Twenty-nine chlorites, seventeen lithium-free micas, and twenty-two lithium-bearing micas from diverse localities have been studied by X-ray diffraction, microprobe, and optical second harmonic generation (SHG) techniques to determine which are noncentric and the cause of acentricity. Manandonite (B-rich chlorite) and cookeite, both crystallizing in the Ia form, are acentric. Sudoite-IIb gave a questionable SHG signal, possibly indicating acentricity. All other chlorites gave null signals. Bityite, a Li, Be mica similar to margarite, was determined from the positive SHG response to be acentric. It crystallizes in the 2M1 form and, by analogy to margarite, is ordered tetrahedrally in subgroup symmetry, Cc. Masutomilite-1M and “cryophyllite“-1M (a zinnwaldite high in Al and Si, but low in Fe) are acentric and most probably crystallize in space group C2, thus allowing a noncentric octahedral ordering pattern. Lepidolites showed a diversity in SHG response with only a few being acentric; a lepidolite-1M from Mesagrande, California, a lepidolite-3T from Windhuk, South West Africa, and a lepidolite-2M2 from Nagatare, Japan, gave positive SHG responses. The Japanese material is complexly intergrown and twinned, and intergrain reflection or refraction may have produced spurious signals.

Most lithium-free micas showed diversity in SHG response and, although most were non-emitters, clintonite from Amity, New York, showed a positive response, but this sample is twinned and shows stacking disorder. A “manganophyllite”-1M (manganoan phlogopite) from Langban, Sweden, showed a very weak positive response; however, the presence of Mn alone is not suffcient to produce octahedral cation ordering in noncentric subgroup symmetry. Two manganoan phlogopites from Japan were refined in subgroup symmetry, and the higher order and ideal symmetry of C2/m was confirmed.

We demonstrate the generation, spectral broadening and post-compression of second harmonic pulses using a thin beta barium borate (BBO) crystal on a fused-silica substrate as the nonlinear interaction medium. By combining second harmonic generation in the BBO crystal with self-phase modulation in the fused-silica substrate, we efficiently generate millijoule-level broadband violet pulses from a single optical component. The second harmonic spectrum covers a range from long wave ultraviolet (down to 310 nm) to visible (up to 550 nm) with a bandwidth of 65 nm. Subsequently, we compress the second harmonic beam to a duration of 4.8 fs with a pulse energy of 0.64 mJ (5 fs with a pulse energy of 1.05 mJ) using chirped mirrors. The all-solid free-space apparatus is compact, robust and pulse energy scalable, making it highly advantageous for generating intense second harmonic pulses from near-infrared femtosecond lasers in the sub-5 fs regime.

Engineered biomaterials provide unique functions to overcome the bottlenecks seen in biomedicine. Hence, a technique for rapid and routine tests of collagen is required, in which the test items commonly include molecular weight, crosslinking degree, purity, and sterilization induced structural change. Among them, the crosslinking degree mainly influences collagen properties. In this study, second harmonic generation (SHG) and coherent anti-Stokes Raman scattering (CARS) microscopy are used in combination to explore the collagen structure at molecular and macromolecular scales. These measured parameters are applied for the classification and quantification among the different collagen scaffolds, which were verified by other conventional methods. It is demonstrated that the crosslinking status can be analyzed from SHG images and presented as the coherency of collagen organization that is correlated with the mechanical properties. Also, the comparative analyses of SHG signal and relative CARS signal of amide III band at 1,240 cm−1 to δCH2 band at 1,450 cm−1 of these samples provide information regarding the variation of the molecular structure during a crosslinking process, thus serving as nonlinear optical signatures to indicate a successful crosslinking.

We report high-energy, high-efficiency second harmonic generation in a near-infrared all-solid-state burst-mode picosecond laser at a repetition rate of 1 kHz with four pulses per burst using a type-I noncritical phase-matching lithium triborate crystal. The pulses in each burst have the same time delay (${\sim}1~\text{ns}$), the same pulse duration (${\sim}100~\text{ps}$) and different relative amplitudes that can be adjusted separately. A mode-locked beam from a semiconductor saturable absorber mirror is pulse-stretched, split into seed pulses and injected into a Nd:YAG regenerative amplifier. After the beam is reshaped by aspheric lenses, a two-stage master oscillator power amplifier and 4f imaging systems are applied to obtain a high power of ${\sim}100~\text{W}$. The 532 nm green laser has a maximum conversion efficiency of 68%, an average power of up to 50 W and a beam quality factor $M^{2}$ of 3.5.

In this paper, the scheme of generation of second harmonics of incident electromagnetic wave having a Hermite–Gaussian intensity profile in an under dense relativistic plasma has been presented. The relativistic mass variation of electrons by the intense electric field of incident beam generates the density gradients in background plasma which further excites the electron plasma wave (EPW) at resonant frequency and coupling of the EPW with the incident beam results in the generation of second harmonics of incident beam. Propagation dynamics of the Hermite–Gaussian laser beam in plasma has been studied by the formulation of differential equation for the spot size of the laser beam with the help of method of moments. Numerical simulations have been carried out to solve the differential equation for the dimensionless beam width parameters. Solution of the nonlinear wave equation for the electric field vector of second harmonics of incident beam gives the expression for second-harmonic yield. It has been observed that second-harmonic yield is affected by the different modes of Hermite–Gaussian laser beam in relativistic plasma.

We demonstrate high efficiency second harmonic generation (SHG) of near infrared femtosecond pulses using a $\text{BiB}_{3}\text{O}_{6}$ crystal in a single-pass tight focusing geometry setup. A frequency doubling efficiency of $63\%$ is achieved, which is, to the best of our knowledge, the highest value ever reported in the femtosecond regime for such low energy (nJ-level) pumping pulses. Theoretical analyses of the pumping scheme focusing waist and the SHG efficiency are performed, by numerically solving the three wave mixing coupled equations in the plane-wave scenario and by running simulations with a commercial full 3D code. Simulations show a good agreement with the experimental data regarding both the efficiency and the pulse spectral profile. The simulated SHG pulse temporal profile presents the characteristic features of the group velocity mismatch broadening in a ‘thick’ crystal.

Enhanced harmonic generation of second order based on exponential density ramp in plasma has been noticed. It is well known that self-focusing of pump laser induces a transverse intensity gradient, which gives rise to the plasma wave at the pump frequency. Highly intense Gaussian laser with exponential density ramp profile generates a second harmonic pulse in plasma. It is noticed that the amplitude of second-harmonic pulse varies periodically with the distance and reaches its peak value in the focal region. Further, it is found that exponential plasma density ramp is useful for stronger self-focusing, which lead to rise second harmonic generation (SHG). Wiggler magnetic field provides the additional angular momentum required for second harmonic photon and aids in growing of resonant process. One may clearly see that exponential plasma density ramp imparts a major role in enhancing the SHG in plasma. Further, the combined effect of exponential density ramp and wiggler magnetic field boosts the SHG in plasma.

The method for measuring synchronization error of ultra-short pulses was introduced based on the principle of non-collinear cross-correlation. The analytical expression for the measurement was deduced according to the cross-correlation signal. The influences of angular error on the measurement were analyzed by simulated experiments. The incident angle and the angular error tolerance were both required to be considered and determined for the synchronization error measurement of ultra-short pulses. The results provide a theoretical basis for the measurement and control of the synchronization error in the coherent beam combination, plasma parameter diagnosis, etc.

This paper presents an investigation of self-focusing of Gaussian laser beam in collisional plasma and its effect on second harmonic generation. Due to non-uniform heating, collisional non-linearity arises, which leads to redistribution of carriers and hence affects the plasma wave, which in turn affects the second harmonic generation. Effect of the intensity of the laser beam/plasma density on the harmonic yield is studied in detail. We have set up the non-linear differential equations for the beam width parameters of the main beam, plasma wave, second harmonic generation and second harmonic yield by taking full non-linear part of the dielectric constant of collisional plasma with the help of moment theory approach. It is predicted from the analysis that harmonic yield increases/decreases due to increase in the plasma density/intensity of the laser beam respectively.

A computational study on the enhancement of the second harmonic generation (SHG) in one-dimensional (1D) photonic crystals is presented. The mathematical model is derived from a nonlinear system of Maxwell’s equations, which partly overcomes the shortcoming of some existing models based on the undepleted pump approximation. We designed an iterative scheme coupled with the finite element method which can be applied to simulate the SHG in one dimensional nonlinear photonic band gap structures in our previous work. For the case that the nonlinearity is strong which is desirable to enhance the conversion efficiency, a continuation method is introduced to ensure the convergence of the iterative procedure. The convergence of our method is fast. Numerical experiments also indicate the conversion efficiency of SHG can be significantly enhanced when the frequencies of the fundamental and the second harmonic wave are tuned at the photonic band edges. The maximum total conversion efficiency available reaches more than 50% in all the cases studied.

The strong azimuthal magnetic fields, observed in many laser plasma experiments, are shown to be a potential source of second harmonic generation. The laser imparts oscillatory velocity to electrons and exerts a longitudinal pondromotive force on them. This force in conjunction with the azimuthal magnetic field and density ripple produces a second harmonic current with significant transverse component. The latter produces resonant second harmonic radiation.

This paper presents the laser beam filamentation at ultra relativistic laser powers, when the paraxial restriction on the beam is relaxed during the filamentation process. On account of laser beam intensity gradient and background density gradients in filamentary regions, the electron plasma wave (EPW) at pump wave frequency is generated. This EPW is found to be highly localized because of the laser beam filaments. The interaction of the incident laser beam with the EPW leads to the second harmonic generation. The second harmonic spectrum has also been studied in detail, and its correlation with the filamentation of the laser beam has been established. Starting almost with a monochromatic component of laser beam propagation, the second harmonic spectrum becomes more complicated, and broadened when the laser beam propagates further, and filamentation takes place. For the typical laser beam and plasma parameters: laser beam with wave length of 1064 nm, power flux of 1018 W/cm2, and plasma with temperature 1 KeV, we found that the conversion efficiency equals about (E2/E0) = 8 × 10−3, and the spectrum is quite broad, which depends upon the laser beam propagation distance. The results (specifically, the second harmonic spectral feature) presented here may be used for the diagnostics of laser produced plasmas.

Two-photon excitation microscopy has become the standard technique for high resolution deep tissue and intravital imaging. It provides intrinsic three-dimensional resolution in combination with increased penetration depth compared to single-photon confocal microscopy. This article will describe the basic physical principles of two-photon excitation and will review its multiple applications to cardiovascular imaging, including second harmonic generation and fluorescence laser scanning microscopy. In particular, the capability and limitations of multiphoton microscopy to assess functional heterogeneity on a cellular scale deep within intact, Langendorff-perfused hearts are demonstrated. It will also discuss the use of two-photon excitation-induced release of caged compounds for the study of intracellular calcium signaling and intercellular dye transfer.