Generation of strong-field spectrally tunable terahertz pulses.

The ideal laser source for nonlinear terahertz spectroscopy offers large versatility delivering both ultra-intense broadband single-cycle pulses and user-selectable multi-cycle pulses at narrow linewidths. Here we show a highly versatile terahertz laser platform providing single-cycle transients with tens of MV/cm peak field as well as spectrally narrow pulses, tunable in bandwidth and central frequency across 5 octaves at several MV/cm field strengths. The compact scheme is based on optical rectification in organic crystals of a temporally modulated laser beam. It allows up to 50 cycles and central frequency tunable from 0.5 to 7 terahertz, with a minimum width of 30 GHz, corresponding to the photon-energy width of ΔE=0.13 meV and the spectroscopic-wavenumber width of Δ(λ-1)=1.1 cm-1. The experimental results are excellently predicted by theoretical modelling. Our table-top source shows similar performances to that of large-scale terahertz facilities but offering in addition more versatility, multi-colour femtosecond pump-probe opportunities and ultralow timing jitter.

Intense, carrier frequency and bandwidth tunable quasi single-cycle pulses from an organic emitter covering the Terahertz frequency gap.

In Terahertz (THz) science, one of the long-standing challenges has been the formation of spectrally dense, single-cycle pulses with tunable duration and spectrum across the frequency range of 0.1-15 THz (THz gap). This frequency band, lying between the electronically and optically accessible spectra hosts important molecular fingerprints and collective modes which cannot be fully controlled by present strong-field THz sources. We present a method that provides powerful single-cycle THz pulses in the THz gap with a stable absolute phase whose duration can be continuously selected between 68 fs and 1100 fs. The loss-free and chirp-free technique is based on optical rectification of a wavelength-tunable pump pulse in the organic emitter HMQ-TMS that allows for tuning of the spectral bandwidth from 1 to more than 7 octaves over the entire THz gap. The presented source tunability of the temporal carrier frequency and spectrum expands the scope of spectrally dense THz sources to time-resolved nonlinear THz spectroscopy in the entire THz gap. This opens new opportunities towards ultrafast coherent control over matter and light.

High efficiency THz generation in DSTMS, DAST and OH1 pumped by Cr:forsterite laser.

We investigated Terahertz generation in organic crystals DSTMS, DAST and OH1 directly pumped by a Cr:forsterite laser at central wavelength of 1.25 µm. This pump laser technology provides a laser-to-THz energy conversion efficiency higher than 3 percent. Phase-matching is demonstrated over a broad 0.1-8 THz frequency range. In our simple setup we achieved hundred µJ pulses in tight focus resulting in electric and magnetic field larger than 10 MV/cm and 3 Tesla.

High-energy terahertz pulses from organic crystals: DAST and DSTMS pumped at Ti:sapphire wavelength.

High-energy terahertz pulses are produced by optical rectification (OR) in organic crystals 4-dimethylamino-N-methyl-4-stilbazolium tosylate (DAST) and 4-N, N-dimethylamino-4'-N'-methyl-stilbazolium 2,4,6-trimethylbenzenesulfonate (DSTMS) by a Ti:sapphire amplifier system with 0.8 µm central wavelength. The simple scheme provides broadband spectra between 1 and 5 THz, when pumped by a collimated 60 fs near-IR pump pulse, and it is scalable in energy. Fluence-dependent conversion efficiency and damage threshold are reported, as well as optimized OR at visible wavelengths.

Nonlinear optical coefficients and phase-matching conditions in Sn(2)P(2)S(6).

Phase matching conditions and second and third order nonlinear optical coefficients of Sn2P2S6 crystals are reported. The coefficients for second harmonic generation (SHG) are given at lambda = 1542 nm and 1907 nm at room temperature. The largest coefficients at these wavelengths are d111 = 17+/-1.5pm/V and d111 = 12+/-1.5pm/V, respectively. The third-order subsceptibilities chi(3) 1111 = (17 +/- 6) . 10-20m2/V2 and chi(3) 2222 = (9 +/- 3) . 10-20m2/V2 were determined at lambda = 1907 nm. All measurements were performed by the Maker-Fringe technique. Based on the recently determined refractive indices, we analyze the phase-matching conditions for second harmonic generation, sum- and difference-frequency generation and parametric oscillation at room temperature. Phase-matching curves as a function of wavelength and propagation direction are given. Experimental phase-matched type I SHG at 1907 nm has been demonstrated. The results agree very well with the calculations. It is shown that phase-matched optical parametrical oscillation is possible in the whole transparency range up to 8 microm with an effective nonlinear coefficient deff approximately 4pm/V.

Structural transitions in holographic polymer-dispersed liquid crystals.

Dynamic light scattering was used to analyze the structural and dynamic properties of nematic director field within liquid crystal domains formed in holographic polymer-dispersed liquid crystal transmission gratings. Samples prepared from two different types of prepolymer mixture: one curable with visible (VIS) and another curable with UV light were investigated. In both formulations a critical slowing down of thermal director fluctuations, signifying the second-order structural transition of the nematic director field was observed in the vicinity of some critical external electric field as well as close to some critical temperature. For VIS samples also the size and the shape of phase separated droplets and viscoelastic and surface anchoring parameters of the liquid crystalline (LC) material forming the droplets were deduced. The viscoelastic constants were found to significantly deviate from the viscoelastic parameters of the pure LC mixture.