On the capabilities of sub-Doppler photoionization spectroscopy in thin gas cells

A high-sensitivity photoionization method of registration of narrow sub-Doppler resonances in the spectral distribution of a flow of metastable atoms (or molecules) excited from the ground quantum term by a monochromatic laser beam propagating at normal incidence through an ultrathin gas cell (with a micrometer-scale or even nanoscale gas layer thickness) is proposed. Based on density matrix equations for atomic particles, various mechanisms of broadening of the considered resonances, such as time-of-flight, field, and Doppler broadening, are analyzed. The requirements for laser beam parameters and gas cell dimensions that allow obtaining the narrowest resonances are established. The proposed method can be used in ultrahigh resolution spectroscopy of atoms and molecules, as well as high-precision optical frequency standards.     

Scattering of atomic beams off a single surface step: An exact solution

The scattering of atomic beams off a single rectangular step on a planar hard-wall surface is calculated exactly using the Wiener-Hopf technique. The diffuse scattering consists of a sharp peak around the specular direction which is due to interference effects between the two surface levels and which oscillates in magnitude with incident angle. A second part then describes a smooth background scattering which strongly depends on the actual shape of the step whereas the former does not. Since the step is an infinitely extended defect a finite part of the incident atoms is scattered into the peak around specular, in contrast to the case of a compact scattering object, where only an infinitesimal part is removed from the specular beam.     

Diffraction from stepped surfaces: I. Reversible surfaces

In electron or atom diffraction experiments on surfaces, the angular shapes of the diffracted beams depend upon the distribution of steps over the surface. In this paper we analyze diffracted beam profiles from stepped surfaces that are reversible. A reversible surface is one in which the pair correlation function over the surface is symmetric with respect to positive and negative directions. We show that the intensity profile across a diffracted beam can be separated into a sharp central spike due to the limit of the correlation function at large separation plus wings or shoulders due to the finite extent of the step disorder. Simple functional expressions for these angular profiles are obtained by a Markov method of treating a one-dimensional geometric distribution of steps. The result explicitly displays the deep structure found for the general case. The method reduces the calculation to a simple eigenvalue problem so that even the continuously changing step distributions that occur in epitaxial growth can be treated easily. As in the general case, the resulting intensity profile is a sharp central spike plus a step-broadened term which now is a sum of Lorentzians. The widths of the Lorentzians are the logarithms of the eigenvalues of the matrix of probabilities which describe the step distribution over the surface. This matrix method, which treats the surface as a Markov chain, also points the correct way to account for correlations between surface atoms for two-dimensional distributions of steps. For a two-dimensional surface one must consider a Markov Random Field as opposed to a simple multiplication of two one-dimensional results. We compare the results of the general calculation to the Si epitaxy experiments of Gronwald and Henzler. The coverage and momentum transfer dependencies of the shapes of the calculated profiles agree with their measurements. The calculation is also applied to the RHEED measurements of Van Hove et al. during GaAs MBE. The measured intensity oscillations can be accounted for by a cyclically changing one-dimensional geometric distribution of steps among three layers in which the third-layer scattering increases with time.     

Surface hydrogen detection by low energy He ion scattering spectroscopy

Hydrogen adsorbed on a Si(100) surface can be detected by angle-resolved LEIS (low-energy ion scattering spectroscopy) which uses a ⁴He⁺ ion beam with incident energies around 1 keV. The scattering peaks from the surface hydrogen are restricted to narrow scattering angles from 0° to 15°, which is in agreement with those expected by the binary elastic collision model.     

On the interpretation of rainbow scattering in gas atom/surface collisions

A model is proposed to explain the scattering of thermal energy atoms from surfaces. The model allows the behaviour of the scattering trajectories to be assessed. It is shown that when a collimated beam of Neon atoms is scattered from the LiF(100) surface, the peaks observed in the inplane distribution of scattered atoms versus angle of reflection arise from trajectories with one and two repulsive collisions with the same surface atom.     

吸收限附近非对称反射条件下X射线的异常透射

研究了原子吸收限附近非对称布拉格条件下完整平板晶体的X射线异常透射．当衍射主要由原子散射因子的虚部引起时，在严格的布拉格角处，晶体内部驻波的波节位于衍射原子面上，从而导致异常透射的发生．透射波主要来源于晶体内部坡印廷矢量指向晶体下表面（入射面为上表面）的波场．该波场的有效吸收系数随非对称因子a的增大而减小，所以整个晶体的透射系数随a的增大而增大．当原子散射因子的实虚部对衍射的贡献之比一定时，晶体内坡印廷矢量偏离色散面实部法向的程度随反射的非对称程度的增大而增大． 关键词：     

Optical phase change in bismuth through structural distortions induced by laser irradiation

ABSTRACT

Semimetal bismuth (Bi) is known to possess a wide range of peculiar properties, owing to its unique electronic band structure. Its electronic band can easily be distorted by structural changes, and thereby undergo transitions between semimetal to either semiconductor or metal states. Utilising a focused laser beam, one can easily introduce structural defects, along with phase changes, oxidation, and morphological modifications. Confocal Raman microscopy indicated that the as-fabricated Bi droplets inhibit the Raman signal from the underlying silicon (Si) substrate. After a laser flash heating step, the intensity of Si optical phonons was strongly enhanced at the positions of Bi droplets, and exceeding the intensity from the bare Si substrate. Thus, such laser irradiating step on the Bi droplets induces an optical phase change. The optical phase change was detected as going from inhibition to strong enhancement of the underlying Si substrate Raman signal. From the observed Bi optical phonon modes (E_g and A_1g), alterations in the Raman peaks due to laser exposure indicated that the ordered crystallinity in pristine Bi droplets became deteriorated. The effects of atomic displacements and loss of structural order in Bi droplets impacts its dielectric response. The observed Si Raman signal enhancement is similar to the surface-enhanced Raman scattering effect typically known for noble metals.     

Raman scattering of light in silicon nanostructures: First-and second-order spectra

First-and second-order Raman scattering spectra in Si nanocrystals have been studied. The shift to lower frequencies and the substantial broadening of first-order Raman scattering lines observed to occur with decreasing nanoparticle size were established to correlate with those in second-order spectra. It is shown that the experimentally observed shifts of peaks and their broadening cannot be predicted based only on the phenomenological model of strong phonon wave function localization. The anharmonic effect originating from the heating of the nanoparticle surface by laser radiation should also be included. Proper fitting of experimental data revealed that the anharmonic constants depend strongly on nanoparticle size. The shape and spectral positions of maxima in second-order Raman scattering spectra have been theoretically described.     

The effect of the crystal structure of the field emitter on field ion energy distributions

The field ionization probability of an atom as a function of distance from the field emitter is discussed in terms of the atomic arrangement and the electron scattering properties of the ion cores of the emitter in the immediate neighborhood of the atom to be ionized, and the electron transmission properties of the potential barrier between the emitter and that atom. This approach to field ionization calculations is somewhat similar to field ionization calculations based on low energy electron diffraction (LEED) procedure in that it takes into account electron scattering from the first few atomic layers of the emitter. It differs from LEED type calculations, because it considers the highly localized nature of the ionization near a surface atom. This localization makes the ionization probability relatively insensitive to the two-dimensional periodicity of the emitter surface. A one-dimensional calculation, in which only the potential barrier and three ion core scatterers in line with the field are considered, shows secondary structure in the predicted field ion energy distributions near the critical energy deficit, as well as the well known, primary field induced resonance peaks. The surface orientation dependence of these distributions arises naturally from this model because the secondary structure depends strongly upon the crystal parameter along a line parallel to the field. This one-dimensional calculation can be no more than an approximation to a complete calculation. It is interesting, however, that such a simple physical model, in which scattering from the image potential and only two or three ion cores is considered, rather than scattering from a complete crystal, can give prodicted field ion onergy distributions which are similar to those experimentally observed.     

Spectral line narrowing in a gas by atoms trapped in a standing light wave

This paper presents results of a theoretical analysis of a new method for eliminating the Doppler broadening of spectral lines and the broadening by the transit time of atoms through a light beam. The atomic motion in a one-dimensional standing wave is studied and the conditions for translational-to-vibrational motion transformation are found. The variation in the Doppler contour by the trapping effect is investigated. It is illustrated, in particular, that the width of the narrow peak at the line centre depends mainly on the finite transit time of the atoms through the light beam. Next it is shown that, by accumulating slow atoms in a three-dimensional standing wave, it is possible, in principle, to observe narrow peaks with their widths determined only by the natural line width. The possibility of experimentally detecting of the phenomenon is discussed.     

On the theory of coherent effects caused by the interaction of a Bose-Einstein condensate of dilute gases with an electromagnetic field

The Schrödinger equation describing the interaction of a Bose-Einstein condensate of an ideal gas with an electromagnetic field is derived. Its solutions allow one to find the evolution of the radiation intensity and that of the populations of coherent atomic states with different recoil momenta and can be used for describing such effects as light scattering, light amplification, amplification of atomic beam intensity (an atomic laser), and induced transparency.     

Molecular and atomic oxygen adsorption on the kinked Pt(321) surface

Oxygen adsorption and desorption were characterized on the kinked Pt(321) surface using high resolution electron energy loss spectroscopy, thermal desorption spectroscopy and Auger electron spectroscopy. Some dissociation of molecular oxygen occurs even at 100 K on the (321) surface indicating that the activation barrier for dissociation is smaller on the Pt(321) surface than on the Pt(111) surface. Molecular oxygen can be adsorbed at 100 K but only in the presence of some adsorbed atomic oxygen. The dominance of the v(OO) molecular oxygen stretching mode in the 810 to 880 cm^?1 range indicates that the molecular oxygen adsorbs as a peroxo-like species with the OO axis parallel or nearly parallel to the surface, as observed previously on the Pt(111) surface [Gland et al., Surface Sci. 95 (1980) 587]. The existence of at least two types of peroxo-like molecular oxygen is suggested by both the unusual breadth of the v(OO) stretching mode and breadth of the molecular oxygen desorption peak. Atomic oxygen is adsorbed more strongly on the rough step sites than on the smooth (111) terraces, as indicated by the increased thermal stability of atomic oxygen adsorbed along the rough step sites. The two forms of adsorbed atomic oxygen can be easily distinguished by vibrational spectroscopy since oxygen adsorbed along the rough step sites causes a v(PtO) stretching mode at 560 cm^?1, while the v(PtO) stretching mode for atomic oxygen adsorbed on the (111) terraces appears at 490 cm^?1, a value typical of the (111) surface. Two desorption peaks are observed during atomic oxygen recombination and desorption from the Pt(321) surface. These desorption peaks do not correlate with the presence of the two types of adsorbed atomic oxygen. Rather, the first order low temperature peak is a result of the fact that about three times more atomic oxygen can be adsorbed on the Pt(321) surface than on the Pt(111) surface (where only a second order peak is observed). The heat of desorption for atomic oxygen decreases from about 290kJ/mol (70 kcal/mol) to about 196 kJ/mol (47 kcal/mol) with increasing coverage. Preliminary results concerning adsorption of molecular oxygen from the gas phase in an excited state are also briefly discussed.     

Selective adsorption resonances at rainbow conditions in the scattering of atoms by stepped surfaces: application to the He/Cu(117) system

For stepped surfaces, dynamics is not parity reversal invariant with respect to the step configuration and the way the atomic beam approaches the surface, downstairs or upstairs scattering, should dramatically change rainbow patterns. We show that only one close-coupling calculation provides us information of the two possible scatterings at once. Furthermore, it is possible to find some incident conditions where surface rainbow is displayed for both configurations. At the same time, if resonances are analysed at rainbow conditions, we could enhance resonant features in the diffraction channel displaying rainbow. An application to the study of diffraction of ⁴He atoms by the Cu(117) surface is presented.     

Doppler-free spectroscopy in driven three-level systems

We demonstrate two techniques for studying the features of three-level systems driven by two lasers (called control and probe), when the transitions are Doppler broadened as in room-temperature vapor. For -type systems, the probe laser is split to produce a counter-propagating pump beam that saturates the transition for the zero-velocity atoms. Probe transmission then shows Doppler-free peaks which can even have sub-natural linewidth. For V-type systems, the transmission of the control beam is detected as the probe laser is scanned. The signal shows Doppler-free peaks when the probe laser is resonant with transitions for the zero-velocity group. Both techniques greatly simplify the study of three-level systems since theoretical predictions can be directly compared without complications from Doppler broadening and the presence of multiple hyperfine levels in the spectrum.Received: 10 September 2003, Published online: 6 January 2004PACS: 42.50.Gy Effects of atomic coherence on propagation, absorption, and amplification of light; electromagnetically induced transparency and absorption - 42.50.-p Quantum optics     

Simulation of the scattering in an atomic beam evaporated from a He film

We have simulated the scattering in a pulsed atomic beam evaporated from a superfluid ⁴He film. Assuming that the atoms leaving the surface of the film have an equilibrium Maxwellian distribution, we find that the experimentally observed deviations from Lambert's law are explained by scattering of the atoms after evaporation.     

A method to obtain kinematic intensities from low-energy electron diffraction data

In order to use low-energy electron diffraction as a tool for surface crystallography, it would be useful to extract the single scattering, or kinematic part, from the intensity data. Details of a method to do this by taking data with different diffraction geometry but at fixed momentum transfer are presented. The method is illustrated by data from Ni and Ag. The temperature dependence of the averaged intensity is presented. The multiple scattering contributions to the averaged intensity can be accounted for by an effective atomic scattering factor. Conditions for the applicability of the method are discussed. From the resulting kinematic intensities, the surface atomic arrangements can be determined by simple modifications of conventional crystallographic analysis.     

Molecular-beam scattering and pressure broadening cross sections for the acetylene-neon system

Integral cross sections and pressure broadening coefficients have been measured for the acetylene — neon system by a molecular beam scattering technique and by high infrared resolution spectroscopy, respectively. We have performed quantal calculations using an ab-initio potential energy surface (PES) [J. Chem. Phys. 109, 8968 (1998)]. Results are found to be in good agreement with both measured integral cross sections and pressure broadening coefficients for the two temperatures investigated (173 and 298 K). We have also derived a semi-empirical PES parameterized using an atom-bond pairwise additive scheme. This PES shows an isotropic component in agreement with the ab-initio calculation, reproduces the scattering data but it only leads to a reasonable agreement for the pressure broadening coefficients.     

Optically guided beam splitter for propagating matter waves

We study experimentally and theoretically a beam splitter setup for guided atomic matter waves. The matter wave is a guided atom laser that can be tuned from quasimonomode to a regime where many transverse modes are populated, and propagates in a horizontal dipole beam until it crosses another horizontal beam at 45°. We show that depending on the parameters of this X configuration, the atoms can all end up in one of the two beams (the system behaves as a perfect guide switch), or be split between the four available channels (the system behaves as a beam splitter). The splitting regime results from a chaotic scattering dynamics. The existence of these different regimes turns out to be robust against small variations of the parameters of the system. From numerical studies, we also propose a scheme that provides a robust and controlled beam splitter in two channels only.     

Model calculations of atom-surface scattering

The elastic scattering of light mass, thermal-energy atoms from simple surfaces is investigated. The surface is represented by the model of a single planar square array of hard spheres. The effect of the surface potential well is treated semiclassically by simply shifting the energy of the incident atom ; furthermore a constant imaginary term is added to the energy to account for inelastic scattering and adsorption. As in the multiple scattering formalism of LEED the total scattering matrix of the lattice is expanded in terms of the individual gas atom-surface atom t-matrices. Propagation of the incident atom on the surface is described in terms of a one particle Green's function propagator with complex energy. The terms in the multiple scattering series are summed to all orders, by using standard matrix inversion techniques. The size of the matrix to be inverted limits to ten the total number of phase shifts that are included in the calculation. Thermal effects are included through angle dependent Debye-Waller factors.Model calculations have been performed to study the intensity of the specular and the diffracted beams as a function of the angles of incidence. The importance of surface temperature (introduced by the Debye-Waller factors), the incident energy and the depth of the potential well of the gas-surface interaction are discussed. The main feature of the results is the decrease of the intensity of the specular beam in going from glancing incidence to normal incidence and the presence of structure due to the appearance and disappearance of diffracted beams across the surface. The azimuthal behavior of the specular beam is in agreement with experimental observations.     

Classical simulation of atomic beam focusing and deposition for atom lithography

We start from the intensity distribution of a standing wave (SW) laser field and deduce the classical equation of atomic motion. The image distortion is analyzed using transfer function approach. Atomic flux density distribution as a function of propagation distance is calculated based on Monte-Carlo scheme and trajectory tracing method. Simulation results have shown that source imperfection, especially beam spread, plays an important role in broadening the feature width, and the focus depth of atom lens for real atomic source is longer than that for perfect source. The ideal focal plane can be easily determined by the variation of atomic density at the minimal potential of the laser field as a function of traveling distance.