HiLASE

Publications

Jan Hrabovský, Lukáš Střižík, Frédéric Désévédavy, Stana Tazlaru, Miroslav Kučera, Lukáš Nowak, Robin Kryštůfek, Jan Mistrík, Václav Dědič, Vladimír Kopecký, Grégory Gadrét, Thomas Wagner, Frédéric Smektala, Martin Veis

The presented work is focused on the optical and magneto-optical characterization of TeO2-ZnO-BaO (TZB) tellurite glasses. We investigated the refractive index and extinction coefficient dispersion by spectroscopic ellipsometry from ultraviolet, λ ≈ 0.193 μm, up to mid-infrared, λ ≈ 25 μm spectral region. Studied glasses exhibited large values of linear (n632 ≈ 1.91–2.09) and non-linear refractive index (n2 ≈ 1.20–2.67×10−11 esu), Verdet constant (V632 ≈ 22–33 radT−1m−1) and optical band gap energy (Eg ≈ 3.7–4.1 eV). The materials characterization revealed that BaO substitution by ZnO leads (at constant content of TeO2) to an increase in linear and nonlinear refractive index as well as Verdet constant while the optical band gap energy decreases. Fiber drawing ability of TeO2–ZnO–BaO glassy system has been demonstrated on 60TeO2–20ZnO–20BaO glass with presented mid-infrared attenuation coefficient. Specific parameters such as dispersion and single oscillator energy, Abbe number, and first-/third-order optical susceptibility are enclosed together with the values of magneto-optic anomaly derived from the calculation of measured dispersion of the refractive index.

Yury V. Ryabchikov, Alexander Zaderko

Fluorescent carbon nanodots are a promising nanomaterial for different applications in biophotonics, sensing and optical nanothermometry fields due to their strong fluorescence properties. However, their multi-modal applications are considerably limited, requiring the use of several nanoagents that could solve different tasks simultaneously. In this paper, we report the first experimental results on a facile “green” laser-based synthesis of multi-modal carbon–metallic nanocomposites with tuned optical performance. This simple approach leads to the appearance of finely controlled plasmonic properties in carbon-based nanocomposites whose spectral position is adapted by using an appropriate material. Thus, longer laser ablation provokes 29-fold increase in the absorption intensity of carbon–gold nanocomposites due to the increase in the metal content from 13% (30 s) to 53% (600 s). Despite strong plasmonic properties, the metal presence results in the quenching of the carbon nanostructures’ fluorescence (2.4-fold for C-Au NCs and 3.6-fold for C-Ag NCs for 600 s ablation time). Plasmonic nanocomposites with variable metal content reveal a ~3-fold increase in the laser-to-heat conversion efficiency of carbon nanodots matching the temperature range for mild hyperthermia applications. The findings presented demonstrate a facile approach to expanding the properties of chemically prepared semiconductor nanostructures due to the formation of novel semiconductor–metallic nanocomposites using a “green” approach. Together with the ease in control of their performance, it can considerably increase the impact of semiconductor nanomaterials in various photonic, plasmonic and biomedical applications.

Yuzhu Cheng, Alexander V. Bulgakov, Nadezhda M. Bulgakova, Jiří Beránek, Martin Zukerstein, Ilya A. Milekhin, Alexander A. Popov, Vladimir A. Volodin

Amorphous germanium films on nonrefractory glass substrates were annealed by ultrashort near-infrared (1030 nm, 1.4 ps) and mid-infrared (1500 nm, 70 fs) laser pulses. Crystallization of germanium irradiated at a laser energy density (fluence) range from 25 to 400 mJ/cm2 under single-shot and multishot conditions was investigated using Raman spectroscopy. The dependence of the fraction of the crystalline phase on the fluence was obtained for picosecond and femtosecond laser annealing. The regimes of almost complete crystallization of germanium films over the entire thickness were obtained (from the analysis of Raman spectra with excitation of 785 nm laser). The possibility of scanning laser processing is shown, which can be used to create films of micro- and nanocrystalline germanium on flexible substrates.

Inam Mirza, Alexander V. Bulgakov, Hanna Sopha, Sergey V. Starinskiy, Hana Turčičová, Ondřej Novák, Jiří Mužík, Martin Smrž, Vladimir A. Volodin, Tomáš Mocek, Jan M. Macak, Nadezhda M. Bulgakova

As-prepared nanostructured semiconductor materials are usually found in an amorphous form, which needs to be converted into a crystalline one for improving electronic properties and achieving enhanced application functionalities. The most utilized method is thermal annealing in a furnace, which however is time- and energy-consuming and not applicable for low-temperature melting substrates. An alternative is laser annealing, which can be carried out in a relatively short time and, additionally, offers the possibility of annealing localized areas. However, laser-annealed nanostructures are often distorted by melting, while preserving the as-prepared morphology is essential for practical applications. In this work, we analyze conditions of non-thermal ultrafast laser annealing of two kinds of nanostructures: anodic TiO2 nanotube layers and Ge/Si multilayer stacks. For both cases, regimes of crystallization have been found, which yield in preserving the initial nanomaterial morphologies without any melting signs. On these examples, ultrafast non-thermal mechanisms of structural material transformation are discussed, which can provide new opportunities for conversion of amorphous semiconductor nanomaterials into a desired crystalline form that is of high demand for existing and emerging technologies.

Ondřej Stránský, Sunil Pathak, Jan Kaufman, Marek Böhm, Jaromír Kopeček, Libor Beránek, František Holeškovský, Šimon Petrášek, Lucie Hlavůňková, Zbyněk Soukup

Laser powder bed fusion (L-PBF) has emerged as one of the most promising technologies for producing complex geometries that are difficult to achieve with other methods. However, its widespread adoption is hindered by issues such as deleterious microstructure, tensile residual stresses, and porous structure, mainly while working with aluminum alloys. To address these challenges, laser shock peening (LSP) offers a potential solution by mitigating the negative effects associated with aluminum L-PBF. This study investigates the impact of the important LSP parameters, namely energy, spot size, and overlap on L-PBF printed thin AlSi10Mg tubes. A total of 17 specimens were examined by varying the mentioned parameters at three levels each. The outcome of the study was evaluated in terms of residual stresses, porosity, microstructure and surface roughness. The results have shown significant improvements in residual stresses, where a maximum improvement of over 200 % was observed and a decrease in porosity by 70 %. Furthermore, the microstructure analysis revealed grain refinement and dislocation redistribution as material reactions, aligning with the observed microhardness increase. These findings demonstrate the viability of LSP as a post-processing method for demanding applications, effectively addressing the limitations of the L-PBF process.

Ultrapure composite nanostructures combining semiconductor and metallic elements as a result of ultrafast laser processing are important materials for applications in fields where high chemical purity is a crucial point. Such nanocrystals have already demonstrated prospects in plasmonic biosensing by detecting different analytes like dyes and bacteria. However, the structure of the nanocomposites, as well as the control of their properties, are still very challenging due to the significant lack of research in this area. In this paper, the synthesis of silicon–gold nanoparticles was performed using various approaches such as the direct ablation of (i) a gold target immersed in a colloidal solution of silicon nanoparticles and (ii) a silicon wafer immersed in a colloidal solution of plasmonic nanoparticles. The formed nanostructures combine both plasmonic (gold) and paramagnetic (silicon) modalities observed by absorbance and electron paramagnetic resonance spectroscopies, respectively. A significant narrowing of the size distributions of both types of two-element nanocrystals as compared to single-element ones is shown to be independent of the laser fluence. The impact of the laser ablation time on the chemical stability and the concentration of nanoparticles influencing their both optical properties and electrical conductivity was studied. The obtained results are important from a fundamental point of view for a better understanding of the laser-assisted synthesis of semiconductor–metallic nanocomposites and control of their properties for further applications.

Ondřej Slezák, David Vojna, Jan Pilař, Martin Divoký, Ondřej Denk, Martin Hanuš, Petr Navrátil, Martin Smrž, Antonio Lucianetti, Tomáš Mocek

The authors report the first-ever demonstration of the optical isolation of a kilowatt average power pulsed laser. A Faraday isolator capable of stable protection of the laser amplifier chain delivering 100 J nanosecond laser pulses at the repetition rate of 10 Hz has been developed and successfully tested. The isolator provided an isolation ratio of 30.46 dB in the course of an hour-long testing run at full power without any noticeable decrease due to the thermal effects. This is the first-ever demonstration of a nonreciprocal optical device operated with such a powerful high-energy, high-repetition-rate laser beam, opening up the possibilities for this type of lasers to be used for a number of industrial and scientific applications.

Jan Hrabovský, Michal Zelenský, Juraj Sládek, Martin Zukerstein, Jan Fischer, Karolina Schwarzová-Pecková, Andrew Taylor, Martin Veis, Soumen Mandal, Oliver Williams, Nadezhda Bulgakova

A thorough study on sp3 to sp2 carbon conversion in undoped and boron-doped diamond (BDD) thin (≈ 500 nm) layers leading to the desired sp2/sp3 carbon ratio and lateral distribution, which utilizes boron atom incorporation and infrared (IR) material laser processing has been performed. Polycrystalline as-grown (AG) or chem-mechanically polished (CMP) undoped diamond/BDD layers were investigated with respect to boron content and laser wavelength (800, 1030 nm). Boron incorporation leads to an increase in IR optical absorption and reduction of required energy fluence (?th ≈ 1 J cm−2 ) needed for sp3 to sp2 carbon conversion. Raman spectroscopy was performed to identify carbon conversion stages and to tailor the ideal parameters for other IR laser sources and required sp2/sp3 carbon ratio. Electrochemical parameters (??p and ?Ap/?Cp ratio) were obtained from cyclic voltammetry measurements of outer-([Ru(NH3 )6 ] 3+/2+) and inner-([Fe(CN)6 ] 3−/4−) sphere redox markers. Values of ??p and ?Ap/?Cp are mainly influenced after conversion of 10% of sp3 to sp2 carbon. This trend is most pronounced for the [Fe(CN)6 ] 3−/4− redox marker, by decrease or increase of these parameters on AG or CMP BDD electrodes respectively. Electrochemical findings were supported by electrochemical impedance spectroscopy where ?ct keeps the same trend as ??p values and double layer capacitance profoundly increases between 10 and 25% of surface conversion.

Xiang Yao, Christof W. Schneider, Nadezhda M. Bulgakova, Alexander V. Bulgakov, Thomas Lipper

The electric field driven acceleration of plasma ions is an intrinsic effect in laser-induced plasma plumes and is responsible for the generation of high-energy ions. At high laser fluences (≥ 2 J/cm2), multiply charged ions are formed and affect the plume expansion dynamics. In this paper, we used kinetic energy-resolved mass spectrometry to investigate the relative abundance and kinetic energy distributions of singly- and doubly-charged ions produced by KrF-laser ablation of nine different oxide targets. The doubly charged metal ions with a lower mass-to-charge (m/z) ratio show narrow energy distributions at high average kinetic energies coinciding with the cutoff energies for the singly-charged ion distributions. The observation suggests that the recombination of higher charged ions plays a prominent role in the formation of the high-energy tail for singly-charged ions. The results are discussed in terms of component volatility and a dynamic double layer, where ions with different m/z values experience different accelerations.

Martin Zukerstein, Vladimir P. Zhukov, Yuri P. Meshcheryakov, Nadezhda M. Bulgakova

Volumetric modification of transparent materials by femtosecond laser pulses is successfully used in a wide range of practical applications. The level of modification is determined by the locally absorbed energy density, which depends on numerous factors. In this work, it is shown experimentally and theoretically that, in a certain range of laser pulse energies, the peak of absorption of laser radiation for doughnut-shaped (DS) pulses is several times higher than for Gaussian ones. This fact makes the DS pulses very attractive for material modification and direct laser writing applications. Details of the interactions of laser pulses of Gaussian and doughnut shapes with fused silica obtained by numerical simulations are presented for different pulse energies and compared with the experimentally obtained data. The effect of absorbed energy delocalization with increasing laser pulse energy is demonstrated for both beam shapes, while at relatively low pulse energies, the DS beam geometry provides stronger local absorption compared to the Gaussian geometry. The implications of a DS pulse action for post-irradiation material evolution are discussed based on thermoelastoplastic modeling.

Sergey Ya. Khmel, Sergey V. Starinskiy, Evgeniy A. Baranov, Alexandr O. Zamchiy, Alexey I. Safonov, Yuri G. Shukhov, Alexander V. Bulgakov

The optical properties of noble metal nanoparticles (NPs) can be efficiently controlled by their incorporation into host matrix films. Here, we report on the fabrication of composite films of gold NPs in a silicon suboxide matrix by a novel approach using a combination of pulsed laser deposition for NP production and gas-jet, electron-beam plasma chemical vapor deposition for low-temperature (300°C) synthesis of a SiOx (x = 0.38-1.55) thin film as a matrix for the NPs. The produced nanocomposite exhibits unexpected plasmonic properties, non-monotonically dependent on the matrix thickness, due to a porous columnar matrix structure grown from the NPs with variable oxygen content along the columns. This implies that low-temperature, gold-catalyzed oxidation of silicon occurs during the structure growth. Calculations based on Mie theory show that the refractive index of the obtained SiOx matrix can be as low as 1.2 at certain film thicknesses. Mechanisms of the columnar structure formation at different deposition stages are discussed. The synthesis approach can be used for the fabrication of optical thin-film materials with controllable low refractive index.

Jose Guadalupe Quiñones-Galvan, Inam Mirza, Jan Hrabovský, Enrique Campos-Gonzalez, Francisco de Moure-Flores, Jose Santos-Cruz, Miguel Angel Santana-Aranda, Alexander V. Bulgakov , Nadezhda M. Bulgakova

MoS2 thin films were grown by the pulsed laser deposition technique using a picosecond laser at a wavelength of 1030 nm. The plasma ion mean kinetic energy and density were estimated from the time-of-flight distributions measured using a Langmuir planar probe. It has been found that the mean kinetic energy decreases with increasing the laser pulse energy. This unusual effect is explained by the difference in the volatility of the vaporized species. Samples were structurally characterized by Raman spectroscopy and grazing angle X-ray diffraction. It was found that thin films of amorphous matrices containing MoS2 nanocrystallites were grown. Optical characterization carried out by UV-vis spectroscopy yielded transmittance values above 90% in the visible spectral range and an indirect electronic transition at 1.4 eV. Chemical oxidation states for molybdenum and sulfur were analyzed by means of X-ray photoelectron emission spectroscopy, which revealed Mo-S bonding states, confirming the growth of MoS2.

Petr Hauschwitz, Markéta Klíčová, Senta Müllerová, Radka Bičišťová, Martin Procházka, Jan Brajer, Michal Chyla, Martin Smrž, Jiří Chvojka, Tomáš Mocek

Biocompatibility is one of the key issues for implants, especially in the case of stainless steel with medium to low biocompatibility, which may lead to a lack of osseointegration and consequently to implant failure or rejection. To precisely control preferential cell growth sites and, consequently, the biocompatibility of prosthetic devices, two types of surfaces were analyzed, containing periodic nanogrooves laser induced periodic surface structure (LIPSS) and square-shaped micropillars. For the fast and efficient production of these surfaces, the unique combination of high energy ultrashort pulsed laser system with multi-beam and beamshaping technology was applied, resulting in increased productivity by 526% for micropillars and 14 570% for LIPSS compared to single beam methods. In vitro analysis revealed that micro and nanostructured surfaces provide a better environment for cell attachment and proliferation compared to untreated ones, showing an increase of up to 496% in the number of cells compared to the reference. Moreover, the combination of LIPSS and micropillars resulted in a precise cell orientation along the periodic microgroove pattern. The combination of these results demonstrates the possibility of mass production of functionalized implants with control over cell organization and growth. Thus, reducing the risk of implant failure due to low biocompatibility.

Xiang Yao, Christof W. Schneider, Nadezhda M. Bulgakova, Alexander V. Bulgakov, Thomas Lippert

Ablation of multi-elemental materials by nanosecond lasers is often used to deposit oxide thin films. Understanding the ablation plume dynamics is of utmost importance to gain a detailed insight into thin film growth of materials with a complex composition. In this study, the plume expansion dynamics of several compound materials (AuCu, La0.33Ca0.67MnO3, and LiMn2O4) were characterized by measuring the angular-dependent kinetic energy (KE) distributions of ionic plasma species produced by KrF- and XeCl-excimer laser ablation in vacuum. The distributions of the lightest plume ions were found to differ fundamentally from those of other ions. The latter are similar to the energy distributions observed in single-component plumes and represent a low-energy peak and high-energy tail, while those for the lightest ions consist of at least two distinct peaks. These observations can be explained by assuming the formation of a dynamic double layer (DL) at the front of the plasma giving rise to different acceleration rates for light and heavier ions. As a consequence, heavier elements stay longer within the dynamic DL and gain larger KEs that leads to the observed ion separation. Extending these considerations into three dimensions yields an anisotropic acceleration concept for the plasma ions with high acceleration rates and longer presence within the DL normal to the target surface and lower acceleration rates and shorter time in the parallel direction.

Sunil Pathak, Marek Böhm, Jan Kaufman, Jaromír Kopeček, Sanin Zulić, Ondřej Stránský, Jan Brajer, Libor Beránek, Tomáš Mocek

The work describes the influence of underwater laser shock peening without coating (LSPwC) on selective laser melting manufactured meso-size (outside diameter ≤ 10 mm) helical gears. Five experiments were conducted using energies in the 200 mJ up to 1 J, while the spot size and overlap were kept constant as 1 mm and 90 %, respectively. Responses were measured and compared in terms of surface residual stresses, surface roughness, and microstructure of LSPwC-treated samples. Results show the development of significant compressive residual stresses in the root of the LSPwC processed helical gear, where it changes the state from tensile +45 MPa to compressive −421 MPa. Surface roughness has shown improvement, while volumetric material peak confirms the reduction by over 50%. Microstructure study was performed at the surface and by cross-section using scanning electron microscopy and electron backscatter diffraction analysis. The grain refinement and change in misorientation were observed, confirming plastic deformation.

Yury Ryabchikov

The design of luminescent multi-functional nanoplatforms that can be simultaneously employed for various applications is still an important research task nowadays. Nanosilicon is one of the most promising nanomaterial having unique structural and optoelectronic properties that can be used in biomedicine, optoelectronics, sensing and nanothermometry. However, its properties do not allow the creation of one luminescent multi-functional nanoplatform requiring merging of different nanomaterials. In this work, temperature-sensitive silicon-based nanocomposites with tuned multi-band emission are demonstrated. One can easily achieve the change of their single- and multi-band photoluminescence spectral position from ∼1.6 eV to ∼2.9 eV by varying the experimental parameters. Moreover, the “white” emission of silicon nitride is also observed that can be further applied for sensing or optoelectronic applications. Furthermore, the presence of silver nanoparticles leads to 80% increase of the temperature sensitivity of the photoluminescence maximum position (from ∼540 μeV/°C to ∼975 μeV/°C). The plasmonic nanostructures also considerably modify the ratiometric temperature behavior of nanocomposite emission. The shown findings suggest perspectives of silicon-based nanostructures as multi-task luminescent nanoplatforms in the fields of nanothermometry, molecule sensing, optoelectronics and biomedicine.

We experimentally investigate the spectral broadening in fused silica in the multiphoton absorption regime. Under standard conditions of laser irradiation, linear polarization of laser pulses is more advantageous for supercontinuum generation. However, with high non-linear absorption, we observe more efficient spectral broadening for circular polarizations for both Gaussian and doughnut-shaped beams. The multiphoton absorption in fused silica is studied by measuring the total transmission of laser pulses and by the intensity dependence of the self-trapped exciton luminescence observation. The strong polarization dependence of multiphoton transitions fundamentally affects the broadening of the spectrum in solids.

Sami Slimi, Venkatesan Jambunathan, Mingyan Pan, Yicheng Wang, Weidong Chen, Pavel Loiko, Rosa Maria Solé, Magdalena Aguiló, Francesc Díaz, Martin Smrž, Tomáš Mocek, Xavier Mateos

We report on the continuous-wave and passively Q-switched operation of a compositionally “mixed” heavily doped 16.6 at.% Yb:(Y,Lu)3Al5O12 garnet crystal at cryogenic temperatures (100–200 K), pumped by a volume Bragg grating stabilized diode laser emitting at 969 nm. At 140 K, in the continuous-wave regime, a maximum output power of 10.65 W was achieved at ~ 1029 nm with a slope efficiency of 56% (versus the incident pump power), a laser threshold of 1.05 W and excellent beam quality. Using Cr4+:YAG as a saturable absorber, the passively Q-switched laser generated pulses with an energy/duration of 0.15 mJ/201 ns, respectively, at a repetition rate of 39.7 kHz, corresponding to a peak power of 0.39 kW.

We report a simple and efficient two-step experimental procedure of glass metallization using laser microstructuring at ambient conditions. An adhesive pattern was created on the glass substrate using a laser, which imposes mechanical interlocking. An adhesive Cu layer was deposited on the glass substrate by magnetron sputtering and then electroplated with a functional Cu layer. Due to the unique surface structure created on the glass using laser, we achieved a thick layer of Cu metal film with high adhesion strength, well-defined grains and grain boundaries, and low surface roughness. The total thickness of the grown film was 11.4 µm, with an average surface roughness of 1.2 µm. The magnetron-sputtered coating did not show delamination from the glass substrate at a critical load of 60 N. The proposed method of glass metallization will lead to the realization of glass-based circuit materials that can be used in high-frequency electronic devices. Also, this procedure will be an alternative to chemical-based copper plating, which involves multiple processing steps and high-cost chemicals.

Thibault J. -Y. Derrien, Yoann Levy, Nadezhda M. Bulgakova

Short and ultrashort laser pulses are nowadays an integral part of up-to-date technological solutions in many areas from material micro-/nanoprocessing and synthesis of new materials to quantum computing and biomedicine. The number of laser applications in science and industries is growing precipitously with tendencies of enhancing laser processing precision and reproducibility toward creation of extremely tiny objects. Coupling more laser energy into a smaller material volume in a controllable way is one of the grand challenges, which can only be achieved through a deep understanding of a wealth of the laser-triggered transient processes at different spatiotemporal scales. The objective of this chapter is to provide a review of the main fundamental linear and nonlinear processes excited by ultrafast lasers in different kinds of materials with the aim to reveal and highlight possible mechanisms, which would enable extreme localization of energy absorption. After summarizing existing knowledge on laser-induced phenomena that includes mechanisms of laser light absorption, heat transfer peculiarities, energy thermalization at ultrafast time scales, and related hydrodynamic phenomena, an overview is given on novel insights into highly nonequilibrium processes gained in recent years via quantum and molecular dynamics simulations. The fundamental part is followed by an analysis of possible techniques and processes, which could enable extreme localization of laser energy absorption both on the surface of material samples and in the bulk. Finally, as an example of laser energy localization alternating at nanoscale, laser-induced periodic surface structures (LIPSS) are discussed. The multiplicity of the mechanisms is demonstrated via a rigorous theoretical analysis and simulations.

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