We have developed a compact ultrafast electron diffractometer, consisting of a laser-driven rf photocathode that generates 3.0 MeV probe electron pulses, three-stage lens optics, and a custom-built detector for relativistic electrons. High-quality single-shot transmission electron diffraction has been detected from 180-nm-thick Si single crystals, with an excellent special resolution for diffracted beams; the spot width of $0.02{\text{A}}^{-1}$ is obtained. The pulse width is estimated to be 100 fs in duration. Characteristics of the electron beam and other diffractometer features are discussed.

We performed relativistic ultrafast electron diffraction (UED) measurements of the structural dynamics of photoexcited gold nanofilms and developed an atomistic model, based on the two-temperature molecular dynamics (2T-MD) method, which allows us to make a direct comparison of the time evolutions of measured and calculated Bragg peaks. The quantitative agreement between the temporal evolutions of the experimental and theoretical Bragg peaks at all fluences suggests that the 2T-MD method provides a faithful atomistic representation of the structural evolution of photoexcited gold films. The results reveal the transition between slow heterogeneous melting at low absorbed photon fluence to rapid homogeneous melting at higher fluence and nonthermally driven melting at very high fluence. At high laser fluence, the time evolution of Bragg peaks calculated using the conventional 2T-MD model disagrees with experiment. We show that using an interatomic potential that directly depends on the electron temperature delivers a much better agreement with UED data. Finally, our ab initio calculations of phonon spectra suggest electronic bond softening, if the nanofilms can expand freely under electronic pressure, and bond hardening, if they are constrained in all three dimensions.

For realization of new informative systems, the memristor working like synapse has drawn much attention. We developed isolated high-density Fe₃O₄ nanocrystals on Ge nuclei/Si with uniform and high resistive switching performance using low-temperature growth. The Fe₃O₄ nanocrystals on Ge nuclei had well-controlled interface (Fe₃O₄/GeO_x/Ge) composed of high-crystallinity Fe₃O₄ and high-quality GeO_x layers. The nanocrystals showed uniform resistive switching characteristics (high switching probability of ~90%) and relatively high Off/On resistance ratio (~58). The high-quality interface enables electric field application to Fe₃O₄ and GeO_x near the interface, which leads to effective positively-charged oxygen vacancy movement, resulting in high-performance resistive switching. Furthermore, we successfully observed memory effect in nanocrystals with well-controlled interface. The experimental confirmation of the memory effect existence even in ultrasmall nanocrystals is significant for realizing non-volatile nanocrystal memory leading to neuromorphic devices. Graphical abstract

The time evolution of the Bragg peaks of photo-excited gold nanofilms is measured using transmission ultrafast electron diffraction (UED) with 3.0 MeV electron pulses and the corresponding structure evolution is calculated using two-temperature molecular dynamics (2T-MD). The good agreement obtained between the measured and calculated Bragg peaks, over the full experimental timescale, enables the lattice temperature effects and the structural changes to be disentangled for the first time. The agreement demonstrates that 2T-MD is a reliable method for solving the inverse problem of structure determination of laser irradiated metals in UED measurements.

Phonon transport in the nano-system has been studied using well-designed nanostructured materials to observe and control the interesting phonon behaviors like ballistic phonon transport. Recently, we observed drastic thermal conductivity reduction in the films containing well-controlled nanodots. Here, we investigate whether this comes from the interference effect in ballistic phonon transport by comparing the thermal properties of the Si or Si_0.75Ge_0.25 films containing Ge nanodots. The experimentally-obtained thermal resistance of the nanodot layer shows peculiar nanodot size dependence in the Si films and a constant value in the SiGe films. From the phonon simulation results, interestingly, it is clearly found that in the nanostructured Si film, phonons travel in a non-diffusive way (ballistic phonon transport). On the other hand, in the nanostructured SiGe film, although simple diffusive phonon transport occurs, extremely-low thermal conductivity (∼0.81 W m⁻¹ K⁻¹) close to that of amorphous Si_0.7Ge_0.3 (∼0.7 W m⁻¹ K⁻¹) is achieved due to the combination of the alloy phonon scattering and Ge nanodot scattering.