We numerically demonstrate the formation of carrier field shocks in various dispersive media for a wide variety of input conditions using two different electric field propagation models. In addition, an investigation of the impact of numerous physical effects on carrier wave shock is performed. It is shown that in many cases a field shock is essentially unavoidable and therefore extremely important in the propagation of intense long wavelength pulses in weakly dispersive nonlinear media such as noble gases, air, and single-crystal diamond. The results presented here are expected to have a significant impact in the field of ultrashort nonlinear optics, attosecond pulse generation, and wavepacket synthesis where the use of mid-IR wavelengths is becoming increasingly more important.
The nonlinear pulse propagation in an optical fibers with varying parameters is investigated. The capture of moving in the frequency domain femtosecond colored soliton by a dispersive trap formed in an amplifying fiber makes it possible to accumulate an additional energy and to reduce significantly the soliton pulse duration. Nonlinear dynamics of the chirped soliton pulses in the dispersion managed systems is also investigated. The methodology developed does provide a systematic way to generate infinite ``ocean'' of the chirped soliton solutions of the nonlinear Schrödinger equation (NSE) wit…
Dispersive wave emission (DWE) in gas-filled hollow-core dielectric waveguides is a promising source of tuneable coherent and broadband radiation, but so far the generation of few-femtosecond pulses using this technique has not been demonstrated. Using in-vacuum frequency-resolved optical gating, we directly characterise tuneable 3fs pulses in the deep ultraviolet generated via DWE. Through numerical simulations, we identify that the use of a pressure gradient in the waveguide is critical for the generation of short pulses.
We propose an efficient method to determine the effective refractive index of step-index optical fibers from the visible to the mid-IR and thus allowing to infer their dispersive properties over a broad spectral range. The validity of the method, based on the writing of an array of fiber Bragg gratings (FBGs) with known periods using the fs scanning phase mask technique, is first confirmed with a standard silica fiber, then applied to various fluoride glass fibers to determine their effective refractive index and dispersion over more than three octaves, i.e. from 550 to 4800 nm.
Generating energetic femtosecond mid-IR pulses is crucial for ultrafast spectroscopy, and currently relies on parametric processes that, while efficient, are also complex. Here we experimentally show a simple alternative that uses a single pump wavelength without any pump synchronization and without critical phase-matching requirements. Pumping a bulk quadratic nonlinear crystal (unpoled LiNbO$_3$ cut for noncritical phase-mismatched interaction) with sub-mJ near-IR 50-fs pulses, tunable and broadband ($\sim 1,000$ cm$^{-1}$) mid-IR pulses around $3.0~μ\rm m$ are generated with excellent spati…
High-energy ultraviolet pulse generation in gas-filled hollow capillary fibers (HCFs) through dispersive-wave-emission process, has attracted considerable attentions in recent several years due to its great application potentials in ultraviolet spectroscopy and photochemistry. While the ability of this technique to deliver high-energy, ultrafast ultraviolet pulses is widely recognized, few-fs duration of μJ-level dispersive-wave (DW) pulses has, however, escaped direct measurements. In this letter, we demonstrate that using several chirped mirrors, few-fs ultraviolet DW pulses can be obtained …
We describe novel optical switching schemes operating at femtosecond time scales by employing free carrier (FC) excitation. Such unprecedented switching times are made possible by spatially patterning the density of the excited FCs. In the first realization, we rely on diffusion, i.e., on the nonlocality of the FC nonlinear response of the semiconductor, to erase the initial FC pattern and, thereby, eliminate the reflectivity of the system. In the second realization, we erase the FC pattern by launching a second pump pulse at a controlled delay. We discuss the advantages and limitations of the…
We numerically investigate the energy and arrival-time noise of ultrashort laser pulses produced via resonant dispersive wave emission in gas-filled hollow-core waveguides under the influence of pump-laser instability. We find that for low pump energy, fluctuations in the pump energy are strongly amplified. However, when the generation process is saturated, the energy of the resonant dispersive wave can be significantly less noisy than that of the pump pulse. This holds for a variety of generation conditions and while still producing few-femtosecond pulses. We further find that the arrival-tim…
Energy carrier evolution is crucial for material performance. Ultrafast microscopy has been widely applied to visualize the spatiotemporal evolution of energy carriers. However, direct imaging of small amounts of energy carriers on nanoscale remains difficult due to extremely weak transient signals. Here we present a method for ultrasensitive and high-throughput imaging of energy carrier evolution in space and time. This method combines femtosecond pump-probe techniques with interferometric scattering microscopy (iSCAT), named Femto-iSCAT. The interferometric principle and unique spatially-mod…
We report that femtosecond surface plasmon polariton pulses can propagate along a metal-dielectric waveguide and that they can be modulated on the femtosecond timescale by direct ultrafast optical excitation of the metal, thereby offering unprecedented terahertz plasmonic bandwidth - a key missing component in the development of surface plasmons as information carriers for next generation nanophotonic devices.
In recent experiments, localized and stationary pulses have been generated in second-order nonlinear processes with femtosecond pulses, whose asymptotic features relate with those of nondiffracting and nondispersing polychromatic Bessel beams in linear dispersive media. We investigate on the nature of these linear waves, and show that they can be identified with the X-shaped (O-shaped) modes of the hyperbolic (elliptic) wave equation in media with normal (anomalous) dispersion. Depending on the relative strengths of mode phase mismatch, group velocity mismatch with respect to a plane pulse, an…
Electronic properties and lattice vibrations are supposed to be strongly correlated in metal-halide perovskites, due to the "soft" fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultra-fast photoexcitation is necessary for understanding the optoelectronic behaviour of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal ground and excited state vibrational modes of methylammonium lead-bromide perovskite. We observe a coherent phonon at 106 cm-1 (13 meV), pertaining to the inorganic octahedral, which is peculiar of the …
Rippled area formed by surface plasmon polaritons upon femtosecond laser double-pulse irradiation of silicon: the role of carrier generation and relaxation processes
Carrier and phonon dynamics in Bi2Se3 crystals are studied by a spatially resolved ultrafast pump-probe technique. Pronounced oscillations in differential reflection are observed with two distinct frequencies, and are attributed to coherent optical and acoustic phonons, respectively. The rising time of the signal indicates that the thermalization and energy relaxation of hot carriers are both sub-ps in this material. We found that the thermalization and relaxation time decreases with the carrier density. The expansion of the differential reflection profile allows us to estimate an ambipolar ca…
The dynamics of photocarriers in reduced graphene oxide thin films is studied by using ultrafast pump-probe spectroscopy. Time dependent differential transmissions are measured with sample temperatures ranging from 9 to 300 K. At each sample temperature and probe delay, the sign of differential transmission remains positive. A fast energy relaxation of hot carriers is observed, and is found to be independent of sample temperature. Our experiments show that the carrier dynamics in reduced graphene oxide is similar to other types of graphene, and that the differential transmission is caused by p…
Resonant dispersive wave (RDW) emission in gas-filled hollow waveguides is a powerful technique for the generation of bright few-femtosecond laser pulses from the vacuum ultraviolet to the near infrared. Here we investigate deep-ultraviolet RDW emission in a hollow capillary fibre filled with a longitudinal gas pressure gradient. We obtain broadly similar emission to the constant-pressure case by applying a surprisingly simple scaling rule for the gas pressure and study the energy-dependent dispersive-wave spectrum in detail using simulations. We further find that in addition to enabling dispe…
Optical solitons-stable waves balancing delicately between nonlinearities and dispersive effects-have advanced the field of ultrafast optics and dynamics, with contributions spanning supercontinuum generation and soliton fission, to optical event horizon, Hawking radiation, and optical rogue waves, amongst others. Here we investigate picojoule soliton dynamics in silicon slow-light photonic-bandgap waveguides under the influence of Drude-modeled free-carrier induced nonlinear effects. Using real-time and single shot amplified dispersive Fourier transform spectroscopy simultaneously with high-f…
Experimental and theoretical studies of laser-induced breakdown in dielectrics provide conflicting conclusions about the possibility to trigger ionization avalanche on the sub-picosecond time scale and the relative importance of carrier-impact ionization over field ionization. On the one hand, current models based on single ionization-rate equations do not account for the gradual heating of the charge carriers which, for short laser pulses, might not be sufficient to start an avalanche. On the other hand, models based on multiple rate equations that track the carriers kinetics rely on several …
We report supercontinuum generation by launching femtosecond Yb fiber laser pulses into a tapered single-mode fiber of 3 um core diameter. A spectrum of more than one octave, from 550 to 1400 nm, has been obtained with an output power of 1.3 W at a repetition rate of 250 MHz, corresponding to a coupling efficiency of up to 60%. By using a typical f-2f interferometer, the carrier envelope offset frequency was measured and found to have a signal-to-noise ratio of nearly 30 dB.
Carrier scattering processes are studied in CH$_3$NH$_3$PbI$_3$ using temperature-dependent four-wave mixing experiments. Our results indicate that scattering by ionized impurities limits the interband dephasing time (T$_2$) below 30~K, with strong electron-phonon scattering dominating at higher temperatures (with a timescale of 125 fs at 100 K). Our theoretical simulations provide quantitative agreement with the measured carrier scattering rate and show that the rate of acoustic phonon scattering is enhanced by strong spin-orbit coupling, which modifies the band-edge density of states. The Ra…
Compact chip-scale comb sources are of significant interest for many practical applications. Here, we experimentally study the generation of supercontinuum (SC) in an axially varying integrated waveguide. We show that the local tuning of the dispersion enables the continuous blue shift of dispersive waves thanks to their trapping by the strongly compressed pump pulse. This mechanism provides new insight into supercontinuum generation in a dispersion varying integrated waveguide. Pumped close to 2.2 $μ$m in the femtosecond regime and at a pulse energy of $\sim$ 4 pJ, the output spectrum extends…
Pulsed Bessel beams of light propagating in free-space experience diffraction effects that resemble those of anomalous dispersion on pulse propagation. It is then shown that a pulsed Bessel beam in a normally dispersive material can remain diffraction- and dispersion-free due to mutual cancellation of diffraction and group velocity dispersion. The size of the Bessel transversal profile for localized transmission is determined by the dispersive properties of the material at the pulse carrier frequency.
Harmonics of femtosecond and continuous-wave radiation for precision spectroscopy: generation efficiency and spectral line shape
P.N. Lebedev Physical Institute of the Russian Academy of Sciences（俄罗斯科学院列别杰夫物理研究所）；Moscow Institute of Physics and Technology（莫斯科物理技术学院）；Russian Quantum Center（俄罗斯量子中心）
Electron and vibrational dynamics of molecules are commonly studied by subjecting them to two interactions with a fast actinic pulse that prepares them in a nonstationary state and after a variable delay period $T$, probing them with a Raman process induced by a combination of a broadband and a narrowband pulse. This technique known as femtosecond stimulated Raman spectroscopy (FSRS) can effectively probe time resolved vibrational resonances. We show how FSRS signals can be modeled and interpreted using the stochastic Liouville equations (SLE) originally developed for NMR lineshapes. The SLE p…
The mechanisms of ripple formation on silicon surface by femtosecond laser pulses are investigated. We demonstrate the transient evolution of the density of the excited free-carriers. As a result, the experimental conditions required for the excitation of surface plasmon polaritons are revealed. The periods of the resulting structures are then investigated as a function of laser parameters, such as the angle of incidence, laser fluence, and polarization. The obtained dependencies provide a way of better control over the properties of the periodic structures induced by femtosecond laser on the …
We use dispersive Fourier transformation to measure shot-to-shot spectral instabilities in femtosecond supercontinuum generation. We study both the onset phase of supercontinuum generation with distinct dispersive wave generation, as well as a highly-unstable supercontinuum regime spanning an octave in bandwidth. Wavelength correlation maps allow interactions between separated spectral components to be identified, even when such interactions are not apparent in shot-to-shot or average measurements. Experimental results are interpreted using numerical simulations. Our results show the clear adv…
Hydrogenated amorphous silicon (a:Si-H) has recently been recognized as a highly nonlinear CMOS compatible photonic platform. We experimentally demonstrate the generation of a supercontinuum (SC) spanning over 500 nm in a-Si:H photonic wire waveguide at telecommunication wavelengths using femtosecond input pulse with energy lower than 5 pJ. Numerical modeling of pulse propagation in the waveguide, based on the experimentally characterized dispersion profile, shows that the supercontinuum is the result of soliton fission and dispersive wave generation. It is demonstrated that the SC is highly c…
We present a theoretical investigation of the yet unexplored ultrafast processes and dynamics of the produced excited carriers upon irradiation of Silicon with femtosecond pulsed lasers in the mid-infrared (mid-IR) spectral region. The evolution of the carrier density and thermal response of the electron-hole and lattice subsystems are analysed for various wavelengths λL in the range between 2.2 μm and 3.3 μm where the influence of two and three-photon absorption mechanisms is explored. The role of induced Kerr effect is highlighted and it manifests a more pronounced influence at smaller wavel…
Quantum-optical theory of the few femtosecond nonlinear optical response of Drude metals with a non-parabolic conduction band
South China Normal University（华南师范大学）；Shiv Nadar Institution of Eminence Deemed to be University（希夫纳达尔卓越大学）；Ben-Gurion University of the Negev（内盖夫本-古里安大学）
We consider the case of surface irradiation by a small number of femtosecond laser shots leading to the formation of surface ripples. To explain this effect, we propose a numerical model that accounts for the following processes: (i) interference of the laser irradiation with an electromagnetic surface wave propagating on a silicon sample; (ii) free carrier formation and laser energy absorption; (iii) energy relaxation and electron-phonon coupling. We perform numerical calculations taking into account the interference of a surface wave with laser; and present the obtained simulation results in…
A real-time ranging lidar with 0.1 Mega Hertz update rate and few-micrometer resolution incorporating dispersive Fourier transformation and instantaneous microwave frequency measurement is proposed and demonstrated. As time-stretched femtosecond laser pulse passing through an all-fiber Mach-Zehnder Interferometer, where the detection light beam is inserted into the optical path of one arm, the displacement is encoded to the frequency variation of the temporal interferogram. To deal with the challenges in storage and real-time processing of the microwave pulse generated on a photodetector, we t…
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…
Using the sensitivity of magneto-induced second harmonic generation to spin currents (SC), we demonstrate in Fe/Au/Fe/MgO(001) pseudo spin valves the generation of 250 fs-long SC pulses. Their temporal profile indicates that superdiffusive hot electron transport across a sub-100~nm Au layer is close to the ballistic limit and the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent Fe/Au interface transmittance we conclude that a non-thermal spin-dependent Seebeck effect is responsible for the generatio…
Femtosecond micromachining offers a contact-free and mask-less technique for material patterning. With ultrafast laser irradiation, permanent modifications to the properties of single layer graphene through material ablation or defect introduction can be induced. Multiple femtosecond pulse interactions with a single layer graphene are studied and a low laser ablation threshold ~9.2 mJ/cm2 is reported for a 15 second illumination time. Clean ablated structures are generated in such a multi pulse irradiation configuration at low pulse energies as an attractive alternative to ablation with single…
This paper reports the observation of ultra-superluminal pulse propagation in GaAs/AlGaAs multiple contact heterostuctures in a superradiant emission regime, and shows definitively that it is a different class of emission from conventional spontaneous or stimulated emission. It is shown that coherent population gratings induced in the semiconductor medium under strong electrical pumping have great impact in causing a decrease of the group refractive index in the range of 5-40%. This decrease is much greater than that which would be observed due to conventional carrier depletion or chirp mechan…
Oscillator-driven broadband femtosecond transient microspectroscopy with supercontinuum probes generated in a photonic crystal fiber
Osaka Metropolitan University（大阪公立大学）；Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)（马德里材料科学研究所）
Optical-field emission from nanostructured solids such as subwavelength nanoantennas can be leveraged to create sub-femtosecond, PHz-scale electronics for optical-field detection. One application that is of particular interest is the detection of an incident optical pulse's carrier-envelope phase. Such carrier-envelope-phase detection requires few-cycle, broadband optical excitation where the resonant properties of the nanoantenna can strongly alter the response of the near field in time. Little quantitative investigation has been performed to understand how the geometry and resonant propertie…
Carrier dynamics in single-layer graphene grown by chemical vapor deposition (CVD) is studied using spatially and temporally resolved pump-probe spectroscopy by measuring both differential transmission and differential reflection. By studying the expansion of a Gaussian spatial profile of carriers excited by a 1500-nm pump pulse with a 1761-nm probe pulse, we observe a diffusion of hot carriers of 5500 square centimeter per second. We also observe that the expansion of the carrier density profile decreases to a slow rate within 1 ps, which is unexpected. Furthermore, by using an 810-nm probe p…
