Lifetimes of image-potential states on the Pt(111) surface probed by time-resolved two-photon photoemission spectroscopy

We have investigated the population dynamics of image-potential states on the clean Pt(111) surface. The first two image-potential states have been resolved exhibiting lifetimes of 26±7 fs and 62±7 fs. Those lifetimes are in contrast to the (111) surfaces of Ag and Cu, where the n=2 state is degenerate with bulk states leading to lifetimes shorter than 20 fs. Received: 30 March 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

Interstitial iron and iron-acceptor pairs in silicon

Deep levels in iron-dopedp-type silicon are investigated by means of Deep Level Transient Spectroscopy (DLTS) and the Hall effect. Pairs of Fe with the acceptors B, Al, and Ga are observed at 0.1, 0.19, and 0.24 eV above the valence band edgeE _v. For interstitial iron, (Fe _i ), a level energy ofE _v+0.39+-0.02 eV is obtained with DLTS after correction with a measured temperature dependence of the capture cross section. The Hall effect yieldsE _v+0.37 eV for Fe_i. The annealing behavior of levels related to Fe is investigated up to 160 °C. Iron participates in at least four different types of impurity states: Fe _i , Fe-acceptor pairs, precipitations (formed above 120 °C) and an additional electrically inactive state, which is formed at room temperature.     

Laser diagnostics of NO reburning in fuel-rich propene flames

Absolute NO concentrations were measured by laser-induced fluorescence (LIF) in three different fuel-rich non-sooting propene flames (φ=1.5, 1.8 and 2.3). The experiments were performed in low-pressure premixed propene flames with 0.2%-1% NO added. Laser diagnostics was applied as a tool for investigating reburn chemistry. The Q₂(25.5) line in the A-X(0,0) band was excited because of the small temperature dependence of its ground state population. The NO fluorescence lifetimes were measured directly and compared to theoretical values. The initial NO levels are strongly reduced in all three flames. According to modeling results, the HCN mole fraction increases strongly with stoichiometry. As guidelines for laser diagnostics applications in such systems, the modeling results were analyzed with respect to the main reaction channels and reaction partners in fuel-rich flames. Received: 1 March 2000 / Revised version: 20 April 2000 / Published online: 20 September 2000     

Thermal behavior of the roughened Cu(110) surface

The roughened Cu(110) surface was prepared by annealing the clean surface at various temperatures ranging from 700 to ∼1000 K. A significant drop in intensity of reflection anisotropy spectroscopy (RAS) peak at 2.1 eV photon energy as a function of increasing sample temperature was found for annealing above the roughening transition at 900 K. The observed change of 2.1 eV peak in RAS spectra is because of the surface state Fermi level shift due to temperature change. The RAS result is in good agreement with an unoccupied surface state energy using inverse photoemission spectroscopy (IPES). New IPES results indicate that the unoccupied surface state intensity decreases with increasing annealing temperature. It was also found that the unoccupied surface state was shifted. IPES results provide that the contributions of the surface state to surface optical properties at 2.1 eV are relevant for the RAS technique.     

Absolute frequency measurement of the iodine-stabilized He-Ne laser at 633 nm

The absolute frequency of an iodine-stabilized He-Ne laser at 633 nm stabilized on the i (or a₁₃) component of the 11-5 R(127) hyperfine transition of the ¹²⁷I₂ molecule is measured using a femtosecond optical comb generator and an iodine-stabilized Nd:YAG laser standard at 1064 nm. We link the measured absolute frequency to the current internationally adopted value via frequency intercomparison between JILA and the Bureau International des Poids et Mesures (BIPM), leading to the determination of the absolute frequency of the BIPM-4 standard laser. The resulting absolute frequency f_i(BIPM) of the BIPM-4 standard laser is f_i(BIPM)=473612214711.9±2.0 kHz, which is 6.9 kHz higher than the value adopted by the Comité International des Poids et Mesures (CIPM) in 1997. Received: 29 May 2000 / Revised version: 13 September 2000 / Published online: 22 November 2000     

Thermal emission of electrons from highly excited sodium clusters

Positively charged sodium clusters can be easily ionized by a fs laser pulse of relatively low intensity (<10¹⁰ W/cm²), if the laser is in resonance with the plasmon excitation of the cluster. This ionization process was investigated in detail by measuring the kinetic energy distribution of electrons emitted from a size-selected Na₉₃ ⁺ as a function of the fs laser intensity. In all cases pure Boltzmann-like energy distributions were observed. A comparison with statistical theory shows that the emission is a purely thermal process. It is different to normal thermionic emission insofar as the electrons are emitted from a hot electron system which is only weakly coupled to a cold ionic background. The results demonstrate purely statistical behaviour of a small fermionic system even for very high excitation energy. Received: 25 May 2000 / Accepted: 6 November 2000 / Published online: 9 February 2001     

Electronic structure of icosahedral alloys: The case of Al65Cu20Os15

Measurements with photoemission spectroscopy in the photon-energy range 35–130 eV have been used to determine the valence band of the stable icosahedral Al₆₅Cu₂₀Os₁₅. Resonant photoemission near the Os 5p 5d and 4f 5d transitions has been employed to show that the feature in the valence band with the maximum intensity at 1.5 (1) eV below the Fermi level is predominantly of the Os 5d character. This has been additionally verified by conducting the photoemission measurements in the constant-initial-state mode and by using the effect of the Cooper minimum in the photoionization cross section of the Os 5d orbitals. The valence band feature with the maximum intensity at 3.7 (1) eV below the Fermi level has been shown as being due mainly to the states of the Cu 3d character. The Os 5d and Cu 3d empirical partial density of states have been determined from the photoemission spectra. The decrease of intensity towards the Fermi level has been interpreted as being indicative of the presence of a theoretically predicted pseudogap around the Fermi level. It has been indicated, however, that the Fermi cut-off also contributes to the observed intensity decrease. It has been demonstrated that the energy resolution of the spectroscopic measurements performed so far on quasicrystals was not high enough to unambiguously determine the presence of such a pseudogap. No unusual features in the valence band of icosahedral Al₆₅Cu₂₀Os₁₅, which could be ascribed to its quasiperiodic nature, have been observed within the resolution of the experiment. High energy-resolution spectroscopic measurements were also shown to be essential to observe the theoretically predicted spikiness of the density of states in quasicrystals. A critical review of published spectroscopic data on the electronic structure of quasicrystals has also been presented.     

Relativistic electronic structure calculations on endohedral Gd@C60, La@C60, Gd@C74, and La@C74

We have investigated the adsorption of Ba on the Si(111) surface at elevated temperatures by using high-resolution electron-energy-loss spectroscopy, low-energy-electron diffraction, and photoelectron spectroscopy with synchrotron photons. We found two new ordered phases 2×1a and 2×1bwith increasing Ba coverage in addition to other ordered phases reported earlier. All the ordered surfaces were found to remain semiconducting with a hybridization band gap of ∼1.1 eV almost independent of Ba coverage. We discuss evidence for the evolution of a Ba s-s hybridization band for Ba coverage beyond 0.5 monolayers and propose structural models for the three ordered phases, which are quite consistent with our experimental data. Received: 16 May 2000 / Accepted: 17 May 2000 / Published online: 16 August 2000     

Optical properties and highly efficient laser oscillation of Nd:YAG ceramics

Optical absorption, emission spectra have been measured for polycrystalline Nd-doped Y₃Al₅O₁₂ ceramics. Fluorescence lifetimes of 257.6 μs, 237.6 μs, 184.2 μs and 95.6 μs have been obtained for 0.6%, 1%, 2% and 4% neodymium-doped YAG ceramics, respectively. For the first time, highly efficient laser oscillation at 1064 nm has been obtained with this kind of ceramics. Slope efficiency of 53% has been achieved on a uncoated 4.8-mm thick 1% Nd:YAG ceramics sample. Optical to optical conversion efficiency is 47.6%. Laser oscillation has also been obtained with a 2% Nd:YAG ceramics. The optical properties and laser output results have been compared with that of Nd:YAG single crystal grown by the Czochralski method. Almost identical results have been achieved including laser experiments results. But fabrication of Nd:YAG ceramics is much easier compared to the single-crystal growth method. And also large size (now of about 400 mm diameter×5 mm is available) and high-concentration (>1%) Nd:YAG ceramics can be fabricated. The results show that this kind of Nd:YAG ceramics is a very good alternative to Nd:YAG single crystal. Received: 20 April 2000 / Published online: 16 August 2000     

Lifetimes of metastable states in Sr II

The lifetimes of the 4d ²D _3/2,5/2 levels of Sr⁺ have been determined both experimentally and theoretically. The experiment was performed at an ion storage ring utilising collinear laser excitation. The calculation was performed by the Hartree-Fock method including relativistic effects and core polarisation. The obtained lifetimes (which are about 0.4 s) are discussed in detail and compared with earlier published results. In addition, calculated lifetimes of a large number of excited states in Sr⁺ are included. Received 15 February 2000 and Received in final form 20 March 2000     

Surface plasmon assisted photoemission from Au nanoparticles on graphite

The resonant multiple excitation of collective modes in metallic nanoparticles using ultrashort laser pulses leads to an enhanced multiphoton photoemission from the particles. This effect is here demonstrated for the surface-plasmon resonance of Au nanoparticles on graphite. The shape of the photoemission spectra is explained by multiphoton photo-assisted thermionic emission from the nanoparticles and resonant emission via the image-potential state on graphite. Tuning the photon energy between 1.7 eV and 3.2 eV allows the identification of an enhancement of the photoemission yield at 2.1±0.1-eV photon energy that is attributed to the resonant excitation of the surface plasmon in the Au nanoparticles. This identification of the surface-plasmon excitation in this energy range is also supported by electron energy loss spectroscopy. Received: 8 August 2001 / Revised version: 13 September 2001 / Published online: 10 October 2001     

Femtosecond electron dynamics at adsorbate–metal interfaces and the dielectric continuum model

2 overlayers adsorbed on Cu(111). With increasing number of adsorbate layers the binding energies of the image potential states are found to decrease while their lifetimes increase (except for the second image potential state on 2 to 3 ML Xe/Cu(111)). These trends are most pronounced for nitrogen, where the binding energy of the first image potential state decreases by a factor of 3.5 from 0 to 2 ML N₂/Cu(111); at the same time the lifetime increases from 22 to 700 fs. The results are discussed in the framework of the dielectric continuum model, which approximates the adsorbate layers by a dielectric slab in front of the metal surface. For Xe, the agreement between measured and calculated lifetimes improves significantly if the full dispersion curve of the Xe 6s conduction band is taken into account. Received: 2 November 1998     

Magnetic and high-pressure magnetotransport properties of cesium-substituted lanthanum calcium manganites

The nature of the double-exchange (DE) interaction in lanthanum manganites is studied through chemical substitutions, Cs for La, and high-pressure measurements. Static and high-frequency magnetic measurements and high-pressure electrical transport studies were carried out on bulk polycrystalline and radio-frequency sputtered thin films of La_0.7-xCs_xCa_0.3MnO₃ for x=0-0.1. The samples are found to be cubic. Curie temperature T_c measurements provide evidence for bond-length-related weakening of DE as x is increased from 0 to 0.03. For higher x, the bond-angle-related changes lead to an increase in the strength of DE. High-pressure mangetoresistance data indicate both bond length and bond-angle-related increase of 10–20 K/GPa in T_c with pressure, with the largest increase measured for x=0.03. The rate of increase in the Curie temperature with pressure decreases with increasing T_c. Anomalies are observed in the magnetic parameters for x=0.03. The Cs-concentration dependence of the low-temperature saturation magnetization shows a minimum close to x=0.03. Ferromagnetic resonance studies at x-band reveal a 5% decrease in the g-value for x=0.03 relative to the end members (x=0 and 0.1). The low-field magnetostriction for x=0.03 indicates a relatively strong electron–phonon spin coupling compared to neighboring compositions. Received: 15 May 2000 / Accepted: 24 July 2000 / Published online: 9 November 2000     

Structural and optical properties of nanophase zinc oxide

Nanophase zinc oxide samples were synthesized by a two-step solid-state reaction method. The phase structure and microstructure were investigated by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The vibrational Raman spectra were compared with those from the bulk and their grain size dependence was also examined. Their photoelectric behavior was studied by X-ray photoelectron spectroscopy (XPS). The peaks at 1044.5 and 1021.4 eV were recorded as corresponding to the respective binding energies of Zn 2p_1/2 and Zn 2p_3/2, and the photoelectron spectrum of O 1s in the as-prepared powder was located at 531.2 eV. A strong visible emission centered at 580 nm was clearly observed in the nanosized zinc oxide at room temperature. Photoluminescence (PL) spectra were investigated as a function of grain size after different heat treatments. The origin of the luminescence is attributed to the recombination of electrons in singly occupied oxygen vacancies with photoexcited holes in the valence band. Received: 30 June 2001 / Accepted: 20 February 2002 / Published online: 3 June 2002 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: mszhang@nju.edu.cn     

Artificially nanostructured Cu:Al2O3 films produced by pulsed laser deposition

The processes leading to the formation of Cu:Al₂O₃ composite films on Si (001) with a well defined nanostructure by alternate pulsed laser deposition (a-PLD) in vacuum are investigated. Alternately amorphous Al₂O₃ layers and Cu nanocrystals nucleated on the Al₂O₃ surface are formed, according to the PLD sequence. The Al₂O₃ deposited on the Cu nanocrystals fills in the space between them until they are completely buried, and subsequently, a continuous dense layer with a very flat surface (within 1 nm) is developed. The nucleation process of the nanocrystals and their resulting oblate ellipsoidal shape are discussed in terms of the role of the energetic species involved in the PLD process and the metal–oxide interface energy. Received: 4 July 2000 / Accepted: 5 July 2000 / Published online: 13 September 2000     

Optical study of erbium-doped La3Ga5.5Ta0.5O14 single crystal

Single crystals of erbium-doped La₃Ga_5.5 Ta_0.5O₁₄, grown by the Czochralski method, have been investigated using methods of optical spectroscopy. Room-temperature absorption spectra were analysed in the framework of the Judd-Ofelt theory. Radiative transition rates, radiative lifetimes and luminescence branching ratios for luminescent levels of Er³⁺ have been evaluated and compared to measured luminescence intensities and lifetimes. The laser potential associated with the ⁴I_13/2-⁴I_15/2 transition near 1.55 μm has been assessed. It has been concluded that La₃Ga_5.5 Ta_0.5,O₁₄:Er crystal is an intermediate gain laser material exhibiting strong inhomogeneous broadening of absorption bands, advantageous for optical pumping with laser diodes.     

First-principle study of extrinsic defects in CuScO2 and CuYO2

Using first-principles methods, we studied the extrinsic defects doping in transparent conducting oxides CuMO₂ (MSc, Y). We chose Be, Mg, Ca, Si, Ge, Sn as extrinsic defects to substitute for M and Cu atoms. By systematically calculating the impurity formation energy and transition energy level, we find that BeCu is the most prominent extrinsic donor and CaM is the prominent extrinsic acceptor. In addition, we find that Mg atom substituting for Sc is the most prominent extrinsic acceptor in CuScO₂. Our calculation results are expected to be a guide for preparing n-type and p-type materials through extrinsic doping in CuMO₂ (MSc,Y).     

Correlation between photoluminescence, optical and structural properties of amorphous nitrogen-rich carbon nitride films

Amorphous nitrogen-rich carbon nitride (CN_x) films have been prepared by inductively coupled plasma chemical vapour deposition (ICP-CVD) utilizing transport reactions from a solid carbon source. The nitrogen atomic fraction N/(C+N) is about 1 or even higher as detected by various surface and bulk sensitive methods. An investigation of the chemical bonding structure showed that the films are composed of >C=N units with a small fraction of C≡N groups. Based on these findings, several structural units derived from cis- and trans-conjugated carbon–nitrogen chains are proposed. The optical properties of the CN_x films were studied by transmission spectroscopy and spectral ellipsometry; the optical Tauc gap was determined to 2.1±0.05 eV. The photoluminescence characteristics were measured at three different excitation wavelengths (476, 488 and 515 nm) and revealed two individual contributions. These data are interpreted in terms of the different structural units comprising the nitrogen-rich CN_x films. Received: 14 July 2000 / Accepted:17 July 2000 / Published online: 22 November 2000     

Fluorescence-lifetime measurements in atmospheric-pressure flames using nanosecond-pulsed lasers

Measurements of fluorescence lifetimes are needed to quantify concentration measurements when using linear laser-induced fluorescence. However, lifetimes are only a few nanoseconds for many important species at atmospheric pressure. When using a typical Q-switched laser with a pulse width of about 10 ns, the fluorescence follows the shape of the laser pulse and the lifetime cannot be easily measured. In this paper, a technique is described for experimentally determining the fluorescence lifetime in atmospheric-pressure flames using a nanosecond-pulsed laser; that is, measurement of a lifetime an order-of-magnitude faster than the laser pulse itself. This technique relies on an observable temporal shift in the fluorescence signal as a function of the lifetime. Simulations show the efficacy of this approach, and data in liquid samples and in an atmospheric-pressure flame show excellent agreement with prior picosecond measurements. This technique is successful because only the temporal shift is examined and details of the fluorescence profile are ignored. Received: 23 August 2001 / Revised version: 19 November 2001 / Published online: 17 January 2002     

Optical functions of tris (8-hydroxyquinoline) aluminum (Alq3) by spectroscopic ellipsometry

Optical functions of tris (8-hydroxyquinoline) aluminum (Alq₃) have been studied in the spectral range from 1.55 eV to 5 eV using spectroscopic ellipsometry. The samples have been deposited by thermal evaporation on glass substrates. Optical functions of Alq₃ deposited on unheated substrates and on substrates kept at 100 °C have been determined. The optical functions have been modeled using point-to-point fitting, with the conventional oscillator model and modified oscillator model. It has been found that point-to-point fitting gives the best agreement with the experimental data, and that the modified oscillator model yields better agreement with the experimental data than the conventional oscillator model. Received: 3 September 2001 / Accepted: 22 March 2002 / Published online: 5 July 2002 RID="*" ID="*"Corresponding author. Fax: +852-2559/8738, E-mail: dalek@eee.hku.hk