Femtosecond Laser Irradiation Research Articles

Femtosecond Laser-Induced Recrystallized Nanotexturing for Identity Document Security With Physical Unclonable Functions.

Counterfeit identity (ID) documents pose a serious threat to personal credit and national security. As a promising candidate, optical physical unclonable functions (PUFs) offer a robust defense mechanism against counterfeits. Despite the innovations in chemically synthesized PUFs, challenges persist, including harmful chemical treatments, low yields, and incompatibility of reaction conditions with the ID document materials. More notably, surface relief nanostructures for PUFs, such as wrinkles, are still at risk of being replicated through scanning lithography or nanoimprint. Here, a femtosecond laser-induced recrystallized silicon nanotexture is reported as latent PUF nanofingerprint for document anti-counterfeiting. With femtosecond laser irradiation, nanotextures spontaneously emerge within 100ms of exposure. By introducing a low-absorption metal layer, surface plasmon polariton waves are excited on the silicon-metal multilayer nanofilms with long-range boosting, ensuring the uniqueness and non-replicability of the final nanotextures. Furthermore, the femtosecond laser induces a phase transition in the latent nanotexture from amorphous to polycrystalline state, rather than creating replicable relief wrinkles. The random nanotextures are easily identifiable through optical microscopy and Raman imaging, yet they remain undetectable by surface characterization methods such as scanning electron and atomic force microscopies. This property significantly hinders counterfeiting efforts, as it prevents the precise replication of these nanostructures.

High-Efficiency Targeted Gene Transfection of Cells Using Temporal and Spatial Shaping Femtosecond Laser Irradiation.

Laser-irradiation-assisted cell gene transfection is sterile and nontoxic, but the low transfection efficiency cannot meet the application requirements. To improve the efficiency, a temporal and spatial shaping method of a femtosecond laser is proposed. Using the time shaping method, we can segment the pulse into subpulses of varying energies and with a defined delay, thereby influencing the interaction between electrons and photons, ultimately enhancing transfection efficiency. The transfection efficiency is further improved by spatially shaping the laser pulse to extend the focusing beam's working distance and reduce the cell's sensitivity to the focal position. Through the characterization of the viability and transfection efficiency of HEK-293T cells, the method achieved efficient and active transfection, with a maximum transfection efficiency of 45.1% and a cell survival rate of 93.6%. This method provides key technical support for femtosecond laser transfection and promotes its further application in clinical practice.

Quenching high-temperature phase in Cu–Sn alloy system by femtosecond and picosecond laser irradiation

Quenching high-temperature phase in Cu–Sn alloy system by femtosecond and picosecond laser irradiation

Fe3+ Assisted Synthesis of Stable 3D‐in‐2D CsPbBr3/CsPb2Br5 Nanocomposites for Optical Gain Media

AbstractMetal halide perovskite nanocrystals are sought after for many optical and optoelectronic applications, such as light‐emitting diode and solar cells, due to their outstanding optical properties. However, their ionic nature makes them susceptible to ambient conditions. One rational solution to this challenge is the passivation or encapsulation of perovskite nanocrystals to isolate them from their environments. Thus, there is an urgent need to develop efficient methods for encapsulating emissive perovskite nanocrystals. A facile post‐synthesis method is proposed to treat CsxFA(1−x)PbBr3 nanocrystals, in the presence of Fe3+ cations, to create a robust and water‐stable nanocomposite structure, where 3D CsPbBr3 nanocrystals are embedded in and thus protected by the 2D CsPb2Br5 nanosheets (named as CsPbBr3/CsPb2Br5 hereafter). These Fe3+ cations facilitate the formation of the CsPbBr3/CsPb2Br5 composite and regulate the growth of 2D CsPb2Br5 sheets. By performing controlled experiments, the possible mechanism of 2D nanosheet growth is proposed and discussed in detail. More importantly, the composite can remain stable in water for three months and exhibits amplified spontaneous emission under femtosecond laser irradiation. This work presents a synthesis pathway for producing durable perovskite composites that are promising for future lasing applications.

Nanochannels in Fused Silica through NaOH Etching Assisted by Femtosecond Laser Irradiation

Sodium hydroxide (NaOH) is increasingly drawing attention as a highly selective etchant for femtosecond laser-modified fused silica. Unprecedented etching contrasts between the irradiated and pristine areas have enabled the fabrication of hollow, high-aspect-ratio structures in the bulk of the material, overcoming the micrometer threshold as the minimum feature size. In this work, we systematically study the effect of NaOH solutions under different etching conditions (etchant concentration, temperature, and etching time) on the tracks created by tightly focused femtosecond laser pulses to assess the best practices for the fabrication of hollow nanostructures in bulk fused silica.

Nonlinear Excitation of Color Centers in a LiF Crystal by Femtosecond Laser Radiation

Experiments were carried out in which the luminescence of color centers in lithium fluoride crystals was excited by two different femtosecond lasers with significantly different energies, durations and pulse repetition rates. It was established that in all experiments the main center, the luminescence of which was excited nonlinearly, was the F3+ color center. Unusual experimental data were obtained; a laser with low pulse energy (4 nJ) excited triplet luminescence of these centers (570 nm) but did not excite singlet luminescence (540 nm). Another laser with a higher pulse energy (0.3 mJ), on the other hand, excited singlet luminescence and did not excite triplet luminescence. A proposed diagram of energy levels and quantum transitions is presented, explaining the possible mechanisms of nonlinear excitation of luminescence in these experiments.

Optoplasmonic tuneable response by femtosecond laser irradiation of glass with deep-implanted gold nanoparticles

The manipulation of the optical properties of plasmonic nanocomposites is of high interest for the development of advanced optical devices with tailored unique properties. Achieving these objectives requires a combination of synthesis techniques and post-fabrication strategies. Here, we combine the use of two well-established physical strategies: MeV ion implantation and femtosecond laser processing. Firstly, we synthesize Au-doped soda lime glass nanocomposite through ion beam implantation (Au2+ at 1.8 MeV) followed by thermal annealing. This synthesis procedure results in a peculiar optical response based on the combination of Au-nanoparticle plasmonic resonance and a Fabry-Perot interference, caused by the deep implantation (centered at 480 nm). Secondly, this dual response is demonstrated to be highly tuneable by non-resonant femtosecond laser irradiation (800-nm wavelength and 130-fs pulse duration). Depending on the laser fluence, three transformation regimes are distinguished: supressing the interferometric response by spallative ablation, inducing vivid blue colors by surface swelling, and producing red-shifted color changes by multi-shot irradiation at low fluences. The proposed method is very versatile, since it is applicable to any dielectric matrix or implanted element. This work paves the way to a new route for the development of scalable and tuneable nanocomposites with several potential applications in optics.

Point defect distributions in ultrafast laser-induced periodic surface structures on β-Ga2O3

β-Ga2O3 has received widespread attention due to its ultrawide bandgap, which potentially permits applications in extreme conditions. Ultrafast laser irradiation of β-Ga2O3 provides a means for exploring the response of the material under such conditions, which could result in the generation of point defects as well as a localized modification of structural features that could yield properties that differ from the pristine surface. However, an understanding of defects generated by femtosecond laser irradiation in the vicinity of laser-induced periodic surface structures (LIPSS) remains to be explored. We correlate topographic features with optical and electronic properties by combining near-nm scale resolution cathodoluminescence with Kelvin probe force microscopy. Defects are found to correlate with crystalline order and near-surface morphology, as well as changes in work function. They are also suggested to be closely related to the formation of high spatial frequency LIPSS. These results suggest a need for precise tuning of laser irradiation conditions as well as possible post-processing to control defects in future Ga2O3 devices.

Nonequilibrium electronic properties and stability consequences in metallic crystalline binary alloys under ultrafast laser excitation

This study undertakes an exhaustive exploration of properties under electron-phonon nonequilibrium for a series of ten industrially pertinent crystalline alloys, namely AlCu, AlNi, AlTi, AuCu, CuNi, CuTi, NbZr, NiTi, NiZr, and ZrCu. This comprehensive investigation encompasses electronic heat capacity, electron-phonon coupling factor, excited electron density, electronic pressure, dielectric function, refractive index, extinction coefficient, reflectivity, and optical penetration depth. Employing ab initio simulations, we meticulously analyze the nonequilibrium optoelectronic attributes inherent to these alloys change under electronic excitation across the temperature range going from 0 to 50,000 K. Additionally, to contextualize the findings, we employ classical Molecular Dynamics coupled with a Two Temperature Model simulation, notably to deliver a deep comprehension of the intricate mechanisms of the CuTi alloy ablation induced by femtosecond laser irradiation.

Measurement of electromagnetic pulse in laser acceleration enhanced by near-critical density targets

High-power laser interactions with solid targets create an abundance of high-energy charged particles, resulting in the generation of intense electromagnetic pulses (EMPs), which are strongly pertinent to the target parameters. In this study, the characteristics of EMPs generated by relativistic femtosecond laser irradiation of double-layer targets composed of near-critical density carbon nanotube foams (CNFs) and an aluminum (Al) foil are investigated. The results demonstrate that the CNF double-layer targets accelerate proton energy by over 1.6 times compared to a single-layer Al plane target, thereby indirectly amplifying the EMP amplitude by over 3.6 times. The findings are beneficial to gaining insight into EMPs induced by femtosecond laser coupling with near-critical density targets and open a new avenue to achieve tunable EMPs by managing the material and structure of the target to optimize the coupling efficiency between the laser and solid targets.

Size Effects of Copper(I) Oxide Nanospheres on Their Morphology on Copper Thin Films under Near-Infrared Femtosecond Laser Irradiation.

The femtosecond laser direct writing of metals has gained significant attention for micro/nanostructuring. Copper (I) oxide nanospheres (NSs), a promising material for multi-photon metallization, can be reduced to copper (Cu) and sintered through near-infrared femtosecond laser pulse irradiation. In this study, we investigated the size effect of copper (I) oxide nanospheres on their morphology when coated on Cu thin films and irradiated by near-infrared femtosecond laser pulses. Three Cu2O NS inks were prepared, consisting of small (φ100 nm), large (φ200 nm), and a mixture of φ100 nm and φ200 nm NSs. A unique phenomenon was observed at low laser pulse energy: both sizes of NSs bonded as single layers when the mixed NSs were used. At higher pulse energies, the small NSs melted readily compared to the large NSs. In comparisons between the large and mixed NSs, some large NSs remained intact, suggesting that the morphology of the NSs can be controlled by varying the concentration of different-sized NSs. Considering the simulation results indicating that the electromagnetic fields between large and small NSs are nearly identical, this differential morphology is likely attributed to the differences in the heat capacity of the NSs.

Femtosecond laser-induced damage threshold incubation in SrTiO3 thin films

This study delved into the microfabrication process on SrTiO3 thin films using femtosecond laser pulses, focusing on characterizing ablation behavior and elucidating on incubation parameters. A combination of microscopy techniques and systematic analysis of laser-material interactions provided insights into the features and fundamental processes governing the laser-induced modification of SrTiO3 thin films. The cutting profile morphology indicated high-resolution material removal, with line widths ranging from 0.6 to 1.6 µm, depending on number of pulses and energy. The study revealed a low incubation parameter for SrTiO3 thin films, quantified as (0.03 ± 0.01), indicating that a considerable number of pulses is required to cause damage to the material. Additionally, threshold energies for damage were determined to be 17.9 nJ for 20,000 pulses and 35.2 nJ for a single pulse. AFM analysis showed that the depth of the micromachined lines increased from approximately 80 nm to 315 nm with higher pulse energies, confirming substantial material removal. The Keldysh parameter provides insights into ionization mechanisms under femtosecond-laser irradiation, highlighting the dominance of tunneling ionization. Using higher pulse energies, the center of the microstructures exhibited significantly reduced Raman signals, correlating with substantial material removal, which was confirmed by atomic force microscopy. EDS analyses indicated that the elemental composition of the irradiated regions closely resembled the stoichiometric composition of SrTiO3, while the center of the microstructures showed significant oxygen levels but lacked titanium and strontium, consistent with the findings from AFM and Raman microscopy.

Accounting for the energy dispersion of free carriers induced by powerful femtosecond laser radiation in dielectrics

Dynamics of free carriers in the conduction band of dielectrics induced by femtosecond near infrared laser radiation is analyzed. It is stressed the importance of accounting for the energy dispersion term in the Fokker-Planck equation describing such dynamics.

Ageing of commercial austenitic, martensitic and duplex stainless steel surfaces after formation of laser-induced periodic surface structures by fs-laser irradiation

The time-dependent wetting behavior was investigated for commercially available austenitic, martensitic and duplex stainless steel surfaces after femtosecond (fs) laser irradiation. For this purpose, highly regular LIPSS with almost identical geometric properties were generated on the stainless steels in an air environment by near-infrared fs-laser processing (λ = 1025 nm, τ = 300 fs, frep = 100 kHz, v = 0.67 m/s, Δx = 6 μm, F = 1.1 J/cm2) and compared to the polished initial surfaces as reference. The wetting with distilled water was evaluated as a function of aging time by contact angle measurements using the sessile drop method. The laser-induced morphological, topographical and chemical alteration of the surface was characterized by scanning electron microscopy, atomic force microscopy, X-ray photoelectron spectroscopy, glow-discharge optical emission spectroscopy as well as high-resolution imaging and scanning transmission electron microscopy. Despite an almost identical LIPSS-based topography alteration, the stainless steels revealed very different ageing behavior. For permanently used samples, it was shown that the ageing effect is less pronounced than for samples that were stored in ambient air following fs-laser irradiation until the wetting measurement. The results obtained make an important contribution to understanding and controlling the ageing effect of metal surfaces and thus facilitate the transfer of LIPSS-based functional surface engineering and design to industrial processes.

Targeted Microforming of Borosilicate Glass Induced by a Laser‐Ablation‐Free Process Using Femtosecond Pulses

AbstractThe use of ultrashort pulse lasers opens up a wide range of possibilities for processing dielectric materials. The present study focuses on the investigation of the ablation‐free microscopic surface modification of borosilicate glass using femtosecond laser radiation (350 fs at 515 nm wavelength) in a scanning machining process. Furthermore, its aim is to analyze the relationship between the laser process parameters and the microscopic changes in the surface topography observed. The characteristic of the generated surface structure, which takes place below the ablation threshold, shows both elevations and depressions within the irradiated field (2 × 2 mm2). The realized structures reach a profile height Peak‐to‐Valley (PV) of up to 10 µm. The amount of surface deformation depends on the selected parameters such as laser fluence, number of passes, and scanning strategy. The microdeformation is detected on both the top and bottom sides of the processed glass material with a thickness ≤1 mm. The influence of the temporal and spatial energy distribution on the material modification is discussed, demonstrating the possibilities of microforming of silicate glasses using ultrashort pulsed laser radiation.

Berberine-loaded nanoemulsions as a natural food preservative; the impact of femtosecond laser irradiation on the antibacterial activity

There is a growing concern among food safety regulators, the food industry, and consumers about foodborne illnesses. To improve food safety and increase shelf life, it is necessary to use natural preservatives. Natural antimicrobials are safer than artificial preservatives because they can prevent microbial resistance while also meeting consumers' demands for healthier food. This study used Berberine to enhance the antibacterial activity of Satureja Khuzistanica essential oil nanoemulsions (SKEO NE) against Staphylococcus aureus (S. aureus) bacteria, making them a promising option as preservatives. Response Surface Methodology (RSM) was employed to determine the optimized Berberine loaded SKEO NE (Berberine/SKEO NE), resulting in a mean droplet size of 88.60 nm at 6.91, 3.21, and 0.08% w/w of surfactant, essential oil, and Berberine, respectively. Berberine utilization in SKEO NE has led to an increase in antibacterial activity. The nanoemulsion samples significantly ruptured the S. aureus bacterial cell membrane, rapidly discharging cell contents. The use of a microfluidic system in tandem based on the conventional approach significantly accelerated this process. Enhancing the interaction between nanodroplets and the bacterial membrane can be achieved through the nanoemulsification process of EOs, which involves modifying their surface characteristics. This enhancement is particularly pronounced when employing microfluidic systems due to their substantial contact surface area. We investigated the potential of using femtosecond laser irradiation at a wavelength of 1040 nm to augment the antibacterial action of nanoemulsions. The combined treatment of laser and nanoemulsions significantly increased the antibacterial effect of nanoemulsions by approximately 15% for each bacterium, suggesting the potential utility of this treatment to bolster the antibacterial activity of nanoemulsions. Bacteria were trapped using optical tweezers for up to 20 min, with bacterial destruction observed starting at 3 min and exhaustive destruction evident after 20 min.

Acousto-optic femtosecond laser beam shaping for bottle-beam generation

Abstract This study explores the properties of a laser beam shaping system comprising an acousto-optic dispersive delay line (AODDL) and an acousto-optic tunable filter (AOTF) for ultrashort laser pulse shaping. The system demonstrates the AODDL’s ability to generate signals with arbitrarily positioned transmission windows and investigates the impact of spectral width on field distributions. The AOTF’s frequency scanning and simultaneous control of two and three spectral components are presented. The experimental setup utilizes femtosecond laser radiation, and the results highlight the system’s versatility for programmable spectral and spatial filtering, offering potential applications in advanced optical manipulation.

Reversible modulations of insulator–metal transition in an epitaxial VO2 film through thermal crystallization and femtosecond laser-induced-amorphization of capping Ge2Sb2Te5 layer

We demonstrate reversible modulation of an insulator–metal transition (IMT) of a VO2 film grown on an Al2O3 (001) substrate through crystallization and re-amorphization of a chalcogenide germanium–antimony–telluride (Ge2Sb2Te5: GST) capping layer. After succeeding in the negative shift of IMT temperature (Tr) of the VO2 film through the crystallization of the GST layer accompanied by volume reduction, we performed re-amorphization of the crystalline GST by femtosecond laser irradiation. Under the optimized conditions of laser irradiation considering the penetration depth, re-amorphization of the GST layer was fully achieved, resulting in the shift-back of Tr toward a high-temperature side. Such a reversal of IMT through the crystallization and re-amorphization of the capping GST layer was demonstrated over two cycles. It was suggested that capping GST effectively induces interfacial strain modifications in the VO2 film underneath. Although the shifts in the IMT are still small, reversible modulation of IMT shown here will be beneficial for applications of VO2 films with controllable IMT.

Ultrafast dynamics and internal processing mechanism of silica glass under double-pulse femtosecond laser irradiation

Femtosecond laser-induced plasma filaments have potential for various applications including attosecond physics, spectroscopy, and microprocessing. However, the use of plasma filaments to generate high-aspect-ratio internal modifications remains low-efficiency. Here, we experimentally demonstrated high-efficiency internal processing using plasma filaments induced by a double-pulse femtosecond laser. The processing mechanism was revealed through an investigation of the ultrafast dynamics of plasma filaments in experiments and simulations. We found that the excitation region of the first pulse (P1) exerted a temporal effect on the propagation and absorption of the second pulse (P2) due to the evolution of excited electrons, thus resulting in different processing characterizations. At a smaller inter-pulse delay (IPD), electrons and self-trapped excitons induced by P1 improved the absorption of P2 in the shallow region. Consequently, the main excitation regions of P1 and P2 were separated, resulting in a lower density of energy deposition and weak modifications. Whereas, at a larger IPD, P2 penetrated a deeper region with the relaxation of electrons and excitons induced by P1, leading to a better overlap of excitation regions between P2 and P1, thus improving the density of energy deposition and achieving efficient microprocessing. Besides, at an infinite IPD, P2 behaved like P1, but no modification was obtained owing to the complete energy diffusion of P1. Therefore, controlling the electron dynamic and energy diffusion contributes to the improvement of modification efficiency. Furthermore, the distribution of electron densities on the cross section was estimated to precisely analyze the microprocessing. These results are expected to aid in a better understanding of the interaction mechanism between dielectrics and intense ultrafast lasers and be useful for microprocessing applications.

Near-Field-Regulated Ultrafast Laser Supra-Wavelength Structuring Directly on Ultrahard Metallic Glasses.

The ultrafast-laser-matter interactions enable "top-down" laser surface structuring, especially for materials difficult to process, with "bottom-up" self-organizing features. The subwavelength scenarios of laser-induced structuring are improved in defects and long-range order by applying positive/negative feedbacks. It is still hardly reported for supra-wavelength laser structuring more associated with complicated thermo/hydro-dynamics. For the first time to the knowledge, the near-field-regulated ultrafast-laser lithography of self-arrayed supra-wavelength micro/nano-pores directly on ultra-hard metallic glass is developed here. The plasmonic hot spots on pre-structures, as the positive feedback, clamped the lateral geometries (i.e., position, size). Simultaneously, it drilled and self-organized into micro/nano-pore arrays by photo-dynamic plasma ablation and Marangoni removal confined under specific femtosecond-laser irradiation, as the negative feedback. The mechanisms and finite element modeling of the multi-physical transduction (based on the two-temperature model), the far-field/near-field coupling, and the polarization dependence during laser-matter interactions are studied. Large-area micro/nano-pore arrays (centimeter scale or larger) aremanufactured with tunable periods (1-5µm) and geometries (e.g., diameters of 500 nm-6µm using 343, 515, and 1030 lasers, respectively). Consequently, the mid/far-infrared reflectivity at 2.5-6.5µm iss decreased from ≈80% to ≈5%. The universality of multi-physical coupling and near-field enhancements makes this approach widely applicable, or even irreplaceable, in various applications.