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     

Second-harmonic generation from metal surfaces: Beyond jellium

The generation of Second-Harmonic (SH) radiation from simple metals has been the subject of numerous investigations for almost three decades. The use of clean metal surfaces in the experiments and increasingly sophisticated jellium-based theoretical models has led to a convergence on the magnitude and some of the dispersion characteristics of SH generation in free-electron metals like aluminum. However, the sensitivity of the SH-generation process to crystal symmetry, surface morphology, and surface electronic states indicates that nonlinear optical properties are influenced by processes which cannot be explained using a model based on an isotropic electron gas. Here, we review some recent experimental work indicating where deviation from jellium-based models occurs and attempts to understand these.Paper presented at the 129th WE-Heraeus-Seminar on Surface Studies by Nonlinear Laser Spectroscopies, Kassel, Germany, May 30 to June 1, 1994     

Helicoidal distributed-feedback cavity action in a ferroelectric liquid crystal

Second-Harmonic (SH) generation was observed in homeotropically aligned ferroelectric liquid-crystal cells using fundamental light propagating along the helicoidal axis. Relatively strong SH light was observed in the helicoidal structure when the optical pitch was nearly the same as the SH-light wavelength, though, otherwise, the cancellation of the generated SH light by the helicoid results in negligibly weak SH intensity. Because the observed SH light is independent of the cell thickness, the SH light is attributed to the one generated from the surface region and the SH light generated inside the cell is confined and lost by the helicoid. This phenomenon indicates the helicoidal Distributed-FeedBack (DFB) cavity action and suggests the possibility of the helicoidal DFB laser using dye-doped ferroelectric liquid-crystal cells.     

Second harmonic generation in a strontium barium niobate crystal with a random domain structure

The phenomenon of the second-harmonic (SH) generation in a strontium barium niobate (SBN) crystal in directions not obeying the conditions of phase matching for spatially homogeneous media has been studied. The appearance of the SH signal is interpreted as resulting from the quasi-phase-matching nonlinear wave interaction due to the random domain structure of the SBN crystal containing acicular ferroelectric microdomains. A theoretical model describing the SH generation in such two-dimensional, spatially inhomogeneous nonlinear optical structures is proposed. An analysis of the second-harmonic emission directivity patterns shows that the main contribution to the noncollinear SH generation in SBN is due to near-surface domains extending to a depth of up to several dozen microns.     

Induced Diffraction in Phase-Mismatched Second-Harmonic Generation

We show analytically that in phase-mismatched second-harmonic generation, an effective diffraction is induced at the second-harmonic （SH） frequency. Numerical simulation results agree with the analytical predictions. Compared to the case of linear propagation, the effect of the overall diffraction at the SH frequency becomes doubled due to the induced diffraction, which causes an interesting result that the SH beam width will be larger than that of the fundamental field.     

Second-harmonic generation at the surface of cubic ionic crystals

The strength of the different source terms in the isotropic Second Harmonic (SH) response of the surface has been measured in different ionic crystals LiF, NaF, GGG(Gadolinium-Gallium-Garnet), and MgF₂, using as excitation beam the fundamental output of a Nd:YAG laser (1.06 m). The azimuthal dependences of the optical second-harmonic generation has also been measured at the LiF(100), LiF(111), GGG(100), and GGG(111) surfaces. No experimental evidence of a bulk contribution to the anisotropic part of the nonlineau polarization has been observed.     

相匹配契伦可夫辐射式倍频

用波导产生倍频波时,如果倍频波进入辐射模区,仍然有相匹配问题。契伦可夫辐射式倍频不是自动地实现相匹配的。相匹配要求导波基波模式场,倍频传输场(自由波),倍频触发场,以及经多次反射透射后的辐射场的迭加形成的总辐射场处于同步的相匹配状态。根据这个相匹配的分析,提出波导契伦可夫相匹配的特有的方法,那就是对波导的模色散进行设计,并指出非对称波导的特有优点,是改变一个边界上的反射相变,即选择不同色散的线性材料作包层,由此可得到相匹配的高效契伦可夫倍频辐射。     

固体板中SH型板波的\

从理论上研究了固体板内SH型板波的\     

Spectral domain second-harmonic optical coherence tomography

Optical coherence tomography (OCT) provides micrometer-scale structural imaging by coherent detection of backscattered light. Molecular contrast in OCT has been demonstrated using transient absorption, coherent anti-Stokes Raman scattering, and second-harmonic (SH) generation. The sensitivity of molecular contrast signals can be enhanced by use of Fourier domain techniques. We have constructed a spectrometer-based Fourier domain SH-OCT system for simultaneous acquisition of the fundamental and SH signals. We report a >30 dB increase in SH sensitivity over a similar time domain SH-OCT system and demonstrate contrast between cartilage and bone using collagen as the contrast agent.     

Demagnetization following optical excitation in nickel and permalloy films

Time-resolved pump–probe second-harmonic (SH) response following optical excitation has been studied in nickel and permalloy films. Experimental data indicate that the odd SH field represents the transient magnetization, i.e. the behavior of the spin subsystem, while the electron subsystem generates the even SH field. Delays between odd and even SH fields of about 200 fs and 650 fs were detected for nickel and permalloy films, respectively. We found that the dynamics of the odd SH field is influenced by the polarization of the pump pulse. This dependence on excitation conditions suggests a difference in surface and bulk magnetization dynamics. Received: 25 November 2001 / Revised version: 27 March 2002 / Published online: 11 June 2002     

Dependence of second-harmonic generation in ferroelectric liquid crystals with a defect on the optical gap

Second-harmonic generation (SHG) in ferroelectric liquid crystal with a twist defect is studied by de Vries' solution. It is shown that the width of the photonic band gap for the SH wave is an important factor to determine the saturation length. SHG is effectively enhanced by using narrow photonic band gaps.     

K-induced surface structural change of Si(1 1 1)-7 × 7 probed by second-harmonic generation

The growth of thin K films on Si(1 1 1)-7 × 7 has been investigated by selecting the input and output polarizations of second-harmonic generation (SHG) at room temperature (RT) and at an elevated temperature of 350 °C. The SH intensity at 350 °C showed a monotonic increase with K coverages up to a saturated level, where low energy electron diffraction (LEED) showed a 3 × 1 reconstructed structure. The additional deposition onto the K-saturated surface at 350 °C showed only a marginal change in the SH intensity. These variations are different from the multi-component variations up to 1 ML and orders of magnitude increase due to excitation of plasmons in the multilayers at RT. The variations of SHG during desorption of K at 350 °C showed a two-step decay with a marked shoulder which most likely corresponds to the saturation K coverage of the Si(1 1 1)-3 × 1-K surface. The dominant tensor elements contributing to SHG are also identified for each surface.     

Coupling of ferroelectric and antiferromagnetic order parameters in hexagonal RMnO3

Second-harmonic generation (SHG) is used as a probe for the coexisting ferroelectric and antiferromagnetic orders in hexagonal RMnO₃. SH contributions coupling to the electric and/or magnetic order parameters are identified on the basis of their spectral dependence and the symmetries of the corresponding order parameters. The SH signals from the ferroelectric and antiferromagnetic orders were employed to image the electric and magnetic domain structures separately. The transformation properties of electric and magnetic domains are discussed with respect to the transformation properties of the corresponding order parameters. An investigation of the mutual coupling between the coexisting electric and magnetic orders reveals apparently independent domain structures, which contradicts the symmetry and transformation properties of electric-dipole-induced SHG in this ferroelectromagnetic group of compounds. Apart from higher-order multipole contributions to SHG, interface contributions from clamped electric and magnetic domains can solve the contradiction. Received: 16 October 2001 / Published online: 24 April 2002     

Second harmonic generation in α-Si:H thin films: Thickness dependence

The second harmonic generation (SHG) technique has been applied to investigate the nonlinear optical properties of thin films of hydrogenated amorphous silicon on a glass substrate. SHG measurements have been performed in two transmission experimental schemes. Modeling of a film as a three-layer structure and considering the interference and absorption at the SH wavelength have been carried out. The dependence of the nonlinear susceptibility on the film thickness was used to separate the bulk electric dipole contribution.     

Efficient generation of a continuous-wave,tunable 780 nm laser via an optimized cavity-enhanced frequency doubling of 1.56 µm at low pump powers

We present the strict design parameters of the experiment for the 780 nm tunable continuous-wave second harmonic (SH) generation by the nonlinear resonator containing a MgO doped periodically poled LiNbO₃ (MgO:PPLN) crystal. Optimization of such critical parameters, including focusing and impedance matching, more than 84% SH conversion efficiency and 3.1 W available output power at 780 nm were obtained from the fundamental wave at 1560 nm with two different input couplers. The thermal saturated behavior of the SH output power has been observed in the experiment. The beam quality factor M² of the generated SH wave is 1.04 (1.03), and the RMS power stability is 1.29% in 3 h. The SH wave was further used to detect the D ₂ transitions of Rb atom, exhibiting a fine tunable characteristic. Such laser source can be a suitable candidate in the atomic physics and quantum optics.     

Stabilization of spatiotemporal solitons in second-harmonic-generating media

We report the results of a systematic analysis of the existence and stability of spatiotemporal (two-dimensional) solitons (STSs) in the model of a planar waveguide with the intrinsic χ⁽²⁾ nonlinearity. Fundamental obstacles to the creation of STSs under physically realistic conditions are the normal sign of the group-velocity dispersion (GVD) at the second harmonic (SH), and the significant group-velocity mismatch (GVM) between the SH and fundamental-frequency (FF) components. To construct STS solutions in a numerical form, we adjust the iterative method, which was recently used for finding temporal (one-dimensional) χ⁽²⁾ solitons in a similar setting. We identify effective existence borders for the STSs, within which the energy loss to the generation of extended “tails” in the SH component (due to the normal sign of the GVD) is negligible. It is demonstrated that the existence region can be made much broader by means of the GVD-management and GVM-management techniques. We also explore interactions between the STSs, and find robust two-soliton bound states, with a moderate separation in the longitudinal (temporal) direction. Head-on collisions between the STSs are always destructive.     

Two-color pulse compression in aperiodically-poled lithium niobate

We experimentally demonstrate engineerable compression of two-colored pulses in a linearly-chirped quasi-phase-matching grating. Quadratic solitons generated from fundamental input are reshaped through cascaded parametric processes of second-harmonic generation (SHG) and the back-conversion. We use type-I (e: o + o) SHG geometry in a 50-mm-long aperiodically-poled MgO:LiNbO₃ device to satisfy the group-velocity matching condition. Simultaneously compressed fundamental and SH pulses of about 55-fs duration with small pedestal are generated from the fundamental input pulses of 95-fs duration.     

Optical harmonic generation in amorphous silicon nitride microcavities

Second harmonic (SH) and third harmonic (TH) generation in amorphous silicon nitride microcavity are experimentally investigated. The transmitted SH and TH signals are measured in the 0.9-1.4 μm spectral range, showing enhanced nonlinear conversion efficiency corresponding to resonant wavelength and optical band edges. The efficiencies of the SH and TH generation processes are found to be enhanced by about two and one orders of magnitude, respectively, in comparison with the case of reference amorphous silicon nitride sample. The SH spectra can be reasonably interpreted as due to surface/interface harmonic generation, while the TH signal is related to bulk isotropic third-order polarization. The results obtained for the TH signal are discussed in terms of the linear optical properties of amorphous silicon nitride thin films.     

Influence of phase transitions on the second harmonic generation in metal nanoparticles

In this work we use nonlinear optical properties of Ga nanoparticles monolayers of different average sizes embedded in dielectric matrices to investigate the liquid-solid phase transitions in these materials. Ga nanoparticles, formed by exploiting the partial wetting of liquid Ga over a SiO_x surface are irradiated with fs laser pulses from a Ti:sapphire source. The resulting Second Harmonic (SH) generated in the reflection and transmission directions is measured along the phase transitions by cooling the sample from 320 K down to liquid nitrogen temperature. Hysteresis cycles are observed in the nonlinear transmission, which exhibit a strong amplification from the solid to liquid values as compared to the linear optical results. A simple model for SH generation, based on Mie scattering calculations which includes the effect of surface plasmon resonance provides a fair key for the interpretation of the observed effects.