Detailed analysis of the tilted-pulse-front pumping scheme used for ultrashort THz pulse generation by optical rectification of femtosecond laser pulses is presented. It is shown that imaging errors in a pulse-front-tilting setup consisting of a grating and a lens can lead to a THz beam with strongly asymmetric intensity profile and strong divergence, thereby limiting applications. Optimized setup parameters are given to reduce such distortions. We also show that semiconductors can offer a promising alternative to LiNbO(3) in high-energy THz pulse generation when pumped at longer wavelengths. This requires tilted-pulse-front pumping, however the small tilt angles allow semiconductors to be easily used in such schemes. Semiconductors can be advantageous for generating THz pulses with high spectral intensity at higher THz frequencies, while LiNbO(3) is better suited to generate THz pulses with very large relative spectral width. By using optimized schemes the upscaling of the energy of ultrashort THz pulses is foreseen.

Ultrashort terahertz pulses derived from femtosecond table-top sources have become a valuable tool for time-resolved spectroscopy during the last two decades. Until recently, the pulse energies and field strengths of these pulses have been generally too low to allow for the use as pump pulses or the study of nonlinear effects in the terahertz range. In this review article we will describe methods of generation of intense single cycle terahertz pulses with emphasis on optical rectification using the tilted-pulse-front pumping technique. We will also discuss some applications of these intense pulses in the emerging field of nonlinear terahertz spectroscopy.

reason for this interest relies on the fact that THz radiation can couple resonantly to numerous fundamental motions of ions, electrons, and electron spins in all phases of matter. For example, in solids, the THz range overlaps with the frequency of lattice vibrations (phonons), the collision rates of conduction electrons, the binding energy of bound electron-hole pairs (excitons), and the precession frequency of spin waves (magnons). Consequently, THz radiation, both continuous-wave and pulsed, has been used for characterization of and gaining insight into elementary processes in complex materials. The majority of these studies used relatively weak THz fields and, thus, probed the linear response of the material, without inducing notable material modifications.Only recently, however, completely new avenues in THz science were opened up by triggering nonlinear THz responses of materials. [3][4][5][6][7][8][9][10][11][12][13] Instead of using weak fields to primarily observe selected THz modes such as phonons or magnons, strong fields allow one to actively drive them to unprecedentedly large amplitudes, potentially thereby resulting in novel states of matter. [6,8,11] For example, simulations suggest that exciting matter with intense THz transients may lead to massive modifications of electrically [14] or magnetically [15] ordered domains and enable the acceleration of free ions to ≈1 MeV, [16] and postacceleration to 50-100 MeV energies. [17] Remarkable experimental results such as switching of magnetic order, [18,19] parametric amplification of optical phonons, [20] novel insights into spin-lattice coupling, [21,22] and acceleration of free electrons in a THz linear accelerator [23] were achieved only recently. This progress has been made possible by the development of laser-driven table-top THz sources routinely providing pulses with unprecedented energies and peak electric and magnetic field strengths throughout the entire THz spectral range. Different laser-based THz pulse generation techniques can be used to access different parts of the spectral range extending from 0.1 to 10 THz. Some of the recently developed technologies enable the generation of radiation with even larger bandwidth or tuning range up to 100 THz and beyond, which lead to an extension of what is called the THz spectral range. An overview of the approximate spectral coverage and the achieved highest pulse energies and peak electric-field strengths of various laserdriven technologies is given in Figure 1. ScopeIn this work, the basic principles of femtosecond-laser-driven intense pulsed THz sources and their recent development are reviewed. These sources are capable of delivering peak electric field strengths on the MV cm −1 scale. Corresponding typical THz pulse energies are on the µJ-to-mJ level, depending on A review on the recent development of intense laser-driven terahertz (THz) sources is provided here. The technologies discussed include various types of sources based on optical rectification (OR), spintronic emitters, and laserfilame...

Recent theoretical calculations predicted an order-of-magnitude increase in the efficiency of terahertz pulse generation by optical rectification in lithium niobate when 500 fs long pump pulses are used, rather than the commonly used ~100 fs pulses. Even by using longer than optimal pump pulses of 1.3 ps duration, 2.5× higher THz pulse energy (125 μJ) was measured with 2.5× higher pump-to-THz energy conversion efficiency (0.25%) than reported previously with shorter pulses. These results verify the advantage of longer pump pulses and support the expectation that mJ-level THz pulses will be available by cooling the crystal and using large pumped area.