Disorder-tuned conductivity in amorphous monolayer carbon.

Correlating atomic configurations-specifically, degree of disorder (DOD)-of an amorphous solid with properties is a long-standing riddle in materials science and condensed matter physics, owing to difficulties in determining precise atomic positions in 3D structures1-5. To this end, 2D systems provide insight to the puzzle by allowing straightforward imaging of all atoms6,7. Direct imaging of amorphous monolayer carbon (AMC) grown by laser-assisted depositions has resolved atomic configurations, supporting the modern crystallite view of vitreous solids over random network theory8. Nevertheless, a causal link between atomic-scale structures and macroscopic properties remains elusive. Here we report facile tuning of DOD and electrical conductivity in AMC films by varying growth temperatures. Specifically, the pyrolysis threshold temperature is the key to growing variable-range-hopping conductive AMC with medium-range order (MRO), whereas increasing the temperature by 25 °C results in AMC losing MRO and becoming electrically insulating, with an increase in sheet resistance of 109 times. Beyond visualizing highly distorted nanocrystallites embedded in a continuous random network, atomic-resolution electron microscopy shows the absence/presence of MRO and temperature-dependent densities of nanocrystallites, two order parameters proposed to fully describe DOD. Numerical calculations establish the conductivity diagram as a function of these two parameters, directly linking microstructures to electrical properties. Our work represents an important step towards understanding the structure-property relationship of amorphous materials at the fundamental level and paves the way to electronic devices using 2D amorphous materials.

Synthesis of centimeter-scale high-quality polycrystalline hexagonal boron nitride films from Fe fluxes.

High-quality hexagonal BN (hBN) crystals, owing to their irreplaceable roles in new functional devices such as universal substrates and excellent layered insulators are exceedingly required in the field of two-dimensional (2D) materials. Although large-scale monolayer hBN crystals have been successfully grown on catalytic metals, the synthesis of large-area continuous hBN films with thickness in microns is challenging, hindering their applications at the mesoscopic level. Herein, we report the single-metal flux growth of centimeter-large, micron-thick, and high-quality continuous hBN films by balancing the grain size and coverage. The as-grown films can be readily exfoliated and transferred onto arbitrary substrates. Isotopically engineered hBN crystals can be obtained as well by the method. The narrow Raman line widths of the intralayer E2g mode peak (2.9 cm-1 for h11BN, 3.3 cm-1 for h10BN, and 7.9 cm-1 for hNaBN) and ultrahigh thermal conductivity (830 W m-1 K-1 for 4L h11BN) demonstrate high crystal quality and low defect density. Our results provide the foundation for the cost-efficient and lab-achievable synthesis of high-quality hBN films aimed at its mesoscopic applications.