100 resultados para f-f transitions


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Non-Markovian behaviour in atomic systems coupled to a structured reservoir of quantum EM field modes, such as in high Q cavities, is treated using a quasimode description, and the pseudo mode theory for single quantum reservoir excitations is obtained via Fano diagonalisation. The atomic transitions are coupled to a discrete set of (cavity) quasimodes, which are also coupled to a continuum set of (external) quasimodes with slowly varying coupling constants. Each pseudomode corresponds to a cavity quasimode, and the original reservoir structure is obtained in expressions for the equivalent atom-true mode coupling constants. Cases of multiple excitation of the reservoir are now treatable via Markovian master equations for the atom-discrete quasimode system.

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With the exception of the sodium D-lines, recent calculations of line broadening cross sections for several multiplets of sodium by Leininger et al (Leininger T, Gadea F X and Dickinson A 2000 J. Phys. B: At. Mol. Opt. Phys. 33 1805) are in substantial disagreement with cross sections interpolated from the tables of Anstee and O'Mara (Anstee and O'Mara 1995 Mon. Not. R. Astron. Soc. 276 859) and Barklem and O'Mara (Barklem P S and O'Mara B J 1997 Mon. Not. R. Astron. Soc. 290 102). The discrepancy is as large as a factor of 3 for the 3p-4d multiplet. The two theories are tested by using the results of each to synthesize lines in the solar spectrum. It is found that generally the data from the theory of Anstee, Barklem and O'Mara produce the best match to the observed solar spectrum. It is found, using a simple model for reflection of the optical electron by the potential barrier between the two atoms, that the reflection coefficient is too large for avoided crossings with the upper states of subordinate lines to contribute to line broadening, supporting the neglect of avoided ionic crossings by Anstee, Barklem and O'Mara for these lines. The large discrepancies between the two sets of calculations is a result of an approximate treatment of avoided ionic crossings for these lines by Leininger et al (Leininger T, Gadea F X and Dickinson A 2000 J. Phys. B: At. Mol. Opt. Phys. 33 1805).

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Motion of chains of poly(ethylene oxide) within the interlayer spacing of 2:1 phyllosilicate/montmorillonite was studied with H-1 and C-13 NMR spectroscopy. Measurements of the H-1 NMR line widths and relaxation times across a large temperature range were used to determine the effect of bulk thermal transitions on polymer chain motion within the nanocomposites. The results were consistent with previous reports of low apparent activation energies of motion. Details of the frequency and geometry of motion were obtained from a comparison of the C-13 cross-polarity/magic-angle spinning spectra and relaxation times of the nanocomposite with those of the pure polymer. (C) 2001 John Wiley & Sons, Inc.

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Mutations in the extracellular M2-M3 loop of the glycine receptor (GlyR) alpha1 subunit have been shown previously to affect channel gating. In this study, the substituted cysteine accessibility method was used to investigate whether a structural rearrangement of the M2-M3 loop accompanies GlyR activation. All residues from R271C to V277C were covalently modified by both positively charged methanethiosulfonate ethyltrimethylammonium (MTSET) and negatively charged methanethiosulfonate ethylsulfonate (MTSES), implying that these residues form an irregular surface loop. The MTSET modification rate of all residues from R271C to K276C was faster in the glycine-bound state than in the unliganded state. MTSES modification of A272C, L274C, and V277C was also faster in the glycine-bound state. These results demonstrate that the surface accessibility of the M2-M3 loop is increased as the channel transitions from the closed to the open state, implying that either the loop itself or an overlying domain moves during channel activation.

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We discuss the connection between quantum interference effects in optical beams and radiation fields emitted from atomic systems. We illustrate this connection by a study of the first- and second-order correlation functions of optical fields and atomic dipole moments. We explore the role of correlations between the emitting systems and present examples of practical methods to implement two systems with non-orthogonal dipole moments. We also derive general conditions for quantum interference in a two-atom system and for a control of spontaneous emission. The relation between population trapping and dark states is also discussed. Moreover, we present quantum dressed-atom models of cancellation of spontaneous emission, amplification on dark transitions, fluorescence quenching and coherent population trapping.

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This paper deals with atomic systems coupled to a structured reservoir of quantum EM field modes, with particular relevance to atoms interacting with the field in photonic band gap materials. The case of high Q cavities has been treated elsewhere using Fano diagonalization based on a quasimode approach, showing that the cavity quasimodes are responsible for pseudomodes introduced to treat non-Markovian behaviour. The paper considers a simple model of a photonic band gap case, where the spatially dependent permittivity consists of a constant term plus a small spatially periodic term that leads to a narrow band gap in the spectrum of mode frequencies. Most treatments of photonic band gap materials are based on the true modes, obtained numerically by solving the Helmholtz equation for the actual spatially periodic permittivity. Here the field modes are first treated in terms of a simpler quasimode approach, in which the quasimodes are plane waves associated with the constant permittivity term. Couplings between the quasimodes occur owing to the small periodic term in the permittivity, with selection rules for the coupled modes being related to the reciprocal lattice vectors. This produces a field Hamiltonian in quasimode form. A matrix diagonalization method may be applied to relate true mode annihilation operators to those for quasimodes. The atomic transitions are coupled to all the quasimodes, and the true mode atom-EM field coupling constants (one-photon Rabi frequencies) are related to those for the quasimodes and also expressions are obtained for the true mode density. The results for the one-photon Rabi frequencies differ from those assumed in other work. Expressions for atomic decay rates are obtained using the Fermi Golden rule, although these are valid only well away from the band gaps.

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Field quantization in unstable optical systems is treated by expanding the vector potential in terms of non-Hermitean (Fox-Li) modes. We define non-Hermitean modes and their adjoints in both the cavity and external regions and make use of the important bi-orthogonality relationships that exist within each mode set. We employ a standard canonical quantization procedure involving the introduction of generalized coordinates and momenta for the electromagnetic (EM) field. Three-dimensional systems are treated, making use of the paraxial and monochromaticity approximations for the cavity non-Hermitean modes. We show that the quantum EM field is equivalent to a set of quantum harmonic oscillators (QHOs), associated with either the cavity or the external region non-Hermitean modes, and thus confirming the validity of the photon model in unstable optical systems. Unlike in the conventional (Hermitean mode) case, the annihilation and creation operators we define for each QHO are not Hermitean adjoints. It is shown that the quantum Hamiltonian for the EM field is the sum of non-commuting cavity and external region contributions, each of which can be expressed as a sum of independent QHO Hamiltonians for each non-Hermitean mode, except that the external field Hamiltonian also includes a coupling term responsible for external non-Hermitean mode photon exchange processes. The non-commutativity of certain cavity and external region annihilation and creation operators is associated with cavity energy gain and loss processes, and may be described in terms of surface integrals involving cavity and external region non-Hermitean mode functions on the cavity-external region boundary. Using the essential states approach and the rotating wave approximation, our results are applied to the spontaneous decay of a two-level atom inside an unstable cavity. We find that atomic transitions leading to cavity non-Hermitean mode photon absorption are associated with a different coupling constant to that for transitions leading to photon emission, a feature consequent on the use of non-Hermitean mode functions. We show that under certain conditions the spontaneous decay rate is enhanced by the Petermann factor.

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We develop a systematic theory of critical quantum fluctuations in the driven parametric oscillator. Our analytic results agree well with stochastic numerical simulations. We also compare the results obtained in the positive-P representation, as a fully quantum-mechanical calculation, with the truncated Wigner phase-space equation, also known as the semiclassical theory. We show when these results agree and differ in calculations taken beyond the linearized approximation. We find that the optimal broadband noise reduction occurs just above threshold. In this region where there are large quantum fluctuations in the conjugate variance and macroscopic quantum superposition states might be expected, we find that the quantum predictions correspond very closely to the semiclassical theory.

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We develop a systematic theory of quantum fluctuations in the driven optical parametric oscillator, including the region near threshold. This allows us to treat the limits imposed by nonlinearities to quantum squeezing and noise reduction in this nonequilibrium quantum phase transition. In particular, we compute the squeezing spectrum near threshold and calculate the optimum value. We find that the optimal noise reduction occurs at different driving fields, depending on the ratio of damping rates. The largest spectral noise reductions are predicted to occur with a very high-Q second-harmonic cavity. Our analytic results agree well with stochastic numerical simulations. We also compare the results obtained in the positive-P representation, as a fully quantum-mechanical calculation, with the truncated Wigner phase-space equation, also known as the semiclassical theory.

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We investigate the influence of a single-mode cavity on the Autler-Townes doublet that arises when a three-level atom is strongly driven by a laser field tuned to one of the atomic transitions and probed by a tunable, weak field coupled to the other transition. We assume that the cavity mode is coupled to the driven transition and the cavity and laser frequencies are equal to the atomic transition frequency. We find that the Autler-Townes spectrum can have one, two or three peaks depending on the relative magnitudes of the Rabi frequencies of the cavity and driving fields. We show that, in order to understand the three-peaked spectrum, it is necessary to go beyond the secular approximation, leading to interesting quantum interference effects. We find that the positions and relative intensities of the three spectral components are affected strongly by the atom-cavity coupling strength g and the cavity damping K. For an increasing g and/or decreasing K the triplet evolves into a single peak. This results in 'undressing' of the system such that the atom collapses into its ground state. We interpret the spectral features in terms of the semiclassical dressed-atom model, and also provide complementary views of the cavity effects in terms of quantum Langevin equations and the fully quantized, 'double -dressing' model.

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l-(BETS)2FeCl4 undergoes transitions from an antiferromagnetic insulator to a metal and then to a superconductor as a magnetic field is increased. We use a Hubbard-Kondo model to clarify the role of the Fe31 magnetic ions in these phase transitions. In the high-field regime, the magnetic field acting on the electron spins is compensated by the exchange field He due to the magnetic ions. We show how He can be extracted from the observed splitting of the Shubnikov–de Haas frequencies. We predict the field range for field-induced superconductivity in other materials.

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The Las Canadas caldera is a nested collapse caldera formed by the successive migration and collapse of shallow magmatic chambers. Among the pyroclastic products of this caldera are phonolitic fallout deposits that crop out in the caldera wall and on the extracaldera slopes. These deposits exhibit an uninterrupted facies gradation from nonwelded to lava-like and record continuous volcanic deposition. Densely welded and lava-like facies result from the extreme attenuation and complete homogenization of juvenile clasts that destroy original clast outlines and any evidence of fallout deposition. Agglutination contributes significantly to the final degree of flattening observed in the welded facies. After deposition, rheomorphic flowage occurs. Emplacement temperatures for one of the welding sequences are calculated from magmatic temperatures and a model of tephra cooling during fallout. Results are 486 degreesC for the nonwelded facies and 740 degreesC for the moderately welded facies. For the same welding sequence, a cooling time between 25 and 54 days is estimated from published experimental and computational data as the possible duration of welding and rheomorphism. Following deposition and agglutination, the lava-like pyroclastic facies had the rheological properties of viscous lavas and flowed down the outer slopes away from the caldera. Some lava-like masses detached from proximal areas to more distal regions. During deposition, the eruptive style evolved from Plinian fallout to fountain-fed spatter deposition. This evolution was accompanied by a decrease in explosive power and a lower height of the eruptive column, which produce higher emplacement temperatures and more effective heat retention of pyroclasts.

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Physical aging of amorphous anhydrous fructose at temperature 5 degreesC and at 22 degreesC was studied using differential scanning calorimetry (DSC). The dynamic glass transitions temperature, T-g0 for unaged samples was 16 degreesC and 13.3 degreesC for heating rate of 10 degreesC/min and 1 degreesC/min, respectively. The fictive temperature, T-f0 for unaged samples calculated by Richardson and Savill method was 12 degreesC, which is close to the dynamic value obtained from the lower DSC heating rate. The fictive temperature T-f of the aged fructose glasses at temperatures both below and above the transition region was fitted well by a non-exponential decay function (Williams-Watts form). Aging above the transition region (22 degreesC) for 18 d increased both the dynamic glass transition temperature T and the fictive temperature T-f. However, aging below the transition region (5 degreesC) for I d increased the dynamic glass transition temperature T-g but decreased the fictive temperature T-f.

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Density functional theory for adsorption in carbons is adapted here to incorporate a random distribution of pore wall thickness in the solid, and it is shown that the mean pore wall thickness is intimately related to the pore size distribution characteristics. For typical carbons the pore walls are estimated to comprise only about two graphene layers, and application of the modified density functional theory approach shows that the commonly used assumption of infinitely thick walls can severely affect the results for adsorption in small pores under both supercritical and subcritical conditions. Under supercritical conditions the Henry's law coefficient is overpredicted by as much as a factor of 2, while under subcritical conditions pore wall heterogeneity appears to modify transitions in small pores into a sequence of smaller ones corresponding to pores with different wall thicknesses. The results suggest the need to improve current pore size distrubution analysis methods to allow for pore wall heterogeneity. The density functional theory is further extended here to allow for interpore adsorbate interactions, and it appears that these interaction are negligible for small molecules such as nitrogen but significant for more strongly interacting heavier molecules such as butane, for which the traditional independent pore model may not be adequate.