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     

Nonlinear optics for surface phase transitions

A general approach of second-harmonic generation (SHG) studies for surface phase transitions (PTs) is presented, with a thermodynamic classification of surface PTs and their relation to SHG parameters. The symmetry aspects of SHG near a surface PT are discussed, including issues connected with separation of surface and bulk contributions and the role of atomic and mesoscopic inhomogeneities. This approach is illustrated by applying it to two systems revealing a (near-) surface PT: single-crystalline SrTiO₃ near a bulk structural PT and single-crystalline Au in an electrochemical cell revealing an order–disorder and a reconstructive PT. Received: 15 January 2002 / Published online: 11 June 2002     

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     

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     

Electrochemical SHG at a Ag (111) single-crystal electrode using the hanging meniscus configuration

We combine in situ electrochemical second-harmonic generation (SHG) with voltammetry measurements using the hanging meniscus configuration. This setup is used to investigate the interface between a Ag (111) electrode and an alkaline electrolyte. The study offers a new in situ insight into the electrochemical processes at the Ag (111) electrode during OH adsorption and subsequent oxidation. The behavior of SHG isotropic and anisotropic contributions as a function of potential is discussed and related to the interfacial electric field. Comparison of the results with previous investigations of the Ag underpotential oxidation in alkaline solutions shows that submonolayer oxidation is followed by bulk oxidation. Received: 16 October 2001 / Revised version: 26 March 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     

Second-harmonic spectroscopy of electronic structure of Si/SiO2 multiple quantum wells

Size effects in the resonant nonlinear optical response of amorphous Si/SiO₂ multiple quantum wells (MQW) are studied by second-harmonic generation (SHG) spectroscopy in a spectral interval of second-harmonic photon energies from 2.5 to 3.4 eV. The sensitivity of SHG spectroscopy to thickness-dependent electronic structure (sub-band energy position and density of states line shape) of MQW is demonstrated. A monotonic red shift of central energies of SHG resonances by 120 m eV upon increase of the well thickness from 2.5 to 10 ? is observed. This is interpreted as a size dependence of the position of singularities in the combined density of states for a 2D gas of electrons moving in an effective potential well. It is shown that, for agreement with experiment, the simplest (rectangular) shape of the well should be modified in order to take into account the lattice-potential distortion at the interfaces. Received: 16 October 2001 / Revised version: 16 April 2002 / Published online: 6 June 2002     

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     

Intracavity second-harmonic generation of 1.06 μm in GdCa4O(BO3)3 crystals

The characteristics of intracavity second-harmonic generation (SHG) at 1.06 μm in GdCa₄O(BO₃)₃ (GdCOB) crystals cut for different type I phase-matching (PM) directions of (θ,φ)=(66.8°, 132.3°); (19.4°, 0°); (90°, 46°) have been investigated. It was found that the intracavity SHG was significantly efficient in the PM direction of (66.8°, 132.3°), and that the intrinsic lower effective nonlinear coefficient (d_eff) was responsible for the less-efficient SHG in the other two directions. A maximum CW SHG output power of 2.81 W was obtained with an optical conversion efficiency of 18.7%, while the corresponding effective intracavity SHG efficiency was determined to be 41.3%. The intracavity SHG efficiency of GdCOB has been found to reach two-thirds of that obtained with type II phase-matching KTiOPO₄ (KTP). Received: 26 April 2000 / Revised version: 3 July 2000 / Published online: 5 October 2000     

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     

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     

Efficient intracavity second-harmonic generation at 1.06 μm in a BiB3O6 (BIBO) crystal

We report, for the first time, efficient intracavity second-harmonic generation (SHG) at 1.06 μm in a non-linear optical crystal, BiB₃O₆ (BIBO), at a type-I phase-matching direction of (θ,ϕ)=(168.9°,90°), performed with a LD end-pumped cw Nd:YVO₄ laser. A cw SHG output power of 364 mW has been obtained using a 1.9-mm-thick BIBO crystal. The optical conversion efficiency was 12.2% and the corresponding effective intracavity SHG efficiency was determined to be 32.4%. It was found that the intracavity SHG efficiency is greater than that obtained with a type-II phase-matching KTiOPO₄ (KTP) crystal with a thickness of 3 mm. The effective non-linear optical coefficient (d_eff) ratio of BIBO to that of KTP, determined experimentally, is 1.23:1. Received: 7 May 2001 / Revised version: 6 July 2001 / Published online: 19 September 2001     

SHG studies of plasmon dephasing in nanoparticles

2 . The necessary high SHG efficiency is obtained by nanoparticles produced by an electron beam lithographic method, which enables us to fabricate a two-dimensional array of nearly identical, parallel oriented particles of designed shape without centrosymmetry, essential for high SHG efficiency and the tuning of the plasmon resonance to the driving laser wavelength of 780 nm. Received: 14 October 1998 / Revised version: 4 January 1999     

Examination of Validity of Paraxial Approximation in Second Harmonic Generation Microscopy under Low Numerical Aperture

By using a vectorial approach, the validity of paraxial approximation in second harmonic generation （SHG） microscopy under low numerical aperture （NA） is examined when the sample is a collagen fibril. Due to the larger value of dzzz and tensorial nature of SHG, the component Ez of the focused fieM may have strong effect on the radiation pattern of SHG. Numerical results indicate that when the value of NA exceeds 0.3, the effect of Ez can not be neglected, which results in the invalidation of paraxial approximation in SHG microscopy despite the fact that SHG microscopy is still under low NA focusing.     

Imaging theory of nonlinear second harmonic and third harmonic generations in confocal microscopy

ItisreportedrecentlythatnonlinearopticalphenomenonofSHGandTHGhasbeenobservedinmanybiologicaltissues[16].SHGandTHGhavebeenusedtoperformthethree-dimensionalimaginginlivingtissuesandhaveattractedmuchattentionrecently.TherearemanyadvantagesofusingSHGandTHGtoperformthethree-dimensionalimaginginlivingtissues,suchasnoninvasiveandnophotobleaching,inadditiontotheimagingpropertiesofmulti-photonfluorescenceimaging[7—9].Firstly,unlikeinthesingle-andmulti-photonfluorescenceprocesses,onlyvirtualstat…     

M-waveguide structures for direct phase matching in AlGaAs

In this paper the potential of M-waveguide structures for direct phase matching in AlGaAs is investigated by numerical simulations. Principal waveguiding characteristics are discussed. The impact of the optical layer thicknesses is analyzed with respect to phase matching and conversion efficiency for second harmonic generation (SHG). An optimization of the M-waveguide parameters yields a normalized conversion efficiency of 153 or 214 %/W respectively. Received: 16 May 2001 / Revised version: 2 August 2001 / Published online: 23 October 2001     

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     

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     

Second-harmonic-generation microscope with a microlens array scanner

We propose a multifocus scanning technique in second-harmonic-generation (SHG) microscopy in which the SHG detection efficiency and the image acquisition rate are improved by several tens of times compared with typical single-focus scanning techniques. Because of a microlens array scanner, the laser beam of a mode-locked Ti:sapphire laser is split into ~100 beamlets, and the same number of foci are formed in the specimen. Parallel scanning of the foci enables us to observe real-time images of the specimen. The imaging properties and the usefulness of the microscope are demonstrated by SHG images of living HeLa cells and rat cardiac myocytes.     

Second harmonic generation microscopy: principles and applications to disease diagnosis

In this review, the authors discuss the underlying principles of SHG and specific factors that affect the generation properties and describe the essential components of a SHG instrument. In addition, results on the recent progress and impact SHG microscopy has made in different areas of biology and medicine are presented. In particular, the authors focus on disease diagnosis and basic research associated with connected tissues, musculo‐skeletal disorders, and epithelial cancers. The presentation is concluded by offering a perspective on the future technical development of SHG microscopy and additional forefronts to be addressed.