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.     

Azimuthal dependence of the two-photon absorption coefficient for CdP2 crystals with tetragonal syngony

We studied the two-photon absorption coefficient (β) for cadmium diphosphide (CdP₂) single crystals in the tetragonal modification vs. the polarization azimuth (φ) of the incident light for intensities close to the optical breakdown (or optical damage) threshold for the crystal (11 MW/cm²). We have established that the value of β_max = 0.16 cm/MW is reached for φ = 0, i.e., for the ordinary wave. At the lasing frequency of a ruby laser, β_⊥/β_|| = 2.13, which suggests anisotropy of the two-photon absorption in the studied crystals. These dependences are needed for design and fabrication of quantum electronics and nonlinear optics elements whose operation is based on the use of the two-photon absorption effect for high radiation fluxes. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 76, No. 1, pp. 117–121, January–February, 2009.     

Nonlinear optical absorption and refraction in Ru, Pd, and Au nanoparticle suspensions

We present the results of studies of the nonlinear optical properties of Pd, Ru, and Au nanoparticles. We studied the nonlinear refraction and nonlinear absorption of suspensions of these nanoparticles at 1064-nm wavelength. A relatively strong nonlinear absorption of the Pd nanoparticles was observed in the case of 1064-nm, 50-ps pulses (β=2×10⁻⁹ m W⁻¹). The Ru and Pd nanoparticles showed weak negative nonlinear refraction (γ∼−(6–8)×10⁻¹⁶ m² W⁻¹) in this spectral range. In the case of the Au nanoparticles, a saturated absorption at 532 nm dominated over other nonlinear optical processes.     

Atomic force microscopy, Raman spectroscopy and nonlinear absorption properties of femtosecond laser irradiated CR-39

Investigations have been performed to explore ultrashort laser irradiation effects on the surface topography as well as structural and nonlinear absorption properties of a polymer CR-39. For this purpose, a CR-39 target was exposed in air to 25 fs, 800 nm Ti:sapphire laser radiation at fluences ranging from 0.25 J cm⁻² to 3.6 J cm⁻². The surface features, structural changes and nonlinear absorption were explored by AFM, Raman Spectroscopy and a Z-scan technique, respectively. Several topographical structures like bumps, explosions and nano cavities have been observed on the irradiated surface. Raman spectroscopy reveals changes in the fundamental structure of the polymer after the irradiation. Nonlinear absorption data contained by the Z-scan technique predict the dominance of three-photon absorption in case of pristine CR-39. Furthermore, nonlinear absorption (three or two photon) increases with increasing laser fluences and is well correlated with surface and structural changes revealed by AFM and Raman spectroscopy.     

Nonlinear optical absorption and refraction of epitaxial Ba0.6Sr0.4TiO3 thin films on (001) MgO substrates

Highly epitaxial Ba_0.6Sr_0.4TiO₃ (BST) ferroelectric thin films were fabricated on (001) MgOsubstrates by pulsed laser deposition. The nonlinear optical absorption coefficients (β) and refraction indices (γ) of the BST thin films on (001) MgO substrates were investigated using the single beam Z-scan technique with femtosecond laser pulses at the wavelengths of 790 nm and 395 nm, respectively, at room temperature. The nonlinear absorption coefficients of BST thin films were measured to be ∼0.087 cm/GW and ∼0.77 cm/GW at 790 nm and 395 nm, respectively. The nonlinear refraction indices of BST thin films exhibit a strong dispersion from a positive value of 6.1×10^-5 cm²/GW at 790 nm to a negative value of -4.0×10^-5 cm²/GW at 395 nm near band gap. The dispersion of γ is roughly consistent with Sheik-Bahae’s theory for the bound electronic nonlinear refraction resulting from the two-photon resonance. These results show that the BST film is a promising material as a candidate for nonlinear optical applications. PACS 42.70.Mp; 78.20.-e; 81.05.-t     

Nonlinear refraction of undoped and Fe-doped KTiOAsO4 crystals in the femtosecond regime

The third-order optical nonlinearities in undoped and Fe-doped KTA crystals have been measured using the Z-scan technique with femtosecond pulses at 780-nm wavelength. The nonlinear refractive index is determined to be 1.7×10⁻¹⁵ cm²/W and 0,9×10⁻¹⁵ cm²/W for undoped and Fe-doped KTA, respectively. No two-photon absorption occurs in these crystals. It is shown that doping with Fe₂O₃ could weaken refractive nonlinearity of KTA, suggesting that Fe:KTA will improve the performance of KTA in high-intensity femtosecond laser applications. In addition, the measured nonlinear index of refraction in KTA crystals is about five times lower than that predicted by the two-band theory. One of the reasons for the discrepancy is given as the applicable limit of the simple theory in which a two-parabolic band model has been assumed in the analysis. Received: 3 June 1999 / Published online: 20 October 1999     

Nonlinear absorption properties correlated with the surface and structural changes of ultra short pulse laser irradiated CR-39

We have investigated femtosecond laser irradiation effects on the surface topography, structural changes and nonlinear absorption properties of CR-39. For this purpose, a CR-39 target was exposed in air to 25 fs, 800 nm Ti: sapphire laser radiation at fluences ranging from 0.25 J cm⁻² to 3.6 J cm⁻². The surface of irradiated CR-39 probed by an Atomic Force Microscope (AFM) exhibits the formation of several topographical structures, like bumps, explosions and nano cavities. Raman spectroscopy is performed to explore chemical and structural modification of the irradiated target. The spectroscopy reveals changes such as cross linking, bond breaking, formation of new bonds etc. in the fundamental structure of the polymer after irradiation. In order to establish a correlation between morphological and structural changes with the changes in the nonlinear absorption of the irradiated CR-39, a Z-scan technique was employed. A comparison of experimentally obtained data from Z-scan measurements with our calculations predicts the dominance of three-photon absorption in the case of pristine CR-39, whereas for irradiated targets concurrence of three- and two-photon absorption is probable. Nonlinear absorption increases with increasing laser fluences and is well correlated by surface and structural changes revealed by AFM and Raman spectroscopy.     

Effect of higher order nonlinear optical processes on optical absorption in the photorefractive BSO and BGO crystals

The processes of nonlinear refraction and nonlinear absorption are studied in the photorefractive Bi₁₂SiO₂₀ (BSO) and Bi₁₂GeO₂₀ (BGO) crystals at a wavelength of a picosecond Nd:YAG laser of 1064 nm. The nonlinear refraction in the crystals is shown to be related to the Kerr effect, and the nonlinear absorption at this wavelength, to three-photon absorption. The three-photon absorption coefficients of the BSO and BGO crystals are equal, respectively, to (2.5±0.8) ×10^?20 and (4.4±1.3) ×10^?20 cm³W^?2.     

Optical absorption in early stage low temperature laser produced plasma

We describe a new technique to measure the UV/visible absorption spectrum of the ablated material during the laser pulse. The technique utilizes the continuum emission from one laser produced plasma as a light source to measure the absorption properties of a second laser produced plasma which is formed on a semi-transparent target with an array of 40 μm holes. A 6 ns, 1064 nm laser was used to ablate a Ag target and the plasma absorption was measured in the range 450–625 nm for a laser fluence of 1 J cm⁻². The total absorption cross-section is (0.5–1.5)×10⁻¹⁷ cm² in the range 450–540 nm. By comparing the measured absorption with a calculation using the plasma spectroscopy code FLYCHK it can be concluded that, in the wavelength region examined here, the absorption is mainly due to bound-bound transitions.     

Dynamics of two-photon picosecond absorption in ZnWO<Subscript>4</Subscript> and PbWO<Subscript>4</Subscript> crystals

A method has been proposed to analyze the dynamics of interband two-photon absorption in a nonlinear medium excited by a sequence of picosecond laser pulses of variable intensity and continuous probe radiation. Induced absorption leading both to hysteresis in the dependence of the absorption on the intensity of laser pump radiation and to the opacity of crystals at the pump wavelength has been revealed in initially transparent ZnWO₄ and PbWO₄ crystals irradiated by a train of 523.5-nm pulses with a duration of 20 ps at pump intensities of 5 to 140 GW/cm². The kinetics of an increase in absorption and its subsequent relaxation at a 523.5-nm picosecond excitation of the crystals have been measured with continuous 633-nm probe radiation. An exponential component of the increase in absorption with the time constant τ = 2−3.5 and 8–9.5 μs depending on the direction of the linear polarization of pump radiation has been revealed at 300 K in ZnWO₄ and PbWO₄ crystals, respectively. The absorption relaxation kinetics in the crystals are complicated and approach an exponential at a late stage with the constant τ = 40−130 and 12–80 ms for the ZnWO₄ and PbWO₄ crystals, respectively.     

Two-photon absorption of high-power picosecond pulses in PbWO<Subscript>4</Subscript>, ZnWO<Subscript>4</Subscript>, PbMoO<Subscript>4</Subscript>, and CaMoO<Subscript>4</Subscript> crystals

The nonlinear process of two-photon interband absorption is studied in tungstate and molybdate oxide crystals excited by a sequence of high-power picosecond pulses with a wavelength of 523.5 nm. The transmission of the crystals is measured for the excitation pulse intensity up to 100 GW/cm². The pulse intensity in the crystals initially transparent at a wavelength of 523.5 nm is strongly limited due to two-photon absorption (TPA), and the reciprocal transmission in PbWO₄ and ZnWO₄ crystals reaches 50–60. In all crystals, TPA induces long-lived one-photon absorption, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the laser excitation intensity. Absorption dichroism manifests itself in a significant difference in the transmission intensities when the principal orthogonal optical axes of the crystals are excited. The TPA coefficients are determined during the excitation of two optical axes of the crystals. TPA coefficients β for the crystals vary over a wide range, namely, from β = 2.4 cm/GW for PbMoO₄ to β = 0.14 cm/GW for CaMoO₄, and the values of β can differ almost threefold when different optical axes of a crystal are excited. Good agreement is achieved between the measured intensities limited by TPA and the estimates calculated from the measured nonlinear coefficients. Stimulated Raman scattering (SRS) upon excitation at a wavelength of 523.5 nm is only detected in two of the four crystals under study. The experimental results make it possible to explain the suppression of SRS by its competition with TPA, and the measured nonlinear coefficients are used to estimate this suppression.     

Effect of ytterbium concentration on cw Yb:YAG microchip laser performance at ambient temperature – Part I: Experiments

The microchip laser performance of Yb:YAG crystals doped with different ytterbium concentrations (C_Yb=10, 15, and 20 at. %) has been investigated at ambient temperature without active cooling of the gain media. Efficient laser oscillation for a 1-mm-thick YAG doped with 10 at. % Yb³⁺ ions was achieved at 1030 and 1049 nm with slope efficiencies of 85% and 81%, correspondingly. The laser performance of heavy-doped Yb:YAG crystals was limited by the thermal population at terminated lasing level and thermal lens effect at room temperature without sufficient cooling of the samples. The laser emitting spectra of Yb:YAG microchip lasers with different Yb concentrations and output couplings are addressed with the local temperature rise, due to the absorption of the pump power inside the gain media under different pump levels. PACS 42.55.Xi; 42.70.Hj; 42.55.Rz     

Nonlinear refraction and absorption in hetero- thiometallic planar clusters

The nonlinear absorption and refraction of the clusters [MoS₄Cu₄Br₂(py)₆] and [Et₄N]₂[MoS₄Cu₄(SCN)₄(2-pic)₄] have been investigated using the z-scan technique with a ns laser at 532 nm wavelength. They have the same planar ‘open’ structures and the same skeleton metal atoms; the only difference is that the former has halogen ligands while the latter possesses pseudo-halogen groups – SCN – as ligands. Alteration of nonlinear refractive index and enhancement of nonlinear absorption were found in these two clusters. A steady state model of excited state nonlinear refraction was proposed to explain this phenomenon. Received: 12 June 2001 / Revised version: 4 September 2001 / Published online: 29 November 2001     

Spectroscopic properties of Pr<Superscript>3 + </Superscript>-doped erbium oxalate crystals

Spectroscopic properties of praseodymium ions-doped erbium oxalate (Er₂(C₂O₄)₃ · nH₂O) crystals have been investigated. The crystals were grown by hydro silica gel method under suitable pH conditions and by single diffusion method. The well-grown crystals are bright and transparent. The dark green colour of these crystals changes with the variation of the concentrations of the dopant ions. The absorption spectra have been measured in the region 200–800 nm at room temperature. Judd–Ofelt intensity parameters for f–f transitions of the Pr³⁺ ions have been determined as Ω₂ = 166.7, Ω₄ = 1.103 and Ω₆ = 2.898. Analyses of the absorption spectra also show a possible energy transfer from the host material to the dopant.     

Influence of impurities and thermal treatment on spectroscopic properties and laser performance of thulium-doped yttrium vanadate crystals

Influence of impurities and thermal treatment on spectroscopic properties and laser performance of thulium-doped yttrium vanadate crystals was examined. YVO₄ crystals nominally pure, single doped with Tm³⁺ and co-doped with Tm³⁺ and Ca²⁺ were grown by the Czochralski method and then thermally treated at 1150 °C for several hours in a reducing atmosphere (vacuum) or oxidizing atmosphere (air). Samples of crystals were investigated by nuclear magnetic resonance spectroscopy (NMR) and by optical spectroscopy methods. Laser performance of samples was examined upon laser diode pumping. For pure YVO₄ and for YVO₄ containing 0.5 at. % of Tm a single-site NMR spectrum of ⁵¹V nuclei was observed with central line widths of 2.5 and 3.2 kHz (FWHM), respectively. For samples containing 5 at. % of Tm the NMR spectrum was a superposition of multi-site spectra indicating at least three kinds of vanadium sites with axial symmetry. Optical absorption spectra did not contain bands that could be ascribed to V⁴⁺ ions in tetragonal sites. Level of matrix absorption in the visible region and its increase with decreasing wavelength from about 600 to 370 nm was found to be substantially dependent on conditions of thermal treatment. Thermal treatment of crystals and additional doping with Ca did not influence the ³ F ₄ lifetime of thulium and laser performance of crystals, however. Infrared absorption spectra revealed OH^- contamination in all samples. It has been concluded that the quenching of the ³ F ₄ emission in samples containing 5 at. % of thulium is related to migration-accelerated energy transfer to hydroxyl ions acting as energy sinks. PACS 42.55.Xi; 42.62.Fi     

Measurements of dynamics of nondegenerate optical nonlinearity in ZnS with pulses from optical parameter generation

We expand the degenerate PO pump-probe technique to nondegenerate field and use it to investigate optical nonlinear dynamics in ZnS single crystal. Excited by 532-nm laser pulses with 21-ps duration, the temporal response of nondegenerate nonlinear absorption and nondegenerate nonlinear refraction are probed by laser pulses from optical parameter generation (OPG) at 600 and 680 nm with pulse width of 10 ps. Based on the theory of free-carrier optical nonlinearity, we study the pure free-carrier refraction in ZnS. By numerically fitting based on the nondegenerate pump-probe theory, the nondegenerate two-photon absorption coefficient, the free-carrier lifetime, the free-carrier absorptive cross section and refractive coefficient at both probe wavelengths are determined respectively. The dispersion of the free-carrier refractive coefficients is discussed.     

Allowance for angular divergence in the generation of the second harmonic in crystals with a regular domain structure

We obtained basic analytical expressions for the efficiency of the second harmonic in nonlinear crystals with a regular domain structure; in these expressions we took into account the angular divergence of the laser beam. The calculation was done in the geometric-optics approximation of the given field of laser radiation. We show that the expressions obtained are similar to the corresponding expressions for homogeneous nonlinear crystals. Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 67, No. 1, pp. 134–138, January–February, 2000.     

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.     

Nonlinear optical and optical limiting studies of alkoxy phthalocyanines in solutions studied at 532 nm with nanosecond pulse excitation

We report our results on the nonlinear optical and optical limiting properties of two alkoxy phthalocyanines namely 2,3,9,10,16,17,23,24-octakis-(heptyloxy) phthalocyanine and 2,3,9,10,16,17,23,24-octakis-(heptyloxy) phthalocyanine zinc(II) studied at a wavelength of 532 nm using 6 ns pulses. Using the standard Z-scan technique we observed that both the phthalocyanines exhibited negative nonlinearity as revealed by the signature of closed aperture data. The magnitude of the nonlinear refractive index n₂ evaluated from the closed aperture data was ∼ 1.61×10^-11 cm²/W for the free-base phthalocyanine and ∼ 1.56×10^-11 cm²/W for the metallic phthalocyanine. Open aperture Z-scan data indicates strong nonlinear absorption in both the phthalocyanines with measured nonlinear coefficients of ∼ 1650 cm/GW and ∼ 1850 cm/GW respectively. We also report optical limiting properties of these phthalocyanines with limiting thresholds (I_1/2) of ∼ 0.5 J/cm². Our studies suggest that these phthalocyanines are one of the best molecules for nonlinear optical applications studied recently. PACS 42.65.-k; 42.70.Jk, 42.65.Jx     

Ultrafast nonlinear absorption and reflection of ZnS/ZnSe periodic nanostructures

ZnS/ZnSe heterostructures under condition of ZnSe interband excitation by a 150 fs laser pulse exhibit strong narrow-band modification of absorption and wide-band modification of reflection. Mean decay time for nonlinear reflection in heterostructures ranges from 2 to 3 ps whereas in bare ZnSe monolayer it exceeds 5 ps. Possible physical processes responsible for nonlinear refraction in the transparency region include interplay of absorption driven nonlinear refraction via Kramers–Kronig relations and intrinsic dielectric properties of dense electron–hole plasma. For nonlinear absorption at ZnSe band edge, interplay of plasma screening effects and states filling effects are relevant.