Enhanced second-harmonic generation from individual metallic nanoapertures

We demonstrate the ability of single-subwavelength-size nanoapertures fabricated in a gold metal thin film to enhance second-harmonic generation (SHG) as compared to a bare metal film. Nonlinear microscopy imaging with polarization resolution is used to quantify the SHG enhancement in circular and triangular nanoaperture shapes. The dependence of the measured SHG enhancement on circular aperture diameters is seen to originate from both phase retardation effects and field enhancements at the nanoaperture edge. Triangular nanoapertures exhibit superior SHG enhancement compared with circular ones, as expected from their noncentrosymmetric shape.     

Generation of 15 W femtosecond laser pulse from a Kerr-lens mode-locked Yb:YAG thin-disk oscillator

We demonstrated a robust power-scalable Kerr-lens mode-locked(KLM) operation based on a Yb:YAG thin-disk oscillator.15-W,272-fs pulses were realized at a repetition rate of 86.7 MHz with an additional Kerr medium and a 2.5 mm hard aperture in the cavity.247-fs pulses with an average power of 11 W could also be obtained by using a 2.4 mm hard aperture.Based on this shorter pulse,high efficient second-harmonic generation(SHG) was performed with a 1.7-mm-long Li B3O5(LBO) crystal.The SHG laser power was up to 5 W with the power fluctuation RMS of 1% measured over one hour.     

Surface second-harmonic generation based on periodically poled LiNbO3 nonlinear optical crystal

We have generated a second-harmonic generation(SHG) of a Q-switched microchip Nd:YAG laser on the surface of a periodically poled LiNbO3(PPLN) nonlinear crystal near the grazing incidence angle.Three individual SHG waves as transmitted homogeneous,inhomogeneous and reflected radiations have been generated and their intensities are measured and characterized within a desirable range of about 10 different incidence angles of the Nd:YAG laser as pump source on the PPLN surface.The basic of surface nonlinear radiation is also investigated and similar results are calculated and extracted from the theory.Comparison between calculated and measured data shows that they are in good agreement with each other.     

Angle-resolved second-harmonic light scattering from colloidal particles

We report angle-resolved second-harmonic generation (SHG) measurements from suspensions of centrosymmetric micron-size polystyrene spheres with surface-adsorbed dye (malachite green). The second-harmonic scattering profiles differ qualitatively from linear light scattering profiles of the same particles. We investigated these radiation patterns using several polarization configurations and particle diameters. We introduce a simple Rayleigh-Gans-Debye model to account for the SHG scattering anisotropy. The model compares favorably with our experimental data. Our measurements suggest scattering anisotropy may be used to isolate particle nonlinear optics from other bulk nonlinear optical effects in suspension.     

Refractive index dispersion properties of collagen for microscopic second-harmonic generation

We theoretically simulate second-harmonic generation (SHG) in collagen under linearly polarized focused laser beam. With this model, the effects of numerical aperture (NA) and refractive index dispersion on SHG emission have been investigated. Dispersion properties of collagen are significant under incident wavelength in the visible range. Our results show that the efficient SHG is obtained by controlling the NA, and the higher NA is a necessity when the dispersion effect is considered. Our theoretical simulation results provide useful clues for experimental study of microscopic SHG emission in collagen excited by focused beam.     

Influence of thermal treatment on second-harmonic generation in silver islands films

A reduction in second-harmonic generation (SHG) efficiency at silver islands films is observed when such submicroscopic structures are tempered at approx. 410K. This behavior can be attributed to two facts: an increase in symmetry in film morphology and changes in the particles' electron plasma resonances causing field enhancements inside the particles. The observed correspondence between submicroscopic surface morphology and obtained second-harmonic signal suggests a SHG microscope for the maplike distinguishing between differently structured surface areas.Dedicated to Prof. Dr. Herbert Welling on the occasion of his 60th birthday     

Nondestructive evaluation of incipient corrosion in a metal beneath paint by second-harmonic tomography

A second-harmonic optical scanning imaging method for nondestructive evaluation of corrosion of painted metals is demonstrated. Two-dimensional images of the sectional structure from a sample of painted metal with corrosion were obtained by detection of second-harmonic generation (SHG). The second-harmonic signals generated from paint, corrosion, and metal can be spatially imaged in ~10-mum sliced subsurface layers. Corroded metal layers covered with paint are found to have more intensity variation than normal polished metal. The spatial mapping of the second-harmonic signals shows depth differentiation of paint, corrosion, and metal surfaces. The depth of corrosion beneath the paint can be measured from the SHG images.     

Measuring the electric charge in cloud droplets by use of second-harmonic generation

We report on the observation of second-harmonic generation (SHG) from electrically charged microdroplets while they are excited with femtosecond laser pulses. The intense SHG emission results from chi(3) coupling between two photons of the incident laser pulse and the electrostatic field induced by the surface charges. For Iinc= 2 x 10(12) W/cm2, we estimate the second-harmonic emission to be ISHG= 2.5 x 10(3) photons per droplet and per pulse. The possibility of using SHG to measure remotely the electric charge of water droplets in thunderclouds is discussed.     

Second-harmonic generation in graded metallic films

We study the effective second-harmonic generation (SHG) susceptibility in graded metallic films by invoking the local field effects exactly and further numerically demonstrate that graded metallic films can serve as a novel optical material for producing a broad structure in both the linear and the SHG response and an enhancement in the SHG signal.     

高斯光束第Ⅱ类二次谐波振荡的离散效应

利用直观推断法(heuristc)讨论了离散效应在高斯光束第Ⅱ类相位匹配(PM)二次谐波振荡(SHG)过程中的影响,导出了适用于任意离散参量B和聚焦参量ξ的高斯光束第Ⅱ类PMSHG转换效率的孔径积分公式.     

Membrane imaging by simultaneous second-harmonic generation and two-photon microscopy

We demonstrate that simultaneous second-harmonic generation (SHG) and two-photon-excited fluorescence (TPEF) can be used to rapidly image biological membranes labeled with a styryl dye. The SHG power is made compatible with the TPEF power by use of near-resonance excitation, in accord with a model based on the theory of phased-array antennas, which shows that the SHG radiation is highly structured. Because of its sensitivity to local asymmetry, SHG microscopy promises to be a powerful tool for the study of membrane dynamics.     

Label-free second-harmonic phase imaging of biological specimen by digital holographic microscopy

We have previously developed a new way for nonscanning second-harmonic generation (SHG) microscopy [Opt. Lett. 34, 2450 (2009)]. Based on digital holography, this technique captures, in single-shot hologram acquisition, both the amplitude and the phase of a coherent SHG radiation, which makes possible second harmonic phase microscopy. In this work, we present holographic SHG phase microscopy of a label-free biological tissue and discuss its added value to SHG microscopy.     

Pulsed-laser annealing of GaAs surface studied by time-resolved second-harmonic generation in reflection

Experimental results are presented on the time dependence of the second-harmonic generation (SHG) of a mode-locked Q-switched Nd: YAG laser in reflection from both amorphous and crystalline GaAs surfaces during the pulsed-laser annealing under ruby laser irradiation. A dramatic increase of SHG by more than two orders of magnitude due to recrystallization of the noncentrosymmetric GaAs lattice in the process of pulsed-laser annealing is observed and the duration of surface recrystallization is measured to be not greater than 30–40 ns. The results can be fully understood in terms of the melting model of laser annealing.     

Photonic band-gap enhanced second-harmonic generation in a planar lithium niobate waveguide

Enhanced second-harmonic generation (SHG) conversion efficiency was theoretically predicted in waveguide geometry with coupling to a one-dimensional grating photonic band gap (PBG). We report a series of experiments using samples made with lithium niobate. A waveguide was fabricated near the surface by applying the proton-exchange technique. The characteristics of waveguide modes were determined by several techniques: prism coupling, diffraction, and Cherenkov radiation. The WKB method was used to analyze the results. Ultraviolet laser lithography was applied to make PBG gratings on the sample. We further investigated Cherenkov second-harmonic generation (CSHG), i.e., SHG radiated into the substrate, under the condition of a band-edge PBG resonance in the waveguides. The SHG inside planar waveguides was also experimentally investigated. We fabricated waveguides with multiple pump modes and found that the second mode was more efficient in enhancing the second harmonic signal. This result is explained by our model. Several samples were investigated in detail; the highest conversion efficiency of CSHG with a PBG was enhanced around 50 times above the CSHG signal without a PBG. A numerical model was constructed with parameters calculated from our sample characterization data to interpret the experimental results.     

Label-free morphometry of retinal nerve fiber bundles by second-harmonic-generation microscopy

We present an application of second-harmonic generation (SHG) microscopy for label-free visualization and quantification of the morphology of nerve fibers in the retina. We show that SHG arises from the retinal nerve fiber layer and that it is specifically associated with uniformly oriented microtubules in the axons. The utility of axonal SHG is demonstrated for imaging the neuroanatomy of fresh ex vivo retina, and the three-dimensional structure of the axons of retinal ganglion cells is quantitatively analyzed.     

Disorder-correlated enhancement of second-harmonic generation in strongly photonic porous gallium phosphide

We report an order of magnitude enhancement of second-harmonic generation (SHG) from porous gallium phosphide relative to SHG in crystalline gallium phosphide. Optical heterodyning measurements of photon free-path length reveal a correlation between SHG enhancement and disorder of the porous material.     

Saturation effect and forward-dominant second-harmonic generation in single-defect photonic crystals with dual localizations

We study the forward-dominant output of second-harmonic generation (SHG) in single-defect and dual-localized photonic crystals within the saturation limit. We propose that an asymmetric structure can be used to improve the performance of the enhanced SHG. We get two empirical expressions for the total saturation SHG efficiency and the forward factor and provide a reasonable explanation. The theoretical results predict a nearly 100% conversion efficiency and a nearly 100% forward output. Our work is very valuable for designing nonlinear photonic devices. As a test, a practical asymmetrical structure is presented.     

Enhanced second-harmonic generation for multiple wavelengths by defect modes in one-dimensional photonic crystals

We present an effective design of aperiodically stacked layers of nonlinear material and air, sandwiched by two truncated photonic crystals, in terms of the simulation annealing method. The constructed structure can achieve multiple-wavelength second-harmonic generation (SHG) at the preassigned wavelengths. We derive a general solution of SHG in 1D inhomogeneous systems and apply it to evaluate the SHG conversion efficiency. Numerical simulations show that the conversion efficiency of SHG can be significantly enhanced when the fundamental wave frequencies are assigned to the designed defect states.     

Second-harmonic generation in quasi-periodically domain-inverted Sr(0.6) Ba(0.4) Nb(2)O(6) optical superlattices

One-dimensional Fibonacci-type quasi-periodically domain-inverted structures have been successfully fabricated in a strontium barium niobate crystal by electric field poling. With a single such structure, type I phase-matched second-harmonic generation (SHG) has been demonstrated at several wavelengths from red to near ultraviolet. The spectral positions of the observed SHG peaks are in good agreement with theoretical predictions. The range of measured conversion efficiencies is 2-10%.     

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