Compression of UV femtosecond laser pulses focused into a gas cell filled with xenon is reported numerically. With a large negative Kerr index and normal dispersion, xenon promotes temporal modulational instability (MI) which can be monitored to shorten ~ 100 fs pulses to robust, singly-peaked waveforms exhibiting a fourfold compression factor. Combining standard MI theory with a variational approach allows us to predict the beam parameters suitable for efficient compression. At powers < 30 MW, nonlinear dispersion is shown to shift the pulse temporal profile to the rear zone.
Direct generation of ultrashort, transform-limited pulses in a laser resonator is observed theoretically and experimentally. This constitutes a new type of ultrashort pulse generation in mode-locked lasers: in contrast to the well-known solitons (hyperbolic secant like), dispersion-managed solitons (Gaussian-like), and parabolic pulses plus external compression, ultrashort pulse solutions to the nonlinear wave equations that describe pulse evolution in the laser cavity are observed. Stable ultrashort, transform-limited pulses exist with optical spectrum broader than the gain bandwidth of the a…
We present a simple and robust technique to retrieve the phase of ultrashort laser pulses, based on a chirped mirror and glass wedges compressor. It uses the compression system itself as a diagnostic tool, thereby making unnecessary the use of complementary diagnostic tools. We used this technique to compress and characterize 7.1 fs laser pulses from an ultrafast laser oscillator.
We report generation of ultrashort UV pulses by soliton self-compression in kagomé-style hollow-core photonic crystal fiber filled with ambient air. Pump pulses with energy 2.6 uJ and duration 54 fs at 400 nm were compressed temporally by a factor of 5, to a duration of ~11 fs. The experimental results are supported by numerical simulations, showing that both Raman and Kerr effects play a role in the compression dynamics. The convenience of using ambient air, and the absence of glass windows that would distort the compressed pulses, makes the setup highly attractive as the basis of an efficien…
Light scattering in inhomogeneous media induces wavefront distortions which pose an inherent limitation in many optical applications. Examples range from microscopy and nanosurgery to astronomy. In recent years, ongoing efforts have made the correction of spatial distortions possible by wavefront shaping techniques. However, when ultrashort pulses are employed scattering induces temporal distortions which hinder their use in nonlinear processes such as in multiphoton microscopy and quantum control experiments. Here we show that correction of both spatial and temporal distortions can be attaine…
We investigate numerically soliton-plasma interaction in a noble-gas-filled silica hollow-core anti-resonant fiber pumped in the mid-IR at 3.0 μm. We observe multiple soliton self-compression stages due to distinct stages where either the self-focusing or the self-defocusing nonlinearity dominates. Specifically, the parameters may be tuned so the competing plasma self-defocusing nonlinearity only dominates over the Kerr self-focusing nonlinearity around the soliton self-compression stage, where the increasing peak intensity on the leading pulse edge initiates a competing self-defocusing plasma…
Delivering femtosecond laser light in the focal plane of a high numerical aperture microscope objective is still a challenge, despite significant developments in the generation of ultrashort pulses. One of the most popular techniques, used to correct phase distortions resulting from propagation through transparent media, is the multiphoton intrapulse interference phase scan (MIIPS). The accuracy of MIIPS however is limited when higher order phase distortions are present. Here we introduce an improvement, called Gated-MIIPS, which avoids shortcomings of MIIPS, reduces the influence of higher or…
We show that higher-order nonlinear indices ($n_4$, $n_6$, $n_8$, $n_{10}$) provide the main defocusing contribution to self-channeling of ultrashort laser pulses in air and Argon at 800 nm, in contrast with the previously accepted mechanism of filamentation where plasma was considered as the dominant defocusing process. Their consideration allows to reproduce experimentally observed intensities and plasma densities in self-guided filaments.
Modern laser sources nowadays deliver ultrashort light pulses reaching few cycles in duration, high energies beyond the Joule level and peak powers exceeding several terawatt (TW). When such pulses propagate through optically-transparent media, they first self-focus in space and grow in intensity, until they generate a tenuous plasma by photo-ionization. For free electron densities and beam intensities below their breakdown limits, these pulses evolve as self-guided objects, resulting from successive equilibria between the Kerr focusing process, the chromatic dispersion of the medium, and the …
We demonstrate generation of 7.6 fs near-UV pulses centered at 400 nm via 8-fold soliton-effect self-compression in an Ar-filled hollow-core kagomé-style photonic crystal fiber with ultrathin core walls. Analytical calculations of the effective compression length and soliton order permit adjustment of the experimental parameters, and numerical modelling of the nonlinear pulse dynamics in the fiber accurately predict the spectro-temporal profiles of the self-compressed pulses. After compensation of phase distortion introduced by the optical elements along the beam path from the fiber to the dia…
Ionization is a fundamental process in intense laser-matter interactions, and is known to cause plasma defocusing and intensity clamping. Here, we investigate theoretically the propagation dynamics of an intense laser pulse in a helium gas jet in the ionization saturation regime, and we find that the pulse undergoes self-focusing and self-compression through ionization-induced reshaping, resulting in a manyfold increase in the laser intensity. This unconventional behavior is associated with the spatiotemporal frequency variation mediated by ionization and spatiotempral coupling. Our results il…
We experimentally observe long-wavelength dispersive waves generation in a BBO crystal. A soliton was formed in normal GVD regime of the crystal by a self-defocusing and negative nonlinearity through phase-mismatched quatradic interaction. Strong temporal pulse compression confirmed the formation of soliton during the pulse propagation inside the crystal. Significant dispersive wave radiation was measured in the anomalous GVD regime of the BBO crystal. With the pump wavelengths from 1.24 to 1.4 $μ$m, tunable dispersive waves are generated around 1.9 to 2.2 $μ$m. The observed dispersive wave ge…
Using numerical simulations, we study propagation of ultrashort light pulses in an inhomogeneously broadened two-level medium. There are two main issues in our study. The first one concerns the transient process of self-induced transparency soliton formation, in particular, the compression of the pulse which seems to be more effective in the case of homogeneous broadening. The second question deals with the collisions of counter-propagating solitons. It is shown that the level of inhomogeneous broadening has a substantial effect on the elasticity of such collisions.
We show numerically that ultrashort self-defocusing temporal solitons colliding with a weak pulsed probe in the near-IR can convert the probe to the mid-IR. A near-perfect conversion efficiency is possible for a high effective soliton order. The near-IR self-defocusing soliton can form in a quadratic nonlinear crystal (beta-barium borate) in the normal dispersion regime due to cascaded (phase-mismatched) second-harmonic generation, and the mid-IR converted wave is formed in the anomalous dispersion regime between $λ=2.2-2.4~μ\rm m$ as a resonant dispersive wave. This process relies on non-dege…
Transparent materials do not absorb light but have profound influence on the phase evolution of transmitted radiation. One consequence is chromatic dispersion, i.e., light of different frequencies travels at different velocities, causing ultrashort laser pulses to elongate in time while propagating. Here we experimentally demonstrate ultrathin nanostructured coatings that resolve this challenge: we tailor the dispersion of silicon nanopillar arrays such that they temporally reshape pulses upon transmission using slow light effects and act as ultrashort laser pulse compressors. The coatings ind…
Supercontinuum (SC) generation based on ultrashort pulse compression constitutes one of the most promising technologies towards an ultra-wide bandwidth, high-brightness and spatially coherent light sources for applications such as spectroscopy and microscopy. Here, multi-octave SC generation in a gas-filled hollow-core antiresonant fiber (HC-ARF) is reported spanning from 200 nm in the deep ultraviolet (DUV) to 4000 nm in the mid-infrared (mid-IR). A measured average output power of 5 mW was obtained by pumping at the center wavelength of the first anti-resonance transmission window (2460 nm) …
We propose a novel method based on the so-called shortcut to adiabatic passage techniques to achieve fast compression of temporal solitons in a nonlinear waveguide. We demonstrate that soliton compression could be achieved, in principle, at an arbitrarily small distance by inverse engineering the pulse width and the nonlinearity of the medium. The proposed scheme could possibly be exploited for various short-distance communication protocols and may be even in nonlinear guided wave-optics devices and generation of ultrashort soliton pulses.
The possibility of soliton self-compression of ultrashort laser pulses down to the few-cycle regime in photonic crystal fibers is numerically investigated. We show that efficient sub-two-cycle temporal compression of nanojoule-level 800 nm pulses can be achieved by employing short (typically 5-mm-long) commercially available photonic crystal fibers and pulse durations of around 100 fs, regardless of initial linear chirp, and without the need of additional dispersion compensation techniques. We envisage applications in a new generation of compact and efficient sub-two cycle laser pulse sources.
We present complete experimental characterisation of the temporal shape of an intense ultrashort 200-TW laser pulse driving a laser wakefield. The phase of the pulse was uniquely measured using (second order) frequency resolved optical gating (FROG). The pulses are asymmetrically compressed, and exhibit a positive chirp consistent with the expected asymmetric self-phase modulation due to photon acceleration/deceleration in a relativistic plasma wave. The measured pulse duration decreases linearly with increasing length and density of the plasma, in quantitative agreement with the intensity dep…
The theoretical calculation for nonlinear refractive index in Cr: ZnSe - active medium predicts the strong defocusing cascaded second-order nonlinearity within 2000 - 3000 nm spectral range. On the basis of this result the optimal cavity configuration for Kerr-lens mode locking is proposed that allows to achieve a sub-100 fs pulse duration. The numerical simulations testify about strong destabilizing processes in the laser resulting from a strong self-phase modulation. The stabilization of the ultrashort pulse generation is possible due to spectral filtering that increases the pulse duration u…
We propose an efficient approach to improve few-cycle soliton compression with cascaded quadratic nonlinearities by using an engineered multi-section structure of the nonlinear crystal. By exploiting engineering of the cascaded quadratic nonlinearities, in each section soliton compression with a low effective order is realized, and high-quality few-cycle pulses with large compression factors are feasible. Each subsequent section is designed so that the compressed pulse exiting the previous section experiences an overall effective self-defocusing cubic nonlinearity corresponding to a modest sol…
In most applications of ultrashort pulse lasers, temporal compressors are used to achieve a desired pulse duration in a target or sample, and precise temporal characterization is important. The dispersion-scan (d-scan) pulse characterization technique usually involves using glass wedges to impart variable, well-defined amounts of dispersion to the pulses, while measuring the spectrum of a nonlinear signal produced by those pulses. This works very well for broadband few-cycle pulses, but longer, narrower bandwidth pulses are much more difficult to measure this way. Here we demonstrate the conce…
We identify a novel regime of soliton-plasma interactions in which high-intensity ultrashort pulses of intermediate soliton order undergo coherent plasma-induced fission. Experimental results obtained in gas-filled hollow-core photonic crystal fibers are supported by rigorous numerical simulations. The cumulative blueshift of higher-order input solitons with ionizing intensities results in pulse splitting before the ultimate self-compression point, leading to the generation of robust pulse pairs with PHz bandwidths. The novel dynamics closes the gap between plasma-induced adiabatic soliton com…
Soliton self-compression is demonstrated during the propagation of high spatial modes in hollow core fibers in the near-infrared spectral region, taking advantage of their negative dispersion response. We have found that there is always an optimum spatial mode to observe this phenomenon, compressing the pulses down to the single-cycle regime without needing any external compression device and with a consequent increase in the output peak power. Our result is relevant for any ultrashort laser application in which few- or single-cycle pulses are crucial.
Controlling the wave function of free electrons is important to improve the spatial resolution of electron microscopes, the efficiency of electron interaction with sample modes of interest, and our ability to probe ultrafast materials dynamics at the nanoscale. In this context, attosecond electron compression has been recently demonstrated through interaction with the near fields created by scattering of ultrashort laser pulses at nanostructures followed by free electron propagation. Here, we show that control over electron pulse shaping, compression, and statistics can be improved by replacin…
We investigate soliton self-compression and ultraviolet resonant dispersive wave emission in the higher-order modes of a gas-filled hollow capillary fibre. Our simple analytical scaling rules predict shorter required waveguides and different energy scales when moving from the fundamental to higher-order modes. Experimentally, we demonstrate soliton self-compression and ultraviolet dispersive wave emission in the double-lobe LP$_{11}$ mode of an argon-filled hollow capillary fibre, which we excite by coupling into the fibre at oblique incidence. We observe the generation of ultraviolet dispersi…
We propose an all-optical, three-dimensional electron pulse compression scheme in which Hermite-Gaussian optical modes are used to fashion a three-dimensional optical trap in the electron pulse's rest frame. We show that the correct choices of optical incidence angles are necessary for optimal compression. We obtain analytical expressions for the net impulse imparted by Hermite-Gaussian free-space modes of arbitrary order. Although we focus on electrons, our theory applies to any charged particle and any particle with non-zero polarizability in the Rayleigh regime. We verify our theory numeric…
Few-cycle lasers are essential for many research areas such as attosecond physics that promises to address fundamental questions in science and technology. Therefore, further advancements are connected to significant progress in the underlying laser technology. Here, two-stage nonlinear compression of a 660 W femtosecond fiber laser system is utilized to achieve unprecedented average power levels of energetic ultrashort or even few-cycle laser pulses. In a first compression step 408 W, 320 uJ, 30fs pulses are achieved, which can be further compressed to 216 W, 170 uJ, 6.3 fs pulses in a second…
The quantum cascade laser (QCL) has evolved to be a compact, powerful source of coherent mid-infrared (mid-IR) light. However, its fast gain dynamics strongly restricts the formation of ultrashort pulses. As such, the shortest pulses reported so far were limited to a few picoseconds with some hundreds of milliwatts of peak power, strongly narrowing their applicability for time-resolved and nonlinear experiments. Here, we demonstrate an alternative approach capable of producing near-transform-limited sub-picosecond pulses with several watts of peak power. Starting from a frequency modulated pha…
Bright and broadband coherent mid-IR radiation is important for exciting and probing molecular vibrations. Using cascaded nonlinearities in conventional quadratic nonlinear crystal like lithium niobate, self-defocusing near-IR solitons have been demonstrated that led to very broadband supercontinuum generation in the visible, near-IR and short-wavelength mid-IR. Here we conduct an experiment where a mid-IR crystal pumped in the mid-IR gives multiple-octave spanning supercontinua. The crystal is cut for noncritical interaction, so the three-wave mixing of a single mid-IR femtosecond pump source…
Broadband mid-infrared (MIR) molecular spectroscopy demands a bright and broadband light source in the molecular fingerprint region. To this end, intra-pulse difference frequency generation (IDFG) has shown excellent properties among various techniques. However, previous IDFG systems have mainly used unconventional long-wavelength 2-$μ$m ultrashort pulsed lasers. A few systems have been demonstrated with 1-$μ$m lasers, but they use bulky 100-W-class high-power Yb thin-disk lasers. In this work, we demonstrate a simple and robust approach of 1-$μ$m-pumped broadband IDFG with a conventional mode…
We theoretically and experimentally investigate the design of a high-repetition rate source delivering well-separated picosecond pulses thanks to the nonlinear compression of a dual-frequency beat signal within a cavity-less normally dispersive fiber-based setup. This system is well described by a set of two coupled NLS equations for which the usual normally dispersive defocusing regime is turned in a focusing temporal lens through a degenerated cross-phase modulation effect. More precisely, the temporal compression of the initial beating is performed by the combined effects of normal GVD and …
We explore parabolic pre-shaping as a means of generating and amplifying ultrashort pulses. We develop a theoretical framework for modeling the technique and use its conclusions to design a femtosecond fiber amplifier. Starting from 9 ps pulses, we obtain 4.3 $μ$J, nearly transform-limited pulses 275 fs in duration, simultaneously achieving over 40 dB gain and 33-fold compression. Finally, we show that this amplification scheme is limited by Raman scattering, and outline a method by which the pulse duration and energy may be further improved and tailored for a given application.
We present the results of an experimental and numerical investigation into temporally non-local coherent interactions between ultrashort pulses, mediated by Raman coherence, in gas-filled kagomé-style hollow-core photonic crystal fiber. A pump pulse first set up the Raman coherence, creating a refractive index grating in the gas that travels at the group velocity of the pump pulse. Varying the arrival time of a second probe pulse allows high degree of control over its evolution as it propagates along the fiber, in particular soliton self-compression and dispersive wave (DW) emission. In the ex…
Propagation of ultrashort optical pulses in a dense resonant medium is considered in the semiclassical limit. In our analysis, we place emphasis on several main points. First, we study transformations of spectra in the process of pulse propagation and interactions with another pulse. The second point involves the transient processes (including pulse compression) connected with self-induced transparency soliton formation inside the medium. Finally, the third aspect is the study of collisions of co- and counter-propagating pulses in the medium. In the last case, the investigation of symmetric an…
The Free-Electron Laser (FEL) FLASH offers the worldwide still unique capability to study ultrafast processes with high-flux, high-repetition rate XUV and soft X-ray pulses. The vast majority of experiments at FLASH are of pump-probe type. Many of them rely on optical ultrafast lasers. Here, a novel FEL facility laser is reported which combines high average power output from Yb:YAG amplifiers with spectral broadening in a Herriott-type multi-pass cell and subsequent pulse compression to sub-100 fs durations. Compared to other facility lasers employing optical parametric amplification, the new …
Ultrashort high-energy pulses at wavelengths longer than 1 $μ$m are nowadays desired for a vast variety of applications in ultrafast and strong-field physics. To date, the main answer to the wavelength tunability for energetic, broadband pulses still relies on optical parametric amplification (OPA), which often requires multiple and complex stages, may feature imperfect beam quality and has limited conversion efficiency into one of the amplified waves. In this work, we present a completely different strategy to realize an energy-efficient and scalable laser frequency shifter. This relies on th…
The propagation of ultrashort pulses in optical fibre displays complex nonlinear dynamics that find important applications in fields such as high power pulse compression and broadband supercontinuum generation. Such nonlinear evolution however, depends sensitively on both the input pulse and fibre characteristics, and optimizing propagation for application purposes requires extensive numerical simulations based on generalizations of a nonlinear Schrödinger-type equation. This is computationally-demanding and creates a severe bottleneck in using numerical techniques to design and optimize exper…
Generation of high-repetition-rate, femtosecond, soliton pulse trains through dual-wavelength pumping of a dispersion-decreasing fiber is studied numerically. The achievable shortest pulse width is found to be limited by third-order dispersion that has a significant effect on the pulse-compression dynamics. The output wavelength is red shifted because of intrapulse Raman scattering and depends heavily on third-order dispersion, whose positive values lead to the most red shifted solitons (>25% of the input pump center wavelength). The proposed scheme allows the generation of ultrashort pulse tr…
Broadband laser sources based on supercontinuum generation by femtosecond laser filamentation have enabled applications from stand-off sensing and spectroscopy to the generation and self-compression of high-energy few-cycle pulses. Filamentation relies on the dynamic balance between self-focusing and plasma defocusing, mediated by the Kerr nonlinearity and multiphoton ionization respectively. The filament properties, including the supercontinuum generation, are therefore highly sensitive to the properties of both the laser source and the propagation medium. Here, we report the anomalous spectr…
Atomic motion dynamics during structural changes or chemical reactions have been visualized by picosecond and femtosecond pulsed electron beams via ultrafast electron diffraction and microscopy. Imaging the even faster dynamics of electrons in atoms, molecules and solids requires electron pulses with sub-femtosecond durations. We demonstrate here the all-optical generation of trains of attosecond free-electron pulses. The concept is based on the periodic energy modulation of a pulsed electron beam via an inelastic interaction with the ponderomotive potential of an optical travelling wave gener…
Streaking of photoelectrons with optical lasers has been widely used for temporal characterization of attosecond extreme ultraviolet pulses. Recently, this technique has been adapted to characterize femtosecond x-ray pulses in free-electron lasers with the streaking imprinted by farinfrared and Terahertz (THz) pulses. Here, we report successful implementation of THz streaking for time-stamping of an ultrashort relativistic electron beam of which the energy is several orders of magnitude higher than photoelectrons. Such ability is especially important for MeV ultrafast electron diffraction (UED…
Although ultraviolet (UV) light is important in many areas of science and technology, there are very few if any lasers capable of delivering wavelength-tunable ultrashort UV pulses at MHz repetition rates. Here we report the generation of deep-UV laser pulses at MHz repetition rates and μJ-energies by means of dispersive wave (DW) emission from self-compressed solitons in gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF). Pulses from an ytterbium fiber laser (~300 fs) are first compressed to ~25 fs in a SR-PCF-based nonlinear compression stage, and subsequently used to pump a …
In-line Dispersion Control of Femtosecond Laser Pulses by Multilayer Huygens' Metasurfaces
Friedrich-Schiller-University Jena（耶拿弗里德里希·席勒大学）；Australian National University（澳大利亚国立大学）；Fraunhofer Institute for Applied Optics and Precision Engineering IOF（弗劳恩霍夫应用光学和精密工程研究所）
Ultrashort electron pulses are crucial for time-resolved electron diffraction and microscopy of fundamental light-matter interaction. In this work, we study experimentally and theoretically the generation and characterization of attosecond electron pulses by optical-field-driven compression and streaking at dielectric or absorbing interaction elements. The achievable acceleration and deflection gradient depends on the laser-electron angle, the laser's electric and magnetic field directions and the foil orientation. Electric and magnetic fields have similar contributions to the final effect and…
We perform a beat-frequency-resolved analysis for two-dimensional electronic spectroscopy using a high-speed and stable 2D electronic spectrometer and few-cycle visible laser pulses to disentangle the vibrational coherences in an artificial fluorescent protein. We develop a highly stable ultrashort light source that generates 5.3-fs visible pulses with a pulse energy of 4.7 uJ at a repetition rate of 10 kHz using multi-plate pulse compression and laser filamentation in a gas cell. The above-5.3-fs laser pulses together with a high-speed multichannel detector enable us to measure a series of 2D…
Continuously Red-Shift and Blue-Shift Wavelength-Tuneable, Narrowband, High Harmonics in the EUV - X-ray Regime for Resonance Imaging and Spectroscopies
