Third and fourth harmonic generation at Si-SiO2 interfaces and in Si-SiO2-Cr MOS structures

2 and Si(110)-SiO₂ interfaces and DC-electric-field induced TH and FH generation is then observed in Si(111)-SiO₂-Cr and Si(110)-SiO₂-Cr MOS structures for the first time. A systematic phenomenological analysis of azimuthal anisotropy of TH and FH generation intensity is performed for (111) and (110) surfaces of O_h symmetric single crystals. A phenomenological model of electro-induced effects in TH and FH generation is then developed and the surface specificity and sensitivity of TH and FH generation are discussed. Optical interference of surface electro-induced and bulk bias-independent contributions to the effective third-order nonlinear polarization is proposed as the mechanism underlying surface sensitivity of electro-modulated TH probe. Received: 16 October 1998     

Separation of interface and bulk contributions in second-harmonic generation from magnetic and non-magnetic multilayers

We discuss the separation problem of bulk vs interface contributions in optical Second-Harmonic Generation (SHG). A new method is presented, which — in special cases — provides a full separation of all interface and bulk tensor components. The method is based on measurements in a thin-film geometry, and the relation between two bulk tensor components obtained from group-theoretical arguments. The separation problem in its strict sense is shown to be absent in Magnetization-induced SHG (MSHG). Though, in practice, also in the MSHG case interface and bulk contributions can be closely resemblant. The approach is illustrated by second-harmonic experiments on C₆₀ thin films. SHG in this system is found to be completely dominated by bulk processes.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

A sensitive detection method for magnetization-induced second-harmonic generation under an externally applied field

We describe the instrumentation related to the first observation of magnetization-induced enhancement of surface second-harmonic generation (SHG) from the paramagnetic Si(111)-7×7 surfaces. A judicious choice of polarization and sample orientation enabled us to isolate the magnetic-field-dependent tensor element of the nonlinear susceptibility. A conductive liquid-nitrogen system, coupled to an ultrahigh-vacuum system that is immune to the high magnetic field of 10 T, cooled the sample to about 120 K. A high extinction that is necessary to detect the magnetization-induced SHG (MSHG) was accomplished by minimizing stray optical effects such as Faraday rotation, photoluminescence and thermal birefringence in all optical components, with extra care taken for the UHV window. Consistent and stable operation of this sensitive measurement system permitted experiments involving MSHG at multiple wavelengths and temperatures. Probing the magnetization-induced optical nonlinearity was validated by quenching the surface states by oxidation of the surface layers. From MSHG measurements at two wavelengths resonant with different surface-state transitions, we were able to suggest that the observed MSHG is proportional to the number of dangling bond states of Si(111)-7×7. Received: 15 January 2002 / Published online: 2 May 2002     

Studies of buried interfaces by optical second-harmonic generation

Optical Second-Harmonic Generation (SHG) has been used to study the technologically very important buried semiconductor-metal and magnetic multilayer interfaces. For the case of GaAs-Au, the SHG intensity is shown to depend on the applied bias and Schottky barrier height, and is strongly affected by the sweepout of the carriers generated by the fs excitation pulses. For the M/Co/M multilayers, with M=Cu or Au, the SHG signals appear to depend strongly on the magnetization and can be shown to be interface specific.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

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     

SHG on ferromagnetic Gd films: indication of surface-state effects

The magnetization of 10-nm Gd films on W (110) has been investigated with second-harmonic generation (SHG). We observed a strong second-harmonic (SH) yield, which we attribute to resonance enhancement by the well-known Gd (0001) d-like surface state above the Fermi level. Since this state is spin-polarized it enhances the magnetic SHG contrast. The contrast, the relative phase between odd and even SH fields, and the amplitude ratio of these fields depend strongly on wavelength, which confirms the resonance enhancement. Further proof is provided by the fact that oxidation of the Gd surface reduces the SH yield by an order of magnitude. Received: 16 October 2001 / Revised version: 21 March 2002 / Published online: 11 June 2002     

Switching behaviour of ferroelectric liquid crystals probed by optical second-harmonic generation

Ferroelectric properties of thin (1.5–4 μm planar cells of a ferroelectric liquid crystal (FLC) mixture are studied using electro-optic measurements, second-harmonic generation (SHG) and SHG interferometry. A switching behaviour of the FLC cells in external dc electric fields is observed. It is characterised by rotation of the polarisation plane of the transmitted light and by changes in the SHG intensity, phase and anisotropy dependences, which are attributed to a collective motion of the system as a ferroelectric uniform state with C₂ symmetry. Received: 16 October 2001 / Revised version: 18 March 2002 / Published online: 6 June 2002     

Phase matching of second-harmonic generation in birefringent porous silicon

Optical second-harmonic generation is investigated in free-standing (110) porous silicon films having strong in-plane birefringence. Based on the measured values of the refractive indices, the conditions of phase matching are calculated and verified in the experiments on angular and polarization dependences of second-harmonic generation. Filling pores with a transparent dielectric liquid allows phase matching to be achieved and the second-harmonic signal to be increased by two orders of magnitude. The results of these experiments suggest an opportunity to form new-type nonlinear-optical media consisting of birefringent porous silicon as a phase-matching matrix for the materials embedded in the pores. Received: 30 April 2001 / Published online: 7 June 2001     

DC-electric-field-modified second-harmonic generation at the Si(100) surface

1 resonances for clean and H covered surfaces shift as a function of the dc field in agreement with experiment. This suggests the presence of built-in electric fields whose strength depends on the H coverage, and which are strongly localized in the subsurface region. Received: 20 September 1998     

Investigation of the phase of the second-order susceptibility measured in off-resonant surface second-harmonic generation

Received: 20 September 1998     

SHG investigations of the magnetization of thin Ni and Co films on Cu(001)

Received: 22 November 1998     

Analytical functions for the optimization of second-harmonic generation and parametric generation by focused Gaussian beams

An analytical function involving four parameters is proposed to express the second-harmonic generation efficiency as well as the parametric generation gain coefficient in the Boyd–Kleinman theory. The analytical function clearly reveals the dependence of conversion efficiency on the focusing parameter and the walk-off parameter. Moreover, the optimum focusing parameter and its corresponding maximum efficiency are explicitly given in the analytical function, leading to a straightforward evaluation of a given crystal performance. Received: 20 January 2003 / Published online: 22 May 2003 RID="*" ID="*"Corresponding author. Fax: +886-35/7291-34, E-mail: yfchen@cc.nctu.edu.tw     

Anisotropy of the optical and magneto-optical response of Au/Co/Au/Cu multilayers grown on vicinal Si (111) surfaces

The optical and magneto-optical second harmonic reflectivity response of Au/Co/Au/Cu multilayers grown on vicinal Si (111) substrates has been studied. These azimuthal optical non-linear experiments check the uniaxial character of the crystallinity of the Au buffer layer and the magnetic behavior of the ultrathin Co films in the metallic multilayer. They clearly show the strong dependence of the growth parameters and the misorientation of the vicinal surface on the SHG reflectivity signals. This uniaxial behavior is also correlated to linear MOKE experiments on the magnetic anisotropy with an easy magnetization axis parallel to the step edges. Received: 16 October 2001 / Published online: 29 May 2002     

Homodyne detection of second-harmonic generation as a probe of electric fields

Received: 16 December 1998     

Magnetic properties of a random diluted spin-1/2, 1, 3/2 superlattice

Using the effective-field theory we studied the magnetic properties of a random diluted spin-1/2, 1, 3/2 superlattice which consists of three different ferromagnetic materials. The critical temperature of the system is studied as a function of the concentration of magnetic atoms and exchange interactions in each layer. The temperature dependence of magnetization shows that the properties of the diluted system are different from those of the corresponding pure system.     

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

Received: 21 December 1998     

Intense femtosecond laser-induced second-harmonic generation in atmospheric-pressure air

Second-harmonic generation (SHG) in atmospheric-pressure air is experimentally studied using single focused linear-polarized Ti:sapphire intense femtosecond laser pulses at 810 nm. The efficiency of SHG is found to reach a maximum at the optical breakdown threshold of ≈2.9×10¹⁴ W/cm². The spectral distribution and polarization property of the second harmonic are investigated. The contribution to SHG from electric-field-induced third-order mixing plays the main role even after the optical breakdown had occurred. Received: 23 May 2000 / Published online: 16 August 2000     

Nonlinear magneto-optical probing of magnetic interfaces

Received: 16 October 1998     

Simultaneous measurements of second-harmonic generation and two-photon photoelectric emission from Au

Received: 1 October 1998 / Accepted: 30 October 1998     

Thin noble metal films on Si (111) investigated by optical second-harmonic generation and photoemission

Thin noble metal films (Ag, Au and Cu) on Si (111) have been investigated by optical second-harmonic generation (SHG) in combination with synchrotron radiation photoemission spectroscopy. The valence band spectra of Ag films show a quantization of the sp-band in the 4-eV energy range from the Fermi level down to the onset of the d-bands. For Cu and Au the corresponding energy range is much narrower and quantization effects are less visible. Quantization effects in SHG are observed as oscillations in the signal as a function of film thickness. The oscillations are strongest for Ag and less pronounced for Cu, in agreement with valence band photoemission spectra. In the case of Au, a reacted layer floating on top of the Au film masks the observation of quantum well levels by photoemission. However, SHG shows a well-developed quantization of levels in the Au film below the reacted layer. For Ag films, the relation between film thickness and photon energy of the SHG resonances indicates different types of resonances, some of which involve both quantum well and substrate states. Received: 16 October 2001 / Revised version: 14 March 2002 / Published online: 29 May 2002