Supercontinuum generation by femtosecond filaments in air is investigated for different laser wavelengths ranging from ultraviolet to infrared. Particular attention is paid on the role of third-harmonic generation and temporal steepening effects, which enlarge the blue part of the spectrum. A unidirectional pulse propagation model and nonlinear evolution equations are numerically integrated and their results are compared. Apart from the choice of the central wavelength, we emphasize the importance of the saturation intensity reached by self-guided pulses, together with their temporal duration and propagation length as key players acting on both supercontinuum generation of the pump wave and emergence of the third harmonics. Maximal broadening is observed for large wavelengths and long filamentation ranges.
We present a technique for the single-shot measurement of the space- and time-resolved spatiotemporal amplitude and phase of an ultrashort laser pulse. The method, transient-grating single-shot supercontinuum spectral interferometry (TG- SSSI), is demonstrated by the space-time imaging of short pulses carrying spatiotemporal optical vortices (STOVs). TG-SSSI is well-suited for characterizing ultrashort laser pulses that contain singularities associated with spin/orbital angular momentum or polarization.
We use a conceptually new approach to theoretical modeling of self-focusing in which we integrated diffractive and geometrical optics in order to explain and predict emission of white light and colored rings observed in ultrashort laser pulse interaction. In our approach laser beam propagation is described by blending solution of linear Maxwell's equation and a correction term that represents nonlinear field perturbation expressed in terms of paraxial ray-optics (eikonal) equation. No attempt is made to create appearance of exhaustive treatment via use of complex mathematical models. Rather, e…
Supercontinuum (SC) light source has advanced ultrafast laser spectroscopy in condensed matter science, biology, physics, and chemistry. Compared to the frequently used photonic crystal fibers and bulk materials, femtosecond laser filamentation in gases is damage-immune for supercontinuum generation. A bottleneck problem is the strong jitters from filament induced self-heating at kHz repetition rate level. We demonstrate stable kHz supercontinuum generation directly in air with multiple mJ level pulse energy. This is achieved by applying an external DC electric field to the air plasma filament…
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 report the amplification of an all-normal dispersion supercontinuum pulse in a Thulium / Holmium co-doped all-fiber chirped pulse amplification system. With a -20 dB bandwidth of more than 300 nm in the range 1800-2100 nm the system delivers high quality 66 fs pulses with more than 70 kW peak power directly from the output fiber. The coherent seeding of the entire emission bandwidth of the doped fiber and the stability of the supercontinuum generation dynamics in the silicate glass all-normal dispersion photonic crystal fiber result in excellent noise characteristics of the amplified ultras…
The ability to measure real-time fluctuations of ultrashort pulses propagating in optical fiber has provided significant insights into fundamental dynamical effects such as modulation instability and the formation of frequency-shifting rogue wave solitons. We report here a detailed study of real-time fluctuations across the full bandwidth of a fiber supercontinuum which directly reveals the significant variation in measured noise statistics across the spectrum, and which allows us to study correlations between widely separated spectral components. For two different propagation distances corres…
In supercontinuum generation, various propa- gation effects combine to produce a dramatic spec- tral broadening of intense ultrashort optical pulses with far reaching possibilities. Different applications place highly divergent and challenging demands on source characteristics such as spectral coverage from the ultraviolet (UV) across the visible (VIS) to the near-infrared (NIR), and into the mid-infrared (MIR). Shot-to-shot repeatability, high spectral energy density, an absence of complicated or non-deterministic pulse splitting are also essential for many applications. Here we present an "a…
A source of ultrashort pulses of light in the 2 μm region was constructed using supercontinuum broadening from an erbium mode-locked laser. The output spectrum spanned 1000 nm to 2200 nm with an average power of 250 mW. A pulse width of 39 fs for part of the spectrum in the 2000 nm region, corresponding to less than six optical cycles, was achieved. A heterodyne measurement of the free-running mode-locked laser with a narrow-linewidth continuous wave laser resulted in a near shot noise-limited beat note with a signal-to-noise ratio of 45 dB in a 10 kHz resolution bandwidth. The relative intens…
The nonlinear propagation of ultrashort pulses in optical fiber depends sensitively on both input pulse and fiber parameters. As a result, optimizing propagation for specific applications generally requires time-consuming simulations based on sequential integration of the generalized nonlinear Schrödinger equation (GNLSE). Here, we train a feed-forward neural network to learn the differential propagation dynamics of the GNLSE, allowing emulation of direct numerical integration of fiber propagation, and particularly the highly complex case of supercontinuum generation. Comparison with a recurre…
Ultrafast broadband ultraviolet radiation is of importance in spectroscopy and photochemistry, since high photon energies enable single-photon excitations and ultrashort pulses allow time-resolved studies. Here we report the use of gas-filled hollow-core photonic crystal fibers (HC-PCFs) for efficient ultrafast nonlinear optics in the ultraviolet. Soliton self-compression of 400 nm pulses of (unprecedentedly low) ~500 nJ energies down to sub-6-fs durations is achieved, as well as resonant emission of tunable dispersive waves from these solitons. In addition, we discuss the generation of a flat…
We measure the detailed spatiotemporal profiles of femtosecond laser pulses in the infrared wavelength range λ=2.5-11μm, and the absolute nonlinear response of major air constituents (N2, O2, and Ar) over this range. The spatiotemporal measurements reveal wavelength-dependent pulse front tilt and temporal stretching in the infrared pulses.
Although supercontinuum sources are readily available for the visible and near infrared, and recently also for the mid-IR, many areas of biology, chemistry and physics would benefit greatly from the availability of compact, stable and spectrally bright deep ultraviolet (DUV) and vacuum ultraviolet (VUV) supercontinuum sources. Such sources have however not yet been developed. Here we report the generation of a bright supercontinuum, spanning more than three octaves from 124 nm to beyond 1200 nm, in hydrogen-filled kagomé-style hollow-core photonic crystal fiber (kagomé-PCF). Few-μJ, 30 fs pump…
Université Bourgogne Europe, CNRS（勃艮第欧洲大学）；University of Calabria（卡拉布里亚大学）；University of Limoges, CNRS（利摩日大学）；Niccolò Cusano University（尼古拉·库萨诺大学）；Sapienza Universit‘a di Roma（罗马第一大学）
Supercontinuum generation in optical fibers is one of the most dramatic nonlinear effects discovered, allowing short pulses to be converted into multi-octave spanning coherent spectra. However, generating supercontinua that are both coherent and broadband requires pulses that are simultaneously ultrashort with high peak power. This results in a reducing efficiency with increasing pulse repetition rate, that has hindered supercontinua at microwave line spacing, i.e. 10s of GHz. Soliton microcombs by contrast, can generate octave-spanning spectra, but with good conversion efficiency only at vast…
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 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…
Polarization dynamics of femtosecond light pulses propagating in air is studied by computer simulation. A rich variety of dynamics is found that depends on the initial polarization state and power of the pulse. Effects of polarization on the plasma and supercontinuum generation are also discussed.
We report on designing, fabrication and experimental characterization of highly nonlinear, tellurite glass photonic crystal fibers with engineered normal dispersion characteristics for coherent supercontinuum generation. Effectively single mode, air-hole lattice fibers, with measured, all-normal dispersion profiles as flat as -10 to -50 ps/mn/km over 1500-2400 nm wavelengths are developed and investigated. Supercontinuum spectra are measured for these fibers, with a spectral width covering 1100-2600 nm wavelengths under pumping with a robust, fixed-wavelength erbium fiber-based femtosecond las…
We designed and developed tapered suspended-core fibers of high-purity As39Se61 glass for supercontinuum generation in the mid-IR with a standard fiber laser pump source at 2 $μ$m. It was shown that microstructuring allows shifting a zero dispersion wavelength to the range shorter than 2 $μ$m in the fiber waist with a core diameter of about 1 $μ$m. In this case, supercontinuum generation in the 1-10 $μ$m range was obtained numerically with 150-fs 100-pJ pump pulses at 2 $μ$m. We also performed experiments on wavelength conversion of ultrashort optical pulses at 1.57 $μ$m from Er: fiber laser s…
Ultrashort long-wave infrared (LWIR) laser pulses can resonantly excite vibrations in N2 and O2 through a two-photon transition. The absorptive, vibrational component of the ultrafast optical nonlinearity grows in time, starting smaller than, but quickly surpassing, the electronic, rotational, and vibrational refractive components. The growth of the vibrational component results in a novel mechanism of 3rd harmonic generation, providing an additional two-photon excitation channel, fundamental + 3rd harmonic. The original and emergent two-photon excitations drive the resonance exactly out of ph…
We experimentally demonstrate that the transmission of a 1030~nm, 1.3~ps laser beam of 100 mJ energy through fog increases when its repetition rate increases to the kHz range. Due to the efficient energy deposition by the laser filaments in the air, a shockwave ejects the fog droplets from a substantial volume of the beam, at a moderate energy cost. This process opens prospects for applications requiring the transmission of laser beams through fogs and clouds.
Recently, there has been growing interest in terahertz (THz) wave generation from liquids under optical excitation. Here, we propose and demonstrate the use of liquid lines in place of liquid films as THz emitters to boost THz signals. The geometry of the emitter eliminates the total internal reflection at the flat liquid-air interface. In addition, we observe that the polarity of the liquid has a significant influence on the THz wave generation. Alpha-pinene, a nonpolar liquid, offers much stronger THz radiation than water does. Besides paving the way to develop intense liquid THz sources, ou…
We measure the nonlinear refractive index coefficients in N$_2$, O$_2$ and Ar from visible through mid-infrared wavelengths (λ= 0.4 - 2.4 μm). The wavelengths investigated correspond to transparency windows in the atmosphere. Good agreement is found with theoretical models of $χ^{(3)}$. Our results are essential for accurately simulating the propagation of ultrashort mid-IR pulses in the atmosphere.
We numerically investigate the conical emission (CE) from ultrashort laser filaments, both considering and disregarding the higher-order Kerr effect (HOKE). While the consideration of HOKE has almost no influence on the predicted CE from collimated beams, differences arise for tightly focused beams. This difference is attributed to the different relative contributions of the non-linear focus and of the modulational instability over the whole filament length.
The critical power of self-focusing in the air for ultrashort UV laser pulses stretched due to dispersion from 90 up to 730 fs was experimentally measured. It was shown that the pulse duration enhancement due to its propagation in condensed media within above mentioned time-range leads to almost linear decrease of self-focusing critical power. It was also observed that when the pulse peak power exceeds the critical one, the maximum of linear plasma distribution along the UV laser filament does not shifted in the direction opposite to the laser pulse propagation as in the case of IR laser filam…
Based on numerical simulations, we show that higher-order nonlinear indices (up to $n_8$ and $n_{10}$, respectively) of air and argon have a dominant contribution to both focusing and defocusing in the self-guiding of ultrashort laser pulses over most of the spectrum. Plasma generation and filamentation are therefore decoupled. As a consequence, ultraviolet wavelength may not be the optimal wavelengths for applications requiring to maximize ionization.
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…
Ultrashort laser pulses that last only a few optical cycles have been transformative tools for studying and manipulating light--matter interactions. Few-cycle pulses are typically produced from high-peak-power lasers, either directly from a laser oscillator, or through nonlinear effects in bulk or fiber materials. Now, an opportunity exists to explore the few-cycle regime with the emergence of fully integrated nonlinear photonics. Here, we experimentally and numerically demonstrate how lithographically patterned waveguides can be used to generate few-cycle laser pulses from an input seed pulse…
We determine the laser-induced ablation threshold fluence in air of aluminum and tungsten excited by single near-infrared laser pulses with duration ranging from 15 fs to 100 fs. The ablation threshold fluence is shown constant for both metals, extending the corresponding scaling metrics to few-optical-cycle laser pulses. Meanwhile, the reflectivity is measured providing access to the deposited energy in the studied materials on a wide range of pulse durations and incident fluences below and above the ablation threshold. A simulation approach, based on the two-temperature model and the Drude-L…
We provide measurements of ablation of four post-transition and transition metals (aluminum, copper, nickel and tungsten) irradiated by single 800 nm laser pulses, in ultrashort regime from 100 fs pulse duration down to 15 fs covering a temporal range little explored yet. For each metal and pulse duration tested, we measure its ablation characteristics (depth and diameter) as a function of incident energy allowing us to determine its laser-induced ablation threshold and ablation rate in single-shot regime. For all metals studied, we observe constant ablation threshold fluence as a function of …
Ultrashort electron beams with femtosecond to picosecond bunch durations offer unique opportunities to explore active research areas ranging from ultrafast structural dynamics to ultra-high dose-rate radiobiological studies. We present a straightforward method to generate MeV-ranged electron beams in ambient air through the tight focusing of a few-cycle, mJ-class femtosecond IR laser. At one meter from the source, the highest measured dose rate of 0.15 Gy/s exceeds the yearly dose limit in less than one second and warrants the implementation of radiation protection. Two-dimensional Particle-In…
Using femtosecond laser pulses at 800 and 400 nm, we characterize the formation of underdense channels in air generated by laser filamentation at the millijoule energy level by means of transverse interferometry. We find that using tight focusing conditions, filamentation generates a shock wave and that the resulting low-density channel lasts for more than 90 ms. Comparison of these results with hydrodynamic simulations using an Eulerian hydrodynamic code gives an good agreement and allows us to estimate the initial gas peak temperature at $\sim$ 1000 K. The influence of experimental parameter…
We provide Python tools enabling numerical simulation and analysis of the propagation dynamics of ultrashort laser pulses in nonlinear waveguides. The modeling approach is based on the widely used generalized nonlinear Schrödinger equation for the pulse envelope. The presented software implements the effects of linear dispersion, pulse self-steepening, and the Raman effect. The focus lies on the implementation of input pulse shot noise, i.e. classical background fields that mimick quantum noise, which are often not thoroughly presented in the scientific literature. We discuss and implement com…
Multiple filamentation in air of high-power ultrashort laser radiation with transverse intensity profile resembling a "corona" composed by incoherent combining of several annularly distributed independent top-hat sub-beams is theoretically studied. Through the numerical solution of time-averaged nonlinear Schrodinger equation, we study the spatio-angular dynamics of synthesized near-infrared "corona-beam" (CB) along the optical path by varying the number and power of the beamlets (corona-spikes). For the first time to our knowledge, the evident advances in the multiple filamentation region man…
The multiple scattering of an ultrashort laser pulse by a turbid dispersive medium (namely a cloud of bubbles in water) is investigated by means of Monte Carlo simulations. The theory of Gouesbet and Gréhan [Part. Part. Syst. Charact. 17 213-224 (2000)] is used to derive an energetic model of the scattering transient. The spreading and extinction of the pulse is decoupled from the transient of scattering to describe each phenomenon individually. The transient of scattering is modeled with the Lorenz-Mie Theory, thus also valid for a relative refractive index lower than one, contrary to the Deb…
Femtosecond laser micromachining provides high precision and less thermal diffusion in surface structuring as a result of the ultrashort temporal duration and ultrahigh peak intensity of the femtosecond laser pulses. To increase the throughput of surface patterning, the focal spot size can be expanded with loose focusing, which, however, could lead to nonlinear self-focusing of the pulses when the pulses propagate in air. We solve the problem by use of spatiotemporally focused femtosecond laser pulses for ablation of metal surfaces, which gives rise to improved surface quality as compared with…
Propagation of a tightly focused high-power ultrashort laser pulse in an optical medium is usually substantially influenced by the medium optical nonlinearity that can noticeably affect the laser pulse parameters around the nonlinear focus and lead to unavoidable and often undesirable spatial distortions of the focal waist. We present the results of our experimental study and numerical simulations on a femtosecond Ti-Sapphire laser pulse propagation in air under different spatial focusing. We concentrated our study on spectral-angular and spatial pulse transformations under different focusing …
We experimentally investigate fluctuations in the spectrum of ultrashort laser pulses propagating in air, close to the critical power for filamentation. Increasing the laser peak power broadens the spectrum while the beam approaches the filamentation regime. We identify two regimes for this transition: In the center of the spectrum, the output spectral intensity increases continuously. In contrast, on the edges of the spectrum the transition implies a bimodal probability distribution function for intermediate incident pulse energies, where a high-intensity mode appears and grows at the expense…
Direct laser writing of surface waveguides with ultrashort pulses is a crucial achievement towards all-laser manufacturing of photonic integrated circuits sensitive to their environment. In this Letter, few-cycle laser pulses (with a sub-10 fs duration) are used to produce subsurface waveguides in a non-doped, non-coated fused silica substrate. The fabrication technique relies on laser-induced microdensification below the threshold for nanopore formation. The optical losses of the fabricated waveguides are governed by the optical properties of the superstrate. We have measured losses ranging f…
We present a systematic study on linear propagation of ultrashort laser pulses in media with dispersion, dispersionless media and vacuum. The applied method of amplitude envelopes gives the opportunity to estimate the limits of slowly warring amplitude approximation and to describe an amplitude integro-differential equation, governing the propagation of optical pulses in single cycle regime. The well known slowly varying amplitude equation and the amplitude equation for vacuum are written in dimensionless form. Three parameters are obtained defining different linear regimes of the optical puls…
