Ultrashort Laser Pulses Research Articles

Characterizing post-compression of mJ-level ultrafast pulses via loose focusing in a gas cell

The ability to generate high-intensity ultrashort laser pulses is a key driver for advancing the strong-field physics and its applications. Post-compression methods aim to increase the peak intensity of amplified laser pulses via spectral broadening through self-phase modulation (SPM), followed by temporal pulse compression. However, other unavoidable nonlinear self-action effects, which typically occur parallel to SPM, can lead to phase distortions and beam quality degradation. Here we study the ability to compress high-energy pulses by loose focusing in a noble gas to induce nonlinear spectral broadening, while limiting unwanted nonlinear effects such as self-focusing. We introduce ptychographic wavefront sensor and FROG measurements to identify the regimes that optimize pulse compression while maintaining high beam quality. Using a 700 mbar argon-filled double-pass-based scheme, we successfully compress 2 mJ, 170 fs, 1030 nm laser pulses to ∼35 fs, achieving 90% overall flux efficiency and excellent stability. This work provides guidelines for optimizing the compressed pulse quality and further energy scaling of double-pass-based post-compression concepts.

Photodiode-based focus monitoring in ultrashort-pulsed laser structuring of graphite anodes for lithium-ion batteries

In recent years, there has been an increased demand for elaborate monitoring techniques in laser material processing. This has been driven by the need for fast and cost-efficient quality assurance processes. At the same time, ultrashort-pulsed (USP) laser radiation has emerged as a promising technology for creating intricate microstructures in lithium-ion battery graphite anodes due to its high precision and negligible thermal impact. However, the integration of process monitoring in USP laser applications for graphite anode structuring is still unexplored. There is a lack of clarity on suitable sensors, observable parameters, and extractable process-relevant insights. The presented study addressed this gap by demonstrating the capability of state-of-the-art photodiode-based monitoring systems in collecting process-relevant data and deriving valuable insights. A sensor equipped with three photodiodes was employed to address these challenges. Exploratory data analysis and machine learning methodologies were leveraged to develop a data pipeline for processing the acquired information. The data were used to train convolutional neural networks that could accurately predict the focal position. At the same time, the limitations of traditional regression approaches could be shown. The findings advanced the understanding of the possibilities of process monitoring in USP laser applications and emphasized the significance of data-driven approaches in optimizing manufacturing processes.

Solid and hollow plasmonic nanoresonators for carrier envelope phase read-out

The geometry of gold plasmonic nanoantennae was numerically optimized to maximize their sensitivity to the carrier envelope phase (CEP) of the exciting ultra-short laser pulses. Three structure types, triangular, teardrop-shaped and plasmonic lens, were optimized in solid and hollow compositions as well. Hollow / solid singlets results in the largest/intermediate CEP dependent (Q1) – to – CEP independent (Q0) integrated current components’ ratio, while their Q1 was the smallest / intermediate. The largest / intermediate Q12/Q0 CEP sensitivity was achieved via solid / hollow plasmonic lenses due to their large near-field enhancement and Q1, while the Q1/Q0 ratio was smaller than for counterpart singlets.

Single-shot ultrafast imaging of plasma dynamics induced by dual-angle ultrashort laser pulses with subpicosecond delay

Abstract Spatiotemporal manipulation of ultrashort laser pulses is crucial for enhancing laser processing and phonon generation. Optimization of these applications requires ultrafast visualization of the underlying processes. In this study, we induced laser ablation using spatiotemporally manipulated double pulses focused from two angles onto a glass surface with a 0.7 ps interval, and captured the images of its dynamics with 5 sequential frames at a frame interval of 0.8 ps. The observed dynamics suggest that the laser profile reflected on the glass surface is influenced by its topography, which in turn affects the behavior of air breakdown plasmas.

Nonlinear optical research on 2D NbSe2 nanosheets and their ultrafast photonics applications

Two-dimensional (2D) NbSe2 is a new material with a variety of excellent properties. In this article, 2D NbSe2 nanosheets are prepared using liquid phase exfoliation (LPE) and spin coating methods. At the same time, the properties of NbSe2 were calculated by using density functional theory (DFT), exploring the changes in the electronic band structure of NbSe2 with the number of layers, and studying the optical properties of NbSe2. The nonlinear optical properties caused by the Pauli blocking effect and the absorption spectra are studied through typical nonlinear testing techniques and an ultraviolet–visible-near-infrared (UV–VIS-IR) spectrophotometer. In addition, 2 µm solid-state pulse lasers have important applications in a variety of fields. For the first time, 2D NbSe2 nanosheets are prepared as saturable absorbers (SA) and applied them to solid-state lasers as nonlinear optical modulation devices, successfully achieving the generation of ultra-short pulse lasers with a pulse duration of 445.4 ps in 2 µm band. Our research results prove that 2D NbSe2 nanosheets is a promising nanomaterial, can be prepared into nonlinear optical modulation devices with excellent performance, and show great application potential as ultrafast photonic devices. It is beneficial to the miniaturization of solid-state pulse lasers in subsequent applications.

Phonon-Induced Geometric Chirality.

Chiral properties have seen increasing use in recent years, leading to the emerging fields of chiral quantum optics, plasmonics, and phononics. While these fields have achieved manipulation of the chirality of light and lattice vibrations, controlling the chirality of materials on demand has yet remained elusive. Here, we demonstrate that linearly polarized phonons can be used to induce geometric chirality in achiral crystals when excited with an ultrashort laser pulse. We show that nonlinear phonon coupling quasistatically displaces the crystal structure along phonon modes that reduce the symmetry of the lattice to that of a chiral point group corresponding to a chiral crystal. By reorienting the polarization of the laser pulse, the two enantiomers can be induced selectively. Therefore, geometric chiral phonons enable the light-induced creation of chiral crystal structures and therefore the engineering of chiral electronic states and optical properties.

Photodiode-based process monitoring for the ultrashort-pulsed laser structuring of the diffusion media for fuel cells

In recent years, the incorporation of process monitoring systems has become an integral part across several laser material processing applications. This is due to the feasibility of inline evaluations, which enable the elimination of downstream quality checks that are typically time-consuming and costly. Simultaneous to recent sensor developments, ultrashort-pulsed (USP) laser material processing has become a promising technology for creating complex microstructures in a wide variety of materials due to its high precision and negligible thermal input. So far, process monitoring has yet to be established in USP applications as it is unknown which sensors are suitable, which parameters can be observed, and which process-relevant information can be detected within the data. Within this work, a state-of-the-art photodiode-based process monitoring system was used to collect spectral data from the process zone and extract relevant information from the process. The laser structuring of the two-layered diffusion media used in polymer electrolyte membrane fuel cells was selected as the use case. This structuring process is challenging due to production-related fluctuations in the material thickness and the surface quality. Within this study, information was acquired from a sensor system employing three photodiodes. Through the application of explorative data analysis techniques and machine learning, AI models were created, focusing on determining the focus position of the laser beam and identifying the transition between the two layers. The developed models were capable of determining the initial focus position with varying accuracies. The best performance was achieved by a convolutional neural network using spectrograms as input data, while the worst accuracy was achieved by a ridge regression model using manually selected features. Furthermore, a clustering model was used, demonstrating the capability to detect the layer transitions within a specified tolerance.

Understanding Selectivity in Product Distributions from Laser Ablation of Organic Liquids.

Pulsed laser ablation in organic solvents is widely used to produce oxide-free metal and metal carbide nanoparticles, often with carbon coatings resulting from laser-induced reactions in the organic solvent. To gain insight into how the molecular structure of the solvent affects these reaction pathways, this work investigates ablation of the C6H14 isomers n-hexane, 2-methylpentane, and 3-methylpentane through characterization of the gas and liquid products with mass spectrometry. Ablation of each C6H14 isomer produces a distinct distribution of product molecular weights and isomers. 2-methylpentane preferentially produces C3 and C9, whereas 3-methylpentane produces C2, C4, C8, and C10 products. These preferential product distributions, along with the lack of such selectivity in n-hexane, arise from differences in the most favorable C-C bond scission pathways in each C6H14 isomer. Moreover, the particular isomers of C8H18, C9H20, C10H22, and C12H26 produced by ablation of each C6H14 isomer indicate that the vast majority of reaction pathways involve addition reactions between a fragment radical and parent C6H14 or between two C6H14 molecules, without molecular rearrangement. This propensity toward direct addition suggests that the chemical reactions induced by ultrashort pulsed laser ablation proceed on faster time scales than those of radical rearrangements.

Review of high-precision femtosecond laser materials processing for fabricating microstructures: Effects of laser parameters on processing quality, ablation efficiency, and microhole shape

Femtosecond lasers are promising tools for achieving high-precision processing of thin materials without causing any thermal surface damage and bulk distortion. However, thermal damage can occur even with ultrashort laser pulses. This is because of high electron penetration depth and heat accumulation at high fluence and high repetition rate. Nanoparticle redeposition can be dramatically altered with variation in repetition rate. The symmetry of microholes and ablation efficiency vary with laser polarization. The laser wavelength affects the ablation efficiency and surface roughness. Therefore, understanding these laser–matter interactions that depend on the laser parameters is essential for high-precision laser processing. This article reviews laser–matter interactions in the 64FeNi alloy, as well as analytical models for designing the desired hole size and taper angles. This can help establish strategies for creating various high-precision microstructures using femtosecond lasers.

Quantum theory of the spin dynamics excited by ultrashort THz laser pulses in rare earth antiferromagnets. DyFeO3

A quantum theory of spin dynamics in the rare-earth orthoferrites excited by terahertz laser pulses is developed. The study demonstrates that dynamic magnetic configurations, triggered by a light pulse, exhibit stability even after the excitation source is ceased. The magnitude of post-excitation oscillations is linked to the ratio between the frequency of rare-earth ion excitations and the frequency of the external source. According to the analysis presented, dynamic response is significantly amplified when the system is exposed to ultrashort terahertz pulses. The physical characteristics of the oscillations emerging after the pulse are determined, and the factors governing their amplitude and phase are identified. The response signal is found to be dependent on the initial part of the pulse, specifically the half-period of the ultrashort light wave, while the subsequent part of the pulse contributes minimally to post-pulse magnetization dynamics. The findings highlight that in DyFeO3, terahertz dynamics primarily result from the influence of the magnetic field of the light, leading to excitations of electrons from the ground state to low-lying electronic levels of Dy3+ions. Additionally, the dynamic magnetoelectric effect excited by the electric field of the pulse is explored, revealing the emergence of odd magnetic modes.

Passively mode-locking fiber laser based on Cr2Si2Te6 saturable absorber

This paper reports on the generation of third-order harmonic mode-locking, double-pulse phenomena, and conventional solitons in an erbium-doped fiber laser using Cr2Si2Te6 as a saturable absorber (SA). The double-balance probing method was employed to examine the nonlinear characteristics of Cr2Si2Te6-SA. Its modulation depth is 2.35 %, and its saturation intensity is 29.74 MW/cm2. We discovered conventional soliton functioning with a center wavelength of 1561.8 nm at a pump power of 34.76 mW. It has a repetition frequency of 6.76 MHz and a signal-to-noise ratio of 45 dB. As the pump power increased, the traditional soliton was able to maintain its existence in the range of 34.76 mW to 80.96 mW. The maximum output power reaches 1.1 mW when the pump power is 80.96 mW, and the maximum single-pulse energy of the conventional soliton is 0.16 nJ. Furthermore, we observed third-order harmonic mode-locking and double-pulse phenomena at pump outputs of 53.65 mW and 71.16 mW. The experimental findings demonstrate the excellent nonlinear effect of the SA based on Cr2Si2Te6. In ultrashort-pulse fiber lasers, Cr2Si2Te6 nanosheets can be employed as an efficient saturable absorption material.

Scaling of ultrashort-pulsed laser structuring processes for electromobility applications using a spatial light modulator

The structuring of lithium-ion battery (LIB) electrodes and the diffusion media (DM) for polymer electrolyte membrane fuel cells (PEMFCs) with ultrashort laser pulses enables improved performance characteristics of both technologies. However, the transfer of the approaches from a laboratory scale to a commercial use has previously been hindered by the low average output power of ultrashort-pulsed (USP) laser beam sources and the limited productivity of single-beam structuring using scanning optics. Recent advancements in the development of USP laser systems have led to a steady increase in the available output power, thereby enabling new fields of applications. This study aims at accelerating the USP laser structuring of LIB electrodes and DM for PEMFCs to industrially relevant processing rates by comparing a single-beam with a multibeam structuring process regarding ablation characteristics and quality. For the multibeam strategy, the shape of the laser beam was modified by a spatial light modulator (SLM). In addition to microholes, the insertion of microchannels was investigated to demonstrate the high flexibility of state-of-the-art SLMs. The geometry of the created structures was measured with a laser scanning microscope, and the different layers were tested for their geometrical and electrochemical properties to compare both technologies. The results confirmed that applying an SLM enables high-quality microstructures with significantly higher structuring rates. Furthermore, this contribution includes a theoretical analysis of the specifications required for a laser setup to reach an industrially relevant productivity of the structuring processes.

All-Optical Control of Bubble and Skyrmion Breathing.

Controlling the dynamics of topologically protected spin objects by all-optical means promises enormous potential for future spintronic applications. Excitation of bubbles and skyrmions in ferrimagnetic [Fe(0.35 nm)/Gd(0.40 nm)]_{160} multilayers by ultrashort laser pulses leads to a periodic modulation of the core diameter of these spin objects, the so-called breathing mode. We demonstrate versatile amplitude and phase control of this breathing using a double excitation scheme, where the observed dynamics is controlled by the excitation delay. We gain insight into both the timescale on which the breathing mode is launched and the role of the spin object size on the dynamics. Our results demonstrate that ultrafast optical excitation allows for precise tuning of the spin dynamics of trivial and nontrivial spin objects, showing a possible control strategy in device applications.

Precise Nanoparticle Manipulation Using Femtosecond Laser Trapping.

Optical tweezers use strongly focused light for trapping, characterizing, and manipulating objects in the microscopic and nanoscopic regimes. However, fully understanding optical trapping at the nanoscale remains a significant challenge. This holds importance because the nanoscale is the frontier for numerous promising advancements, ranging from enhancing single-molecule investigations in biology to developing hybrid devices for nanoelectronics and photonics and exploring fundamental quantum phenomena in opto-mechanics. We report an experimental and theoretical study of nanoparticles of various sizes, showing the advantages of the immense peak power of ultrashort laser pulses over conventional optical tweezers. We also demonstrate highly stable trapping of nanoparticles for extended durations at low average laser power using femtosecond lasers.

Numerical study of multi-phase flow in ultrashort pulse laser processing

Ultrashort pulse laser processing is highly valued due to its enormous potential for high micromachining quality while it comprises complicated physical mechanisms especially when the pulse width falls in the regime about 10 ps. This study presents a complete mathematical modeling on multi-phase phenomena in ultrashort pulse laser processing, such as melting, vaporization, and solidification. The volume of fluid (VOF) technique is used to capture the interface during phase transition. Based on this hybrid model, the transport of energy and mass are investigated to study the influence of laser parameters on the formation of laser ablation hole. This work develops the incompressible multiphase laser ablation solver based on PIMPLE algorithm. The calculation results are validated by different references under different laser processing parameters which emphasize the importance of mechanism on thermal ablation and hydrodynamics in picosecond laser processing. More calculation results about the trends in hole depth over pulse laser width, laser fluence, and the number of pulses show the intricate influence of laser parameters.

Geometrical modeling of ultrashort pulse laser ablation with redeposition and analysis of the influence of spot size and shape

Ultrashort-pulse lasers are an established technology for micromachining and have a great future. A major challenge remains the search for suitable laser parameters and a scanning strategy. To date, this has been achieved mainly by conducting experiments and measuring the resulting surfaces. The use of modeling methods for this purpose is not yet practical for industrial processing. In this work, the recently introduced geometric modeling method for pulsed laser ablation is applied to ultrashort laser ablation and extended to consider the power dependence of the process footprint and the pointing stability during ablation. This work highlights this modeling method to cover a wide range of process parameters in a time-saving manner and to simulate laser micromachining in real time. Furthermore, the influence of the processing height compared to the focal height on oxygen-free copper and steel 1.4034 was investigated. For both the ablation depth is decreased while simultaneously increasing the ablation width. For oxygen-free copper, the ablated volume is insensitive to changes in the processing height, which is not the case for steel 1.4034. The results also show the influence of the pulse repetition rate on the change in the shape of material removal and its influence on process stability.

A new method for direct welding of alumina and zirconia ceramics by ultrashort pulse laser for high temperature application

The direct welding of alumina and zirconia ceramics by ultrashort pulse laser is presented for the first time. Compared to traditional dissimilar ceramic joining techniques such as brazing and diffusion welding, this method shows various advantages, including operation at room-temperature, higher welding efficiency, and negligible impact on base materials. The joint microstructure consists of a combination of Al2O3 and ZrO2 phases, without new phases detected. By adjusting the laser focal point position, the phase content within joint is effectively regulated, successfully preventing crack formation in alumina substrate. The influence of laser power and welding speed on joint morphology and mechanical property is fully investigated. The highest four-point bending strength of 365.5MPa and shear strength of 33.4MPa are achieved. After experiencing thermal cycling test at 1000°C, the joint strength and microstructure does not exhibit significant changes, demonstrating the excellent high-temperature durability of the sample.

Flow analysis and fabrication of micro scale controlled surfaces by ultrashort pulse laser for microfluidic device applications

Microfluidics finds a wide range of industrial applications mainly in fields such as biomedical, clinical, electrical, and thermal engineering. Microchannels are the building blocks of most microfluidic devices. Thus, it becomes evident to understand the properties and the effect of the surfaces on the outcomes of devices. In this study, the effect of the shape of microchannels and the roughness elements on the flow is evaluated. Microchannels with three cross-sections and roughness elements of three different geometries are considered. The effect of varying Reynolds numbers on the flow parameters such as Friction factor, Nusselt number, Poiseuille number, pressure drop and surface temperature at the base of the substrate is studied. It is observed that rough microchannels and rectangular roughness elements showed a higher Nusselt number than smooth microchannels. The rough microchannels with triangular roughness elements showed higher friction factors. The surface temperature is higher for the smooth microchannels with triangular roughness elements. Furthermore, to demonstrate the manufacturability of microfluidic channels with controlled surfaces and to validate the preliminary results of the numerical simulations, the ultrashort pulse laser micromachining technique is used to fabricate the microchannels with structures on Polymethyl Methacrylate (PMMA) material.

Tracing the Background‐Suppressed Vibrational Decay Time of a Molecular Monolayer with Time‐Resolved Surface‐Enhanced Broadband Coherent Anti‐Stokes Raman Scattering

AbstractThe sensitivity of molecular spectroscopy based on surface‐enhanced coherent anti‐Stokes Raman scattering (SECARS) is limited by the spectrally overlapping background from nonresonant four‐wave mixing (FWM). While the SECARS signal is mediated by the molecular vibrational eigenstates and exhibits long lifetime (a few picoseconds), the FWM background stems from the instantaneous electronic polarization and decays rapidly with the vanishment of excitation. Therefore, CARS and FWM can be separated by time‐resolved CARS (trCARS) using ultrashort pulsed lasers. The broad spectral bandwidth also enables broadband CARS (BCARS) for simultaneous identification of multiple vibrational signatures. This work combines trCARS and BCARS with an optimized plasmonic system to demonstrate time‐resolved surface‐enhanced BCARS) and show its capability in obtaining background‐suppressed broadband vibrational spectra from a monolayer of 4‐Aminothiophenol (4‐ATP) molecules self‐assembled on a gold grating. The vibrational dephasing time of the ring‐breathing mode for the 4‐ATP monolayer on the gold grating (≈1.00 ± 0.17 ps) is significantly shortened compared to that for 4‐ATP powder on a glass substrate (2.10 ± 0.05 ps). This work presents an effective method to suppress FWM background and investigate the vibrational dynamics of molecules in the vicinity of plasmonic nanostructures.

Micro/nano-scale transient thermo-viscoelastic responses for 1D temperature-dependent polymer-based rod heated by the ultra-short pulse laser based on nonlocal single-phase-lag heat conduction and Eringen’s differential elasticity

Micro/nano-scale transient thermo-mechanical responses are significantly important with rapid development and applications of ultra-short pulse in micro-machining of viscoelastic structure. This work aims to establish non-Fourier thermo-viscoelastic model based on nonlocal single-phase-lag heat conduction and Eringen’s differential elasticity. The developed model is applied to study thermo-viscoelastic responses for 1D temperature-dependent polymer-based rods subjected to non-Gaussian laser pulse excitation by Kirchhoff and Laplace transformation techniques. The results reveal that the parameters of the deformation, pulse laser, and nonlocal single-phase-lag heat conduction remarkably affect the wave propagations and thermo-viscoelastic response at micro/nano-scale nanoscale.