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Nadezhda M. Bulgakova

Publications and source records attributed to Nadezhda M. Bulgakova.

At least 19 recordsLinked to original sources

Enhanced LIBS Emission Using Laser Beam Splitting: Interacting Multi-Plume Plasma Dynamics

The optical emission in laser-induced breakdown spectroscopy (LIBS) is governed by the spatial intensity distribution of the incident laser beam, which influences plasma formation and evolution. Beam shaping therefore offers a route to control plasma dynamics and emission yield; however, its effects in LIBS remain insufficiently quantified, particularly under conditions relevant to compact instrumentation. In this work, a diffractive optical element (DOE) is used to transform a Gaussian beam into a 2x2 array, producing simultaneously expanding, co-propagating ablation plumes that interact during expansion. Plasma evolution from Cu and Si targets is investigated in vacuum using a Nd:YAG laser (1064 nm, 5 ns, 10 J/cm2), combining time-resolved imaging with optical emission spectroscopy. The multi-spot configuration results in enhanced emission intensity compared to single-spot irradiation, with increases of ~9 for Si and ~3 for Cu. The observed enhancement is attributed to plume-plume interaction effects that modify plasma density and emission characteristics. These results demonstrate that DOE-based beam shaping provides an effective and technically simple approach to increasing the LIBS signal without additional system complexity.

physics.app-ph↗

Hybrid Femtosecond Laser and Ion-Implantation Processing for Controlled, Deep, High-Efficiency Ablation in Fused Silica

Femtosecond laser modification of fused silica enables precise surface tailoring for the fabrication of micro-optical components such as microlenses and diffractive elements. However, the process is governed by laser-matter interactions where the local fluence determines the processing depth, often limiting control over feature geometry and efficiency. Here, we present a hybrid approach combining localized Au implantation (1.8 MeV Au2+ ions) into SiO2 samples with femtosecond laser irradiation (250 fs), effectively tuning the laser-matter interaction and resulting morphology. At both 515 nm and 1030 nm irradiation wavelengths, single-shot femtosecond pulses produce cylindrical craters with sharp edges and flat-bottom profiles. Independently of the fluence, these craters exhibit a constant depth of 550 nm, corresponding to the region of maximum Au concentration. The effect manifests already at moderate fluence (app. 4 J/sq.cm) and yields high ablation efficiency, up to 15 cubic micrometers per microjoule. The hybrid method also works effectively at lower implantation doses that preserve the excellent transmission of fused silica, offering a promising pathway for the high-quality fabrication of flat optical components such as binary phase masks, phase lenses, or fused-silica micromolds.

physics.optics↗

Light in Slices: How to Enable Precise Laser Processing?

Ultrashort (femtosecond, fs) laser pulses have fascinating properties as they allow to confine optical energy on extreme scales in space and time. Such fs-laser pulsed beams can be seen as spatially thin slices of intense light that are radially and axially constrained to the micrometer scale, while simultaneously propagating at the extremely high speed of light. Their high peak intensities and their short time lapse makes such laser pulses unique tools for materials processing, as their duration is shorter than the time required to transfer absorbed optical energy, via electron-phonon coupling, from the electronic system of the solid to its lattice. Hence, the laser pulse energy remains localized during the interaction and does not spread via diffusion into the area surrounding the irradiated region. As one consequence, the fs-laser thus offers increased precision for material modification or ablation accompanied by a reduced heat-affected zone of only a few hundred nanometers. On the other hand, the high laser peak intensities can enable nonlinear material interactions that are rendering unique material excitation and relaxation pathways possible. In this chapter, we briefly review the reasons for the enormous success of ultrashort pulse lasers in materials processing - both for the processing of the surface or in the bulk of solids. We identify the underlying fundamental processes that can limit the precision or the up-scaling of the laser processing towards large volumes, areas, or processing rates. Strategies to overcome such limitations will be outlined and questions on the ultimate limits of laser material processing will be answered.

physics.optics↗

Thermomechanical investigation of silicon wafer dynamics within the melting regime driven by picosecond laser pulses for surface structuring

Laser-induced periodic surface structures (LIPSS) on silicon, generated by ultrashort pulsed lasers, provide an efficient means to tailor surface functionality. This work presents a multiphysics finite element study on the thermomechanical dynamics of silicon wafers irradiated by picosecond laser pulses, focusing on the melting regime where thermomechanical and hydrodynamic effects dominate. To illustrate the sequential nature of laser scanning, single-pulse irradiation models are developed as thermomechanical analogues of double-pulse interactions. By positioning the laser focus near reflective boundaries and corners of the target, these models reproduce the stress-wave interference that would occur between successive pulses in scanning. The results show that periodic surface structures originate from mechanical standing wave interference within the molten layer, forming ripples with near-wavelength periodicity. The penetration depth (PD) is identified as a key factor controlling the duration and stability of these ripples: shallow PDs (75-150 nm) yield distinct, persistent patterns, while deeper PDs (app. 2.5 micrometers) lead to extended melting and hydrodynamic smoothing. Simulations of sequential double-pulse irradiation confirm that residual stresses and strains from the first pulse amplify deformation during the second, enhancing ripple amplitude and uniformity. Controlled excitation of mechanical standing waves governed by PD, boundary geometry, and pulse sequencing - thus represents a fundamental mechanism for deterministic LIPSS formation on silicon.

cond-mat.mtrl-sci↗

Femtosecond Laser Crystallization of Ultrathin a-Ge Films in Multilayer Stacks with Silicon Layers

Ultrashort pulsed laser annealing is an efficient technique for crystallizing amorphous semiconductors with the possibility to obtain polycrystalline films at low temperatures, below the melting point, through non-thermal processes. Here, a multilayer structure consisting of alternating amorphous silicon and germanium films was annealed by mid-infrared (1500 nm) ultrashort (70 fs) laser pulses under single-shot and multi-shot irradiation conditions. We investigate selective crystallization of ultrathin (3.5 nm) a-Ge film, promising for the generation of highly photostable nanodots. Based on Raman spectroscopy analysis, we demonstrate that, in contrast to thicker (above 10 nm) Ge films, explosive stress-induced crystallization is suppressed in such ultrathin systems and proceeds via thermal melting. This is likely due to the islet structure of ultrathin films which results in the formation of nanopores at the Si-Ge interface and reduces stress confinement during ultrashort laser heating.

physics.optics↗

The Roadmap of New Capabilities of High-Intensity Lasers in Material Design and Manipulation

One of the current trends of laser applications in material science is using high-intensity lasers to provide fast and efficient surface or volume modifications for achieving controllable material properties, synthesis of novel materials with desired functionalities, and upscaling laser technologies with industry-demanded throughputs. Depending on the parameters, lasers can offer versatile solutions for scientific and industrial applications, starting from exploring the fundamental physics of warm dense matter and molecular chemistry at ultrashort timescales to large-scale fabrication of surfaces with anti-bacterial, tribological, hydrophobic, or hydrophilic properties. The objectives of this Chapter are to provide a review of recent advancements in several laser application fields, which involve high-intensity lasers, both ultrashort (femto- and picosecond) and short (nanosecond). After summarizing general trends in high-intensity laser processing of materials, we will first focus on the new opportunities offered by high-intensity lasers for the controlled synthesis of multielement nanoparticles for catalytic and theranostic applications. Then, the blister-based laser-induced forward transfer (BB-LIFT) technique will be presented, allowing a one-step, high-precision printing of nanomaterials on any substrates. The next section will discuss the selective crystallization of amorphous (as prepared) semiconductor nanoscale materials. The processes enabling high selectivity of crystallization into the desired phase using ultrashort powerful lasers will be analyzed. After that, opportunities for using high-power lasers will be discussed for upscaling surface nanostructuring with high throughput for bio-medical and industrial applications. Finally, an introduction to the Open Access program of the HiLASE Centre, which is targeted at offering users high-intensity beam time, will be given.

physics.optics↗

On Space Debris Removal by Lasers: Can Spatially and Temporally Shaped Laser Pulses Be Advantageous for Propulsion?

For exploration of space, in particular in attempts to find new extra-terrestrial resources, human society has encountered the problem of space pollution with human-made debris, which represents high risks for space missions. This prompted extensive activities for cleaning the space using various techniques, which are briefly overviewed here. But the main focus of this paper is on using lasers for space debris removal. The attention is drawn to laser beam shaping techniques, which are discussed as potential technologies for deorbiting space debris, providing more energetically favorable laser propulsion compared to conventional laser beams.

physics.optics↗

Laser-Induced Gas-Phase Transfer and Direct Stamping of Nanomaterials: Comparison of Nanosecond and Femtosecond Pulses

The two-dimensional nanomaterial, hexagonal boron nitride (hBN) was cleanly transferred via a blister-based laser-induced forward-transfer method. The transfer was performed utilizing femtosecond and nanosecond laser pulses for separation distances of ~16 and ~200 micrometers between a titanium donor film deposited on a glass substrate and a silicon/silicon dioxide receiver. Transfer efficiency was examined for isolated laser pulses as well as for series of overlapping pulses and single layer transfer was confirmed. It was found that hBN is transferable for all tested combinations of pulse duration and transfer distances. The results indicate that transfer proceeds via direct stamping for short donor-to-receiver distances while, for the larger distance, the material is ejected from the donor and lands on the receiver. Furthermore, with overlapping pulses, nanosecond laser pulses enable a successful printing of hBN lines while, for fs laser pulses, the Ti film can be locally disrupted by multiple pulses and molten titanium may be transferred along with the hBN flakes. For reproducibility, and to avoid contamination with metal deposits, low laser fluence transfer with ns pulses and transfer distances smaller than the blister height provide the most favourable and reproducible condition.

physics.optics↗

Coherence effects in LIPSS formation on silicon wafers upon picosecond laser pulse irradiations

Using different laser irradiation patterns to modify of silicon surface, it has been demonstrated that, at rather small overlapping between irradiation spots, highly regular laser-induced periodic surface structures (LIPSS) can be produced already starting from the second laser pulse, provided that polarization direction coincides with the scanning direction. If the laser irradiation spot is shifted from the previous one perpendicular to light polarization, LIPSS are not formed even after many pulses. This coherence effect is explained by a three-wave interference, - surface electromagnetic waves (SEWs) generated within the irradiated spot, SEWs scattered from the crater edge formed by the previous laser pulse, and the incoming laser pulse, - providing conditions for amplification of the periodic light-absorption pattern. To study possible consequences of SEW scattering from the laser-modified regions, where the refractive index can change due to material melting, amorphization, and the residual stress formed by previous laser pulses, hydrodynamic modelling and simulations have been performed within the melting regime. The simulations show that stress and vertical displacement could be amplified upon laser scanning. Both mechanisms, three-wave interference and stress accumulation, could enable an additional degree of controlling surface structuring.

physics.optics↗

Dual-wavelength femtosecond laser-induced low-fluence single-shot damage and ablation of silicon

A study of damage and ablation of silicon induced by two individual femtosecond laser pulses of different wavelengths, 1030 and 515 nm, is performed to address the physical mechanisms of dual-wavelength ablation and reveal possibilities for increasing the ablation efficiency. The produced ablation craters and damaged areas are analyzed as a function of time separation between the pulses and are compared with monochromatic pulses of the same total energy. Particular attention is given to low-fluence irradiation regimes when the energy densities in each pulse are below the ablation threshold and thus no shielding of the subsequent pulse by the ablation products occurs. The sequence order of pulses is demonstrated to be essential in bi-color ablation with higher material removal rates when a shorter-wavelength pulse arrives first at the surface. At long delays of 30-100 ps, the dual-wavelength ablation is found to be particularly strong with the formation of deep smooth craters. This is explained by the expansion of a hot liquid layer produced by the first pulse with a drastic decrease in the surface reflectivity at this timescale. The results provide insight into the processes of dual-wavelength laser ablation offering a better control of the energy deposition into material.

physics.optics↗

Volumetric glass modification with Gaussian and doughnut-shaped pulses: From localized laser energy absorption to absorption delocalization

Volumetric modification of glass materials by ultrashort laser pulses is a powerful technique enabling direct writing of three-dimensional structures for fabrication of optical, photonic, and microfluidic devices. The level of modification is determined by the locally absorbed energy density, which depends on numerous factors. In this work, the effect of the spatial pulse shape on the ultrashort laser excitation of fused silica was investigated experimentally and theoretically for the volumetric modification regimes. We focused on two shapes of laser pulses, Gaussian and doughnut-shaped (DS) ones. It was found that, at relatively low pulse energies, in the range of 1-5 microjoules, the DS pulses are more efficient in volumetric structural changes than Gaussian pulses. It is explained by the intensity clamping effect for the Gaussian pulses, which leads to the delocalization of the laser energy absorption. In the DS case, this effect is overcome due to the geometry of the focused beam propagation, accompanied by the electron plasma formation, which scatters light toward the beam axis. The thermoelastoplastic modeling performed for the DS pulses revealed intriguing dynamics of the shock waves generated because of tubular-like energy absorption. It is anticipated that such a double shock wave structure can induce the formation of high-pressure polymorphs of transparent materials that can be used for investigations of nonequilibrium thermodynamics of warm dense matter. The DS laser pulses of low energies of the order of 100 nanojoules which generate a gentle tubular-like modification can be perspective for a miniature waveguide writing in glass.

cond-mat.mtrl-sci↗

Melting of gold by ultrashort laser pulses: Advanced two-temperature modeling and comparison with surface damage experiments

The ultrafast laser-induced solid-liquid phase transition in metals is still not clearly understood and its accurate quantitative description remains a challenge. Here we systematically investigated, both experimentally and theoretically, the melting of gold by single femto- and picosecond near-infrared laser pulses. Two laser systems with wavelengths of 800 and 1030 nm and pulse durations ranging from 124 fs to 7 ps were used and the damage and ablation thresholds were determined for each irradiation condition. The theoretical analysis was based on two-temperature modeling. Different expressions for the electron-lattice coupling rate and contribution of ballistic electrons were examined. In addition, the number of free electrons involved in the optical response is suggested to be dependent on the laser intensity and the influence of the fraction of involved electrons on the damage threshold was investigated. Only one combination of modelling parameters was able to describe consistently all the measured damage thresholds. Physical arguments are presented to explain the modeling results.

cond-mat.mtrl-sci↗

Photoionization and transient Wannier-Stark ladder in silicon: First principle simulations versus Keldysh theory

Nonlinear photoionization of dielectrics and semiconductors is widely treated in the frames of the Keldysh theory whose validity is limited to small photon energies compared to the band gap and relatively low laser intensities. The time-dependent density functional theory (TDDFT) simulations, which are free of these limitations, enable to gain insight into non-equilibrium dynamics of the electronic structure. Here we apply the TDDFT to investigate photoionization of silicon crystal by ultrashort laser pulses in a wide range of laser wavelengths and intensities and compare the results with predictions of the Keldysh theory. Photoionization rates derived from the simulations considerably exceed the data obtained with the Keldysh theory within the validity range of the latter. Possible reasons of the discrepancy are discussed and we provide fundamental data on the photoionization rates beyond the limits of the Keldysh theory. By investigating the features of the Stark shift as a function of photon energy and laser field strength, a manifestation of the transient Wannier-Stark ladder states have been revealed which become blurred with increasing laser field strength. Finally, it is shown that the TDDFT simulations can potentially provide reliable data on the electron damping time that is of high importance for large-scale modeling.

cond-mat.mtrl-sci↗

LIPSS on thin metallic films: New insights from multiplicity of laser-excited electromagnetic modes and efficiency of metal oxidation

Thin Cr films 28-nm thick deposited on glass substrates were processed by scanning low-intensity femtosecond laser pulses with energy well below single-pulse damage threshold. Two types of laser-induced periodic surface structures (LIPSS) were produced, depending on the scanning velocity, (1) parallel to laser light polarization with periodicity somewhat smaller than laser wavelength and (2) perpendicular to polarization with spatial period much smaller than wavelength. All structures are formed as protrusions above the initial film surface and exhibit a high degree of oxidation. To explain formation of the LIPSS and their conversion from one to another type, a rigorous numerical approach for modeling surface electromagnetic waves in thin-film geometry has been developed, which takes into account the change of optical properties of material due to laser-induced oxidation and porosity. The approach addresses the multiplicity of electromagnetic modes allowed for thin films. It has been found that the low spatial frequency LIPSS parallel to laser polarization, which are formed at low scanning velocities, are well described by the Sipe theory for surfaces of low roughness. The SEW mode responsible for high spatial frequency LIPSS formation at high scanning velocities has been identified. The mechanisms of optical feedback and transformation between types of LIPSS with scanning velocity have been proposed.

physics.app-ph↗

Selective Delamination upon Femtosecond Laser Ablation of Ceramic Surfaces

We report on the experimental observation of selective delamination of semi-transparent materials on the example of yttria-stabilized zirconia ceramics upon femtosecond laser processing of its surface with low numerical aperture lens. The delamination of a ceramic layer of dozens of micrometers takes place as a by-side effect of surface processing and is observed above the surface ablation threshold. The onset of delamination (delamination threshold) depends on the degree of overlap of the irradiation spots from consecutive laser pulses upon beam scanning over material surface. Analysis of the delaminated layer indicates that the material undergoes melting on its both surfaces. The mechanism of delamination is identified as a complex interplay between the optical response of laser-generated free-electron plasma and nonlinear effects upon laser beam propagation in semi-transparent ceramics. The discovered effect enables controllable laser microslicing of brittle ceramic materials.

physics.app-ph↗

Mechanism of the single-pulse ablative generation of laser induced periodic surface structures

One of the remarkable capabilities of ultrashort polarized laser pulses is the generation of laser-induced periodic surface structures (LIPSS). The origin of this phenomenon is largely attributed to the interference of the incident laser wave and surface electromagnetic wave that creates a periodic absorption pattern. Although, commonly, LIPSS are produced by repetitive irradiation of the same area by multiple laser pulses in the regime of surface melting and resolidification, recent reports demonstrate the formation of LIPSS in the single pulse irradiation regime at laser fluences well above the ablation threshold. In this paper, we report results of a large-scale molecular dynamics simulation aimed at providing insights into the mechanisms of single pulse ablative LIPSS formation. The simulation performed for a Cr target reveals an interplay of material removal and redistribution in the course of spatially modulated ablation, leading to the transient formation of an elongated liquid wall extending up to ~600 nm above the surface of the target at the locations of the minima of the laser energy deposition. The upper part of the liquid wall disintegrates into droplets while the base of the wall solidifies on the timescale of ~2 ns, producing a ~100 nm-long frozen surface feature extending above the level of the initial surface of the target. The properties of the surface region of the target are modified by the presence of high densities of dislocations and vacancies generated due to the rapid and highly nonequilibrium nature of the melting and resolidification processes. The insights into the LIPSS formation mechanisms may help in designing approaches for increasing the processing speed and improving the quality of the laser-patterned periodic surface structures.

cond-mat.mtrl-sci↗

Wavelength Dependence of Picosecond Laser-Induced Periodic Surface Structures on Copper

The physical mechanisms of the laser-induced periodic surface structures (LIPSS) formation are studied in this paper for single-pulse irradiation regimes. The change in the LIPSS period with wavelength of incident laser radiation is investigated experimentally, using a picosecond laser system, which provides 7-ps pulses in near-IR, visible, and UV spectral ranges. The experimental results are compared with predictions made under the assumption that the surface-scattered waves are involved in the LIPSS formation. Considerable disagreement suggests that hydrodynamic mechanisms can be responsible for the observed pattern periodicity.

cond-mat.mes-hall↗

Role of the temperature instabilities for formation of nano-patterns upon single femtosecond laser pulses on gold

In this paper we investigate whether the periodic structures on metal surfaces exposed to single ultrashort laser pulses can appear due to an instability induced by two-temperature heating dynamics. The results of two-temperature model (TTM) 2D simulations are presented on the irradiation of gold by a single 800 nm femtosecond laser pulse whose intensity is modulated in order to reproduce a small initial temperature perturbation, which can arise from incoming and scattered surface wave interference. The growing (unstable) modes of the temperature distribution along the surface may be responsible for the LIPSS (Laser Induced Periodic Surface Structures) formation. After the end of the laser pulse and before the complete coupling between lattice and electrons occurs, the evolution of the amplitude of the subsequent modulation in the lattice temperature reveals different tendencies depending on the spatial period of the initial modulation. This instability-like behaviour is shown to arise due to the perturbation of the electronic temperature which relaxes slower for bigger spatial periods and thus imparts more significant modulations to the lattice temperature. Small spatial periods of the order of 100 nm and smaller experience stabilization and fast decay from the more efficient lateral heat diffusion which facilitates the relaxation of the electronic temperature amplitude due to in-depth diffusion. An analytical instability analysis of a simplified version of the TTM set of equations supports the lattice temperature modulation behaviour obtained in the simulations and reveals that in-depth diffusion length is a determining parameter in the dispersion relation of unstable modes. Finally it is discussed how the change in optical properties can intensify the modulation-related effects.

physics.optics↗