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1.
Phys Chem Chem Phys ; 17(30): 19751-8, 2015 Aug 14.
Article in English | MEDLINE | ID: mdl-26109211

ABSTRACT

The ability of some materials with a perfectly ordered crystal structure to mimic the heat conduction of amorphous solids is a remarkable physical property that finds applications in numerous areas of materials science, for example, in the search for more efficient thermoelectric materials that enable to directly convert heat into electricity. Here, we unveil the mechanism in which glass-like thermal conductivity emerges in tetrahedrites, a family of natural minerals extensively studied in geology and, more recently, in thermoelectricity. By investigating the lattice dynamics of two tetrahedrites of very close compositions (Cu12Sb2Te2S13 and Cu10Te4S13) but with opposite glasslike and crystal thermal transport by means of powder and single-crystal inelastic neutron scattering, we demonstrate that the former originates from the peculiar chemical environment of the copper atoms giving rise to a strongly anharmonic excess of vibrational states.

2.
Nanoscale ; 7(28): 12030-7, 2015 Jul 28.
Article in English | MEDLINE | ID: mdl-26111776

ABSTRACT

Degenerate metal oxide nanoparticles are promising systems to expand the significant achievements of plasmonics into the infrared (IR) range. Among the possible candidates, Ga-doped ZnO nanocrystals are particularly suited for mid IR, considering their wide range of possible doping levels and thus of plasmon tuning. In the present work, we report on the tunable mid IR plasmon induced in degenerate Ga-doped ZnO nanocrystals. The nanocrystals are produced by a plasma expansion and exhibit unprotected surfaces. Tuning the Ga concentration allows tuning the localized surface plasmon resonance. Moreover, the plasmon resonance is characterized by a large damping. By comparing the plasmon of nanocrystal assemblies to that of nanoparticles dispersed in an alumina matrix, we investigate the possible origins of such damping. We demonstrate that it partially results from the self-organization of the naked particles and also from intrinsic inhomogeneity of dopants.

3.
Phys Chem Chem Phys ; 16(48): 26653-7, 2014 Dec 28.
Article in English | MEDLINE | ID: mdl-25387904

ABSTRACT

Sub-monolayer thin film morphologies obtained by deposition of size-selected CoxPt1-x clusters on graphite have been analyzed for different values of x. In all cases, the preformed clusters can easily diffuse on the surface and gather to form islands of clusters. By changing the cluster stoichiometry, very different morphologies can be obtained, going from large ramified islands to "bunches" of non-contacting incident clusters. We put into evidence that the introduction of platinum atoms in the incident particles drastically changes the interaction between clusters and offers the opportunity to control the coalescence process between them. In this way, by modifying the cluster reactivity, a local self-organization of size-selected magnetic nanoparticles can be achieved.

4.
Nanotechnology ; 24(16): 165703, 2013 Apr 26.
Article in English | MEDLINE | ID: mdl-23535555

ABSTRACT

We investigate the luminescence properties of 10 nm yttrium aluminum garnet (YAG) nanoparticles doped with Ce ions at 0.2%, 4% and 13% that are designed as active probes for scanning near-field optical microscopy. They are produced by a physical method without any subsequent treatment, which is imposed by the desired application. The structural analysis reveals the amorphous nature of the particles, which we relate to some compositional defects as indicated by the elemental analysis. The optimum emission is obtained with a doping level of 4%. The emission of the YAG nanoparticles doped at 0.2% is strongly perturbed by the crystalline disorder whereas the 13% doped particles hardly exhibit any luminescence. In the latter case, the presence of Ce(4+) ions is confirmed, indicating that the Ce concentration is too high to be incorporated efficiently in YAG nanoparticles in the trivalent state. By a unique procedure combining cathodoluminescence and Rutherford backscattering spectrometry, we demonstrate that the enhancement of the particle luminescence yield is not proportional to the doping concentration, the emission enhancement being larger than the Ce concentration increase. Time-resolved photoluminescence reveals the presence of quenching centres likely related to the crystalline disorder as well as the presence of two distinct Ce ion populations. Eventually, nano-cathodoluminescence indicates that the emission and therefore the distribution of the doping Ce ions and of the defects are homogeneous.

5.
J Phys Condens Matter ; 23(44): 442202, 2011 Nov 09.
Article in English | MEDLINE | ID: mdl-21997363

ABSTRACT

Recent ab initio studies have theoretically predicted room temperature ferromagnetism in several oxide materials of the type AO(2) in which the cation A(4+) is substituted by a non-magnetic element of the 1 A column. Our purpose is to address experimentally the possibility of magnetism in Ti(1-x)K(x)O(2) compounds. The samples have been synthesized via the solid state route method at equilibrium. Our study has shown that Ti(1-x)K(x)O(2) is thermodynamically unstable and leads to a phase separation, in contradiction with the hypothesis of ab initio calculations. In particular, the crystalline TiO(2) grains appear to be surrounded by K-based phase. The oxidization state of the Ti ion is found to be in Ti(4+) as confirmed from the x-ray photoelectron spectra measurement. Nevertheless, K:TiO(2) compounds exhibit weak paramagnetism with the highest magnetic moment of ~0.5 µ(B) K(-1) but no long-range ferromagnetic order. The observed moment in these compounds remains much smaller than the predicted moment of 3 µ(B) by ab initio calculation. The apparent contradictions between our experiments and first-principles studies are discussed.

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