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

The design of semiconductor-metallic nanostructures using pulsed laser ablation in liquids (PLAL) is a very demanding task for biomedical applications being at an early stage of its development. Only few recent papers show the possibility of such a synthesis of composite nanoparticles as well as their perspectives for biosensing applications. However, mechanisms of the laser-stimulated formation of semiconductor-metallic nanoparticles involving several processes are not clarified yet being considerably depended on experimental conditions. In this work, we demonstrated an impact of the laser irradiation of colloidal solutions of silicon nanoparticles at different exposure time in the presence/absence of a gold target. In particular, longer ablation of the metal led to a stronger plasmonic maximum in silicon nanoparticles at around 520 nm. It also decreased the hydrodynamic size from 165 nm to 85 nm as well as the ξ-potential from –46 mV to –30 mV by increasing the ablation time from 0 s to 600 s. At the same time, the lowest electrical conductivity value (~1.5 μS/cm) of the plasmonic nanocomposites was detected at 120 s irradiation time. The highest concentration of synthesized composite nanoparticles (~3·1011 NPs/mL) was achieved at 180 s ablation time. Another purpose of the paper was to reveal an influence of the used laser irradiation on properties of the colloidal solutions of silicon nanoparticles themselves. It was found a considerable decrease of their absorbance with the increase of the laser exposure time that can be associated with the change of their properties (e.g. concentration, size, oxidation state etc.). Thus, the laser irradiation strongly affects properties of colloidal solutions of silicon nanoparticles that must also be taken into account considering possible mechanisms of the formation of composite nanostructures. Presented in the paper fast optical diagnostic can help to determine properties of colloidal solutions of nanocomposites formed by PLAL prior their biomedical or catalytic applications.

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.

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.

Laser-assisted material processing using ultrafast laser sources is an important and promising research direction aiming surface or volumetric modifications of different materials. In particular, pulsed laser ablation in liquids (PLALs) method allows forming a wide set of nanostructures in the form of colloidal solutions. Recently, this approach has also been demonstrated as an effective facile route of the successful formation of silicon-gold nanoparticles (Si-Au NPs) [1] that extended the application of silicon nanostructures in the field of plasmonics [2]. Nevertheless, the laser-assisted nanosynthesis of multi-element semiconductor-metallic nanoparticles is still challenging being at the initial stage of its development.

Multicomponent nanostructures consisting of several elements have attracted a broad research interest being served for various aspects in the field of biosensing, catalysis, photovoltaics and biomedicine. Their synthesis by a pulsed laser ablation in a water enables eliminating various side effects originated from chemical contamination. Variable experimental conditions lead to tuning plasmonic and magnetic features influenced by physicochemical reactions during synthesis, thus enhancing their functionality. In this work, we performed synthesis of hybrid AuSi nanoparticles (NPs) with novel modalities by ultrashort laser ablation of bulk gold in water containing silicon NPs. The Au/Si atomic ratio in the nanohybrids was finely varied from 0.5 to 3.5 when changing the initial Si NPs concentration in water from 70 µg/mL to 10 µg/mL respectively. It has been found that the laser-fluence-insensitive silicon content depends on the mass of nanohybrids. A high concentration of paramagnetic defects (2.2 ꞏ1018 spin/g) in polycrystalline plasmonic NPs has been achieved. Our findings can open further prospects for plasmonic nanostructures as contrast agents in optical and magnetic resonance imaging techniques, biosensing and cancer theranostics.

Multicomponent nanostructures consisting of several elements have attracted a broad research interest being served for various aspects in the field of biosensing, catalysis, photovoltaics and biomedicine. Their synthesis by a pulsed laser ablation in a water enables eliminating various side effects originated from chemical contamination. Variable experimental conditions lead to tuning plasmonic and magnetic features influenced by physicochemical reactions during synthesis, thus enhancing their functionality. In this work, we performed synthesis of hybrid AuSi nanoparticles (NPs) with novel modalities by ultrashort laser ablation of bulk gold in water containing silicon NPs. The Au/Si atomic ratio in the nanohybrids was finely varied from 0.5 to 3.5 when changing the initial Si NPs concentration in water from 70 µg/mL to 10 µg/mL respectively. It has been found that the laser-fluence-insensitive silicon content depends on the mass of nanohybrids. A high concentration of paramagnetic defects (2.2 ꞏ1018 spin/g) in polycrystalline plasmonic NPs has been achieved. Our findings can open further prospects for plasmonic nanostructures as contrast agents in optical and magnetic resonance imaging techniques, biosensing and cancer theranostics.

An environment-friendly method of pulsed laser ablation in liquids is successfully employed for structural modification of silicon nanoparticles leading to a considerable narrowing of their size distribution accompanied with a reduction of the mean size. Contamination-free conditions of synthesis ensure the chemical purity of formed nanostructures that may reduce toxicity issues. Such a laser-induced modification leads to the appearance of plasmonic properties in semiconductor-based nanomaterials. Their spectral position can easily be varied in the whole visible range. Combined in one nanoparticle properties of semiconductors and noble metals can strongly promote applications of composite laser-synthesized nanoparticles for biosensing (using their plasmonic-based surface-enhanced ability) and bioimaging (using their both optical and magnetic abilities) purposes.

Multicomponent nanostructures consisting of several elements reveal a large research interest being served for various aspects in the field of biomedicine [1, 2]. Combining different elements in a nanoparticle one can easily vary their physicochemical properties in a wide range adjusting their functionality. However, using chemical-based methods for synthesis can considerably obstruct their applications in biomedical fields due to their contamination by chemical residuals. To overcome the aforementioned issues a versatile method of pulsed laser ablation in liquids is widely employed for the synthesis of pure one-and bi-metallic nanostructures widening their functional properties. As a result, they show wide prospects for applications in various fields of biomedicine, eg as contrast agents for magnetic resonance imaging [3, 4]. However, manufacturing of composite metallic-based nanoparticles doped with semiconductor elements by means of pulsed laser ablation method is still challenging being at the early stage of its development. Nevertheless, laser-synthesized metallic-semiconductor nanocomposites have already shown promising perspectives for molecule detection using surface-enhanced Raman scattering (SERS) or infrared absorption techniques (SEIRA) having tracking features as Raman modality or paramagnetic defect labels at the same time [5, 6]. In this work, gold-silicon nanocomposites with dual modalities were fabricated by direct femtosecond laser ablation in deionized water and characterized by structural and optical techniques. A method of chemical content variation is developed allowing fine-tuning of ratio between gold and …

Surfactant-free multifunctional semiconductor-metallic nanostructures possessing several modalities are formed due to laser-induced structural modification of pure silicon nanoparticles in the presence of gold. It results to variable size-dependent chemical composition examined by energy-dispersive X-ray spectroscopy. Laser-synthesized silicon-based nanocomposites exhibit remarkable both plasmonic and paramagnetic properties. Their plasmonic maxima are found to be easily adjusted in the whole visible spectral range. Influence of resonant laser irradiation on spin behaviour of silicon-gold nanoparticles is established. Their spin–lattice and spin–spin relaxation processes are investigated as well. Such multifunctional nanoparticles can reveal a huge potential for different applications in field of nanomedicine, in particular, for biosensing and bioimaging.