The dielectric constant of a bilayer graphene interface.

The interlayer relative dielectric constant, ε r, of 2-dimensional (2D) materials in general and graphitic materials in particular is one of their most important physical properties, especially for electronic applications. In this work, we study the electromechanical actuation of nano-scale graphitic contacts. We find that beside the adhesive forces there are capacitive forces that scale parabolically with the potential drop across the sheared interface. We use this phenomena to measure the intrinsic dielectric constant of the bilayer graphene interface i.e. ε r = 6 ± 2, which is in perfect agreement with recent theoretical predictions for multi-layer graphene structures. Our method can be generally used to extract the dielectric properties of 2D materials systems and interfaces and our results pave the way for utilizing graphitic and other 2D materials in electromechanical based applications.

Fast turnaround fabrication of silicon point-contact quantum-dot transistors using combined thermal scanning probe lithography and laser writing.

The fabrication of high-performance solid-state silicon quantum-devices requires high resolution patterning with minimal substrate damage. We have fabricated room temperature (RT) single-electron transistors (SETs) based on point-contact tunnel junctions using a hybrid lithography tool capable of both high resolution thermal scanning probe lithography and high throughput direct laser writing. The best focal z-position and the offset of the tip- and the laser-writing positions were determined in situ with the scanning probe. We demonstrate <100 nm precision in the registration between the high resolution and high throughput lithographies. The SET devices were fabricated on degenerately doped n-type >1020/cm3 silicon on insulator chips using a CMOS compatible geometric oxidation process. The characteristics of the three devices investigated were dominated by the presence of Si nanocrystals or phosphorous atoms embedded within the SiO2, forming quantum dots (QDs). The small size and strong localisation of electrons on the QDs facilitated SET operation even at RT. Temperature measurements showed that in the range 300 K > T > âˆ¼100 K, the current flow was thermally activated but at <100 K, it was dominated by tunnelling.

Experimental Observation of Current Reversal in a Rocking Brownian Motor.

A reversal of the particle current in overdamped rocking Brownian motors was predicted more than 20 years ago; however, an experimental verification and a deeper insight into this noise-driven mechanism remained elusive. Here, we investigate the high-frequency behavior of a rocking Brownian motor for 60 nm gold spheres based on electrostatic interaction in a 3D-shaped nanofluidic slit and electro-osmotic forcing of the particles. We measure the particle probability density in situ with 10 nm spatial and 250 µs temporal resolution and compare it with theory. At a driving frequency of 250 Hz, we observe a current reversal that can be traced to the asymmetric and increasingly static probability density at high frequencies.

Explaining the Transition from Diffusion Limited to Reaction Limited Surface Assembly of Molecular Species through Spatial Variations.

Surface assembly is often decomposed into two classes: diffusion and reaction limited processes. The transition between the two cases is complex because the dynamics are so different. In this article, we simulate, explain, and experimentally discuss the evolution of the spatial distribution for surface assemblies with diffusion limited and reaction limited processes. Explicitly, we demonstrate that diffusion limited and reaction limited processes show some temporal differences, but more importantly, we show that the spatial arrangements are different enough to discriminate between the two cases. Using fundamental properties, such as the diffusion constant, we calculate the evolution of the spatial profile and derive from physical, heuristic models the assembly rate for reaction and diffusion limited processes based on the individual particle's interactions with the surface. Finally, we confirm the spatial profile differences between diffusion and reaction limited cases by experimentally measuring the surface assembly between two molecules of similar size, but having different assembly routes. Unique to our description is that we have derived and simulated everything through the particle picture in place of ensemble descriptions such as the diffusion equation, and we show the equivalence between our heuristic formulas and those derived from the diffusion equation.

Testing the Equivalence between Spatial Averaging and Temporal Averaging in Highly Dilute Solutions.

Diffusion relates the flux of particles to the local gradient of the particle density in a deterministic way. The question arises as to what happens when the particle density is so low that the local gradient becomes an ill-defined concept. The dilemma was resolved early last century by analyzing the average motion of particles subject to random forces whose magnitude is such that the particles are always in thermal equilibrium with their environment. The diffusion dynamics is now described in terms of the probability density of finding a particle at some position and time and the probabilistic flux density, which is proportional to the gradient of the probability density. In a time average sense, the system thus behaves exactly like the ensemble average. Here, we report on an experimental method and test this fundamental equivalence principle in statistical physics. In the experiment, we study the flux distribution of 20 nm radius polystyrene particles impinging on a circular sink of micrometer dimensions. The particle concentration in the water suspension is approximately 1 particle in a volume element of the dimension of the sink. We demonstrate that the measured flux density is exactly described by the solution of the diffusion equation of an infinite system, and the flux statistics obeys a Poissonian distribution as expected for a Markov process governing the random walk of noninteracting particles. We also rigorously show that a finite system behaves like an infinite system for very long times despite the fact that a finite system converges to a zero flux empty state.

Control of the interaction strength of photonic molecules by nanometer precise 3D fabrication.

Applications for high resolution 3D profiles, so-called grayscale lithography, exist in diverse fields such as optics, nanofluidics and tribology. All of them require the fabrication of patterns with reliable absolute patterning depth independent of the substrate location and target materials. Here we present a complete patterning and pattern-transfer solution based on thermal scanning probe lithography (t-SPL) and dry etching. We demonstrate the fabrication of 3D profiles in silicon and silicon oxide with nanometer scale accuracy of absolute depth levels. An accuracy of less than 1nm standard deviation in t-SPL is achieved by providing an accurate physical model of the writing process to a model-based implementation of a closed-loop lithography process. For transfering the pattern to a target substrate we optimized the etch process and demonstrate linear amplification of grayscale patterns into silicon and silicon oxide with amplification ratios of ∼6 and ∼1, respectively. The performance of the entire process is demonstrated by manufacturing photonic molecules of desired interaction strength. Excellent agreement of fabricated and simulated structures has been achieved.

Understanding How Charged Nanoparticles Electrostatically Assemble and Distribute in 1-D.

The effects of increasing the driving forces for a 1-D assembly of nanoparticles onto a surface are investigated with experimental results and models. Modifications, which take into account not only the particle-particle interactions but also particle-surface interactions, to previously established extended random sequential adsorption simulations are tested and verified. Both data and model are compared against the heterogeneous random sequential adsorption simulations, and finally, a connection between the two models is suggested. The experiments and models show that increasing the particle-surface interaction leads to narrower particle distribution; this narrowing is attributed to the surface interactions compensating against the particle-particle interactions. The long-term advantage of this work is that the assembly of nanoparticles in solution is now understood as controlled not only by particle-particle interactions but also by particle-surface interactions. Both particle-particle and particle-surface interactions can be used to tune how nanoparticles distribute themselves on a surface.

Coherent commensurate electronic states at the interface between misoriented graphene layers.

Graphene and layered materials in general exhibit rich physics and application potential owing to their exceptional electronic properties, which arise from the intricate π-orbital coupling and the symmetry breaking in twisted bilayer systems. Here, we report room-temperature experiments to study electrical transport across a bilayer graphene interface with a well-defined rotation angle between the layers that is controllable in situ. This twisted interface is artificially created in mesoscopic pillars made of highly oriented pyrolytic graphite by mechanical actuation. The overall measured angular dependence of the conductivity is consistent with a phonon-assisted transport mechanism that preserves the electron momentum of conduction electrons passing the interface. The most intriguing observations are sharp conductivity peaks at interlayer rotation angles of 21.8° and 38.2°. These angles correspond to a commensurate crystalline superstructure leading to a coherent two-dimensional (2D) electronic interface state. Such states, predicted by theory, form the basis for a new class of 2D weakly coupled bilayer systems with hitherto unexplored properties and applications.

Accurate Location and Manipulation of Nanoscaled Objects Buried under Spin-Coated Films.

Detection and precise localization of nanoscale structures buried beneath spin-coated films are highly valuable additions to nanofabrication technology. In principle, the topography of the final film contains information about the location of the buried features. However, it is generally believed that the relation is masked by flow effects, which lead to an upstream shift of the dry film's topography and render precise localization impossible. Here we demonstrate, theoretically and experimentally, that the flow-shift paradigm does not apply at the submicrometer scale. Specifically, we show that the resist topography is accurately obtained from a convolution operation with a symmetric Gaussian kernel whose parameters solely depend on the resist characteristics. We exploit this finding for a 3 nm precise overlay fabrication of metal contacts to an InAs nanowire with a diameter of 27 nm using thermal scanning probe lithography.

Surface science. Adhesion and friction in mesoscopic graphite contacts.

The weak interlayer binding in two-dimensional layered materials such as graphite gives rise to poorly understood low-friction characteristics. Accurate measurements of the adhesion forces governing the overall mechanical stability have also remained elusive. We report on the direct mechanical measurement of line tension and friction forces acting in sheared mesoscale graphite structures. We show that the friction is fundamentally stochastic in nature and is attributable to the interaction between the incommensurate interface lattices. We also measured an adhesion energy of 0.227 ± 0.005 joules per square meter, in excellent agreement with theoretical models. In addition, bistable all-mechanical memory cell structures and rotational bearings have been realized by exploiting position locking, which is provided solely by the adhesion energy.

Thermal probe maskless lithography for 27.5 nm half-pitch Si technology.

Thermal scanning probe lithography is used for creating lithographic patterns with 27.5 nm half-pitch line density in a 50 nm thick high carbon content organic resist on a Si substrate. The as-written patterns in the poly phthaladehyde thermal resist layer have a depth of 8 nm, and they are transformed into high-aspect ratio binary patterns in the high carbon content resist using a SiO2 hard-mask layer with a thickness of merely 4 nm and a sequence of selective reactive ion etching steps. Using this process, a line-edge roughness after transfer of 2.7 nm (3σ) has been achieved. The patterns have also been transferred into 50 nm deep structures in the Si substrate with excellent conformal accuracy. The demonstrated process capabilities in terms of feature density and line-edge roughness are in accordance with today's requirements for maskless lithography, for example for the fabrication of extreme ultraviolet (EUV) masks.

Nanoscale thermomechanics of wear-resilient polymeric bilayer systems.

We explore the effect of an ultrathin elastic coating to optimize the mechanical stability of an underlying polymer film for nanoscale applications. The coating consists of a several nanometer thin plasma-polymerized norbornene layer. Scanning probes are used to characterize the system in terms of shear-force-induced wear and thermally assisted indentation. The layer transforms a weakly performing polystyrene film into a highly wear-resistive system, ideal for high-density and low-power data storage applications. The result can be understood from the indentation characteristics with a hot and sharp indenter tip. The latter gives rise to a deformation mode in the fully plastic regime, enabling a simple interpretation of the results. The softening transition and the yield stress of the system on a microsecond time scale and a nanometer size scale were obtained. We show that the plastic deformation is governed by yielding in the polystyrene sublayer, which renders the overall system soft for plastic deformation. The ultrathin protection layer contributes as an elastic skin, which shields part of the temperature and pressure and enables the high wear resistance against lateral forces. Moreover, the method of probing polymers at microsecond and nanometer size scales opens up new opportunities for studying polymer physics in a largely unexplored regime. Thus, we find softening temperatures of more than 100 °C above the polystyrene glass transition, which implies that for the short interaction time scales the glassy state of the polymer is preserved up to this temperature.

Directed placement of gold nanorods using a removable template for guided assembly.

We have used a temperature sensitive polymer film as a removable template to position, and align, gold nanorods onto an underlying target substrate. Shape-matching guiding structures for the assembly of nanorods of size 80 nm × 25 nm have been written by thermal scanning probe lithography. The nanorods were assembled into the guiding structures, which determine both the position and the orientation of single nanorods, by means of capillary interactions. Following particle assembly, the polymer was removed cleanly by thermal decomposition and the nanorods are transferred to the underlying substrate. We have thus demonstrated both the placement and orientation of nanorods with an overall positioning accuracy of ≈10 nm onto an unstructured target substrate.

Rapid turnaround scanning probe nanolithography.

Scanning probe nanolithography (SPL) has demonstrated its potential in a variety of applications like 3D nanopatterning, 'direct development' lithography, dip-pen deposition or patterning of self-assembled monolayers. One of the main issues holding back SPL has been the limited throughput for patterning and imaging. Here we present a complete lithography and metrology system based on thermomechanical writing into organic resists. Metrology is carried out using a thermoelectric topography sensing method. More specifically, we demonstrate a system with a patterning pixel clock of 500 kHz, 20 mm s(-1) linear scan speed, a positioning accuracy of 10 nm, a read-back frequency bandwidth of 100, 000 line-pairs s(-1) and a turnaround time from patterning to qualifying metrology of 1 min. Thus, we demonstrate a nanolithography system capable of implementing rapid turnaround.

Nanoscale three-dimensional patterning of molecular resists by scanning probes.

For patterning organic resists, optical and electron beam lithography are the most established methods; however, at resolutions below 30 nanometers, inherent problems result from unwanted exposure of the resist in nearby areas. We present a scanning probe lithography method based on the local desorption of a glassy organic resist by a heatable probe. We demonstrate patterning at a half pitch down to 15 nanometers without proximity corrections and with throughputs approaching those of Gaussian electron beam lithography at similar resolution. These patterns can be transferred to other substrates, and material can be removed in successive steps in order to fabricate complex three-dimensional structures.

Ultraflat templated polymer surfaces.

The roughness of spin-cast polymer films arises from thermally activated capillary waves during preparation and typically amounts to about 0.5 nm(rms) measured on a micrometer-sized surface area. Templating from atomically flat mica substrates allows the creation of polymer films with a surface roughness approaching the molecular scale. Three regimes of spatial frequencies are identified in which the roughness is controlled by different physical mechanisms. We find that frozen-in elastic pressure waves ultimately limit the flatness of polymer films.

Controlling nanowear in a polymer by confining segmental relaxation.

Molecular relaxation of a copolymer designed for nano-electromechanical systems was chemically confined by varying the spacing between cross-links, delta(c). A critical cross-link spacing of 1-3 nm marks a transition in the nano-mechanical properties evaluated by atomic force microscopy. The transition reveals an interplay between the cross-link spacing and the length scale for backbone relaxation, xi(alpha), in cooperatively rearranging regions. For delta(c) >> xi(alpha), the natural backbone relaxation process is relatively unaffected by the cross-links and a ductile, low hardness behavior results. For delta(c) < xi(alpha), the cross-links directly interfere with backbone relaxation and confine segmental mobility, leading to a brittle, high hardness response.