Intense pulses at low terahertz (THz) frequencies of 0.1-2 THz are an enabling tool for constructing compact particle accelerators and for strong-field control of matter. Optical rectification in lithium niobate provided sub-mJ THz pulse energies, but it is challenging to increase it further. Semiconductor sources suffered from low efficiency. Here, a semiconductor (ZnTe) THz source is demonstrated, collinearly pumped at an infrared wavelength beyond the three-photon absorption edge and utilizing a contact grating for tilting the pump-pulse front. Suppression of free-carrier absorption at THz frequencies in this way resulted in 0.3% THz generation efficiency, two orders of magnitude higher than reported previously from ZnTe. Scaling the THz energy to the mJ level is possible simply by increasing the pumped area. This unique THz source with excellent focusability, pumped by novel, efficient infrared sources, opens up new perspectives for THz high-field applications. Terahertz (THz) pulses with high energy and field strength are enabling novel applications [1-4], including resonant control over ionic motion, bound and free electrons, as well as nonresonant and strong-field interactions [3]. Intense THz pulses hold promise for the development of a new generation of compact particle and x-ray sources [1,2]. Laser-and THz-driven particle accelerators with unprecedented flexibility can be important for free-electron lasers [2,5] and materials science and could revolutionize medical therapy with x-ray, electron, or proton beams [1,2].Single-cycle or nearly single-cycle THz pulses with high energy can be generated by optical rectification of femtosecond laser pulses. The highest so far THz pulse energy reported from such a source, utilizing the novel organic nonlinear material DSTMS, was 0.9 mJ [6]. The spectrum obtained from organic materials is typically centered in the 2 to 10 THz range, well suited for nonlinear spectroscopic studies. THz sources with lower frequencies are optimally fitted to the requirements of particle acceleration [1,2,7]. The frequency range below 2 THz can be better accessed with another nonlinear material, lithium niobate, utilizing pump pulses with a tilted intensity front for non-collinear phase matching [8]. THz pulses with more than 0.4 mJ energy were generated with 0.77% efficiency using this technique [7]. However, increasing the THz energy further turned out to be very challenging because of the large pulse-front tilt angle (63°) and the associated large angular dispersion of the pump [9,10]. The effect of a strong THz field on the pump pulse, owing to their nonlinear interaction, leads to additional difficulties involving the reduction of the THz generation efficiency [11] and the distortion of the THz beam [12].Semiconductor nonlinear materials have been extensively used to access the low-frequency part of the THz spectrum. The most popular material is ZnTe, where collinear phase matching is possible at the commonly used 0.8 μm pump wavelength of Ti:sapphire lasers. The highest THz pu...

Abstract:A new route to efficient generation of THz pulses with high-energy was demonstrated using semiconductor materials pumped at an infrared wavelength sufficiently long to suppress both two-and three-photon absorption and associated free-carrier absorption at THz frequencies. For pumping beyond the three-photon absorption edge, the THz generation efficiency for optical rectification of femtosecond laser pulses with tilted intensity front in ZnTe was shown to increase 3.5 times, as compared to pumping below the absorption edge. The four-photon absorption coefficient of ZnTe was estimated to be ( ) THz pulses with 14 μJ energy were generated with as high as 0.7% efficiency in ZnTe pumped at 1.7 µm. It is shown that scaling the THz pulse energy to the mJ level by increasing the pump spot size and pump pulse energy is feasible.

Near-and far-field beam profiles were measured for THz pulses generated in LiNbO 3 by optical rectification of 200 fs pulses with a tilted pulse front. The variation of the THz beam size and a dramatically increasing divergence angle with increasing pump fluence were observed in the (horizontal) plane of the pulse front tilt. No significant variation was observed in the vertical direction. The reason for the observed nonlinear beam distortion is the shortening of the effective interaction length for THz generation caused by the combined effect of pump spectral broadening and angular dispersion in the tilted pulse front geometry. Our results indicate that nonlinear THz beam distortion effects have to be taken into account when designing intense THz sources and related experiments.

Multicycle THz pulse generation by optical rectification in GaP semiconductor nonlinear material is investigated by numerical simulations. It is shown that GaP can be an efficient and versatile source with up to about 8% conversion efficiency and a tuning range from 0.1 THz to about 7 THz. Contact-grating technology for pulse-front tilt can ensure an excellent focusability and scaling the THz pulse energy beyond 1 mJ. Shapeable infrared pump pulses with a constant intensity-modulation period can be delivered for example by a flexible and efficient dual-chirped optical parametric amplifier. Potential applications include linear and nonlinear THz spectroscopy and THz-driven acceleration of electrons.

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