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A study of bulk second harmonic generation (SHG) response of lithium niobium silicate glass‐ceramics is presented. The observed macroscopic SHG signals have an isotropic 3D nature. To interpret this particular nonlinear optical response, a multiscale approach is used in which clear correlations between structure and optical response are characterized from the sub‐micrometer to the millimeter scale. In particular, it is inferred that the radial distribution of the LiNbO3 crystallites in spherulite domains is at the origin of the isotropic bulk second order optical property. It is suggested that spherulitic crystallization in glass‐ceramic is a challenging method to elaborate isotropic nonlinear optical properties in inorganic materials.

The focusing property of a focal spot of a femtosecond laser pulse is presented under tight focusing conditions (below f-number of 1). The spatial and temporal intensity distributions of a focused electric field are calculated by vector diffraction integrals and coherent superposition method. The validity of the calculation method is examined by comparing the intensity distribution obtained under a high f-number condition to that obtained with the fast Fourier transform method that assumes the scalar paraxial approximation. The spatial and temporal modifications under tight focusing conditions are described for a focused femtosecond laser pulse. The calculation results show that a peak intensity of about 2.5x10(24) W/cm2 can be achievable by tightly focusing a 12-fs, 10 PW laser pulse with a f/0.5 parabolic optic. The precise information on intensity distributions of a femtosecond focal spot obtained under a tight focusing condition will be crucial in assessing a focused intensity and in describing the motion of charged particles under an extremely strong electric field in ultra-relativistic and/or relativistic laser matter-interaction studies.

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An extended study of lithium niobium silicate glass crystallization with the molar composition 35Li2O–25Nb2O5–40SiO2 is presented. Depending on the heat treatments, both surface and/or bulk crystallizations of the LiNbO3 crystalline phase were observed. X‐ray diffraction together with second harmonic generation (SHG) measurements have revealed a net preferred orientation of the ferroelectric crystallites at the surface which is quite different in the bulk. A striking and promising SHG response estimated to be five times larger than α‐quartz has been observed in the bulk.

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