Ultrahigh-resolution saturation spectroscopy using slow molecules in an external cell

We present the narrowest molecular lines so far recorded in the 10 µm spectral region. A linewidth of 80 Hz (HWHM) has been obtained for theP(39)A ₁ ³ (–) line of OsO₄, by selecting slow molecules (T _eff=0.6 K) in saturation spectroscopy at low laser fields (30 nW) and low pressures (2 × 10^–6 Torr). In these conditions, the contribution of the fast molecules is greatly reduced because of the finite size of the beam. This method, applied previously to methane at 3.39 µm, is used for the first time in an external cell and improves by a factor 8 the best resolution of our spectrometer. Heterodyne detection and double frequency modulation have been necessary to extract a signal at a contrast of only 10^–6. The physical ideas concerning this regime are described and a detailed analysis of the line shape is given.     

Spectroscopic properties of Cr4+-doped LiAlO2

The spectroscopic properties of the new potential laser material Cr⁴⁺:LiAlO₂ are presented. LiAlO₂ exhibits tetrahedrally coordinated lattice sites only. Doping the crystal with chromium only as well as additional codoping with magnesium yields the incorporation of Cr⁴⁺ on the Al site. The Cr⁴⁺ emission extends from 1.1 to 1.7µm. In the case of doping just with chromium, the lifetime is single exponential in the whole temperature range between 12 and 550 K with a room-temperature lifetime of 29µs and a low-temperature lifetime of 95µs, which are the longest lifetimes observed until now for Cr⁴⁺ systems. Codoping with magnesium yields an additional Cr⁴⁺ center, which is clearly observed both in the decay dynamics and in the low-temperature emission spectrum.     

Quantized infrared-optical triple resonance on a single cold barium ion

A single trapped and cooled Ba⁺ ion is irradiated by resonant visible light (493, 650 nm) alternating with light at 1.76 µm which may excite the ion to its² D _5/2 metastable state. The (absence of) visible resonance scattering probes the excitation, tuning spectra of which show vibrational sidebands that characterize the ion's temperature. Observed values as low as 120 µK, one-eighth the Doppler limit, are ascribed to electronic Raman cooling by the visible light. Tuning spectra of the events of stimulated deexcitation indicate ion heating by the IR interaction. The results demonstrate the feasibility of vibrational spectrometry on a single particle that oscillates in a potential well, forming a quasi-molecule.     

Magnetic anisotropy in (, .44, .55, .67, and .78) alloy film grown on and MgO(001) by molecular beam epitaxy

Fe_xPd_1−x (x=.30, .44, .55, .67, and .78) films were directly grown on SrTiO₃(001) and MgO(001) by molecular beam epitaxy at 500 C. The thickness of all films is 50 nm. X-ray diffraction shows epitaxial quality and face-center- tetragonal (00l), (002), and (003) peaks indicating an FePd L1₀ order state for films of x=.30, .44 and .55. X-ray diffraction only shows (002) peaks with a relatively weak intensity for the film of x=.67 and no (00l) peak is observed, but a broad body-center-cubic Fe(002) is identified for the film of x=.78. Magnetic hysteresis curves are carried out by a vibrating sample magnetometer (VSM) with an applied field within 12 kOe. Magnetization of both in-plane and perpendicular-to- the-plane measurements show a linear increase of the magnetization saturation from 560 emu/cm³ to 1250 emu/cm³ as x increasing from .30 to .78. For the results of the in-plane measurements, remanence (M_r), however, shows a minimum while the anisotropy field (H_k) shows a maximum for the film with x=.44 indicating the optimal content ratio of Fe/Pd for perpendicular anisotropy in the present alloy films. Further, negative remanence is observed in the hysteresis curves where the field is perpendicular to the film of x=.78 This may indicate that the L1₀order state still affects the magnetic anisotropy for high Fe content films even though the film has a body-center-cubic structure.     

Spectroscopic studies of laser-produced plasmas formed in CO and CO2 using 193, 266, 355, 532 and 1064 nm laser radiation

The wavelength dependence of laser-produced breakdown in air, CO and CO₂ has been studied using the four Nd:YAG harmonics (266 nm, 355 nm, 532 nm and 1064 nm) and the ArF-excimer laser (193 nm). Breakdown thresholds at these wavelengths are reported for air, CO and CO₂. A significant reduction in the breakdown thresholds for both CO and CO₂ is apparent when comparing 193 nm with the four Nd:YAG harmonics. This reduction is attributed to the resonance-enhanced two-photon ionization of metastable carbon atoms generated in the laser focus at the ArF-laser wavelength. In addition to reporting breakdown thresholds, the laser-produced plasmas in CO and CO₂ are characterized in terms of plasma temperatures and electron densities which are measured by time-resolved emission spectroscopy. Electron densities range from 9 × 10¹⁷ cm^–3 to 1 × 10₁₇ cm^–3. Excitation temperatures range from 22 000 K at 0.2 µs to 11 000 K at 2 µs. Ionization temperatures range from 22 000 K at 0.1 µs to 16 000 K at 2 µs. Evidence is presented to indicate that, like ArF-laser-produced plasmas, Nd:YAG-laser-produced plasmas formed in CO and CO₂ are in or near a state of Local Thermodynamic Equilibrium (LTE) soon after their formation.     

Fluorescence and attenuation properties of Er3+ -doped phosphate-glass fibers and efficient infrared-to-visible up-conversion

Fluorescence spectra of phosphate glasses with different erbium doping have been measured. The flourescence intensity reaches its maximum at an Er³⁺-doping concentration of 0.75 mol%. When the Er³⁺ doping exceeds 0.75 mol%, the fluorescence intensity decreases due to concentration quenching. The attenuation at 1.53 µm of the fiber is 12.8 db/m. The fluorescence up-conversion of 1.064 µm Nd:YAG laser pulses into intense green 547 and 667 nm light in the fiber has been measured. The fluorescence output power of green (547 nm) and red (667 nm) light is 178 and 42 W, respectively with an excitation power of 1 W. The two signals are referred to as⁴ S _3/2 ⁴ I _{1 5/2} and⁴ F _9/2 ⁴ I _{1 5/2} transitions through two-photon absorption fluorescence.     

Rotational and vibrational temperature determination by DFWM spectroscopy

Using the DFWM technique we determined rotational and vibrational temperatures of NaH molecules in a dynamical system consisting of NaH, Na, H and H₂ for several heat-pipe oven temperatures. We applied a new way to determine the dependence of the DFWM signalI _c ^int on the power of the transition dipole momentµ without previous knowledge of the temperature. The revealed dependence isI _c ^int µ ⁴. In this case the laser intensities were found to be of the same order as the saturation intensity in accordance with simple DFWM theory. A usual Boltzmann plot was employed for the determination of the relevant rotational temperatures, which displayed higher values than the oven temperature.     

Large-scale collisional energy transfer in laser-pumped metastable Ca atoms: Excitation of resonance states of Ca II

We report the first experimental observation of the excitation of the 4p ² P _{3/2, 1/2} resonance states of Ca II (located at 74 720.4 and 74 497.5 cm^–1 above the ground state of Ca I) following pulsed-laser pumping of the 4s ^{2 1} S _O–4s4p ³P₁ intercombination transition of Ca I (E _ex = 15 210 cm^–1). Large scale collisional transfer of energy between the laser-excited atoms is believed to be responsible for this. This is possibly because sufficient time is available (_rad of the 4s4p ³ P ₁ state is approximately 350 µs) for collisions to build such a high level of excitation. Some interesting additional features of the fluorescence spectra of the laser-pumped Ca vapor, such as temperature dependence of the fluorescence intensities and evolution in time of some selected states, are also presented.     

Muonic atom-nucleus collisions in the energy region of dtµ, resonant states

We calculated the (dµ) _n=1 +t scattering in the energy region of the (dtµ)^* resonant states below then=2 level of the tµ atom. From the cross sections, we estimated the resonant energies, widths and branching ratios. We found eleven resonant states with angular momentumJ=0, and some of their resonant energies relative to then=2 level of tµ are small enough to form the [(dtµ)^* dee] by the Vesman mechanism. These resonant states decay to (dµ)[inn=1 +t or (tµ) _n=1 + d scattering states. The total decay rates are about 10¹¹ s^–1 which is three orders of magnitude larger than the fusion rates of (dtµ)^*4 He + n+ 17.6 MeV + µ. The main part of the decaying channel from the shallow resonant states is the (dµ) _n=1 +t channel. The branching ratios of the (dµ) _n=1 +t decay channel are around 0.9. Most of the muons that reach to then=2 states of tµ can transfer to then=1 state of du through (tµ) _n=2 + D₂ [(dtµ)^*dee] and (dtµ)^* (dµ) _n=1 +t processes.     

Single α-particle orbits and Bose-Einstein condensation in <Superscript>12</Superscript>C

Bosonic properties of α particles such as single-α orbits and occupation numbers in J^π = 0⁺, 2⁺, 1^- and 3^- states of ¹²C around the 3α threshold are investigated with the semi-microscopic 3α cluster model. As in other studies, we found that the 0⁺₂ (2⁺₂) state has dilute-3α-condensate-like structure in which the α particle is occupied in the single S (D) orbit with about 70% (80%) probability. The radial behaviors of the single-α orbits as well as the occupation numbers are discussed in detail in comparison with those for the 0⁺₁ and 2⁺₁ states together with the 1^-₁ and 3^-₁ states.     

Spectroscopic characterization and laser performance of diode-laser-pumped Nd: GdVO4

We have carried out a detailed spectroscopic characterization of Nd: GdVO₄, a new laser crystal with high effective absorption and emission cross sections. The accidental degeneracy of the upper⁴ F _3/2 laser level decreases the number of emission lines and creates -together with the anisotropic crystal field - high emission cross sections (7.6 × 10^–19 cm² at 1.06 µm and 300 K). In addition, the lines are strongly homogeneously broadened (1.6 nm for the 808.4 nm diode-laser pump transition). The temperature dependences of lifetime, linewidths, and cross sections have been determined. Slope efficiencies up to 57% with respect to the absorbed diode-laser pump power and output powers up to 0.8 W have been achieved at 1.06 µm from a 2 mm long crystal. Intracavity second-harmonic generation, using a KTP crystal, is demonstrated.     

Electrochemical behaviour of sputtered c-V2O5 and LiCoO2 thin films for solid state lithium microbatteries

Here are reported for the first time electrochemical data on all-solid-state lithium microbatteries using crystalline sputtered V₂O₅ thin films as cathode materials and LiPON as solid electrolyte. The stable specific capacity of 30 µAh/cm² found with a 2.4 µm thick film competes very well with the best values obtained for solid state microbatteries using amorphous films. With the challenge of decreasing the temperature of heat treatment for sputtered LiCoO₂ thin films, we show that a temperature of 500 °C combined with an optimized bias sputtering (-50 V) allows to get highly crystalline deposits, to minimize the presence of Co₃O₄ and to suppress any trace of the cubic phase. At the same time the theoretical specific capacity is reached in the 4.2 V-3 V range and a good cycling behaviour is achieved with a high capacity of 50 µAh/cm²/µm after 140 cycles at 10 µA.cm².     

CO-laser side-band spectrometer: Sub-Doppler heterodyne frequency measurements around 5 µm

We report the realization of a tunable sub-Doppler heterodyne spectrometer with high absolute accuracy, employing side-band generation with a CO laser. The fixed-frequency CO-gas laser, working from 4.7 to 8.4µm, is made partially tunable by the use of microwave side-band generation in a CdTe Electro-Optical Modulator (EOM). This leads to tunable radiation of high spectral purity. We describe the design of the microwave EOM, adapted to the CO laser, its performance and its first application to highly accurate frequency measurements. The side-band radiation is used for sub-Doppler stabilization of the CO laser, while the carrier frequency is mixed with the frequencies of two CO₂ reference lasers. As a first result, we present measurements of OCS transitions in the 4.9µm (61 THz) region, reaching an absolute accuracy of 30 kHz (/ = 5×1O^–10). Further application of our spectrometer to calibration gases will establish a variety of InfraRed (IR) calibration standards with a new quality of accuracy. On visit from: Fachbereich Physik, Humboldt-Universität zu Berlin     

The prediction of periods of high volatility in exchange markets

A statistical connection is identified between the current spread in a market over a given time period and the drift of the market during previous time periods. It is shown that periods of high spread are likely to be preceded by periods with relatively large market drifts. Several markets, including the UK pound per US Dollar, US Dollar per Yen, UK pound per Euro, and the UK FT100 index have been analysed from 1991 to 2000 over variable periods of weeks, months and quarters. Within each period, i the natural logarithm of the daily end-of-trade market value has been least squares fitted to a linear regression line, and evaluations made of the regression line slope μ _i, the direct spread s_i with respect to the mean value, and the regression spread r_i of the deviations from the regression line. Significant correlations have been observed between the current monthly direct spread s_i for each period i and the absolute value of the drifts |μ _i-j| evaluated j periods earlier. This correlation coefficient is as high as 0.746 for a period of one quarter (j = 1) and appears to die away after around 9 months for quarterly averages, after around 4 months for monthly averages and after around 2 months for weekly averages. Received 11 October 2000     

Shear mechanical anisotropy of side chain liquid-crystal elastomers: Influence of sample preparation

We study the mechanical anisotropy of a series of uniaxial side chain nematic elastomers prepared with the same chemical composition but with different preparation protocols. For all the compounds, the experiments performed as a function of temperature show no discontinuity in both G' _// and G' _⊥ (the labels // and ⊥ stand for the director parallel, respectively perpendicular to the shear displacement) around the nematic-isotropic (N-I) phase transition temperature determined by DSC. They also all show a small decrease in G' _// starting at temperatures well above this temperature (from ∼ 4^° C to ∼ 20^° C depending on the compound studied) and leading to a small hydrodynamic value of the G' _⊥/G' _// ratio. The measurements taken as a function of frequency show that the second plateau in G' _// and the associated dip in G _//” expected from dynamic semi-soft elasticity are not observed. These results can be described by the de Gennes model, which predicts small elastic anisotropy in the hydrodynamic and linear regimes. They correspond to the behavior expected for compounds beyond the mechanical critical point, which is consistent with the NMR and specific heat measurements taken on similar compounds. We also show that a reduction in the cross-linking density does not change the non-soft character of the mechanical response. From the measurements taken as a function of frequency at several temperatures we deduce that the time-temperature superposition method does not apply. From these measurements, we also determine the temperature dependence of the longest relaxation time τ_E of the network for the situations where the director is either parallel or perpendicular to the shear velocity. Finally, we discuss the influence on the measurements of the mechanical constraint associated with the fact that the samples cannot change their shape around the pseudo phase transition, because of their strong adherence on the sample-bearing glass slides.     

High frequency sound and the boson peak in amorphous silica

We present the results of extensive molecular dynamics computer simulations in which the high frequency dynamics of silica, i.e. for frequencies ν > 0.5 THz, is investigated in the viscous liquid state as well as in the glass state. We characterize the properties of high frequency sound modes by analyzing J _l(q,ν) and J _t(q,ν), the longitudinal and transverse current correlation function, respectively. For wave-vectors q > 0.4 ?^-1 the spectra are sitting on top of a flat background. The dynamic structure factor S(q,ν) exhibits for q > 0.23 ?^-1 a boson peak which is located nearly independent of q around 1.7 THz and for which the intensity scales approximately linearly with temperature. We show that the low frequency part of the boson peak is mainly due to the elastic scattering of transverse acoustic modes with frequencies around 1 THz. The strength of this scattering depends on q and is largest around q = 1.7 ?^-1, the location of the first sharp diffraction peak in the static structure factor. By studying S(q,ν) for different system sizes we show that strong finite size effects are present in the low frequency part of the boson peak in that for small systems part of its intensity is missing. We discuss the consequences of these finite size effects for the structural relaxation. Received 27 June 2000 and Received in final form 9 January 2001     

Photoproduction of neutral pion pairs from the proton

Double neutral pion photoproduction from the proton has been measured at MAMI for photon energies between threshold and 820 MeV. The reaction was identified by an invariant mass and missing mass analysis. From threshold up to 370 MeV the total cross-section does not exceed 30 nb. For higher energies it shows a smooth rise until it reaches a maximum of about 10 μb at E _γ = 740 MeV. Dalitz plots of m ²(π⁰π⁰) versus m ²(p,π⁰) for seven bins of incident photon energy have been analysed. For E _γ > 610 MeV, a strong contribution of a sequential decay is observed with the Δ(1232)-resonance as intermediate state. A comparison to model calculations shows that these sequential decays presumably originate from the D ₁₃(1520) and also the P ₁₁(1440)-resonance. Received: 6 June 2000 / Accepted: 18 August 2000     

Frequency chain towards the Ca intercombination line based on laser diodes: First step

Stable, narrow linewidth operation of red and 1.3 µm free-running laser diodes with external gratings in non-Littrow geometry is demonstrated. The resonance of the saturated fluorescence of an atomic beam with a contrast of 25% and a linewidth of 400 ± 50 kHz of the Ca intercombination line 4¹ S ₀–4³ P ₁ ( = 657 nm) is shown. A high-power (110 mW) single-mode external cavity laser diode at 1.3 µm is used for second-harmonic generation in a KTP crystal. The beat signal (signal to noise ratio about 25 dB) of 10 nW second-harmonic radiation at 1.3 µm and the radiation of a laser diode in the visible spectrum, as a step to realize a frequency chain, is observed.     

Vibrational wave packet dynamics in the silver tetramer probed by NeNePo femtosecond pump-probe spectroscopy

We present results on the ultrafast dynamics of mass-selected neutral Ag₄ clusters using NeNePo (negative ion - neutral - positive ion) femtosecond pump-probe spectroscopy. One-color pump-probe spectra of the Ag₄ ^-/Ag₄/Ag₄ ⁺ system measured at 385 nm and an internal cluster temperature of 20 K display a complex beat structure over more than 60 ps. The oscillatory structure is attributed to vibrational wave packet dynamics in an excited “dark" state of neutral Ag₄. A dominant 740 fs wave packet period as well as wave packet dephasing and rephasing are observed in the spectra. Fourier analysis of the spectra yields a group of frequencies centered around 45 cm^-1 and an anharmonicity χ _e2νχ _eχ _e of 2.65 cm^-1 for the active vibrational mode. Received 30 November 2000     

Efficient laser isotope separation of 13C using novel linear multi-pass cavity

¹³C isotope has been separated in the form of enriched product C₂F₄ by selective multi-photon dissociation (MPD) of Freon-22 (CHClF₂) using the 9P(26) laser line of a transversely excited atmospheric CO₂ laser. The non-linearity factor, γ, that determines the dependence of the yield of ¹³C isotope on the fluence (J/cm²) has been determined for various laser rotational lines (9P(20)–9P(26)) and the advantage of a lower γ in the case of 9P(26) is highlighted for macroscopic production of ¹³C isotope. It is also shown that a higher value of the optimum fluence at 9P(26) not only results in a higher enrichment efficiency but in a relatively lower value of γ also. The laser pulse energy is efficiently utilized for selective MPD of Freon-22 by focusing the pulse energy repeatedly with the help of a novel linear multi-pass cavity (LMPC). The novelty of this optical arrangement lies in its ability to maintain the laser fluence around an optimum value for a desired enrichment of ¹³C in the product. This also ensures a higher quantity of enriched product because of the higher reaction volume. The advantage of the LMPC over the conventionally used Herriott multi-pass cell has also been presented. The gain in reaction volume in the present optical cavity having 20 passes with a constant fluence in each pass is as high as 12. Isotope-selective MPD of Freon in a LMPC with constant fluence in each pass showed a distinct advantage in energy utilization to separate ¹³C isotope over the gradually reducing fluence case.This revised version was published online in August 2005 with a corrected cover date.