Hexagonal boron nitride (h-BN) is the only known material aside from graphite with a structure composed of simple, stable, non-corrugated atomically thin layers. While historically used as lubricant in powder form, h-BN layers have become particularly attractive as an ultimately thin insulator. Practically all emerging electronic and photonic device concepts rely on h-BN exfoliated from small bulk crystallites, which limits device dimensions and process scalability.Here, we address this integration challenge for mono-layer h-BN via a chemical vapour deposition process that enables crystal sizes exceeding 0.5 mm starting from commercial, reusable platinum foils, and in unison allows a delamination process for easy and clean layer transfer. We demonstrate sequential pick-up for the assembly of graphene/h-BN heterostructures with atomic layer precision, while minimizing interfacial contamination. Our process development builds on a systematic understanding of the underlying mechanisms. The approach can be readily combined with other layered materials and opens a scalable route to h-BN layer integration and reliable 2D material device layer stacks.

Membranes that selectively filter for both anions and cations are central to technological applications from clean energy generation to desalination devices. 2D materials have immense potential as these ion-selective membranes due to their thinness, mechanical strength, and tunable surface chemistry; however, currently, only cation-selective membranes have been reported.Here we demonstrate the controllable cation and anion selectivity of both monolayer graphene and hexagonal boron nitride. In particular, we measure the ionic current through membranes grown by chemical vapor deposition containing well-known defects inherent to scalably produced and wet-transferred 2D materials. We observe a striking change from cation selectivity with monovalent ions to anion selectivity by controlling the concentration of multivalent ions and inducing charge inversion on the 2D membrane. Furthermore, we find good agreement between our experimental data and theoretical predictions from the Goldman− Hodgkin−Katz equation and use this model to extract selectivity ratios. These tunable selective membranes conduct up to 500 anions for each cation and thus show potential for osmotic power generation.

We systematically study the effects of residual oxygen in the bulk of Cu foil catalysts on the chemical vapour deposition (CVD) of graphene. While oxidation is widely used to remove impurities in metal catalysts and to control the nucleation density of graphene, we show that minute concentrations of residual bulk oxygen can significantly deteriorate the quality of as-grown graphene highlighted by an increased Raman D/G ratio, increased propensity to post-growth etching and increased fraction of multi-layer graphene nucleation. Starting from commercial Cu foils, we show that a simple hydrogen annealing step after the initial oxidation allows us to lower the residual oxygen level as measured by time-of-flight secondary ion mass spectrometry to produce graphene of significantly higher quality. This can be effectively combined with a short hydrocarbon exposure time of 10 min to achieve near full mono-layer graphene coverage, suitable for emerging industrial applications. We show that residual oxygen can have an equally significant impact on Fe catalysed h-BN CVD, and discuss the underlying mechanisms with parallels to well-known processes in metallurgy, catalysis and vacuum science.

Hexagonal boron nitride (hBN) is a promising host material for room-temperature, tunable solid-state quantum emitters. A key technological challenge is deterministic and scalable spatial emitter localization, both laterally and vertically, while maintaining the full advantages of the 2D nature of the material. Here, we demonstrate emitter localization in hBN in all three dimensions via a monolayer (ML) engineering approach. We establish pretreatment processes for hBN MLs to either fully suppress or activate emission, thereby enabling such differently treated MLs to be used as select building blocks to achieve vertical (z) emitter localization at the atomic layer level. We show that emitter bleaching of ML hBN can be suppressed by sandwiching between two protecting hBN MLs, and that such thin stacks retain opportunities for external control of emission. We exploit this to achieve lateral (x−y) emitter localization via the addition of a patterned graphene mask that quenches fluorescence. Such complete emitter site localization is highly versatile, compatible with planar, scalable processing, allowing tailored approaches to addressable emitter array designs for advanced characterization, monolithic device integration, and photonic circuits.

We report on an approach to bring together single crystal metal catalyst preparation and graphene growth in a combined process flow using a standard cold-wall chemical vapor deposition (CVD) reactor. We employ a sandwich arrangement between a commercial polycrystalline Cu foil and c-plane sapphire wafer and show that close-spaced vacuum sublimation across the confined gap can result in an epitaxial, single-crystal Cu(111) film at high growth rate. The arrangement is scalable (we demonstrate 2″ wafer scale) and suppresses reactor contamination with Cu. While starting with an impure Cu foil, the freshly prepared Cu film is of high purity as measured by time-of-flight secondary ion mass spectrometry. We seamlessly connect the initial metallization with subsequent graphene growth via the introduction of hydrogen and gaseous carbon precursors, thereby eliminating contamination due to substrate transfer and common lengthy catalyst pretreatments. We show that the sandwich approach also enables for a Cu surface with nanometer scale roughness during graphene growth and thus results in high quality graphene similar to previously demonstrated Cu enclosure approaches. We systematically explore the parameter space and discuss the opportunities, including subsequent dry transfer, generality, and versatility of our approach particularly regarding the cost-efficient preparation of different single crystal film orientations and expansion to other material systems.