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The fundamental sensitivity limit of atomic force microscopy is strongly correlated to the thermal noise of cantilever oscillation. A method to suppress this unwanted noise is to reduce the bandwidth of the measurement, but this approach is limited by the speed of the measurement and the width of the cantilever resonance, commonly defined through the quality factor Q. However, it has been shown that optomechanical resonances in interferometers might affect cantilever oscillations resulting in an effective quality factor Q eff . When the laser power is sufficiently increased cantilever oscillations might even reach the regime of self-oscillation. In this self-oscillation state, the noise of the system is partially determined by the interaction with laser light far from equilibrium. Here, we show and discuss how tuning of laser power leads to nonlinear optomechanical effects that can dramatically increase the effective quality factor of the cantilever leading to out-of-equilibrium noise. We model the effects using a fourth order nonlinearity of the damping coefficient. [ABSTRACT FROM AUTHOR]

Graphene nanoribbons show exciting electronic properties related to the exotic nature of the charge carriers and to local confinement as well as atomic-scale structural details. The local work function provides evidence for such structural, electronic, and chemical variations at surfaces. Kelvin prove force microscopy can be used to measure the local contact potential difference (LCPD) between a probe tip and a surface, related to the work function. Here we use this technique to map the LCPD of graphene nanoribbons grown on a Au(111) substrate. The LCPD data shows charge transfer between the graphene nanoribbons and the gold substrate. Our results are corroborated with density functional theory calculations, which verify that the maps reflect the doping of the nanoribbons. Our results help to understand the relation between atomic structure and electronic properties both in high-resolution images and in the distance dependence of the LCPD., (Copyright © 2024, Rothhardt et al.)

C 60 is a model system to study molecule-surface interactions and phase transitions due to its high symmetry and strong covalent π bonding within the molecule versus weak van-der-Waals coupling between neighboring molecules. In the solid, at room temperature, the molecule rotates and behaves as a sphere. However, the pentagonal and hexagonal atomic arrangement imposes deviations from the spherical symmetry that become important at low temperatures. The orientation of the C 60 can be viewed to represent classic spins. For geometrical reasons the preferred orientation of neighboring C 60 cannot be satisfied for all of the neighboring molecules, making C 60 a model for disordered spin systems with frustration. We study several molecular layers of C 60 islands on highly oriented pyrolytic graphite using scanning tunneling microscopy at liquid nitrogen temperatures. By imaging several layers we obtain a limited access to the three-dimensional rotational structure of the molecules in an island. We find one rotationally disordered layer between two partially rotationally ordered layers with hexagonal patterns. This exotic pattern shows an example of the local distribution of order and disorder in geometrically frustrated systems. Scanning tunneling spectroscopy data confirms the weak interactions of neighboring molecules., (Creative Commons Attribution license.)

Electromigration in interconnects continues to be an important field of study in integrated circuits as the interconnects are planned to shrink in size at comparable pace as the semiconductor functional elements. Through shrinking the interconnects approach the regime where quantum size effects become important. The observation of quantum size and shell effects is usually restricted either to low-temperatures or vacuum conditions or to chemically inert materials such as Au. Here, we show that in electromigrated Cu nanocontacts such effects can be observed at room temperature and room pressure even in the presence of oxidation. Our data provide evidence that the nanocontacts are nearly spherical objects with a triangular-cylindrical symmetry of their electronic wave functions with a stronger free-electron-like character compared to previous results. We do not observe a detrimental effect of oxygen. The presence of shell effects has implications for the technological use of Cu nanocontacts as interconnects in integrated circuits and could lead to the use of electronic wave functions of shells in such interconnects., (Creative Commons Attribution license.)

We have investigated the self-assembly of the graphene nanoribbon molecular precursor 10,10'-dibromo-9,9'-bianthryl (DBBA) on Au(111) with frequency modulation scanning force microscopy (FM-SFM) at room temperature combined with ab initio calculations. For low molecular coverages, the molecules aggregate along the substrate herringbone reconstruction main directions while remaining mobile. At intermediate coverage, two phases coexist, zigzag stripes of monomer chains and decorated herringbones. For high coverage, the molecules assemble in a dimer-striped phase. The adsorption behaviour of DBBA molecules and their interactions are discussed and compared with the results from ab initio calculations.

We have revealed processes of the tip apex distortion in the measurements of non-contact scanning force microscopy. High-spatial-resolution two-dimensional force mapping on KCl(100) surfaces for a large number of tips, seven tips, enabled us to see the complex behavior of the tip apex distortion. The tips are from Si without additional coating, but are altered by the tip-sample interaction and show the behavior of different atomic species. On the KCl(001) surfaces, the tip apex, consisting of K and Cl atoms or of Si, distorted several times while changing the distance even in a weak attractive region. There are variations in rigidity of the tip apex, but all tips distorted in the small attractive region. This complex behavior was categorized in patterns by our analyses. We compare the experimental force-distance data to atomistic simulations using rigid KCl-terminated tips and KCl-terminated tips with an additional KCl-pair designed to perform atomic jumps. We also compare the experimental force-distance data to first principles simulations using Si tips. We mainly find K-terminated tips and Si-terminated tips. We find that Si tips show only one force minimum whereas KCl-terminated tips show two force minima in line with the stronger rigidity of Si compared to KCl. At room temperature, the tip apex atoms can perform atomic jumps that change the atomic configuration of the tip apex.

Graphene nanoribbons' electronic transport properties strongly depend on the type of edge, armchair, zigzag or other, and on edge functionalization that can be used for band-gap engineering. For only partly hydrogenated edges interesting magnetic properties are predicted. Electric charge accumulates at edges and corners. Scanning force microscopy has so far shown the centre of graphene nanoribbons with atomic resolution using a quartz crystal tuning fork sensor of high stiffness. Weak long-range electrostatic forces related to the charge accumulation on the edges of graphene nanoribbons could not be imaged so far. Here, we show the electrostatic forces at the corners and edges of graphene nanoribbons are amenable to measurement. We use soft cantilevers and a bimodal imaging technique to combine enhanced sensitivity to weak long-range electrostatic forces with the high resolution of the second-frequency shift. Additionally, in our work the edges of the nanoribbons are mainly hydrogen-free, opening to the route to investigations of partly hydrogenated magnetic nanoribbons.

Insulating substrates allow for in-plane contacted molecular electronics devices where the molecule is in contact with the insulator. For the development of such devices it is important to understand the interaction of molecules with insulating surfaces. As substrates, ionic crystals such as KBr, KCl, NaCl and CaF 2 are discussed. The surface energies of these substrates are small and as a consequence intrinsic properties of the molecules, such as molecule-molecule interaction, become more important relative to interactions with the substrates. As prototypical molecules, three variants of graphene-related molecules are used, pentacene, [Formula: see text] and PTCDA. Pentacene is a good candidate for molecular electronics applications due to its high charge carrier mobility. It shows mainly an upright standing growth mode and the morphology of the islands is strongly influenced by dewetting. A new second flat-lying phase of the molecule has been observed. Studying the local work function using the Kelvin method reveals details such as line defects in the center of islands. The local work function differences between the upright-standing and flat-lying phase can only be explained by charge transfer that is unusual on ionic crystalline surfaces. [Formula: see text] nucleation and growth is explained by loosely bound molecules at kink sites as nucleation sites. The stability of [Formula: see text] islands as a function of magic numbers is investigated. Peculiar island shapes are obtained from unusual dewetting processes already at work during growth, where molecules 'climb' to the second molecular layer. PTCDA is a prototypical semiconducting molecule with strong quadrupole moment. It grows in the form of elongated islands where the top and the facets can be molecularly resolved. In this way the precise molecular arrangement in the islands is revealed.

In nano-structures such as thin films electron confinement results in the quantization of energy levels in the direction perpendicular to the film. The discretization of the energy levels leads to the oscillatory dependence of many properties on the film thickness due to quantum size effects. Pb on Si(111) is a specially interesting system because a particular relationship between the Pb atomic layer thickness and its Fermi wavelength leads to a periodicity of the oscillation of two atomic layers. Here, we demonstrate how the combination of scanning force microscopy (SFM) and Kelvin probe force microscopy (KPFM) provides a reliable method to monitor the quantum oscillations in the work function of Pb ultra-thin film nano-structures on Si(111). Unlike other techniques, with SFM/KPFM we directly address single Pb islands, determine their height while suppressing the influence of electrostatic forces, and, in addition, simultaneously evaluate their local work function by measurements close to equilibrium, without current-dependent and non-equilibrium effects. Our results evidence even-odd oscillations in the work function as a function of the film thickness that decay linearly with the film thickness, proving that this method provides direct and precise information on the quantum states.

We study the structure and the electronic properties of Au nanocontacts created by controlled electromigration of thin film devices, a method frequently used to contact molecules. In contrast to electromigration testing, a current is applied in a cyclic fashion and during each cycle the resistance increase of the metal upon heating is used to avoid thermal runaway. In this way, nanometer sized-gaps are obtained. The thin film devices with an optimized structure at the origin of the electromigration process are made by shadow evaporation without contamination by organic materials. Defining rounded edges and a thinner area in the center of the device allow to pre-determine the location where the electromigration takes place. Scanning force microscopy images of the pristine Au film and electromigrated contact show its grainy structure. Through electromigration, a 1.5 μm-wide slit is formed, with extensions only on the anode side that had previously not been observed in narrower structures. It is discussed whether this could be explained by asymmetric heating of both electrodes. New grains are formed in the slit and on the extensions on both, the anode and the cathode side. The smaller structures inside the slit lead to an electrode distance below 150 nm. Kelvin probe force microscopy images show a local work function difference with fluctuations of 70 mV on the metal before electromigration. Between the electrodes, disconnected through electromigration, a work function difference of 3.2 V is observed due to charging. Some of the grains newly formed by electromigration are electrically disconnected from the electrodes.

Stepped well-ordered semiconductor surfaces are important as nanotemplates for the fabrication of 1D nanostructures. Therefore, a detailed understanding of the underlying stepped substrates is crucial for advances in this field. Although measurements of step edges are challenging for scanning force microscopy (SFM), here we present simultaneous atomically resolved SFM and Kelvin probe force microscopy (KPFM) images of a silicon vicinal surface. We find that the local contact potential difference is large at the bottom of the steps and at the restatoms on the terraces, whereas it drops at the upper part of the steps and at the adatoms on the terraces. For the interpretation of the data we performed density functional theory (DFT) calculations of the surface dipole distribution. The DFT images accurately reproduce the experiments even without including the tip in the calculations. This underlines that the high-resolution KPFM images are closely related to intrinsic properties of the surface and not only to tip-surface interactions.

The study of magnetic domain walls in constrained geometries is an important topic, yet when dealing with extreme nanoscale magnetic systems artefacts can often dominate the measurements and obscure the effects of intrinsic magnetic origin. In this work we study the evolution of domain wall depinning in electromigrated ferromagnetic junctions which are both initially fabricated and subsequently tailored in-situ in clean ultra-high vacuum conditions. Carefully designed Ni(80)Fe(20) (Permalloy) notched half-ring structures are fabricated and investigated as a function of constriction width by tailoring the size of the contact using controlled in-situ electromigration. It is found that the domain wall pinning strength is increased on reducing the contact size in line with a reduction of the wall energy in narrower constrictions. Furthermore, the angular dependency and symmetry of the depinning field is measured to determine the full pinning potential for a domain wall in a system with a narrow constriction.

In the field of molecular electronics, thin films of molecules adsorbed on insulating surfaces are used as the functional building blocks of electronic devices. Control of the structural and electronic properties of the thin films is required for reliably operating devices. Here, noncontact atomic force and Kelvin probe force microscopies have been used to investigate the growth and electrostatic landscape of pentacene on KBr(001) and KCl(001) surfaces. We have found that, together with molecular islands of upright standing pentacene, a new phase of tilted molecules appears near step edges on KBr. Local contact potential differences (LCPD) have been studied with both Kelvin experiments and density functional theory calculations. Our images reveal that differently oriented molecules display different LCPD and that their value is independent of the number of molecular layers. These results point to the formation of an interface dipole, which may be explained by a partial charge transfer from the pentacene to the surface. Moreover, the monitoring of the evolution of the pentacene islands shows that they are strongly affected by dewetting: Multilayers build up at the expense of monolayers, and in the Kelvin images, previously unknown line defects appear, which reveal the epitaxial growth of pentacene crystals.

We determine magnetoresistance effects in stable and clean Permalloy nanocontacts of variable cross section, fabricated by UHV deposition and in situ electromigration. To ascertain the magnetoresistance (MR) effects originating from a magnetic domain wall, we measure the resistance values with and without such a wall at zero applied field. In the ballistic transport regime, the MR ratio reaches up to 50% and exhibits a previously unobserved sign change. Our results can be reproduced by recent atomistic calculations for different atomic configurations of the nanocontact, highlighting the importance of the detailed atomic arrangement for the MR effect.

The growth of pentacene on KCl(001) at submonolayer coverage was studied by dynamic scanning force microscopy. At coverages below one monolayer pentacene was found to arrange in islands with an upright configuration. The molecular arrangement was resolved in high-resolution images. In these images two different types of patterns were observed, which switch repeatedly. In addition, defects were found, such as a molecular vacancy and domain boundaries.