Charged defects in graphene and the ionicity of hexagonal boron nitride in direct images

We report on the detection and charge distribution analysis for nitrogen substitutional dopants in single layer graphene membranes by aberration-corrected high-resolution transmission electron microscopy (HRTEM). Further, we show that the ionicity of single-layer hexagonal boron nitride can be confirmed from direct images. For the first time, we demonstrate by a combination of HRTEM experiments and first-principles electronic structure calculations that adjustments to the atomic potentials due to chemical bonding can be discerned in HRTEM images. Our experiments open a way to discern electronic configurations in point defects or other non-periodic arrangements or nanoscale objects that can not be analyzed in an electron or x-ray diffraction experiment.

Imaging and Dynamics of Light Atoms and Molecules on Graphene

Observing the individual building blocks of matter is one of the primary goals of microscopy. The invention of the scanning tunneling microscope [1] revolutionized experimental surface science in that atomic-scale features on a solid-state surface could finally be readily imaged. However, scanning tunneling microscopy has limited applicability due to restrictions, for example, in sample conductivity, cleanliness, and data aquisition rate. An older microscopy technique, that of transmission electron microscopy (TEM) [2, 3] has benefited tremendously in recent years from subtle instrumentation advances, and individual heavy (high atomic number) atoms can now be detected by TEM [4 - 7] even when embedded within a semiconductor material [8, 9]. However, detecting an individual low atomic number atom, for example carbon or even hydrogen, is still extremely challenging, if not impossible, via conventional TEM due to the very low contrast of light elements [2, 3, 10 - 12]. Here we demonstrate a means to observe, by conventional transmision electron microscopy, even the smallest atoms and molecules: On a clean single-layer graphene membrane, adsorbates such as atomic hydrogen and carbon can be seen as if they were suspended in free space. We directly image such individual adatoms, along with carbon chains and vacancies, and investigate their dynamics in real time. These techniques open a way to reveal dynamics of more complex chemical reactions or identify the atomic-scale structure of unknown adsorbates. In addition, the study of atomic scale defects in graphene may provide insights for nanoelectronic applications of this interesting material.