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Register a new userImaging graphene moire superlattices via scanning Kelvin probe microscopy
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Added by
Rajiv Giridharagopal
Publication date
2021
fields
Physics
and research's language is
English
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Moire superlattices in van der Waals heterostructures are gaining increasing attention because they offer new opportunities to tailor and explore unique electronic phenomena when stacking 2D materials with small twist angles. Here, we reveal local surface potentials associated with stacking domains in twisted double bilayer graphene (TDBG) moire superlattices. Using a combination of both lateral Piezoresponse Force Microscopy (LPFM) and Scanning Kelvin Probe Microscopy (SKPM), we distinguish between Bernal (ABAB) and rhombohedral (ABCA) stacked graphene and directly correlate these stacking configurations with local surface potential. We find that the surface potential of the ABCA domains is ~15 mV higher (smaller work function) than that of the ABAB domains. First-principles calculations based on density functional theory further show that the different work functions between ABCA and ABAB domains arise from the stacking dependent electronic structure. We show that, while the moire superlattice visualized by LPFM can change with time, imaging the surface potential distribution via SKPM appears more stable, enabling the mapping of ABAB and ABCA domains without tip-sample contact-induced effects. Our results provide a new means to visualize and probe local domain stacking in moire superlattices along with its impact on electronic properties.
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The graphene moire structures on metals, as they demonstrate both long (moire) and short (atomic) scale ordered structures, are the ideal systems for the application of scanning probe methods. Here we present the complex studies of the graphene/Ir(111) system by means of 3D scanning tunnelling and atomic force microscopy/spectroscopy as well as Kelvin-probe force microscopy. All results clearly demonstrate a variation of the moire and atomic scale contrasts as a function of the bias voltage as well as the distance between the scanning probe and the sample, allowing to discriminate between topographic and electronic contributions in the imaging of a graphene layer on metals. The presented results are accompanied by the state-of-the-art density functional theory calculations demonstrating the excellent agreement between theoretical and experimental data.
We review a new implementation of Kelvin probe force microscopy (KPFM) in which the dissipation signal of frequency modulation atomic force microscopy (FM-AFM) is used for dc bias voltage feedback (D-KPFM). The dissipation arises from an oscillating electrostatic force that is coherent with the tip oscillation, which is caused by applying the ac voltage between the tip and sample. The magnitude of the externally induced dissipation is found to be proportional to the effective dc bias voltage, which is the difference between the applied dc voltage and the contact potential difference. Two different implementations of D-KPFM are presented. In the first implementation, the frequency of the applied ac voltage, $f_mathrm{el}$, is chosen to be the same as the tip oscillation ($f_mathrm{el} = f_mathrm{m}$: $1omega$D-KPFM). In the second one, the ac voltage frequency, $f_mathrm{el}$, is chosen to be twice the tip oscillation frequency ($f_mathrm{el}= 2 f_mathrm{m}$: $2omega$D-KPFM). In $1omega$D-KPFM, the dissipation is proportional to the electrostatic force, which enables the use of a small ac voltage amplitude even down to $approx 10$,mV. In $2omega$D-KPFM, the dissipation is proportional to the electrostatic force gradient, which results in the same potential contrast as that obtained by FM-KPFM. D-KPFM features a simple implementation with no lock-in amplifier and faster scanning as it requires no low frequency modulation. The use of a small ac voltage amplitude in $1omega$D-KPFM is of great importance in characterizing of technically relevant materials in which their electrical properties can be disturbed by the applied electric field. $2omega$D-KPFM is useful when more accurate potential measurement is required. The operations in $1omega$ and $2omega$D-KPFM can be switched easily to take advantage of both features at the same location on a sample.
An anisotropic charge distribution on individual atoms, such as e.g. {sigma}-hole, may strongly affect material and structural properties of systems. Nevertheless, subatomic resolution of such anisotropic charge distributions represents a long-standing experimental challenge. In particular, the existence of the {sigma}-hole on halogen atoms has been demonstrated only indirectly through determination of crystal structures of organic molecules containing halogens or via theoretical calculations. Nevertheless, its direct experimental visualization has not been reported yet. Here we demonstrate that Kelvin probe force microscopy, with a properly functionalized probe, can reach subatomic resolution imaging the {sigma}-hole or a quadrupolar charge of carbon monoxide molecule. This achievement opens new way to characterize biological and chemical systems where anisotropic atomic charges play decisive role.
Fast scanning probe microscopy enabled via machine learning allows for a broad range of nanoscale, temporally resolved physics to be uncovered. However, such examples for functional imaging are few in number. Here, using piezoresponse force microscopy (PFM) as a model application, we demonstrate a factor of 5.8 improvement in imaging rate using a combination of sparse spiral scanning with compressive sensing and Gaussian processing reconstruction. It is found that even extremely sparse scans offer strong reconstructions with less than 6 % error for Gaussian processing reconstructions. Further, we analyze the error associated with each reconstructive technique per reconstruction iteration finding the error is similar past approximately 15 iterations, while at initial iterations Gaussian processing outperforms compressive sensing. This study highlights the capabilities of reconstruction techniques when applied to sparse data, particularly sparse spiral PFM scans, with broad applications in scanning probe and electron microscopies.
Epitaxial graphene grown on transition metal surfaces typically exhibits a moire pattern due to the lattice mismatch between graphene and the underlying metal surface. We use both scanning tunneling microscopy (STM) and atomic force microscopy (AFM) experiments to probe the electronic and topographic contrast of the graphene moire on the Ir(111) surface. While STM topography is influenced by the local density of states close to the Fermi energy and the local tunneling barrier height, AFM is capable of yielding the true surface topography once the background force arising from the van der Waals (vdW) interaction between the tip and the substrate is taken into account. We observe a moire corrugation of 35$pm$10 pm, where the graphene-Ir(111) distance is the smallest in the areas where the graphene honeycomb is atop the underlying iridium atoms and larger on the fcc or hcp threefold hollow sites.
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