Xe-Kr laser induced collisional ionization system and experimental preparation of its initial state: Four-photon resonant excitation

This paper proposes a novel one-colour Xe-Kr laser induced collisional ionization system. Considering the level scheme of the system, it finds that the initial state of the reaction--the four 4f levels with even J of Xe-can be prepared through method of four-photon resonant excitation by dye laser with wavelength of -440 nm. Absorption of an additional photon （the transfer laser） of the same wavelength will complete the laser induced collisional ionization process. The resonance enhanced ionization spectrum of Xe by four laser photons at -440nm is measured through time-of-flight mass spectrometry, this aims at the preparation of the initial state of the system proposed. The Stark broadening of the measured spectrum is observed and consistent with the previous study. Analysis of the measured resonance ionization spectrum implies the feasibility of -440 nm four-photon resonant excitation of the initial 4f state of the Xe Kr system proposed in this paper, which prepares for a further experiment of laser induced collisional ionization.     

Independent electron theory of multiple ionization of xenon by intense laser pulses

The intensity dependence of the multiphoton ionization spectra of Xe atoms has been investigated with an improved accuracy and well-controlled laser parameters. In particular, we have examined the ionization rates for X³⁺, X²⁻, X⁺ as functions of the laser intensity and the pressure in the target chamber. The apparatus used for these measurements is characterized by a high-energy resolution (better than 200 meV) and a completely digital acquisition system. The time-of-flight spectra clearly show the contributions of the different isotopes present in Xe gas. The laser pulses have been characterized with great accuracy by monitoring the energy, pulse width and divergence shot by shot. The ionization rates of the different ions have been used for testing the basic assumption of the Geltman theory of multiple ionization based on the single electron ionization model. We have found that for the small intensity range investigated the quantity (dXe ⁺/dI)·(dXe ³⁺/dI)/(dXe ²⁺/dI)² appears to be quite close to the value 0.5 predicted by this model.     

Strong Enhancement of Electron–Ion Recombination Owing to Free–Bound and Bound–Bound Resonance Transitions

The effect of free–bound and bound–bound resonance nonadiabatic transitions of an electron on electron–ion recombination rates in the plasma of a Ne/Xe and Ar/Xe inert gas mixture has been studied. A kinetic model of recombination has been proposed including energy relaxation in collisions with electrons, resonant electron capture to Rydberg states through three-body collisions of Xe⁺ ions with Ne or Ar atoms and dissociative recombination of NeXe⁺ or ArXe⁺ ions, and n → n' resonance transitions. It has been shown that effective resonance processes occurring in quasimolecular systems sharply increase both the recombination coefficient and the effect of collisions with neutral particles even at quite high degrees of ionization of the plasma.     

Effect of the ionization energy loss density of high-energy bismuth,krypton, and xenon ions on the development of hydrogen blisters in silicon

Radiation-induced athermal hydrogen removal from single-crystal silicon subjected to irradiation by high-energy heavy Bi⁺ (E = 710 MeV), Kr⁺ (E = 85 and 250 MeV), and Xe⁺ (130 MeV) ions is detected experimentally. The decrease in the hydrogen concentration depends on the specific ionization energy losses of high-energy heavy ions. At high specific ionization losses of Bi⁺ ions with E = 710 MeV (22.5 keV/nm), the hydrogen concentration decreases to a level at which blisters cannot be observed in an optical or electron microscope (which is likely to be 1 at % hydrogen at the peak of the calculated hydrogen concentration profile). At medium specific ionization losses of Xe⁺ ions with E = 130 MeV (12.5 keV/nm) and Kr⁺ ions with E = 250 and 85 MeV (9.5 and 8.5 keV/nm, respectively), the hydrogen concentration decreases to a level that does not affect blister formation but determines the blister failure (flaking) conditions.     

Energy distribution of photoelectrons generated from highly charged ions in a circularly polarized intense laser field

We observed the energy distribution of the photoelectrons generated from the highly charged ions in the tunneling regime by using a circularly polarized Ti:Sapphire laser (745 nm, 100 fs). The peaks for each successive charge state up to Ar³⁺, Kr⁴⁺, and Xe⁵⁺ were clearly resolved, and the peaks due to higher charge states were flattened in the high-energy region and deviated from those predicted by the quasistatic model. This deviation is explained by pondero-motive acceleration in the strong field gradient. In Xe, Xe⁸⁺ was generated at a peak intensity of 2.0 × 10¹⁶ W/cm².     

NO(3+1)共振增强的多光子离化谱

用皮秒脉冲高功率Nd∶YAG激光器抽运的光学参量发生/放大器作激发源,获得了NO分子在420～500 nm波长范围内的多光子离化谱,光谱图呈现分离谱的特征,表明在该波长区间NO分子以多光子共振方式离化。离化信号随激光强度的近四次方变化关系表明,在420～500 nm波长范围内NO分子吸收4个光子而离化。通过对谱线的标识,首次分离出NO分子以E 2Σ激发电子态为中间共振态的(3+1)多光子离化光谱序列,由谱线序列峰值波长得到NO分子E 2Σ电子态的振动常数,从而实现了采用多光子离化技术对该态能级结构的实验研究。     

Tunable VUV light generation for resonance ionization mass spectrometry of Krypton

Tunable coherent VUV radiation from 115.8 to 116.9 nm has been produced by non-linear four-wave sum frequency mixing in a xenon-argon mixture. 116.5 nm light generated by this means has been used as the first step in a three color, doubly resonant ionization scheme for Kr. In the process of validating the system the xenon refractive index per atom (STP) at 116.5 nm has been determined to be (n_(Xe) − 1)/N_Xe = −6.8(±0.8) × 10⁻²³ cm³.     

Quenching of vacuum ultraviolet fluorescence emission from electron beam excited quasi-molecular xenon

A pressure dependent quenching of the VUV broad-band fluorescence (bandwidth 15 nm centred at λ 173 nm) from high pressure xenon has been measured for pressures from 25 to 215 p.s.i. The experimental results can be explained by collisional de-excitation of the excited Xe₂ molecules by Xe atoms. A quenching cross section of ≈ 10^-17 cm², and molecular radiative lifetime of 16 nsec have been derived. The implications for the design of VUV molecular xenon lasers are discussed.     

Xe2Cl fluorescence and absorption in self-sustained discharge XeCl lasers

Fluorescence at 490 nm from the triatomic excimer Xe₂Cl^* has been investigated to determine the 308 nm absorption due to this species in an x-ray preionized, self-sustained gas discharge XeCl laser. The dependence of Xe₂Cl^* density on laser intensity (at 308 nm), buffer gas and Xe and HCl partial pressures has been determined for discharges with a peak electrical power deposition of 2.5 GWl^–1. Xe₂Cl^* absorption is estimated to reach 0.6% cm^–1 under non-lasing conditions but decreases to a non-saturable 0.2% cm^–1 for intracavity laser intensity>1 MW cm^–2. XeCl^* and Xe₂Cl^* fluorescence intensities were found to be a similar for both helium and neon buffer gases but laser output was a factor of two greater with a neon buffer.     

Multiphoton mass spectra of Xe2 molecules in the range of excited Xe*(6p, 5d) atoms

The (2 + 1) photoionization mass spectra of Xe₂ molecules are studied in a supersonic jet upon excitation by laser radiation in the energy range 80321.3–77821 cm^?1, corresponding to the dissociation of the Xe₂ molecule into atoms Xe(¹ S ₀) + Xe*(6p, 5d). Several vibrational progressions are observed, which are attributed to two-photon transitions of Xe₂ from the ground state to the excited states of the O ⁺ _g, 1_g, and 2_g symmetries. Based on the analysis of these progressions, the molecular constants of a number of excited states of Xe₂ are estimated.     

Resonant charging of Xe clusters in helium nanodroplets under intense laser fields

We theoretically investigate the impact of multiple plasmon resonances on the charging of Xe clusters embedded in He nanodroplets under intense pump-probe laser excitation (τ = 25 fs, I ₀ = 2.5 × 10¹⁴   W/cm², λ = 800 nm). Our molecular dynamics simulations on Xe₃₀₉He_10 000 and comparison to results for free Xe₃₀₉ give clear evidence for selective resonance heating in the He shell and the Xe cluster, but no corresponding double hump feature in the final Xe charge spectra is found. Though the presence of the He shell substantially increases the maximum charge states, the pump-probe dynamics of the Xe spectra from the embedded system is similar to that of the free species. In strong contrast to that, the predicted electron spectra do show well-separated and pronounced features from highly efficient plasmon assisted electron acceleration for both resonances in the embedded clusters. A detailed analysis of the underlying ionization and recombination dynamics is presented and explains the apparent disaccord between the resonance features in the ion and electron spectra.     

The study of ungerade electronic states of the Xe2 molecules in the region of Xe*(5p 56p, 5d, 7s, 6d) by the resonance multiphoton ionization method

Electronic spectra of the Xe2 molecules in the energy range of 77700?C89300 cm^?1 are recorded. The method of resonance enhanced multiphoton ionization of molecules in a supersonic molecular beam was used, in which excitation of the molecules by three photons was followed by ionization caused by a fourth photon (the (3+1) REMPI method). Analysis of the vibrational structure of observed systems of bands yielded information about the dissociation energy and the molecular constants for ungerade states of molecules. On the basis of the Franck-Condon principle, the equilibrium distances for potential curves were estimated from the relative intensities in vibrational progressions. Data on 16 new electronic states of diatomic xenon molecules with the dissociation limits Xe ₂ ^* ?? XE(5p ^{6 1} S ₀) + Xe*(5p ⁵6p,5d, 7s, 7p) were obtained.     

Multiphoton ionization of iodine atoms and CF<Subscript> 3</Subscript>I molecules by XeCl laser radiation

We report about effective ionization of iodine atoms and CF₃I molecules under the action of intense XeCl laser radiation (308 nm). The only ion fragment resulting from the irradiation of the CF₃I molecules is the I⁺ ion. We have studied the influence of the intensity, spectral composition, and polarization of the laser radiation used on the intensity of the ion signal and the shape of its time-of-flight peak. Based on the analysis of the results obtained, we have suggested the mechanism of this effect. The conclusion drawn is that the ionization of the iodine atoms by the ordinary XeCl laser with a nonselective cavity results from a three- (2 + 1)-photon REMPI process. This process is in turn due to the presence of accidental two-photon resonances between various spectral components of the laser radiation and the corresponding intermediate excited states of the iodine atom. The probability of ionization of the atoms from their ground state I(²P_3/2) by the radiation of the ordinary XeCl laser is more than two orders of magnitude higher than the probability of their ionization from the metastable state I^*(²P_1/2). The ionization of the CF₃I molecules by the XeCl laser radiation occurs as a result of a four-photon process involving the preliminary one-photon dissociation of these molecules and the subsequent (2 + 1)-photon REMPI of the resultant neutral iodine atoms.     

Formation of the XeI excimer sustained by dielectric barrier discharge in Xe／I2 at low pressure

Dielectric barrier discharge is used to study the mechanism of XeI excimer formation in the mixture of Xe and I₂ at low pressures (<1330 Pa). Fluorescence emission in the spectral region of 200－260 nm is examined. We report on the characteristics of the 253 nm emission intensity which varied with different total pressure. The results indicate that under the present experimental conditions, electron impact is the major reaction producing the excimer XeI(B), interpreted as Xe⁺+I₂^-→XeI(B)+ I^*, then radiating 253 nm fluorescence from transition B→X. The 253 nm emission increases with the total gas pressure up to a maximum value at a pressure of about 540 Pa, then decreases as the gas pressure is further increased. The 206 nm emission is determined by I^* from ionic recombination between Xe⁺ and I₂^-. This result differs from previous works under other experimental conditions.     

Formation of Xe12 by collision pair absorption at 158 nm

Pair absorption from colliding Xe atoms of the molecular fluorine laser radiation is reported. The absorption coefficient for this process at 300 K was found to be α = (4.32 ± 0.1) × 10^-9Torr^-2cm^-1. Fluorescence at 172 nm originating predominantly from the ${}^1\text{Σ}{}^{\mathrm{+}}{}_{\mathrm{u}}$ state of Xe¹₂ indicates that by this mechanism the Xe dimer laser can be pumped optically.     

Doubly charged clusters - neutral atom charge transfer: the role of the Coulombic repulsion

We have studied experimentally the collisional charge transfer between a neutral atom and a multicharged metal-atom cluster. The charge transfer cross section measured for Na ₃₁ ^{+ +} + Cs is in the range of 400 ?². The time-of-flight mass analysis of the singly charged collision products demonstrates that an energy of about 0.5 eV is deposited in the cluster fragment during the charge transfer collision. This effect can be interpreted as a charge transfer to an excited state of the metal cluster. The measured cross section for Na ₃₁ ^{+ +} + Cs is larger than the one for Na ₃₁ ⁺ + Cs collisions. This difference between these two systems is due to the existence, for the first one, of a Coulombic repulsion term in the collision output channel. Received 24 October 2000     

Evidences of a double resonant ionization mechanism in sputtering of metals

We present a theory of resonant charge exchanges, between sputtered atoms and metal surfaces, in which surface effects occur as quasi-molecular correlations in the diatomic systems formed, in the collision cascade, between secondary emitted atoms and their nearest-neighbor substrate atoms that have provided the last impulse for ejection. We set up a generalized Anderson-Newns Hamiltonian, from first principles, using a truncated and orthonormal set of states obtained from the valence orbitals of the diatomic system and from a continuous basis of jellium wave functions. We calculate the one-electron matrix elements appearing in the equations of motion for the annihilation operators of the truncated set in comparison with those resulting from the basic theory of resonant charge transfer. We determine the ionization probability of secondary emitted atoms versus their final emission velocities and we find it to be in good agreement with experimentally derived data on the Cu⁺/Cu-system. We support the hypothesis that the bare Anderson-Newns hopping mechanism needs to be completed with another charge transfer channel at the low energies of secondary ion emission.     

Characterization of collisionally pumped optical-field-ionization soft X-ray lasers

We give an overview of recent experimental results on optical-field-ionization collisional soft X-ray lasers developed at LOA. By focusing a 30-fs, circularly polarized Ti-sapphire laser pulse at an intensity of up to 8×10¹⁷ Wcm^-2 into a low-density gas cell containing Xe or Kr, we produced a few mm long plasma column for soft X-ray amplifier. Saturated amplification has been achieved on the 4d⁹5d(¹S₀)–4d⁹5p(¹P₁) transition at 41.8 nm in Xe⁸⁺, and on the 3d⁹4d(¹S₀)–3d⁹4p(¹P₁) transition in Kr⁸⁺ at 32.8 nm. Under optimum pumping conditions the Xe⁸⁺ laser provides about (5±2)×10⁹ photons per pulse whilst the Kr⁸⁺ laser delivers up to (2.5±1)×10⁹ photons per shot. The repetition rate of these soft X-ray lasers is 10 Hz. The beam wavefront of the Xe⁸⁺ laser has been measured by a Shack–Hartmann soft X-ray wavefront sensor, and the pulse duration by a cross-correlation technique. PACS 42.55.Vc; 32.30.Rj; 52.50.Jm     

Luminescence spectra of solid xenon excited by volume discharge

The luminescence spectra of solid xenon excited by a volume discharge are studied for the first time. The majority of the energy is emitted in the VUV spectral region due to the radiative decay of excitons. A specific feature of the spectra in the UV and visible regions is the complete absence of lines belonging to neutral excited particles (one-center Xe* and two-center Xe ₂ ^* excitons) and to diatomic Xe ₂ ⁺ ions. Numerous lines of the Xe⁺ ion are shifted by 0.1–0.3 nm with respect to their positions in the gas; the larger the shift, the stronger the distortion of the line shape. Based on the data obtained, a mechanism by which solid xenon is excited and ionized by fast drifting electrons is proposed.     

Atomic nitrogen laser action in a hollow cathode discharge

Near-infrared laser action of nitrogen atoms was obtained in a hollow cathode discharge. Four laser lines at wavelengths of 1358.2, 939.3, 938.7, and 862.9 nm were observed in the cw mode. In addition, the laser line at 904.6 nm was observed in quasi-cw operation in the afterglow for the first time. It is supposed that resonant charge exchange between He⁺ and N₂ followed by predissociation of N ₂ ⁺ is an important way of populating the upper laser levels.