We calculated third order non-linear polarization to estimate the two-photon absorption of non-interacting two-level molecules in the transmission-type degenerate pump-probe geometry. The spectral intensity and the phase changes of the laser pulses when passing through a thin dielectric slab composed of the molecules were considered. We also investigated the effect of the decay rate of the molecules and the chirp of the pulses on their spectral intensity and phase changes.
In this work, we identify and characterize intra-pulse intensity noise shaping by saturable absorbers applied in mode-locked lasers and ultra-low noise nonlinear fiber amplifiers. Reshaped intra-pulse intensity noise distributions are shown to be inevitably interconnected with self-amplitude modulation, the fundamental physical mechanism for initiation and stabilization of ultra-short pulses in the steady-state of a mode-locked laser. A theoretical model is used to describe the ultrafast saturation dynamics by an intra-pulse noise transfer function for widely-applied slow and fast saturable ab…
The phase noise and intensity noise of a pulse train are theoretically analyzed in the demodulation measurement. The effect of pulse asymmetry is discussed for the first time using Fourier series. Experimentally, photodetectors with different bandwidth and incident power levels are compared to achieve minimum pulse distortion.
A theoretical and experimental investigation of the intensity noise reduction induced by two-photon absorption in a Er,Yb:Glass laser is reported. The time response of the two-photon absorption mechanism is shown to play an important role on the behavior of the intensity noise spectrum of the laser. A model including an additional rate equation for the two-photon-absorption losses is developed and allows the experimental observations to be predicted.
The main effects of an intense THz pulse on gas high harmonic generation are studied via trajectory analysis on the single atom level. Spectral and temporal modifications to the generated radiation are highlighted.
We present an approach to create pulse sequences extending beyond 150~picoseconds in duration, comprised of $100~μ$J femtosecond pulses. A quarter of the pulse train is produced by a high-resolution pulse shaper, which allows full controllability over the timing of each pulse. Two nested Michelson interferometers follow to quadruple the pulse number and the sequence duration. To boost the pulse energy, the long train is sent through a multi-pass Ti:Sapphire amplifier, followed by an external compressor. A periodic sequence of 84~pulses of 120~fs width and an average pulse energy of 107~$μ$J, s…
Analytical analysis of the decrease in the focal intensity of a femtosecond laser pulse caused by an imperfect surface of compressor diffraction gratings
We show that a pulse of electromagnetic radiation launched into a cavity can be completely absorbed into an infinitesimal region of space, provided one has a high degree of control over the current flowing through this region. We work out explicit examples of this effect in a cubic cavity and a cylindrical one, and experimentally demonstrate the effect in the microwave regime.
We firstly report mode-locked square-wave pulse in Yb-doped fiber laser based on graded index multimode fiber of reverse suturable absorption. By adjusting the pump power, the width of the square-wave can be tuned range from 350 ps to 52.6 ns with 3dB bandwidth spectrum of 0.73 nm. The supermode suppression ratio exceeds ~ 65 dB, which indicates excellent mode-locked operation state, and we also study the characteristic of pulse by the chirp measurement system. The mode-locked square-wave pulse fiber laser can sever as high power light source for industrial applications.
We report on a reflective wave-plate system utilizing phase-shifting mirrors (PSM) for a continuous variation of elliptical polarization without changing the beam position and direction. The scalability of multilayer optics to large apertures and the suitability for high-intensity broad-bandwidth laser beams make reflective wave-plates an ideal tool for experiments on relativistic laser-plasma interaction. Our measurements confirm the preservation of the pulse duration and spectrum when a 30-fs Ti:Sapphire laser beam passes the system.
Single-shot ultrafast absorbance spectroscopy based on the frequency encoding of the kinetics is analyzed theoretically and implemented experimentally. In Part II of the series, arbitrary thickness sample is analysed theroretically. The model is then used to simulate the results for a-Si:H films.
We report on the dependence of the frequency-to-intensity noise conversion in the locking of an ultrafast laser against a high-finesse optical resonator from the Carrier Envelope Offset (CEO) frequency. By a proper combination of the cavity finesse and laser CEO frequency it is possible to optimize the signal-to-noise ratio of the laser intensity trapped into the optical resonator. The theoretical description of the problem together with the numerical simulations and experimental results are presented with the aim of a strong suppression of the intensity fluctuations of the trapped laser field…
We use an open-aperture Z-scan technique to show how intense few-cycle terahertz pulses can experience a nonlinear bleaching of absorption in an n-doped semiconductor due to terahertz-electric-field-driven intervalley scattering of electrons in the conduction band. Coherent detection of the transmitted terahertz pulse waveform also allows the nonlinear conductivity dynamics to be followed with sub-picosecond time resolution. Both the Z-scan and time-domain results are found to be in agreement with our theoretical analysis.
We show that by manipulating the momentum (k) of a propagating optical pulse, the intensity can be controlled and highly enhanced in a linear binary photonic time crystal (PTC) system. The optical pulse equipped with k lying within the bandgap of the PTC gets amplified and gives rise to reflected and transmitted pulses with an equal growth in intensity moving in opposite directions. We predict and quantify the amount of amplification of the transmitted and reflected pulse and show the amplifications achieve a maximum at the centre of the k-gap accompanied by weaker growth in intensity at the e…
We report on measurements of second-order intensity correlations at the high brilliance storage ring PETRA III using a prototype of the newly developed Adaptive Gain Integrating Pixel Detector (AGIPD). The detector recorded individual synchrotron radiation pulses with an x-ray photon energy of 14.4 keV and repetition rate of about 5 MHz. The second-order intensity correlation function was measured simultaneously at different spatial separations that allowed to determine the transverse coherence length at these x-ray energies. The measured values are in a good agreement with theoretical simulat…
Self-consistent simulations of the ultrafast electron dynamics in thin metal films are performed. A regime of nonlinear oscillations is observed, which corresponds to ballistic electrons bouncing back and forth against the film surfaces. When an oscillatory laser field is applied to the film, the field energy is partially absorbed by the electron gas. Maximum absorption occurs when the period of the external field matches the period of the nonlinear oscillations, which, for sodium films, lies in the infrared range. Possible experimental implementations are discussed.
Collinear phase-matched optical rectification is studied in ZnGeP$_{2}$ pumped with near-infrared light. The pump-intensity dependence is presented for three crystal lengths (0.3, 1.0 and 3.0 mm) to determine the effects of linear optical absorption, nonlinear optical absorption and terahertz free-carrier absorption on the generation. Critical parameters such as the coherence length (for velocity matching), dispersion length (for linear pulse broadening) and nonlinear length (for self-phase modulation) are determined for this material. These parameters provide insight into the upper limit of p…
We predict that parametric sum-frequency generation of an ultra-short pulse may result from the mixing of an ultra-short optical pulse with a quasi-continuous wave control. We analytically show that the intensity, time duration and group velocity of the generated idler pulse may be controlled in a stable manner by adjusting the intensity level of the background pump.
Strong mid-infrared light-matter interaction has attracted extensive attention as it opens up new frontiers in nonlinear optics. Here we observe through simulations a novel aspect of mid-infrared pulse dynamics in a high-pressure gas-filled capillary, where a pulse with a power well below the critical power for Kerr self-focusing undergoes an astonishing rise of the peak intensity following an extremely efficient spectral broadening. This intensity enhancement is attributed to the Kerr-induced focusing of the supercontinuum. Our study provides an interesting perspective for controlling the las…
We present theoretical and experimental results on the generation and detection of pulsed, relative-intensity squeezed light in a hot Rb87 vapor. The intensity noise correlations between a pulsed probe beam and its conjugate, generated through nearly-degenerate four-wave mixing in a double-lambda system, are studied numerically and measured experimentally via time-resolved balanced detection. We predict and observe about -1 dB of time-resolved relative intensity squeezing with 50 nanosecond pulses at 1 MHz repetition rate. (-1.34 dB corrected for loss).
Group delay for a reflected light pulse from a weakly absorbing dielectric slab is theoretically investigated, and large negative group delay is found for weak absorption near a resonance of the slab ($Re(kd)=mπ$). The group delays for both the reflected and transmitted pulses will be saturated with the increase of the absorption.
Laser Pulse Diagnostics of Ultrafast <8 fs Pulses Through Two-Photon Absorption Fluorescence In Liquid Media -- The Role of GVD and Third-Order Dispersion
Self-compression of femtosecond laser pulses and more than an order of magnitude increase of the peak intensity is found in a positive dispersion medium in low dispersion regime based on the (3+1)-dimensional nonlinear Schr{ö}dinger equation. A method of high-intensity femtosecond pulse formation can be developed on that basis.
We report on the design and whole characterization of low-noise and affordable-cost Yb-doped double-clad fiber amplifiers operating at room temperature in the near-infrared spectral region at pulse repetition rate of 160 MHz. Two different experimental configurations are discussed. In the first one, a broadband seed radiation with a transform limited pulse duration of 71 fs, an optical spectrum of 20 nm wide at around 1040 nm, and 20 mW average power is adopted. In the second configuration, the seed radiation is constituted by stretched pulses with a time duration as long as 170 ps, with a 5-n…
The quantum dynamics of a system of Rb atoms, modeled by a V-type three-level system interacting with intense probe and pump pulses, are studied. The time-delay-dependent transient-absorption spectrum of an intense probe pulse is thus predicted, when this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model, which allows us to quantify the oscillating features of the resulting transient-absorption spectra in terms of the atomic populations and phases generated by the intense pulses. Strong-field-induced phases and their influence on …
We have measured the evolution of the light intensity of a random laser during a nanosecond pump pulse. Relaxation oscillations in a titania random laser were observed in the time trace of the total emitted intensity. We compare our experimental results with a simple model, based on the four-level rate equations for a single mode laser.
The recent remark by G. Mourou and T. Tajima (Science 331, 41 (2011)) on the intensity of the driver laser pulse and the duration of the created pulse that higher driver beam intensities are needed to reach shorter pulses of radiation remains a conjecture without clear theoretical reasoning so far. Here we offer its extension to the case of relativistic electron bunches as the laser's radiating medium (free-electron laser). This also bolsters the understanding of the underlying physical principle of the Conjecture.
We outline an approach for improving the temporal contrast of a high-intensity laser system by $>$8 orders of magnitude using non-collinear sum-frequency generation with the signal and idler of an optical parametric amplifier. We demonstrate the effectiveness of this technique by cleaning pulses from a millijoule-level chirped-pulse amplification system to provide $>$10$^{12}$ intensity contrast relative to all pre-pulses and amplified spontaneous emission $>$5~ps prior to the main pulse. The output maintains percent-level energy stability on the time scales of a typical user experiment at our…
We investigate how the quantum control of a two-level system (TLS) coupled to photons can modify and tune the TLS's photon absorption spectrum. Tuning and controlling the emission and the absorption is of much interest e.g.\ for the development of efficient interfaces between stationary and flying qubits in modern architectures for quantum computation and quantum communication. We consider the periodic pulse control, where the TLS is subjected to a periodic sequence of the near-resonant Rabi driving pulses, each pulse implementing a 180$^\circ$ rotation. For small inter-pulse delays, the absor…
A parallel 2D+1 split-step Fourier method with Crank-Nicholson scheme running on multi-core shared memory architectures is developed to study the propagation of ultra-short high-intensity laser pulses in air. The parallel method achieves a near linear speed-up with results for the efficiency of more than 95% on a 24-core machine. This method is of great potential application in studying the long-distance propagation of the ultra-short high intensity laser pulses.
The two most commonly used models for passively modelocked lasers with fast saturable absorbers are the Haus modelocking equation (HME) and the cubic-quintic modelocking equation (CQME). The HME corresponds to a special limit of the CQME in which only a cubic nonlinearity in the fast saturable absorber is kept in the model. Here, we use singular perturbation theory to demonstrate that the CQME has a stable high-energy solution for an arbitrarily small but non-zero quintic contribution to the fast saturable absorber. As a consequence, we find that the CQME predicts the existence of stable model…
The predictability of extreme intensity pulses emitted by an optically injected semiconductor laser is studied numerically, by using a well-known rate equation model. We show that symbolic ordinal time-series analysis allows to identify the patterns of intensity oscillations that are likely to occur before an extreme pulse. The method also gives information about patterns which are unlikely to occur before an extreme pulse. The specific patterns identified capture the topology of the underlying chaotic attractor and depend on the model parameters. The methodology proposed here can be useful fo…
The creation of attosecond pulses via laser-plasma interaction has been a subject of great scientific interest for more than three decades. This process is investigated by using particle-in-cell simulation with varying the plasma and laser parameters. The steepness of the density gradient at the plasma-vacuum interface is examined to see how this parameter affects the high-order harmonic generations and isolated-attosecond pulse creation. The optimal density gradient lengths $L$ are explored within the relativistic oscillating mirror mechanism. Although the ideal gradient lengths for the full …
The transient-absorption spectrum of a $V$-type three-level system is investigated, when this is periodically excited by a train of equally spaced, $δ$-like pump pulses as, e.g., from an optical-frequency-comb laser. We show that, even though the probe pulse is not assumed to be much shorter than the pump pulses, light-induced states appear in the absorption spectrum. The frequency- and time-delay-dependent features of the absorption spectra are investigated as a function of several laser control parameters, such as the number of pump pulses used, their pulse area, and the pulse-to-pulse phase…
The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is performed based on higher-order Feynman diagrams and non-perturbative numerical simulations of the system response. It is shown that higher-order contributions may lead to a fundamental change of the static appearance and beating-maps of the 2D spectra and that chirped pulses enhance or suppress distinct higher-order pathways. We further give an estimate of the t…
Today's high-power laser systems are capable of reaching photon intensities up to $10^{22}$ W/cm^2, generating plasmas when interacting with material. The high intensity and ultrashort laser pulse duration (fs) make direct observation of plasma dynamics a challenging task. In the field of laser-plasma physics and especially for the acceleration of ions, the spatio-temporal intensity distribution is one of the most critical aspects. We describe a novel method based on a single-shot (i.e. single laser pulse) chirped probing scheme, taking nine sequential frames at framerates up to THz. This tech…
We employed open-aperture Z-scan technique to unveil the third-order optical nonlinearity in ZnCo2O4 (ZCO) microflowers. Our results indicate that intersystem crossing (ISC) lifetime can be used as simple tool to demonstrate remarkably contrasting optical nonlinearity in ZCO. Ultrafast transient absorption measurements reveal that ISC from singlet to triplet state takes place in 5 ps. For femtosecond laser pulses, when the pulse duration is shorter than ISC lifetime, saturable absorption (SA) takes place for all intensities. On the contrary, when the pulse duration is longer than ISC for nanos…
We perform a theoretical investigation of the clamped laser intensity inside the filament plasma as a function of gas pressure with external focusing. Unlike the clamped intensity under the selffocusing condition, which is independent on the gas pressure, the clamped intensity with external focusing decreases with the gas pressure. Our findings can explain the changes of the signals of femtosecond-laser-induced 391-nm forward emission and fluorescence with the nitrogen gas pressure.
To shorten the duration of x-ray pulses, we present a nonlinear optical technique using atoms with core-hole vacancies (core-hole atoms) generated by inner-shell photoionization. The weak Coulomb screening in the core-hole atoms results in decreased absorption at photon energies immediately above the absorption edge. By employing this phenomenon, referred to as saturable absorption, we successfully reduce the duration of x-ray free-electron laser pulses (photon energy: 9.000 keV, duration: 6-7 fs, fluence: 2.0-3.5$\times$10$^5$ J/cm$^2$) by $\sim$35%. This finding that core-hole atoms are appl…
Spatiotemporal pulse shaping provides control over the trajectory and range of an intensity peak. While this control can enhance laser-based applications, the optical configurations required for shaping the pulse can constrain the transverse or temporal profile, duration, or orbital angular momentum (OAM). Here we present a novel technique for spatiotemporal control that mitigates these constraints by using a "stencil" pulse to spatiotemporally structure a second, primary pulse through cross-phase modulation (XPM) in a Kerr lens. The temporally shaped stencil pulse induces a time-dependent foc…
We present experimental studies on the generation and detection of pulsed, relative-intensity squeezed light in a warm rubidium vapor. The noise correlations between a pulsed probe beam and its conjugate -generated through nearly-degenerate four-wave mixing in a double-lambda system- are studied via time-resolved balanced detection. We observe -0.96 dB of time-resolved relative intensity squeezing with 50 nanosecond pulses at 1 MHz repetition rate. (-1.34 dB corrected for loss).
Using spectral interferometry technique, we measured subpicosecond time-resolved pre-plasma scale lengths and early expansion ($<$ 12 ps) of the plasma produced by a high intensity (2$\times$10$^{18}$ W/cm$^{2}$) pulse with ultra-high contrast (10$^{-9}$). We measured pre-plasma scale lengths in the range of 3-15 nm. This measurement plays a crucial role in understanding the mechanism of laser coupling its energy to hot electrons and hence important for laser-driven ion acceleration and fast ignition approach to fusion.
Intensity-dependent enhancement of saturable absorption in a film of PbS-Au4 nanohybrid composites has been observed by femtosecond time-resolved transient absorption measurement at 780 nm. The nonlinear absorption coefficient of saturable absorption in PbS-Au4 nanohybrid composites is found to be dependent on excitation irradiance and it is determined to be -2.9 cm/GW at 78 GW/cm2, an enhancement of nearly fourfold in comparison with that of pure PbS quantum dots (QDs). The enhancement is attributed to excitation of surface plasmon by resonant energy transfer between PbS QDs and Au nanopartic…
We study x-ray photon scattering in the head-on collision of an XFEL pulse and a focused high-intensity laser pulse, described as paraxial Laguerre-Gaussian beam of arbitrary mode composition. For adequately chosen relative orientations of the polarization vectors of the colliding laser fields, this gives rise to a vacuum birefringence effect manifesting itself in polarization flipped signal photons. Throughout this article the XFEL is assumed to be mildly focused to a waist larger than that of the high-intensity laser beam. As previously demonstrated for the special case of a fundamental para…
We investigate the population dynamics of the three-level system in the two-photon absorption (TPA) process, mainly focusing the influence of pulse width and Rabi frequency on the population dynamics of the system. We observe the dependency of the population with the Rabi frequency and the pulse width. We also show that the arbitrary superposition state consisted in two states, upper state and lower state, is possible by controlling the pulse width and Rabi frequency. The results obtained can be used to the case of more complex multilevel system and they can be valuable for coherent quantum co…
We propose a simple all-in-line single-shot scheme for diagnostics of ultrashort laser pulses, consisting of a multi-mode fiber, a nonlinear crystal and a CCD camera. The system records a 2D spatial intensity pattern, from which the pulse shape (amplitude and phase) are recovered, through a fast Deep Learning algorithm. We explore this scheme in simulations and demonstrate the recovery of ultrashort pulses, robustness to noise in measurements and to inaccuracies in the parameters of the system components. Our technique mitigates the need for commonly used iterative optimization reconstruction …
Attosecond transient absorption spectroscopy has thus far been lacking the capability to simultaneously characterize the intense laser pulses at work within a time-resolved quantum-dynamics experiment. However, precise knowledge of these pulses is key to extracting quantitative information in strong-field highly nonlinear light-matter interactions. Here, we introduce and experimentally demonstrate an ultrafast metrology tool based on the time-delay-dependent phase shift imprinted on a strong-field driven resonance. Since we analyze the signature of the laser pulse interacting with the absorbin…
We investigate the non-linear response and energy absorption in bulk silicon irradiated by intense 12-fs near-infrared laser pulses. Depending on the laser intensity, we distinguish two regimes of non-linear absorption of the laser energy: for low intensities, energy deposition and photoionization involve perturbative three-photon transition through the direct bandgap of silicon. For laser intensities near and above 10$^{14}$ W/cm$^2$, corresponding to photocarrier density of order 10$^{22}$ cm$^{-3}$, we find that absorption at near-infrared wavelengths is greatly enhanced due to excitation o…
The theory for the electric and magnetic fields energy absorption by small metallic particles subjected to the irradiation by ultrashort laser pulses of different duration in the region of surface plasmon excitation is developed. For the particles of the oblate or prolate spheroidal shape there has been found the dependence of the absorbed energy on a number of factors, including a particle radius, a degree of the shape deviation from a spherical one, a pulse duration, the orientation of the magnetic field upon particle, the magnitude of carrier frequency, and the value of a shift of the carri…
We experimentally investigate the propagation of optical pulses through a fast-light medium with competing absorption and gain. The combination of strong absorption and optical amplification in a potassium-based four-wave mixing process results in pulse peak advancements up to $88\%$ of the input pulse width, more than $35 \times$ that which is achievable without competing absorption. We show that the enhancement occurs even when the total gain of the four-wave mixer is unity, thereby rendering the medium transparent. By varying the pulse width, we observe a transition between fast and slow li…
We present intensity-resolved above threshold ionization (ATI) spectra of xenon using an intensity scanning and deconvolution technique. Experimental data were obtained with laser pulses of 58 fs and central wavelength of 800 nm from a chirped-pulse amplifier. Applying a deconvolution algorithm, we obtained spectra that have higher contrast and are in excellent agreement with characteristic 2 $U_p$ and 10 $U_p$ cutoff energies contrary to that found for raw data. The retrieved electron ionization probability is consistent with the presence of a second electron from double ionization. This reco…
We present the first fully ab initio calculations for attosecond transient absorption spectroscopy of atomic krypton with overlapping pump and probe pulses. Within the time-dependent configuration interaction singles (TDCIS) approach, we describe the pump step (strong-field ionization using a near-infrared pulse) as well as the probe step (resonant electron excitation using an extreme- ultraviolet pulse) from first principles. We extent our TDCIS model and account for the spin-orbit splitting of the occupied orbitals. We discuss the spectral features seen in a recent attosecond transient absor…
