Hyper spectral resolution stimulated Raman spectroscopy with amplified fs pulse bursts.

We present a novel approach for Stimulated Raman Scattering (SRS) spectroscopy in which a hyper spectral resolution and high-speed spectral acquisition are achieved by employing amplified offset-phase controlled fs-pulse bursts. We investigate the method by solving the coupled non-linear Schrödinger equations and validate it by numerically characterizing SRS in molecular nitrogen as a model compound. The spectral resolution of the method is found to be determined by the inverse product of the number of pulses in the burst and the intraburst pulse separation. The SRS spectrum is obtained through a motion-free scanning of the offset phase that results in a sweep of the Raman-shift frequency. Due to high spectral resolution and fast motion-free scanning the technique is beneficial for a number SRS-based applications such as gas sensing and chemical analysis.

Analysis of high-contrast all-optical dual-wavelength switching in asymmetric dual-core fibers.

We systematically present experimental and theoretical results for the dual-wavelength switching of 1560 nm, 75 fs signal pulses (SPs) driven by 1030 nm, and 270 fs control pulses (CPs) in a dual-core fiber (DCF). We demonstrate a switching contrast of 31.9 dB, corresponding to a propagation distance of 14 mm, achieved by launching temporally synchronized SP-CP pairs into the fast core of the DCF with moderate inter-core asymmetry. Our analysis employs a system of three coupled propagation equations to identify the compensation of the asymmetry by nonlinearity as the physical mechanism behind the efficient switching performance.

Spectral peak recovery in parametrically amplified THz-repetition-rate bursts.

Multi-photon resonant spectroscopies require tunable narrowband excitation to deliver spectral selectivity and, simultaneously, high temporal intensity to drive a nonlinear-optical process. These contradictory requirements are achievable with bursts of ultrashort pulses, which provides both high intensity and tunable narrowband peaks in the frequency domain arising from spectral interference. However, femtosecond pulse bursts need special attention during their amplification [Optica7, 1758 (2020)10.1364/OPTICA.403184], which requires spectral peak suppression to increase the energy safely extractable from a chirped-pulse amplifier (CPA). Here, we present a method combining safe laser CPA, relying on spectral scrambling, with a parametric frequency converter that automatically restores the desired spectral peak structure and delivers narrow linewidths for bursts of ultrashort pulses at microjoule energies. The shown results pave the way to new high-energy ultrafast laser sources with controllable spectral selectivity.

HHG at the Carbon K-Edge Directly Driven by SRS Red-Shifted Pulses from an Ytterbium Amplifier.

In this work, we introduce a simplified approach to efficiently extend the high harmonic generation (HHG) cutoff in gases without the need for laser frequency conversion via parametric processes. Instead, we employ postcompression and red-shifting of a Yb:CaF2 laser via stimulated Raman scattering (SRS) in a nitrogen-filled stretched hollow core fiber. This driving scheme circumvents the low-efficiency window of parametric amplifiers in the 1100-1300 nm range. We demonstrate this approach being suitable for upscaling the power of a driver with an optimal wavelength for HHG in the highly desirable XUV range between 200 and 300 eV, up to the carbon K-edge. Due to the combination of power scalability of a low quantum defect ytterbium-based laser system with the high conversion efficiency of the SRS technique, we expect a significant increase in the generated photon flux in comparison with established platforms for HHG in the water window. We also compare HHG driven by the SRS scheme with the conventional self-phase modulation (SPM) scheme.

Ionization rate and plasma dynamics at 3.9 micron femtosecond photoionization of air.

The introduction of mid-IR optical parametric chirped pulse amplifiers has catalyzed interest in multimillijoule, infrared femtosecond pulse-based filamentation. As tunneling ionization is a fundamental first stage in these high-intensity laser-matter interactions, characterizing the process is critical to understand derivative topical studies on femtosecond filamentation and self-focusing. Here, we report direct nonintrusive measurements of total electron count and electron number densities generated at 3.9 µm femtosecond midinfrared tunneling ionization of atmospheric air using constructive-elastic microwave scattering. Subsequently, we determine photoionization rates to be in the range 5.0×10^{8}-6.1×10^{9}s^{-1} for radiation intensities of 1.3×10^{13}-1.9×10^{14}W/cm^{2}, respectively. The proposed approach paves the wave to precisely tabulate photoionization rates in mid-IR for a broad range of intensities and gas types and to study plasma dynamics at mid-IR filamentation.

Complex study of solitonic ultrafast self-switching in slightly asymmetric dual-core fibers.

We present a complex study of pulse-energy-controlled solitonic self-switching of femtosecond pulses at wavelengths of 1700 and 1560 nm in two nonlinear high-index contrast dual-core fibers having different levels of slight asymmetry. In the case of the fiber with higher dual-core asymmetry excited by 1700 nm pulses, the highest switching contrast of 20.8 dB at 40 mm fiber length was demonstrated. It was accompanied by multiple exchanges of the dominant core at the fiber output, which is a strong signature of the soliton-based switching process. In the case of the fiber with lower dual-core asymmetry, excited by 1560 nm pulses, the highest switching contrast of 21.4 dB at 35 mm fiber length was achieved with a broadband character of the switching in the spectral range of 1450-1650 nm. Both demonstrations represent progress in all-optical switching studies at these particular wavelengths thanks to a comparison between their results, which reveals the requirement of a higher level of dual-core symmetry for applicable C-band operation.

Polarization Dependent Excitation and High Harmonic Generation from Intense Mid-IR Laser Pulses in ZnO.

The generation of high order harmonics from femtosecond mid-IR laser pulses in ZnO has shown great potential to reveal new insight into the ultrafast electron dynamics on a few femtosecond timescale. In this work we report on the experimental investigation of photoluminescence and high-order harmonic generation (HHG) in a ZnO single crystal and polycrystalline thin film irradiated with intense femtosecond mid-IR laser pulses. The ellipticity dependence of the HHG process is experimentally studied up to the 17th harmonic order for various driving laser wavelengths in the spectral range 3-4 µm. Interband Zener tunneling is found to exhibit a significant excitation efficiency drop for circularly polarized strong-field pump pulses. For higher harmonics with energies larger than the bandgap, the measured ellipticity dependence can be quantitatively described by numerical simulations based on the density matrix equations. The ellipticity dependence of the below and above ZnO band gap harmonics as a function of the laser wavelength provides an efficient method for distinguishing the dominant HHG mechanism for different harmonic orders.

Observation of extremely efficient terahertz generation from mid-infrared two-color laser filaments.

Extreme nonlinear interactions of THz electromagnetic fields with matter are the next frontier in nonlinear optics. However, reaching this frontier in free space is limited by the existing lack of appropriate powerful THz sources. Here, we experimentally demonstrate that two-color filamentation of femtosecond mid-infrared laser pulses at 3.9 µm allows one to generate ultrashort sub-cycle THz pulses with sub-milijoule energy and THz conversion efficiency of 2.36%, resulting in THz field amplitudes above 100 MV cm-1. Our numerical simulations predict that the observed THz yield can be significantly upscaled by further optimizing the experimental setup. Finally, in order to demonstrate the strength of our THz source, we show that the generated THz pulses are powerful enough to induce nonlinear cross-phase modulation in electro-optic crystals. Our work paves the way toward free space extreme nonlinear THz optics using affordable table-top laser systems.

Strong Light-Field Driven Nanolasers.

Einstein established the quantum theory of radiation and paved the way for modern laser physics including single-photon absorption by charge carriers and finally pumping an active gain medium into population inversion. This can be easily understood in the particle picture of light. Using intense, ultrashort pulse lasers, multiphoton pumping of an active medium has been realized. In this nonlinear interaction regime, excitation and population inversion depend not only on the photon energy but also on the intensity of the incident pumping light, which can be still described solely by the particle picture of light. We demonstrate here that lowering significantly the pump photon energy further still enables population inversion and lasing in semiconductor nanowires. The extremely high electric field of the pump bends the bands and enables tunneling of electrons from the valence to the conduction band. In this regime, the light acts by the classical Coulomb force and population inversion is entirely due to the wave nature of electrons, thus the excitation becomes independent of the frequency but solely depends on the incident intensity of the pumping light.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua.

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV. Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K- and L-absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 10^{9} photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 10^{26} photons/s/mrad^{2}/mm^{2}/1% bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

High-energy pulse stacking via regenerative pulse-burst amplification.

Here we present a coherent pulse stacking approach for upscaling the energy of a solid-state femtosecond chirped pulse amplifier. We demonstrate pulse splitting into four replicas, amplification in a burst-mode regenerative Yb:CaF2 amplifier, designed to overcome intracavity optical damage by colliding pulse replicas, and coherent combining into a single millijoule level pulse. The thresholds of pulse-burst-induced damage of optical elements are experimentally investigated. The scheme allows achieving an enhancement factor of 2.62 using a single-stage stacker cavity and, potentially, much higher enhancement factors using cascaded stacking.

Parametric amplification of 100 fs mid-infrared pulses in ZnGeP2 driven by a Ho:YAG chirped-pulse amplifier.

We report on the parametric generation of 100 fs sub-6-cycle 40 µJ pulses with the center wavelength at 5.2 µm using a 1 ps 2.1 µm pump laser and a dispersion management scheme based on bulk material. Our optically synchronized amplifier chain consists of a Ho:YAG chirped-pulse amplifier and white-light-seeded optical parametric amplifiers providing simultaneous passive carrier-envelope phase locking of three ultrashort longwave pulses at the pump, signal, and idler wavelengths corresponding, respectively, to 2.1, 3.5, and 5.2 µm. We also demonstrate bandwidth enhancement and efficient control over nonlinear spectral phase in the regime of cascaded χ2 nonlinearity in ZnGeP2.

Combined Yb/Nd driver for optical parametric chirped pulse amplifiers.

We report on the developed front-end/pump system for optical parametric chirped pulse amplifiers. The system is based on a dual output fiber oscillator/power amplifier which seeds and assures all-optical synchronization of femtosecond Yb and picosecond Nd laser amplifiers operating at a central wavelength of 1030 nm and 1064 nm, respectively. At the central wavelength of 1030 nm, the fiber oscillator generates partially stretched 4 ps pulses with the spectrum supporting a <120 fs pulse duration and pulse energy of 0.45 nJ. The energy of generated 1064 nm pulses is 0.15 nJ, which is sufficient for the efficient seeding of high-contrast Nd:YVO chirped pulse regenerative amplifier/post amplifier systems generating 9 mJ pulses compressible to 16 ps duration. The power amplification stages, based on Nd:YAG crystals, provide 62 mJ pulses compressible to 20 ps pulse duration at a repetition rate of 1 kHz. Further energy scaling currently is prevented by limited dimensions of the diffraction gratings, which, because of the fast progress in MLD grating manufacturing technologies is only a temporary obstacle.

Broadband mid-infrared pulses from potassium titanyl arsenate/zinc germanium phosphate optical parametric amplifier pumped by Tm, Ho-fiber-seeded Ho:YAG chirped-pulse amplifier.

We present a concept of a white-light-seeded-cascaded mid-infrared (mid-IR) optical parametric amplifier (OPA) based on potassium titanyl arsenate and zinc germanium phosphate nonlinear optical crystals and producing 100-µJ level pulses centered at 5300 nm, with the spectrum supporting four-optical-cycle pulse duration. The OPA is pumped by 2090-nm master oscillator/power amplifier based on a Tm,Ho-fiber laser seeder and a Ho:YAG regenerative amplifier delivering 3.8-mJ sub-ps pulses at a repetition rate of 1 kHz. We validate that output parameters of the OPA are scalable by means of increasing the pulse energy, decreasing the pulse duration and redshifting the central wavelength.

Bright coherent ultrahigh harmonics in the keV x-ray regime from mid-infrared femtosecond lasers.

High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.

White light generation over three octaves by femtosecond filament at 3.9 µm in argon.

We report the first (to our knowledge) experimental results and numerical simulations on mid-IR femtosecond pulse filamentation in argon using 0.1 TW peak-power, 80 fs, 3.9 µm pulses. A broadband supercontinuum spanning the spectral range from 350 nm to 5 µm is generated, whereby about 4% of the mid-IR pulse energy is converted into the 350-1700 nm spectral region. These mid-IR-visible coherent continua offer a new, unique tool for time-resolved spectroscopy based on a mid-IR filamentation laser source.

90 GW peak power few-cycle mid-infrared pulses from an optical parametric amplifier.

We demonstrate a compact 20 Hz repetition-rate mid-IR OPCPA system operating at a central wavelength of 3900 nm with the tail-to-tail spectrum extending over 600 nm and delivering 8 mJ pulses that are compressed to 83 fs (<7 optical cycles). Because of the long optical period (∼13 fs) and a high peak power, the system opens a range of unprecedented opportunities for tabletop ultrafast science and is particularly attractive as a driver for a highly efficient generation of ultrafast coherent x-ray continua for biomolecular and element specific imaging.

Carrier envelope phase stabilization of a Yb:KGW laser amplifier.

In this paper we report on the active stabilization of the carrier envelope phase (CEP) of a Yb:KGW chirped pulse amplifier laser system seeded by a Yb-doped solid-state Kerr-lens mode-locked oscillator. The regenerative amplifier delivers 180 fs CEP stable pulses of 30 µJ-1 mJ energy at a repetition rate tunable from 1 to 200 kHz. The bandwidth of the feedback loop was extended by a factor of 5 using a specially designed high-pass filter, which resulted in a dramatic decrease of CEP jitter below 0.45 rad after the amplifier.

Optically induced cis-trans isomerisation of (eta6-cis-stilbene)Cr(CO)3.

The femto- and picosecond time resolved spectroscopy of (eta(6)-cis-stilbene)Cr(CO)(3) provides evidence for three optically accessible excited states one leading to cis-trans isomerisation of the coordinated stilbene ligand and another which results in a slow release of CO.

Self-compression of millijoule 1.5 microm pulses.

We demonstrate a four-stage optical parametric chirped-pulse amplification system that delivers carrier-envelope phase-stable approximately 1.5 microm pulses with energies up to 12.5 mJ before recompression. The system is based on a fusion of femtosecond diode-pumped solid-state Yb technology and a picosecond 100 mJ Nd:YAG pump laser. Pulses with 62 nm bandwidth are recompressed to a 74.4 fs duration close to the transform limit. To show the way toward a terawatt-peak-power single-cycle IR source, we demonstrate self-compression of 2.2 mJ pulses down to 19.8 fs duration in a single filament in argon with a 1.5 mJ output energy and 66% energy throughput.