Structural,optical, and nonlinear optical properties of indium nanoparticles prepared by laser ablation

A study of indium nanoparticles prepared by two laser ablation techniques is reported. The suspensions of indium nanoparticles were prepared using the laser ablation of bulk indium in liquids. The prepared suspensions of indium nanoparticles were analyzed by the X-ray fluorescence spectroscopy and absorption spectroscopy. The position of the surface plasmon resonance of In-containing suspensions (350 nm) was consistent with the estimations taking into account the average size of In nanoparticles (43 nm) measured using the X-ray fluorescence spectroscopy. The nonlinear optical parameters of indium nanoparticles-containing liquids were studied by the z-scan technique using a picosecond Nd:YAG laser. We compare the laser ablation in liquids with the laser ablation of indium in vacuum at the tight and weak focusing conditions of a Ti:sapphire laser and analyze the 60 nm indium nanoparticles synthesized in the latter case. PACS 42.65.An; 42.65.Hw; 42.65.Jx; 61.46.Df; 78.67.Bf     

Synthesis and nonlinear light scattering of microemulsions and nanoparticle suspensions

Microemulsions composed of normal or inverse micellar solutions and aqueous suspensions of pristine (uncoated) or silica-coated iron oxide nanoparticles, mainly γ-Fe₂O₃, were synthesised and their optical limiting properties investigated. The microemulsions are colorless solutions with high transparency for visible wavelengths while the aqueous suspensions of iron oxide are of pale yellow colour. Optical limiting experiments performed in 2 mm cells using a f/5 optical system with a frequency doubled Nd:YAG laser delivering 5 ns pulses with 10 Hz repetition rate, showed clamping levels of ∼3 μJ for the suspensions of both pristine and silica-coated iron oxide nanoparticles. A strong photoinduced nonlinear light scattering was observed for the water-in-oil microemulsion and the aqueous suspensions of nanoparticles while oil-in-water microemulsions did not show a significant nonlinear effect. Measurements carried out using an integrating sphere further verified that the photoinduced nonlinear light scattering is the dominating nonlinear mechanism while the nonlinear absorption of iron oxide nanoparticles is negligible at 532 nm.     

Characterization of the nonlinear refractive index of the laser crystal Yb:KGd(WO<Subscript>4</Subscript>)<Subscript>2</Subscript>

We present results of the characterization of the nonlinear refractive index of the laser crystal Yb:KGd(WO₄)₂ using a z-scan technique over the 800–1600 nm wavelength range. Based on our experimental and theoretical results we conclude that Yb:KGW crystal is a good candidate for efficient Kerr-lens mode locking. PACS 42.65.An; 42.65.Hw; 42.55.Rz; 42.65.Re     

Nonlinear optical properties of gold nanoparticles dispersed in different optically transparent matrices

The nonlinear optical properties of gold nanoparticles dispersed in optically transparent matrices Al₂O₃, ZnO, and SiO₂ are investigated using the classical and off-axis techniques of the Z-scan method at a wavelength of 532 nm (radiation from a nanosecond Nd: YAG laser). The experimental data on the nonlinear refraction in composite materials are obtained. The nonlinear refractive indices and the light absorption coefficients are determined, and the real and imaginary parts of the third-order nonlinear susceptibility for the structures under investigation are calculated. It is demonstrated that, for the composite materials under consideration, the nonlinear properties of the medium under the chosen conditions of laser irradiation are predominantly determined by the Kerr effect and the contribution of this effect exceeds the contribution of the thermal lens.     

Giant nonlinear optical response of nanoporous anatase layers

A giant nonlinear optical response has been observed for nanoporous layers of titanium dioxide (anatase) under picosecond laser excitation with photon energy below the gap. At excitation intensity of 10 MW/cm² the nonlinear refractive index variation at the wavelength of 1064 nm corresponds to ⁽³⁾=2×10^-5 esu which is six orders of magnitude higher than the respective value of bulk TiO₂. This effect is explained by resonant excitation of electronic states of defects at the developed surface of anatase nanoparticles. PACS 42.65.-k; 73.20.At; 78.67.Bf; 81.07.Bc     

Short pulse Z -scan investigations of optical nonlinearities of a novel organometallic complex: [(C2H5)4N]2[Cu(dmit)2] at 532 and 1064?nm

A novel dmit organometallic complex: [(C₂H₅)₄N]₂[Cu(dmit)₂] (dmit^2-=1,3-dithiole-2-thione-4,5-dithiolate), abbreviated as EtCu, was synthesized. Afterwards its optical nonlinearities in acetone solution at 532 nm and 1064 nm were studied by the Z-scan technique with laser pulses of picosecond duration. The two-photon absorption at 1064 nm and the saturable absorption at 532 nm were observed. The Z-scan curves also revealed that EtCu sample solutions exhibited self-defocusing effects at both wavelengths. The origins were analyzed for the differences between the results. All the outcomes suggest that this material is potential for nonlinear optical device applications. PACS 42.65.An; 42.65.Hw; 42.65.Jx; 81.20.Ka; 78.30.Jw     

Nonlinear refractive properties of Yb3+-doped KY(WO4)2 and YVO4 laser crystals

The nonlinear refractive indices of Yb³⁺: KY(WO₄)₂ and Yb³⁺:YVO₄ laser crystals are characterized using a Z-scan technique at a wavelength of 1.08 μm for different polarizations. The results reveal that the nonlinear refractive index of Yb³⁺:YVO₄ is superior to that of Yb³⁺:KY(WO₄)₂ and is found to be 1.9×10^-15 cm²/W and 1.5×10^-15 cm²/W for E⊥c and E∥c polarizations, respectively. PACS 42.65.Hw; 42.55.Rz; 42.65.Re; 42.70.Hj     

Femtosecond laser-induced nonlinear spectroscopy for remote sensing of methane

Femtosecond laser-induced nonlinear molecular spectroscopy is applied for sensing atmospheric greenhouse gas methane (CH₄). The high intensity inside the Ti-sapphire femtosecond laser filaments can dissociate the CH₄ molecules into small fragments which emit characteristic fluorescence. Backward CH radical fluorescence is used to quantitatively analyze the pollutant concentration and its remote detection limit. PACS 42.68.Wt; 42.65.Jx; 95.75.Fg     

Investigation of the spatial profile of stimulated Raman scattering beams in D<Subscript>2</Subscript> and H<Subscript>2</Subscript> gases using a pulsed Nd:YAG laser at 266 nm

The stimulated Raman scattering (SRS) beam spatial mode structure is studied in H₂ and D₂ gases, in a 60 cm-long high-pressure Raman cell, using a pulsed Nd:YAG laser at 266 nm. The conversion efficiencies of the first and second Stokes in H₂, D₂ and H₂/D₂ mixtures have been measured precisely in the 1–14 atm range. The SRS beam profiles were recorded for different gas pressures in the high-pressure Raman cell and interesting behaviour is revealed. Homogeneous SRS spatial profiles were obtained only for pressures higher than 7 atm. For lower pressures the profiles are either in the form of a ring or of a more complicated shape. The results are explained in terms of nonlinear self-focusing processes during the pump beam propagation in the Raman cell. Also, from our measurements, a more precise value of the nonlinear index of refraction for the H₂ and D₂ at 266 nm is proposed. PACS 42.65.Dr; 42.60.Jf; 42.60.Lh; 42.65.Jx     

Optical and nonlinear optical characteristics of the Ge and GaAs nanoparticle suspensions prepared by laser ablation

The laser ablation of Ge and GaAs targets placed in water and ethanol was carried out using the fundamental radiation of nanosecond Nd:YLF laser. The results of preparation and the optical and nonlinear optical characterization of the Ge and GaAs nanoparticle suspensions are presented. The considerable shift of the band gap energy of the nanoparticles compared to the bulk semiconductors was observed. The distribution of nanoparticle sizes was estimated in the range of 1.5-10 nm on the basis of the TEM and spectral measurements. The nonlinear refractive indices and nonlinear absorption coefficients of Ge and GaAs nanoparticles were defined by the z-scan technique using second harmonic radiation of picosecond Nd:YAG laser (λ = 532 nm).     

A novel optical limiting coordination polymer with ladder-like framework

The optical limiting (OL) properties of a novel coordination polymer {[Et₄N][Ag₂I₃]}_n with a ladder-like framework were investigated using 532-nm nanosecond laser pulses. The coordination polymer in dimethylformamide solution exhibits better OL performance than C₆₀ in toluene. The results were discussed using a phenomenological model based on excited-state nonlinear absorption. PACS 42.70.Mp; 42.65.-k; 42.70.Hj; 36.20.Hb     

Studies of the second-order nonlinear optical properties of cubic boron nitride

Cubic boron nitride (cBN) is a kind of artificial wide-energy-gap semiconductor crystal, which has zinc blende structure with Td symmetry. The second-order nonlinear optical properties of cBN single crystal were investigated for the first time. Using a Q-switching Nd:YAG laser, the optical rectification and the second-harmonic generation at 532 nm from cBN single crystal were observed. In order to determine the nonlinear optical coefficient of a minute-size cBN sample, a simple method based on modified transverse linear electro-optic modulation was also introduced. This approach is convenient because it is unnecessary to know the absolute intensity of a probing beam for measuring the half-wave voltage of a cBN sample. Finally, cBN’s linear electro-optic coefficient γ₄₁=1.07×10^-14 m/V and nonlinear optical coefficient d₁₄(0,ω,-ω)=1.07×10^-13 m/V were obtained. PACS 42.65.An; 42.65.Ky; 78.20.Jq     

Linear and nonlinear optical properties of yttrium formate dihydrate,Y(HCOO)<Subscript>3</Subscript>·2H<Subscript>2</Subscript>O

Yttrium formate dihydrate, Y(HCOO)₃·2H₂O (point group 222), a promising new material for Raman laser frequency converters, has been reinvestigated with respect to the linear and nonlinear optical (second-harmonic generation, SHG) properties. High-precision data of refractive indices and their dispersion in the wavelength range 365–1083 nm are given, together with the three independent components of the tensor of nonlinear optical susceptibility (SHG) [d_ijk ^SHG]. A calculation of the macroscopic nonlinear optical susceptibility from the hyperpolarizabilities of the formate groups results in good agreement with the experimental values. This signals that the nonlinear optical interaction in Y(HCOO)₃·2H₂O can mainly be attributed to the formate groups. PACS 42.65.Ky; 42.70.Mp; 78.20.Ci     

Room temperature femtosecond optical parametric generation in MgO-doped stoichiometric LiTaO3

We demonstrate room temperature femtosecond optical parametric generation with high average output power in periodically poled MgO-doped stoichiometric LiTaO₃. Direct pumping with 725-fs pulses from a passively mode-locked thin disk laser at 1030 nm resulted in stable 1.5 W average signal power at 1484 nm at the full laser repetition rate of 59 MHz. With this demonstration we achieved a significant simplification of our recently presented red-green-blue laser source because no temperature stabilization of any nonlinear crystal is required. PACS 42.65.Yj; 42.70.Mp; 42.79.Nv     

Quasi-phase matching in LiNbO3 using nonlinear coefficients in the XY plane

We report quasi-phase-matched second-harmonic generation in periodically poled lithium niobate (PPLN), where both fundamental and second-harmonic waves are ordinary waves. It provides a lower-limit value for d₂₂ of 1.1 pm/V. The measured temperature and wavelength bandwidth of the second-harmonic signal are in good agreement with the theoretical predictions. Since the d₂₂=d_YYY nonlinear coefficient of LiNbO₃ changes its sign as a result of electric field periodic poling along the Z direction, we deduce that all tensor components of the second-order susceptibility χ⁽²⁾ of trigonal 3m crystals are reversed, thereby expanding the quasi-phase-matching possibilities in these crystals. Furthermore, it enables the realization of all-optical processes based on the nonlinear coefficients in the XY plane, such as all-optical polarization rotation in PPLN, as well as multipartite entanglement experiments based on simultaneous phase matching using different elements of χ⁽²⁾ in a single LiNbO₃ crystal. PACS 42.65.-k; 42.65.Ky; 42.65.Lm     

Stimulated Low-Frequency Raman Scattering in LaF<Subscript>3</Subscript> Suspensions

We observe stimulated low-frequency Raman scattering (SLFRS) caused by laser pulse interaction with acoustic vibrations of nanoparticles in water suspensions of LaF₃ nanoparticles. We show that frequency shifts of the scattering correspond to the eigenfrequencies of nanoparticles vibrations. LaF₃ nanoparticles were synthesized in the presence of glycine by a double jet precipitation technique at various initial concentrations of reagents. We investigate the morphologies and particle sizes as well as size distributions of the particles prepared using transmission electron microscopy (TEM) and dynamical light scattering (DLS). In view of the absorption spectroscopy, we show that the reaction system components and products have no absorption in the visible region, including λ = 694.3 nm. From the luminescence spectroscopy, we find also that they do not emit at λ = 694.3 nm excitation.     

Origins of waveguiding in femtosecond laser-structured LiNbO<Subscript>3</Subscript>

Femtosecond laser-induced structural changes in LiNbO₃ are studied. Depending on the laser processing parameters two different types of modification are identified and their origin is discussed. Both types of modification can be described within the framework of induced lattice defects. For strong material damage a refractive index increase can be obtained due to the induced stress field. By appropriate tailoring of this stress field thermally stable and highly symmetric waveguides can be obtained well suited for nonlinear integrated-optical applications. PACS 61.80.Ba; 77.84.Dy; 42.65.Re; 42.82.Et     

Bismuth triborate (BiB3O6) optical parametric oscillators

We report the phase matching of parametric frequency conversion in the nonlinear material BiB₃O₆ (BiBO) and on an investigation of optical parametric oscillators (OPOs) of this new crystal. Based on the calculation of collinear type I and type II phase matching within the refractive-index planes, the most favorable directions for phase matching are identified for OPOs pumped by the fundamental or the harmonics of 1064-nm Nd-doped lasers. Based on these results, pulsed 532-nm-pumped ns OPOs are realized. The pump source is either a Q-switched high repetition rate (10 kHz) Nd:YVO₄ laser (with a pulse energy of 24 J) or a low repetition rate (10 Hz), high pulse energy (120 mJ) Nd:YAG laser system. The BiBO OPO pumped by the Nd:YVO₄ laser showed a very low threshold of 0.047 J/cm². At an average pump power of 2.4 W the total OPO output power was 630 mW. By changing the phase-matching angle within the yz plane from 0 to 11.6° the signal wavelength was tuned from 735 nm to 970 nm, while the spectral width changed from 0.2 nm to 1.4 nm. By pumping the OPO with the Nd:YAG laser, the OPO had a threshold of 0.12 J/cm², a steep slope (59%) and a high total efficiency (of up to 48%). Due to divergence broadening the spectral width changes from 8.5 nm at 800 nm to 70 nm near degeneracy. The properties of BiBO determined from the experimental results are compared with those of well-known nonlinear materials such as BBO, LBO and KTP. PACS 42.65.-k; 42.65.Yj; 42.70.-a; 42.70.Mp     

Pulsed laser induced synthesis of scheelite-type colloidal nanoparticles in liquid and the size distribution by nanoparticle tracking analysis

Pulsed laser ablation (PLA) of ceramic target in liquid phase was successfully employed to prepare calcium tungstate (CaWO₄) and calcium molybdate (CaMoO₄) colloidal nanoparticles. The crystalline phase, particle morphology and optical property of the colloidal nanoparticles were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and Raman spectroscopy. The produced stable colloidal suspensions consisted of the well-dispersed nanoparticles showing a spherical shape. The mechanism for the laser ablation and nanoparticle forming was discussed under consideration of photo-ablation process. Nanoparticle tracking analysis using optical microscope combined with image analysis was proposed to determine the size distribution function of the prepared colloidal nanoparticles. The mean size of the CaWO₄ and CaMoO₄ colloidal nanoparticles were 16 and 29 nm, with a standard deviations of 2.1 and 5.2 nm, respectively.     

Influence of phase transitions on the second harmonic generation in metal nanoparticles

In this work we use nonlinear optical properties of Ga nanoparticles monolayers of different average sizes embedded in dielectric matrices to investigate the liquid-solid phase transitions in these materials. Ga nanoparticles, formed by exploiting the partial wetting of liquid Ga over a SiO_x surface are irradiated with fs laser pulses from a Ti:sapphire source. The resulting Second Harmonic (SH) generated in the reflection and transmission directions is measured along the phase transitions by cooling the sample from 320 K down to liquid nitrogen temperature. Hysteresis cycles are observed in the nonlinear transmission, which exhibit a strong amplification from the solid to liquid values as compared to the linear optical results. A simple model for SH generation, based on Mie scattering calculations which includes the effect of surface plasmon resonance provides a fair key for the interpretation of the observed effects.