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Although fabrication capabilities of Silicon Dangling Bonds have rapidly advanced from manual labor-driven laboratory work to automated manufacturing in just recent years, sub-nanometer substrate defects still pose a hindrance to production due to the need for atomic precision. In essence, unpassivated or missing surface atoms, contaminants, and structural deformations disturb the fabricated logic or prevent its realization altogether. Moreover, design automation techniques in this domain have not yet adopted any defect-aware behavior to circumvent the present obstacles. In this paper, we derive a surface defect model for design automation from experimentally verified defect types that we apply to identify sensitivities in an established gate library in an effort to generate more robust designs. Furthermore, we present an automatic placement and routing algorithm that considers scanning tunneling microscope data obtained from physical experiments to lay out dot-accurate circuitry that is resilient against the presence of atomic surface defects. This culminates in a holistic evaluation on surface data of varying defect rates that enables us to quantify the severity of such defects. We project that fabrication capabilities must achieve defect rates of around 0.1 %, if charged defects can be completely eliminated, or < 0.1 %, otherwise. This realization sets the pace for future efforts to scale up this promising circuit technology., Comment: 7 pages, 5 figures

Recent research interest in emerging logic systems based on quantum dots has been sparked by the experimental demonstration of nanometer-scale logic devices composed of atomically sized quantum dots made of silicon dangling bonds (SiDBs), along with the availability of SiQAD, a computer-aided design tool designed for this technology. Latest design automation frameworks have enabled the synthesis of SiDB circuits that reach the size of $32\times10^3\,\text{nm}^{2}$ -- orders of magnitude more complex than their hand-designed counterparts. However, current SiDB simulation engines do not take defects into account, which is important to consider for these sizable systems. This work proposes a formulation for incorporating fixed-charge simulation into established ground state models to cover an important class of defects that has a non-negligible effect on nearby SiDBs at the $10\,\text{nm}$ scale and beyond. The formulation is validated by implementing it into SiQAD's simulation engine and computationally reproducing experiments on multiple defect types, revealing a high level of accuracy. The new capability is applied towards studying the tolerance of several established logic gates against the introduction of a single nearby defect to establish the corresponding minimum required clearance. These findings are compared against existing metrics to form a foundation for logic robustness studies., Comment: 7 pages, 5 figures, 2 tables

Using a non-contact atomic force microscope (nc-AFM), we examine continuous DB wire structures on the hydrogen-terminated silicon (100) 2x1 surface. By probing the DB structures at varying energies, we identify the formation of previously unobserved ionic charge distributions correlated to the net charge of DB wires and their predicted lattice distortion. Performing spectroscopic analysis, we identify higher energy configurations corresponding to alternative lattice distortions as well as tip-induced charging effects. By varying the length and orientation of these DB structures, we further highlight key features in the formation of these ionic surface phases.

The hydrogen-terminated Silicon(100)-2x1 surface (H-Si(100)-2x1) provides a promising platform for the development of atom scale devices, with recent work showing their creation through precise desorption of surface hydrogen atoms. While samples with relatively large areas of the hydrogen terminated 2x1 surface are routinely created using an in-situ methodology, surface defects are inevitably formed as well reducing the area available for patterning. Here, we present a catalog of several commonly found defects of the H-Si(100)-2x1 surface. By using a combination of scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM), we are able to extract useful information regarding the atomic and electronic structure of these defects. This allowed for the confirmation of literature assignments of several commonly found defects, as well as proposed classification of previously unreported and unassigned defects. By better understanding the structure and origin of these defects, we make the first steps toward enabling the creation of superior surfaces ultimately leading to more consistent and reliable fabrication of atom scale devices.

Many new material systems are being explored to enable smaller, more capable and energy efficient devices. These bottom up approaches for atomic and molecular electronics, quantum computation, and data storage all rely on a well-developed understanding of materials at the atomic scale. Here, we report a versatile scanning tunneling microscope (STM) charge characterization technique, which reduces the influence of the typically perturbative STM tip field, to develop this understanding even further. Using this technique, we can now observe single molecule binding events to atomically defined reactive sites (fabricated on a hydrogen-terminated silicon surface) through electronic detection. We then developed a new error correction tool for automated hydrogen lithography, directing molecular hydrogen binding events using these sites to precisely repassivate surface dangling bonds (without the use of a scanned probe). We additionally incorporated this molecular repassivation technique as the primary rewriting mechanism in new ultra-dense atomic data storage designs (0.88 petabits per in$^{2}$).

With nanoelectronics reaching the limit of atom-sized devices, it has become critical to examine how irregularities in the local environment can affect device functionality. Here, we characterize the influence of charged atomic species on the electrostatic potential of a semiconductor surface at the sub-nanometer scale. Using non-contact atomic force microscopy, two-dimensional maps of the contact potential difference are used to show the spatially varying electrostatic potential on the (100) surface of hydrogen-terminated highly-doped silicon. Three types of charged species, one on the surface and two within the bulk, are examined. An electric field sensitive spectroscopic signature of a single probe atom reports on nearby charged species. The identity of one of the near-surface species has been uncertain. That species, suspected of being boron or perhaps a negatively charged donor species, we suggest is of a character more consistent with either a negatively charged interstitial hydrogen or a hydrogen vacancy complex.

As the development of atom scale devices transitions from novel, proof-of-concept demonstrations to state-of-the-art commercial applications, automated assembly of such devices must be implemented. Here we present an automation method for the identification of defects prior to atomic fabrication via hydrogen lithography using deep learning. We trained a convolutional neural network to locate and differentiate between surface features of the technologically relevant hydrogen-terminated silicon surface imaged using a scanning tunneling microscope. Once the positions and types of surface features are determined, the predefined atomic structures are patterned in a defect-free area. By training the network to differentiate between common defects we are able to avoid charged defects as well as edges of the patterning terraces. Augmentation with previously developed autonomous tip shaping and patterning modules allows for atomic scale lithography with minimal user intervention.

This paper introduces SiQAD, a computer-aided design tool enabling the rapid design and simulation of atomic silicon dangling bond quantum dot patterns capable of computational logic. Several simulation tools are included, each able to inform the designer on various aspects of their designs: a ground-state electron configuration finder, a non-equilibrium electron dynamics simulator, and an electric potential landscape solver with clocking electrode support. Simulations have been compared against past experimental results to inform the electron population estimation and dynamic behavior. New logic gates suitable for this platform have been designed and simulated, and a clocked wire has been demonstrated. This work paves the way for the exploration of the vast and fertile design space of atomic silicon dangling bond quantum dot circuits.

Atomic scale characterization and manipulation with scanning probe microscopy rely upon the use of an atomically sharp probe. Here we present automated methods based on machine learning to automatically detect and recondition the quality of the probe of a scanning tunneling microscope. As a model system, we employ these techniques on the technologically relevant hydrogen-terminated silicon surface, training the network to recognize abnormalities in the appearance of surface dangling bonds. Of the machine learning methods tested, a convolutional neural network yielded the greatest accuracy, achieving a positive identification of degraded tips in 97% of the test cases. By using multiple points of comparison and majority voting, the accuracy of the method is improved beyond 99%. The methods described here can easily be generalized to other material systems and nanoscale imaging techniques.

We report on tuning the carrier capture events at a single dangling bond (DB) midgap state by varying the substrate temperature, doping type, and doping concentration. All-electronic time-resolved scanning tunneling microscopy (TR-STM) is employed to directly measure the carrier capture rates on the nanosecond time scale. A characteristic negative differential resistance (NDR) feature is evident in the scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS) measurements of DBs on both n and p-type doped samples. It is found that a common model accounts for both observations. Atom-specific Kelvin probe force microscopy (KPFM) measurements confirm the energetic position of the DB's charge transition levels, corroborating STS studies. It is shown that under different tip-induced fields the DB can be supplied from two distinct reservoirs: the bulk conduction band and/or the valence band. We measure the filling and emptying rates of the DBs in the energy regime where electrons are supplied by the bulk valence band. By adding point charges in the vicinity of a DB, Coulombic interactions are shown to shift observed STS and NDR features.

Using a non-contact atomic force microscope we track and manipulate the position of single electrons confined to atomic structures engineered from silicon dangling bonds (DBs) on the hydrogen terminated silicon surface. By varying the probe-sample separation we mechanically manipulate the equilibrium position of individual surface silicon atoms and use this to directly switch the charge state of individual DBs. Because this mechanism is based on short range interactions and can be performed without applied bias voltage, we maintain both site-specific selectivity and single-electron control. We extract the short range forces involved with this mechanism by subtracting the long range forces acquired on a dimer vacancy site. As a result of relaxation of the silicon lattice to accommodate negatively charged DBs we observe charge configurations of DB structures that remain stable for many seconds at 4.5 K. Subsequently we use charge manipulation to directly prepare the ground state and metastable charge configurations of DB structures composed of up to six atoms.

The miniaturization of semiconductor devices to the scales where small numbers of dopants can control device properties requires the development of new techniques capable of characterizing their dynamics. Investigating single dopants requires sub-nanometer spatial resolution which motivates the use of scanning tunneling microscopy (STM), however, conventional STM is limited to millisecond temporal resolution. Several methods have been developed to overcome this shortcoming. Among them is all-electronic time-resolved STM, which is used in this work to study dopant dynamics in silicon with nanosecond resolution. The methods presented here are widely accessible and allow for local measurement of a wide variety of dynamics at the atomic scale. A novel time-resolved scanning tunneling spectroscopy technique is presented and used to efficiently search for dynamics.

It has long been anticipated that the ultimate in miniature circuitry will be crafted of single atoms. Despite many advances made in scanned probe microscopy studies of molecules and atoms on surfaces, challenges with patterning and limited thermal stability have remained. Here we make progress toward those challenges and demonstrate rudimentary circuit elements through the patterning of dangling bonds on a hydrogen terminated silicon surface. Dangling bonds sequester electrons both spatially and energetically in the bulk band gap, circumventing short circuiting by the substrate. We deploy paired dangling bonds occupied by one movable electron to form a binary electronic building block. Inspired by earlier quantum dot-based approaches, binary information is encoded in the electron position allowing demonstration of a binary wire and an OR gate.

We report the mechanically induced formation of a silicon-hydrogen covalent bond and its application in engineering nanoelectronic devices. We show that using the tip of a non-contact atomic force microscope (NC-AFM), a single hydrogen atom could be vertically manipulated. When applying a localized electronic excitation, a single hydrogen atom is desorbed from the hydrogen passivated surface and can be transferred to the tip apex as evidenced from a unique signature in frequency shift curves. In the absence of tunnel electrons and electric field in the scanning probe microscope junction at 0 V, the hydrogen atom at the tip apex is brought very close to a silicon dangling bond, inducing the mechanical formation of a silicon-hydrogen covalent bond and the passivation of the dangling bond. The functionalized tip was used to characterize silicon dangling bonds on the hydrogen-silicon surface, was shown to enhance the scanning tunneling microscope (STM) contrast, and allowed NC-AFM imaging with atomic and chemical bond contrasts. Through examples, we show the importance of this atomic scale mechanical manipulation technique in the engineering of the emerging technology of on-surface dangling bond based nanoelectronic devices., Comment: 9 pages (including references and Supplementary Section), 8 figures (5 in the main text, 3 in Supplementary)

Negative differential resistance remains an attractive but elusive functionality, so far only finding niche applications. Atom scale entities have shown promising properties, but viability of device fabrication requires fuller understanding of electron dynamics than has been possible to date. Using an all-electronic time-resolved scanning tunneling microscopy technique and a Green's function transport model, we study an isolated dangling bond on a hydrogen terminated silicon surface. A robust negative differential resistance feature is identified as a many body phenomenon related to occupation dependent electron capture by a single atomic level. We measure all the time constants involved in this process and present atomically resolved, nanosecond timescale images to simultaneously capture the spatial and temporal variation of the observed feature.

We present linear ensembles of dangling bond chains on a hydrogen terminated Si(100) surface, patterned in the closest spaced arrangement allowed by the surface lattice. Local density of states maps over a range of voltages extending spatially over the close-coupled entities reveal a rich energetic and spatial variation of electronic states. These artificial molecules exhibit collective electronic states resulting from covalent interaction of the constituent atoms. A pronounced electrostatic perturbation of dangling bond chain structure is induced by close placement of a negatively dangling bond. The electronic changes so induced are entirely removed, paradoxically, by addition of a second dangling bond.

As the ultimate miniaturization of semiconductor devices approaches, it is imperative that the effects of single dopants be clarified. Beyond providing insight into functions and limitations of conventional devices, such information enables identification of new device concepts. Investigating single dopants requires sub-nanometre spatial resolution, making scanning tunnelling microscopy an ideal tool. However, dopant dynamics involve processes occurring at nanosecond timescales, posing a significant challenge to experiment. Here we use time-resolved scanning tunnelling microscopy and spectroscopy to probe and study transport through a dangling bond on silicon before the system relaxes or adjusts to accommodate an applied electric field. Atomically resolved, electronic pump-probe scanning tunnelling microscopy permits unprecedented, quantitative measurement of time-resolved single dopant ionization dynamics. Tunnelling through the surface dangling bond makes measurement of a signal that would otherwise be too weak to detect feasible. Distinct ionization and neutralization rates of a single dopant are measured and the physical process controlling those are identified.

A new technique for the fabrication of highly sensitive qPlus sensor for atomic force microscopy (AFM) is described. Focused ion beam was used to cut then weld onto a bare quartz tuning fork a sharp micro-tip from an electrochemically etched tungsten wire. The resulting qPlus sensor exhibits high resonance frequency and quality factor allowing increased force gradient sensitivity. Its spring constant can be determined precisely which allows accurate quantitative AFM measurements. The sensor is shown to be very stable and could undergo usual UHV tip cleaning including e-beam and field evaporation as well as in-situ STM tip treatment. Preliminary results with STM and AFM atomic resolution imaging at $4.5\,K$ of the silicon $Si(111)-7\times 7$ surface are presented., Comment: 5 pages, 3 figures

We report the study of single dangling bonds (DB) on the hydrogen terminated silicon (100) surface using a low temperature scanning tunneling microscope (LT-STM). By investigating samples prepared with different annealing temperatures, we establish the critical role of subsurface arsenic dopants on the DB electronic properties. We show that when the near surface concentration of dopants is depleted as a result of $1250{\deg}C$ flash anneals, a single DB exhibits a sharp conduction step in its I(V) spectroscopy that is not due to a density of states effect but rather corresponds to a DB charge state transition. The voltage position of this transition is perfectly correlated with bias dependent changes in STM images of the DB at different charge states. Density functional theory (DFT) calculations further highlight the role of subsurface dopants on DB properties by showing the influence of the DB-dopant distance on the DB state. We discuss possible theoretical models of electronic transport through the DB that could account for our experimental observations., Comment: 21 pages, 6 figures

We review our recent efforts in building atom-scale quantum-dot cellular automata circuits on a silicon surface. Our building block consists of silicon dangling bond on a H-Si(001) surface, which has been shown to act as a quantum dot. First the fabrication, experimental imaging, and charging character of the dangling bond are discussed. We then show how precise assemblies of such dots can be created to form artificial molecules. Such complex structures can be used as systems with custom optical properties, circuit elements for quantum-dot cellular automata, and quantum computing. Considerations on macro-to-atom connections are discussed., Comment: 28 pages, 19 figures

The Si(111) - 7 x 7 surface is one of the most interesting semiconductor surfaces because of its complex reconstruction and fascinating electronic properties. While it is known that the Si - 7 x 7 is a conducting surface, the exact surface conductivity has eluded consensus for decades as measured values differ by 7 orders of magnitude. Here we report a combined STM and transport measurement with ultra-high spatial resolution and minimal interaction with the sample, and quantitatively determine the intrinsic conductivity of the Si - 7 x 7 surface. This is made possible by the capability of measuring transport properties with or without a single atomic step between the measuring probes: we found that even a single step can reduce the surface conductivity by two orders of magnitude. Our first principles quantum transport calculations confirm and lend insight to the experimental observation., Comment: 7 pages (main text+EPAPS), 5 figures

We devise a scheme to characterize tunneling of an excess electron shared by a pair of tunnel-coupled dangling bonds on a silicon surface -- effectively a two-level system. Theoretical estimates show that the tunneling should be highly coherent but too fast to be measured by any conventional techniques. Our approach is instead to measure the time-averaged charge distribution of our dangling-bond pair by a capacitively coupled atomic-force-microscope tip in the presence of both a surface-parallel electrostatic potential bias between the two dangling bonds and a tunable midinfrared laser capable of inducing Rabi oscillations in the system. With a nonresonant laser, the time-averaged charge distribution in the dangling-bond pair is asymmetric as imposed by the bias. However, as the laser becomes resonant with the coherent electron tunneling in the biased pair the theory predicts that the time-averaged charge distribution becomes symmetric. This resonant symmetry effect should not only reveal the tunneling rate, but also the nature and rate of decoherence of single-electron dynamics in our system.

Here we report the direct observation of single electron charging of a single atomic Dangling Bond (DB) on the H-Si(100) 2x1 surface. The tip of a scanning tunneling microscope is placed adjacent to the DB to serve as a single electron sensitive charge-detector. Three distinct charge states of the dangling bond, positive, neutral, and negative, are discerned. Charge state probabilities are extracted from the data, and analysis of current traces reveals the characteristic single electron charging dynamics. Filling rates are found to decay exponentially with increasing tip-DB separation, but are not a function of sample bias, while emptying rates show a very weak dependence on tip position, but a strong dependence on sample bias, consistent with the notion of an atomic quantum dot tunnel coupled to the tip on one side and the bulk silicon on the other., Comment: 7 pages, 6 figures

This report demonstrates the most spatially-coherent electron source ever reported. A coherence angle of 14.3 +/- 0.5 degrees was measured, indicating a virtual source size of 1.7 +/-0.6 Angstrom using an extraction voltage of 89.5 V. The nanotips under study were crafted using a spatially-confined, field-assisted nitrogen etch which removes material from the periphery of the tip apex resulting in a sharp, tungsten-nitride stabilized, high-aspect ratio source. The coherence properties are deduced from holographic measurements in a low-energy electron point source microscope with a carbon nanotube bundle as sample. Using the virtual source size and emission current the brightness normalized to 100 kV is found to be 7.9x10^8 A/sr cm^2.

Quantum-dot Cellular Automata (QCA) provides a basis for classical computation without transistors. Many simulations of QCA rely upon the so-called Intercellular Hartree Approximation (ICHA), which neglects the possibility of entanglement between cells. Here, we present computational results that treat small groups of QCA cells with a Hamiltonian analogous to a quantum mechanical Ising-like spin chain in a transverse field, including the effects of intercellular entanglement. When energy relaxation is included in the model, we find that intercellular entanglement changes the qualitative behaviour of the system, and new features appear. In clocked QCA, isolated groups of active cells experience oscillations in their polarization states as information propagates. Additionally, energy relaxation tends to bring groups of cells to an unpolarized ground state. This contrasts with the results of previous simulations which employed the ICHA. The ICHA is a valid approximation in the limit of very low tunneling rates, which can be realized in lithographically defined quantum-dots. However, in molecular and atomic implementations of QCA, entanglement will play a greater role. The degree to which entanglement poses a problem for memory and clocking depends upon the interaction of the system with its environment, as well as the system's internal dynamics.

During fabrication and scanning-tunneling-microscope (STM) imaging of dangling bonds (DBs) on a hydrogenated silicon surface, we consistently observed halo-like features around isolated DBs for specific imaging conditions. These surround individual or small groups of DBs, have abnormally sharp edges, and cannot be explained by conventional STM theory. Here we investigate the nature of these features by a comprehensive 3-dimensional model of elastic and inelastic charge transfer in the vicinity of a DB. Our essential finding is that non-equilibrium current through the localized electronic state of a DB determines the charging state of the DB. This localized charge distorts the electronic bands of the silicon sample, which in turn affects the STM current in that vicinity causing the halo effect. The influence of various imaging conditions and characteristics of the sample on STM images of DBs is also investigated., Comment: 33 pages, 9 figures

Point Projection Microscopy (PPM) is used to image suspended graphene using low-energy electrons (100-200eV). Because of the low energies used, the graphene is neither damaged or contaminated by the electron beam. The transparency of graphene is measured to be 74%, equivalent to electron transmission through a sheet as thick as twice the covalent radius of sp^2-bonded carbon. Also observed is rippling in the structure of the suspended graphene, with a wavelength of approximately 26 nm. The interference of the electron beam due to the diffraction off the edge of a graphene knife edge is observed and used to calculate a virtual source size of 4.7 +/- 0.6 Angstroms for the electron emitter. It is demonstrated that graphene can be used as both anode and substrate in PPM in order to avoid distortions due to strong field gradients around nano-scale objects. Graphene can be used to image objects suspended on the sheet using PPM, and in the future, electron holography.

Motivated by the need for less destructive imaging of nanostructures, we pursue point-source in-line holography (also known as point projection microscopy, or PPM) with very low energy electrons (-100 eV). This technique exploits the recent creation of ultrasharp and robust nanotips, which can field emit electrons from a single atom at their apex, thus creating a path to an extremely coherent source of electrons for holography. Our method has the potential to achieve atom resolved images of nanostructures including biological molecules. We demonstrate a further advantage of PPM emerging from the fact that the very low energy electrons employed experience a large elastic scattering cross section relative to many-keV electrons. Moreover, the variation of scattering factors as a function of atom type allows for enhanced elemental contrast. Low energy electrons arguably offer the further advantage of causing minimum damage to most materials. Model results for small molecules and adatoms on graphene substrates, where very small damage is expected, indicate that a phase contrast is obtainable between elements with significantly different Z-numbers. For example, for typical setup parameters, atoms such as C and P are discernible, while C and N are not., Comment: 15 pages, 5 figures

Two closely spaced dangling bonds positioned on a silicon surface and sharing an excess electron are revealed to be a strong candidate for a charge qubit. Based on our study of the coherent dynamics of this qubit, its extremely high tunneling rate ~ 10^14 1/s greatly exceeds the expected decoherence rates for a silicon-based system, thereby overcoming a critical obstacle of charge qubit quantum computing. We investigate possible configurations of dangling bond qubits for quantum computing devices. A first-order analysis of coherent dynamics of dangling bonds shows promise in this respect., Comment: 17 pages, 3 EPS figures, 1 table

We report on the synthesis, scanning tunneling microscopy (STM) and theoretical modeling of the electrostatic and transport properties of one-dimensional organic heterostructures consisting of contiguous lines of CF3- and OCH3-substituted styrene molecules on silicon. The electrostatic fields emanating from these polar molecules are found, under appropriate conditions, to strongly influence electrical conduction through nearby molecules and the underlying substrate. For suitable alignment of the OCH3 groups of the OCH3-styrene molecules in the molecular chain, their combined electric fields are shown by ab initio density functional calculations to give rise to potential profiles along the OCH3-styrene chain that result in strongly enhanced conduction through OCH3-styrene molecules near the heterojunction for moderately low negative substrate bias, as is observed experimentally. Under similar bias conditions, dipoles associated with the CF3 groups are found in both experiment and in theory to depress transport in the underlying silicon. Under positive substrate bias, simulations suggest that the differing structural and electrostatic properties of the CF3-styrene molecules may lead to a more sharply localized conduction enhancement near the heterojunction at low temperatures. Thus choice of substituents, their attachment site on the host styrene molecules on silicon and the orientations of the molecular dipole and higher multipole moments provide a means of differentially tuning transport on the molecular scale., Comment: 31 pages including 13 figures

One-dimensional organic heterostructures consisting of contiguous lines of CF3- and OCH3-substituted styrene molecules on silicon are studied by scanning tunneling microscopy and ab initio simulation. Dipole fields of OCH3-styrene molecules are found to enhance conduction through molecules near OCH3-styrene/CF3-styrene heterojunctions. Those of CF3-styrene depress transport through the nearby silicon. Thus choice of substituents and their attachment site on host molecules provide a means of differentially tuning molecule and substrate transport at the molecular scale., Comment: 4 pages, 4 figures. To be published in Physical Review Letters

It is discovered that the zero-dimensional character of the silicon atom dangling bond (DB) state allows controlled formation and occupation of a new form of quantum dot assemblies. Whereas on highly doped n-type substrates isolated DBs are negatively charged, it is found that Coulomb repulsion causes DBs separated by less than ~2 nm to experience reduced localized charge. The unoccupied states so created allow a previously unobserved electron tunnel-coupling of DBs, evidenced by a pronounced change in the time-averaged view recorded by scanning tunneling microscopy. Direct control over net electron occupation and tunnel-coupling of multi-DB ensembles through separation controlled is demonstrated. Through electrostatic control, it is shown that a pair of tunnel-coupled DBs can be switched from a symmetric bi-stable state to one exhibiting an asymmetric electron occupation. Similarly, the setting of an antipodal state in a square assembly of four DBs is achieved, demonstrating at room temperature the essential building block of a quantum cellular automata device., Comment: 19 pages, six figure - Supporting Information included

We report on the synthesis, STM imaging and theoretical studies of the structure, electronic structure and transport properties of linear chains of styrene and methyl-styrene molecules and their heterojunctions on hydrogen-terminated dimerized silicon (001) surfaces. The theory presented here accounts for the essential features of the experimental STM data including the nature of the corrugation observed along the molecular chains and the pronounced changes in the contrast between the styrene and methyl-styrene parts of the molecular chains that are observed as the applied bias is varied. The observed evolution with applied bias of the STM profiles near the ends of the molecular chains is also explained. Calculations are also presented of electron transport along styrene linear chains adsorbed on the silicon surface at energies in the vicinity of the molecular HOMO and LUMO levels. For short styrene chains this lateral transport is found to be due primarily to direct electron transmission from molecule to molecule rather than through the silicon substrate, especially in the molecular LUMO band. Differences between the calculated position-dependences of the STM current around a junction of styrene and methyl-styrene molecular chains under positive and negative tip bias are related to the nature of lateral electron transmission along the molecular chains and to the formation in the LUMO band of an electronic state localized around the heterojunction., Comment: 17 pages plus 11 figures. To appear in Physical Review B

We have performed the most realistic simulation to date of the operation of a scanning tunneling microscope. Probe-sample distances from beyond tunneling to actual surface contact are covered. We simultaneously calculate forces, atomic displacements, and tunneling currents, allowing quantitative comparison with experimental values. A distance regime below which the probe becomes unstable is identified. It is shown that the real distance differs substantially from previous estimates because of large atomic displacements on the surface and at the probe-tip., Comment: Four pages (RevTeX) and four figures (EPS). Now published in PRL