4D spatio-temporal electric field characterization of ultrashort light pulses undergoing filamentation.

We present an experimental method capable of capturing the complete spatio-temporal dynamics of filamenting ultrashort laser pulses. By employing spatially resolved Fourier transform spectrometry in combination with the capability to terminate the filament at any length, we can follow the nonlinear dynamics in four dimensions, i.e. the transverse domain, time and filament length. Our method thus not only enables the full characterization of the filamentation process throughout its evolution, but also allows to identify and select laser pulses with desired parameters.

Potential hazards and mitigation of X-ray radiation generated by laser-induced plasma from research-grade laser systems.

A large range of laser-matter applications employ ultrashort pulses and high laser intensity. Such processes can lead to unrequired X-ray generation, which represents a hazardous radiation factor even for common laboratory research-grade laser systems. We present here an analysis of the radiation dose rate and X-ray spectrum emitted during ablation of a rotating copper cylinder with respect to several laser parameters. The results show that focused sub-picosecond pulses with intensity above 1013 W/cm2 can exceed the annual irradiation limit even in one hour, requiring appropriate shielding for the safety of the researchers.

Self-probed ptychography from semiconductor high-harmonic generation.

We demonstrate a method to image an object using a self-probing approach based on semiconductor high-harmonic generation. On the one hand, ptychography enables high-resolution imaging from the coherent light diffracted by an object. On the other hand, high-harmonic generation from crystals is emerging as a new source of extreme-ultraviolet ultrafast coherent light. We combine these two techniques by performing ptychography measurements with nanopatterned crystals serving as the object as well as the generation medium of the harmonics. We demonstrate that this strong field in situ approach can provide structural information about an object. With the future developments of crystal high harmonics as a compact short-wavelength light source, our demonstration can be an innovative approach for nanoscale imaging of photonic and electronic devices in research and industry.

Generating Ultrabroadband Deep-UV Radiation and Sub-10 nm Gap by Hybrid-Morphology Gold Antennas.

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

Few-cycle optical pulse characterization via cross-polarized wave generation dispersion scan technique.

We demonstrate a dispersion scan (d-scan) pulse characterization scheme employing cross-polarized wave (XPW) generation as a nonlinear optical process. XPW generation is a degenerate four-wave mixing process with no phase-matching limitations. Therefore, its implementation in the d-scan method is a good choice for the characterization of few-cycle pulses in remote spectral regions. We fully characterize 5-10 fs pulses delivered through a hollow-core fiber in the near-IR region and compare the results with the second-harmonic generation (SHG) frequency-resolved optical gating and SHG d-scan characterization methods.

Direct observation of pulse dynamics and self-compression along a femtosecond filament.

We report on the direct experimental observation of pulse-splitting dynamics along a femtosecond filament. The fundamental pulse experiences a significant self-shortening during the propagation leading to pulse durations of 5.3 fs, corresponding to sub-3 cycles, which is measured without external pulse compression. A compression factor of eight could be achieved in a single filamentary stage. Theoretical modeling of the fundamental pulse propagation confirms our observed pulse structures and durations and gives further insight into the nonlinear dynamics during filamentation.

Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy.

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+ state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

Sub-1.5-cycle pulses from a single filament.

The temporal dynamics of ultrashort laser pulses undergoing filamentary propagation are investigated with a real-time stereographic above-threshold ionization (ATI) phasemeter. The experimental setup is capable of measuring the pulse duration as well as the carrier-envelope phase distribution of pulses originating from a femtosecond filament, which is either truncated in length or fully propagated. Truncation, by means of a semi-infinite gas cell, allows to elucidate the nonlinear evolution and temporal dynamics of ultrashort laser pulses as a function of the propagation length. We observe the formation of few-cycle pulses as well as temporal pulse splitting dynamics during the propagation of the pulse inside the filament. For the first time, we demonstrate the compression of 35 fs pulses down to a duration of sub-4 fs in a single femtosecond filament. This corresponds to sub-1.5 cycles of the electric field.

Tracking spectral shapes and temporal dynamics along a femtosecond filament.

The spectral evolution of a high-intensity light channel formed by filamentation is investigated in a detailed experimental study. We also track the spatio-temporal dynamics by high-order harmonic generation along the filament. Both the spectral and temporal diagnostics are performed as a function of propagation distance, by extracting the light pulses directly from the hot filament core into vacuum via pinholes that terminate the nonlinear propagation. We compare the measured spectral shapes to simulations and analyze numerically the temporal dynamics inside the filament.

Gradient enhanced third harmonic generation in a femtosecond filament.

The third harmonic generated during femtosecond filamentation in air is studied. By establishing a gradient from atmospheric pressure to vacuum conditions, we truncate the filament abruptly at defined positions. The introduction of the pressure gradient leads to an enhancement of the generated third harmonic radiation by 3 orders of magnitude. This effect is attributed to an improved on-axis phase-matching condition. We investigate the spectral shape and the conversion efficiency of the third harmonic during the propagation in the filament.

X-ray Dose Rate and Spectral Measurements during Ultrafast Laser Machining Using a Calibrated (High-Sensitivity) Novel X-ray Detector.

Ultrashort pulse laser machining is subject to increase the processing speeds by scaling average power and pulse repetition rate, accompanied with higher dose rates of X-ray emission generated during laser-matter interaction. In particular, the X-ray energy range below 10 keV is rarely studied in a quantitative approach. We present measurements with a novel calibrated X-ray detector in the detection range of 2-20 keV and show the dependence of X-ray radiation dose rates and the spectral emissions for different laser parameters from frequently used metals, alloys, and ceramics for ultrafast laser machining. Our investigations include the dose rate dependence on various laser parameters available in ultrafast laser laboratories as well as on industrial laser systems. The measured X-ray dose rates for high repetition rate lasers with different materials definitely exceed the legal limitations in the absence of radiation shielding.

Author Correction: All semiconductor enhanced high-harmonic generation from a single nanostructured cone.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

A synchronized VUV light source based on high-order harmonic generation at FLASH.

Ultrafast measurements in the extreme ultraviolet (XUV) spectral region targeting femtosecond timescales rely until today on two complementary XUV laser sources: free electron lasers (FELs) and high-harmonic generation (HHG) based sources. The combination of these two source types was until recently not realized. The complementary properties of both sources including broad bandwidth, high pulse energy, narrowband tunability and femtosecond timing, open new opportunities for two-color pump-probe studies. Here we show first results from the commissioning of a high-harmonic beamline that is fully synchronized with the free-electron laser FLASH, installed at beamline FL26 with permanent end-station including a reaction microscope (REMI). An optical parametric amplifier synchronized with the FEL burst mode drives the HHG process. First commissioning tests including electron momentum measurements using REMI, demonstrate long-term stability of the HHG source over more than 14 hours. This realization of the combination of these light sources will open new opportunities for time-resolved studies targeting different science cases including core-level ionization dynamics or the electron dynamics during the transformation of a molecule within a chemical reaction probed on femtosecond timescales in the ultraviolet to soft X-ray spectral region.

Generation of high-order harmonics with ultra-short pulses from filamentation.

7-fs-pulses with 0.3 mJ are obtained after filamentation in argon and compression by double-chirped-mirrors. These pulses are used to generate high-order harmonics in a semi-infinite gas cell in different noble gases. Spectral broadening of high-order harmonics in xenon and argon is observed. In neon, an extended continuous cut-off region down to 10 nm (124 eV) is observed which is to the best of our knowledge the highest cut-off energy obtained by filamented pulses. Our result suggests the feasibility of single attosecond-pulse-generation at both high photon flux and high cut-off energy.

All semiconductor enhanced high-harmonic generation from a single nanostructured cone.

The enhancement and control of non-linear phenomena at a nanometer scale has a wide range of applications in science and in industry. Among these phenomena, high-harmonic generation in solids is a recent focus of research to realize next generation petahertz optoelectronic devices or compact all solid state EUV sources. Here, we report on the realization of the first nanoscale high harmonic source. The strong field regime is reached by confining the electric field from a few nanojoules femtosecond laser in a single 3D semiconductor waveguide. We reveal a strong competition between enhancement of coherent harmonics and incoherent fluorescence favored by excitonic processes. However, far from the band edge, clear enhancement of the harmonic emission is reported with a robust sustainability offering a compact nanosource for applications. We illustrate the potential of our harmonic nano-device by performing a coherent diffractive imaging experiment. Ultra-compact UV/X-ray nanoprobes are foreseen to have other applications such as petahertz electronics, nano-tomography or nano-medicine.

Nano-plasmonic near field phase matching of attosecond pulses.

Nano-structures excited by light can enhance locally the electric field when tuned to plasmonic resonances. This phenomenon can be used to boost non-linear processes such as harmonic generation in crystals or in gases, Raman excitation, and four wave mixing. Here we present a theoretical investigation of the near-field phase matching of attosecond pulses emitted by high-order harmonic generation (HHG) of an atom immersed in a multi-cycle femtosecond infrared laser field and a spatially inhomogeneous plasmonic field. We demonstrate that the spatial inhomogeneity factor of the plasmonic field strongly affects the electron trajectory and recombination time which can be used to control the attosecond emission. For further insight into the plasmonic field effect, we monitor the phase of each quantum path as a function of the inhomogeneity strength. Moreover, we investigate the attosecond emission as a function of near-field phase matching effects. This is achieved by calculating the coherent field superposition of attosecond pulses emitted from various intensities or field inhomogeneities. Finally, far-field and near-field phase matching effects are combined to modulate the harmonic spectral phase towards the emission of a single attosecond pulse.

Microjoule pulse energy from a chirped-pulse Ti:sapphire oscillator with cavity dumping.

We demonstrate a chirped-pulse Ti:sapphire laser oscillator with both Kerr-lens and semiconductor- saturable-absorber-mirror-assisted mode locking generating 1.1 microJ pulses at 1 MHz pulse repetition rate. The pulses are coupled out of the laser cavity by means of an acousto-optical cavity dumper, have a spectral width that supports a Fourier limit of 74 fs, and currently have a chirped-pulse duration of 5 ps. After compressing the pulses, this laser will be an ideal tool for efficient high-harmonic generation directly from a laser oscillator.