Absolute desorption yields of metastable atoms from the surface of solid rare gases induced by exciton creation

Absolute yields of the metastable excited atoms desorbed from the surfaces of solid Ne and Ar by the creation of surface and bulk excitons have been measured using monochromated synchrotron radiation as a selective excitation source. We have obtained the absolute yields of (2.3 ± 0.7) × 10⁻³, (1.4 ± 0.4) × 10⁻³, and (7.8 ± 2.3) × 10⁻⁴ atoms/photon at the excitation of S1, B1 and S′ exciton for Ne, respectively, and 1 × 10⁻⁵ atoms/photon at S1 excitation for Ar. The probability for metastable atom desorption is found to be about 2 to 10% at the excitation of S1 exciton on the surface of solid Ne.     

Electronic and geometric structure of doped rare-gas clusters: surface, site and size effects studied with luminescence spectroscopy

The electronic and geometric structure of rare gas clusters doped with rare-gas atoms Rg = Xe, Kr or Ar is investigated with fluorescence excitation spectroscopy in the VUV spectral range. Several absorption bands are observed in the region of the first electronic excitations of the impurity atoms, which are related to the lowest spin-orbit split atomic ³P₁ and ¹P₁ states. Due to influence of surrounding atoms of the cluster, the atomic lines are shifted to the blue and broadened (“electronical cage effect”). From the known interaction potentials and the measured spectral shifts the coordination of the impurity atom in Ar_N, Kr_N, Ne_N and He_N could be studied in great detail. In the interior of Kr_N and Ar_N the Xe atoms are located in substitutional sites with 12 nearest neighbours and internuclear distances comparable to that of the host matrix. In Ne_N and He_N the cluster atoms (18 and 22, respectively) arrange themselves around the Xe impurity with a bondlength comparable to that of the heteronuclear dimer. The results confirm that He clusters are liquid while Ne clusters are solid for N≥ 300. Smaller Ne clusters exhibit a liquid like behaviour. When doping is strong, small Rg_m-clusters (Rg = Xe, Kr, Ar, m≤10 ²) are formed in the interior sites of the host cluster made of Ne or He. Specific electronically excited states, assigned to interface excitons are observed. Their absorption bands appear and shift towards lower energy when the cluster size m increases, according to the Frenkel exciton model. The characteristic bulk excitons appear in the spectra, only when the cluster radius exceeds the penetration depth of the interface exciton, which can be considerably larger than that in free Rg_m clusters. This effect is sensitive to electron affinities of the guest and the host cluster.     

Momentum-resolved lifetimes of image-potential States on cu(100)

The dependence of the inelastic lifetime of electrons in the image-potential states of Cu(100) on their momentum parallel to the surface has been studied experimentally by means of time- and angle-resolved two-photon photoemission and theoretically by evaluating the electron self-energy within the GW approximation. The pronounced decrease of the n = 1 lifetime from 40 fs at normal emission (k(parallel) = 0) to 20 fs for k(parallel) = 0.33 A(-1) cannot be accounted for by interband decay processes to bulk states. We show that intraband transitions within the image-state band give a contribution to this decrease comparable in magnitude with the interband channel.     

Bulk and Surface Effects in X-Ray Magnetic Circular Dichroism of Iron Clusters

General trends in x-ray magnetic circular dichroism (XMCD) spectra of iron clusters of different sizes are theoretically investigated using the fully-relativistic spin-polarized multiple-scattering formalism. Purely geometrical effects of clustering and cluster-size effects are explored separately from effects of various scattering potentials and/or treatment of the surface barrier. We found that a high portion of non-bulk atoms makes the XMCD spectra of iron clusters to appear significantly different from bulk spectrum, even for quite large clusters. If the vacuum surrounding the cluster is taken into account, XMCD spectra of iron clusters change essentially (in comparison with clusters cut out of the bulk or with clusters embedded in a sea of free electrons).     

Evolution of small copper clusters and dissociative chemisorption of hydrogen

The structural evolution of small copper clusters of up to 15 atoms and the dissociative chemisorption of H2 on the minimum energy clusters are studied systematically using density functional theory. The preferred copper sites for chemisorption are identified and the transition state structures and activation barriers for clusters four to nine atoms are determined and found to be inconsistent with the empirical Bronsted-Evans-Polanyi relationship. The physicochemical properties of the clusters are computed and compared with the bulk and surface values. The results indicate that a phase transition must occur in the going from cluster to bulk.     

Interaction of argon clusters with intense VUV-laser radiation: the role of electronic structure in the energy-deposition process

The response of Ar clusters to intense vacuum-ultraviolet pulses is investigated with photoion spec-troscopy. By varying the laser wavelength, the initial excitation was either tuned to absorption bands of surface or bulk atoms of clusters. Multiple ionization is observed, which leads to Coulomb explosion. The efficiency of resonant 2-photon ionization for initial bulk and surface excitation is compared with that of the nonresonant process at different laser intensities. The specific electronic structure of clusters plays almost no role in the explosion dynamics at a peak intensity larger than 1.8 x 10(12) W/cm(2). The inner ionization of atoms for resonant and nonresonant excitation is then saturated and the energy deposition is mainly controlled by the plasma heating rate. Molecular dynamics simulations indicate that standard collisional heating cannot fully account for the strong energy absorption.     

Ultrafast hot-electron dynamics observed in Pt( -)(3) using time-resolved photoelectron spectroscopy

Time-resolved two-photon photoelectron spectra have been measured for free Pt( -)(3) using femtosecond pulses of 1.5 eV photon energy in a pump-probe configuration. The time-dependent photoelectron distribution reveals a lifetime of optically excited states of less than 70 fs. Such an unexpected fast electron relaxation in Pt( -)(3) suggests the existence of inelastic electron-electron scattering processes in a triatomic cluster which result in a lifetime similar to those of bulk metals.     

Observation of subpicosecond x-ray emission from laser-cluster interaction

We present the first experimental evidence of the subpicosecond duration of x-ray pulses emitted from laser-irradiated clusters, demonstrating the suitability of such a debris free target for ultrafast x-ray science applications. The K-shell emission (approximately 3 keV) from large Ar clusters (6 x 10(5) to 4 x 10(6) atoms) is time resolved, when irradiated by ultrashort (40 fs to 5 ps) and intense laser pulses (10(15-17) W/cm2). The observations are supported by hydrodynamical and collisional-radiative calculations, that reproduce the extremely short x-ray pulse duration.     

Surface state lifetime in quasi-one-dimensional oxygen stripes on Cu(1 1 0)

Scanning tunneling spectroscopy data on the lifetime and bottom energy of a surface state band in quasi-one-dimensional stripes are presented as a function of stripe width. The adsorbate system Cu(1 1 0)-p(2 × 1)O has been used to prepare a two-dimensional adsorbate layer and almost defect free quasi-one-dimensional stripes with a width of 3-15 CuO rows, respectively. The onset of an unoccupied surface state band (at 0.56 eV above Fermi-energy on the fully covered surface) has been analyzed with respect to the quasi-particle lifetime at the crossover from two to one dimension. A drastic increase of the onset-width with decreasing stripe width is observed. It can be explained by a decrease of quasi-particle lifetime using a Fabry-Pérot-like model. We obtain a reduction of lifetime from 37 ± 8 fs on the two-dimensional adsorbate layer to 5 ± 1 fs on a three CuO rows wide stripe.     

双波长自由载流子吸收技术测量半导体载流子体寿命和表面复合速率

提出了采用双波长自由载流子吸收技术同时测量半导体材料载流子体寿命和前表面复合速率的方法.通过数值模拟,定性分析了不同载流子体寿命和前表面复合速率对信号的影响,同时对测量参数的可接受范围和不确定度进行计算并与传统频率扫描自由载流子吸收方法测量结果进行比较.结果表明：提出的双波长自由载流子吸收方法可明显减小载流子体寿命和前表面复合速率的测量不确定度,提高参数测量精度;表面杂质和缺陷越多的样品,其前表面复合速率测量不确定度越小.进一步分析表明,此现象与不同波长激光抽运产生的过剩载流子浓度分布不同有关.     

Molecular dynamics study of Laplace pressure in solid-state nanostructures

The paper provides a comprehensive molecular dynamics study of nanostructures compressed by a system of surface atoms to analyze their surface tension. Surface tension is here understood as phenomena resulting from the presence of surface atoms. All main properties of nanostructures are conditioned by a highly developed surface. The number of surface atoms and their energy are comparable to those of bulk atoms.It is shown that at cryogenic temperatures, spherical solid-state clusters of size up to 10 nm reveal excess pressure. This pressure owes to compression of the clusters by surface atoms.The molecular dynamics study of thermodynamic properties of the nanostructures demonstrates that the increase in pressure in clusters of size from 2 to 9 nm with temperature is due to the gas component and the slope on the temperature dependence of thermal pressure does not depend on the cluster size. It is also shown that the surface tension coefficient decreases with an increase in temperature. A theoretical expression for this dependence is derived suggesting that there exists a certain Laplace temperature at which compressive pressure in a cluster is balanced by thermal gas pressure.     

Synchrotron radiation studies of mass-selected Fe nanoclusters deposited in situ

A portable UHV-compatible gas aggregation cluster source, capable of depositing clean mass-selected nanoclusters in situ, has been used at synchrotron radiation facilities to study the magnetic behaviour of exposed and Co-coated Fe clusters in the size range 250 to 540 atoms. X-ray magnetic circular dichroism (XMCD) studies of isolated and exposed 250-atom clusters show a 10% enhancement in the spin magnetic moment and a 75% enhancement in the orbital magnetic moment relative to bulk Fe. The spin moment monotonically approaches the bulk value with increasing cluster size but the orbital moment does not measurably decay till the cluster size is above ∼ 400 atoms. The total magnetic moments for the supported particles though higher than the bulk value are less than those measured in free clusters. Coating the deposited particles with Co in situ increases the spin moment by a further 10% producing a total moment per atom close to the free cluster value. At low coverages the deposited clusters are super-paramagnetic at temperatures above 10 K but a magnetic remanence at higher temperature emerges as the cluster density increases and for cluster films with a thickness greater than 50 ?(i.e. 2-3 layers of clusters) the remanence becomes greater than that of an Fe film of the same thickness produced by a conventional deposition source. Thick cluster-assembled film show a strong in-plane anisotropy. Received 14 December 2000     

Influence of the size and shape of free nanoparticles on the local changes in the lattice parameter and on the structural stability of body-centered cubic zirconium and iron

The influence of the shape and size of nanocrystals on the lattice relaxation of body-centered cubic metals (zirconium, iron) at a constant temperature has been investigated using the molecular dynamics method with the many-body interatomic interaction potential obtained in terms of the embedded-atom model. The calculations have been performed for isolated clusters with sizes ranging from 2.5 to 17 nm for zirconium and from 2 to 14 nm for iron. It has been demonstrated that, in free zirconium and iron particles, the relaxation of the lattice constant along the [100], [010], and [001] directions has an oscillatory character. Irrespective of the size of the zirconium and iron particles, the equilibrium distances between atoms at the center of cubic clusters are minimum compared to those observed in near-surface layers and the equilibrium value of the lattice parameter for the bulk sample. In spherical clusters, the region of a maximum contraction corresponds to a depth approximately equal to 0.2 particle diameter from the surface. An increase in the size of both cubic and spherical clusters leads to a decrease in the deviation of the local lattice parameter from the equilibrium value for the bulk sample. It has been established that the size and shape of the cluster substantially affect the temperature and mechanism of the structural transformation from the body-centered cubic phase into the hexagonal close-packed phase.     

Charged clusters in liquid helium

The appropriateness of the experimental study of charged clusters in liquid helium has been supported. The interaction potential of negative ions (electron bubbles) with inert clusters formed by Ne, Ar, Kr, and Xe atoms or H₂ and N₂ molecules has been found. Small clusters levitate at a distance of 13–16 Å above the negative ion. The scalings laws for the properties of charged inert clusters have been discovered and grounded; the number of quantum levels and states of such clusters has been determined. The mobility measurement of charged clusters may provide a new technique of probing the properties of impurity nanoparticles in helium.     

Computed positron lifetimes in vacancies and vacancy-iron clusters in gold

Annihilation characteristics are calculated for positrons trapped in clean and impurity decorated vacancy clusters in Au. The positron lifetime depends strongly on the structure of the clusters. In a strongly relaxed vacancy cluster, the lifetime can become smaller than the lifetime in a single vacancy. The substitution of some neighbour atoms of a vacancy cluster by Fe atoms has only a minor effect on the positron lifetimes.     

Magnetism of free and supported clusters: a comparative study

The presented work investigates the differences in magnetic properties of free and supported clusters via ab-initio calculations. The electronic structure of the clusters was calculated using a spin polarized relativistic multiple-scattering Green’s function formalism. We focus on Fe clusters of 2–9 atoms, either free or supported by Ni(001), and on Co clusters of 2–7 atoms, either free or supported by Au(111). For the supported clusters, the spin and orbital magnetic moments depend on the cluster size nearly monotonically, while for the free clusters large quasi-oscillations of magnetic moments with the cluster size were observed. Similarly, for supported clusters, the local spin magnetic moments decrease nearly linearly with increasing coordination number, while for free clusters of the same size range the trend is much more complicated. These findings are consistent with the fact that the spectral distribution function contains much sharper features for free clusters than for supported clusters.      

DSA lifetime measurements in21Ne at high recoil velocity

States in²¹Ne up to 5 MeV excitation energy have been populated using the inverted reaction²H(²⁰Ne,pγ). The Doppler shift attenuation (DSA) analysis of thepγ coincidence spectra taken in a Ge(Li) detector at 45° and 135° and an annular silicon surface barrier detector near 0° yielded the lifetimes of 8 states in²¹Ne. Due to the large recoil ofπ _i/c～ 4% three new lifetimes were determined for the short lived levels at 2.80, 4.68 and 4.73 MeV, namely 10±4 fs, 16±4 fs and 10±4 fs, respectively. The results are compared with rotational and shell model calculations.     

Quantitative auger electron analysis of homogeneous binary alloys: Chromium in gold

Quantitative Auger electron analysis of Cr/Au alloys with up to 20% Cr has been accomplished. The surface composition of scribed areas were compared to bulk compositions and it was shown that corrections for variation of density, escape depth, and electron backscattering must be included; these corrections change the measured surface Cr concentrations by approximately 15%. Alloy sputter yield ratios have been calculated from surface concentrations after sputtering with Ar or Ne (0.5, 1.0, 1.5, and 2.0 keV). The sputter yield ratio of Cr to Au was 0.5 at 1% Cr (significant preferred sputtering) but was near unity at 20% Cr (no preferred sputtering). The sputter yield ratio was nearly independent of ion species and ion energy. The 2 keV argon ion sputter yields for pure Cr and Au were determined to be 2.0 and 7.9 atoms/ion, respectively. However, the 2 keV argon ion sputter yield for Au in the alloys drops rapidly from 7.9 atoms/ion for pure Au, to 5 atoms/ion at 10–20% Cr. The sputter yield for Cr in alloys (5 atoms/ion) is relatively independent of composition and is 2.5 times higher than the yield of pure Cr. No simple model is known by which pure elements sputter yields could be used to predict alloy sputtering behavior.     

High-Intensity Femtosecond Laser Interaction with Rare Gas Clusters

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High-Intensity Femtosecond Laser Interaction with Rare Gas Clusters

With a 45 fs multiterawatt 790 nm laser system and jets of argon and krypton atomic clusters, a study of the interaction of fs intense laser pulses with large size rare gas dusters was conducted. The maximum laser intensity of about 7 × 1016 W/cm2 and dusters composed of thousands of atoms which were determined through Rayleigh scattering measurements were involved inthe experiments. On the one hand, the results indicate that the interaction is strongly cluster size dependent. The stronger the interaction, the larger the clusters are. On the other hand, a saturation followed by a drop of the energy of ions ejected from the interaction will occur when the laser intensity exceeds a definite value for clusters of a certain size.