Effect of group velocity dispersion on supercontinuum generation and filamentation in transparent solids

We experimentally investigate the spectral extent and spectral profile of the supercontinuum (SC) generated in transparent solids: barium fluoride, calcium fluoride, and fused silica upon irradiation by intense femtosecond-long pulses of 800, 1,380, and 2,200 nm light. These wavelengths correspond to the normal and anomalous group velocity dispersion (GVD) regimes in fused silica calcium fluoride and barium fluoride. We observe an isolated (anti-Stokes) wing on the blue side most prominently in fused silica but also in CaF₂. The SC conversion efficiency is measured for the long wavelengths used in our experiments. We also present results on filamentation in BaF₂ in the anomalous GVD regime, including visualization of focusing–refocusing events within the crystal; the size of a single filament is also determined. The 15-photon absorption cross section in BaF₂ is deduced to be 6.5 × 10^?190 cm³⁰ W^?15 s^?1.     

Plasma effects and the modulation of white light spectra in the propagation of ultrashort, high-power laser pulses in barium fluoride

We report the results of a study of white light generation in a 7.5 cm long crystal of a high band-gap material, barium fluoride, using ultrashort (<42 fs) laser pulses over a range of values of incident laser power that extend up to more than three orders of magnitude larger than the critical power for self-focusing (P_cr). We explore white light generation and the intensity and spectral distributions within filaments that are formed as a result of the interplay of self-focusing and plasma-induced defocusing. The onset of plasma effects occurs at power levels in excess of 7 GW for ultrashort pulses in BaF₂. For incident power levels that are three orders of magnitude larger than the critical power, blue-shifting of the incident laser wavelength is observed in addition to asymmetric continuum generation. The blue shift enables us to estimate the temporal variation of the electron density in the plasma that is generated within the BaF₂ crystal. PACS 52.38.Hb; 42.65.Jx; 42.65.Tg; 33.80.Wz; 52.35.Mw     

Visualization of focusing–refocusing cycles during filamentation in BaF<Subscript>2</Subscript>

Filamentation occurs within a 1.5 cm-long crystal of BaF₂ during the propagation of intense, ultrashort (40 fs) pulses of 800 nm light; a systematic study as a function of incident power enables us to extract quantitative information on laser intensity within the condensed medium, the electron density and the six-photon absorption cross section. At low incident power, a single filament is formed within the crystal; two or more filaments are observed along the direction transverse to laser propagation at higher incident powers. Further, due to fluorescence from six-photon absorption (6PA), we are able to map the intensity variation in the focusing–refocusing cycles along the direction of laser propagation. At still higher incident powers, we observe splitting of multiple filaments. By measuring the radius (L _min) of single filament inside BaF₂, we obtain estimates of peak intensities (I _max) and electron densities (ρ _max) to be 3.26×10¹³ W cm⁻² and 2.81×10¹⁹ cm⁻³, respectively. Use of these values enables us to deduce that the 6PA cross-section in BaF₂ is 0.33×10⁻⁷⁰ cm¹² W⁻⁶ s⁻¹.     

Nonlinear photoionization and laser-induced damage in silicate glasses by infrared ultrashort laser pulses

We show that photoionization of wide band gap silicate glasses by infrared ultrashort laser pulses can occur without laser-induced damage. Two glasses are studied, fused silica and a multi-component silicate photo-thermo-refractive (PTR) glass. Experiments are performed by low numerical aperture focusing of ultrashort laser pulses (100 fsec<τ<1.5 psec) at the wavelengths 780 nm, 1430 nm, and 1550 nm. Filaments form inside both glasses and are visibly observable due to intrinsic luminescence. Keldysh’s theory of nonlinear photoionization is used to model the formation of filaments and values of about 10¹³ W cm⁻² for the laser intensity and 10¹⁹ cm⁻³ for the free electron density are estimated for stable filaments to arise. Laser-induced damage is studied by the generation of a third harmonic from an interface created between a damage site and the surrounding glass matrix. It is found that third harmonic generation occurs only after several thousands of laser shots indicating that damage is not a single-shot phenomena. The ability to photoionize PTR glass without damage by ultrashort laser pulses offers a new approach for fabricating diffractive optical elements in photosensitive glass.     

Systematic study of highly efficient white light generation in transparent materials using intense femtosecond laser pulses

We report the results of a systematic study of white light generation in different high band-gap optical media (BaF₂, acrylic, water and BK-7 glass) using ultrashort (45 fs) laser pulses. We have investigated the influence of different parameters, such as focal position of the incident laser light within the medium, the polarization state of the incident laser radiation and the pulse duration of the incident laser beam on the white light generation. Our results indicate that for intense, ultrashort pulses, the position of physical focus inside the media is crucial in the generation, with high efficiency, of white light spectra over the wavelength range 400–1100 nm. Linearly polarized incident laser light generates white light with higher intensity in the blue region than circularly polarized light. Ultrashort (45 fs) pulses generate a flatter spectrum with higher white light conversion efficiency than longer (300 fs) pulses of the same laser power. We believe that a flat response over a wide range of wavelengths in the continuum may be efficiently compressed for generation of sub-10 fs pulses. PACS 52.38.Hb; 42.65.Jx; 42.65.Tg; 33.80.Wz; 52.35.Mw     

Direct laser fabrication of blaze gratings in fused silica

Results of our investigations on direct laser fabrication of blaze gratings in fused silica using a special fluorine-laser mask projection technology allowing to produce plane and smooth reflecting areas and optimum blaze geometry will be presented. In particular, it will be shown that gratings with nearly optimum blaze geometry and relatively low surface roughness of the reflecting areas can be produced. The technique is a one-step method and has a high variability with regard to grating geometry and also substrate materials. We use masks made of tantalum foil, projected onto a fused silica substrate surface with a demagnification ratio of 26:1 and also novel scattering masks made of calcium fluoride. In these masks, up to 25 times smaller transmission apertures can be manufactured allowing thus grating constants in the range of a few μm. The average surface roughness of the reflecting areas along a blaze grating line was measured to be R _a=38 nm without any surface smoothing. The maximum variance of the blaze angle within one grating is about 0.5 degree.     

High upconversion optical gain of Er3+-doped tellurite glass

The upconversion technique of rare-earth-doped glasses or crystals is a potential route for achieving short-wavelength lasers (SWLs). The optical gain is an important parameter for evaluating lasing medium performance. Therefore, upconversion luminescence in glass with composition of 70TeO₂–9PbF₂–10AlF₃–10BaF₂–1Er₂O₃ was demonstrated, and the small-signal optical gain was measured via an amplified spontaneous emission technique when the sample was excited with a 980 nm laser. It was found that the optical gain was as large as 4.0 dB/cm, thus indicating that this glass may be a good medium for SWLs.     

Thermally poled fused silica as a second-order autocorrelation crystal

Autocorrelation is one of the most commonly used methods for ultrashort pulses (<1 ps) characterization. Many measurement devices have been made with various nonlinear materials: second-harmonic generation in nonlinear crystals and Langmuir-Blodgett films, fluorescence in fused silica, absorption in semiconductors. We propose the use of a poled fused-silica glass as an autocorrelation crystal. This cheap and robust material can be an interesting alternative for ultrashort pulses autocorrelation.     

104 nm period grating fabrication in fused silica by immersion two-beam interferometric laser induced backside wet etching technique

A substantial extension of the method of two-beam interferometric laser induced backside wet etching (TWIN-LIBWE), the immersion TWIN-LIBWE, is used to fabricate fused silica gratings with a 104 nm period. The spatially filtered fourth harmonic of Nd:YAG laser (λ=266 nm, τ_FWHM=8 ns) pulses were split into two parts which then interfered at the backside of the fused silica target in contact with a liquid absorber (naphthalene methyl methacrylate saturated solution with a concentration of 1.85 mol/dm³). The hypotenuse of a rectangular fused silica prism is attached to the fused silica target with the use of distilled water as the immersion liquid. On steering the beams through the sides of the prisms, the angle between the two laser beams has been substantially increased. The resulting period of 104 nm is the minimal grating constant achievable under such experimental conditions and, to our knowledge, the smallest laser generated grating period in fused silica at present. PACS 42.62; 42.79; 81.65     

Generation of high-energy broadband femtosecond deep-ultraviolet pulses by highly nondegenerate noncollinear four-wave mixing in a thin transparent solid

We present a simple and efficient technique for the generation of ultrashort deep-ultraviolet pulses based on four-wave mixing of noncollinear laser pulses in a thin solid. Sub-30-fs pulses (Fourier-limit of 13 fs) centered at 270 nm, with energies up to 6 μJ, were obtained by mixing the fundamental and the second harmonic of a Ti:sapphire amplifier in fused silica. Temporal characterization was performed with a dispersionless self-diffraction FROG setup. Spectra as broad as 20 nm were also obtained that can in principle support sub-4-fs deep-ultraviolet pulses.The results are well described by two-dimensional numerical simulations.     

Ion implantation effects in glasses

Abstract

Ion implantation can be used to introduce network damage and to alter the chemical composition in glasses. Structural changes can be inferred from IR measurements near 1000 cm^?1 and by optical absorption near 2150 Å. Implantation-induced damage decreases the implanted volume in fused silica with consequent changes in the refractive index, the near-surface hardness, and the tensile surface stress. Prior work in these areas is reviewed. Implantation into alkali silicate glasses depletes the alkali content in the implanted region. These changes allow preferential surface crystallization in Li₂O-2SiO₂ glasses. Crystallization of amorphous SiO2 can be induced by implantation of Li. Insight into the crystallization process is obtained by following the associated ion movement by elastic recoil detection (ERD) and optical techniques. Implantation of 20keV H shows that saturation of implanted H-sites in fused silica occurs at about 2.2 × 10²¹ H/cm³ in agreement with free volume estimates of the maximum number of available interstitial sites. Details of H and D interactions in fused silica were studied as a function of fluence and temperature. Results are of interest in studies of corrosion in glasses considered for nuclear waste encapsulation and for components in fusion reactors.

IV Summary     

Theoretical Investigation of the Electronic and Spatial Structures of the La Impurity in a BaF2 Crystal

The results of theoretical investigations of the electronic structure of BaF₂ and LaF₃ crystals and BaF₂–LaF₃ complexes without and with La impurity are presented. Changes in the structure of the state density, electronic spectrum, and effective charges caused by defects are analyzed. It is demonstrated that the NNN position of the [La³⁺F_i ^-] defect in BaF₂ is more stable than the NN position.     

Intensity-induced nonlinear effects in UV window materials

Intensity-induced nonlinear effects in optical window materials have been investigated at 308 nm. The absolute two-photon absorption coefficients for fused silica, CaF₂, BaF₂, Al₂O₃ and ADP crystals have been measured by using a single 120 ps, transform-limited pulse from the second harmonic of a distributed feedback (DFB) dye laser. The nonlinear refractive index coefficient has been obtained from measurements of far-field intensity distributions.     

Ultrafast laser-induced melting of glass

The interaction of intense femtosecond laser pulses with wide band-gap fused silica and quartz is investigated. It is shown that during target irradiation, melting of SiO₂ occurs. Laser pulses with fluences above the damage threshold induce partial phase transition of fused silicia into quartz and vice-versa. PACS 42.62.-b; 61.46.+w; 81.30.Hd     

Optical properties of Yb3+ ions in fluorophosphate glasses for 1.0 μm solid-state infrared lasers

Yb³⁺-doped fluorophosphate glasses were prepared by melt-quenching technique and characterized their spectroscopic properties to assess the laser performance parameters. The magnitude of absorption (emission) cross-sections at 975 nm for all the studied Yb³⁺-doped glasses is found to be in the range of 0.29–1.50 × 10^?20 (0.59–1.99 × 10^?20 cm²) which is much higher than those of commercial Kigre QX/Yb: 1.06 × 10^?20 (0.5 × 10^?20 cm²) laser glass. The luminescence lifetimes of ²F_5/2 level decrease (1.15–0.45 ms) with increase in Yb₂O₃ concentration (0.1–4.0 mol%). Effect of OH^? content on luminescence properties of Yb³⁺ ions has also been investigated. The effect of radiative trapping has been discussed by using McCumber (McC) and Fuchtbauer–Ladenburge (F–L) methods. The product of experimental lifetimes and emission cross-sections for 0.1 mol% Yb₂O₃-doped glass is found to be 2.28 × 10^?20 cm² ms which indicates that the higher energy storage and extraction capability could be possible. The detailed spectroscopic results suggest that the studied glasses can be considered for high-power and ultrashort pulse laser applications.     

Thermoluminescence and opitical absorption of BaF2 crystals

Abstract

Nominally pure and Dy-doped BaF₂ crystals were investigated concerning their optical absorption (OA) and thermoluminescence (TL) properties. Peaks at 120—150 and 200°C were observed for a heating rate of 1.7°C/s. The TL response for γ-rays and the TL emission spectra were obtained for these peaks. Except for the purest crystal, all BaF₂ crystals produced OA bands before irradiation typical of Ce³⁺ ions. After irradiation, Dy doped crystals showed bands due to Dy²⁺ ions. A nominally pure sample gave bands related to Ce²⁺ ions and photochromic centers of Ce³⁺ ions. and photochromic centres of Ce³⁺ ions. The correlation between some OA bands and TL peaks is discussed.     

Design of a contact grating setup for mJ-energy THz pulse generation by optical rectification

According to the recent calculations, more efficient THz pulse generation is possible using relief grating on the front surface of the generating LiNbO₃ (LN) crystal for tilted-pulse-front-excitation rather than imaging the pump spot on a reflection grating into the LN crystal. Very recently, it was shown that—compared to a free-standing LN surface-relief grating—significantly higher diffraction efficiency can be reached if the grating profiles are filled with fused silica. Since realisation of such a setup is technically very challenging, in the present paper, we analyse the case where the input side of the LN grating is immersed into a refractive index matching liquid (RIML) instead of a solid material. Our results showed that the diffraction efficiency remains above 90?% for a refractive index ranging 1.45–1.60 of the applied RIML, and it is as high as 99?% for using the RIML for BK7. For this case, we carried out detailed calculations for various grating parameters. We propose a practical setup applying tilted input and slightly tilted output surfaces resulting in low losses and high diffraction efficiency for the pump. We conclude that a contact grating setup using BK7 RIML is suitable for producing THz pulses even in the mJ-energy range.     

Photolytical XeF(C–A) laser amplifier of femtosecond optical pulses: gain measurements and pump efficiency

Gain characteristics of a photolytically driven XeF(C–A) laser amplifier are studied experimentally in the unsaturated amplification regime. The gaseous active medium is optically pumped by vacuum-ultraviolet (VUV) radiation from two large-area multichannel surface discharges initiated along opposite walls of the amplifier chamber. A total gain factor of 10² is obtained for the ultrashort optical pulses under multipass amplification in the active volume of 40?×?18?×?4 cm³ dimensions with a spatially homogeneous gain distribution. Spectral measurements reveal a good conservation of the seed pulse spectrum. Small-signal gain reaching 2×10^-3 cm^-1 is observed for the blue-green seed pulses of 150 fs duration, as well as for the continuous seed radiation at 488 nm. The obtained gain values, being compared with the gain calculated for the measured pumping radiation power, indicate that the quantum yield of the XeF(B) formation as a result of the XeF₂ photodissociation is high and approaches unity within the spectral band of the XeF₂ VUV photodissociation continuum.     

Submicrometer grating fabrication in fused silica by interferometric laser-induced backside wet etching technique

Submicrometer period fused silica gratings were produced by two-beam interferometric laser-induced backside wet etching technique (TWIN LIBWE). The fourth harmonic of a Nd:YAG laser beam was spatially filtered in two steps, and the smoothened beam was split into two parts and interfered at incident angles of 60°, 30°, 14°, and 7.7°, respectively, on the backsides of fused silica plates that were in contact with a liquid absorber. The periods of the produced fused silica gratings were, respectively, 154 nm, 266 nm, 550 nm, and 990 nm. In the next step, TWIN-LIBWE setup was completed by using a coupling rectangular prism in order to reach immersion setup, which made possible to fabricate 104 nm period fused silica grating. This is the smallest laser-generated grating constant in fused silica at present. The morphology of the etched gratings was characterized by atomic force microscope. Important parameters (modulation depth, low-pass filtered waviness, quality factor) of the produced gratings were determined. Evolution of the grating parameters was also studied in the 990 nm case: the dependence of modulation depth, waviness, and quality factor on the number of laser pulses was investigated.