Femtosecond dynamics of spin-dependent SHG response from NiO (001)

Based on a parameterized electronic many-body theory we calculate the spectrum of optical second-harmonic generation (SHG) on an antiferromagnetic (AF) surface: NiO (001). The occurrence of AF spectral lines is further exploited for the calculation of ultra-fast spin dynamics. This spin dynamics is observable in SHG. It is characterized by both a sharp drop of the AF signal within a few femtoseconds and a long persistence (up to nanoseconds) of the spin coherence. These two features constitute an ideal system for possible applications in both magnetic recording and quantum computing. Received: 16 October 2001 / Revised version: 21 March 2002 / Published online: 6 June 2002     

Femtosecond electron and spin dynamics probed by nonlinear optics

Received: 20 September 1998     

Time-resolved photo-induced nonlinear magneto-optical Kerr effect for the study of spin dynamics at a GaAs(001) surface

Received: 20 September 1998     

Enhanced magneto-optical Kerr effects in nanocrystalline Sc-doped CoFe2O4 thin films

Nanocrystalline CoFe_2−xSc_xO₄ (x=0-0.4) thin films were prepared on silicon substrates at reduced temperature by a sol-gel process, and the doping effects of scandium on the microstructure, magnetism and polar magneto-optical Kerr effects of the as-deposited films were examined. It was shown that the intensities of both of the Kerr rotation peaks increase with the doping content x of Sc³⁺. The increase for the peak at 540 nm is due to the decrease of the electrostatic polarization of O²⁻ resulting from the relatively large radius of Sc³⁺, and that for the peak at 620 nm was a result of the migration of Co²⁺ from octahedral to tetrahedral sites in the presence of the dopant of Sc³⁺.     

Dephasing of optically induced excitonic coherences in semiconductor heterostructures

Resonant optical excitation of a direct bandgap semiconductor below the band edge induces excitonic coherences. Experiments based on transient four-wave mixing or cw spectral-hole burning provide an excellent approach to eliminate inhomogeneous broadening and enable determination of the time scale and origin of the decay of the optically induced quantum coherence. Such measurements are of interest in basic physics since they reflect fundamental interactions between the exciton and the surrounding environment including, for example, lattice vibrations and interface fluctuations. They also relate to potential applications of these excitations such as in coherent control or quantum information processing. Received: 30 March 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

Ultrafast dynamics in ZnO thin films irradiated by femtosecond lasers

The damage morphologies, threshold fluences in ZnO films were studied with femtosecond laser pulses. Time-resolved reflectivity and transmissivity have been measured by the pump-probe technique at different pump fluences and wavelengths. The results indicate that two-phase transition is the dominant damage mechanism, which is similar to that in narrow band gap semiconductors. The estimated energy loss rate of conduction electrons is 1.5 eV/ps.     

Ultrafast electron and magnetization dynamics of thin Ni and Co films on Cu(001) observed by time-resolved SHG

Received: 21 December 1998     

Revelation of Ni magnetic moment in GdNi single crystal by soft X-ray magnetic circular dichroism

Magnetic moment of Ni in GdNi single crystal was studied through the soft X-ray absorption spectra (XAS) and the magnetic circular dichroism (MCD) at the Ni L_2,3-edges and the Gd M_4,5-edges. Our experiment revealed for the first time that the Ni 3d band is not filled completely even at the content of 50 at.% of Gd and the Ni does retain a total magnetic moment coupling antiparallel to that of Gd. This result implied that the Ni in GdNi holds an intrinsic magnetic moment even at 50 at.% of Gd and contradicts the well-known charge transfer model. Further by employing the magneto-optical sum rule, the spin and orbital angular magnetic moment were evaluated and discussed.     

Magnetic properties of disordered ferrite and ilmenite-hematite thin films

We have synthesized thin films of disordered zinc ferrite (ZnFe₂O₄) and ilmenite-hematite (FeTiO₃-Fe₂O₃) solid solution, the former and the latter of which are interesting from the viewpoints of magnetooptics and spintronics, respectively, by utilizing sputtering and pulsed laser deposition methods, and have explored their magnetic, magnetooptical, and electrical properties. Although ZnFe₂O₄ possesses a normal spinel structure as its stable phase, some of the Fe³⁺ ions occupy the tetrahedral as well as the octahedral sites in ZnFe₂O₄ of which the sputtered thin film is composed. Consequently, the as-deposited thin film manifests large magnetization even at room temperature although the magnetic phase transition temperature of the stable phase of ZnFe₂O₄ is as low as 10 K. Also, the thin film exhibits a cluster spin glass transition at a temperature as high as 325 K. Furthermore, the ZnFe₂O₄ thin films exhibit large Faraday effects at a wavelength of 400 nm or so. The ilmenite-hematite solid solution is one of the ferrimagnetic semiconductors. Most of the compositions possess Curie temperatures higher than room temperature, and the type of carrier can be tuned only by changing the composition. We have succeeded in synthesizing solid-solution thin films of various compositions grown epitaxially on sapphire substrates with a (0 0 0 1) plane, and have shown that the thin films are ferrimagnetic semiconductors.     

About the depth sensitivity of second-harmonic radiation in ultra-thin metal films

Second-harmonic generation (SHG) results for Ni and Co films on Cu (001) have been reinvestigated regarding the depth sensitivity of this technique for thin films. We find that tangential components of the nonlinear susceptibility are much more sensitive to real film properties than normal components, which are confined to surfaces and interfaces. In consequence, for SHG experiments on ultra-thin metal films, polarization combinations should be favored that possess only tangential susceptibility components, even though the yield is weaker. Additional phase measurements are necessary to obtain full information about the film. Received: 20 January 2002 / Published online: 6 June 2002     

Optical emission spectroscopy investigation of an ultra-short laser induced titanium plasma reheated by a ns laser pulse

The dynamics of a titanium plasma species, induced in air by coupling a fs-ablating laser pulse with an orthogonal ns-reheating laser source placed at the fixed distance of 1.0 mm from the target surface, has been followed by temporally resolved emission spectroscopy. The temporal evolutions of plasma features such as excitation temperatures and electron densities have been evaluated by using two different laser energies of the first fs-ablating laser pulse (0.8 mJ and 3.0 mJ). Optimum inter-pulse delay times, experimentally determined, of 250 μs and 500 μs were used for the fs laser energy of 3.0 mJ and 0.8 mJ, respectively. By experimental inspections of the main plasma species electronic transitions so obtained, a strong enhancement was evaluated up to one and two orders of magnitude for Ti(I) and Ti(II), respectively. Independently from the fs laser energy employed, the plasma features showed the same temporal behaviour implying that the ns-reheating characteristics of this process belong to the reheating mechanism itself. The experimental results have been discussed and the excited species evolutions and elementary processes involved, as well as, the local thermodynamic equilibrium departures, have been outlined.     

Femtosecond dynamics of chemical reactions at surfaces

One of the major goals in physical chemistry is to obtain a microscopic understanding of chemical reactions. Recent developments in femtosecond laser techniques provide the opportunity to resolve the timescale of elementary steps of chemical reactions at surfaces. This is exemplified for the femtosecond laser-induced oxidation of CO on Ru(001). Among other adsorbate-specific probes vibrational sum-frequency generation spectroscopy offers the possibility to monitor adsorbates or reaction intermediates directly at the surface. Recently, we have employed this technique to investigate the dynamics of the CO-stretch vibration of CO adsorbed on Ru(001) after optical excitation leading to CO desorption. Received: 4 August 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

Quantum theory of the magneto-optical effect induced by Ni ions in barium ferrites

To reveal the physical origin of the giant magneto-optical enhancement of Ni²⁺ ions in barium ferrite, quantitative calculations of the contributions of both the intra-ionic electric dipole transition between the 3d⁸ and 3d^{7 4p} configurations of the Ni²⁺ ions and the intra-ionic electric dipole transition induced by odd-parity crystal field terms are presented. It is deduced that the transition is important in the origin of the considered magneto-optical enhancement. The most important factor is the Ni-Fe superexchange interaction; since it is strong enough, the Faraday rotation produced by the Ni²⁺ ions is large though the energy difference between the 3d⁸ and 3 d7 4 p configurations is large. It is demonstrated that though the intra-ionic electric dipole transition does produce Faraday rotation peaks in the visible range, their magnitude is too small to explain the observed Faraday rotation. The effect of the spin-orbit interaction on the Faraday rotation is analysed. The spin-orbit interaction of the ground configuration plays a very important role in the occurrence of Faraday effects, but the Faraday rotation does not increase linearly with the strength of the spin-orbit coupling. On the contrary, the spin-orbit interaction of the excited configuration has almost no effect on the Faraday rotation. It is shown that the mixing of the different multiplets of the ground term induced by the crystal field has a great influence on the magneto-optical properties. Received 7 January 1998     

Coupling-probe laser spectroscopy of degenerate two-level systems: An experimental survey of various polarisation combinations

Several absorption and dispersion spectra of a probe and a coupling laser of different polarisations generating electromagnetically induced absorption in atomic caesium were measured and compared. In the case of at least one linearly polarised laser, electromagnetically induced absorption and absorption within transparency were observed for the probe and coupling laser, respectively. For laser beams of counter-rotating circular polarisation the coupling absorption spectra changed from absorption within transparency to transparency within transparency once the medium was saturated. However, the corresponding parametric dispersion spectra remained unchanged in structure.     

Time-resolved thermoreflectivity of thin gold films and its dependence on film thickness

\valunit{10}{nm} to have been measured by femtosecond time-resolved pump-probe experiments. A conspicuous change of the relaxation behavior was found around for pump pulse fluences of . Thicker films show a nearly exponential decay of the transient linear reflectivity, which turns into a linear decay during the first for films with thicknesses of or less. This observation is evidence of a mean free path of about for hot electrons with temperatures around . Received: 17 December 1996     

Fast Fourier transform analysis in cavity ring-down spectroscopy: application to an optical detector for atmospheric NO2

A fast Fourier transform (FFT) method for analysis of ring-down decays from a cavity ring-down (CRD) spectrometer has been tested and compared with alternative fitting methods. The ring-down times derived from the FFT method are obtained with a precision close to that of the Levenberg–Marquardt non-linear least-squares method, but the fitting algorithm is ~100 times faster, allowing real-time fitting of individual ring-down traces on a personal computer. Advantages of the FFT method are discussed, and the method is demonstrated for the measurement of NO₂ partial pressures equivalent to mixing ratios of 150 pptv and above in laboratory air, using a CRD spectrometer based on an external cavity diode laser operating at wavelengths around 410 nm. The absorption by NO₂ is distinguished from other cavity losses either by using synthetic (zero) air reference samples, or by diverting the sampled laboratory airflow through an NO₂ chemical scrubber consisting of hydroxyapatite on a TiO₂ substrate. Typical mixing ratios of NO₂ in the laboratory air are ~25 ppbv.     

ns- and fs-LIBS of copper-based-alloys: A different approach

A self-calibrated analytical technique, based on plasmas induced by either 250 fs or 7 ns laser pulses, is presented. This approach is comparable to other calibration-free methods based on LTE assumption. In order to apply this method to very different laser pulse durations, the partial-local thermodynamic equilibrium (p-LTE) has been considered within the energy range of 30,000-50,000 cm⁻¹. In order to obtain the neutral species densities, the detected plasma species emission lines intensities have been treated together with the experimental evaluated background black-body Planck-like emission distribution. For validating the followed method, three certified copper-based-alloys standards were employed and their minor components (Ni, Pb and Sn) amounts were determined. As a result, it arises, that this standardless method, independently from the laser source pulse durations, provides good quantitative analysis, and, consequently, that the composition of the plasma plume emitting species induced is not affected by the laser pulse time width.     

Magnetic field-induced cluster formation and variation of magneto-optical signals in zinc-substituted ferrofluids

Fine magnetic particles (size≅100 Å) belonging to the series Zn_xFe_1−xFe₂O₄ were synthesized by cold co-precipitation methods and their structural properties were evaluated using X-ray diffraction. Magnetization studies have been carried out using vibrating sample magnetometry (VSM) showing near-zero loss loop characteristics. Ferrofluids were then prepared employing these fine magnetic powders using oleic acid as surfactant and kerosene as carrier liquid by modifying the usually reported synthesis technique in order to induce anisotropy and enhance the magneto-optical signals. Liquid thin films of these fluids were prepared and field-induced laser transmission through these films was studied. The transmitted light intensity decreases at the centre with applied magnetic field in a linear fashion when subjected to low magnetic fields and saturate at higher fields. This is in accordance with the saturation in cluster formation. The pattern exhibited by these films in the presence of different magnetic fields was observed with the help of a CCD camera and was recorded photographically.     

The effect of the excitation and of the temperature on the photoluminescence circular polarization of AlInAs/AlGaAs quantum dots

In this paper, we present a study of photoluminescence (PL) from AlInAs/AlGaAs quantum dots (QDs) structures grown by molecular beam epitaxy. Specifically, we describe the effects of the temperature and of the excitation density on the photoluminescence circular polarization. We have found that the circular polarization degree depends on temperature. On the other hand, the study of the excitation density dependent circular polarization PL degree shows that the last increases in the case of the sample of weak dot density. However, in the case of large dot density, it is almost constant in the excitation density range from 0.116 W cm⁻² to 9 W cm⁻².     

Mechanism of gain narrowing in conjugated polymer thin films

Received: 19 January 1998