Subpicosecond Pulses Research Articles

Enhancement of reactive oxygen species production by ultra-short electron pulses.

The development of laser-driven accelerators-on-chip has provided an opportunity to miniaturize devices for electron radiotherapy delivery. Laser-driven accelerators produce highly time-compressed electron pulses, on the 100 fs to 1 ps scale. This delivers electrons at high peak power yet low average beam current compared with conventional delivery devices, which generate pulses of approximately 3 µs. The biophysical effects of this time structure, however, are unclear. Here, we use a Monte Carlo simulation approach to explore the effects of the electron beam time structure on the production of reactive oxygen species (ROS) in water. Our results show a power law increase in the generation of hydroxyl ions per deposited electron with decreasing pulse length over the pulse length range of 10 µs to 100 fs. Similar trends were observed for hydrogen peroxide, superoxide, hydroperoxyl, hydronium and solvated electrons. In practical terms, this indicates a fourfold increase in the efficiency of free radical production for sub-picosecond pulses, relative to that of conventional microsecond pulses, for the same number of deposited electrons.

Multi-geometric discrete spectral problem with several pairs of zeros for Sasa–Satsuma equation

Sasa–Satsuma equation is proposed to model the propagation and interaction of the sub-picosecond or femtosecond pulses in a monomode optical fiber. Different from several integrable equations in the Ablowitz–Kaup–Newell–Segur system, the higher-order zeros of Riemann–Hilbert problem for the Sasa–Satsuma appear in quadruples. A new approach to study the multi-geometric discrete spectral problem with several pairs of zeros for the Sasa–Satsuma equation is proposed. Thus, the complete soliton solutions corresponding to the higher-order zeros with arbitrary geometric and algebraic multiplicities are derived. Moreover, the inelastic interactions between or among the solitons corresponding to the higher-order non-elementary zeros exhibit the shape-changing phenomena.

Multishot laser damage of multilayer dielectric mirrors in the near-infrared subpicosecond regime

The laser damage resistance of dielectric components of high-power laser facilities to laser irradiation depends significantly on the irradiation sequence. In the short pulse (fs) regime, it is known that continuous irradiation of these components leads to a reduction in the damage threshold, reflecting a laser fatigue effect. Conversely, in the long pulse (ns) regime, progressive irradiation of these components leads to an increase in the damage threshold, reflecting a laser conditioning effect. In this article, we experimentally evaluate the competition between the effects of laser fatigue and laser conditioning for multilayer dielectric components irradiated in the subpicosecond pulse regime in the infrared (∼1µm) through different test sequences. For this purpose, we implemented an original test sequence derived from an S-on-1 type protocol, which consists of irradiating the component until damage. By repeating this sequence at different set points, it was possible to estimate the progressive reduction in damage threshold with the number of laser irradiations and to compare it with that observed during the fluence ramps. Particular attention was also paid to the precise knowledge of the test beam irradiating the component, as a dependence of the beam surface on the test set point was highlighted.

Velocimetry of GHz elastic surface waves in quartz and fused silica based on full-field imaging of pump–probe reflectometry

This study reports an imaging method for gigahertz surface acoustic waves in transparent layers using infrared subpicosecond laser pulses in the ablation regime and an optical pump–probe technique. The reflectivity modulations due to the photoelastic effect of generated multimodal surface acoustic waves were imaged by an sCMOS camera illuminated by the time-delayed, frequency-doubled probe pulses. Moving the delay time between 6.0nsto11.5ns, image stacks of wave field propagation were created.Two representative samples were investigated: wafers of isotropic fused silica and anisotropic x-cut quartz. Rayleigh (SAW) and longitudinal dominant high-velocity pseudo-surface acoustic wave (HVPSAW) modes could be observed and tracked along a circular grid around the excitation center, allowing the extraction of angular profiles of the propagation velocity. In quartz, the folding of a PSAW was observed. A finite element simulation was developed to predict the measurement results. The simulation and measurement were in good agreement with a relative error of 2% to 5%.These results show the potential for fast and full-field imaging of laser-generated ultrasonic surface wave modes, which can be utilized for the characterization of thin transparent samples such as semiconductor wafers or optical crystals in the gigahertz frequency range.

Sub-picosecond pulses in single-mode optical fibres with the Kaup–Newell model via two innovative methods

Sub-picosecond pulses in single-mode optical fibres with the Kaup–Newell model via two innovative methods

Characterization of bright betatron radiation generated by direct laser acceleration of electrons in plasma of near critical density

Directed x-rays produced in the interaction of sub-picosecond laser pulses of moderate relativistic intensity with plasma of near-critical density are investigated. Synchrotron-like (betatron) radiation occurs in the process of direct laser acceleration (DLA) of electrons in a relativistic laser channel when the electrons undergo transverse betatron oscillations in self-generated quasi-static electric and magnetic fields. In an experiment at the PHELIX laser system, high-current directed beams of DLA electrons with a mean energy ten times higher than the ponderomotive potential and maximum energy up to 100 MeV were measured at 1019 W/cm2 laser intensity. The spectrum of directed x-rays in the range of 5–60 keV was evaluated using two sets of Ross filters placed at 0° and 10° to the laser pulse propagation axis. The differential x-ray absorption method allowed for absolute measurements of the angular-dependent photon fluence. We report 1013 photons/sr with energies >5 keV measured at 0° to the laser axis and a brilliance of 1021 photons s−1 mm−2 mrad−2 (0.1%BW)−1. The angular distribution of the emission has an FWHM of 14°–16°. Thanks to the ultra-high photon fluence, point-like radiation source, and ultra-short emission time, DLA-based keV backlighters are promising for various applications in high-energy-density research with kilojoule petawatt-class laser facilities.

Gigahertz electromagnetic pulse emission from femtosecond relativistic laser-irradiated solid targets.

The interactions between high-intensity laser and matter produce particle flux and electromagnetic radiation over a wide energy range. The generation of extremely intense transient fields in the radio frequency-microwave regime has been observed in femtosecond-to-nanosecond laser pulses with 1011-1020-W/cm2 intensity on both conductive and dielectric targets. These fields typically cause saturation and damage to electronic equipment inside and near an experimental chamber; nevertheless, they can also be effectively used as diagnostic tools. Accordingly, the characterization of electromagnetic pulses (EMPs) is extremely important and currently a popular topic for present and future laser facilities intended for laser-matter interaction. The picosecond and sub-picosecond laser pulses are considerably shorter than the characteristic electron discharge time (∼0.1 ns) and can be efficient in generating GHz EMPs. The EMP characterization study of femtosecond laser-driven solid targets is currently mainly in the order of 100 mJ laser energy, in this study, the EMP generated by intense (Joule class) femtosecond laser irradiation of solid targets has been measured as a function of laser energy, laser pulse duration, focal spot size, and target materials. And a maximum electric field of the EMP reaching up to 105 V/m was measured. Analyses of experimental results confirm a direct correlation between measured EMP energy and laser parameters in the ultrashort pulse duration regime. The EMP signals generated by femtosecond laser irradiation of solid targets mainly originate from the return current inside the target after hot electron excitation. Numerical simulations of EMP are performed according to the target charging model, which agree well with the experimental results.

In situ generation and reaction of a sub-picosecond electron pulse: ultrafast broadband spectroscopy.

A sub-picosecond resolved broadband transient absorption spectrometer for in situ generation and study of ultrafast reaction of short pulse electrons in water has been reported. A femtosecond near infrared (NIR) laser driven multiphoton ionization of water was used for the in situ generation of an ultra-short electron pulse in aqueous media. The dynamics of such electrons have been investigated using a broadband pump-probe spectrometer with a temporal resolution of sub-picosecond. The formation of the pre-hydrated electron having absorption in the NIR region and its subsequent solvation process leading to the formation of the hydrated electron has been monitored in real time using pump-probe spectroscopy. As a proof of concept, a reaction of pre-hydrated electrons and hydrated electrons with a highly oxidizing agent, methyl viologen, has been carried out. The competition of the reaction with methyl viologen and solvent relaxation of the pre-hydrated electron has been demonstrated by broadband ultrafast spectroscopy. Our results show that the reactivity of pre-hydrated electrons with methyl viologen is almost two orders of magnitude higher as compared to the hydrated electrons. Unlike complicated laser driven accelerators, the present table-top setup for the generation of an in situ ultrashort electron pulse and its reaction with different classes of molecules, especially biomolecules, will help us understand the early events of radiation-induced processes under reductive stress.

Sub-picosecond tunable mid-infrared light source for driving high-efficiency optical rectification.

Optical rectification (OR) is a popular way to generate coherent terahertz radiation. Here, we develop a sub-picosecond mid-infrared (mid-IR) light source with a tailored wavelength and pulse duration for enhancing the OR efficiency. Numerical simulations for a LiNbO3-based OR with tilted pulse-front excitation are first conducted to determine the optimal parameters of pump wavelength and pulse duration, demonstrating that the OR efficiency pumped by 4-µm sub-picosecond (0.5-0.6 ps) pulses is approximately twice the value with 0.8-µm pump at the same conditions. Guided by the simulation results, we build a BaGa4Se7-based optical parametric chirped-pulse amplification system with 1030-nm thin-disk pump and broadband mid-IR seeds. The output performances of >200-µJ pulse energy, ∼600-fs pulse duration and 1-kHz pulse repetition rate are achieved in a spectral range tunable from 3.5 to 5 µm. The large energy scalability and high parameter tunability make the light source attractive to high-efficiency OR in various materials.

High-Field Nonresonant Response of Zundel Cations to Intense Terahertz Radiation

The fundamental unit for comprehending the physicochemical properties of water, the Zundel cation configuration H5O2+, has yet to be exhaustively evaluated in terms of its interaction with terahertz (THz) electromagnetic waves, characterized by sub-picosecond oscillation periods or pulse widths. In this study, we embark on an investigation of the broad resonance and high-field nonresonant effects of intense THz radiation (ITR) on Zundel cations, utilizing a multifaceted methodological approach that includes density functional theory (DFT) calculations, finite difference time domain (FDTD) algorithm of the Schrödinger equation, and ab initio molecular dynamics (AIMD) simulations. Our analysis reveals that the proton potential energy surface (PES) varies in response to the external electric (E) field, suggesting that the interaction frequency of the central proton with the electromagnetic wave encompasses the THz band. This resonance effect is associated with proton behavior that may oscillate or demonstrate periodic tunneling. Moreover, our work uncovers the high-field nonresonant effects of ITR on Zundel cations, manifesting in proton transfer and vibrational excitation of the system. Our findings contribute to the understanding of the interaction between Zundel species and electromagnetic waves by presenting a microscopic view of proton transfer as informed by wavefunction evolution.

Electro-Optic Sampling of a Free-Running Terahertz Quantum-Cascade-Laser Frequency Comb

Quantum-cascade-laser (QCL) frequency combs are compact semiconductor light sources operating in the mid-IR and terahertz frequencies. Achieving subpicosecond laser pulses with high peak power is of vital importance for performing nonlinear time-resolved spectroscopy as well for exploring nonlinear phenomena. Therefore, investigation and characterization of time-resolved free-running laser emission is a key for further improvement and optimization of these intersubband devices. In this work, we demonstrate a direct electric field measurement of a free-running terahertz QCL frequency comb using electro-optic sampling in combination with computational phase correction, where we retrieve the electric field profile and access the comb parameters. The demonstrated method is of high interest for time-resolved low-power laser emission characterization, typical for ring terahertz QCL frequency combs and investigation of phase-compensated emission via waveguide dispersion engineering for broadband comb operation.

Free electron laser stochastic spectroscopy revealing silicon bond softening dynamics

Time-resolved x-ray emission/absorption spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires x-ray pulses with both a narrow bandwidth and subpicosecond pulse duration, a combination that in principle finds its optimum with Fourier transform-limited pulses. In this work, we explore an alternative experimental approach, capable of simultaneously retrieving information about unoccupied (XAS) and occupied (XES) states from the stochastic fluctuations of broadband extreme ultraviolet pulses of a free electron laser. We used this method, in combination with singular-value decomposition and Tikhonov regularization procedures, to determine the XAS/XES response from a crystalline silicon sample at the ${L}_{2,3}$ edge, with an energy resolution of a few tens of meV. Finally, we combined this spectroscopic method with a pump-probe approach to measure structural and electronic dynamics of a silicon membrane. Tr-XAS/XES data obtained after photoexcitation with an optical laser pulse at 390 nm allowed us to observe perturbations of the band structure, which are compatible with the formation of the predicted precursor state of a nonthermal solid-liquid phase transition associated with a bond softening phenomenon.

Three-dimensional printing of silica glass with sub-micrometer resolution

Silica glass is a high-performance material used in many applications such as lenses, glassware, and fibers. However, modern additive manufacturing of micro-scale silica glass structures requires sintering of 3D-printed silica-nanoparticle-loaded composites at ~1200 °C, which causes substantial structural shrinkage and limits the choice of substrate materials. Here, 3D printing of solid silica glass with sub-micrometer resolution is demonstrated without the need of a sintering step. This is achieved by locally crosslinking hydrogen silsesquioxane to silica glass using nonlinear absorption of sub-picosecond laser pulses. The as-printed glass is optically transparent but shows a high ratio of 4-membered silicon-oxygen rings and photoluminescence. Optional annealing at 900 °C makes the glass indistinguishable from fused silica. The utility of the approach is demonstrated by 3D printing an optical microtoroid resonator, a luminescence source, and a suspended plate on an optical-fiber tip. This approach enables promising applications in fields such as photonics, medicine, and quantum-optics.

Simulation of the response of a diamond-based radiation detector to ultra-short and intense high-energy electron pulses

Single-crystal synthetic diamond sensors have been widely used in radiation dosimetry and beam diagnostics. The foreseen harsh radiation environment in electron-positron colliders at the luminosity frontier requires a thorough investigation of diamond’s response to large radiation bursts, in particular, to intense high-energy electron pulses. In this article, a two-step numerical simulation approach (Sentaurus + LTspice) is proposed to explore this topic. The time response of the diamond detector is simulated using TCAD-Sentaurus while the transmission effect of the electronic circuit is taken into account using LTspice. Good agreement is observed between results of the numerical simulation and preliminary experimental data from detector’s exposure to high-energy sub-picosecond electron pulses, on both the amplitude and the shape of the induced signals. This simulation combination is a novel approach to designing and optimizing diamond detectors for radiation and beam loss monitoring in particle physics experiments.

100-GHz ultra-short high-peak-power colliding-pulse mode-locked laser with asymmetric coating.

By using colliding-pulse mode-locking (CPM) configuration with asymmetric cladding layer and coating, 1.5-µm AlGaInAs/InP multiple quantum well (MQW) CPM lasers with high-power and ultra-short pulse generation capability at a repetition rate of 100 GHz are reported. The laser adopts a high-power epitaxial design, with four pairs of MQWs and an asymmetrical dilute waveguide cladding layer to reduce the internal loss, maintaining good thermal conductivity while increasing the saturation energy of the gain region. The asymmetric coating is introduced, as compared to conventional CPM laser with symmetric reflectivity, to further increase the output power and shorten the pulse width. With a high reflection (HR) coating of 95% on one facet and another facet as cleaved, 100-GHz sub-picosecond optical pulses with peak power on a Watt level are demonstrated. Two mode-locking states, the pure CPM state and the partial CPM state, are investigated. Pedestal-free optical pulses are obtained for both states. For the pure CPM state, a pulse width of 564 fs, an average power of 59 mW, a peak power of 1.02 W, and an intermediate mode suppression ratio over 40 dB are demonstrated. For the partial CPM state, a pulse width of 298 fs is demonstrated.

Genetic algorithm optimization of broadband operation in a noise-like pulse fiber laser

The noise-like pulse regime of optical fiber lasers is highly complex, and associated with multiscale emission of random sub-picosecond pulses underneath a much longer envelope. With the addition of highly nonlinear fiber in the cavity, noise-like pulse lasers can also exhibit supercontinuum broadening and the generation of output spectra spanning 100’s of nm. Achieving these broadest bandwidths, however, requires careful optimization of the nonlinear polarization rotation based saturable absorber, which involves a very large potential parameter space. Here we study the spectral characteristics of a broadband noise-like pulse laser by scanning the laser operation over a random sample of 50,000 polarization settings, and we quantify that these broadest bandwidths are generated in only sim 0.5% of cases. We also show that a genetic algorithm can replace trial and error optimization to align the cavity for these broadband operating states.

Self-synchronized temporal-spectral characterization system for revealing ultrafast fiber laser dynamics

Due to the electronic bottleneck limited real-time measurement speed of common temporal-spectral detection and the particle-like nature of optical soliton enabled nonrepeatable transient behaviors, capturing the ultrafast laser pulses with unknown times of arrival and synchronously characterizing their temporal-spectral dynamic evolution is still a challenge. Here, using the Raman soliton frequency shift based temporal magnifier and dispersive Fourier transform based spectral analyzer, we demonstrate a self-synchronized, ultrafast temporal-spectral characterization system with a resolution of 160 fs and 0.05 nm, and a recording length above milliseconds. The synchronized nonlinear process makes it possible to image full-filled temporal sub-picosecond pulse trains regardless of their arrival times and without extra pump lasers and photoelectric conversion devices. To demonstrate the significance of this improvement, a buildup dynamic process of a soliton laser with a complex breakup and collisions of multisolitons is visually displayed in the spectral and temporal domains. The soliton dynamic evolution processes observed by our characterization system are in one-to-one correspondence with the numerical simulation results. We believe this work provides a new multidimensional technique to break the electronic bottleneck to gain additional insight into the dynamics of ultrafast lasers and nonlinear science.

Post-compression of high-energy, sub-picosecond laser pulses

Abstract The post-compression technique based on self-phase modulation of high-energy pulses leads to an increase in achievable peak power and intensity. Typically, the pulses considered in experiments have been less than 100 fs in duration. Here, the method is applied to the ELFIE laser system at the LULI facility, for a pulse of 7 J energy and an initial measured duration of 350 fs. A 5-mm-thick fused silica window and a 2 mm cyclic-olefin polymer were used as optical nonlinear materials. The 9 cm diameter beam was spectrally broadened to a bandwidth corresponding to 124 fs Fourier-limited pulse duration, and then it was partly post-compressed to 200 fs. After measuring the spatial spectra of the beam fluence, a uniform gain factor of 4 increase in the fluctuations over the studied range of frequencies is observed, due to small-scale self-focusing.

Intense and Superflat White Laser with 700-nm 3-dB Bandwidth and 1-mJ Pulse Energy Enabling Single-Shot Subpicosecond Pulse Laser Spectroscopy.

An optical spectrometer is a basic spectral instrument that probes microscopic physical and chemical properties of macroscopic objects but generally suffers from difficulty in broadband time-resolved measurement. In this work, we report the creation of ultrabroadband white-light laser with a 3-dB bandwidth covering 385 to 1,080 nm, pulse energy of 1.07 mJ, and pulse duration of several hundred femtoseconds by passing 3-mJ pulse energy, 50-fs pulse duration Ti:Sapphire pulse laser through a cascaded fused silica plate and chirped periodically poled lithium niobate crystal. We utilize this unprecedented superflat, ultrabroadband, and intense femtosecond laser light source to build a single-shot (i.e., single-pulse) subpicosecond pulse laser ultraviolet-visible-near-infrared spectrometer and successfully measure various atomic and molecular absorption spectra. The single-shot ultrafast spectrometer may open up a frontier to monitor simultaneously the ultrafast dynamics of multiple physical and chemical processes in various microscopic systems.

Ultrafast Buildup Dynamics of Terahertz Pulse Generation in Mode-Locked Quantum Cascade Lasers

Ultrashort terahertz pulse generation is essential for a range of proven terahertz applications, from time-resolved spectroscopy of fundamental excitations to nondestructive testing and imaging. Recently, it has been shown that semiconductor-based terahertz quantum cascade lasers (QCLs) can be used to generate pulses as short as a few picoseconds through active mode locking. However, further progress for subpicosecond and high peak power pulse generation is hampered by poor knowledge on how the electric field actually forms in these lasers. Here, we theoretically and experimentally show the amplitude- and phase-resolved buildup of pulse generation through active mode locking, from initiation of pulse generation to the nanosecond steady state. The experimental results, using an ultrafast coherent seeding technique to probe the laser from femtosecond to nanosecond time scales, are in full agreement with the theoretical calculations based on a theoretical model using multimode reduced rate equations. In particular, we show that the electric field buildup to achieve short pulse operation is extremely fast, requiring only a few photon round trips, owing to the ultrafast gain dynamics of the lasers. Further, this shows a gain recovery time of the order of a few picoseconds, an order of magnitude smaller than the photon round-trip time, highlighting that terahertz QCLs are categorically class-A lasers. This demonstration marks an important formulism for future progress towards exploring the ultrafast pulse generation buildup dynamics of these complex semiconductor lasers.