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.

Broadband and narrowband laser-based terahertz source and its application for resonant and non-resonant excitation of antiferromagnetic modes in NiO.

A versatile table-top high-intense source of terahertz radiation, enabling to generate pulses of both broadband and narrowband spectra with a tunable frequency up to 3 THz is presented. The terahertz radiation pulses are generated by optical rectification of femtosecond pulses of Cr:forsterite laser setup in nonlinear organic crystal OH1. Electric field strengths of broadband and narrowband terahertz pulses were achieved close to 20 MV/cm and more than 2 MV/cm, correspondingly. Experiments on excitation of spin subsystem oscillations of an antiferromagnetic NiO were carried out. Selective excitation of 0.42 THz mode was observed for the first time at room temperature by a narrowband terahertz pulses tuned close to mode frequency.

Fourier transform spectroscopy in the vibrational fingerprint region with a birefringent interferometer.

We introduce a birefringent interferometer for Fourier transform (FT) spectroscopy in the mid-infrared, covering the vibrational fingerprint region (5-10 µm, 1000-2000 cm-1), which is crucial for molecular identification. Our interferometer employs the crystal calomel (Hg2Cl2), which combines high birefringence (ne-no≈0.55) with a broad transparency range (0.38-20 µm). We adopt a design based on birefringent wedges, which is simple and compact and guarantees excellent delay accuracy and long-term stability. We demonstrate FTIR spectroscopy, with a frequency resolution of 3 cm-1, as well as two-dimensional IR (2DIR) spectroscopy. Our setup can be extended to other spectroscopic modalities such as vibrational circular dichroism and step-scan FT spectroscopy.

Short X-ray pulses from third-generation light sources.

High-brightness X-ray radiation produced by third-generation synchrotron light sources (TGLS) has been used for numerous time-resolved investigations in many different scientific fields. The typical time duration of X-ray pulses delivered by these large-scale machines is about 50-100 ps. A growing number of time-resolved studies would benefit from X-ray pulses with two or three orders of magnitude shorter duration. Here, techniques explored in the past for shorter X-ray pulse emission at TGLS are reviewed and the perspective towards the realisation of picosecond and sub-picosecond X-ray pulses are discussed.

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.

Towards enabling femtosecond helicity-dependent spectroscopy with high-harmonic sources.

Recent advances in high-harmonic generation gave rise to soft X-ray pulses with higher intensity, shorter duration and higher photon energy. One of the remaining shortages of this source is its restriction to linear polarization, since the yield of generation of elliptically polarized high harmonics has been low so far. We here show how this limitation is overcome by using a cross-polarized two-colour laser field. With this simple technique, we reach high degrees of ellipticity (up to 75%) with efficiencies similar to classically generated linearly polarized harmonics. To demonstrate these features and to prove the capacity of our source for applications, we measure the X-ray magnetic circular dichroism (XMCD) effect of nickel at the M2,3 absorption edge around 67 eV. There results open up the way towards femtosecond time-resolved experiments using high harmonics exploiting the powerful element-sensitive XMCD effect and resolving the ultrafast magnetization dynamics of individual components in complex materials.

Generation of 0.9-mJ THz pulses in DSTMS pumped by a Cr:Mg2SiO4 laser.

We report on high-field terahertz transients with 0.9-mJ pulse energy produced in a 400 mm² partitioned organic crystal by optical rectification of a 30-mJ laser pulse centered at 1.25 µm wavelength. The phase-locked single-cycle terahertz pulses cover the hard-to-access low-frequency range between 0.1 and 5 THz and carry peak fields of more than 42 MV/cm and 14 Tesla with the potential to reach over 80 MV/cm by choosing appropriate focusing optics. The scheme based on a Cr:Mg2SiO4 laser offers a high conversion efficiency of 3% using uncooled organic crystal. The collimated pump laser configuration provides excellent terahertz focusing conditions.

Intense sub-two-cycle infrared pulse generation via phase-mismatched cascaded nonlinear interaction in DAST crystal.

Octave-spanning, 12.5 fs, (1.9 cycle) pulses with 115 µJ energy in the short-wavelength mid-infrared spectral range (1-2.5 µm) have been generated via phase-mismatched cascaded nonlinear frequency conversion using organic DAST (4-N, N-dimethylamino-4'-N'-methylstilbazolium tosylate) crystal. Such ultrafast cascading effect is ensured by the interaction of a pump pulse with the exceptionally large effective nonlinearity of the DAST crystal and experiencing nonresonant, strongly phase-mismatched, Kerr-like negative nonlinearity.

Large-amplitude spin dynamics driven by a THz pulse in resonance with an electromagnon.

Multiferroics have attracted strong interest for potential applications where electric fields control magnetic order. The ultimate speed of control via magnetoelectric coupling, however, remains largely unexplored. Here, we report an experiment in which we drove spin dynamics in multiferroic TbMnO3 with an intense few-cycle terahertz (THz) light pulse tuned to resonance with an electromagnon, an electric-dipole active spin excitation. We observed the resulting spin motion using time-resolved resonant soft x-ray diffraction. Our results show that it is possible to directly manipulate atomic-scale magnetic structures with the electric field of light on a sub-picosecond time scale.

High-precision x-ray FEL pulse arrival time measurements at SACLA by a THz streak camera with Xe clusters.

The accurate measurement of the arrival time of a hard X-ray free electron laser (FEL) pulse with respect to a laser is of utmost importance for pump-probe experiments proposed or carried out at FEL facilities around the world. This manuscript presents the latest device to meet this challenge, a THz streak camera using Xe gas clusters, capable of pulse arrival time measurements with an estimated accuracy of several femtoseconds. An experiment performed at SACLA demonstrates the performance of the device at photon energies between 5 and 10 keV with variable photon beam parameters.

Pump pulse width and temperature effects in lithium niobate for efficient THz generation.

We present a study on THz generation in lithium niobate pumped by a powerful and versatile Yb:CaF(2) laser. The unique laser system delivers transform-limited pulses of variable duration (0.38-0.65 ps) with pulse energies up to 15 mJ and center wavelength of 1030 nm. From previous theoretical investigations, it is expected that such laser parameters are ideally suited for efficient THz generation. Here, we present experimental results on both the conversion efficiency and the THz spectral shape for variable pump pulse durations and for different crystal temperatures, down to 25 K. We experimentally verify the optimum pump parameters for the most efficient and broadband THz generation.

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.

Large charge extraction from metallic multifilamentary Nb3Sn photocathode.

The current density limit for photoemission from metals was measured in an rf photogun to be below 10(9) A/m2. We have achieved 1.6×10(11) A/m2 by photofield emission from a new type of photocathode made from a metallic-composite, multifilamentary Nb3Sn wire driven by a 266 nm picosecond laser pulse and a 2 ns, 50 kV accelerating voltage. This cathode has a micrometer arrayed structure with tens of thousands of Nb/Nb3Sn filaments embedded in a bronze matrix. Our measurements revealed the existence of a new electron emission regime at high laser fluence (100 mJ/cm2). We have extracted stably, and without any surface ablation, up to 4800 pC of charge. This corresponds to 0.9% quantum efficiency, 100 times larger than what is measured from conventional metallic photocathodes. The unexpected large and stable charge extraction cannot be explained by the 3-step model. Thanks to the small emitting area, the measured emittance (0.6 mm·mrad) is low in spite of the high current density and space charge effects. This cathode will be of benefit for many applications based on short and bright electron bunches.

Self-referenced spectral interferometry for ultrashort infrared pulse characterization.

We demonstrate for the first time (to our knowledge) characterization of ultrashort IR pulses by self-referenced spectral interferometry. Both sub-55-fs pulses from 1.4 µm to 2 µm and broadband 2.5-cycle pulses at 1.65 µm (13 fs FWHM) are characterized.

Deep-ultraviolet picosecond flat-top pulses by chirp-matched sum frequency generation.

Picosecond, flat-top, deep-UV pulses are needed to generate high-brightness electron beams to efficiently drive x-ray free electron lasers. Current metal photocathodes have low efficiency and therefore require high-energy pulses, and the generation of high-energy, flat-top pulses in the deep UV is still challenging. The low efficiencies of both the harmonic generation and deep-UV pulse shapers restrict the accessible pulse energy. Moreover, the acceptance bandwidth of the harmonic generation limits the minimum rise time of the flat-top profile. We present the generation of few-hundred microjoule, picosecond, deep-UV pulses using chirp-matched sum frequency generation. This scheme combined with IR spectral manipulation is a novel approach for deep-UV pulse shaping. It permits flat-top pulses with high energy and fast rise time, highly suited for high-brightness photoelectron beam production.

Intrinsic emittance reduction of an electron beam from metal photocathodes.

Electron beams in modern linear accelerators are now becoming limited in brightness by the intrinsic emittance of the photocathode electron source. Therefore it becomes important for large scale facilities such as free electron lasers to reduce this fundamental limit. In this Letter we present measurements of the intrinsic emittance for different laser wavelength (from 261 to 282 nm) and for different photocathode materials such as Mo, Nb, Al, Cu. Values as low as 0.41±0.03 mm·mrad/mm laser spot size (rms) were measured for a copper photocathode illuminated with a 282 nm laser wavelength. The key element for emittance reduction is a uv laser system which allows adjustment of the laser photon energy to match the effective work function of the cathode material and to emit photoelectrons with a lower initial kinetic energy. The quantum efficiency over the explored wavelength range varies by less than a factor of 3.

Control and characterization of multiple circularly polarized femtosecond filaments in argon.

We provide what is believed to be the first experimental evidence of spatial control on multiple filamentation (MF) using circularly polarized femtosecond laser pulses. The exceptional shot-to-shot reproducibility of the MF pattern allowed complete characterization of the two copropagating high-energy filaments, revealing for the first time temporal (self-) compression of circularly polarized filamenting pulses to a fifth of the initial 57 fs laser pulse duration without any sophisticated chirp control. Compared with LP MF, an enhancement in spatial stability and an increase in energy throughput are reported for circular input polarization.

Intense self-compressed, self-phase-stabilized few-cycle pulses at 2 microm from an optical filament.

We report the compression of intense, carrier-envelope phase stable mid-IR pulses down to few-cycle duration using an optical filament. A filament in xenon gas is formed by using self-phase stabilized 330 microJ 55 fs pulses at 2 microm produced via difference-frequency generation in a Ti:sapphire-pumped optical parametric amplifier. The ultrabroadband 2 microm carrier-wavelength output is self-compressed below 3 optical cycles and has a 270 microJ pulse energy. The self-locked phase offset of the 2 microm difference-frequency field is preserved after filamentation. This is to our knowledge the first experimental realization of pulse compression in optical filaments at mid-IR wavelengths (lambda>0.8 microm).

Frequency-sheared, time-delayed extreme-ultraviolet pulses produced by high-harmonic generation in argon.

We report the production of frequency-sheared high harmonics in argon by control of the envelope and chirp of the electric field of the femtosecond driving laser pulse. Using the classic three-step model of high-harmonic generation, we established a direct link between the properties of the harmonics and the fully characterized driving pulses. A simulation of the single-atom response in the strong-field approximation confirms the simple picture and shows good agreement with the experimental results.