Showing papers on "Femtosecond published in 1999"

Q-switching stability limits of continuous-wave passive mode locking

Abstract: The use of a saturable absorber as a passive mode locker in a solid-state laser can introduce a tendency for Q-switched mode-locked operation. We have investigated the transition between the regimes of cw mode locking and Q-switched mode locking. Experimental data from Nd:YLF lasers in the picosecond domain and soliton mode-locked Nd:glass lasers in the femtosecond domain, both passively mode locked with semiconductor saturable absorber mirrors, were compared with predictions from an analytical model. The observed stability limits for the picosecond lasers agree well with a previously described model, while for soliton mode-locked femtosecond lasers we have developed an extended theory that takes into account nonlinear soliton-shaping effects and gain filtering. © 1999 Optical Society of America [S0740-3224(99)01001-2] OCIS codes: 140.3580, 140.4050, 140.3540, 140.7090.

Near-Field Fluorescence Microscopy Based on Two-Photon Excitation with Metal Tips

Abstract: We present a new scheme for near-field fluorescence imaging using a metal tip illuminated with femtosecond laser pulses of proper polarization. The strongly enhanced electric field at the metal tip ( $\ensuremath{\approx}15\mathrm{nm}$ end diameter) results in a localized excitation source for molecular fluorescence. Excitation of the sample via two-photon absorption provides good image contrast due to the quadratic intensity dependence. The spatial resolution is shown to be better than that of the conventional aperture technique. We used the technique to image fragments of photosynthetic membranes, as well as $J$-aggregates with spatial resolutions on the order of 20 nm.

Laser photothermal melting and fragmentation of gold nanorods: Energy and laser pulse-width dependence

Abstract: We studied the shape transformation (by use of TEM and optical absorption spectroscopy) of gold nanorods in micellar solution by exposure to laser pulses of different pulse width (100 fs and 7 ns) and different energies (μJ to mJ) at 800 nm, where the longitudinal surface plasmon oscillation of the nanorods absorb At moderate energies, the femtosecond irradiation melts the nanorods to near spherical particles of comparable volumes while the nanosecond pulses fragment them to smaller near-spherical particles At high energies, fragmentation is also observed for the femtosecond irradiation A mechanism involving the rate of energy deposition as compared to the rate of electron−phonon and phonon−phonon relaxation processes is proposed to determine the final fate of the laser-exposed nanorods, ie, melting or fragmentation

Picosecond–milliångström lattice dynamics measured by ultrafast X-ray diffraction

Abstract: Fundamental processes on the molecular level, such as vibrations and rotations in single molecules, liquids or crystal lattices and the breaking and formation of chemical bonds, occur on timescales of femtoseconds to picoseconds. The electronic changes associated with such processes can be monitored in a time-resolved manner by ultrafast optical spectroscopic techniques1, but the accompanying structural rearrangements have proved more difficult to observe. Time-resolved X-ray diffraction has the potential to probe fast, atomic-scale motions2,3,4,5. This is made possible by the generation of ultrashort X-ray pulses6,7,8,9,10, and several X-ray studies of fast dynamics have been reported6,7,8,11,12,13,14,15. Here we report the direct observation of coherent acoustic phonon propagation in crystalline gallium arsenide using a non-thermal, ultrafast-laser-driven plasma — a high-brightness, laboratory-scale source of subpicosecond X-ray pulses16,17,18,19. We are able to follow a 100-ps coherent acoustic pulse, generated through optical excitation of the crystal surface, as it propagates through the X-ray penetration depth. The time-resolved diffraction data are in excellent agreement with theoretical predictions for coherent phonon excitation20 in solids, demonstrating that it is possible to obtain quantitative information on atomic motions in bulk media during picosecond-scale lattice dynamics.

Femtosecond spectroscopy of condensed phases with chirped supercontinuum probing

Abstract: Pump--supercontinuum-probe (PSCP) spectroscopy with femtosecond time resolution is developed theoretically and experimentally. The connection to previous theoretical results on nonchirped probing is established. It is experimentally shown that the supercontinuum can be described as a single chirped pulse. A key problem of the technique---the precise time correction of transient spectra---is solved by monitoring the nonresonant electronic response from a pure solvent (liquids) or from a transparent substrate (solid films). This allows for an adequate characterization of the supercontinuum, in particular, for directly measuring the spectral dependence of the pump-probe cross correlation. For 50-fs pump pulses, a theoretical estimate gives an accuracy for the time correction of 10 fs, which is typically \ensuremath{\approx}1/30 of the supercontinuum pulse duration. Hence a time resolution of 10--20 fs can be experimentally realized. Contributions to the nonresonant transient signal from high-frequency Raman excitations and from low-frequency impulsive-stimulated Raman processes are discussed. The PSCP technique is illustrated by results from experiments with fused silica and several common solvents and with a chromophore in solution.

Infrared photosensitivity in silica glasses exposed to femtosecond laser pulses

Abstract: We investigate the use of infrared femtosecond laser pulses to induce highly localized refractive-index changes in fused-silica glasses. We characterize the magnitude of the change as a function of exposure and measure index changes as large as 3x10(-3) and 5x10(-3) in pure fused silica and boron-doped silica, respectively. The potential of this technique for writing three-dimensional photonic structures in bulk glasses is demonstrated by the fabrication of a Y coupler within a sample of pure fused silica.

Corneal refractive surgery with femtosecond lasers

Abstract: We investigated the use of ultrashort pulsed (femtosecond) laser technology in corneal refractive surgery. When compared to longer pulsewidth nanosecond or picosecond laser pulses, femtosecond laser-tissue interactions are characterized by significantly smaller and more deterministic photodisruptive energy thresholds, as well as reduced shock waves and smaller cavitation bubbles. We utilized a highly reliable all-solid-state femtosecond laser system for all studies to demonstrate practicality in real-world operating conditions. Contiguous tissue effects were achieved by scanning a 5-/spl mu/m focused laser spot below the corneal surface at pulse energies of approximately 2-4 /spl mu/J. A variety of scanning patterns was used to perform three prototype procedures in animal eyes; corneal flap cutting, keratomileusis, and intrastromal vision correction. Superior dissection and surface quality results were obtained for lamellar procedures (corneal flap cutting and keratornileusis). Preliminary in vivo studies of intrastromal vision correction suggest that consistent refractive changes can also be achieved with this method. We conclude that femtosecond laser technology may be able to perform a variety of corneal refractive procedures with high precision, offering advantages over current mechanical and laser devices and techniques.

Femtosecond laser pulses : principles and experiments

Abstract: Laser Basics.- Pulsed Optics.- Methods for the Generation of Ultrashort Laser Pulses: Mode-Locking.- Further Methods for the Generation of Ultrashort Optical Pulses.- Pulsed Semiconductor Lasers.- How to Manipulate and Change the Characteristics of Laser Pulses.- How to Measure the Characteristics of Laser Pulses.- Spectroscopic Methods for Analysis of Sample Dynamics.- Coherent Effects in Femtosecond Spectroscopy: A Simple Picture Using the Bloch Equation.- Terahertz Femtosecond Pulses.- Coherent Control in Atoms, Molecules and Solids.- Attosecond Pulses.

Femtosecond dynamics of hydrogen bonds in liquid water : a real time study

Abstract: A pump-probe experiment is described to study femtosecond dynamics of hydrogen bonds in liquid water. The key element of the experimental setup is a laser source emitting 150 fs pulses in the 2.5– 4.4 mm spectral region, at a 10 mJ power level. The OH-stretching band is recorded for different excitation frequencies and different pump-probe delay times. Time-dependent solvatochromic shifts are observed and are interpreted with the help of statistical mechanics of nonlinear optical processes. Using these spectral data, the OH · · · O motions are “photographed” in real time. [S0031-9007(98)08298-2]

Pulse-length dependence of cellular response to intense near-infrared laser pulses in multiphoton microscopes

Abstract: The influence of the pulse length, ?, of ultrashort laser pulses at 780 and 920??nm on cell vitality and cellular reproduction has been studied. A total of 2400 nonlabeled cells were exposed to a highly focused scanning beam from a mode-locked 80-MHz Ti:sapphire laser with 60??s pixel dwell time. For the same pulse energy, destructive effects were more pronounced for shorter pulses. The damage behavior was found to follow approximately a P2/? dependence (P, mean power), indicating that cell destruction is likely based on a two-photon excitation process rather than a one- or a three-photon event. Therefore, femtosecond as well as picosecond pulses provide approximately the same relative optical window for safe two-photon fluorescence microscopy.

The role of electron–phonon coupling in femtosecond laser damage of metals

Abstract: Femtosecond laser pulses were applied to study the energy deposition depth and transfer to the lattice for Au, Ni, and Mo films of varying thickness. The onset of melting, defined here as damage threshold, was detected by measuring changes in the scattering, reflection and transmission of the incident light. Experiments were done in multi-shot mode and single-shot threshold fluences were extracted by taking incubation into account. Since melting requires a well-defined energy density, we found the threshold depends on the film thickness whenever this is smaller than the range of electronic energy transport. The dependence of the threshold fluence on the pulse length and film thickness can be well described by the two-temperature model, proving that laser damage in metals is a purely thermal process even for femtosecond pulses. The importance of electron–phonon coupling is reflected by the great difference in electron diffusion depths of noble and transition metals.

Charge Carrier Dynamics of Standard TiO2 Catalysts Revealed by Femtosecond Diffuse Reflectance Spectroscopy

Abstract: Dynamics of charge carriers generated by femtosecond UV (160 fs, 390 nm) excitation in five standard TiO2 photocatalytic powders (JRC-TIO-1, -2, -3, -4, and -5 supplied by the Catalysis Society of Japan) in a vacuum and air was investigated by means of time-resolved femtosecond diffuse reflectance spectroscopy, and was discussed from the viewpoints of crystal structure (anatase and rutile), particle size, and surrounding condition around the particles. Anatase TiO2 catalysts showed very rapid (less than 1 ps) and very slow electron−hole recombination processes, while rutile ones did not show any rapid decay. For catalysts composed of small particles, slower electron−hole recombination was observed in air compared with that in a vacuum, which was well explained in terms of upward band bending near the surface due to adsorption of oxygen. The relationship between the observed charge carrier dynamics and photocatalytic reactivity is also discussed.

Optically Turbulent Femtosecond Light Guide in Air

Abstract: The onset and recurrence of multiple light filaments during the long-distance propagation of intense femtosecond infrared pulses in air is shown to share features with strong turbulence in other physical systems. Here, however, space-time collapse events drive the turbulence, and plasma defocusing, not dissipation, is the dominant mechanism regularizing the collapse.

Parametric Generation of Tunable Light from Continuous-Wave to Femtosecond Pulses

Abstract: By exploiting nonlinear optical effects, a technology of unprecedented flexibility for the production of tunable coherent light has been developed. Referred to as optical parametric generation, it provides sources with spectral coverage extending all the way from the ultraviolet to the mid-infrared, and with temporal coverage extending over all time domains from the femtosecond pulse to the continuous wave. Such sources generate coherent light of outstanding optical quality and are now finding wide-ranging applications.

Coherent acoustic mode oscillation and damping in silver nanoparticles

Abstract: Using a femtosecond pump-probe technique, the fundamental mechanical radial mode of silver nanoparticles is coherently excited and probed via its interaction with the electron gas. The mechanical oscillations are launched by an indirect displacive process and are detected via the induced modulation of the surface plasmon resonance frequency. The measured fundamental radial mode period and damping time are found to be proportional to the nanoparticle radius in the range of 3–15 nm, in agreement with theoretical predictions.

Femtosecond time-resolved photoelectron-photoion coincidence imaging studies of dissociation dynamics

Abstract: We present the first results using a new technique that combines femtosecond pump–probe methods with energy- and angle-resolved photoelectron–photoion coincidence imaging. The dominant dissociative multiphoton ionization (DMI) pathway for NO2 at 375.3 nm is identified as three-photon excitation to a repulsive potential surface correlating to NO(C 2Π)+O(3P) followed by one-photon ionization to NO+(X 1Σ+). Dissociation along this surface is followed on a femtosecond timescale.

Mechanism for vibrational relaxation in water investigated by femtosecond infrared spectroscopy

Abstract: We present a study on the relaxation of the O–H stretch vibration in a dilute HDO:D2O solution using femtosecond mid-infrared pump-probe spectroscopy. We performed one-color experiments in which the 0→1 vibrational transition is probed at different frequencies, and two-color experiments in which the 1→2 transition is probed. In the one-color experiments, it is observed that the relaxation is faster at the blue side than at the center of the absorption band. Furthermore, it is observed that the vibrational relaxation time T1 shows an anomalous temperature dependence and increases from 0.74±0.01 ps at 298 K to 0.90±0.02 ps at 363 K. These results indicate that the O–H⋯O hydrogen bond forms the dominant accepting mode in the vibrational relaxation of the O–H stretch vibration.

Ablation characteristics of Au, Ag, and Cu metals using a femtosecond Ti:sapphire laser

Abstract: Femtosecond laser ablation of metallic bulk crystals of Au, Ag and Cu was experimentally studied with laser pulse widths ranging from 120 fs through 800 fs at a center wavelength of 780 nm for micro-machining applications. Two different ablation regimes were found in terms of the laser fluence. The characteristic length of different ablation regimes was explained in terms of the optical skin depth and thermal diffusion length; it was determined by the peak electron temperature in the two-temperature model. The lateral feature of the two ablation regimes is discriminated by the amount of particles accumulated by the evaporation process. Ablated particle was observed less in the lower fluence regime than in the higher fluence regime, but there was no significant difference on the ablated surface. The parameters used in the two-temperature model, are discussed in order to model the ultrashort pulsed laser ablation process theoretically. It is shown that the obtainable range of the lower fluence regime is enhanced with the shorter pulse lasers, because the ablation etch rate is decreased with longer pulse width.

Compact system of wavelength-tunable femtosecond soliton pulse generation using optical fibers

Abstract: Using passively mode-locked femtosecond (fs) fiber laser and polarization maintaining fibers, the compact system of wavelength-tunable femtosecond (fs) fundamental soliton pulse generation is realized. The monocolored soliton pulse, not multicolored ones, with the ideal sech/sup 2/ shape is generated, and its wavelength can be linearly shifted by varying merely the fiber-input power in the wide wavelength region of 1.56-1.78 /spl mu/m for a 75-m fiber. The soliton pulses of less than 200 fs are generated with the high conversion efficiency of 75%-85%. This system can be widely used as a portable and practical wavelength-tunable fs optical pulse sources.

Resonant and Off-Resonant Light-Driven Plasmons in Metal Nanoparticles Studied by Femtosecond-Resolution Third-Harmonic Generation

Abstract: We report on a femtosecond-resolution study of the plasmon fields in gold nanoparticles using third-harmonic generation. Controlled resonant and off-resonant plasmon excitation is achieved by tailoring the nanoparticle sample by an electron-beam-lithographic method. Comparing the measured third order interferometric autocorrelation function of the plasmon field with simulations based on a simple harmonic oscillator model we extract the temporal characteristic of the plasmon oscillation. For off-resonant excitation of particle plasmons we find a beating between the driving laser field and the plasmon field which demonstrates clearly the nature of the plasmon as a collective electron oscillation.

Aligning molecules with intense nonresonant laser fields

Abstract: Molecules in a seeded supersonic beam are aligned by the interaction between an intense nonresonant linearly polarized laser field and the molecular polarizability. We demonstrate the general applicability of the scheme by aligning I2, ICl, CS2, CH3I, and C6H5I molecules. The alignment is probed by mass selective two dimensional imaging of the photofragment ions produced by femtosecond laser pulses. Calculations on the degree of alignment of I2 are in good agreement with the experiments. We discuss some future applications of laser aligned molecules.

Low-repetition-rate high-peak-power Kerr-lens mode-locked Ti:Al 2 O 3 laser with a multiple-pass cavity

Abstract: We demonstrate a novel, long, multiple-pass cavity (MPC) to obtain low repetition rates and high peak intensities from Kerr-lens mode-locked lasers. We show that the MPC provides a zero effective length by a unity transformation of the q parameter after a given number of transits of the laser beam. Pulse durations of 16.5??fs with 0.7??MW of power at a 15-MHz repetition rate are achieved. This is, to our knowledge, the lowest repetition rate ever achieved directly from a femtosecond laser resonator without use of additional active devices and cavity dumping. The combination of low repetition rates and high peak intensity is extremely useful for femtosecond pump–probe and other nonlinear experiments because it permits the application of high peak intensity without excessive average power.

Coherent zone-folded longitudinal acoustic phonons in semiconductor superlattices : excitation and detection

Abstract: Coherent zone-folded acoustic phonons are excited in GaAsyAlAs superlattices by femtosecond laser pulses via resonant impulsive stimulated Raman scattering in both forward and backward scattering directions. The relative amplitudes of three distinct modes of first and second backfolded order match well with scattering intensities calculated within an elastic continuum model. The detection of the coherent acoustic modes is based on the modulation of the interband transitions via the acoustic deformation potential and exhibits a strong enhancement at interband transitions. [S0031-9007(98)08288-X]

Femtosecond laser-induced periodic structure writing on diamond crystals and microclusters

Abstract: Three-dimensional (3D), periodic nanowriting on diamond clusters is reported in this letter. Concentric circular rings were observed on diamond microclusters, nucleated near the periphery of a laser-irradiated region, when chemical-vapor deposited diamond was processed in air, with laser pulses of 380 fs duration and at a wavelength of 248 nm. Periodic ripples also have been observed on single-crystal and polycrystalline diamond surfaces. Further, it is experimentally shown that the periodicity of these corrugated two-dimensional and 3D structures is shorter than that of the laser wavelength used (248 nm for the excimer fs laser and 825 nm for the Ti–sapphire fs laser).

Femtosecond Dynamics of Double Proton Transfer in a Model DNA Base Pair: 7-Azaindole Dimers in the Condensed Phase

Abstract: The dynamics of double proton transfer in 7-azaindole (7-AI) dimers, a model DNA base pair, are investigated in real time using femtosecond transient absorption and fluorescence upconversion techniques. In nonpolar solvents we examine the isotope effect, the excitation energy dependence, and the structure analogue of the tautomer (7-MeAI). A detailed molecular picture of the nuclear dynamics in the condensed phase emerges with the relationship to the dynamics observed in molecular beams: Following the femtosecond excitation there are three distinct time scales for structural relaxation in the initial pair, proton (hydrogen) transfers, and vibrational relaxation or cooling of the tautomer. The molecular basis of tunneling and concertedness are elucidated by careful examination of the isotope effect and the time resolution. Comparison with the results in the isolated pair indicates the critical role of the N−H and N···N nuclear motions in determining the effective potential, and the thermal excitation in solution. Because the barrier is small, ∼1.3 kcal/mol, both are important factors and experiments at much higher energies will be unable to test either tunneling or concertedness. Finally, we compare the experimental results and the dynamical picture with detailed ab initio and molecular dynamics simulations.

Full-field characterization of femtosecond pulses by spectrum and cross-correlation measurements.

Abstract: We present a practical and accurate technique for retrieving the amplitude and the phase of ultrashort pulses from a nonlinear (second-order) intensity cross correlation and the spectrum that overcomes shortcomings of previous attempts. We apply the algorithm to theoretical and experimental data and compare it with frequency-resolved optical gating.

Simultaneous measurement of pure-optical and thermo-optical nonlinearities induced by high-repetition-rate, femtosecond laser pulses: application to CS 2

Abstract: A simple experimental technique is presented capable of separating the contribution of purely optical Kerr effects from that of thermo-optical effects in the nonlinear response of materials under high-repetition-rate laser irradiation. The technique has been realized by combining the single-beam Z-scan method with the single-beam thermal lens measurement method. We demonstrate this technique by analysing the nonlinear response at 770 nm of CS2 which exhibits cumulative thermal effects when irradiated by very intense femtosecond laser pulses at a 76-MHz repetition rate.