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Register a new userReal-space imaging of {sigma}-hole by means of Kelvin probe force microscopy with subatomic resolution
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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.
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We report a new experimental technique for Kelvin probe force microscopy (KPFM) using the dissipation signal of frequency modulation atomic force microscopy for bias voltage feedback. It features a simple implementation and faster scanning as it requires no low frequency modulation. The dissipation is caused by the oscillating electrostatic force that is coherent with the tip oscillation, which is induced by a sinusoidally oscillating voltage applied between the tip and sample. We analyzed the effect of the phase of the oscillating force on the frequency shift and dissipation and found that the relative phase of 90$^circ$ that causes only the dissipation is the most appropriate for KPFM measurements. The present technique requires a significantly smaller ac voltage amplitude by virtue of enhanced force detection due to the resonance enhancement and the use of fundamental flexural mode oscillation for electrostatic force detection. This feature will be of great importance in the electrical characterizations of technically relevant materials whose electrical properties are influenced by the externally applied electric field as is the case in semiconductor electronic devices.
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.
We report a Kelvin probe force microscopy (KPFM) implementation using the dissipation signal of a frequency modulation atomic force microscopy that is capable of detecting the gradient of electrostatic force rather than electrostatic force. It features a simple implementation and faster scanning as it requires no low frequency modulation. We show that applying a coherent ac voltage with two times the cantilever oscillation frequency induces the dissipation signal proportional to the electrostatic force gradient which depends on the effective dc bias voltage including the contact potential difference. We demonstrate the KPFM images of a MoS$_2$ flake taken with the present method is in quantitative agreement with that taken with the frequency modulated Kelvin probe force microscopy technique.
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.
Kelvin probe force microscopy at normal pressure was performed by two different groups on the same Au-coated planar sample used to measure the Casimir interaction in a sphere-plane geometry. The obtained voltage distribution was used to calculate the separation dependence of the electrostatic pressure $P_{rm res}(D)$ in the configuration of the Casimir experiments. In the calculation it was assumed that the potential distribution in the sphere has the same statistical properties as the measured one, and that there are no correlation effects on the potential distributions due to the presence of the other surface. Within this framework, and assuming that the potential distribution does not vary significantly at low pressure, the calculated $P_{rm res}(D)$ does not explain the magnitude or the separation dependence of the difference $Delta P (D)$ between the measured Casimir pressure and the one calculated using a Drude model for the electromagnetic response of Au.
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