Control of cluster multielectron ionization in ultraintense laser fields

We performed classical molecular dynamics simulations to explore the controllability of the inner ionization process in Xe_n clusters (n = 2?2171), driven by ultraintense infrared Gaussian laser fields (peak intensity I _M = 10¹⁵?10¹⁸ W cm^?2, temporal pulse length τ = 10?100 fs, and frequency ν = 0.35 fs^?1). Controllability of ion charge abundances and of their spatial distributions inside the cluster emerges from the different pulse length dependences of classical barrier suppression ionization (BSI) and of electron impact ionizations (EII), as well as from the time scale of the Coulomb explosion (CE). For large clusters (Xe₂₁₇₁), low intensities (10¹⁵ W cm^?2), and long pulses (τ = 100 fs), EII is the dominating ionization channel, which favors the formation of maximum charged ions (Xe¹⁰⁺, Xe¹¹⁺) in the cluster center. In contrast, BSI forms an inverse radial charge ordering with the highest charges in the exterior cluster shells. This suggests that the production of the two inverse radial charge distributions with an equal average ion charge can be forced by the choice of multiple pulses with different intensities and pulse lengths. At high intensities (10¹⁷?10¹⁸ W cm^?2), where EII is insignificant and CE sets in much earlier, the BSI radial charge ordering and the enhancement of the ion charges beyond the single-atom limit by the ignition effect is observed only for short pulses.     

Retelling the old story

When diatomic and triatomic molecules are exposed to subpicosecond laser pulses (focused intensities well in excess of 10¹⁴ W cm^?2; wavelengths of the order 600 nm), they are highly ionized. The laser electric fields are so large that they compete with, and in some cases exceed, the internal fields binding the valence electrons. The result is that conventional perturbation theory is inapplicable and one has to resort to alternative approaches. A simple starting point is the field ionization, Coulomb explosion model. This model is partially successful in explaining the ionization and subsequent fragmentation of the heavy molecule, I₂, exposed to short (sub-100 fs) laser pulses, but even here the fine details are not understood. The dynamics of the fragmentation of the lighter molecules such as N₂ and CO are not understood at all; one complication is that the time scales of dissociation and stepwise ionization overlap. In the case of the simplest molecular ion, H⁺ ₂, there has been some progress, leading to the tentative conclusion that bond softening and laser-induced bound states will be important ingredients of a successful theory of multielectron dissociative ionization.     

Analysis and control of ultrafast photodissociation processes in organometallic molecules

In this paper we characterize the ultrafast fragmentation in electronically excited Fe(CO)₂(NO)₂ and CpMn(CO)₃ by means of femtosecond time-resolved spectroscopy combined with mass spectrometry. From the transient two-color multi-photon ionization data, it was possible to record the transients of the parent molecule ions and their photofragment ions. The experimentally observed decay times indicated an ultrafast loss of the first ligands (sub-100 fs decay times). Further we performed a feedback control experiment on the photofragmenting CpMn(CO)₃ molecular system in order to maximize the yield of desired ionic products through pulse modulation. The shape of the pulses obtained from optimization reflect well the intrinsic molecular dynamics during photofragmentation and the change of the CpMn(CO)⁺/CpMn(CO)₃ ⁺ ratio shows a clear evidence for the capability of the optimization method to find tailor-made system-specific pulses. Received 9 January 2001     

Charge-state resolved above threshold ionization

Photoelectron energy resolved spectra recorded in coincidence with singly and doubly ionized atoms are reported for the interaction of xenon with 60 fs laser pulses at 800 nm and 1x10(14) W/cm(2). Double ionization contributions in the spectrum have been established. The appearance of a single ionization plateau in above threshold ionization is verified. A hotter electron distribution is found for the double ionization.     

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     

Electron impact ionization of atomic clusters in ultraintense laser fields

In this paper we report on inner ionization of Xe_n clusters (n = 55- 2171) in ultraintense Gaussian laser fields (peak intensity I = 10¹⁵- 10²⁰ Wcm^-2, pulse width τ= 25 fs, frequency 0.35 fs^-1). The cluster inner ionization process is induced by the barrier suppression ionization (BSI) mechanism and by electron impact ionization (EII), which occurs sequentially with the BSI. We address electron impact ionization of clusters, which pertains to inelastic reactive processes of the high-energy (100 eV–1 keV per electron) nanoplasma. We utilized experimental data for the energy dependence of the electron impact ionization cross-sections of Xe^j+ (j = 1-10) ions, which were fit by an empirical three-parameter Lotz-type equation, to explore EII in clusters by molecular dynamics simulations. Information was obtained on the yields and time-resolved dynamics of the EII levels (i.e., number n_imp of electrons per cluster atom) in the Xe_n clusters and their dependence on the laser intensity and cluster size. The relative long-time (t = 90 fs) yields for EII, n_imp/n_ii (where n_ii is the total inner ionization yield) are rather low and increase with decreasing the laser intensity. In the intensity range I = 10¹⁵-10¹⁶ Wcm^-2, n_imp/n_ii = 0.21 for n = 2171 and n_imp/n_ii = 0.09-0.14 for n = 459, while for I = 10¹⁸-10²⁰ Wcm^-2, n_imp/n_ii = 0.01-0.05. The difference Δn_imp between the EII yield at long time and at the termination of the laser pulse reflects on ionization dynamics by the nanoplasma when the laser pulse is switched off. For Xe₂₁₇₁ in the lower intensity domain, Δ n_imp = 0.9 at I = 10¹⁵ Wcm^-2 and Δn_imp = 0.4 at 10¹⁶ Wcm^-2, reflecting on EII by the persistent nanoplasma under “laser free” conditions, while in the higher intensity domain of I = 10¹⁷ - 10¹⁸ Wcm^-2, Δn_imp is negligibly small due to the depletion of the transient nanoplasma.     

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     

Dynamics of phase transitions induced by femtosecond laser pulse irradiation of indium phosphide

The structural transformation dynamics of single-crystalline indium phosphide (InP) irradiated with 150 fs laser pulses at 800 nm has been investigated by means of time-resolved reflectivity measurements covering a time window from 150 fs up to 500 ns. The results obtained show that for fluences above a threshold of 0.16 J/cm² thermal melting of the material occurs on the timescale of 1–2 ps. The evolution of the reflectivity on a longer timescale reveals the reflectivity of the liquid phase and shows resolidification times typically around 10–30 ns after which an amorphous layer several tens of nanometers thick is formed on the surface. This amorphous layer significantly alters the optical properties of the surface and finally leads to a reduced ablation threshold for subsequent laser pulses. Single-pulse ablation at higher fluences (>0.23 J/cm²) is preceded by an ultrafast phase transition (non-thermal melting) occurring within 400 fs after the arrival of the pulse to the surface. PACS 79.20.Ds; 78.47.+p; 64.70.-p     

Features of current carrier scattering in epitaxial films

The properties of epitaxial cadmium selenide films obtained by condensation in a vacuum on mica substrates under almost equilibrium conditions are investigated. The temperature dependences of the conductivity and current carrier mobility and concentration are studied. The electron concentration in the films depended on the gas phase composition (coevaporation of CdSe + Se or CdSe + In) and varied between 5·10¹⁰cm^–3 and 3.5·10¹⁸. It is shown that the current carrier scattering mechanism depends on their concentration and production conditions. For n₁ 10¹⁶ cm^–2 (T_S520C),n₂ < 10¹⁵ (T_S=630C), scattering on intercrystallite barriers predominated. For n₁ and n₂ greater than the quantities mentioned, scattering by ionized defects becomes dominant. It is established that the magnitude of the intercrystallite barrier in films with 10¹⁵ < n < 10¹⁶ cm^–3 is comparatively small and does not exceed 4·10^–3 eV, whereupon scattering at the barriers is not explicitly manifest. Concentrations of the ionized centers, magnitudes of the intercrystallite barriers, and ionization energies of the donor levels are determined for films obtained under different conditions.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 9, pp. 98–103, September, 1977.     

Collective stopping and ion heating in relativistic-electron-beam transport for fast ignition

The photoelectron spectra of C60 ionized using a 790 nm laser with pulse durations varying from 25 fs to 5 ps have been determined. For 25 fs pulses, in the absence of fragmentation, the ionization mechanism is direct multiphoton ionization with clear observation of above threshold ionization. As the pulse duration is increased, this becomes dominated by a statistical ionization due to equilibration among the electronic degrees of freedom. For pulse durations on the order of a ps coupling to the vibrational degrees of freedom occurs and the well-known phenomenon of delayed (&mgr;s) ionization is observed.     

Surface plasmon resonance in nano-gold antimony glass–ceramic dichroic nanocomposites: One-step synthesis and enhanced fluorescence application

A single-step melt-quench in situ thermochemical reduction technique has been used to synthesize a new series of Au° nanoparticles embedded antimony glass–ceramic (K₂O–B₂O₃–Sb₂O₃–ZnO) dichroic nanocomposites. X-ray and selected area electron diffractions manifest growth of Au° nanoparticles along (2 0 0) planes. The particle sizes obtained from X-ray diffraction patterns are found to vary in the range 4–21 nm. Dichroic behavior is attributed to the elliptical shape gold nanoparticles having aspect ratio 1.2, as observed from the transmission electron microscopy (TEM) images. The Au° nanoparticles exhibit surface plasmon resonance band (SPR) around 600 nm, which experiences red-shifts with increasing Au concentration. These nanocomposites when co-doped with Sm₂O₃ and excited at 949 nm, exhibit 2-fold intensification of 636 nm red emission transition (⁴G_5/2 → ⁶H_9/2) due to SPR induced local field enhancement of Au° nanoparticles and are promising materials for display applications.     

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     

High-order harmonic generation and multi-photon ionization of Na2 in laser fields

In this paper high-order harmonic generation （HHG） spectra and the ionization probabilities of various charge states of small cluster Na2 in the multiphoton regimes are calculated by using time-dependent local density approximation （TDLDA） for one-colour （1064 nm） and two-colour （1064 nm and 532 nm） ultrashort （25 fs） laser pulses. HHG spectra of Na2 have not the large extent of plateaus due to pronounced collective effects of electron dynamics. In addition, the two-colour laser field can result in the breaking of the symmetry and generation of the even order harmonic such as the second order harmonic. The results of ionization probabilities show that a two-colour laser field can increase the ionization probability of higher charge state.     

Widely tunable ultraviolet sub-30-fs pulses from supercontinuum for transient spectroscopy

Focusing 800-nm pulses of 10–20 fs and ≤0.4 mJ into atmospheric-pressure argon gives rise to a supercontinuum extending down to 250 nm. We show that spectral cuts from this radiation can be shortened by a simple prism compressor down to 30 fs even near the UV cut-off. The resulting pulses have enough energy (several hundred nanojoules) to serve as a simple and rugged broadly tunable pump source in ultra-fast transient spectroscopy. Such an application is demonstrated for the first time, using pulses tuned over 280–320 nm to excite Cr(CO)₆; probing it by intense-field ionization at 800 nm, we determine the lifetime of initially populated states to be as short as 14 fs.PACS 42.65.Jx; 42.65.Ky; 42.65.Re; 42.72.Bj; 82.20.-w; 82.53.-k     

飞秒激光激发空气电离的阈值研究

报道在脉宽50fs—22ps,波长800nm脉冲激光作用下的空气电离阈值的研究结果.利用探测等离子体发光信号的方法,实验测量了激发空气电离所需的阈值激光强度.结果表明,当激光脉冲宽度从50fs增加到22ps时,阈值光强I_th从8.7×10¹⁴W/cm²下降到2.7×10¹³W/cm²;I_th经历了由迅速降低逐渐发展为缓慢降低的过程.在50fs—1p 关键词： 飞秒激光 阈值 多光子电离 碰撞电离     

Femtosecond-pulse laser ablation of human corneas

A femtosecond pulse laser in the visible spectral region shows promise as a potentially new powerful corneal sculpting tool. It combines the clinical and technical advantages of visible wavelengths with the high ablation quality observed with nanosecond-pulse excimer lasers at 193 nm. A femtosecond and a nanosecond dye laser with pulse durations of 300 fs and 7 ns, and centre wavelengths at 615 nm and 600 nm, respectively, both focused to an area of the order of 10^–5 cm², have been applied to human corneal ablation. Nanosecond laser pulses caused substantial tissue disruption within a 30–100 m range from the excision edge at all fluences above the ablation threshold of F _th60 J cm^–2 (I _th9 GW cm^–2). Completely different excisions are produced by the femtosecond-pulse laser: high quality ablations of the Bowman membrane and the stroma tissue characterised by damage zones of less than 0.5 m were observed at all fluences above ablation threshold of F _th1 J cm^–2 or I _th3 TW cm^–2 (3×10¹² W cm^–2). The transparent cornea material can be forced to absorb ultrashort pulses of extremely high intensity. The fs laser generates its own absorption by a multiphoton absorption process.     

Optical field enhancement effects in laser-assisted particle removal

We report on the role of local optical field enhancement in the neighborhood of particles during dry laser cleaning (DLC) of silicon wafer surfaces. Samples covered with spherical colloidal particles (PS, SiO₂) and arbitrarily shaped Al₂O₃ particles with diameters from 320–1700 nm were cleaned using laser pulses with durations from 150 fs to 6.5 ns and wavelengths ranging from 400–800 nm. Cleaned areas were investigated with scanning electron and atomic force microscopy. Holes in the substrate with diameters of 200–400 nm and depths of 10–80 nm, depending on the irradiation conditions, were found at the former positions of the particles. For all pulse durations analyzed (fs, ps, ns), holes are created at laser fluences as small as the threshold fluence. Calculations of the optical field intensities in the particles’ neighbourhood by applying Mie theory suggest that enhancement of the incident laser intensity in the near field of the particles is responsible for these effects. DLC for sub-ns pulses seems to be governed by the local ablation of the substrate rather than by surface acceleration. Received: 31 May 2000 / Accepted: 7 September 2000 / Published online: 22 November 2000     

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     

Non-critically phase-matched,Ti:Sapphire-pumped picosecond optical parametric oscillator using LiB3O5

We report a new source of high-repetition rate and widely tunable picosecond pulses for the near infrared. A singly resonant, cw, picosecond optical parametric oscillator based on temperature-tuned LiB₃O₅ and synchronously pumped by 1.8 ps pulses from a self-mode-locked Ti:Sapphire laser is demonstrated. The oscillator can provide average output powers of up to 90 mW under non-critical type-I phase matching at a pulse repetition rate of 81 MHz. Without dispersion compensation, transform-limited signal pulses with 720 fs durations have been generated at 1.2 times threshold. With the available mirror set, signal tuning over 1.374–1.530 µm and idler tuning over 1.676–1.828 µm is demonstrated for a range of pump wavelengths and phase-matching temperatures. With additional mirrors, continuous tuning throughout 1–2.7 µm should be readily attainable with a single LiB₃O₅ crystal.