays have great potential for future optical devices.     

Optimization of optical parametric chirped pulse amplification with different pump wavelengths

Optical parametric chirped pulse amplification with different pump wavelengths was investigated using LBO crystal, at signal central wavelength of 800 nm. According to our theoretical simulation, when pump wavelength is 492.5 nm, there is a maximal gain bandwidth of 190 nm centered at 805 nm in optimal noncollinear angle using LBO. Presently, pump wavelength of 492.5 nm can be obtained from second harmonic generation of a Yb:Sr₅(PO₄)₃F laser. The broad gain bandwidth can completely support ∼6 fs with a spectral centre of seed pulse at 800 nm. The deviation from optimal noncollinear angle can be compensated by accurately tuning crystal angle for phase matching. The gain spectrum with pump wavelength of 492.5 nm is much better than those with pump wavelengths of 400, 526.5 and 532 nm, at signal centre of 800 nm.     

Nonlinear mixing between the emission of a cw laser and a femtosecond laser

We mix the emission of a femtosecond Ti:sapphire laser with the emission of a continuous wave infrared laser in a beta-barium borate crystal. Green light with a center wavelength of 527 nm and a spectral width of 2.5 nm resulting from sum frequency generation is detected. An intensity study verifies that a nonlinear χ⁽²⁾ process is at the origin of the green light generation. The experimentally obtained conversion efficiency of 7 × 10⁻¹⁰ is in good agreement to simple theoretical considerations.     

Theoretical and experimental studies on laser-induced transient gratings in laser dyes

Laser-induced transient grating technique has been used to measure the diffraction efficiency (η) and calculate the third-order nonlinear susceptibility (χ⁽³⁾) of some laser dyes. Theoretical simulations have been carried out on η and χ⁽³⁾ as a function of wavelength covering the spectral range corresponding to the first excited singlet state of the dyes. Theoretically simulated values have been found in agreement to those observed experimentally. The decay profiles for these dyes have been measured by using diffraction of a delayed probe laser pulse to estimate the relaxation times in the excited state.     

Light-induced ultrafast phase transitions in VO2 thin film

Vanadium dioxide shows a passive and reversible change from a monoclinic insulator phase to a metallic tetragonal rutile structure when the sample temperature is close to and over 68 °C. As a kind of functional material, VO₂ thin films deposited on fused quartz substrates were successfully prepared by the pulsed laser deposition (PLD) technique. With laser illumination at 400 nm on the obtained films, the phase transition (PT) occurred. The observed light-induced PT was as fast as the laser pulse duration of 100 fs. Using a femtosecond laser system, the relaxation processes in VO₂ were studied by optical pump-probe spectroscopy. Upon a laser excitation an instantaneous response in the transient reflectivity and transmission was observed followed by a relatively longer relaxation process. The alteration is dependent on pump power. The change in reflectance reached a maximum value at a pump pulse energy between 7 and 14 mJ/cm². The observed PT is associated with the optical interband transition in VO₂ thin film. It suggests that with a pump laser illuminating on the film, excitation from the d_θ,? - state of valence band to the unoccupied excited mixed d_θ,?-π* - state of the conduction band in the insulator phase occurs, followed by a resonant transition to an unoccupied excited mixed d_θ,?-π* - state of the metallic phase band.     

Time resolved magnetic ordering and photo-induced gyrotropy at room temperature in CdMgTe-CdMnTe semiconductor micro-cavities

Using a picosecond pump and probe time-resolved technique we evidence a single pump pulse photo-induced magnetic ordering in a Mn-doped semiconductor magneto-photonic microcavity operating in the strong coupling regime at room temperature. This nanosecond duration magnetization is attributed to a magnetic ordering of the Mn-impurities mediated through photo-generated holes and enhanced through the confinement. It is distinct from the preceding short lived photo-induced spin orientation of carriers also evidenced by our technique for circularly polarized pump beams. The photo-generated magnetic flux density amounts to a 1 kG for beam fluences of few tens μJ cm⁻² and effective Mn concentrations of 5 nm⁻³; large photo-induced magneto-optic Kerr rotations are also evidenced.     

Femtosecond optical Kerr effect study of Ge10As40S30Se20 film

The results of the femtosecond optical heterodyne detection of optical Kerr effect at 805 nm with the 80 fs ultrafast pulses in amorphous Ge₁₀As₄₀S₃₀Se₂₀ film is reported in this paper. The film shows an optical non-linear response of 200 fs under ultrafast 80 fs-pulse excitation, and the values of real and imaginary parts of non-linear susceptibility χ⁽³⁾ were 9.0×10⁻¹² and −4.0×10⁻¹² esu, respectively. The large third-order non-linearity and ultrafast response are attributed to the ultrafast distortion of the electron orbits surrounding the average positions of the nucleus of Ge, As, S and Se atoms. This Ge₁₀As₄₀S₃₀Se₂₀ chalcogenide glass would be expected as a promising material for optical switching technique.     

Z-scan measurements of optical nonlinearity in acid blue 29 dye

The third order nonlinear optical properties of acid blue 29 solutions have been studied using Z-scan technique. Experiments are performed using a CW He–Ne laser at 632.8 nm wavelength and 3 mW power. The linear absorption coefficient α₀, nonlinear absorption coefficient β, nonlinear refractive index n₂, Re χ³, and Im χ³ are measured at three different concentrations. Our results show that higher concentration gives better nonlinear optical properties. Also, it was found that there is an increasing trend in the value of the nonlinear refractive index n₂ as the concentration increases.     

Cascaded compression of the first and second Stokes pulses during forward transient stimulated Raman amplification

The results of numerical modelling of cascaded compression of the first and second Stokes pulses during regenerative regime of the forward transient stimulated Raman amplification are presented for the case when the walk-off length of the first Stokes pulse due to group velocity mismatch is shorter than the length of the nonlinear medium. The influence of the initial amplitudes of the seed first Stokes pulses, its durations and its time delay with respect to the pump pulse, the Kerr nonlinearity of the medium on the conversion efficiency, duration and propagation factor M² of the first and second Stokes pulse are studied. It is demonstrated that for the pump pulse duration of 1 ps the duration of the compressed second Stokes pulses in a KGW crystal near the beam axis may be approximately 14 times shorter than the pump pulse duration. It is shown that the propagation factor of the compressed pulses increases significantly because of complex spatial-temporal dynamics of compression and the influence of Kerr nonlinearity of Raman medium.     

On the distribution of 1550-nm photon pairs efficiently generated using a periodically poled lithium niobate waveguide

We report on efficient generation of 1550-nm photon pairs in a periodically poled lithium niobate waveguide using the spontaneous parametric down-conversion process. Such photon pairs are expected to find applications in fiber-based long-distance quantum communication. Pumping the waveguide with a pulsed semiconductor laser with a pulse rate of 800 kHz and a maximum average pump power of 50 μW, we obtain a coincidence rate of 600 s⁻¹. Despite only two single-photon detectors are used, we gain some information about the photon-number distribution. Our measurements are found to be in agreement with a Poissonian photon-pair distribution, but clearly differ from the expected outcomes for both conventional and two-mode squeezed states, the latter corresponding to a thermal photon-pair distribution. The Poissonian photon-pair distribution is also explained by comparing the coherence time of the pump light and of the detected photons. An average of 0.9 generated photon pairs per pulse can thus be inferred.     

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.