Enhancing the resolution of the forward second harmonic imaging using the two-photon laser scanning microscope

The effect of increasing the numerical aperture and changing the immersion imaging medium of the objective in the forward second harmonic imaging of the grana and intergranal parts of chloroplasts in the leaves of shade moss Plagiomnium affine plant were demonstrated. Also the enhancement of the forward second harmonic generation images and simultaneously records the forward and backward second harmonic signals were demonstrated. The second harmonic signals in the forward and backward directions are generated by a tightly focused linearly polarized femtosecond pulses laser.

Conclusions

Forward second harmonic signals were successfully enhanced by capturing higher order of diffraction rays from the samples using high numerical aperture water immersion objective.     

Effects of weak localization of photons in nonlinear optics: Second harmonic generation

The angular distribution of the second harmonic generation (SHG) in disordered nonlinear media is shown to exhibit sharp peaks due to the weak localization of photons. The shape of these peaks is related to the spatial structure of the electric field for strongly scattered second harmonic (SH) radiation and is sensitive to the Anderson localization effects. The angular distribution of the second harmonic energy flux is calculated for the case of steady state and pulse generation in a slab of thickness d ≫ l (l is the elastic mean free path). For the case of pulse generation the time dependence of the SHG is discussed.     

Optically stimulated optical effects in the ZnO:Tm nanorods

We have performed the studies of photoinduced second harmonic generation in the ZnO nanorods doped by Thulium with different content (0.1; 0.2;0.5% of Tm). The illumination was performed with the Er:glass laser emitting at 1540 nm wavelength of the 10 ns laser and the output second harmonic generation (SHG) was studied. The AFM data analysis was performed. The role of the rare earth Tm ions on the morphology and the optically stimulated SHG is discussed. The SHG yield was found to be strongly dependent on Thulium content and Root Mean Square roughness of the studied layers.     

Second harmonic generation from thick leaves using the two-photon laser scanning microscope

A laser-scanning microscope using second harmonic generation (SHG) as a probe is shown to produce high-resolution images of duckweed Lemna minuta leaves. These leaves are multi-cell layer thick. Second harmonic light is generated by a tightly focused short pulse laser beam and is collected by two objectives yielding forward and backward second harmonic digital images. This measurement shows that the signal of the second harmonic imaging in the forward and backward directions depends on the thickness of the chloroplast and that the forward-SH image was brighter than the backward-SH image. The image intensity also depended on the orientation of the chloroplast in relation to the illuminating polarization direction. Their light-induced re-orientation which was affected by the intensity of the illumination could be observed during the experiments.The novelty of this work is to establish new compact technique in which one can use the SH imaging to investigate the true architecture of the sensitive samples, the unknown samples and the samples which is not producing auto-fluorescence. Moreover, investigation of new or unknown samples needs a long time for looking at details of the sample. Thereby the sample will be exposed for long time to the laser radiation that will cause photobleaching and photodamage. Since the SHG does not undergo photobleaching and photodamage this will be the promising technique for investigating the sensitive and new unknown samples. Then one can move to acquire fluorescence images after complete investigation of the true architecture of the sample. The other advantage of SHG is that it has the ability to image highly ordered structural proteins without any exogenous labels. The SHG is an intrinsic and a coherent process. Imaging of intrinsic compounds avoids the complications of slicing and labeling, and samples can be investigated under physiological conditions.     

Laser-induced,second-order optical susceptibilities of YAB:Cr3+ single crystals

Complex temperature studies of optically stimulated second harmonic generation (SHG) at 1064?nm for pulsed 10?ns Nd:YAG laser radiation under illumination of two coherent laser beams (at 1064?nm and its 532?nm second harmonic) were carried out by means of the Maker fringe method. The bicolour coherent process allowed detection of some additionally induced non-centrosymmetry. The effect was studied at different temperatures and experimental geometries in YAB:Cr³⁺ single crystals. We found that Cr³⁺ ions play a principal role in the observed effects. The output of optically stimulated SHG was generally non-spherical in the sequence profile, contrary to the traditional non-stimulated SHG. Moreover, we also established that the optimal conditions for obtaining SHG corresponded to the fundamental/writing beam intensities ratio 6:1. A specially performed control of the photo-thermal sample heating showed that the increase of temperature did not exceed 1.2?K, which allowed the influence of photo-thermal heating to be neglected. The optimal input–output laser geometry corresponded to s-p polarisation and to the angle of about 32° between the photo-inducing and fundamental beams. Additionally in the studied temperature range (77–295?K) there was observed an enhancement of the output second-order susceptibilities from 0.72?pm/V up to 1.02?pm/V.     

Optical properties of a GaAs cone-like quantum dot: Second and third-harmonic generation

In the present work, we have studied numerically the second harmonic generation (SHG) and third harmonic generation (THG) in a cone-like quantum dot. For this purpose, we firstly obtained the energy levels and wave functions of this system. Then, we have used an expression for the SHG and THG by a compact density matrix approach and an iterative procedure. The SHG and THG enhance and shift toward lower energy by increasing the height h and vertex angle α. According to the results it is found that the structural parameters have great influence on the THG in this system.     

Absolute signs of the second harmonic generation,electro-optic,and piezoelectric coefficients of CuCl and ZnS

The absolute signs of the second harmonic generation (SHG) and electro-optic coefficients have been determined for CuCl, and for both the zincblende (z) form and a hexagonal polytype (h) form of ZnS. In addition, the absolute signs of the piezoelectric coefficients for CuCl and ZnS(Z) were also obtained. The sign of the piezoelectric coefficient for ZnS (z) is in agreement with earlier work, while that for CuCl agrees with a recent theoretical calculation. The signs of the SHG coefficients for ZnS(z) and ZnS (h) also agree with predictions. However, the SHG coefficient for CuCl is found to be negative, the first sign measurement in conflict with two highly successful theories.     

Polar Fe(IO<Subscript>3</Subscript>)<Subscript>3</Subscript> nanocrystals as local probes for nonlinear microscopy

We have investigated nanocrystals of Fe(IO₃)₃ by polarization-sensitive second harmonic generation (SHG) microscopy. As the nonlinear optical properties of this material were only poorly characterized, we have first determined the relative values of the elements of its second-order susceptibility tensor, by the global fitting of the polarization-resolved SHG response of an ensemble of nanocrystals. This information allows one to optically retrieve the orientation of individual particles in the sample. The high SHG efficiency measured for nanocrystals of Fe(IO₃)₃ and their polar nature could make them very attractive for nonlinear microscopy of biological samples. PACS 42.70.Mp; 78.67.Bf     

Towards sympathetic cooling of trapped ions with laser-cooled Mg + ions for mass spectrometry and laser spectroscopy

Sympathetic cooling by laser cooled Mg ions has been proposed as a method for fast cooling of highly charged ions to a very low temperature. The paper describes the construction of the solid state laser system at 279.63 nm required for laser cooling of the Mg ions. The laser system is composed of a fiber laser at 1,118.54 nm and two successive second harmonic generation (SHG) ring cavities for frequency quadrupling. In the first SHG cavity, non-critical phase matching of a lithium triborate (LBO) crystal is used for doubling from 1,118.54 to 559.27 nm. The second SHG cavity uses critical phase matching of a β-barium borate (BBO) crystal for doubling from 559.27 to 279.63 nm. With the aid of Boyd–Kleinmann theory, optimum experimental parameters are calculated and used for an efficient SHG. Besides this, the paper intends to be a shortcut for practical applications of the Boyd–Kleinmann theory for SHG.     

Optical second harmonic generation in asymmetric double triangular quantum wells

The second harmonic generation (SHG) in the asymmetric double triangular quantum wells (DTQWs) is investigated theoretically. The dependence of the SHG coefficient on the right-well width of the DTQWs is studied, and the influence of the applied electric field on SHG coefficient is also taken into account. The analytical expression of the SHG coefficient is analyzed by using the compact density-matrix approach and the iterative method. Finally, the numerical calculations are presented for the typical GaAs/Al_xGa_1−xAs asymmetric DTQWs. The results show that the calculated SHG coefficient in this coupled system can reach the magnitude of 10⁻⁵ m/V, 1–2 orders of magnitude higher than that in step quantum well, and that in double square quantum wells. Moreover, the SHG coefficient is not a monotonic function of the right-well width, but has complex relationship with it. The calculated results also reveal that an applied electric field has a great influence on the SHG coefficient. Applying an appropriate electric field to a DTQW with a wider right well can induce a sharper peak of the SHG coefficient due to the double-resonant enhancement.     

Theoretical analysis of the TE mode Cerenkov type second harmonic generation in ion-implanted X-cut lithium niobate channel waveguides

Optical second harmonic generation (SHG) in the form of Cerenkov radiation from ion-implanted lithium niobate (LiNbO₃) channel waveguides is analyzed by directly resolving the wave equations. Useful formula of the SHG efficiency is derived and expressed in terms of waveguide parameters. Numerical examples are plotted for LiNbO₃ crystals. The results enable the optimization of waveguide design for efficient second harmonic generation in the Cerenkov configuration.     

Frequency doubling of Nd:YAG- and GaAs-lasers by KNbO3: Ta crystals

Abstract

For KNb_1-xTa_xO₃ crystals the influence of the Ta-concentration on the phase-matching properties for optical second harmonic generation (SHG) was measured. For non-critical phase matched SHG of the Nd:YAG-laser (1064nm) the coefficient d₃₁ of the tensor of the nonlinear susceptibility was applied, while for the GaAs-laser (905 nm) the coefficient d₃₂ was used. For both laser wavelengths the phase-matching temperature decreases with increasing Ta-concentration. Non-critical phase-matching at room temperature can be reached with the GaAs-laser for a Ta-concentration of ≈9%. The corresponding value for the Nd:YAG-laser is ≈14%.     

Synthesis and characterization of TiOx nanoparticles prepared by pulsed-laser ablation of Ti target in water

Nanoparticles (NPs) creation by pulsed-laser ablation of targets in a liquid environment has recently become a promising technique, which has several relative advantages, such as simplicity and low cost. This technique was employed in the present work for preparation of TiO_x NPs suspension by ablation of metal Ti targets into twice-distilled water. A second harmonic generation (SHG) pulsed Nd:YAG laser was used in the experiments. Preferential formation of spherical NPs and their TiO_x nature was established. Aggregation of the created particles during aging was found. Transition of the NPs’ structure from amorphous to crystalline with increasing the laser energy was revealed. A difference was observed in the transmittance of the suspensions obtained depending on the laser intensity.     

Corrugated-enhanced second harmonic generation in metal–insulator–metal plasmonic waveguides

Nonlinear effects such as second-harmonic generation (SHG) are important for applications such as switching and wavelength conversion. In this study, the generation of second harmonic in metal–insulator–metal (MIM) plasmonic waveguides was investigated for both symmetric and asymmetric structures. Symmetric means that the metals at the top and bottom of the dielectric layer are the same and asymmetric means that the metals at the top and bottom of the dielectric layer are different. Two different structures are considered here as plasmonic waveguide for generation of second harmonic and analyzed using finite-difference time domain method. Besides the structure has grating on both sides for more coupling between photons and plasmons. The wavelength duration of grating per length unit (number of grooves) will be optimized to reach the highest second harmonic generation. To perform this optimization, the wavelength of operation λ = 458 nm is considered. It was shown that field enhancement in symmetric MIM waveguides can result in enhancement of SHG magnitude compared to the literature values and asymmetric device results in more than two orders of magnitude enhancement in SHG compared to symmetric structure. It is also shown that the electric field of second harmonic depends on the thickness of crystal (insulator). So, its thickness is optimized to achieve the highest electric field.     

Analysis of carrier injection,accumulation and transport process of pentacene field effect transistors using a Maxwell–Wagner model

Carrier injection, carrier transport and carrier accumulation are three key process to understand the characteristics of organic field effect transistor (OFET) devices. In our previous studies, we showed the evidence of carrier injection from source electrode by means of optical second harmonic generation (SHG) measurement and capacitance–voltage (C–V) measurements, and explained the FET characteristics using a Maxwell–Wagner model. In this paper, to further clarify the behavior of the carrier transport and hole injection from source electrode, we focused on the hysteresis behavior observed in the current–voltage (I–V) and C–V characteristics of pentacene FETs. Employing the electric field induced SHG (EFISHG) and C–V measurements, we could show that the origin of the hysteresis behavior is caused by holes, which are injected and subsequently trapped in FET channel.     

Development of coherent tunable source in 2–16 μm region using nonlinear frequency mixing processes

A very convenient way to obtain widely tunable source of coherent radiation in the infrared region is through nonlinear frequency mixing processes like second harmonic generation (SHG), difference-frequency mixing (DFM) or optical parametric oscillation (OPO). Using commonly available Nd:YAG laser and its harmonic pumped dye laser radiation as parent beams, we have been able to generate coherent tunable infrared radiation (IR) in 2–16 μm region using different nonlinear crystals by DFM and OPO. We have also generated such IR source in the 4–5 μm region through SHG of CO₂ laser in different infrared crystals. In the process we have characterized a large number of nonlinear crystals like different borate group of crystals, KTP, KTA, LiIO₃, MgO:LiNbO₃, GaSe, AgGaSe₂, ZnGeP₂, AgGa_1?x In _x Se₂, HgGa₂S₄ etc. To improve the conversion efficiencies of such frequency conversion processes, we have developed some novel schemes, like multipass configuration (MC) and positive optical feedback (POF). The significance of the obtained results lies in the fact that to get the same conversion in SHG or DFM, one now requires fundamental input radiation with much lower intensity.     

Relative merit of χ and χ SHG by charged water microdroplets - Implications for LIDAR

We investigated second harmonic generation (SHG) from neutral and electrically charged water microdroplets of uniform size. We found that angular distribution, polarization, and conversion efficiency of the SHG emission did not change within applied surface charge densities from 0 to 7.2 × 10⁻⁵ C/m². The latter is consistent with previously observed charge sensitive SHG efficiency on water interfaces if one considers particular experimental conditions. A brief discussion of the applicability of SHG for optical detection of charges in atmospheric clouds is given.     

Investigation on high efficiency temporal phase modulated broadband second harmonic laser

In this paper, it is the first time to experimentally demonstrate the second harmonic generation (SHG) of temporal phase modulated broadband laser. The SHG conversion efficiency and the characteristic of SHG spectrum are investigated in detail and the relation between SHG conversion efficiency and incident fundamental light intensity is obtained. The highest efficiency of nearly 70% is achieved at the fundamental pulse intensity of 1.6 GW/cm². The experimental results show that the SHG spectrum widths under high and low intensity are both half of the incident fundamental lights, and don’t result in the spectrum narrowing. The obtained results are very useful for operation at the second harmonic wavelength in inertial confinement fusion (ICF) laser facility.     

Surface ferroelectric phase transition in multilayer polymer Langmuir films

The ferroelectric phase transition on the free surface of a polymer ferroelectric Langmuir-Blodgett film was studied by the optical second harmonic generation (SHG) technique. A hysteresis in the temperature dependence of the SHG intensity observed for a multilayer film of a poly(vinylidene fluoride)-trifluoroethylene copolymer in the vicinity of T≈15°C is a manifestation of the first-order ferroelectric phase transition in the topmost surface monolayer of the film.     

Characterization of Ag and Au nanoparticles created by nanosecond pulsed laser ablation in double distilled water

Pulsed laser ablation of Ag and Au targets, immersed in double-distilled water is used to synthesize metallic nanoparticles (NPs). The targets are irradiated for 20 min by laser pulses at different wavelengths—the fundamental and the second harmonic (SHG) (λ = 1064 and 532 nm, respectively) of a Nd:YAG laser system. The ablation process is performed at a repetition rate of 10 Hz and with pulse duration of 15 ns. Two boundary values of the laser fluence for each wavelength under the experimental conditions chosen were used—it varied from several J/cm² to tens of J/cm². Only as-prepared samples were measured not later than two hours after fabrication. The NPs shape and size distribution were evaluated from transmission electron microscopy (TEM) images. The suspensions obtained were investigated by optical transmission spectroscopy in the near UV and in the visible region in order to get information about these parameters. Spherical shape of the NPs at the low laser fluence and appearance of aggregation and building of nanowires at the SHG and high laser fluence was seen. Dependence of the mean particle size at the SHG on the laser fluence was established. Comments on the results obtained have been also presented.