Owing to the extraordinary richness of its physical properties, congruent lithium niobate has attracted multidecade-long interest both for fundamental science and applications. The combination of ferro-, pyro-, and piezoelectric properties with large electro-optic, acousto-optic, and photoelastic coefficients as well as the strong photorefractive and photovoltaic effects offers a great potential for applications in modern optics. To provide powerful optical components in high energy laser applications, tailoring of key material parameters, especially stoichiometry, is required. This paper reviews the state of the art of growing large stoichiometric LiNbO 3 (sLN) crystals, in particular, the defect engineering of pure and doped sLN with emphasis on optical damage resistant (ODR) dopants (e.g., Mg, Zn, In, Sc, Hf, Zr, Sn). The discussion is focused on crystals grown by the high temperature top seeded solution growth (HTTSSG) technique using alkali oxide fluxing agents. Based on high-temperature phase equilibria studies of the Li 2 O-Nb 2 O 5 -X 2 O ternary systems (X ¼ Na, K, Rb, Cs), the impact of alkali homologue additives on the stoichiometry of the lithium niobate phase will be analyzed, together with a summary of the ultraviolet, infrared, and far-infrared absorption spectroscopic methods developed to characterize the composition of the crystals. It will be shown that using HTTSSG from K 2 O containing flux, crystals closest to the stoichiometric composition can be grown characterized by a UV-edge position of at about 302 nm and a single narrow hydroxyl band in the IR with a linewidth of less than 3 cm À1 at 300 K. The threshold concentrations for ODR dopants depend on crystal stoichiometry and the valence of the dopants; Raman spectra, hydroxyl vibration spectra, and Z-scan measurements prove to be useful to distinguish crystals below and above the photorefractive threshold. Crystals just above the threshold are preferred for most nonlinear optical applications apart holography and have the additional advantage to minimize the absorption even in the far-infrared (THz) range. The review also provides a discussion on the progress made in the characterization of non-stoichiometry related intrinsic and extrinsic defect structures in doped LN crystals, with emphasis on ODR-ion-doped and/or closely stoichiometric systems, based on both spectroscopic measurements and theoretical modelling, including the results of first principles quantum mechanical calculations on hydroxyl defects. It will also be shown that new perspective applications, e.g., the generation of high energy THz pulses with energies on the tens-of-mJ scale, are feasible with ODR-doped sLN crystals if optimal conditions, including the contact grating technique, are applied. V C 2015 AIP Publishing LLC.

Time domain THz spectroscopy measurements were performed on a series of undoped and Mg-doped congruent lithium niobate crystals with 1.2, 6.1, and 8.4 mol% Mg concentrations and on undoped and Mg-doped stoichiometric lithium niobate crystals with 0.7, 1.5, and 4.2 mol% Mg concentrations with polarization parallel (extraordinary) and perpendicular (ordinary) to the z axis of the crystal at 300 K. The absorption coefficient and refractive index spectra were determined in the THz frequency range from 0.25 to~2.5 THz. In the case of congruent samples for both polarizations, both the refractive index and the absorption coefficient have minimal values for compositions close to the photorefractive threshold. In the case of stoichiometric samples, similar tendencies close to the photorefractive threshold at lower Mg concentration were observed but only for extraordinary polarization, while for ordinary polarization the measured values, especially for the absorption coefficient, were only weakly dependent on the Mg content.

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The acceleration of single electrons and electron bunches by focused THz pulse pairs has been investigated by numerical simulations. The effect of the choice of the beam waist radius, the carrier-envelope phase, and the propagation direction of the THz pulses on the energy of the accelerated electrons was investigated. The acceleration of electron bunches from rest up to 150 keV was predicted using single-cycle THz pulses with 1 mJ energy and a central frequency in the 0.1 THz to 3.0 THz range. The post-acceleration of electrons by pairs of focused THz pulses has also been proposed.

Index of refraction and absorption coefficient spectra of pure paratellurite (α-TeO 2 ) crystal as a potential material for terahertz (THz) applications were determined in the 0.25-2 THz frequency range at room temperature by THz time domain spectroscopy (THz-TDS). The investigation was performed with beam polarization both parallel (extraordinary polarization) and perpendicular (ordinary polarization) to the optical axis