987 resultados para LASER-DRIVEN REACTIONS


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The behavior of population transfer in an excited-doublet four-level system driven by linear polarized few-cycle ultrashort laser pulses is investigated numerically. It is shown that almost complete population transfer can be achieved even when the adiabatic criterion is not fulfilled. Moreover, the robustness of this scheme in terms of the Rabi frequencies and chirp rates of the pulses is explored.

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Using time-of-flight spectrometry, the interaction of intense femtosecond laser pulses with argon clusters has been studied by measuring the energy and yield of emitted ions. With two different supersonic nozzles, the dependence of average ion energy (E) over bar on cluster size (n) over bar in a large range of (n) over bar approximate to 3 x 10(3) similar to 3 x 10(6) has been measured. The experimental results indicate that when the cluster size (n) over bar <= 3 x 10(5), the average ion energy (E) over bar proportional to (n) over bar (0.5), Coulomb explosion is the dominant expansion mechanism. Beyond this size, the average ion energy gets saturated gradually, the clusters exhibit a mixed Coulomb-hydrodynamic expansion behavior. We also find that with the increasing gas backing pressure, there is a maximum ion yield, the ion yield decreases as the gas backing pressure is further increased.

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Particle-in-cell simulations are performed to study the acceleration of ions due to the interaction of a relativistic femtosecond laser pulse with a narrow thin target. The numerical results show that ions can be accelerated in a cascade by two electrostatic fields if the width of the target is smaller than the laser beam waist. The first field is formed in front of the target by the central part of the laser beam, which pushes the electron layer inward. The major part of the abaxial laser energy propagates along the edges to the rear side of the target and pulls out some hot electrons from the edges of the target, which form another electrostatic field at the rear side of the target. The ions from the front surface are accelerated stepwise by these two electrostatic fields to high energies at the rear side of the target. The simulations show that the largest ion energy gain for a narrow target is about four times higher than in the case of a wide target. (c) 2006 American Institute of Physics.

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We theoretically demonstrate the generation of extreme ultraviolet supercontinua in an orthogonally polarized two-color few-cycle laser field. We show that the ionized electrons can be driven back to their parent ion after traveling along curved trajectories in a plane perpendicular to the beam propagation direction, giving rise to a train of attosecond pulses at different polarization angles. A single isolated attosecond pulse can be obtained by blocking the low-order high harmonics, which contribute to the formation of the satellite pulses. (C) 2008 Optical Society of America.

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With the development of photocathode rf electron gun, electrons with high-brightness and mono-energy can be obtained easily. By numerically solving the relativistic equations of motion of an electron generated from this facility in laser fields modelled by a circular polarized Gaussian laser pulse, we find the electron can obtain high energy gain from the laser pulse. The corresponding acceleration distance for this electron driven by the ascending part of the laser pulse is much longer than the Rayleigh length, and the light amplitude experienced on the electron is very weak when the laser pulse overtakes the electron. The electron is accelerated effectively and the deceleration can be neglected. For intensities around 10(19) W(.)mu m(2)/cm(2), an electron's energy gain near 0.1 GeV can be realized when its initial energy is 4.5 MeV, and the final velocity of the energetic electron is parallel with the propagation axis. The energy gain can be up to 1 GeV if the intensity is about 10(21) W(.)mu m(2)/cm(2). The final energy gain of the electron as a function of its initial conditions and the parameters of the laser beam has also been discussed.

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The explosion dynamics of hydrogen clusters driven by an ultrashort intense laser pulse has been analyzed analytically and numerically by employing a simplified Coulomb explosion model. The dependence of average and maximum proton kinetic energy on cluster size, pulse duration, and laser intensity has been investigated respectively. The existence of an optimum cluster size allows the proton energy to reach the maximum when the cluster size matches with the intensity and the duration of the laser pulse. In order to explain our experimental results such as the measured proton energy spectrum and the saturation effect of proton energy, the effects of cluster size distribution as well as the laser intensity distribution on the focus spot should be considered. A good agreement between them is obtained.

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Three separate topics, each stimulated by experiments, are treated theoretically in this dessertation: isotopic effects of ozone, electron transfer at interfaces, and intramolecular directional electron transfer in a supramolecular system.

The strange mass-independent isotope effect for the enrichment of ozone, which has been a puzzle in the literature for some 20 years, and the equally puzzling unconventional strong mass-dependent effect of individual reaction rate constants are studied as different aspects of a symmetry-driven behavior. A statistical (RRKM-based) theory with a hindered-rotor transition state is used. The individual rate constant ratios of recombination reactions at low pressures are calculated using the theory involving (1) small deviation from the statistical density of states for symmetric isotopomers, and (2) weak collisions for deactivation of the vibrationally excited ozone molecules. The weak collision and partitioning among exit channels play major roles in producing the large unconventional isotope effect in "unscrambled" systems. The enrichment studies reflect instead the non-statistical effect in "scrambled" systems. The theoretical results of low-pressure ozone enrichments and individual rate constant ratios obtained from these calculations are consistent with the corresponding experimental results. The isotopic exchange rate constant for the reaction ^(16)O + ^(18)O ^(18)O→+ ^(16)O ^(18)O + ^(18)O provides information on the nature of a variationally determined hindered-rotor transition state using experimental data at 130 K and 300 K. Pressure effects on the recombination rate constant, on the individual rate constant ratios and on the enrichments are also investigated. The theoretical results are consistent with the experimental data. The temperature dependence of the enrichment and rate constant ratios is also discussed, and experimental tests are suggested. The desirability of a more accurate potential energy surface for ozone in the transition state region is also noted.

Electron transfer reactions at semiconductor /liquid interfaces are studied using a tight-binding model for the semiconductors. The slab method and a z-transform method are employed in obtaining the tight-binding electronic structures of semiconductors having surfaces. The maximum electron transfer rate constants at Si/viologen^(2-/+) and InP /Me_(2)Fc^(+/O) interfaces are computed using the tight-binding type calculations for the solid and the extended-Huckel for the coupling to the redox agent at the interface. These electron transfer reactions are also studied using a free electron model for the semiconductor and the redox molecule, where Bardeen's method is adapted to calculate the coupling matrix element between the molecular and semiconductor electronic states. The calculated results for maximum rate constant of the electron transfer from the semiconductor bulk states are compared with the experimentally measured values of Lewis and coworkers, and are in reasonable agreement, without adjusting parameters. In the case of InP /liquid interface, the unusual current vs applied potential behavior is additionally interpreted, in part, by the presence of surface states.

Photoinduced electron transfer reactions in small supramolecular systems, such as 4-aminonaphthalimide compounds, are interesting in that there are, in principle, two alternative pathways (directions) for the electron transfer. The electron transfer, however, is unidirectional, as deduced from pH-dependent fluorescence quenching studies on different compounds. The role of electronic coupling matrix element and the charges in protonation are considered to explain the directionality of the electron transfer and other various results. A related mechanism is proposed to interpret the fluorescence behavior of similar molecules as fluorescent sensors of metal ions.

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The phase-matching condition of high-order harmonic generation driven by intense few-cycle pulses could be controlled by adding second-harmonic pulses to change the ionization fraction of the gaseous medium. The harmonic generation efficiency could be improved by moving the phase-matching point with an all-optical control of the ionization fraction or a proper change of the confocal parameter. A specific order of harmonics could be easily controlled to reach phase matching at a fixed higher gas pressure by adding second-harmonic pulses with a suitable intensity. Such an all-optical phase-matching control was demonstrated to be dependent upon the temporal delay between the fundamental-wave and second harmonic pulses.

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An analytical fluid model is proposed for the generation of strong quasistatic magnetic fields during normal incidence of a short ultraintense Gaussian laser pulse with a finite spot size on an overdense plasma. The steepening of the electron density profile in the originally homogeneous overdense plasma and the formation of electron cavitation as the electrons are pushed inward by the laser are included self-consistently. It is shown that the appearance of the cavitation plays an important role in the generation of quasistatic magnetic fields: the strong plasma inhomogeneities caused by the formation of the electron cavitation lead to the generation of a strong axial quasistatic magnetic field B-z. In the overdense regime, the generated quasistatic magnetic field increases with increasing laser intensity, while it decreases with increasing plasma density. It is also found that, in a moderately overdense plasma, highly intense laser pulses can generate magnetic fields similar to 100 MG and greater due to the transverse linear mode conversion process.

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By means of the Huygens-Fresnel diffraction integral, the field representation of a laser beam modulated by a hard-edged aperture is derived. The near-field and far-field transverse intensity distributions of the beams with different bandwidths are analyzed by using the representation. The numerical calculation results indicate that the amplitudes and numbers of the intensity spikes decrease with increasing bandwidth, and beam smoothing is achieved when the bandwidth takes a certain value in the near field. In the far field, the radius of the transverse intensity distribution decreases as the bandwidth increases, and the physical explanation of this fact is also given. (c) 2005 Optical Society of America.

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A model of plasma formation induced by UV nanosecond pulselaser interaction with SiO2 thin film based on nanoabsorber is proposed. The model considers the temperature dependence of band gap. The numerical results show that during the process of nanosecond pulsed-laser interaction with SiO2 thin film, foreign inclusion which absorbs a fraction of incident radiation heats the surrounding host material through heat conduction causing the decrease of the band gap and consequently, the transformation of the initial transparent matrix into an absorptive medium around the inclusion, thus facilitates optical damage. Qualitative comparison with experiments is also provided. (C) 2008 Optical Society of America.

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Wavelength conversion in the 1550 nm regime was achieved in an integrated semiconductor optical amplifier (SOA)/DFB laser by modulating the output power of the laser with a light beam of a different wavelength externally injected into the SOA section. A 12 dB output extinction ratio was obtained for an average coupled input power of 75 μW with the laser section driven at 65 mA and the amplifier section at 180 mA. The response time achieved was as low as 13 ps with the laser biased at 175 mA even with low extinction ratios. The laser exhibits a similar recovery time allowing potentially very high bit-rate operation.

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We bring together two areas of terahertz (THz) technology that have benefited from recent advancements in research, i.e., graphene, a material that has plasmonic resonances in the THz frequency, and quantum cascade lasers (QCLs), a compact electrically driven unipolar source of THz radiation. We demonstrate the use of single-layer large-area graphene to indirectly modulate a THz QCL operating at 2.0 THz. By tuning the Fermi level of the graphene via a capacitively coupled backgate voltage, the optical conductivity and, hence, the THz transmission can be varied. We show that, by changing the pulsing frequency of the backgate, the THz transmission can be altered. We also show that, by varying the pulsing frequency of the backgate from tens of Hz to a few kHz, the amplitude-modulated THz signal can be switched by 15% from a low state to a high state. © 2009-2012 IEEE.

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We report an erbium-doped, nanotube mode-locked fiber oscillator generating 74 fs pulses with 63 nm spectral width. This all-fiber-based laser is a simple, low-cost source for time-resolved optical spectroscopy, as well as for many applications where high resolution driven by short pulse durations is required. © 2012 American Institute of Physics.