The precise spatiotemporal characterization of broadband ultrafast laser beams is essential for accurate laser control and holds significant potential in photochemistry and high-intensity laser physics. Existing methods for spatiotemporal characterization, such as frequency-resolved optical gating (FROG) and compressed ultrafast photography (CUP), are often spatially averaged or suffer from limited spatial resolution. Recent advances in imaging techniques based on multiplexed ptychography have enabled high-spatial-resolution diagnostics of ultrafast laser beams. However, the discrete spectral assumption inherent in multiplexed ptychographic algorithms does not align with the continuous spectral structure of ultrafast laser pulses, leading to significant crosstalk between different wavelength channels (WCs). This paper presents a method to reduce the bandwidth of each wavelength channel through spectral modulation, followed by the discretization of the continuous spectrum using interference techniques, which significantly improves the convergence and accuracy of the reconstruction. Using this method, the experiment accurately measured chromatic dispersion, spatial chirp, and other spatiotemporal coupling effects in femtosecond laser beams, achieving a spatial resolution of 9.4 μm, close to the pixel size resolution limit of the angular spectrum method.
Combining high peak power and high average power has long been a key challenge of ultrafast laser technology, crucial for applications such as laser-plasma acceleration and strong-field physics. A promising solution lies in post-compressed ytterbium lasers, but scaling these to high pulse energies presents a major bottleneck. Post-compression techniques, particularly Herriott-type multi-pass cells (MPCs), have enabled large peak power boosts at high average powers but their pulse energy acceptance reaches practical limits defined by setup size and coating damage threshold. In this work, we address this challenge and demonstrate, to our knowledge, a novel type of compact, energy-scalable MPC (CMPC). By employing a novel MPC configuration and folding the beam path, the CMPC introduces a new degree of freedom for downsizing the setup length, enabling compact setups even for large pulse energies. We experimentally and numerically verify the CMPC approach, demonstrating post-compression of 8 mJ pulses from 1 ps down to 51 fs in atmospheric air using a cell roughly 45 cm in length at low fluence values. Additionally, we discuss the potential for energy scaling up to 200 mJ with a setup size reaching 2.5 m. Our work presents a new approach to high-energy post-compression, with up-scaling potential far beyond the demonstrated parameters. This opens new routes for achieving the high peak and average powers necessary for demanding applications of ultrafast lasers.
We present a novel, to our knowledge, optical arbitrary waveform generation (OAWG) technique, termed four-wave optical-waveguided chirp-free ultrafast shaping (FOCUS), which utilizes four-wave mixing (FWM)-based spectral transcription. FOCUS enables the generation of chirp-free pulse sequences with independently adjustable duration, intensity, interval, and central wavelength of sub-pulses. Experimental validation demonstrates that the system achieves a 2 ps temporal resolution and a 400 ps record length while maintaining <1 nm spectral bandwidth, >30 dB extinction ratio, ∼1 nJ pulse energy consumption, and 3.5 nm continuous wavelength tunability. Fundamental analysis reveals that three key parameters govern temporal resolution: spectral shaper resolution (the current limiting factor), pump bandwidth (potentially expandable to 30 nm), and engineered group delay dispersion (GDD). Recent advancements in chip-scale mode-locked lasers, dispersion-engineered waveguides, and nonlinear FWM modules position the FOCUS platform as a promising candidate for next-generation ultrafast photonic systems designed for simultaneous sub-picosecond temporal resolution and nanosecond-scale waveform programmability within compact integrated architectures.
Through achieving high-spatial-frequency laser-induced periodic surface structures (HSFLs) on a gold/graphene hybrid film, we introduce a high-speed, high-resolution, and wide-gamut chromotropic color printing technique. This method effectively addresses the trade-off between throughput and resolution in laser coloring. To realize Au HSFL, disordered lattice structures and high transmittance of amorphous Au (a-Au) thin film are used to overcome the rapid hot-electron diffusion and loss of plasmonic coherence typically observed on low-loss metal surfaces, respectively. Coupled with crystallization in Au and modulated surface plasmon polaritons by artificial “seed” pre-structure growing in a SiO2/Si substrate, HSFL emerged with a period of 100 nm on crystalline Au after single and rapid femtosecond laser scanning. This equips the proposed color printing with high-resolution and high-speed features simultaneously. In addition, the crystallization process is demonstrated to initiate change in the complex refractive index of Au, which causes wide-gamut colors. The chromotropic capability, which facilitates the background color to be tailored in color as well as into desirable shapes independently, enables three-level anti-counterfeiting based on the proposed color printing. Therefore, the proposed color printing is amenable for practical implementation in diverse applications, including security marking and data storage, ranging from nanoscale to large-scale fabrication.
Conservation of parity plays a fundamental role in our understanding of various quantum processes. However, it is difficult to observe in atomic and molecular processes induced by a strong laser field due to their multiphoton character and the large number of states involved. Here we report an effect of parity in strong-field Rydberg-state excitation (RSE) by comparing the RSE probabilities of the N2 molecule and its companion atom Ar, which has a similar ionization potential but opposite parity of its ground state. Experimentally, we observe an oscillatory structure as a function of intensity with a period of about 50 TW/cm2 in the ratio between the RSE yields of the two species, which can be reproduced by simulations using the time-dependent Schrödinger equation (TDSE). We analyze a quantum-mechanical model, which allows for interference of electrons captured in different spatial regions of the Rydberg-state wave function. In the intensity-dependent RSE yield, it results in peaks with alternating heights with a spacing of 25 TW/cm2 and at the same intensity for both species. However, due to the opposite parities of their ground states, pronounced RSE peaks in Ar correspond to less pronounced peaks in N2 and vice versa, which leads to the period of 50 TW/cm2 in their ratio. Our work reveals a novel parity-related interference effect in the coherent-capture picture of the RSE process in intense laser fields.
Solid-state high-order harmonic generation (HHG) presents a promising approach for achieving controllable broadband coherent light sources and dynamically detecting materials. In this study, we demonstrate the all-optical control of HHG in a strongly correlated system, vanadium dioxide (VO2), through photo-carrier doping. It has been discovered that HHG can be efficiently modified using a pump laser, achieving modulation depths approaching 100% (extinction ratio ≥40 dB) on femtosecond timescales. Quantitative analysis reveals that the driving forces behind pump-dependent HHG are attributed to two distinct many-body dynamics: the scattering-induced dephasing and the insulator-to-metal transition (IMT) caused by photo-induced electron shielding. These two dynamics play a crucial role in defining the intensity and transient response of the HHG. Furthermore, we demonstrate that it is possible to quantitatively extract the metallic phase fraction from time-resolved HHG (tr-HHG) signals throughout the IMT. This study highlights the benefits of utilizing many-body dynamics for controlling HHG and underscores the necessity for further theoretical research on HHG in strongly correlated systems.
The realization of spatiotemporal vortex structure of various physical fields with transverse orbital angular momentum (OAM) has attracted much attention and is expected to expand the research scope and open new opportunities in their respective fields. Here we present theoretically the first, to the best of our knowledge, study on the generation of attosecond pulse trains featuring a spatiotemporal optical vortex (STOV) structure by a two-color femtosecond light field, with each color carrying transverse OAM. Through careful optimization of relative phase and intensity ratio, we validate the efficient upconversion of the infrared pulse into its tens of order harmonics, showing that each harmonic preserves a corresponding intact topological charge. This unique characteristic enables the synthesis of an extreme ultraviolet attosecond pulse train with transverse OAM. In addition, we reveal that ionization depletion plays an outsize role therein. Our studies pave the way for the generation and utilization of light fields with STOV in the attosecond regime.
Resonant metasurfaces provide a promising solution to overcome the limitations of nonlinear materials in nature by enhancing the interaction between light and matter and amplifying optical nonlinearity. In this paper, we design an aluminum (Al) metasurface that supports surface lattice resonance (SLR) with less nanoparticle filling density but more prominent saturable absorption effects, in comparison to a counterpart that supports localized surface plasmon resonance (LSPR). In detail, the SLR metasurface exhibits a narrower resonance linewidth and a greater near-field enhancement, leading to a more significant modulation depth (9.6%) at a low incident fluence of 25 μJ/cm2. As an application example, we have further achieved wavelength-tunable Q-switched pulse generation from 1020 to 1048 nm by incorporating the SLR-based Al metasurface as a passive saturable absorber (SA) in a polarization-maintaining ytterbium-doped fiber laser. Typically, the Q-switched pulse with a repetition rate of 33.7 kHz, pulse width of 2.1 μs, pulse energy of 141.7 nJ, and signal-to-noise ratio (SNR) of greater than 40 dB at the fundamental frequency can be obtained. In addition, we have investigated the effects of pump power and central wavelength of the filter on the repetition rate and pulse width of output pulses, respectively. In spite of demonstration of only using the Al metasurface to achieve a passive Q-switched fiber laser, our work offers an alternative scheme to build planar, lightweight, and broadband SA devices that could find emerging applications from ultrafast optics to neuromorphic photonics, considering the fast dynamics, CMOS-compatible fabrication, and decent nonlinear optical response of Al-material-based nanoplasmonics.
Self-assembly of dissipative solitons arouses versatile configurations of molecular complexes, enriching intriguing dynamics in mode-locked lasers. The ongoing studies fuel the analogy between matter physics and optical solitons, and stimulate frontier developments of ultrafast optics. However, the behaviors of multiple constituents within soliton molecules still remain challenging to be precisely unveiled, regarding both the intramolecular and intermolecular motions. Here, we introduce the concept of “soliton isomer” to elucidate the molecular dynamics of multisoliton complexes. The time-lens and time-stretch techniques assisted temporal-spectral analysis reveals the diversity of assembly patterns, reminiscent of the “isomeric molecule”. Particularly, we study the fine energy exchange during the intramolecular motions, therefore gaining insights into the degrees of freedom of isomeric dynamics beyond temporal molecular patterns. All these findings further answer the question of how far the matter-soliton analogy reaches and pave an efficient route for assisting the artificial manipulation of multisoliton structures.
Mid-infrared frequency-comb spectroscopy enables measurement of molecules at megahertz spectral resolution, sub-hertz frequency accuracy, and microsecond acquisition speed. However, the widespread adoption of this technique has been hindered by the complexity and alignment sensitivity of mid-infrared frequency-comb sources. Leveraging the underexplored mid-infrared window of silica fibers presents a promising approach to address these challenges. In this study, we present the first, to the best of our knowledge, experimental demonstration and quantitative numerical description of mid-infrared frequency-comb generation in silica fibers. Our all-silica-fiber frequency comb spans over two octaves (0.8 μm to 3.4 μm) with a power output of 100 mW in the mid-infrared region. The amplified quantum noise is suppressed using four-cycle (25 fs) driving pulses, with the carrier-envelope offset frequency exhibiting a signal-to-noise ratio of 40 dB and a free-running bandwidth of 90 kHz. Our developed model provides quantitative guidelines for mid-infrared frequency-comb generation in silica fibers, enabling all-fiber frequency-comb spectroscopy in diverse fields such as organic synthesis, pharmacokinetics processes, and environmental monitoring.
Colliding of two counter-propagating laser pulses is a widely used approach to create a laser field or intensity surge. We experimentally demonstrate broadband coherent terahertz (THz) radiation generation through the interaction of colliding laser pulses with gas plasma. The THz radiation has a dipole-like emission pattern perpendicular to the laser propagation direction with a detected peak electric field 1 order of magnitude higher than that by single pulse excitation. As a proof-of-concept demonstration, it provides a deep insight into the physical picture of laser–plasma interaction, exploits an important option to the promising plasma-based THz source, and may find more applications in THz nonlinear near-field imaging and spectroscopy.
Two-color plasma, induced by two lasers of different colors, can radiate ultra-broadband and intense terahertz (THz) pulses, which is desirable in many technological and scientific applications. It was found that the polarization of the emitted THz depends on the phase difference between the fundamental laser wave and its second harmonic. Recent investigation suggests that chirp-induced change of pulse overlap plays an important role in the THz yield from two-color plasma. However, the effect of laser chirp on THz polarization remains unexplored. Hereby, we investigate the impact of laser chirp on THz polarization. It is unveiled that the chirp-induced phase difference affects THz polarization. Besides, positive and negative chirps have opposite effects on the variation of the THz polarization versus the phase difference. The polarization of THz generated by a positively chirped pump laser rotates clockwise with an increasing phase difference, while it rotates anticlockwise when generated by a negatively chirped pump laser.
Spectral fingerprint and terahertz (THz) field-induced carrier dynamics demands the exploration of broadband and intense THz signal sources. Spintronic THz emitters (STEs), with high stability, a low cost, and an ultrabroad bandwidth, have been a hot topic in the field of THz sources. One of the main barriers to their practical application is lack of an STE with strong radiation intensity. Here, through the combination of optical physics and ultrafast photonics, the Tamm plasmon coupling (TPC) facilitating THz radiation is realized between spin THz thin films and photonic crystal structures. Simulation results show that the spectral absorptance can be increased from 36.8% to 94.3% for spin THz thin films with TPC. This coupling with narrowband resonance not only improves the optical-to-spin conversion efficiency, but also guarantees THz transmission with a negligible loss (∼4%) for the photonic crystal structure. According to the simulation, we prepared this structure successfully and experimentally realized a 264% THz radiation enhancement. Furthermore, the spin THz thin films with TPC exhibited invariant absorptivity under different polarization modes of the pump beam and weakening confinement on an obliquely incident pump laser. This approach is easy to implement and offers possibilities to overcome compatibility issues between the optical structure design and low energy consumption for ultrafast THz opto-spintronics and other similar devices.
Frequency detuning of mode-locked fiber lasers displays many remarkable nonlinear dynamical behaviors. Here we report for the first time the evolution of pulses from mode-locking through period pulsation to Q-switched mode-locking for three fundamental cases. Our experiments are performed in a hybrid actively and passively amplitude-modulated all-fiber polarization-maintaining mode-locked fiber laser, where the amplitude modulation frequency artificially deviates from the fundamental frequency of the cavity. We design and numerically simulate the laser with coupled Ginzburg–Landau equations. The experimentally observed dynamics of the mode detuning process is discussed with the assistance of the fitted model and numerical simulations, showing the generalizability of the optical mode detuning variation process. Our work provides fundamental insights for understanding perturbations in nonlinear optical resonant cavities and expands the ideas for studying chaotic path theory in hybrid mode-locked fiber lasers.
High-precision time interval measurement is a fundamental technique in many advanced applications, including time and distance metrology, particle physics, and ultra-precision machining. However, many of these applications are confined by the imprecise time interval measurement of electrical signals, restricting the performance of the ultimate system to a few picoseconds, which limits ultrahigh precision applications. Here, we demonstrate an optical means for the time interval measurement of electrical signals that can successfully achieve femtosecond (fs) level precision. The setup is established using the optical frequency comb (OFC) based linear optical sampling (LOS) technique to realize timescale-stretched measurement. We achieve a measurement precision of 82 fs for a single LOS scan measurement and 3.05 fs for the 100-times average with post-processing, which is three orders of magnitude higher than the results of older electrical methods. The high-precision time interval measurement of electrical signals can substantially improve precision measurement technologies.
Launching, tracking, and controlling picosecond acoustic (PA) pulses are fundamentally important for the construction of ultrafast hypersonic wave sources, ultrafast manipulation of matter, and spatiotemporal imaging of interfaces. Here, we show that GHz PA pulses can be all-optically generated, detected, and manipulated in a 2D layered MoS2/glass heterostructure using femtosecond laser pump–probe. Based on an interferometric model, PA pulse signals in glass are successfully decoupled from the coexisting temperature and photocarrier relaxation and coherent acoustic phonon (CAP) oscillation signals of MoS2 lattice in both time and frequency domains. Under selective interface excitations, temperature-mediated interfacial phonon scatterings can compress PA pulse widths by about 50%. By increasing the pump fluences, anharmonic CAP oscillations of MoS2 lattice are initiated. As a result, the increased interatomic distance at the MoS2/glass interface that reduces interfacial energy couplings can markedly broaden the PA pulse widths by about 150%. Our results open new avenues to obtain controllable PA pulses in 2D semiconductor/dielectric heterostructures with femtosecond laser pump–probe, which will enable many investigations and applications.
In spintronic applications, there is a constant demand for lower power consumption, high densities, and fast writing speed of data storage. All-optical switching (AOS) is a technique that uses laser pulses to switch the magnetic state of a recording medium without any external devices, offering unsurpassed recording rates and a simple structure. Despite extensive research on the mechanism of AOS, low energy consumption and fast magnetization reversing remain challenging engineering questions. In this paper, we propose a newly designed cavity-enhanced AOS in GdCo alloy, which promotes optical absorption by twofold, leading to a 50% reduction in energy consumption. Additionally, the time-resolved measurement shows that the time of reversing magnetization reduces at the same time. This new approach makes AOS an ideal solution for energy-effective and fast magnetic recording, paving the way for future developments in high-speed, low-power-consumption data recording devices.
Characterization of the state of polarization (SOP) of ultrafast laser emission is relevant in several application fields such as field manipulation, pulse shaping, testing of sample characteristics, and biomedical imaging. Nevertheless, since high-speed detection and wavelength-resolved measurements cannot be simultaneously achieved by commercial polarization analyzers, single-shot measurements of the wavelength-resolved SOP of ultrafast laser pulses have rarely been reported. Here, we propose a method for single-shot, wavelength-resolved SOP measurements that exploits the method of division-of-amplitude under far-field transformation. A large accumulated chromatic dispersion is utilized to time-stretch the laser pulses via dispersive Fourier transform, so that spectral information is mapped into a temporal waveform. By calibrating our test matrix with different wavelengths, wavelength-resolved SOP measurements are achieved, based on the division-of-amplitude approach, combined with high-speed opto-electronic processing. As a proof-of-concept demonstration, we reveal the complex wavelength-dependent SOP dynamics in the build-up of dissipative solitons. The experimental results show that the dissipative soliton exhibits far more complex wavelength-related polarization dynamics, which are not shown in single-shot spectrum measurement. Our method paves the way for single-shot measurement and intelligent control of ultrafast lasers with wavelength-resolved SOP structures, which could promote further investigations of polarization-related optical signal processing techniques, such as pulse shaping and hyperspectral polarization imaging.
In pursuit of efficient high-order harmonic conversion in semiconductor devices, modeling insights into the complex interplay among ultrafast microscopic electron–hole dynamics, nonlinear pulse propagation, and field confinement in nanostructured materials are urgently needed. Here, a self-consistent approach coupling semiconductor Bloch and Maxwell equations is applied to compute transmission and reflection high-order harmonic spectra for finite slab and sub-wavelength nanoparticle geometries. An increase in the generated high harmonics by several orders of magnitude is predicted for gallium arsenide nanoparticles with a size maximizing the magnetic dipole resonance. Serving as a conceptual and predictive tool for ultrafast spatiotemporal nonlinear optical responses of nanostructures with arbitrary geometry, our approach is anticipated to deliver new strategies for optimal harmonic manipulation in semiconductor metadevices.
Classic interferometry was commonly adopted to realize ultrafast phase imaging using pulsed lasers; however, the reference beam required makes the optical structure of the imaging system very complex, and high temporal resolution was reached by sacrificing spatial resolution. This study presents a type of single-shot ultrafast multiplexed coherent diffraction imaging technique to realize ultrafast phase imaging with both high spatial and temporal resolutions using a simple optical setup, and temporal resolution of nanosecond to femtosecond scale can be realized using lasers of different pulse durations. This technique applies a multiplexed algorithm to avoid the data division in space domain or frequency domain and greatly improves the spatial resolution. The advantages of this proposed technique on both the simple optical structure and high image quality were demonstrated by imaging the generation and evaluating the laser-induced damage and accompanying phenomenon of laser filament and shock wave at a spatial resolution better than 6.96 μm and a temporal resolution better than 10 ns.
The spatiotemporal measurement of ultrashort laser beams usually involves techniques with complex set-ups or limited by instabilities that are unable to accurately retrieve the frequency-resolved wavefront. Here, we solve these drawbacks by implementing a simple, compact, and ultra-stable spatiotemporal characterization technique based on bulk lateral shearing spectral interferometry using a birefringent uniaxial crystal. We apply it to retrieve complex spatiotemporal structures by characterizing ultrafast optical vortices with constant and time-varying orbital angular momentum. This technique can operate in all the transparency range of the anisotropic elements, enabling the characterization in different spectral ranges like infrared, visible, or ultraviolet.
We demonstrate numerically and experimentally the generation of powerful supercontinuum vortices from femtosecond vortex beams by using multiple thin fused silica plates. The supercontinuum vortices are shown to preserve the vortex phase profile of the initial beam for spectral components ranging from 500 nm to 1200 nm. The transfer of the vortex phase profile results from the inhibition of multiple filamentation and the preservation of the vortex ring with relatively uniform intensity distribution by means of the thin-plate scheme, where the supercontinuum is mainly generated from the self-phase modulation and self-steepening effects. Our scheme works for vortex beams with different topological charges, which provides a simple and effective method to generate supercontinuum vortices with high power.
Precise and stable synchronization between an optical frequency comb (femtosecond mode-locked laser oscillator or microresonator-based comb) and a microwave oscillator is important for various fields including telecommunication, radio astronomy, metrology, and ultrafast X-ray and electron science. Timing detection and synchronization using electro-optic sampling with an interferometer has been actively used for low-noise microwave generation, long-distance timing transfer, comb stabilization, time-of-flight sensing, and laser-microwave synchronization for ultrafast science facilities. Despite its outstanding performance, there has been a discrepancy in synchronization performance of more than 10 dB between the projected shot-noise-limited noise floor and the measured residual noise floor. In this work, we demonstrate the shot-noise-limited performance of an electro-optic timing detector-based comb-microwave synchronization, which enabled an unprecedented residual phase noise floor of -174.5 dBc/Hz at 8 GHz carrier frequency (i.e., 53 zs/Hz1/2 timing noise floor), integrated rms timing jitter of 88 as (1 Hz to 1 MHz), rms timing drift of 319 as over 12 h, and frequency instability of 3.6×10-20 over 10,000 s averaging time. We identified that bandpass filtering of the microwave signal and optical pulse repetition-rate multiplication are critical for achieving this performance.
We demonstrate generation of 7.6 fs near-UV pulses centered at 400 nm via 8-fold soliton-effect self-compression in an Ar-filled hollow-core kagomé-style photonic crystal fiber with ultrathin core walls. Analytical calculations of the effective compression length and soliton order permit adjustment of the experimental parameters, and numerical modeling of the nonlinear pulse dynamics in the fiber accurately predicts the spectrotemporal profiles of the self-compressed pulses. After compensation of phase distortion introduced by the optical elements along the beam path from the fiber to the diagnostics, 71% of the pulse energy was in the main temporal lobe, with peak powers in excess of 0.2 GW. The convenient setup opens up new opportunities for time-resolved studies in spectroscopy, chemistry, and materials science.
Intense laser fields focused into ambient air can be used to generate high-bandwidth current densities in the form of plasma channels and filaments. Excitation with bichromatic fields enables us to adjust the amplitude and sign of these currents using the relative phase between the two light pulses. Two-color filamentation in gas targets provides a route to scaling the energy of terahertz pulses to microjoule levels by driving the plasma channel with a high-energy laser source. However, the structure of plasma channels is highly susceptible to drifts in both the relative phase and other laser parameters, making control over the waveform of the radiated terahertz fields delicate. We establish a clear link between the phase dependence of plasma currents and terahertz radiation by comparing in situ detection of current densities and far-field detection of terahertz electric fields. We show that the current measurement can be used as a feedback parameter for stabilizing the terahertz waveform. This approach provides a route to energetic terahertz pulses with exceptional waveform stability.
Ultrafast visible radiation is of great importance for many applications ranging from spectroscopy to metrology. Because some regions in the visible range are not covered by laser gain media, optical parametric oscillators offer an added value. Besides a high-power broadband laser source, the ability to rapidly tune the frequency of pulses with high-power spectral density offers an extra benefit for experiments such as multicolor spectroscopy or imaging. Here, we demonstrate a broadband, high-power, rapidly tunable femtosecond noncollinear optical parametric oscillator with a signal tuning range of 440–720 nm in the visible range. The oscillator is pumped by the third harmonic of an Yb-fiber laser at 345 nm with a repetition rate of 50.2 MHz. Moreover, the signal wavelength is tuned by changing the cavity length only, and output powers up to 452 mW and pulse durations down to 268 fs are achieved. This is, to the best of our knowledge, the first demonstration of a quickly tunable femtosecond optical parametric oscillator that covers nearly the entire visible spectral range with high output power.
Complex Swift Hohenberg equation (CSHE) has attracted intensive research interest over the years, as it enables realistic modeling of mode-locked lasers with saturable absorbers by adding a fourth-order term to the spectral response. Many researchers have reported a variety of numerical solutions of CSHE which reveal interesting pulse patterns and structures. In this work, we have demonstrated a CSHE dissipative soliton fiber laser experimentally using a unique spectral filter with a complicated transmission profile. The behavior and performance of the laser agree qualitatively with the numerical simulations based on CSHE. Our findings bring insight into dissipative soliton dynamics and make our mode-locked laser a powerful testbed for observing dissipative solitons of CSHE, which may open a new course in ultrafast fiber laser research.
Recent developments in ultrafast laser technology have resulted in novel few-cycle sources in the mid-infrared. Accurately characterizing the time-dependent intensities and electric field waveforms of such laser pulses is essential to their applications in strong-field physics and attosecond pulse generation, but this remains a challenge. Recently, it was shown that tunnel ionization can provide an ultrafast temporal “gate” for characterizing high-energy few-cycle laser waveforms capable of ionizing air. Here, we show that tunneling and multiphoton excitation in a dielectric solid can provide a means to measure lower-energy and longer-wavelength pulses, and we apply the technique to characterize microjoule-level near- and mid-infrared pulses. The method lends itself to both all-optical and on-chip detection of laser waveforms, as well as single-shot detection geometries.
Femtosecond laser-induced periodic surface structures (LIPSS) have several applications in surface structuring and functionalization. Three major challenges exist in the fabrication of regular and uniform LIPSS: enhancing the periodic energy deposition, reducing the residual heat, and avoiding the deposited debris. Herein, we fabricate an extremely regular low-spatial-frequency LIPSS (LSFL) on a silicon surface by a temporally shaped femtosecond laser. Based on a 4f configuration zero-dispersion pulse shaping system, a Fourier transform limit (FTL) pulse is shaped into a pulse train with varying intervals in the range of 0.25–16.2 ps using periodic π-phase step modulation. Under the irradiation of the shaped pulse with an interval of 16.2 ps, extremely regular LSFLs are efficiently fabricated on silicon. The scan velocity for fabricating regular LSFL is 2.3 times faster, while the LSFL depth is 2 times deeper, and the diffraction efficiency is 3 times higher than those of LSFL using the FTL pulse. The formation mechanisms of regular LSFL have been studied experimentally and theoretically. The results show that the temporally shaped pulse enhances the excitation of surface plasmon polaritons and the periodic energy deposition while reducing the residual thermal effects and avoiding the deposition of the ejected debris, eventually resulting in regular and deeper LSFL on the silicon surface.
The combined effect of short (picosecond) optical and (nanosecond) electrical pulses on dielectric breakdown is investigated both theoretically and experimentally. It was demonstrated that nanosecond electrical pulses (nsEPs), being applied simultaneously with picosecond optical pulses, reduce the threshold for optical breakdown. Experimental results are discussed with respect to an extended model for opto-electrical-induced breakdown. The newly unveiled effect is expected to play a significant role in spatially confined electroporation and further advances in laser-ablation-based processes while also allowing for measurements of ambipolar diffusion constants.
Molecular ions, produced via ultrafast ionization, can be quantum emitters with the aid of resonant electronic couplings, which makes them the ideal candidates to study strong-field quantum optics. In this work, we experimentally and numerically investigate the necessary condition for observing a collective emission arising from macroscopic quantum polarization in a population-inverted N2+ gain system, uncovering how the individual ionic emitters proceed into a coherent collection within hundreds of femtoseconds. Our results show that for a relatively high-gain case, the collective emission behaviors can be readily initiated for all the employed triggering pulse area. However, for a low-gain case, the superradiant amplification is quenched since the building time of macroscopic interionic quantum coherence exceeds the dipole dephasing time, in which situation the seed amplification and free induction decay play an essential role. These findings not only clarify the contentious key issue regarding to the amplification mechanism of N2+ lasing but also show the unique characteristics of ultrashort laser-induced amplification in a molecular ion system where both the microscopic and macroscopic quantum coherence might be present.
In the diagnosis of severe contagious diseases such as Ebola, severe acute respiratory syndrome, and COVID-19, there is an urgent need for protein sensors with large refractive index sensitivities. Current terahertz metamaterials cannot be used to develop such protein sensors due to their low refractive index sensitivities. A simple method is proposed that is compatible with all geometrical structures of terahertz metamaterials to increase their refractive index sensitivities. This method uses patterned photoresist to float the split-ring resonators (SRRs) of a terahertz metamaterial at a height of 30 μm from its substrate that is deposited with complementary SRRs. The floating terahertz metamaterial has an extremely large refractive index sensitivity of 532 GHz/RIU because its near field is not distributed over the substrate and also because the complementary SRRs confine the field above the substrate. The floating terahertz metamaterial senses bovine serum albumin (BSA) and the protein binding of BSA and anti-BSA as BSA, and anti-BSA solutions with low concentrations that are smaller than 0.150 μmol/L are sequentially dropped onto it. The floating terahertz metamaterial is a great achievement to develop protein sensors with extremely large refractive index sensitivities, and has the potential to sense dangerous viruses.
Ultra-intense femtosecond vortex pulses can provide an opportunity to investigate the new phenomena with orbital angular momentum (OAM) involved in extreme cases. This paper reports a high gain optical vortex amplifier for intense femtosecond vortex pulses generation. Traditional regeneration amplifiers can offer high gain for Gaussian mode pulses but cannot amplify optical vortex pulses while maintaining the phase singularity because of mode competition. Here, we present a regeneration amplifier with a ring-shaped pump. By controlling the radius of the pump, the system can realize the motivation of the Laguerre–Gaussian [LG0,1(?1)] mode and the suppression of the Gaussian mode. Without seeds, the amplifier has a donut-shaped output containing two opposite OAM states simultaneously, as our prediction by simulation. If seeded by a pulse of a topologic charge of 1 or ?1, the system will output an amplified LG0,1(?1) mode pulse with the same topologic charge as the seed. To our knowledge, this amplifier can offer the highest gain as 1.45×106 for optical vortex amplification. Finally, we obtain a 1.8 mJ, 51 fs compressed optical vortex seeded from a 2 nJ optical vortex.
A new method to make an all-fiber nonlinear optic device for laser pulse generation is developed by depositing multi-layer graphene oxide (GO) selectively onto the core of the cleaved fiber facet by combining the electrical arc discharge and the laser-driven self-exfoliation. Using the GO colloid droplet with sub-nanoliter volume, we obtained a GO bulk layer deposited on a fiber facet of the order of milliseconds by using an electric arc. The prepared fiber facet was then included in an Er-doped fiber laser (EDFL) cavity and we obtained a few layers of GO having nonlinear optic two-dimensional (2D) characteristics selectively on the fiber core by the laser-driven self-exfoliation. The 2D GO layers on the fiber core served as a stable and efficient saturable absorber enabling robust pulse train generation at λ=1600.5 nm, the longest Q-switched laser wavelength in EDFLs. Pulse characteristics were analyzed as we varied the pump power at λ=980 nm from 105.2 mW to 193.6 mW, to obtain the maximum repetition rate of 17.8 kHz and the maximum output power of 2.3 mW with the minimum pulse duration of 7.8 μs. The proposed method could be further applied to other novel inorganic 2D materials opening a window to explore their novel nonlinear optic laser applications.
Optically driven photoconductive switches are one of the predominant sources currently used in terahertz imaging systems. However, owing to their low average powers, only raster-based images can be taken, resulting in slow acquisition. In this work, we show that by placing a photoconductive switch within a cavity, we are able to generate absolute average THz powers of 181 μW with the frequency of the THz emission centered at 1.5 THz—specifications ideally adapted to applications such as non-destructive imaging. The cavity is based on a metal–insulator–metal structure that permits an enhancement of the average power by almost 1 order of magnitude compared to a standard structure, while conserving a broadband spectral response. We demonstrate proof-of-principle real-time imaging using this source, with the broadband spectrum permitting to eliminate strong diffraction artifacts.
The origin of terahertz (THz) generation in a gas-phase medium is still in controversy, although the THz sources have been applied across many disciplines. Herein, the THz generation in a dual-color field is investigated experimentally by precisely controlling the relative phase and polarization of dual-color lasers, where the accompanying third-harmonic generation is employed for in situ determination of the relative phase up to sub-wavelength accuracy. Joint studies with the strong approximation (SFA) theory reveal that the continuum-continuum (CC) transition within an escaped electron wave packet in the single atom gives birth to THz emission, without the necessity of considering the plasma effect. Meanwhile, we develop the analytic form from SFA-based CC description, which is able to reproduce and decompose the classical photocurrent model from the viewpoint of microscopic quantum theory, establishing the quantum-classical correspondence and bringing a novel insight into the mechanism of THz generation. Present studies leave open the possibility for probing the ultrafast dynamics of continuum electrons and a new dimension for the study of THz-related science and methodology.
The year 2019 marks the 10th anniversary of the first report of ultrafast fiber laser mode-locked by graphene. This result has had an important impact on ultrafast laser optics and continues to offer new horizons. Herein, we mainly review the linear and nonlinear photonic properties of two-dimensional (2D) materials, as well as their nonlinear applications in efficient passive mode-locking devices and ultrafast fiber lasers. Initial works and significant progress in this field, as well as new insights and challenges of 2D materials for ultrafast fiber lasers, are reviewed and analyzed.
While the performance of mode-locked fiber lasers has been improved significantly, the limited gain bandwidth restricts them from generating ultrashort pulses approaching a few cycles or even shorter. Here we present a novel method to achieve few-cycle pulses (~5 cycles) with an ultrabroad spectrum (~400 nm at ?20 dB) from a Mamyshev oscillator configuration by inserting a highly nonlinear photonic crystal fiber and a dispersion delay line into the cavity. A dramatic intracavity spectral broadening can be stabilized by the unique nonlinear processes of a self-similar evolution as a nonlinear attractor in the gain fiber and a “perfect” saturable absorber action of the Mamyshev oscillator. To the best of our knowledge, this is the shortest pulse width and broadest spectrum directly generated from a fiber laser.
Diverse ultrafast dynamics have been reported on different graphene prepared by different methods. Chemical-vapor-deposited (CVD) growth is regarded as a very promising method for highly efficient production of graphene. However, CVD-grown graphene usually presents only one of the diverse ultrafast dynamics. Thus, control of the ultrafast photo-electronic dynamics of CVD-grown graphene is vital to present the diversity for different photodetection applications of CVD-grown graphene. In this paper, we report on the first realization to our knowledge of control of the ultrafast dynamics of CVD-grown graphene and the manifestation of diverse ultrafast dynamics on sole CVD-grown graphene. We study the ultrafast photoelectronic dynamics of CVD-grown graphene with different degrees of oxidation caused by ozone oxidation using femtosecond time-resolved transient differential transmission spectroscopy, and we find that the ultrafast dynamics can evolve obviously with the time of ozone oxidation. The diverse ultrafast dynamics reported previously on different monolayer graphenes prepared by different methods are achieved on the sole CVD-grown graphene by controlling oxidation time. The mechanism for manipulation of the ultrafast dynamics by ozone oxidation is revealed by Raman spectroscopy as the control of the Fermi level of CVD-grown graphene. Simulations of dynamics based on the optical conductivity model of graphene and Fermi level change well reproduce the observed diverse ultrafast dynamics. Our results are very important for the diverse applications of graphene and open a new path toward the diverse ultrafast dynamics on the sole graphene prepared by any method.
Acousto-optic interactions, employed in the ultrafast laser regulation, possess remarkable advantages for fast tuning performance in a wide spectral range. Here, we propose an ultrafast fiber laser whose wideband tunability is provided by an acousto-optic structure fabricated with an etched single-mode fiber. Because of the laser polarization conversion induced by the coupling between the core and cladding vector modes in the etched fiber, a band-pass characteristic of the acousto-optic interaction is achieved to effectively regulate the inner-cavity gain range. Cooperating with a saturable absorber based on single-wall carbon nanotubes (SWCNTs) with polarization robustness, a soliton operating state is achieved in the tunable erbium-doped fiber laser. By controlling the acoustical wave frequency from 1.039 to 1.069 MHz, this soliton laser can be conveniently tuned in a wide spectral range from 1571.52 to 1539.26 nm. Meanwhile, the laser pulses have near-transform-limited durations stably maintaining less than 2 ps at different wavelength channels, owing to the broadband nonlinear absorption of SWCNTs.
We demonstrate, for the first time, to the best of our knowledge, an all-fiber figure-of-9 double-clad Tm-doped fiber laser operating in the dissipative soliton resonance (DSR) regime. Stable mode-locked rectangular pulses are obtained by using the nonlinear amplifying loop mirror (NALM) technique. A long spool of high-nonlinearity fiber (HNLF) and a segment of SMF-28 fiber are used to enhance the nonlinearity of the NALM loop and to obtain a large all-anomalous regime. Output power and pulse energy are further boosted by using a three-stage master oscillator power amplifier (MOPA) system. At the maximum pump power, average output power of up to 104.3 W with record pulse energy of 0.33 mJ is achieved with a 2 μm DSR-based MOPA system.
The ability to control the energy transfer in rare-earth ion-doped luminescent materials is very important for various related application areas such as color display, bio-labeling, and new light sources. Here, a phase-shaped femtosecond laser field is first proposed to control the transfer of multiphoton excited energy from Tm3+ to Yb3+ ions in co-doped glass ceramics. Tm3+ ions are first sensitized by femtosecond laser-induced multiphoton absorption, and then a highly efficient energy transfer occurs between the highly excited state Tm3+ sensitizers and the ground-state Yb3+ activators. The laser peak intensity and polarization dependences of the laser-induced luminescence intensities are shown to serve as proof of the multiphoton excited energy transfer pathway. The efficiency of the multiphoton excited energy transfer can be efficiently enhanced or completely suppressed by optimizing the spectral phase of the femtosecond laser with a feedback control strategy based on a genetic algorithm. A (1+2) resonance-mediated three-photon excitation model is presented to explain the experimental observations. This study provides a new way to induce and control the energy transfer in rare-earth ion-doped luminescent materials, and should have a positive contribution to the development of related applications.
1.2 μJ pulses with average power of 9 W were directly generated from a passively mode-locked picosecond oscillator based on a Nd:GdVO4 bulk crystal. Short cavity operation in continuous wave and mode-locking regimes was conducted first to confirm the resonator performance and proper alignment. With a carefully calibrated q-preserving multi-pass cell inserted into the laser cavity, the cavity length of the original short cavity was extended while the mode-matching condition was maintained fairly well. Compared with the short cavity, nearly fivefold energy enhancement was achieved while the diffraction-limited beam quality was undisturbed. To the best of our knowledge, this is the highest output power ever produced from a mode-locked oscillator based on a single bulk crystal at a repetition rate below 10 MHz without cavity dumping.
We propose a simple and efficient method to optimize two-color chirped laser pulses by forming a “temporal gate” for the generation of isolated attosecond pulses (IAPs) in soft X rays. We show that the generation process for higher and cutoff harmonics can be effectively limited within the temporal gate, and the harmonic emission interval can be further reduced with the help of phase-matching by only selecting the contribution from short-trajectory electrons. This two-color gating mechanism is verified by increasing the pulse duration, raising the gas pressure, and extending the target cutoff. Compared to the five-color waveform in Phys. Rev. Lett.102, 063003 (2009)PRLTAO0031-900710.1103/PhysRevLett.102.063003, our waveform can be used to generate the IAP in the long-duration laser pulse while the cutoff energy is higher without the reduction of harmonic yields. Our work provides an alternative temporal gating scheme for the generation of IAPs by simultaneously improving the harmonic conversion efficiency, thus making the attosecond soft X rays an intense and highly time-resolved tabletop light source for future applications.
There exists an increasing demand of industrial-scale production of high-purity ligand-free nanoparticles due to the continuous development of biomedicine, catalysis, and energy applications. In this contribution, a simultaneous spatial and temporal focusing (SSTF) setup is first proposed for increasing nanoparticle productivity of the eco-friendly pulsed laser ablation in liquids (PLAL) technique. In spite of the fact that femtosecond pulses have proved to achieve higher ablation rates in air than picosecond pulses, in PLAL this is reversed due to the nonlinear energy losses in the liquid. However, thanks to the incorporation of SSTF, the energy delivered to the target is increased up to 70%, which leads to a nanoparticle production increase of a 2.4 factor. This breaks a barrier toward the employment of femtosecond lasers in high-efficiency PLAL.
Taking advantage of the dispersive Fourier transformation technique, the decaying evolution processes of double-pulse mode-locking in a single-walled carbon-nanotube-based Er-doped fiber laser are observed in detail for the first time to our knowledge. The decaying dynamics of the double-pulse mode-locking state is analyzed in the spectral and temporal domains. We reveal that the two pulses in one cluster disappear either simultaneously or one by one during the decaying processes of double-pulse mode-locking states. In addition, the spectral evolution patterns of the special double-pulse states (i.e., bound states) are extremely distinct at different decline rates of the pump power.
Periodic surface structures were fabricated by irradiating lithium niobate (LN) crystals with femtosecond laser pulses at sample temperatures ranging from 28°C to 800°C. Carrier density and conductivity of the samples were increased via heating LN, which inhibited coulomb explosion to obtain a uniform periodic surface structure. The periodic surface structures cover an area of 8 mm×8 mm and have an average spacing of 174±5 nm. Meanwhile, the absorption of the processed sample is about 70% in the spectral range of 400–1000 nm, which is one order of magnitude higher than that of pure LN. Fabrication of periodic surface structures on heating LN with femtosecond laser pulses provides a possibility to generate nanogratings or nanostructures on wide-bandgap transparent crystals.
Perovskite nanocrystals (NCs) have strong nonlinear optical responses with a number of potential applications, ranging from upconverted blue-lasing to the tagging of specific cellular components in multicolor fluorescence microscopy. Here, we determine the one-photon linear absorption cross section of two kinds of blue-emitting perovskite NCs, i.e., CsPbCl3 and CsPb(Cl0.53Br0.47)3, by utilizing femtosecond transient absorption spectroscopy. The wavelength-dependent nonlinear refraction and two-photon absorption have been measured at wavelengths from 620 to 720 nm by performing Z-scan measurements. The nonlinear optical responses of CsPb(Cl0.53Br0.47)3 are much more pronounced than those of CsPbCl3 due to the larger structural destabilization of the former.
The role of chirp on the light–matter interaction of femto- and pico-second laser pulses with functional structured surfaces is studied using drag-reducing riblets as an example. The three-dimensional, periodic microstructure naturally gives rise to a mutual interplay of (i) reflection, (ii) scattering, and (iii) diffraction phenomena of incident coherent light. Furthermore, for femtosecond pulses, the structure induces (iv) an optical delay equivalent to a consecutive temporal delay of 230 fs in places of the pulse. These features enable studying experimentally and numerically the effect of tuning both pulse duration τ and spectral bandwidth Δω on the features of the wide-angle scattering pattern from the riblet structure. As a result, we discovered a significant breakdown of fringes in the scattering pattern with decreasing pulse duration and/or increasing spectral bandwidth. This unique type of chirp control is straightforwardly explained and verified by numerical modeling considering the spectral and temporal interaction between different segments within the scattered, linearly chirped pulse and the particular geometric features of the riblet structure. The visibility of the fringe pattern can be precisely adjusted, and the off-state is achieved using τ<230 fs or Δω>2.85×1013 rad/s.
We demonstrate the suppression of soft X-ray high harmonics generated by two-color laser pulses interacting with Ne gas in a gas cell. We show that harmonic suppression can occur at the proper combination of the propagation distance and gas pressure. The physical mechanism behind is the phase mismatch between “short”-trajectory harmonics generated at the early and later times through the interplay of geometric phase, dispersion, and plasma effects. In addition, we demonstrate that the position and depth of harmonic suppression can be tuned by increasing the gas pressure. Furthermore, the suppression can be extended to other laser focusing configurations by properly scaling macroscopic parameters. Our investigation reveals a simple and novel experimental scheme purely relying on the phase mismatch for selectively controlling soft X-ray tabletop light sources without adopting the filters for applications.
In this work, it has been demonstrated that in order to fully understand the terahertz (THz) pulse generation process during femtosecond laser filamentation, the interaction between THz wave and air plasma has to be taken into account. This interaction is mainly associated with the spatial confinement of the THz pulse by the plasma column, which could be described by the one-dimensional negative dielectric (1DND) waveguide model. By combining the 1DND model with the conventional four-wave mixing (4WM) and photocurrent (PC) models, the variation of THz spectral amplitude and width obtained in experiments could be better understood. Finally, a three-step procedure, with 1DND bridging 4WM and PC processes, has been established for the first time to describe the underlying mechanism of THz radiation from plasma sources.
To seek high signal-to-noise ratio (SNR) is critical but challenging for single-shot intense terahertz (THz) coherent detection. This paper presents an improved common-path spectral interferometer for single-shot THz detection with a single chirped pulse as the probe for THz electro-optic (EO) sampling. Here, the spectral interference occurs between the two orthogonal polarization components with a required relative time delay generated with only a birefringent plate after the EO sensor. Our experiments show that this interferometer can effectively suppress the noise usually suffered in a non-common-path interferometer. The measured single-shot SNR is up to 88.85, and the measured THz waveforms are independent of the orientation of the used ZnTe EO sensor, so it is easy to operate and the results are more reliable. These features mean that the interferometer is quite qualified for applications where strong THz pulses, usually with single-shot or low repetition rate, are indispensable.
The ability to manipulate the valence state conversion of rare-earth ions is crucial for their applications in color displays, optoelectronic devices, laser sources, and optical memory. The conventional femtosecond laser pulse has been shown to be a well-established tool for realizing the valence state conversion of rare-earth ions, although the valence state conversion efficiency is relatively low. Here, we first propose a femtosecond laser pulse shaping technique for improving the valence state conversion efficiency of rare-earth ions. Our experimental results demonstrate that the photoreduction efficiency from Sm3+ to Sm2+ in Sm3+-doped sodium aluminoborate glass using a π phase step modulation can be comparable to that using a transform-limited femtosecond laser field, while the peak laser intensity is decreased by about 63%, which is very beneficial for improving the valence state conversion efficiency under the laser-induced damage threshold of the glass sample. Furthermore, we also theoretically develop a (2+1) resonance-mediated three-photon absorption model to explain the modulation of the photoreduction efficiency from Sm3+ to Sm2+ under the π-shaped femtosecond laser field.
The principle of optical trapping is conventionally based on the interaction of optical fields with linear-induced polarizations. However, the optical force originating from the nonlinear polarization becomes significant when nonlinear optical nanoparticles are trapped by femtosecond laser pulses. Herein we develop the time-averaged optical forces on a nonlinear optical nanoparticle using high-repetition-rate femtosecond laser pulses, based on the linear and nonlinear polarization effects. We investigate the dependence of the optical forces on the magnitudes and signs of the refractive nonlinearities. It is found that the self-focusing effect enhances the trapping ability, whereas the self-defocusing effect leads to the splitting of the potential well at the focal plane and destabilizes the optical trap. Our results show good agreement with the reported experimental observations and provide theoretical support for capturing nonlinear optical particles.
Spectral anti-crossings between the fundamental guided mode and core-wall resonances alter the dispersion in hollow-core anti-resonant-reflection photonic crystal fibers. Here we study the effect of this dispersion change on the nonlinear propagation and dynamics of ultrashort pulses. We find that it causes emission of narrow spectral peaks through a combination of four-wave mixing and dispersive wave emission. We further investigate the influence of the anti-crossings on nonlinear pulse propagation and show that their impact can be minimized by adjusting the core-wall thickness in such a way that the anti-crossings lie spectrally distant from the pump wavelength.
Extending the length of femtosecond laser filamentation has always been desired for practical applications. Here, we demonstrate that significant extending of a single filament in BK7 glass can be achieved by constructing phase-nested beams. The filamentation and the following energy replenishment are assembled in a single phase-nested beam. The central part of the phase-nested beam is an apertured Gaussian beam, which is focused into one focal spot to produce a short filament. In contrast, the rest of the annular part converges gradually towards the central axis to continuously replenish the energy for supporting the regeneration of filaments. The common-path generating system ensures the stability of generated filaments and easily optimizes the beam parameters to obtain the longest high-quality filament due to its flexibility. In addition, we discuss the significance of continuous replenishment for extending filaments and the potential for generating more extended filaments based on this method.