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We report on the dynamics of a magnetic-field-driven antiferromagnetic-to-paramagnetic quantum phase transition in monocrystalline Ce3Al via transverse-field muon spin rotation (TF-µSR) experiments down to low temperature of ∼ 80 mK. The quantum phase transition is of a spin-flip type and takes place on the Ce–Al magnetic chains as a result of competition between the indirect exchange and the Zeeman interaction of the Ce moments with the external field, applied along the chain direction (also the direction of the antiferromagnetic axis). The Ce moments are not static at T → 0, but fluctuate in their direction due to the Heisenberg uncertainty principle. Upon applying the magnetic field sweep, the fluctuations exhibit the largest amplitude at the quantum critical point, manifested in a maximum of the muon transverse relaxation rate at the critical field. The quantum nature of fluctuations observed in the TF-µSR experiments is reflected in the temperature independence of the average local magnetic field component along the external magnetic field at the muon stopping site(s) and the muon transverse relaxation rate within the investigated temperature range 1.5 K–80 mK. Quantum fluctuations are fast on the muon Larmor frequency scale, τ 0 < 10–10 s. [ABSTRACT FROM AUTHOR]

Complex intermetallic compounds such as transition metal (TM) aluminides are promising alternatives to expensive Pd-based catalysts, in particular for the semi-hydrogenation of alkynes or alkadienes. Here, we compare the gas-phase butadiene hydrogenation performances of o-Al13Co4(100), m-Al13Fe4(010) and m-Al13Ru4(010) surfaces, whose bulk terminated structural models exhibit similar cluster-like arrangements. Moreover, the effect of the surface orientation is assessed through a comparison between o-Al13Co4(100) and o-Al13Co4(010). As a result, the following room-temperature activity order is determined: Al13Co4(100) < Al13Co4(010) < Al13Ru4(010) < Al13Fe4(010). Moreover, Al13Co4(010) is found to be the most active surface at 110°C, and even more selective to butene (100%) than previously investigated Al13Fe4(010). DFT calculations show that the activity and selectivity results can be rationalized through the determination of butadiene and butene adsorption energies; in contrast, hydrogen adsorption energies do not scale with the catalytic activities. Moreover, the calculation of projected densities of states provides an insight into the Al13TM4 surface electronic structure. Isolating the TM active centers within the Al matrix induces a narrowing of the TM d-band, which leads to the high catalytic performances of Al13TM4 compounds. [ABSTRACT FROM AUTHOR]

The results of an investigation of the electronic structure of the valence band of various Al-based complex intermetallic alloys, carried out using the X-ray emission spectroscopy technique, are presented and discussed. It is shown that the electronic structure results from an interplay between covalency and repulsive interactions that contributes to the formation of a pseudo-gap at the Fermi level in the Al electronic distributions. [ABSTRACT FROM AUTHOR]

Complex intermetallic compounds such as transition metal (TM) aluminides are promising alternatives to expensive Pd-based catalysts, in particular for the semi-hydrogenation of alkynes or alkadienes. Here, we compare the gas-phase butadiene hydrogenation performances of o- Al 13 Co 4 (100), m -Al 13 Fe 4 (010) and m -Al 13 Ru 4 (010) surfaces, whose bulk terminated structural models exhibit similar cluster-like arrangements. Moreover, the effect of the surface orientation is assessed through a comparison between o- Al 13 Co 4 (100) and o- Al 13 Co 4 (010). As a result, the following room-temperature activity order is determined: Al 13 Co 4 (100) < Al 13 Co 4 (010) < Al 13 Ru 4 (010) < Al 13 Fe 4 (010). Moreover, Al 13 Co 4 (010) is found to be the most active surface at 110°C, and even more selective to butene (100%) than previously investigated Al 13 Fe 4 (010). DFT calculations show that the activity and selectivity results can be rationalized through the determination of butadiene and butene adsorption energies; in contrast, hydrogen adsorption energies do not scale with the catalytic activities. Moreover, the calculation of projected densities of states provides an insight into the Al 13 TM 4 surface electronic structure. Isolating the TM active centers within the Al matrix induces a narrowing of the TM d-band, which leads to the high catalytic performances of Al 13 TM 4 compounds.

Following the recent determination of the Al 3 AuIr structure, a new ternary phase has been identified in the Al-Au-Ir phase diagram. It has a chemical composition Al 9 (Au;Ir) 4 with an apparently low gold content. Its crystal structure has been determined with single-crystal X-ray diffraction. The new compound crystallizes in the tetragonal crystal system and has been successfully solved in space group I4 1 /acd (Pearson symbol tI104) with lattice parameters a = 8.6339 (2) and c = 21.8874 (7) Å. Atomic environments are described as well as similarities with the BGa 8 Ir 4 compound.