The role of electron localization in the atomic structure of transition-metal 13-atom clusters: the example of Co(13), Rh(13), and Hf(13)

The crystalline structure of transition-metals (TM) has been widely known for several decades, however, our knowledge on the atomic structure of TM clusters is still far from satisfactory, which compromises an atomistic understanding of the reactivity of TM clusters. For example, almost all density functional theory (DFT) calculations for TM clusters have been based on local (local density approximation-LDA) and semilocal (generalized gradient approximation-GGA) exchange-correlation functionals, however, it is well known that plain DFT fails to correct the self-interaction error, which affects the properties of several systems. To improve our basic understanding of the atomic and electronic properties of TM clusters, we report a DFT study within two nonlocal functionals, namely, the hybrid HSE (Heyd, Scuseria, and Ernzerhof) and GGA + U functionals, of the structural and electronic properties of the Co(13), Rh(13), and Hf(13) clusters. For Co(13) and Rh(13), we found that improved exchange-correlation functionals decrease the stability of open structures such as the hexagonal bilayer (HBL) and double simple-cubic (DSC) compared with the compact icosahedron (ICO) structure, however, DFT-GGA, DFT-GGA + U, and DFT-HSE yield very similar results for Hf(13). Thus, our results suggest that the DSC structure obtained by several plain DFT calculations for Rh(13) can be improved by the use of improved functionals. Using the sd hybridization analysis, we found that a strong hybridization favors compact structures, and hence, a correct description of the sd hybridization is crucial for the relative energy stability. For example, the sd hybridization decreases for HBL and DSC and increases for ICO in the case of Co(13) and Rh(13), while for Hf(13), the sd hybridization decreases for all configurations, and hence, it does not affect the relative stability among open and compact configurations.

Denisiuk-type reflection holography display with sillenite crystals for imaging and interferometry of small objects

A novel setup for imaging and interferometry through reflection holography with Bi12TiPO20(BTO) sillenite photorefractive crystals is proposed. A variation of the lensless Denisiuk arrangement was developed resulting in a compact, robust and simple interferometer. A red He-Ne laser was used as light source and the holographic recording occurred by diffusion with the grating vector parallel to the crystal [0 0 1]-axis. In order to enhance the holographic image quality and reduce noise a polarizing beam splitter (PBS) was positioned at the BTO input and the crystal was tilted around the [0 0 1]-axis. This enabled the orthogonally polarized transmission and diffracted beams to be separated by the PBS, providing the holographic image only. The possibility of performing deformation and strain analysis as well as vibration measurement of small objects was demonstrated. (C) 2007 Elsevier B.V. All rights reserved.

Assignment of the absolute configuration at the sulfur atom of thioridazine metabolites by the analysis of their chiroptical properties: The case of thioridazine 2-sulfoxide

Thioridazine (THD) is a commonly prescribed phenotiazine neuroleptic drug, which is extensively biotransformed in the organism producing as main metabolites sulfoxides and a sulfone by sulfur oxidation Significant differences have been observed in the activity of the THD enantiomers as well as for its main metabolites, and enantioselectivity phenomena have been proved in the metabolic pathway. Here the assignment of the absolute configuration at the sulfur atom of enantiomeric THD-2-sulfoxide (THD-2-SO) has been carried out by circular dichroism (CD) spectroscopy The stereoisomers were separated by HPLC on Chiralpak AS column, recording the CD spectra for the two collected enantiomeric fractions The theoretical electronic CD spectrum has been obtained by the TDDFT/B3LYP/6-31G*. as Boltzmann averaging of the contributions calculated for the most stable conformations of the drug The comparison of the simulated and experimental spectra allowed the absolute configuration at the sulfur atom of the four THD-2-SO stereoisomers to be assigned The developed method should be useful for a reliable correlation between stereochemistry and activity and/or toxicity

Experimental study of the quantum driven pendulum and its classical analog in atom optics

We present experimental results for the dynamics of cold atoms in a far detuned amplitude-modulated optical standing wave. Phase-space resonances constitute distinct peaks in the atomic momentum distribution containing up to 65% of all atoms resulting from a mixed quantum chaotic phase space. We characterize the atomic behavior in classical and quantum regimes and we present the applicable quantum and classical theory, which we have developed and refined. We show experimental proof that the size and the position of the resonances in phase space can be controlled by varying several parameters, such as the modulation frequency, the scaled well depth, the modulation amplitude, and the scaled Planck’s constant of the system. We have found a surprising stability against amplitude noise. We present methods to accurately control the momentum of an ensemble of atoms using these phase-space resonances which could be used for efficient phase-space state preparation.

Foil based atom chip for Bose-Einstein condensates

We describe a novel method of fabricating atom chips that are well suited to the production and manipulation of atomic Bose–Einstein condensates. Our chip was created using a silver foil and simple micro-cutting techniques without the need for photolithography. It can sustain larger currents than conventional chips, and is compatible with the patterning of complex trapping potentials. A near pure Bose–Einstein condensate of 4 × 104 87Rb atoms has been created in a magnetic microtrap formed by currents through wires on the chip. We have observed the fragmentation of atom clouds in close proximity to the silver conductors. The fragmentation has different characteristic features to those seen with copper conductors.

Enhanced flow visualisation using near-resonant holographic interferometry

Holographic interferometry measurements have been performed on high-speed, high-temperature gas flows with a laser output tuned near a resonant sodium transition. The technique allows the detection and quantification of the sodium concentration in the flow. By controlling the laser detuning and seeded sodium concentration, we performed flow visualization in low-density flows that are not normally detectable with standard interferometry. The technique was also successfully used to estimate the temperature in the boundary layer of the flow over a flat plate.

Quantum trajectory simulations of the fluorescence intensity from a two-level atom driven by a multichromatic field

The quantum trajectories method is illustrated for the resonance fluorescence of a two-level atom driven by a multichromatic field. We discuss the method for the time evolution of the fluorescence intensity in the presence of bichromatic and trichromatic driving fields. We consider the special case wherein one multichromatic field component is strong and resonant with the atomic transition whereas the other components are much weaker and arbitrarily detuned from the atomic resonance. We find that the phase-dependent modulations of the Rabi oscillations, recently observed experimentally [Q. Wu, D. J. Gauthier, and T. W. Mossberg, Phys. Rev. A 49, R1519 (1994)] for the special case when the weaker component of a bichromatic driving field is detuned from the atomic resonance by the strong-field Rabi frequency, appear also for detunings close to the subharmonics of the Rabi frequency. Furthermore, we show that for the atom initially prepared in one of the dressed states of the strong field component the modulations are not sensitive to the phase. We extend the calculations to the case of a trichromatic driving field and find that apart from the modulations of the amplitude there is a modulation of the frequency of the Rabi oscillations. Moreover, the time evolution of the fluorescence intensity depends on the phase regardless of the initial conditions and a phase-dependent suppression of the Rabi oscillations can be observed when the sideband fields are tuned to the subharmonics of the strong-field Rabi frequency. [S1050-2947(98)03501-X].

An atom-optical Maxwell demon

The separation, by an optical standing wave, of a beam of two-level atoms prepared in a thermal mixture of ground and excited states, is considered as an example of a Maxwell demon. By including the momentum exchanged with the cavity, it is shown how no violation of the second law is possible. A classical and quantum analysis is given which illustrates this principle in some detail.

Index of refraction of a two-level atom in a squeezed vacuum field

We study the index of refraction of a two-level atom replacing the usually applied coherent driving fields by a squeezed vacuum field. This system can produce a large index of refraction accompanied by vanishing absorption when the carrier frequency of the squeezed vacuum is detuned from the atomic resonance. (C) 1998 Elsevier Science B.V.

Stationary lineshape of a two-level atom in a narrow-bandwidth squeezed vacuum

The stationary lineshape of a two-level atom driven by low-intensity narrow-bandwidth squeezed light is shown to exhibit significant differences in behaviour compared to the lineshape for broadband squeezed light. We find that for narrow-bandwidth squeezed light the lineshape is composed of two Lorentzians whose amplitudes depend on the squeezing correlations. Moreover, one of the Lorentzians has a negative weight which leads to narrowing of the line. These features are absent in the broadband case, where the stationary lineshape is the same as for a thermal field. (C) 1998 Elsevier Science B.V.

Analytical solution for the Mollow and Autler-Townes probe absorption spectra of a three-level atom in a squeezed vacuum

The Mellow and Autler-Townes probe absorption spectra of a three-level atom in a cascade configuration with the lower transition coherently driven and also coupled to a narrow bandwidth squeezed-vacuum field are studied. Analytical studies of the modifications caused by the finite squeezed-vacuum bandwidth to the spectra are made for the case when the Rabi frequency of the driving field is much larger than the natural linewidth. The squeezed vacuum center frequency and the driving laser frequency are assumed equal. We show that the spectral features depend on the bandwidth of a squeezed vacuum field and whether the sources of the squeezing field are degenerate (DPA) or nondegenerate (NDPA) parametric amplifiers. In a broadband or narrow bandwidth squeezed vacuum generated by a NDPA, the central component of the Mellow spectrum can be significantly narrower than that in the normal vacuum. When the source of the squeezed vacuum is a DPA, the central feature is insensitive to squeezing. The Rabi sidebands, however, can be significantly narrowed only in the squeezed vacuum produced by the DPA. The two lines of the Autler-Townes absorption spectrum can be narrowed only in a narrow bandwidth squeezed vacuum, whereas they are independent of the phase and are always broadened in a broadband squeezed vacuum.

Emission and holographic interferometry measurements in a superorbital expansion tube

Free-piston-driven expansion tubes are capable of generating flaw conditions over a wide range of enthalpies ranging from orbital up to superorbital velocities. Initial optical measurements aimed at investigating the flow in such a facility are presented. Emission studies were used to identify impurities in the how and to investigate spectral regions that are accessible by optical techniques. At moderate enthalpies, it was found that significant radiation resulted from metallic contaminants. At high enthalpies, the spectrum consisted of a number of atomic lines together with a broadband background component indicative of the presence of electrons. The presence of this radiation may limit the applicability of optical techniques that require spectral regions free from the influence of atomic transitions or background radiation. Emission spectroscopy (through Stark broadened hydrogen lines) and two-wavelength holographic interferometry were used to measure the electron number density behind a bow shock on a blunt body at conditions where significant ionization was observed. They yielded average concentrations of (3 +/- 1) x 10(17) cm(-3) from the emission measurements and (3.8 +/- 0.6) x 10(17) cm(-3) from the interferometry.

Shift of the subharmonic resonances and suppression of fluorescence in a two-level atom driven by a bichromatic field

We study the behavior of a two-level atom that is driven by a bichromatic field consisting of a strong resonant component and a weaker tunable component. In addition to the splitting of the energy levels (the multiphoton AC Stark effect), we find that the weaker component also shifts the subharmonic resonances, an effect we attribute to a dynamic Stark shift. When the weaker component is tuned to a shifted resonance, no fluorescence occurs at either the frequency of the strong component or the three-photon mixing frequency. Results are obtained with numerical techniques and explained in terms of the dressed-atom model of the system. (C) 1998 Optical Society of America [S0740-3224(98)01508-2] OCIS codes: 270.4180, 270.6620, 270.0270.

Multiphoton ac Stark effect in a bichromatically driven two-level atom

We study the interaction of a two-level atom with two lasers of different frequencies and amplitudes: a strong laser of Rabi frequency 2 Ohm(1) on resonance with the atomic transition, and a weaker laser detuned by subharmonics (2 Ohm(1)/n) of the Rabi frequency of the first. We find that under these conditions the second laser couples the dressed states created by the first in an n-photon process, resulting in doubly dressed states and in a ''multiphoton ac Stark'' effect. We calculate the eigenstates of the doubly dressed atom and their energies, and illustrate the role of this multiphoton ac Stark effect in its fluorescence, absorption, and Autler-Townes spectra. [S1050-2947(98)07607-0].

Two-level atom in a squeezed vacuum with finite bandwidth

The resonance fluorescence of a two-level atom driven by a coherent laser field and damped by a finite bandwidth squeezed vacuum is analysed. We extend the Yeoman and Barnett technique to a non-zero detuning of the driving field from the atomic resonance and discuss the role of squeezing bandwidth and the detuning in the level shifts, widths and intensities of the spectral lines. The approach is valid for arbitrary values of the Rabi frequency and detuning but for the squeezing bandwidths larger than the natural linewidth in order to satisfy the Markoff approximation. The narrowing of the spectral lines is interpreted in terms of the quadrature-noise spectrum. We find that, depending on the Rabi frequency, detuning and the squeezing phase, different factors contribute to the line narrowing. For a strong resonant driving field there is no squeezing in the emitted field and the fluorescence spectrum exactly reveals the noise spectrum. In this case the narrowing of the spectral lines arises from the noise reduction in the input squeezed vacuum. For a weak or detuned driving field the fluorescence exhibits a large squeezing and, as a consequence, the spectral lines have narrowed linewidths. Moreover, the fluorescence spectrum can be asymmetric about the central frequency despite the symmetrical distribution of the noise. The asymmetry arises from the absorption of photons by the squeezed vacuum which reduces the spontaneous emission. For an appropriate choice of the detuning some of the spectral lines can vanish despite that there is no population trapping. Again this process can be interpreted as arising from the absorption of photons by the squeezed vacuum. When the absorption is large it may compensate the spontaneous emission resulting in the vanishing of the fluorescence lines.