3D atomic structure determination with ultrashort-pulse MeV electron diffraction
Abstract
Understanding structure at the atomic scale is fundamental for understanding the functioning and the development of materials with improved properties. Compared with other probes providing atomic resolution, electrons offer the strongest interaction in combination with minimal radiation damage, which makes them an ideal tool for investigating very small and radiation-sensitive samples [Henderson (1995), Q. Rev. Biophys. 28, 171-193]. However, these benefits are often offset by the laborious preparation of nanometre-sized samples that are not visible using a light microscope, and the fact that experiments are largely restricted to ultra-high vacuum [Duyvesteyn et al. (2018), Proc. Natl Acad. Sci. USA 115, 9569-9573; Gruene et al. (2021), Nat. Rev. Chem. 5, 660-668]. Here, we report the successful implementation of MeV electron diffraction for ab initio 3D structure determination of the quasi-2D material muscovite and the quantum material 1T-TaS2 at atomic resolution. By employing ultrashort electron pulses from the REGAE (Relativistic electron gun for atomic exploration) accelerator, we obtained high-quality diffraction datasets suitable for structural refinements based on dynamical scattering theory, enabling precise localization of even hydrogen atoms. The increased penetration depth of MeV electrons significantly expands the applicable thickness range of samples, overcoming previous restrictions associated with traditional electron diffraction. These findings establish MeV…
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