Enhanced soft X-ray emission from carbon nanofibers irradiated with ultra-short laser pulses

A comparative experimental study of the X-ray emission in the water-window spectral region has been performed using carbon nanofibers (CNFs) of different sizes and graphite plate targets, irradiated with ultra-short (Ti:sapphire) laser pulses. More than an order of magnitude enhancement in the X-ray yield is observed from CNFs of 60-nm diameter with respect to graphite targets. The X-ray emission from CNFs of 160-nm diameter was also high. The integrated X-ray yield of these carbon-based targets scales with the laser intensity (I _L) as I_L ^{~ 1.3-1.4}I_{\mathrm{L}}^{\sim 1.3-1.4} in the intensity range of 4×10¹⁶–4×10¹⁷ W/cm². The effect of the laser pulse duration on the X-ray emission from the CNFs was also studied by varying the pulse duration from 45 fs up to 3 ps at a constant fluence of 2×10⁴ J/cm². The optimum laser pulse duration for maximum X-ray emission increases with the diameter of the CNFs used. The results are explained from physical considerations of heating and hydrodynamic expansion of the CNF plasma in which resonance field enhancement takes place while passing through two times the critical density. The results add to the efforts towards achieving an efficient low-cost water-window X-ray source for microscopy.     

Excitation of X rays by electrons accelerated in air in the wake wave of a laser pulse

The characteristics of X rays of a laser plasma generated in the interaction of a femtosecond pulse with solid targets in an air atmosphere have been investigated. It has been shown that the mechanism for the generation of X rays in the interaction of short intense laser pulses with solid targets in a gas atmosphere is attributed to the generation of fast electrons in the region of the filamentation of a laser pulse. It has been proven experimentally that under such conditions, the solid target irradiated by laser radiation of even a low density of about 10¹⁵ W/cm² very efficiently emits ∼10-keV photons. It has been shown theoretically that the maximum energy of accelerated electrons can reach ɛ_max ∼ 100–200 keV under these conditions. This means that the proposed method can provide characteristic radiation with the energy of photons much higher than 10 keV.     

Mid-infrared laser-induced grating experiments of C2H4 and NH3 from 0.1–2 MPa and 300–800 K

Laser-induced thermal gratings (LITG) were generated in mixtures of ethylene and ammonia in nitrogen using mid-infrared laser radiation from a grating-tuned, low-pressure, pulsed (5 ms pulse width) CO₂ laser, and read out with a continuous wave Nd:YLF laser. The LITG signal intensity was measured as a function of pressure (0.1–2 MPa) and temperature (300–800 K, at 0.1 and 1 MPa) by tuning the laser to the accidental coincidences of the 10P(14) and 10R(6) emission lines with molecular absorption transitions of C₂H₄ and NH₃, respectively. Comparisons are made with theoretical predictions for the grating efficiency from a simple thermalization model. A theoretical comparison of the temporal LITG signal response for three excitation pulse shapes – a delta function, a realistic pulse, and a square wave is presented. Furthermore, it is shown that for NH₃, most of the decrease of the LITG signal intensity with increasing temperature is due to the corresponding decrease in fractional molecular absorption of the pump beam radiation. The diagnostic capabilities of the mid-infrared LITG experiment is demonstrated for spatially resolved ethylene measurements with long laser pulses in a premixed stoichiometric CH₄–air flame at atmospheric pressure. Received: 17 March 2000 / Revised version: 23 March 2000 / Published online: 13 September 2000     

Dielectric breakdown of rubber materials by femtosecond irradiation

We report the reversible micro-structuring of a synthetic rubber polymer (cis1,4-polybutadiene (PB)) by femtosecond laser illumination. Visco-elastic relaxation of the optically damaged region was observed. The recovery time, typically 10²–10⁴ ms, can be varied by changing the irradiation pulse energy. Multi-shot-induced damage recovers on the much longer scale of 10¹–10² s. It was found that the doping of PB by 4 wt. % of pentazadiene ([4-NO₂]–phenyl–N=N–N(C₃H₇)–N=N–phenyl–[4-NO₂]) reduces the threshold of light-induced photo-modification by 20%. This is explained by photo-induced (homolytic) cleavage of the pentazadiene bonds and formation of gaseous N₂, which facilitates material failure at the irradiated spot. The recovery of optical transmission can be applied to optical memory, optical and micro-mechanical applications. The underlying mechanism of the phenomenon is discussed in terms of anelastic α- and β-relaxation (polymer backbone and chains/coils relaxation, respectively). Received: 11 October 2001 / Accepted: 9 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +81-88/656-7598, E-mail: misawa@eco.tokushima-u.ac.jp     

Corrugated neat thin-film conjugated polymer distributed-feedback lasers

Wave-guided thin-film distributed-feedback (DFB) polymer lasers are fabricated by spin coating a PPV-derived semiconducting polymer, thianthrene-DOO-PPV, onto oxidised silicon wafers with corrugated second-order periodic gratings. The gratings are written by reactive ion beam etching. Laser action is achieved by transverse pumping with picosecond laser pulses (wavelength 347.15 nm, duration 35 ps). The DFB-laser surface emission and edge emission are analysed. Outside the grating region the polymer film is used for comparative wave-guided travelling wave laser (amplified spontaneous emission (ASE)) studies. The pump pulse threshold energy density for wave-guided DFB-laser action (4–9 μJ cm^-2) is found to be approximately a factor of two lower than the threshold for wave-guided travelling wave laser action. The spectral width of the DFB laser (down to Δλ_DFB≈0.07 nm) is considerably narrower than that of the travelling wave laser (Δλ_TWL≈14 nm). The DFB-laser emission is highly linearly polarised transverse to the grating axis (TE mode). Only at high pump pulse energy densities does an additional weak TM mode build up. The surface-emitted DFB-laser radiation has a low divergence along the grating direction. For both the DFB lasers and the travelling wave lasers, gain saturation occurs at high excitation energy densities. Received: 7 January 2002 / Revised version: 15 February 2002 / Published online: 14 March 2002     

The dependence of the Fe <Emphasis Type="Italic">K</Emphasis><Subscript><Emphasis Type="BoldItalic">α</Emphasis></Subscript> yield on the chirp of the femtosecond exciting laser pulse

The hard X-ray yield generated with femtosecond laser pulses is studied for differently chirped irradiating laser pulses. The radiation of a Ti:sapphire CPA laser system (29 fs, 750 μJ, 1 kHz) is focused onto an iron containing solid state target producing incoherent hard X-ray radiation, Bremsstrahlung as well as target-specific K_α and K_β lines. The hard X-ray yield has been optimized by introducing negative and positive group delay dispersion (GDD) and third order dispersion (TOD) to the femtosecond laser pulse. The K_α yield could be enhanced by a factor of 1.7 and reached 1.9×10⁸ Fe K_α photons/s in 4π with the laser pulse positively chirped, and 1.5×10⁸ Fe K_α photons/s with the pulse negatively chirped. When the pulse energy is lowered to about 400 μJ the yield maximum at negative chirp vanishes and only the maximum at positive chirp remains. We explain this behavior with an increased electron temperature caused by the induced GDD and TOD in the pulse. PACS 42.65.Re; 52.38.Ph; 52.50.Jm     

Convergent-beam diffraction of ultra-short hard X-ray pulses focused by a capillary lens

We report the generation of diffraction patterns using X-ray pulses from a fs-laser plasma focused by an X-ray capillary lens to a spot size smaller than 100 μm. A thin moving iron tape is irradiated at 10 Hz with 200 mJ/130 fs titanium–sapphire laser pulses. [ _Fe]Kα (λ=0.194 nm) radiation emitted from the rear side of the tape is focused to a spot by the capillary lens resulting in an intensity enhancement of about 1600. The ability of this system to effectively allow diffraction from samples of micron size is demonstrated by producing well-illuminated diffractograms from a Si(111) crystal with good signal to noise ratio obtained in only about 10 s. The different path lengths of propagation in the lens induce an angle-encoded delay of the converging X-ray pulse and thus provide the possibility of realizing a novel ultra-fast streak camera. PACS 52.59.Px; 52.38.Ph; 41.50.+h; 61.10.Nz     

CO2 laser-induced crystallization of sol–gel-derived indium tin oxide films

Indium tin oxide (ITO) thin films prepared by the sol–gel method have been deposited by the dip-coating process on silica substrates. CO₂ laser is used for annealing treatments. The electrical resistivity of sol–gel-derived ITO thin films decreased following crystallization after exposure to CO₂ laser beam. The topological and electrical properties of the irradiated surfaces have been demonstrated to be strongly related to the coating solution and to the laser processing parameters. Optimal results have been obtained for 5 dip-coating layers film from 0.4 mol/l solution irradiated by 0.6 W/m² laser power density. In this case, homogeneous and optically transparent traces were obtained with a measured sheet resistance of 1.46×10² Ω/□.     

Near IR laser light visualizators using nonlinear GaSe and other layered crystallites

Two methods of preparation of the devices for visualization of pulsed and continuous near-IR (near infrared) are described and the results of conversion of pulsed and continuous IR (800–1360 nm) laser radiation into the visible range of spectra (400–680 nm) by using a transparent substrate covered with the particles (including nanoparticles) of effective nonlinear materials of GaSe _x S_{1 − x} (0.2 ≤ x ≤ 0.8) are presented. Converted light can be detected in transmission or reflection geometry as a visible spot corresponding to the real size of the incident laser beam. Developed device structures can be used for checking if the laser is working or not, for optical adjustment, for visualization of distribution of laser radiation over the cross of the beam and for investigation of the content of the laser radiation. Low energy (power density) limit for visualization of the IR laser pulses with 2–3 ps duration for these device structures are: between 4.6–2.1 μJ (3 × 10⁻⁴−1 × 10⁻⁴ W/cm²) at 1200 nm; between 8.4–2.6 μJ (4.7 × 10⁻⁴−1.5 × 10⁻⁴ W/cm²) at 1300 nm; between 14.4–8.1 μJ (8.2 × 10⁻⁴–4.6 × 10⁻⁴ W/cm²) at 1360 nm. Threshold damage density is more than 10 MW/cm² at λ = 1060 nm, pulse duration τ = 35 ps. The results are compared with commercially existing laser light visualizators.     

Synchrotron investigations of electronic and atomic-structure peculiarities for silicon-oxide films’ surface layers containing silicon nanocrystals

Films obtained using molecular-beam deposition of SiO powder on c-Si (111) substrates for the purpose of SiO2 system formation with silicon nanocrystals were investigated before and after 900–1100°C annealing by photoluminescence, ultrasoft X-ray emission spectroscopy, X-ray photoelectron spectroscopy, X-ray absorption near-edge structure spectroscopy, and X-ray diffraction. The appearance of (111)-oriented luminescent silicon nanoclusters in considerable amounts upon annealing at T = 1000–1100°C is established in the investigated films. An anomalous phenomenon of X-ray absorption quantum yield intensity reversal for the L _2,3 elementary silicon edge is detected. Models for this phenomenon are suggested.     

Femtosecond laser plasma in CaF<Subscript>2</Subscript> crystal microchannel and effective generation of characteristic X-ray radiation

The dependence of the characteristic X-ray radiation yield from CaF₂ crystal on the formed microchannel depth under highly intensive (I ∼ 3 × 10¹⁵ W/cm²) laser pulses with different contrast was obtained. The maximum of the characteristic X-ray radiation yield at these experimental conditions corresponded to the microchannel depth of 30–50 μm. The efficiency of the laser radiation conversion to the characteristic X-ray radiation increased from 6 × 10⁻⁸ for the surface up to 10⁻⁷ in the microchannel. The dependence of the characteristic X-ray radiation yield on the viewing angle showed that the source of X-ray radiation was located near the surface inside the microchannel.     

A comparative study of the ionic keV X-ray line emission from plasma produced by the femtosecond,picosecond and nanosecond duration laser pulses

We report here an experimental study of the ionic keV X-ray line emission from magnesium plasma produced by laser pulses of three widely different pulse durations (FWHM) of 45 fs, 25 ps and 3 ns, at a constant laser fluence of ∼1.5 × 10⁴ J cm^− 2. It is observed that the X-ray yield of the resonance lines from the higher ionization states such as H- and He-like ions decreases on decreasing the laser pulse duration, even though the peak laser intensities of 3.5 × 10¹⁷ W cm^− 2 for the 45 fs pulses and 6.2 × 10¹⁴ W cm^− 2 for the 25 ps pulses are much higher than 5 × 10¹² W cm^− 2 for the 3 ns laser pulse. The results were explained in terms of the ionization equilibrium time for different ionization states in the heated plasma. The study can be useful to make optimum choice of the laser pulse duration to produce short pulse intense X-ray line emission from the plasma and to get the knowledge of the degree of ionization in the plasma.     

Table-top kHz hard X-ray source with ultrashort pulse duration for time-resolved X-ray diffraction

The interaction of ultrashort laser pulses with solid state targets is studied concerning the production of short X-ray pulses with photon energies up to about 10 keV. The influence of various parameters such as pulse energy, repetition rate of the laser system, focusing conditions, the application of prepulses, and the chirp of the laser pulses on the efficiency of this highly nonlinear process is examined. In order to increase the X-ray flux, the laser pulse energy is increased by a 2nd multipass amplifier from 750 μJ to 5 mJ. By applying up to 4 mJ of the pulse energy a X-ray flux of 4×10¹⁰ Fe K _α photons/s or 2.75×10¹⁰ Cu K _α photons/s are generated. The energy conversion efficiency is therefore calculated to η _Fe≈1.4×10⁻⁵ and η _Cu≈1.0×10⁻⁵. The X-ray source size is determined to 15×25 μm². By focusing the produced X-rays using a toroidally bent crystal a quasi-monochromatic X-ray point source with a diameter of 56 μm×70μm is produced containing ≈10⁴ Fe K _α1 photons/s which permits the investigation of lattice dynamics on a picosecond or even sub-picosecond time scale. The lattice movement of a GaAs(111) crystal is shown as a typical application.     

Selective infrared multiphoton dissociation of molecules in a pulsed gasdynamic flow of small extent

The isotopically selective IR multiphoton dissociation of molecules (here CF₃I) in a pulsed gasdynamic flow of small extent (the length of the flow in space is Δx _fl⩽1 cm) is investigated under conditions such that the entire flow is irradiated by high-intensity IR laser radiation. The use of a flow of small extent permits achieving high dissociation yields of resonantly excited molecules in the entire volume of the flow and thus to obtain a highly enriched residual gas in one radiation cycle. The method described gives a 400-fold enrichment of the residual gas in the isotope ¹³C when a pulsed molecular flow of CF₃I of natural isotopic composition is irradiated by just a single laser pulse. The dissociation yield in this case is practically unity, and the selectivity α⩾10. Zh. Tekh. Fiz. 69, 35–41 (January 1999)     

Morphology and composition on Al surface irradiated by femtosecond laser pulses

We study the surface chemicals and structures of aluminum plates irradiated by scanning femtosecond laser pulses in air for a wide range of laser fluence from 0.38 to 33.6 J/cm². X-ray photoelectron spectroscopy and X-ray diffraction analyses indicate clearly that crystalline anorthic Al(OH)₃ is formed under femtosecond laser pulse irradiation. Besides aluminum hydroxide, crystalline Al₂O₃ is also found in the samples irradiated at high laser fluence. Field emission scanning electron microscopy demonstrates that the surfaces of the samples irradiated with low laser fluence are colloidal-like and that nanoparticles with a few nanometers in size are embedded in glue-like substances. For high laser fluence irradiated samples, the surfaces are highly porous and covered by nanoparticles with uniform size of less than 20 nm.     

Growth and use of metal nanocrystal assemblies on high-density silicon nanowires formed by chemical vapor deposition

In this paper, we describe the growth and potential application of metal nanocrystal assemblies on metal-catalyzed, CVD-grown silicon nanowires (SiNWs). The nanowires are decorated by chemical assembly of closely spaced (1–5 nm) Ag (30–100 nm diameter) and Au (5–25 nm diameter) nanocrystals formed from solutions of AgNO₃ and NaAuCl₄·2H₂O, respectively. The formation and growth of metal nanocrystals is believed to involve the galvanic reduction of metal ions from solution and the subsequent oxidation of available Si-hydride sites on the surfaces of the nanowires. A native oxide layer suppresses formation of metal nanocrystals; adding HF to the ionic solutions significantly increases the density of nanocrystals on the surfaces of the nanowires. The nanocrystals coating the nanowires were characterized by X-ray photoelectron spectroscopy, scanning electron microscopy, and X-ray diffraction. Ag nanocrystals on the nanowires afford sensitive detection of Rhodamine 6G (R6G) molecules in the 100 picomolar–micromolar range by surface enhanced Raman spectroscopy. In addition, Au nanocrystals formed on selected surfaces of a substrate of arbitrary shape can serve as effective nuclei for localized nanowire growth. PACS 81.07.b; 81.15.Gh     

Formation of conical microstructures upon laser evaporation of solids

The formation and development of the large-scale periodic structures on a single crystal Si surface are studied upon its evaporation by pulsed radiation of a copper vapor laser (wavelength of 510.6 nm, pulse duration of 20 ns). The development of structures occurs at a high number of laser shots (∼10⁴) at laser fluence of 1–2 J/cm² below optical breakdown in a wide pressure range of surrounding atmosphere from 1 to 10⁵ Pa. The structures are cones with angles of 25, which grow towards the laser beam and protrude above the initial surface for 20–30 μm. It is suggested that the spatial period of the structures (10–20 μm) is determined by the capillary waves period on the molten surface. The X-ray diffractometry reveals that the modified area of the Si substrate has a polycrystalline structure and consists of Si nanoparticles with a size of 40–70 nm, depending on the pressure of surrounding gas. Similar structures are also observed on Ge and Ti. Received: 12 February 2000 / Accepted: 28 March 2000 / Published online: 20 June 2001     

Structural changes induced on strontium barium niobate glass by femtosecond laser irradiation

Localized modification of the optical properties of erbium doped strontium barium niobate (SBN) glass has been performed using femtosecond laser irradiation. The samples, with composition SrO–BaO–Nb₂O₅–B₂O₅ and doped with 5%mol of Er³⁺, were fabricated using a melt-quenching method. The samples were irradiated with different number of pulses per spot (1–50 pulses) at two different laser fluences (2.6 and 5.6 J/cm²) by using an fs laser amplifier operating at 800 nm and generating pulses with a duration of 120 fs. Micro-luminescent microscopy, using an Ar⁺ laser as excitation source, has been used to analyze the modifications of the luminescent properties of the sample upon fs laser exposure. The emissions of the Er³⁺: ⁴I_11/2→⁴I_15/2 and ⁴I_13/2→⁴I_15/2 transitions allow appreciating the structural modifications caused by femtosecond laser exposure. The lifetimes of the levels involved in these transitions were measured inside and outside the laser irradiated region. These measurements have been compared with those obtained in bulk glass ceramic sample, which is obtained from the glass precursor by a thermal treatment in order to estimate the optimal conditions to produce nanocrystals in a localized region by ultrafast laser irradiation.     

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.     

The effect of screening in an erosion flare on the recoil momentum and on the measurement of the reflection coefficient

Experimental investigations have been carried out to measure the transmission coefficient of laser light through an erosion flare, the coefficient of reflection from the irradiated solid surface, and the recoil momentum of insulating and metal targets in the range of pulsed laser intensities from 10⁶ to 10⁷ W/cm² with variation in the pressure of the surrounding medium from 10⁻² to 10⁵ Pa. An analysis is made of how the screening properties of the erosion flare affect the recoil momentum, and it is found necessary to take into account absorption of the radiation in the flare in determining the coefficient of reflection of the radiation from the surface. Zh. Tekh. Fiz. 67, 58–62 (March 1997)