Structural and electronic properties of Ren (${\sf n} \leq$ 8) clusters by density-functional theory

The structures, stabilities and electronic properties of small-sized Re_n (n ≤ 8) clusters have been systematically investigated by density-functional theory. The lowest-energy structures of Re_n clusters favor 3-dimensional configuration. The results of second-order difference of energies indicate that Re₄ and Re₆ possess relatively higher stability in structure. Importantly, our theoretical results of electron affinity are in agreement with experimental values, which can be responsible for the reliability of the structures.     

Absorption measurements in InSe:Ho single crystal under an electric field

InSe:Ho single crystal was grown by Bridgman-Stockberger method. Electric field effects on the absorption measurements have been investigated as a function of temperature in InSe:Ho single crystal. The absorption edge shifted towards longer wavelengths and a decrease of intensity in absorption spectra occurred under an electric field of 7.5 kV/cm. Using absorption measurements, steepness parameter and Urbach energy were calculated under electric field. Applied electric field caused an increase in the Urbach energy. At 10 K and 320 K, the first exciton energies were calculated as 1.322 and 1.301 eV for zero voltage and 1.245 and 1.232 eV for applied electric field, respectively.     

Inverse pulsed laser deposition

Since the advent of pulsed laser deposition (PLD), several different target-substrate arrangements have been proposed. Besides the most common on-axis PLD, several off-axis geometries were studied, mainly to protect the substrate from the agglomerated species (clusters, droplets, particulates) of the plasma plume, which are detrimental to the homogeneity of films. Recently we introduced a novel geometry, termed inverse pulsed laser deposition (IPLD), in which the substrate is placed parallel to and slightly above the target plane. In this paper we summarize our results on this new geometry, and show how it can extend the perspectives of pulsed laser deposition, e.g., by improving the surface morphology of the films. Effects of ambient pressure are presented and exemplified on metallic and compound IPLD films, including Ti, CN _x , and Ti-oxides. AFM topographic images are used to prove that under optimized conditions IPLD is capable of growing compact and smooth films that are superior to PLD ones. A special—but easy-to-implement—IPLD arrangement is also introduced that considerably improves the homogeneity of IPLD films. In this geometry, the properties (e.g., deposition rate and roughness) of the films grown in the 1–25 Pa pressure domain are examined.     

Adaptive clustering of a quantum solvent: the LiH+ cation in bosonic helium from stochastic calculations

Calculations of the quantum structures describing the initial solvation shells of bosonic helium atoms around a polar, ionic system like LiH⁺ are reported, together with the corresponding quantum energies. The calculations were carried out using the Diffusion Monte Carlo (DMC) approach and parametric trial functions. Its final radial and angular distributions for clusters of varying size are analysed and discussed. The solvation of this ionic dopant is shown to occur in a way which is strongly affected by the orientational induction forces between the latter molecule and the solvent atoms, indicating the onset of “snowball" structures at the location of the dopant and the clear distinction between “heliophilic" and “heliophobic" regions of microsolvation.     

Propagation of terawatt laser pulses in the air

One of the problems when increasing the intensity of a femtosecond laser pulse is the propagation of the beam. As the intensity increases nonlinear effects begin to play a significant role. When arriving to the terawatt domain, nonlinear effects and filamentation give rise to a new phenomenology in the propagation. The aim of this paper is to analyze new possibilities to control the beam shape to Taylor the interaction of the beam with the target at large distances.     

The control of near-field optics: imposing direction through coupling with off-resonant laser light

The well-known spatially distributed form of the near field, associated with a dipolar source, is usually unsuitable for effecting the excitation of a location-specific detector in the vicinity. It is of interest, therefore, to identify a means of producing a much more greatly directed character to such a near field, imposing features that are more commonly associated with longer-range, wave-zone electromagnetic propagation. In this paper, it is shown that nonlinear optical coupling with off-resonant, throughput laser light can achieve this effect. Based on a quantum electrodynamical analysis it is shown that two mechanisms contribute; one requires both the source and detector to be irradiated by the throughput radiation, the other can operate with the source alone irradiated. The analysis leads to results identifying the dependence of each mechanism on the relative directions of the laser beam and the source–detector displacement. Contour maps of the ensuing near field, at the source emission frequency, exhibit a directionality that grows with the off-resonant beam intensity. The phenomenon affords a means of achieving optical control over the near-field distribution.     

High repetition rate femtosecond laser nano-machining of thin films

Thin film laser micromachining has been utilized for repairing semiconductor masks, creating solar cells and fabricating MEMS devices. A unique high repetition rate femtosecond fiber laser system capable of variable repetition rates from 200 KHz to 25 MHz along with helium gas assist was used to study the effect of pulse repetition rate and pulse energy on femtosecond laser machining of gold-coated silicon wafer. It was seen that high repetition rates lead to smaller craters with uniform line width. Craters created at 13 MHz pulse repetition rate with 2.042 J/cm² beam energy fluence measured 110 nm in width and had a heat affected zone of 0.79 μm. It was found that pulse repetition rate only played a significant role in the size of the heat affected zone in the lower pulse energy ranges. In the future, a 1 W laser system will be acquired to find the optimal repetition rate that would create the minimal feature size with the least heat affected zone. Using this kind of setup along with techniques such as radial polarization and a different gas assist may enable us to create sub 100 nm feature size with good quality.     

Ionization potentials in alkali-metal clusters

The ionization potentials in alkali metal clusters are calculated using a jellium-background model for positive-ion cores and the local-spin-density functional approximation for valence electrons. The computed results compare reasonably with previous experimental and theoretical values in the cases of Li, Na, K and Cs.     

Potential scattering in Dirac field theory

We develop the potential scattering of a spinor within the context of perturbation field theory. As an application, we reproduce, up to second order in the potential, the diffusion results for a potential barrier of quantum mechanics. An immediate consequence is a simple generalization to arbitrary potential forms, a feature not possible in quantum mechanics.     

Growth of gas phase nanoparticles with an accretion mechanism

Nano-droplet growth in a supersaturated vapor has been investigated in a gas aggregation source using laser-ionization time-of-flight mass spectrometry. During its propagation into an atomic vapor, a small particle grows by sticking atoms on its surface. This accretion process has been highlighted through the clustering of homogeneous particles M_n and heterogeneous M_n(M₂O) and M_n(MOH)₂ particles in a metallic vapor and a helium buffer gas (M = Na or K). A modelization is introduced so as to connect the measured cluster mass distributions to the pertinent physical parameters. The mass distribution width is particularly sensitive to the efficiency of the first steps in the growth sequence. We used this property to compare the ability of this vapor-condensed matter phase transition to occur around various homogeneous and heterogeneous nucleation seeds.     

Formation of mixed clusters in a pulsed supersonic helium-oxygen-isoprene jet

An experimental study of the formation of mixed van der Waals oxygen-isoprene complexes, generated in an expanding supersonic helium-oxygen-isoprene jet at various stagnation pressures and at diverse oxygen and isoprene concentrations, has been performed. To measure the composition and distribution of the partial densities of the individual components, molecular beam mass spectrometry was adapted to pulsed modes of gas source operation. The particularities of applying mass spectrometry to studying clustered isoprene streams in a pulsed mode have been discussed. The composition of small clusters generated in a free supersonic jet has been checked for dependencies upon the initial mixture composition and stagnation pressure. The mechanism of nucleation has been identified for different partial concentrations of impurities in the helium stream. It has been shown that, even at a 0.3% concentration of isoprene in the mixture, nucleation starts with the formation of hydrocarbon complexes. The specific features of the dissociative ionization of van der Waals complexes, consisting of pure isoprene and mixed complexes, have been discussed. The conditions needed for the formation of binary oxygen-isoprene van der Waals complexes have been identified.     

Considerations about Z-scan sensitivity improvement: theory versus experiments

This paper reports an experimental demonstration of the improvement of the Z-scan technique’s sensitivity. It is shown that this sensitivity can be multiplied by a factor equal to almost 400 with the help of simple binary diffractive elements. Such a possibility was actually predicted theoretically in one of our previous papers. In this study, the interpretation is investigated in a wider context taking into account the definition of the signal normalisation as introduced by Z-scan and the well-known eclipsing Z-scan (EZ-scan) experiments. In particular, advantages and drawbacks are compared, by looking at the normalised or the unnormalised aperture transmission.     

Electron impact ionization studies with the amino acid valine in the gas phase and (hydrated) in helium droplets

Here we report electron impact ionization studies with the amino acid valine in different environments, i.e., (i) isolated in the gas phase, (ii) embedded in superfluid helium droplets and (iii) co-embedded with water in superfluid helium droplets. Mass spectra are presented for all three environments for which changes in the fragmentation pattern of valine upon ionization are investigated. Comparison is made with previous electron impact ionization and photoionization studies with valine in the gas phase which confirms the fragile nature of this amino acid. Embedding valine in cold superfluid helium droplets leads to the formation of highly abundant protonated valine clusters. Co-embedding water with valine in helium droplets reduces fragmentation of valine.     

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.     

Characteristic functions in the statisticalR-matrix theory

The characteristic functions of the statistical Wigner'sR-matrix for the case of one-channel scattering in competition with multichannel radiative capture have been drown. Different approximations and their relevance in neutron physics applications are discussed.Communicated by: X. Campi     

Corrections to the density-functional theory electronic spectrum: copper phthalocyanine

A method for improving the electronic spectrum of standard Density-Functional Theory (DFT) calculations (i.e., LDA or GGA approximations) is presented, and its application is discussed for the case of the copper phthalocyanine (CuPc) molecule. The method is based on a treatment of exchange and correlation in a many-body Hamiltonian, and it leads to easy-to-evaluate corrections to the DFT eigenvalues. Self-interaction is largely corrected, so that the modified energy levels do not suffer from spurious crossings, as often encountered for CuPc in DFT, and they remedy the standard underestimation of the gap. As a specific example we study the sequence and position of the CuPc molecular orbitals, which are wrongly calculated by standard DFT, and show that they are correctly reproduced after our corrections are included. The suggested method is fast and simple and, while not as accurate as hybrid or semiempirical functionals for molecular levels, it can be easily applied to any local-orbital DFT approach, improving on several important limitations of standard DFT methods.     

dt nuclear fusion within a single Coulomb exploding composite nanodroplet

We present a computational study of dt fusion driven by Coulomb explosion within a single, large, heteronuclear two-component D₂/T₂nanodroplet, originating from kinematic overrun effects between deuterons and tritons. Scaled electron and ion dynamics simulations have been used to explore the size dependence and the isotopic composition dependence of the intra-nanodroplet (INTRA) dt fusion yield in a composite D_2n-2kT_2k nanodroplet, initially consisting of an inner sphere of D₂ molecules surrounded by an outer sphere of T₂ molecules (n = 1.4×10⁸–2.0×10⁹, k/n = 0.10–0.60, and initial radii R₀= 1100–2700 Å) driven by a single, ultraintense, near-infrared, Gaussian laser pulse (peak intensity 10²⁰ W?cm^-2, pulse length 25 fs). INTRA dt fusion in D_2n-2kT_2k nanodroplets with neutron yields of 30–90 (per nanodroplet, per laser pulse) were attained in the size domain R₀ = 2000–2700 Å with the optimal composition in the range of k/n = 0.2–0.4. INTRA yields in D_2n-2kT_2k nanodroplets are similar (within 20–40%) to those in initially homogeneous (DT)_n nanodroplets of the same size. These INTRA yields are sufficiently large to warrant experimental observation in a single nanodroplet. The INTRA dt fusion can be distinguished from the inter-nanodroplet dt fusion reaction, which occurs inside and outside the macroscopic plasma filament, by the nanodroplet size dependence of the yield and by the different energies of the neutrons produced in these two channels.     

Diode end pumped Nd:YAG laser at 946 nm with high pulse energy limited by thermal lensing

Diode lasers with peak powers in the kW range and pulse durations of micro- to milli-seconds have been available since several years. Pumping solid state lasers with such sources yield high output pulse energies in spiking or Q-switched operation. The output energy is limited by the thermal lens effects, which are measured and calculated. The time dependent heat conduction equation in the laser crystal is solved numerically to predict the overall temperature rise and thermal lensing. The thermally induced optical path difference is approximated by a quadratic distribution to obtain the focal length f of the thermal lens. The thermal lens coefficient K=1/(f⋅P _av), which depends only weakly on the heat transfer coefficient H of the laser crystal to the heat sink, decreases exponentially with increasing pump frequency until the steady state is reached. Experiments were done with a Nd:YAG crystal at different pump frequencies up to 100 Hz. The thermal lens coefficients obtained by the power maxima of asymmetric flat-flat resonators agree with our calculations.