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Register a new userDirect observation of the lattice dynamics of transition metals using ultrafast electron diffraction
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We report the lattice dynamics of transition metal thin films by using the ultrafast electron diffraction. We observe a suppression of the diffraction intensity in a few picosecond after the photoexcitation, which is directly interpreted as the lattice heating via the electron-phonon interaction. The electron-phonon coupling constants for Au, Cu and Mo are quantitatively evaluated by employing the two-temperature model, which are consistent with those obtained by optical pump-probe methods. The variation in the lattice dynamics of the transition metals are systematically explained by the strength of the electron-phonon coupling, arising from the elemental dependence of the electronic structure and atomic mass.
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It has been technically challenging to concurrently probe the electrons and the lattices in materials during non-equilibrium processes, allowing their correlations to be determined. Here, in a single set of ultrafast electron diffraction patterns taken on the charge-density-wave (CDW) material 1T-TaSeTe, we discover a temporal shift in the diffraction intensity measurements as a function of scattering angle. With the help of dynamic models and theoretical calculations, we show that the ultrafast electrons probe both the valence-electron and lattice dynamic processes, resulting in the temporal shift measurements. Our results demonstrate unambiguously that the CDW is not merely a result of the periodic lattice deformation ever-present in 1T-TaSeTe but has significant electronic origin. This method demonstrates a novel approach for studying many quantum effects that arise from electron-lattice dephasing in molecules and crystals for next-generation devices.
Accurate low-order structure factors (Fg) measured by quantitative convergent beam electron diffraction (QCBED) were used for validation of different density functional theory (DFT) approximations. 23 low-order Fg were measured by QCBED for the transition metals Cr, Fe, Co, Ni, and Cu, and the transition metal based intermetallic phases {gamma}-TiAl, {beta}-NiAl and {gamma}1-FePd using a multi-beam off-zone axis (MBOZA) method and then compared with Fg calculated ab-initio by DFT using the local spin density approximation (LDA) and LDA+U, and different generalized gradient approximations (GGA) functionals. Different functionals perform very differently for different materials and crystal structures. Among the GGA functionals, PW91 and EV93 achieve the best overall agreement with the experimentally determined low-order Fg for the five metals, while PW91 performs the best for the three intermetallics. The LDA+U approach, through careful selection of U, achieves excellent matches with the experimentally measured Fg for all the metallic systems investigated in this paper. Similar to the band gap for semiconductors, it is proposed that experimentally determined low-order Fg can be used to tune the U term in LDA+U method DFT calculations for metals and intermetallics.
Using femtosecond time-resolved X-ray diffraction, we investigate optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches first-principles calculations and previously measured elastic properties. We find an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. Our study underscores the benefit of using off-axis crystal orientations when optically exciting shear deformations in topological semimetals, allowing one to transiently change their crystal structure and potentially their topological properties.
The scope of magnetic neutron scattering has been expanded by the observation of electronic Dirac dipoles (anapoles) that are polar (parity-odd) and magnetic (time-odd). A zero-magnetization ferromagnet Sm0.976Gd0.024Al2 with a diamond-type structure presents Dirac multipoles at basis-forbidden reflections that include the standard (2, 2, 2) reflection. Magnetic amplitudes measured at four such reflections are in full accord with a structure factor calculated from the appropriate magnetic space group.
We report on ultrafast electron diffraction on high quality single crystal silicon. The ultrafast dynamics of the Bragg peaks exhibits a giant photo-induced response which can only be explained in the framework of dynamical diffraction theory, taking into account multiple scattering of the probing electrons in the sample. In particular, we show that lattice heating following photo-excitation can cause an unexpected increase of the Bragg peak intensities, in contradiction with the well-known Debye-Waller effect. We anticipate that multiple scattering should be systematically considered in ultrafast electron diffraction on high quality crystals as it dominates the Bragg peak dynamics. In addition, taking into account multiple scattering effects opens the way to quantitative studies of non-equilibrium dynamics of defects in quasi-perfect crystals.
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