The main features of ultra-short laser ablation of various materials (metals, semiconductors or insulators) have been studied through the complementary analyses of the plasma plume induced by laser irradiation, and of the deposited films. The generation of nanoparticles (in the 10–100 nm range) was observed and these findings were investigated in order to obtain information on the relevant parameters governing the formation of these nanoparticles. By the use of polyatomic targets, the non-congruent formation of nanoparticles was evidenced, demonstrating the existence of complex phenomena (phase separation, chemical reactions and interaction with the residual gas) during the laser–matter interaction and plasma expansion. An unexpected finding was the influence of the laser beam spot size on nanoparticle emission during femtosecond laser ablation. The comparison of these results with the currently admitted explanations of ultra-short laser–matter interactions clearly indicates that the existing models and simulations do not describe or explain the overall phenomena taking place during femtosecond laser ablation, and another approach has to be envisaged including the influence of the parameters evidenced in this work.
The electronic properties of redox-active transition metal clusters (Re 6 Se 8 ) covalently immobilized on modified Si(111) surfaces through linear alkyl spacers have been studied as a function of the cluster coverage (1 × 10 13 -6 × 10 13 cm -2 ). The latter is controlled by using Si(111)/H surfaces modified by dense mixed alkyl/ acid-terminated monolayers with variable fraction of the acid grafting sites from 5 to 100% in solution. Quantitative X-ray photoemission analysis, spectroscopic ellipsometry, and scanning tunnelling microscopy indicate a covalent attachment of a submonolayer to densely packed monolayer of Re 6 Se 8 clusters, while the vibrational Raman signature confirms the cluster integrity within the monolayer. Electrical band gaps as deduced from scanning tunnelling spectroscopy have been obtained for low Re 6 Se 8 cluster coverage. Using ultraviolet photoemission spectroscopy, electronic properties such as ionization potential changes and energy level alignments at organic/inorganic interfaces are studied. We show that the lowest unoccupied molecular orbital of the Re 6 Se 8 cluster is close to the bottom of the Si conduction band. At high cluster coverage, this affects the current-voltage characteristics measured using a weakly interacting top mercury contact onto the organic monolayer/silicon junctions. Indeed, on n-type silicon, the high level current at low bias and the shape of the conductance G(V) curve indicate a Schottky barrier height lowering. On the other hand, the current-voltage characteristics are the same for both acid-terminated and low coverage Re 6 Se 8 cluster junctions at low bias; the high Schottky barrier height limits the current at low bias. When the forward bias increases, the current is tunnelling limited. As expected from the band alignment deduced from photoemission data, the opposite behavior is obtained on p-type silicon.
Chalcogenide semiconducting systems are of growing interest for mid-temperature range (~500 K) thermoelectric applications. In this work, Ge20Te77Se3 glasses were intentionally crystallized by doping with Cu and Bi. These effectively-crystallized materials of composition (Ge20Te77Se3)100−xMx (M = Cu or Bi; x = 5, 10, 15), obtained by vacuum-melting and quenching techniques, were found to have multiple crystalline phases and exhibit increased electrical conductivity due to excess hole concentration. These materials also have ultra-low thermal conductivity, especially the heavily-doped (Ge20Te77Se3)100−xBix (x = 10, 15) samples, which possess lattice thermal conductivity of ~0.7 Wm−1 K−1 at 525 K due to the assumable formation of nano-precipitates rich in Bi, which are effective phonon scatterers. Owing to their high metallic behavior, Cu-doped samples did not manifest as low thermal conductivity as Bi-doped samples. The exceptionally low thermal conductivity of the Bi-doped materials did not, alone, significantly enhance the thermoelectric figure of merit, zT. The attempt to improve the thermoelectric properties by crystallizing the chalcogenide glass compositions by excess doping did not yield power factors comparable with the state of the art thermoelectric materials, as these highly electrically conductive crystallized materials could not retain the characteristic high Seebeck coefficient values of semiconducting telluride glasses.
By combining x-ray excited Auger electron diffraction experiments and multiple scattering calculations we reveal a layer-resolved shift for the Mg KL23L23 Auger transition in MgO ultrathin films (4-6 Å) on Ag(001). This resolution is exploited to demonstrate the possibility of controlling Mg atom incorporation at the MgO/Ag(001) interface by exposing the MgO films to a Mg flux. A substantial reduction of the MgO/Ag(001) work function is observed during the exposition phase and reflects both band-offset variations at the interface and band bending effects in the oxide film.
Spatial and temporal distributions of species emitted from ablation of zinc oxide target by a pulsed-electron beam are studied by the complementary use of optical emission spectroscopy and camera fast imaging. We show that the slowest electrons produced by the accelerating tube in the pulsed-electron beam deposition (PED) system interact with the plasma plume and involve a further excitation of the neutrals species. The velocities of atoms and ions are found to be similar to those obtained in the well-known pulsed-laser deposition (PLD) process while the plasma temperature and the electron density are lower. The low absorption of the electron beam by the expanding plasma compared with that experienced in PLD leads to a higher removal of ablated material and consequently to a higher deposition rate ten times greater than in PLD. The PED ZnO films grown at room temperature on silicon substrate are constituted by the stacking of small aggregates without large macroscopic droplets. These results are in agreement with the ICCD images recorded at long time delays from the electron impact which do not evidence bright trails correlated with the propagation of slow and large particles.
PbTe based materials are well known for their high performance thermoelectric properties. Here, a systematic study of thermoelectric transport properties of n-type Pb-deficit Pb0.98-xSbxTe alloys with carrier concentrations in the range of 10 -19 cm -3 is presented from room temperature to 623 K. A maximum thermoelectric figure of merit (zT) of 0.81 was achieved at 623 K for 4 mol% Sb containing Pb-deficit composition, by the cumulative integration of enhanced power factor and significant reduction in thermal conductivity. The scattering of phonons at Pb vacancies, contributed to the reduction of lattice thermal conductivity, and thereby strikingly boosted the zT of the Pb-deficit samples when compared with the pristine Pb1-xSbxTe.
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