Three-photon and four-photon absorption in lithium niobate measured by the Z-scan technique.

Open-aperture Z-scan measurements have been carried out to investigate the three-photon (3 PA) and four-photon absorption (4 PA) coefficients at 800 nm and 1030 nm wavelengths, respectively in congruent and stoichiometric lithium niobate (cLN, sLN) with different concentrations of Mg doping. The laser pulse duration at the two wavelengths were 40 and 190 fs. The peak intensity inside the crystals varied between approximately 110 and 550 GW/cm2. The 3 PA and 4 PA coefficients were evaluated using a theoretical model and the results suggest that their minima are at or around the Mg doping level corresponding to the threshold for suppressing photo-refraction for both cLN and sLN. This result can be attributed to the contribution of crystal defects to the 3 PA and 4 PA processes. Furthermore, the 4 PA at 1030 nm exhibited greater nonlinear absorption than the 3 PA at 800 nm under the same intensity level. Possible reasons for this unexpected behavior are discussed. Overall, comparing the 3 PA and 4 PA values of these crystals will enable for selection of the optimum composition of LN crystal for efficient THz generation and for other nonlinear optical processes requiring high pump intensities.

Possibility of CO2 laser-pumped multi-millijoule-level ultrafast pulse terahertz sources.

In the last decade, intense research has been witnessed on developing compact, terahertz (THz) driven electron accelerators, producing electrons with a sub-MeV-few tens of MeV energy. Such economical devices could be used in scientific and material research and medical treatments. However, until now, the extremely high-energy THz pulses needed by the THz counterparts of the microwave accelerators were generated by optical rectification (OR) of ultrafast Ti:sapphire or Yb laser pulses. These lasers, however, are not very effective. Because of this, we use numerical simulations to investigate the possibility of generating high-energy THz pulses by the OR of pulses produced by CO2 lasers, which can have high plug-in efficiency. The results obtained supposing optical rectification (OR) in GaAs demonstrate that consideration of the self-phase-modulation (SPM) and the second-harmonic-generation (SHG) processes is indispensable in the design of CO2 laser-based THz sources. More interestingly, although these two processes hinder achieving high laser-to-THz conversion efficiency, they can still surpass the 1.5% value, ensuring high system efficiency and making the CO2 laser OR system a promising THz source. Our finding also has important implications for other middle-infrared laser-pumped OR-based THz sources.

Subcycle surface electron emission driven by strong-field terahertz waveforms.

The advent of intense terahertz (THz) sources opened a new era when the demonstration of the acceleration and manipulation of free electrons by THz pulses became within reach. THz-field-driven electron emission was predicted to be confined to a single burst due to the single-cycle waveform. Here we demonstrate the confinement of single-cycle THz-waveform-driven electron emission to one of the two half cycles from a solid surface emitter. Either the leading or the trailing half cycle was active, controlled by reversing the field polarity. THz-driven single-burst surface electron emission sources, which do not rely on field-enhancement structures, will impact the development of THz-powered electron acceleration and manipulation devices, all-THz compact electron sources, THz waveguides and telecommunication, THz-field-based measurement techniques and solid-state devices.

Tilted pulse front pumping techniques for efficient terahertz pulse generation.

Optical rectification of femtosecond laser pulses has emerged as the dominant technique for generating single- and few-cycle terahertz (THz) pulses. The advent of the tilted pulse front pumping (TPFP) velocity matching technique, proposed and implemented two decades ago, has ushered in significant advancements of these THz sources, which are pivotal in the realm of THz pump-probe and material control experiments, which need THz pulses with microjoule energies and several hundred kV/cm electric field strengths. Furthermore, these THz sources are poised to play a crucial role in the realization of THz-driven particle accelerators, necessitating millijoule-level pulses with tens of MV/cm electric field strengths. TPFP has enabled the efficient velocity matching in lithium niobate crystals renowned for their extraordinary high nonlinear coefficient. Moreover, its adaptation to semiconductor THz sources has resulted in a two-hundred-times enhancement in conversion efficiency. In this comprehensive review, we present the seminal achievements of the past two decades. We expound on the conventional TPFP setup, delineate its scaling limits, and elucidate the novel generation TPFP configurations proposed to surmount these constraints, accompanied by their preliminary outcomes. Additionally, we provide an in-depth analysis of the THz absorption, refractive index, and nonlinear coefficient spectra of lithium niobate and widely used semiconductors employed as THz generators, which dictate their suitability as THz sources. We underscore the far-reaching advantages of tilted pulse front pumping, not only for LN and semiconductor-based THz sources but also for selected organic crystal-based sources and Yb-laser-pumped GaP sources, previously regarded as velocity-matched in the literature.

Demonstration of an imaging-free terahertz generation setup using segmented tilted-pulse-front excitation.

A novel, to the best of our knowledge, compact, imaging-free, tilted-pulse-front (TPF) pumped terahertz (THz) source based on a LiNbO3 slab with a small wedge angle (< 8°) and with an echelon microstructure on its input surface has been demonstrated. Single-cycle pulses of more than 40-µJ energy and 0.28-THz central frequency have been generated by 100-mJ, 400-fs pump pulses with 4.1 × 10-4 efficiency and excellent focusability. The peak electric field value focused by a single parabolic mirror was 540 kV/cm. Using 200-fs-long pump pulses, the efficiency increased to 1.0 × 10-3, which is in qualitative agreement with the measured increased diffraction efficiency in the velocity matched diffraction order. A further ∼8x increase in efficiency is expected by pumping a cryogenically cooled wedged echelon with appropriate step sizes, better microstructured surface quality, and antireflection coating on both the input and the output sides. THz generation efficiency maxima were found at ∼2.7-mm crystal thickness for both pump pulse durations. The focused THz beam was diffraction limited within 5% accuracy. Compared to conventional THz sources, this setup is very compact, easy to align, can be pumped by larger beam sizes maintaining the high THz generation efficiency, and produces THz pulses with superior focusability.

Scalable microstructured semiconductor THz pulse sources.

In recent years several microstructured lithium niobate THz pulse source were suggested for high-energy applications. Two types of those, the reflective and the transmissive nonlinear slab are adopted here for semiconductors. These new sources are scalable both in THz energy and size. Furthermore, they can outperform the already demonstrated contact grating source in diffraction and THz generation efficiency. Compared to the lithium niobate sources, they are more feasible, thanks to the easier manufacturing and the longer pump wavelength. They can produce intense, nearly single-cycle THz pulses at higher frequencies. With 20 mJ pumping at 1.8 µm wavelength, 45 µJ THz energy, and 17 MV/cm focused peak electric field can be expected at 3 THz phase matching frequency from the transmissive nonlinear echelon slab setup consisting of a 4 mm thick structured plan-parallel gallium phosphide crystal.

Waveguide structure based electron acceleration using terahertz pulses.

We have developed a waveguide structure for electron acceleration using a few µJ energy THz pulse. The metallic device focuses the incoming linearly polarized nearly single-cycle THz pulse, hence increasing the peak electric field strength. We experimentally verified the gain and the temporal profile of the electric field in the structure using electro-optic sampling technique. The acceleration of the electron bunch from rest up to 8 keV was predicted using single-cycle THz pulses with µJ-energy level.

Spatiotemporal modeling of direct acceleration with high-field terahertz pulses.

We present an improved model for electron acceleration in vacuum with high-energy THz pulses that includes spatiotemporal effects. In our calculations, we examined the acceleration with 300 GHz and 3.0 THz central frequency THz pulses with properties corresponding to common sources, and compared the Gaussian and Poisson spectral amplitudes and the associated time profiles of the electric fields. Our calculation takes into account both the longitudinal field and the spatio-spectral evolution around the focus. These aspects of the model are necessary due to the tight focusing and the duration towards a single-cycle of the THz pulses, respectively. The carrier-to-envelope phase (CEP) and the tilting angle of the coincident few- or single-cycle THz pulses must be tuned in all cases in order to optimize the acceleration scheme. We reveal additionally that electron beams with different final energies and different divergences can be generated based on simulated THz pulses having different Porras factors, describing the frequency dependence of the spatiotemporal amplitude profile, which may depend strongly on the method used to generate the single-cycle THz pulses.

Uniformly scalable lithium niobate THz pulse source in transmission geometry.

A novel THz source, based on optical rectification in LiNbO3 using the tilted-pulse-front technique, is proposed and experimentally demonstrated. The pulse-front tilt is introduced by a volume phase holographic grating, efficiently used at perpendicular incidence in transmission, and the THz pulses are produced in a LiNbO3 plane-parallel nonlinear echelon slab, arranged parallel to the grating. As a unique feature, the entire setup has a plane-parallel, transmission-type configuration, which straightforwardly enables distortion-free scaling to large sizes, high pulse energies and high THz field strengths. The possibility of operating the setup at cryogenic temperature for increased THz generation efficiency is also investigated. Calculations predict efficiencies of 95% for diffraction and 2% for THz generation at room temperature with a refractive-index-matching liquid between the grating and the echelon slab.

Terahertz pulses induce segment renewal via cell proliferation and differentiation overriding the endogenous regeneration program of the earthworm Eisenia andrei.

Terahertz (THz) irradiation of excised Eisenia andrei earthworms is shown to cause overriding of the genetically determined, endogenously mediated segment renewing capacity of the model animal. Single-cycle THz pulses of 5 µJ energy, 0.30 THz mean frequency, 293 kV/cm peak electric field, and 1 kHz repetition rate stimulated the cell proliferation (indicated by the high number of mitotic cells) and both histogenesis and organogenesis, producing a significantly higher number of regenerated segments. The most conspicuous alteration in THz-treated animals was the more intense development of the new central nervous system and blood vessels. These results clearly demonstrate that THz pulses are capable to efficiently trigger biological processes and suggest potential applications in medicine.

Lithium niobate and lithium tantalate based scalable terahertz pulse sources in reflection geometry.

A new type of THz source, working in reflection geometry, is proposed, where the pulse-front-tilt is introduced by a periodically micro-structured metal profile. For optical coupling, high refractive index nanocomposite fluid is used between the nonlinear optical material and the structured metal surface. Numerical simulations predict ∼87 and ∼85% optimized diffraction efficiencies for lithium niobate and lithium tantalate at 1030 and 800 nm pump wavelengths. The largest diffraction efficiencies can be achieved for a larger refractive index of the nanocomposite fluid than the index of the nonlinear material, for both cases. THz generation efficiencies of ∼3 and ∼1% are predicted for lithium niobate and lithium tantalate, respectively.

Single-cycle scalable terahertz pulse source in reflection geometry.

A tilted-pulse-front pumped terahertz pulse source is proposed for the generation of extremely high field single-cycle terahertz pulses. The very simple and compact source consists of a single crystal slab having a blazed reflection grating grooved in its back surface. Its further important advantages are the energy scalability and the symmetric THz beam profile. Generation of ∼50 MV/cm focused field with 10.8 mJ terahertz pulse energy is predicted for a 7 cm diameter LiNbO 3 crystal, if the pump pulse is of 870 mJ energy, 1030 nm central wavelength and 1 ps pulse duration. Such sources can decisively promote the realization of THz driven electron and proton accelerators and open the way for a new generation concept of terahertz pulses having extreme high field.

Numerical investigation of imaging-free terahertz generation setup using segmented tilted-pulse-front excitation.

Recently a hybrid-type terahertz (THz) pulse source was proposed for high energy terahertz pulse generation. It is the combination of the conventional tilted-pulse-front setup and a nonlinear crystal with a transmission stair-step echelon of period in the hundred-micrometer range etched into the front face. The tilt angle introduced by the conventional tilted-pulse-front setup (pre-tilt) was chosen to be equal to the tilt-angle needed inside the nonlinear crystal (62° for lithium niobate (LN)) in order to fulfill velocity-matching. In this case, plane-parallel nonlinear optical crystals can be used. The possibility of using a plane-parallel nonlinear optical crystal for producing good-quality, symmetric THz beams was considered the most important advantage of this setup. In the present paper, a thorough numerical investigation of a modified version of that setup is presented. In the new version, the tilted pulse-front is created by a transmission grating without any imaging optics, and a wedged nonlinear optical crystal with a small wedge angle is supposed. According to a 1D numerical code, significantly higher THz generation efficiency can be achieved with a transmission stair-step echelon-faced nonlinear crystal having a 5 - 15-degree wedge angle than with a plane-parallel one or with the conventional tilted-pulse-front setup. Because of the spatially-dependent group-delay dispersion introduced by the transmission grating, a small wedge in the nonlinear crystal improves the spatial homogeneity of the THz-generation process, resulting in higher efficiencies and better beam profiles. At 100 K temperature, and by using 800 nm pump pulses with 20 mJ pulse energy, 100 fs pulse length and 8 mm beam spot radius, approximately 4.5% conversion efficiency and close to 1 mJ terahertz pulse energy can be reached with the newly-proposed setup.

Demonstration of a tilted-pulse-front pumped plane-parallel slab terahertz source.

A new type of tilted-pulse-front pumped terahertz (THz) source has been demonstrated, which is based on a LiNbO3plane-parallel slab with an echelon structure on its input surface. Single-cycle pulses of 1 µJ energy and 0.30 THz central frequency have been generated with 5×10-4 efficiency from such a source. One order-of-magnitude increase in efficiency is expected by pumping a cryogenically cooled echelon of increased size and thickness with a Ti:sapphire laser. The use of a plane-parallel nonlinear optical crystal slab enables straightforward scaling to high THz pulse energies and the production of a symmetric THz beam with a uniform pulse shape for good focusability and high field strength.

Attosecond single-cycle undulator light: a review.

Research at modern light sources continues to improve our knowledge of the natural world, from the subtle workings of life to matter under extreme conditions. Free-electron lasers, for instance, have enabled the characterization of biomolecular structures with sub-ångström spatial resolution, and paved the way to controlling the molecular functions. On the other hand, attosecond temporal resolution is necessary to broaden our scope of the ultrafast world. Here we discuss attosecond pulse generation beyond present capabilities. Furthermore, we review three recently proposed methods of generating attosecond x-ray pulses. These novel methods exploit the coherent radiation of microbunched electrons in undulators and the tailoring of the emitted wavefronts. The computed pulse energy outperforms pre-existing technologies by three orders of magnitude. Specifically, our simulations of the proposed Soft X-ray Laser at MAX IV (Lund, Sweden) show that a pulse duration of 50-100 as and a pulse energy up to 5 [Formula: see text]J is feasible with the novel methods. In addition, the methods feature pulse shape control, enable the incorporation of orbital angular momentum, and can be used in combination with modern compact free-electron laser setups.

Ultrafast tunable modulation of light polarization at terahertz frequencies.

Controlling light polarization is one of the most essential routines in modern optical technology. Since the demonstration of optical pulse shaping by spatial light modulators and its potential in controlling the quantum reaction pathways, it paved the way for many applications as a coherent control of the photoionization process or as polarization shaping of terahertz (THz) pulses. Here, we evidenced efficient nonresonant and noncollinear χ(2)-type light-matter interaction in femtosecond polarization-sensitive time-resolved optical measurements. Such nonlinear optical interaction of visible light and ultrashort THz pulses leads to THz modulation of visible light polarization in bulk LiNbO3 crystal. Theoretical simulations based on the wave propagation equation capture the physical processes underlying this nonlinear effect. Apart from the observed tunable polarization modulation of visible pulses at ultrahigh frequencies, this physical phenomenon can be envisaged in THz depth-profiling of materials.

The effect of the flexibility of hydrogen bonding network on low-frequency motions of amino acids. Evidence from Terahertz spectroscopy and DFT calculations.

Low-frequency modes of L-Asp and L-Asn were studied in the range from 0.1 to 3.0THz using time-domain Terahertz spectroscopy and density functional theory calculation. The results show that PBE-D2 shows more success than BLYP-D2 in prediction of THz absorption spectra. To compare their low-frequency modes, we adopted "vibrational character ID strips" proposed by Schmuttenmaer and coworkers [Journal of Physical Chemistry B, 117, 10444(2013)]. We found that the most intense THz absorption peaks of two compounds both involve severe distortion of their hydrogen bonding networks. Due to less rigid hydrogen bonding network in L-Asp, the side chain (carboxyl group) of L-Asp exhibits larger motions than that (carboxamide group) of L-Asn in low-frequency modes.

Numerical investigation of a scalable setup for efficient terahertz generation using a segmented tilted-pulse-front excitation.

A hybrid-type terahertz pulse source is proposed for high energy terahertz pulse generation. It is the combination of the conventional tilted-pulse-front setup and a transmission stair-step echelon-faced nonlinear crystal with a period falling in the hundred-micrometer range. The most important advantage of the setup is the possibility of using plane parallel nonlinear optical crystal for producing good-quality, symmetric terahertz beam. Another advantage of the proposed setup is the significant reduction of imaging errors, which is important in the case of wide pump beams that are used in high energy experiments. A one dimensional model was developed for determining the terahertz generation efficiency, and it was used for quantitative comparison between the proposed new hybrid setup and previously introduced terahertz sources. With lithium niobate nonlinear material, calculations predict an approximately ten-fold increase in the efficiency of the presently described hybrid terahertz pulse source with respect to that of the earlier proposed setup, which utilizes a reflective stair-step echelon and a prism shaped nonlinear optical crystal. By using pump pulses of 50 mJ pulse energy, 500 fs pulse length and 8 mm beam spot radius, approximately 1% conversion efficiency and 0.5 mJ terahertz pulse energy can be reached with the newly proposed setup.

Photorefractive damage resistance threshold in stoichiometric LiNbO3:Zr crystals.

Several optical methods including ultraviolet absorption, infrared absorption of the hydroxyl ions, Raman spectroscopy, and the Z-scan method have been used to determine the damage resistance threshold in 0-0.72 mol. % Zr-containing, flux-grown, nearly stoichiometric LiNbO3 single crystals. All spectroscopical methods used indicate that samples containing at least ≈0.085 mol. % Zr in the crystal are above the threshold while Z-scan data locate the photorefractive damage threshold between 0.085 and 0.314 mol. % Zr.

Quasi-phase-matching high-harmonic radiation using chirped THz pulses.

High-order harmonic generation in the presence of a chirped THz pulse is investigated numerically with a complete 3D nonadiabatic model. The assisting THz pulse illuminates the high-order harmonic generation gas cell laterally inducing quasi-phase-matching. We demonstrate that it is possible to compensate the phase mismatch during propagation and extend the macroscopic cutoff of a propagated strong IR pulse to the single-dipole cutoff. We obtain 2 orders of magnitude increase in the harmonic efficiency of cutoff harmonics (≈170 eV) using a THz pulse of constant wavelength, and a further factor of 3 enhancement when a chirped THz pulse is used.