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.     

Electro-optic response of second-harmonic generation membrane potential sensors

We quantify and ascertain the nature of the second-harmonic generation (SHG) response of amphiphilic push-pull chromophores to a transmembrane electric field. Our technique is based on the application of an alternating field across labeled giant unilamelar vesicles. For chromophore responses that are purely electro-optic, our technique provides an estimate of photoinduced charge shifts based on the observed dispersion of the field response, in accord with a two-level perturbation theory. These results are applicable to the optimization of membrane potential sensors for SHG microscopy.     

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.     

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.     

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.     

Macromolecular structure of cellulose studied by second-harmonic generation imaging microscopy

The macromolecular structure of purified cellulose samples is studied by second-harmonic generation (SHG) imaging microscopy. We show that the SHG contrast in both Valonia and Acetobacter cellulose strongly resembles that of collagen from animal tissues, both in terms of morphology and polarization anisotropy. Polarization analysis shows that microfibrils in each lamella are highly aligned and ordered and change directions by 90 degrees in adjacent lamellae. The angular dependence of the SHG intensity fits well to a cos2 theta distribution, which is characteristic of the electric dipole interaction. Enzymatic degradation of Valonia fibers by cellulase is followed in real time by SHG imaging and results in exponential decay kinetics, showing that SHG imaging microscopy is ideal for monitoring dynamics in biological systems.     

Monitoring the thermally induced structural transitions of collagen by use of second-harmonic generation microscopy

The thermal disruption of collagen I in rat tail tendon is investigated with second-harmonic generation (SHG) microscopy. We investigate its effects on SHG images and intensity in the temperature range 25 degrees-60 degrees C. We find that the SHG signal decreases rapidly starting at 45 degrees C. However, SHG imaging reveals that breakage of collagen fibers is not evident until 57 degrees C and worsens with increasing temperature. At 57 degrees C, structures of both molten and fibrous collagen exist, and the disruption of collagen appears to be complete at 60 degrees C. Our results suggest that, in addition to intensity measurement, SHG imaging is necessary for monitoring details of thermally induced changes in collagen structures in biomedical applications.     

Evaluating cutaneous photoaging by use of multiphoton fluorescence and second-harmonic generation microscopy

The photoaging process of facial skin is investigated by use of multiphoton fluorescence and second-harmonic generation (SHG) microscopy. We obtain the autofluorescence (AF) and SHG images of the superficial dermis from the facial skin of three patients aged 20, 40, and 70 years. The results show that areas of AF increase with age, whereas areas of SHG decrease with age. The results are consistent with the histological findings in which collagen is progressively replaced by elastic fibers. The AF and SHG changes in photoaging are quantified by a SHG to autofluorescence aging index of dermis (SAAID). Our results suggest that SAAID can be a good indicator of the severity of photoaging.     

Nanoscopic study of second-harmonic generation in organic crystals with collection-mode near-field scanning optical microscopy

Collection-mode near-field scanning optical microscopy (NSOM) is used to map nanoscopic second-harmonic generation (SHG) in N -(4-nitrophenyl)- (L) -prolinol crystals. A spatial resolution of 98 nm is achieved. Near-field polarization-dependent SHG measurement is performed, and a local effective SHG susceptibility of 224+/-18 pm/V is obtained.     

Two-photon autofluorescence spectroscopy and second-harmonic generation of epithelial tissue

A spectroscopy system is developed for studying the two-photon excited fluorescence (TPEF) and second-harmonic generation (SHG) of epithelial tissue in backscattering geometry. Our findings show that TPEF signals from epithelial and underlying stromal layers exhibit different spectral characteristics, providing information on the biomorphology and biochemistry of tissue. The SHG signal serves as a sensitive indicator of collagen to separate the epithelial layer from underlying stroma. The polarization dependence of the SHG signal reveals a well-ordered orientation of collagen fibers in the stromal layer. The results demonstrate the potential of depth-resolved TPEF and SHG in determining the pathology of epithelial tissue.     

Two-photon optical characteristics of zinc oxide in bulk, low dimensional and nanoforms

We report the two-photon luminescence (TPL) and second-harmonic generation (SHG) characteristics of zinc oxide (ZnO) in ceramic, thick film and nanorod. Sintering, physical vapour deposition (PVD), and hydrothermal methods were used in preparing the three forms of samples, respectively. Wide-band luminescence in the visible wavelength was observed with green/yellow emission in ceramic and nano-crystal, and blue emission in the film. We attributed interstitial zinc and interstitial oxygen for the luminescence at blue and green bands. Images acquired by TPL and SHG microscopy are presented, interpretation is provided for granular structure exhibiting strong SHG at granular boundaries.     

Analysis of second-harmonic generation microscopy under refractive index mismatch

On the basis of the vector diffraction theory and Green＇s function method, this paper investigates the effects of refractive index mismatch on second-harmonic generation （SHG） microscopy. The polarization distribution and SHG intensity are calculated as functions of the sample radius and probe depth. The numerical results show that refractive index mismatch can result in peak intensity degradation, increase secondary lobes and extension of second- harmonic polarization distribution. Because of the attenuation of polarization intensity, the detected SHG intensity significantly decreases with increasing probe depth, which can limit the imaging depth of SHG microscopy inside thick samples. Forward SHG intensity decays slowly than backward SHG, due to the combination of extension second-harmonic polarization distribution and strong dependency of forward SHG on sample radius.[第一段]     

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.     

Enhanced nonlinear optical conversion from a periodically nanostructured metal film

We demonstrate an approximately10(4) increase in conversion efficiency for optical second-harmonic generation (SHG) from a periodically nanostructured metal structure consisting of a single subwavelength aperture in a thin silver film surrounded by a set of concentric surface grooves. The forward-transmitted second-harmonic radiation from this structure is measured relative to that from an identical aperture with no surrounding surface periodicity. We explain the observed SHG enhancement quantitatively in terms of a measured 120x increase in the strength of the fundamental radiation in the vicinity of the aperture resulting from the periodic nanostructuring.     

Photoinduced stable second-harmonic generation in chalcogenide glasses

We report on photoinduced second-harmonic generation (SHG) in chalcogenide glasses. Fundamental and second-harmonic waves from a nanosecond pulsed Nd:YAG laser were used to induce second-order nonlinearity in chalcogenide glasses. The magnitude of SHG in 20G?20A?60S glass was 10(4) larger than that of tellurite glass with a composition of 15Nb(2)O (5) 85TeO(2) (mol.%). Moreover, no apparent decay of photoinduced SHG in 20G?20A?60S glass was observed after optical poling at room temperature. We suggest that the large and stable value of chi((2)) is due to the induced defect structures and large chi((3)) of the chalcogenide glasses.     

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.     

Amplitude ambiguities in second-harmonic generation frequency-resolved optical gating

We construct field shapes with distinct amplitude profiles that have nearly identical second-harmonic generation frequency-resolved optical gating (SHG FROG) traces. Although such fields are not true mathematical ambiguities, they result in experimentally indistinguishable FROG traces. These fields are neither time-reversed copies nor pulselets with a mere relative phase difference, which are well known nontrivial ambiguities for SHG FROG. We also show that for certain example fields, second-order interferometric autocorrelation is more sensitive to the pulse shape than is SHG FROG.     

Effect of dimension variation for second-harmonic generation in lithium niobate on insulator waveguide

We study the effect of dimension variation for second-harmonic generation[SHG]in lithium niobate on insulator[LNOI]waveguides.Non-trivial SHG profiles in both t...     

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.     

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.