Ultrafast Research Articles

Ultrafast Laser Hyperdoped Black Silicon and Its Application in Photodetectors: A Review

Based on the ultrafast and extremely strong interaction between laser pulses and materials, ultrafast laser irradiation can break the solid solubility constraints and enable hyperdoping of impurities. This process overcomes the bandgap constraints of crystalline silicon, resulting in heightened absorption across a broad spectral range spanning from ultraviolet to infrared wavelengths, therefore commonly referred to as black silicon (b‐Si). The b‐Si demonstrates significant changes in optoelectronic properties, making it highly promising for applications in silicon photonics. Specifically, b‐Si photodetectors exhibit distinct advantages in terms of high photoelectric gain at low voltage, ultrabroadband spectral responsivity, large dynamic range, and suitability for operation over a wide temperature range. These properties address the limitations of traditional silicon photodetectors, showcasing great potential for applications in optoelectronic integration, artificial intelligence, information technology, energy devices, and beyond. This review focuses on b‐Si achieved through ultrafast laser processing, with a special emphasis on its applications in photodetectors. The mechanism of ultrafast laser irradiation and the properties of hyperdoped silicon are discussed. Then, the research progresses and state‐of‐the‐art b‐Si photodetectors are introduced, as well as working mechanism and potential application expansion. Finally, the development prospects of b‐Si photodetectors based on ultrafast laser hyperdoping are predicted.

Reducing wavelength jitter in white-light seeded femtosecond optical parametric chirped-pulse amplifiers

White light generation (WLG) in bulk material can be used as a versatile broadband seed source for optical parametric chirped pulse amplification (OPCPA) stages. In this case, it is beneficial to optimize the performance of the WLG seeder in combination with the subsequent OPCPA stage. Here, we characterize how small variations in the drive pulse energy affect the white light seeder performance, in particular the wavelength stability of the amplified OPCPA spectrum. To isolate the influence of drive pulse energy on the OPCPA central wavelength, we introduce a phase-sensitive amplitude measurement and carefully optimize the drive pulse focus position (at the bulk) to minimize the sensitivity to the jitter of the drive pulse energy. With additional active stabilization of the delay between pump and seed pulses in the OPCPA, we achieve a central wavelength jitter of 2 × 10−4. With this performance, our source is an ideal front-end for applications in laser-plasma acceleration or free-electron laser seeding.

Nanophotonics with Plasmonic Nanorod Metamaterials

AbstractTaking advantage of their unique and tuneable electromagnetic properties, plasmonic metamaterials constitute a versatile platform for a variety of applications ranging from high‐resolution imaging, sensing and spontaneous emission engineering to ultrafast nonlinear optics and light polarization control. Here, recent advances in the design and applications of plasmonic metamaterials based on aligned metallic nanorod assemblies are reviewed, and the fast‐developing trends in their exploitation in nanophotonics are outlined. The fabrication of the nanorod‐based metamaterials is introduced and their linear and nonlinear optical properties are presented from both microscopic and phenomenological considerations. Multiscale structuring allowing precise engineering of the electromagnetic modes supported by the nanorod metamaterials, as well as nonlocal spatial dispersion effects and their impact on nanophotonic performance are discussed. To illustrate the developing field of practical applications of these metamaterials, some of their main application domains in sensing, photochemistry and nonlinear optics are overviewed and novel designs of anisotropic metamaterials directly derived from the nanorod architecture are introduced.

Ultrafast supercontinuum sculpting for two-photon spectroscopy and microscopy of ratiometric fluorescent indicators

We present a compact laser system for quantitative two-photon excitation spectra measurements and ratiometric two-photon imaging of fluorescent protein indicators. The fundamental of the system is a short segment of photonic crystal fiber (PCF), which supports a nonlinear transformation of low-power ultrashort pulses by preserving temporal coherence, and this generates an ultrafast almost octave-spanning supercontinuum (SC). Accurate sculpting of the SC by its amplitude and phase modulation provides implementation of the spectroscopic and microscopic modalities. The spectroscopic one was exhibited by two-photon action cross section spectra measuring for the genetically encoded fluorescent sensing proteins of the vital biochemical parameters: acidity (SypHer3s), concentration of hydrogen peroxide (HyPer3 and HyPer7), redox status of NADH and glutathione (RexYFP and Grx1-roGFP2), hypohalous acids and their derivatives (Hypocrates). For the microscopy, we investigated and optimized the intensity pump pulse profiles under the high numerical objective by dispersion scan technique. We conducted real-time monitoring of the dynamics of hydrogen peroxide in HeLa cells with subcellular spatial resolution by means of ratiometric two-photon imaging of Hyper7 sensors. The presented hybrid laser system provides an ideal optical toolbox in order to develop ratiometric fluorescent sensors, which can be visualized in vivo using two-photon microscopy.

Transmission of soliton for a coupled Radhakrishnan–Kundu–Lakshmanan equation in an optical fiber using the Jacobi elliptical sn function method

We examine a coupled Radhakrishnan–Kundu–Lakshmanan (cRKL) equation that includes self-phase modulation, third order dispersion, self-steepening, and cross-phase modulation effects. A propagating ultrafast pulse in nonlinear systems is described by the given equation. Utilizing the coupled Radhakrishnan–Kundu–Lakshmanan (cRKL) model, we explored the dynamics of various innovative optical solitons, such as wing-shaped, W-shaped, and brilliant solitons. We used mathematical methods like the Jacobi elliptical sn function method to get the exact analytical solution. Our results demonstrate that the self-phase modulation (SPM), self-steepening (SS), cross-phase modulation (XPM), and third order dispersion (TOD) can be effectively varied to influence the structure of the solitons. It is demonstrated that the precise balance between the self-steepening effect, the self-phase modulation, and the group velocity dispersion forms these novel W-shaped chirp-free dark solitons and dark and bright solitonic structures. By choosing appropriate settings for the physical variables, it is possible to create a graphic representation of the properties of optical solitons. The study and application of nonlinear materials with third order dispersion, cross-phase modulation, self-phase modulation effect, and self-steepening nonlinearity may take new paths as a result of our findings.

Spectroscopy of phononic switching of magnetization in the terahertz gap

All-optical schemes for switching magnetization offer a pathway towards the creation of more advanced data-storage technologies, both in terms of recording speed and energy-efficiency. It has previously been shown that picosecond-long optical pulses with central frequencies ranging between 12 and 30 THz are capable of driving magnetic switching in yttrium-iron-garnet films, provided that the excitation frequency matches the characteristic frequency of longitudinal optical phonons. Here, we explore how the phononic mechanism of magnetic switching in three distinct ferrimagnetic iron-garnet films evolves at optical frequencies below 10 THz, within the so-called terahertz gap. We find that at long wavelengths the magnetic switching rather correlates with phonon modes associated with the substrate. Our results show that the process of phononic switching of magnetization, previously discovered in the mid- to far-infrared spectral range, becomes much more complex at frequencies within the terahertz gap.

Accurate optical dispersion identification for linear deformable mirror with spatial-spectral interferometry

In ultrashort laser pulse systems, optical dispersion can cause severe distortion of the spectral phase and thus significantly affect the pulse shape. To address this problem, this study places a linear deformable mirror (LDM) at the Fourier plane of a blazed grating for dispersion control, and reconstructs the spectral phase modulated by the LDM using single-shot spatial-spectral interferometry. An iterative algorithm and closed-loop optimization process are used to drive the LDM to generate orthogonal modes of Legendre polynomials with a signal-to-background ratio (SBR) of more than 10 dB. The identified LDM modes are then used as the basis for spectral phase modulation. It is shown that the group delay dispersion (GDD), third order dispersion (TOD), fourth order dispersion (FOD), and fifth order dispersion (5OD) can be accurately obtained by the linear combination of identified Legendre modes. In addition, the maximum phase error between the generated and target dispersions is less than 0.15 rad, while the error between the pulse widths produced by the generated dispersion and the target dispersion, respectively, is less than 3.5 %. Overall, the results confirm that the linear superposition of the generated Legendre modes enables the accurate dispersion modulation of ultrashort laser pulses.

Soliton generation and conservation laws for vector light pulses propagating in weakly birefringent waveguides

The principal algebra Lp of coupled nonlinear Schrödinger equations describing the propagation of polarized optical pulses and involving four-wave mixing terms is obtained in terms of the three arbitrary labelling parameters of the system of equations. This algebra is found to be five-dimensional, indicating the richness in symmetries of the system. The most general symmetry group transformation by generators of Lp is found and it is shown that this transformation preserves the boundedness of solutions, and an example of transformation of a soliton solution into a completely new soliton of a different type is presented. Moreover, it is explained how an infinite sequence of bounded solutions can thus be generated, yielding new solitons. Several other important properties of solutions and symmetry group transformations of the system are also demonstrated. As the system of Schrödinger equations under study turns out to be of Lagrange type, conservation laws associated with all variational symmetries of Lp are constructed and interpreted. Some symmetry reductions of the system are also derived.

Microstructured large-area photoconductive terahertz emitters driven at high average power

Emitters based on photoconductive materials excited by ultrafast lasers are well-established and popular devices for THz generation. However, so far, these emitters – both photoconductive antennas and large area emitters - were mostly explored using driving lasers with moderate average powers (either fiber lasers with up to hundreds of milliwatts or Ti:Sapphire systems up to few watts). In this paper, we explore the use of high-power, MHz repetition rate Ytterbium (Yb) based oscillator for THz emission using a microstructured large-area photoconductive emitter, consist of semi-insulating GaAs with a 10 × 10 mm2 active area. As a driving source, we use a frequency-doubled home-built high average power ultrafast Yb-oscillator, delivering 22 W of average power, 115 fs pulses with 91 MHz repetition rate at a central wavelength of 516 nm. When applying 9 W of average power (after an optical chopper with a duty cycle of 50%) on the structure without optimized heatsinking, we obtain 65 µW THz average power, 4 THz bandwidth; furthermore, we safely apply up to 18 W of power on the structure without observing damage. We investigate the impact of excitation power, bias voltage, optical fluence, and their interplay on the emitter performance and explore in detail the sources of thermal load originating from electrical and optical power. Optical power is found to have a more critical impact on large area photoconductive emitter saturation than electrical power, thus optimized heatsinking will allow us to improve the conversion efficiency in the near future towards much higher emitter power. This work paves the way towards achieving hundreds of MHz or even GHz repetition rates, high-power THz sources based on photoconductive emitters, that are of great interest for example for future THz imaging applications.

On the analysis of optical pulses to the fractional extended nonlinear system with mechanism of third-order dispersion arising in fiber optics

On the analysis of optical pulses to the fractional extended nonlinear system with mechanism of third-order dispersion arising in fiber optics

Dynamic convergent shock compression initiated by return current in high-intensity laser–solid interactions

We investigate the dynamics of convergent shock compression in solid cylindrical targets irradiated by an ultrafast relativistic laser pulse. Our particle-in-cell simulations and coupled hydrodynamic simulations reveal that the compression process is initiated by both magnetic pressure and surface ablation associated with a strong transient surface return current with density of the order of 1017 A/m2 and lifetime of 100 fs. The results show that the dominant compression mechanism is governed by the plasma β, i.e., the ratio of thermal pressure to magnetic pressure. For targets with small radius and low atomic number Z, the magnetic pressure is the dominant shock compression mechanism. According to a scaling law, as the target radius and Z increase, the surface ablation pressure becomes the main mechanism generating convergent shocks. Furthermore, an indirect experimental indication of shocked hydrogen compression is provided by optical shadowgraphy measurements of the evolution of the plasma expansion diameter. The results presented here provide a novel basis for the generation of extremely high pressures exceeding Gbar (100 TPa) to enable the investigation of high-pressure physics using femtosecond J-level laser pulses, offering an alternative to nanosecond kJ-laser pulse-driven and pulsed power Z-pinch compression methods.

Construction of microstructures on the Cu substrate using ultrafast laser processing to enhance the bonding strength of sintered Ag nanoparticles

Silver nanoparticle (Ag NP) pastes become a potential die-attachment material with the increased electronic power density. However, the weakness of bonding interface between sintered Ag NPs and bare Cu substrate limits the applications of the Ag NPs paste, thereby reducing the shear strength of the sintered joint. In this work, ultrafast laser processing is utilized to enhance the bonding strength of the sintered Ag joint by fabricating a microstructure interface. The microstructure dimensions are tunable by controlling laser parameters, and then high-strength joints could be obtained. Different substrate microstructures were constructed, and the enhanced bonding mechanism was analyzed by characterizing the cross section and fracture surface morphologies of joints. The ultrafast laser processing could increase the surface energy of Cu substrates to form a more reliable connection with Ag NPs and more energy required for crack extension with the increasing connection area, thereby resulting in a significant improvement in the shear strength of the Ag NP joints. The patterned microstructures on the Cu substrate using this technique showed improved surface energy and increased number of connection areas on the substrate, showing potential for the use in third-generation semiconductors for highly reliable packaging.

Stochastic circular persistent currents of exciton polaritons

We monitor the orbital degree of freedom of exciton-polariton condensates confined within an optical trap and unveil the stochastic switching of persistent annular polariton currents under pulse-periodic excitation. Within an elliptical trap, the low-lying in energy polariton current states manifest as a two-petaled density distribution with a swirling phase. In the stochastic regime, the density distribution, averaged over multiple excitation pulses, becomes homogenized in the azimuthal direction. Meanwhile, the weighted phase, extracted from interference experiments, exhibits two compensatory jumps when varied around the center of the trap. Introducing a supplemental control optical pulse to break the reciprocity of the system enables the transition from a stochastic to a deterministic regime, allowing for controlled polariton circulation direction.

Precise mode control of laser-written waveguides for broadband, low-dispersion 3D integrated optics

Three-dimensional (3D) glass chips are promising waveguide platforms for building hybrid 3D photonic circuits due to their 3D topological capabilities, large transparent windows, and low coupling dispersion. At present, the key challenge in scaling down a benchtop optical system to a glass chip is the lack of precise methods for controlling the mode field and optical coupling of 3D waveguide circuits. Here, we propose an overlap-controlled multi-scan (OCMS) method based on laser-direct lithography that allows customizing the refractive index profile of 3D waveguides with high spatial precision in a variety of glasses. On the basis of this method, we achieve variable mode-field distribution, robust and broadband coupling, and thereby demonstrate dispersionless LP21-mode conversion of supercontinuum pulses with the largest deviation of <0.1 dB in coupling ratios on 210 nm broadband. This approach provides a route to achieve ultra-broadband and low-dispersion coupling in 3D photonic circuits, with overwhelming advantages over conventional planar waveguide-optic platforms for on-chip transmission and manipulation of ultrashort laser pulses and broadband supercontinuum.

Improving zirconia ceramics grinding surface integrity through innovative laser bionic surface texturing

Zirconia ceramics have become an important material for the manufacture of key components in aerospace, military, energy, and other fields due to their excellent mechanical properties. However, their inherent high hardness and brittleness make them difficult to machine with high efficiency and low damage, resulting in poor surface integrity. Inspired by the ribbed groove structure of shark skin and the fractal structure of insect wing veins, two zirconia ceramics with different bionic textures are designed in this paper, and zirconia ceramic surfaces are bionically textured by using an ultrafast picosecond pulse laser. The effects of the special bionic textures on the grinding behavior of zirconia ceramics, specifically surface morphology, surface roughness, edge morphology, and subsurface damage, were investigated. The experimental results show that the surface integrity of the bionic textured zirconia ceramics is better compared to the untextured surface. In particular, the bionic insect wing veins texture exhibits the best surface quality with the least sub-surface damage, and the surface roughness Sa is reduced by a maximum of 21.46 %, and Sz is reduced by a maximum of 18.87 %. However, the best edge morphology is exhibited by the bionic shark skin texture. Additionally, bionic texturing improves grinding lubrication and cooling conditions. The results confirm that applying bionic texturing to zirconia ceramics effectively enhances grinding performance and improves grinding surface integrity.

Highly efficient nonlinear compression of mJ pulses at 2 μm wavelength to 20 fs in a gas-filled multi-pass cell

Within this work we demonstrate the highly efficient nonlinear spectral broadening and subsequent temporal compression of 1.49 mJ pulses at 101 kHz repetition rate from an ultrafast thulium-doped fiber laser system employing a gas-filled multi-pass cell (MPC). To achieve spectral broadening, we use a krypton and helium-filled Herriott-type MPC with highly reflective broadband dielectric mirrors. The spectrally broadened pulses are subsequently compressed using fused-silica plates, resulting in a pulse duration of 20 fs and an overall excellent transmission of 96%. Furthermore, the beam quality is preserved up to the maximum output power of 144 W. It provides, to the best of our knowledge, the highest average power with few-cycle pulses at 2 µm wavelength with almost 10 times more pulse energy and 3 times more average power than previous 2 µm MPCs, enabling future secondary source experiments.

New Insights into Photo-Fenton Chemistry: The Overlooked Role of Excited IronIII Species.

Direct photoreduction of FeIII is a widely recognized route for accelerating FeIII/FeII cycle in photo-Fenton chemistry. However, most of the wavelengths covering the full spectral range are insufficient to supply enough photon energy for the direct reduction process. Herein, the hitherto neglected mechanism of FeIII reduction that the FeIII indirect reduction pathway initiated by light energy-dependent reactivity variation and reactive excited state (ES) was explored. Evolution of excited-state FeIII species (*FeIII) resulting from metal-centered charge excitation (MCCE) of FeIII is experimentally verified using pulsed laser femtosecond transient absorption spectroscopy with UV-vis detection and theoretically verified by quantum chemical calculation. Intense photoinduced intravalence charge transition was observed at λ = 380 and 466 nm, revealing quartet 4MCCE and doublet 2MCCE and their exponential processes. Light energy-dependent variation of *FeIII reactivity was kinetically certified by fitting the apparent rate constant of the radical-chain sequence of photo-Fenton reactions. Covalency is found to compensate for the intravalence charge separation following photoexcitation of the metal center in the MCCE state of Fenton photosensitizer. The *FeIII is established as a model, demonstrating the intravalence hole delocalization in the ES can be leveraged for photo-Fenton reaction or other photocatalytic schemes based on electron transfer chemistry.

Current Oscillations and Resonances in Nanocrystals of Narrow-gap Semiconductors

In single colloidal nanocrystals of narrow-gap semiconductors PbS and InSb, current instability in the form of quasi-periodic spikes and current resonance peaks was studied by measuring on a scanning probe microscope and analyzing Current-Voltage Characteristics (CVC). The observed phenomena are explained in models of the wave de Broglie process and Bloch oscillations. Statistically, the percentages of such samples and the parameters of oscillations on the current-voltage characteristic are higher, the larger the size quantization parameter, determined by the de Broglie wavelength. A possible practical use is the generation and recording of terahertz radiation modulated by ultrashort pulses.

Memristive Control of Plasmon-Mediated Nonlinear Photoluminescence in Au Nanowires.

Nonlinear photoluminescence (N-PL) is a broadband photon emission arising from a nonequilibrium heated electron distribution generated at the surface of metallic nanostructures by ultrafast pulsed laser illumination. N-PL is sensitive to surface morphology, local electromagnetic field strength, and electronic band structure, making it relevant to probe optically excited nanoscale plasmonic systems. It also has been key to accessing the complex multiscale time dynamics ruling electron thermalization. Here, we show that plasmon-mediated N-PL emitted by a gold nanowire can be modified by an electrical architecture featuring a nanogap. Upon voltage activation, we observe that N-PL becomes dependent on the electrical transport dynamics and can thus be locally modulated. This finding brings an electrical leverage to externally control the photoluminescence generated from metal nanostructures and constitutes an asset for the development of emerging nanoscale interface devices managing photons and electrons.

Encoding control system for twin-field quantum key distribution

The Twin-Field Quantum Key Distribution (TF-QKD) protocol has the potential to realize secure key distribution over extremely long distances, which is an important technique for realizing a global quantum network. Compared to the conventional BB84 protocol, practical TF-QKD and its variant protocols require an accurate phase modulation to at least 16 different values with randomized encoding. In this work, we developed an encoding control system for TF-QKD. Optical pulses with five different intensities and 16 different phases can be modulated with a clock frequency of 100 MHz with a field programmable gate array based arbitrary waveform generator (AWG). With the assistance of DDR4 memory, waveforms exceeding 200 ms in length can be output simultaneously on 4 pairs of differential channels, making the random number pairing between two different encoding systems close to the expected ratio when using cyclic random numbers for experimental demonstration. The AWG boasts a long-term amplitude stability better than 0.03% and supports seamless concatenation and cyclic output of waveforms, demonstrating a strong and sustained performance in long-duration experiments. Sending-or-not-sending TF-QKD was demonstrated with the encoding control system, with a secure key rate of 1.33 × 10−5 per pulse under the total channel loss of ∼32 dB.