Femtosecond laser-induced dynamic alignment in Coulomb explosion of CO: Roles of laser wavelength, intensity and pulse duration

Dependences of dynamic alignment of CO molecules induced by intense femtosecond laser fields on laser wavelength, intensity and pulse duration are investigated by numerical simulations. A counting approach and a fourth-order Runge-Kutta algorithm are used to calculate the angular distribution and the time evolution of molecules. A two-step Coulomb explosion model of diatomic molecules in intense laser fields is used to determine the instant that CO molecular dynamic alignment is over. Our calculating results show that the linear polarizability and the damping force play an important role in the angular rotation of CO molecule in conditions of 800 nm laser wavelength and 10¹⁵ W/cm² laser intensity. The contributions of the second-order field-induced dipole moment and the higher-order correction term to molecular rotation acceleration comparing to the linear polarizability and damping force are negligible. The extent of dynamic alignment of CO molecules reduces with the increasing of laser intensity. The dynamic alignment time of CO molecules is tightly connected to the laser pulse duration. The angular distributions of CO molecules as the laser pulse length varied from 50 to 250 fs at laser intensity of 3×10¹⁴ W/cm² are shown and discussed.     

Expansion velocities of 0.5 ps KrF excimer laser induced plasma by Doppler-shift analysis of pump and probe measurements

High gradient laser plasma is formed by focused KrF laser pulses (248.3 nm, 450 fs, 10¹³ W/cm²) on liquids (water, styrene) and solids (silicon, aluminum, and polyimide). The hydrodynamic expansion of the plasma was studied by measuring the blue Doppler-shift of reflected probe pulses which was produced by a delayed dye laser (496.6 nm, 450 fs). The Doppler-shift corresponds to the velocity of the reflecting surface of the plasma which is defined by the critical electron density. Expansion is investigated as a function of delay time and laser intensity. The reflecting surface of the plasma accelerates over 1–2 ps after the onset of the ablating laser pulse. With increasing intensity up to 2×10¹³ W/cm² the maximum average velocities are monotonously increasing up to 1–2×10⁵ m/s. PACS 52.38.Kd; 52.50.Jm, 52.70.Kz     

Effects of electron relaxation on multiple harmonic generation from metal surfaces with femtosecond laser pulses

Calculations are presented for the first four (odd and even) harmonics of an 800 nm laser from a gold surface, with pulse widths ranging from 100 down to 14 fs. For peak laser intensities above 1 GW/cm² the harmonics are enhanced because of a partial depletion of the initial electron states. At 10¹¹ W/cm² of peak laser intensity the calculated conversion efficiency for 2nd-harmonic generation is 3 × 10⁻⁹, while for the 5th-harmonic it is 10⁻¹⁰. The generated harmonic pulses are broadened and delayed relative to the laser pulse because of the finite relaxation times of the excited electronic states. The finite electron relaxation times cause also the broadening of the autocorrelations of the laser pulses obtained from surface harmonic generation by two time-delayed identical pulses. Comparison with recent experimental results shows that the response time of an autocorrelator using nonlinear optical processes in a gold surface is shorter than the electron relaxation times. This seems to indicate that for laser pulses shorter than ∼30 fs, the fast nonresonant channel for multiphoton excitation via continuum-continuum transitions in metals becomes important as the resonant channel becomes slow (relative to the laser pulse) and less efficient.     

Recombination emissions and spectral blueshift of pump radiation from ultrafast laser induced plasma in a planar water microjet

We report spectroscopic investigations of an ultrafast laser induced plasma generated in a planar water microjet. Plasma recombination emissions along with the spectral blueshift and broadening of the pump laser pulse contribute to the total emission. The laser pulses are of 100 fs duration, and the incident intensity is around 10¹⁵ W/cm². The dominant mechanisms leading to plasma formation are optical tunnel ionization and collisional ionization. Spectrally resolved polarization measurements show that the high frequency region of the emission is unpolarized whereas the low frequency region is polarized. Results indicate that at lower input intensities the emission arises mainly from plasma recombinations, which is accompanied by a weak blueshift of the incident laser pulse. At higher input intensities strong recombination emissions are seen, along with a broadening and asymmetric spectral blueshift of the pump laser pulse. From the nature of the blueshifted laser pulse it is possible to deduce whether the rate of change of free electron density is a constant or variable within the pulse lifetime. Two input laser intensity regimes, in which collisional and tunnel ionizations are dominant respectively, have been thus identified.     

Ionization spectrum transformation and compression of powerful femtosecond laser pulses in experiments on the propagation in gas-filled dielectric capillaries

The propagation of an intense (I≤10⁶ W/cm²) femtosecond laser radiation with a duration of ～100 fs through gas-filled dielectric capillaries was studied. The radiation with a power up to 0.2 TW propagates along the paths up to 20 cm with a transmission efficiency of ～45%. The beam transverse structure at the output is close to the capillary fundamental mode under gas-ionization conditions. The transformation of pulse spectrum was studied as a function of input intensity. It is demonstrated experimentally that the pulse is compressed to a duration of ～30 fs due to the compensation of ionization-induced self-phase modulation in a linear dispersive element at the capillary output.     

Hot electrons produced from long scale-length laser-produced droplet plasmas

Microplasmas produced from 15 μm methanol droplets irradiated by 100 fs laser pulses in the intensity range 10¹⁴–10¹⁶ W cm^?2 are investigated via measurements of the hot electron temperature and x-ray yields under different conditions of intensity, polarization state, and plasma scale-length. The scale length of the drop-let plasma is increased with an intentional prepulse that is 10 ns ahead of the main pulse. Hot electron temperatures up to 48 keV have been measured at intensities of 2.5 × 10¹⁵W cm^?2 and the scaling of temperature as a function of intensity is determined for a long scale-length droplet plasma. The polarization and ellipticity dependence of the hard x-ray yield from the microdroplet plasmas are used to probe the shape of the droplet after irradiation by a prepulse.     

Simulation of THz emission from laser interaction with plasmas

One-dimensional particle-in-cell (PIC) program is used to simulate the generation of high power terahertz (THz) emission from the interaction of an ultrashort intense laser pulse with underdense plasma. The spectra of THz radiation are discussed under different laser intensity, pulse width, incident angle and density scale length. High-amplitude electron plasma wave driven by a laser wakefield can produce powerful THz emission through linear mode conversion under certain conditions. With incident laser intensity of 10¹⁸ W/cm², the generated emission is computed to be of the order of several MV/cm field and tens of MW level power. The corresponding energy conversion efficiency is several ten thousandths, which is higher then the efficiency of other THz source and suitable for the studies of THz nonlinear physics.     

Effects of an ultrashort prepulse on soft X-ray generation from an aluminium plasma produced by femtosecond Ti:Sapphire laser pulses

The influence of a prepulse on soft X-ray emission in the range of 50–200 from an aluminium plasma produced by 130 fs Ti: Sapphire laser pulses with an intensity of 10¹⁴ W/cm² at normal incidence is studied. An ultrashort prepulse with an intensity of 10¹³ W/cm² significantly enhances soft X-ray emission when there is a long time separation ( > 100 ps) between the prepulse and an intense main pulse. It is also observed for the first time that a prepulse with a short pulse time separation can slightly reduce soft X-ray emission, contrary to the previous work done using 248 nm laser pulses. This can be explained qualitatively in terms of the dependence of absorption on the length scale.     

Thermal emission of electrons from highly excited sodium clusters

Positively charged sodium clusters can be easily ionized by a fs laser pulse of relatively low intensity (<10¹⁰ W/cm²), if the laser is in resonance with the plasmon excitation of the cluster. This ionization process was investigated in detail by measuring the kinetic energy distribution of electrons emitted from a size-selected Na₉₃ ⁺ as a function of the fs laser intensity. In all cases pure Boltzmann-like energy distributions were observed. A comparison with statistical theory shows that the emission is a purely thermal process. It is different to normal thermionic emission insofar as the electrons are emitted from a hot electron system which is only weakly coupled to a cold ionic background. The results demonstrate purely statistical behaviour of a small fermionic system even for very high excitation energy. Received: 25 May 2000 / Accepted: 6 November 2000 / Published online: 9 February 2001     

High-order harmonic generation from organic molecules in ultra-short pulses

We have studied high-order harmonic generation (HHG) from organic molecules irradiated with near-infrared high intensity laser pulses of 70 fs and 240 fs duration. The molecular systems studied were the aromatics benzene and naphthalene and the alkanes cyclopropane and cyclohexane (cyclic) and n-hexane (linear). Harmonic intensities were measured both as a function of laser intensity (in the range 5×10¹³-5×10¹⁵ W cm^-2) and as a function of ellipticity of the laser field polarisation. The results were compared with those from the xenon atom. For 70 fs pulses, harmonic generation from the organic systems was similar to that of xenon, revealing an atom-like behaviour for molecules when the laser pulse duration is shorter than the fragmentation timescale of the molecule. We note significant differences between molecules with respect to HHG efficiencies and the suppression of HHG in larger species. We discuss these differences in the context of the molecular properties, electronic structure and behaviour of ionisation and fragmentation that result in enhancement of field ionisation in larger systems. Study of the polarisation ellipticity dependence of HHG shows that the harmonic yield in molecules is less sensitive to the polarisation than for atoms (xenon). This is consistent with the expected behaviour given the larger recollision cross-section presented by the core in the molecular system compared to the atom. Our results suggest that study of HHG from molecules exposed to ultra-short pulses is potentially a powerful tool for understanding the electron dynamics of molecules exposed to an intense field. Received 14 September 2000 and Received in final form 6 December 2000     

VUV-heating of plasma layers and their use as ultrafast switches

We report on new possibilities to generate solid-density plasma at extreme energy density by intense VUV beams. Here we consider 100 fs pulses of 30 eV photons focused to 10¹⁶ and 10¹⁸ W/cm². The temperature evolution in 50 nm thick aluminum foils is discussed on the basis of simulations, performed with the one-dimensional radiation hydrodynamics code MULTI-fs. For 30 eV photons, the foil is shown to switch from transmission to reflection mode on a femto-second time-scale; this is due to the rapid change of the plasma frequency during laser heating which may turn an initially transparent Al-foil into an opaque one. The switching-time depends on the intensity of the laser pulse. Also layered heating structures inside the foil are discussed which occur due to reflection at the rear surface.     

Femtosecond petawatt laser

The high‐power femtosecond laser has now become an excellent scientific tool for the study of not only relativistic laser–matter interactions but also scientific applications. The high‐power femtosecond laser depends on the Kerr‐lens modelocking (KLM) and chirped‐pulse amplification (CPA) technique. An all‐Ti:sapphire‐based 30‐fs PW CPA laser, which is called the PULSER (Petawatt Ultrashort Laser System for Extreme Science Research) has been recently constructed and is being used for accelerating the charged particles (electrons and protons) and generating ultrashort high‐energy photon (X‐ray and γ‐ray) sources. In this review, the world‐wide PW‐level femtosecond laser systems are first summarized, the output performances of the PULSER‐I & II are described, and the future upgrade plan of the PULSER to the multi‐PW level is also discussed. Then, several experimental results on particle (electron and proton) acceleration and X‐ray generation in the intensity range of mid‐10¹⁸ W/cm² to mid‐10²⁰ W/cm² are described. Experimental demonstrations for the newly proposed phenomena and the understanding of physical mechanisms in relativistic and ultrarelativistic regimes are highly expected as increasing the laser peak intensity up to over 10²² W/cm² ～10²³ W/cm².     

Energetic ion generation by Coulomb explosion in cluster gas and a low-density plastic foam with an intense femtosecond laser

The energy distributions of protons emitted from the Coulomb explosion of hydrogen clusters by an intense femtosecond laser have been experimentally obtained. Ten thousand hydrogen clusters were exploded, emitting 8.1-keV protons under laser irradiation of intensity 6 × 10¹⁶W/cm². The energy distributions are interpreted well by a spherical uniform cluster analytical model. The maximum energy of the emitted protons can be characterized by cluster size and laser intensity. The laser intensity scale for the maximum proton energy, given by a spherical cluster Coulomb explosion model, is in fairly good agreement with the experimental results obtained at a laser intensity of 10¹⁶–10¹⁷ W/cm² and also when extrapolated with the results of three-dimensional particle simulations at 10²⁰–10²¹ W/cm². Energetic proton generation in low-density plastic (C₅H₁₀) foam by intense femtosecond laser pulse irradiation has been studied experimentally and numerically. Plastic foam was successfully produced by a sol-gel method, achieving an average density of 10 mg/cm³. The foam target was irradiated by 100-fs pulses of a laser with intensity 1 × 10¹⁸ W/cm². A plateau structure extending up to 200 keV was observed in the energy distribution of protons generated from the foam target, with the plateau shape explained well by Coulomb explosion of lamella in the foam. The laser-foam interaction and ion generation were studied qualitatively by two-dimensional particle-in-cell simulations, which indicated that energetic protons are mainly generated by the Coulomb explosion. From the results, the efficiency of energetic ion generation in a low-density foam target by Coulomb explosion is expected to be higher than in a gas-cluster target.     

A coincidence technique for the study of intense laser atom interactions

A new device for charged particle coincidence experiments in strong-field, short pulse laser-atom/molecule interactions is presented. The device consists of a single time of flight spectrometer, common for both positive and negative charge detection. Experimental parameters required for the use of the device in the high intensity regime are discussed. A demonstration of electron-ion coincidence measurements in the interaction of Xe atoms with 60 fs laser pulses at 800 nm and an intensity of W/cm² is reported. Received 22 November 1999     

Absorption and second harmonic emission from interaction of femtosecond laser pulses with microspherical droplets

In this paper, the interaction of femtosecond laser pulses with droplets microplasma at the intensity of 10¹⁶ W/cm² is theoretically studied. Laser absorption, suprathermal electron generation, and second harmonic generation are discussed. Using an analytical model and a 2D particle-in-cell code, we find that the dominated mechanism is resonant absorption in the interaction of femtosecond laser pulses with droplets for the misrospherical geometry.     

Microdroplet evolution induced by a laser pulse

Interaction between high-power ultrashort laser pulse and giant clusters (microdroplets) consisting of 10⁹ to 10¹⁰ atoms is considered. The microdroplet size is comparable to the laser wavelength. A model of the evolution of a microdroplet plasma induced by a high-power laser pulse is developed, and the processes taking place after interaction with the pulse are analyzed. It is shown theoretically that the plasma is superheated: its temperature is approximately equal to the ionization potential of an ion having a typical charge. The microdroplet plasma parameters are independent of the pulse shape and duration. The theoretical conclusions are supported by experimental studies of x-ray spectra conducted at JAERI, where a 100-terawatt Ti-sapphire laser system was used to irradiate krypton and xenon microdroplets by laser pulses with pulse widths of 30 to 500 fs and intensities of 6×10¹⁶ to 2×10¹⁹W/cm².     

Spatio-temporal evolution scenarios of femtosecond laser pulse filamentation in fused silica

We investigated the evolution of femtosecond laser pulses at different wavelengths corresponding to normal, zero, and anomalous regimes of group velocity dispersion (GVD) in fused silica. The laser pulse filamentation in different GVD regimes under the same similarity parameters was first considered. It was established numerically that the scenario of the pulse filamentation depends both on temporal factors, which are determined by pulse GVD and self-phase modulation, and spatial factors associated with Kerr self-focusing and plasma defocusing. In presence of strong normal GVD the dispersive stretching causes, a pulse power decrease followed by lowering of the intensity in filament, electron density reduction in plasma channel, and suppressing of the refocusing. For zero GVD the multipeak regime of radiation propagation is realized in the filament as a result of recurring self-focusings of powerful pulse tail, which was defocused in laser plasma. When GVD is anomalous a sequence of ??light bullets?? with duration about 10 fs forms in the filament. And the peak intensity in ??light bullet?? stays the same ?? 5 × 10¹³ W/cm². In the regime of anomalous GVD power is transferred from the pulse edges to its center, where the repeated self-focusings occur and form a ??light bullet?? sequence.     

On the effect of surface rippling on the generation of harmonics in laser plasmas

Experiments were carried out using a tightly focused, prepulse-free KrF laser of 700 fs pulse duration. Harmonics up to 20 eV were generated at an intensity of 1.5×10¹⁷ W/cm² from the plasma on the surface of solid targets. The observation of diffuse harmonics propagation for intensities above 10¹⁶ W/cm² and the fact that polarization of the harmonics appears to be mixed for the highest intensities are attributed to the surface rippling which is an intrinsic consequence of the unstable balance between plasma expansion and light pressure. PACS 52.25.Os; 52.35.Py; 52.50.Jm     

“冷沉积”的Ag-BaO薄膜在超短脉冲激光作用下的光电发射

研究了冷沉积制备条件下获得的Ag-BaO薄膜在超短激光脉冲串作用下的光电发射．得到Ag-BaO薄膜的阈值光强为10W/cm²，光量子效率达10^-4数量级．光电流密度与入射光强的关系主要表现为一段曲率随光强增大而逐步减小的曲线．其光量子效率是一个可变值，它的变化规律同入射光强及薄膜本身的性能有关 关键词：     

Resonant coupling of small size-controlled lead clusters with an intense laser field

We exposed small size-controlled lead clusters with a few hundreds of atoms to laser pulses with peak intensities up to 10¹⁵ W cm^-2 and durations between 60 fs to 2.5 ps. We measured kinetic energies and ionic charge of fragments as a function of the laser intensity and pulse duration. Highly charged Pbⁿ⁺ ions up to n = 26 have been detected presenting kinetic energies up to 15 keV. For comparison with our experimental results, we have performed simulations of the laser coupling with a cluster-sized lead nanoplasma using a qualitative model that was initially proposed by Ditmire and co-workers at LLNL for the case of rare gas clusters. From these simulations we conclude that two mechanisms are responsible for the explosion dynamics of small lead clusters. As already observed for large rare gas clusters (n = 10⁶), fragments with charge states below +10 are driven by Coulomb forces, whereas the higher charged fragments are accelerated by hydrodynamic forces. The latter mechanism is a direct consequence of the strong laser heating of the electron cloud in the nanoplasma arising from a plasmon-like resonance occurring at n _e = 3n _c. In order to obtain an optimized laser-nanoplasma coupling, our results suggest that the plasma resonance should occur at the peak intensity of the laser pulse. Due to inertial effects, even for such small-sized clusters, the observed optimum pulse duration is in the order of 1 ps which is in good agreement with our theoretical results. Received 18 March 2002 Published online 19 July 2002