Inelastic electron tunneling spectroscopy is a powerful technique for investigating lattice dynamics of nanoscale systems including graphene and small molecules, but establishing a stable tunnel junction is considered as a major hurdle in expanding the scope of tunneling experiments. Hexagonal boron nitride is a pivotal component in two-dimensional Van der Waals heterostructures as a high-quality insulating material due to its large energy gap and chemical-mechanical stability. Here we present planar graphene/h-BN-heterostructure tunneling devices utilizing thin h-BN as a tunneling insulator. With much improved h-BN-tunneling-junction stability, we are able to probe all possible phonon modes of h-BN and graphite/graphene at Γ and K high symmetry points by inelastic tunneling spectroscopy. Additionally, we observe that low-frequency out-of-plane vibrations of h-BN and graphene lattices are significantly modified at heterostructure interfaces. Equipped with an external back gate, we can also detect high-order coupling phenomena between phonons and plasmons, demonstrating that h-BN-based tunneling device is a wonderful playground for investigating electron-phonon couplings in low-dimensional systems.

Defects have crucial effects on the electronic and optoelectronic properties of two‐dimensional materials. In this work, we measured the changes in the Raman spectra and electrical conductance of monolayer molybdenum disulfide (MoS2) with increasing defects via thermal annealing in a reducing atmosphere. Raman spectra of the basal plane MoS2 on SiO2 differed from those of the edge and revealed intricate changes upon annealing up to 550°C due to the substitution of adsorbed molecules and the creation of highly concentrated defects. On the other hand, MoS2 on hexagonal boron nitride (h‐BN) presented homogenous Raman spectra over the entire area and showed no noticeable changes in its Raman spectra upon annealing. For MoS2 on h‐BN, the charge transfer between MoS2 and adsorbed molecules and the number of defects created by annealing up to 550°C are not sufficient to change the Raman spectra. The distinct behaviors of the two sample spectra are ascribed to different substrate‐induced doping and interfacial adhesion strengths.

Graphene bubbles are often formed when graphene and other layered two-dimensional materials are vertically stacked as van der Waals heterostructures. Here, we investigate how graphene bubbles and their related disorder impact the quantum transport behavior of graphene in the absence and presence of external magnetic fields. By combining experimental observations and numerical simulations, we find that the disorder induced by the graphene bubbles is mainly from p-type dopants and the charge transport in pristine graphene can be severely influenced by the presence of bubbles via long- and short-range scattering even with a small bubble-coverage of 2% and below. Upon bubble density increase, we observe an overall decrease in carrier mobility, and the appearance of a second Dirac point on the electron carrier side. At high magnetic fields, the disorder from graphene bubbles primarily impacts the quantization of the lowest Landau level, resulting in quantum Hall features associated with a new Dirac cone at high charge carrier density.