The atomic structure at the interface between two-dimensional (2D) and three-dimensional (3D) materials influences properties such as contact resistance, photo-response, and high-frequency electrical performance. Moiré engineering is yet to be utilized for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D interfaces. Using epitaxially aligned MoS2/Au{111} as a model system, we demonstrate the use of advanced scanning transmission electron microscopy (STEM) combined with a geometric convolution technique in imaging the crystallographic 32 Å moiré pattern at the 2D/3D interface. This moiré period is often hidden in conventional electron microscopy, where the Au structure is seen in projection. We show, via ab initio electronic structure calculations, that charge density is modulated according to the moiré period, illustrating the potential for (opto-)electronic moiré engineering at the 2D/3D interface. Our work presents a general pathway to directly image periodic modulation at interfaces using this combination of emerging microscopy techniques.

Understanding structure at the interface between two-dimensional (2D) materials and 3D metals is crucial for designing novel 2D/3D heterostructures and improving the performance of many 2D material devices. Here, we quantify and discuss the 2D/3D interface structure and the 3D morphology in several materials systems. We first deposit faceted Au nanoislands on graphene and transition metal dichalcogenides, using measurements of the equilibrium island shape to determine values for the 2D/ Au interface energy and examining the role of surface reconstructions, chemical identity, and defects on the grown structures. We then deposit the technologically relevant metals Ti and Nb under conditions where kinetic rather than thermodynamic factors govern growth. We describe a transition from dendritic to faceted islands as a function of growth temperature and discuss the factors determining island shape in these materials systems. Finally, we show that suspended 2D materials enable the fabrication of a novel type of 3D/2D/3D heterostructure and discuss the growth mechanism. We suggest that emerging nanodevices will utilize versatile fabrication of 2D/3D heterostructures with well-characterized interfaces and morphologies.

Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, defects in mono‐ to multilayer CrSBr are correlated with structural, vibrational, and magnetic properties. Resonant Raman scattering is used to reveal distinct vibrational defect signatures. In pristine CrSBr, it is shown that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. Environmental exposure is shown to cause drastic degradation in monolayers, with the formation of intralayer defects. This is in contrast to multilayers that predominantly show bromine surface defects. Through deliberate ion irradiation, the formation of defect modes is tuned: these are strongly polarized and resonantly enhanced, reflecting the quasi‐‐1D electronic character of CrSBr. Strikingly, pronounced signatures of spin‐phonon coupling of the intrinsic phonon modes and the ion beam‐induced defect modes are observed throughout the magnetic transition temperature. Overall, defect engineering of magnetic properties is possible, with resonant Raman spectroscopy serving as a direct fingerprint of magnetic phases and defects in CrSBr.

The ability to vary the temperature of an electrochemical cell provides opportunities to control reaction rates and pathways and to drive processes that are inaccessible at ambient temperature. Here, we...