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Register a new userIn situ synthesis of polyynes in a polymer matrix by pulsed laser ablation in liquid
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Added by
Carlo Spartaco Casari
Publication date
2020
fields
Physics
and research's language is
English
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Polyynes are finite chains formed by sp-hybridized carbon atoms with alternating single and triple bonds and displaying intriguing electronic and optical properties. Pulsed laser ablation in liquid (PLAL) is a well assessed technique for the physical synthesis of hydrogen-capped polyynes in solution, however, their limited stability prevents further exploitation in materials for different applications. In this work, polyynes in poly(vinyl alcohol) (PVA) were produced in a single-step PLAL process by ablating graphite directly in aqueous solution of PVA, investigating the role of polymer concentration. The presence of PVA solution, as a participating medium for PLAL, is shown to favour the formation of polyynes. The addition of Ag colloids to the aqueous PVA/polyynes solution allowed surface-enhanced Raman spectroscopy (SERS) measurements, carried out both on liquid samples and on free-standing nanocomposites, obtained after solvent evaporation. We show that polyynes in the nanocomposite remain stable at least for 11 months, whereas the corresponding PVA/Ag/polyynes solution displayed a strong polyyne reduction already after 3 weeks. These results open the view to further characterizations of the properties of polyyne-based films and materials.
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In recent years there has been a growing interest in sp-carbon chains as possible novel nanostructures. An example of sp-carbon chains are the so-called polyynes, characterized by the alternation of single and triple bonds that can be synthesized by pulsed laser ablation in liquid (PLAL) of a graphite target. In this work, by exploiting different solvents in the PLAL process, e.g. water, acetonitrile, methanol, ethanol, and isopropanol, we systematically investigate the solvent role in polyyne formation and stability. The presence of methyland cyano-groups in the solutions influences the termination of polyynes, allowing to detect, in addition to hydrogen-capped polyynes up to HC22H, methyl-capped polyynes up to 18 carbon atoms (i.e. HCnCH3) and cyanopolyynes up to HC12CN. The assignment of each species was done by UV-Vis spectroscopy and supported by density functional theory simulations of vibronic spectra. In addition, surface-enhanced Raman spectroscopy allowed to observe differences, due to different terminations (hydrogen, methyl-and cyano group), in the shape and positions of the characteristic Raman bands of the size-selected polyynes. The evolution in time of each polyyne has been investigated evaluating the chromatographic peak area, and the effect of size, terminations and solvents on polyynes stability has been individuated.
We report on how different cluster deposition regimes can be obtained and observed by in situ Scanning Tunneling Microscopy (STM) by exploiting deposition parameters in a pulsed laser deposition (PLD) process. Tungsten clusters were produced by nanosecond Pulsed Laser Ablation in Ar atmosphere at different pressures and deposited on Au(111) and HOPG surfaces. Deposition regimes including cluster deposition-diffusion-aggregation (DDA), cluster melting and coalescence and cluster implantation were observed, depending on background gas pressure and target-to-substrate distance which influence the kinetic energy of the ablated species. These parameters can thus be easily employed for surface modification by cluster bombardment, deposition of supported clusters and growth of films with different morphologies. The variation in cluster mobility on different substrates and its influence on aggregation and growth mechanisms has also been investigated.
Ge-Sn alloys with a sufficiently high concentration of Sn is a direct bandgap group IV material. Recently, ion implantation followed by pulsed laser melting has been shown to be a promising method to realize this material due to its high reproducibility and precursor-free process. A Ge-Sn alloy with ~9 at.% Sn was shown to be feasible by this technique. However, the compressive strain, inherently occurring in heterogeneous epitaxy of the film, evidently delays the material from the direct bandgap transition. In this report, an attempt to synthesize a highly-relaxed Ge-Sn alloy will be presented. The idea is to produce a significantly thicker film with a higher implant energy and doses. X-ray reciprocal space mapping confirms that the material is largely-relaxed. The peak Sn concentration of the highest dose sample is 6 at.% as determined by Rutherford backscattering spectrometry. Cross-sectional transmission electron microscopy shows unconventional defects in the film as the mechanism for the strain relaxation. Finally, a photoluminescence (PL) study of the strain-relaxed alloys shows photon emission at a wavelength of 2045 nm, suggesting an active incorporation of Sn concentration of ~6 at.%. The results of this study pave way to produce high quality relaxed GeSn alloy using an industrially scalable method.
Organometal trihalide perovskite solar cells have been rapidly developed and attracted much attention in recent years due to their high photoelectric conversion efficiency and low cost. Pulsed laser deposition (PLD) is a widely adopted technology which is used in the preparation of thin films, especially oxide thin films. With this technology, the thickness and composition of films can be conveniently and accurately controlled. In the structure of perovskite solar cells, TiO$_2$ layer working as the n-type semiconductor is used to block holes and transport electrons into electrode, which is crucial for the performance of whole devices. We introduced the PLD technique into preparation of TiO$_2$ layer. In comparison with common spin coating method, TiO$_2$ layer prepared by this technique is ultrathin and more compact. Compact TiO$_2$ (c-TiO$_2$) layers with optimized thickness of 32 nm have been prepared by the PLD method and the highest efficiency of 13.95 % for the MAPbI$_3$-based solar cell devices has been achieved.
Laser-cleaning of the electrodes in a planar micro-fabricated ion trap has been attempted using ns pulses from a tripled Nd:YAG laser at 355nm. The effect of the laser pulses at several energy density levels has been tested by measuring the heating rate of a single 40Ca+ trapped ion as a function of its secular frequency. A reduction of the electric-field noise spectral density by ~50% has been observed and a change in the frequency dependence also noticed. This is the first reported experiment where the anomalous heating phenomenon has been reduced by removing the source as opposed to reducing its thermal driving by cryogenic cooling. This technique may open the way to better control of the electrode surface quality in ion microtraps.
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