RESUMO
Crystallization is a fundamental process in materials science, providing the primary route for the realization of a wide range of new materials. Crystallization rates are also considered to be useful probes of glass-forming ability1-3. At the microscopic level, crystallization is described by the classical crystal nucleation and growth theories4,5, yet in general solid formation is a far more complex process. In particular, the observation of apparently different crystal growth regimes in many binary liquid mixtures greatly challenges our understanding of crystallization1,6-12. Here, we study by experiments, theory and computer simulations the crystallization of supercooled mixtures of argon and krypton, showing that crystal growth rates in these systems can be reconciled with existing crystal growth models only by explicitly accounting for the non-ideality of the mixtures. Our results highlight the importance of thermodynamic aspects in describing the crystal growth kinetics, providing a substantial step towards a more sophisticated theory of crystal growth.
RESUMO
The dynamics of color centers, being a promising quantum technology, is strongly dependent on the local environment. A synergistic approach of X-ray fluorescence analysis and X-ray excited optical luminescence (XEOL) using a hard X-ray nanoprobe is applied. The simultaneous acquisition provides insights into compositional and functional variations at the nanoscale demonstrating the extraordinary capabilities of these combined techniques. The findings on cobalt doped zinc oxide nanowires show an anticorrelation between the band edge emission of the zinc oxide host and the intra-3d cobalt luminescence, indicating two competing recombination paths. Moreover, time-resolved XEOL measurements reveal two exponential decays of the cobalt luminescence. The fast and newly observed one can be attributed to a recombination cascade within the cobalt atom, resulting from direct excitation. Thus, this opens a new fast timescale for potential devices based on cobalt color centers in ZnO nanowires in photonic circuits.
RESUMO
Nanowire chip-based electrical and optical devices such as biochemical sensors, physical detectors, or light emitters combine outstanding functionality with a small footprint, reducing expensive material and energy consumption. The core functionality of many nanowire-based devices is embedded in their p-n junctions. To fully unleash their potential, such nanowire-based devices require - besides a high performance - stability and reliability. Here, we report on an axial p-n junction GaAs nanowire X-ray detector that enables ultra-high spatial resolution (~200 nm) compared to micron scale conventional ones. In-operando X-ray analytical techniques based on a focused synchrotron X-ray nanobeam allow probing the internal electrical field and observing hot electron effects at the nanoscale. Finally, we study device stability and find a selective hot electron induced oxidization in the n-doped segment of the p-n junction. Our findings demonstrate capabilities and limitations of p-n junction nanowires, providing insight for further improvement and eventual integration into on-chip devices.
RESUMO
Chalcogenide Cu(In,Ga)Se2 solar cells yield one of the highest efficiencies among all thin-film photovoltaics. However, the variability of the absorber compositions and incorporated alkali elements strongly affect the conversion efficiency. Thus, effective strategies for spatially resolved tracking of the alkali concentration and composition during operation are needed to alleviate this limitation. Here, using a hard X-ray nanoprobe, we apply a synergistic approach of X-ray fluorescence analysis and X-ray beam-induced current techniques under operando conditions. The simultaneous monitoring of both compositional and functional properties in complete solar cells illustrates the exceptional capabilities of this combination of techniques in top-view geometry, where high spatial resolution resulted even underneath the electrical contacts. Our observations reveal Rb agglomerations in selected areas and compositional variations between different grains and their boundaries. The concurrent detection of the functionality exhibits negligible effects on the collection efficiency for Rb-enriched grain boundaries in comparison to their neighboring grains, which indicates the passivation of detrimental defects.
RESUMO
Thin-film solar cells based on Cu(In,Ga)Se2 (CIGS) absorbers have achieved conversion efficiencies close to 23%. Such a high performance could be reached by incorporating heavy alkali elements into the CIGS absorber using an alkali fluoride post-deposition treatment (PDT). In order to improve the understanding of the effect of the PDT, we investigated a highly efficient CIGS solar cell whose absorber was subjected to a RbF-PDT. By applying synchrotron-based X-ray fluorescence analysis in combination with scanning transmission electron microscopy and electron backscatter diffraction to a cross-sectional lamella of the whole device, we were able to correlate the local composition of the absorber with its microstructure. The incorporated Rb accumulates at grain boundaries, with a random misorientation of the adjacent grains, at the p-n junction, and at the interface between the absorber and the MoSe2 layer. The accumulation of Rb at the grain boundaries is accompanied by a reduced Cu concentration and slightly increased In and Se concentrations. Additionally, variations in the local composition of the absorber at the p-n junction indicate the formation of a secondary phase, which exhibits a laterally inhomogeneous distribution. The improved solar cell performance due to RbF-PDT can thus be expected to originate from a favorable modification of the back contact interface, the random grain boundaries, the p-n junction, or a combination of these effects.