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Spin states in semiconductors provide exceptionally stable and noise-resistant environments for qubits, positioning them as optimal candidates for reliable quantum computing technologies. The proposal to use nuclear and electronic spins of donor atoms in silicon, introduced by Kane in 1998, sparked a new research field focused on the precise positioning of individual impurity atoms for quantum devices, utilising scanning tunnelling microscopy and ion implantation. This roadmap article reviews the advancements in the 25 years since Kane's proposal, the current challenges, and the future directions in atomic-scale semiconductor device fabrication and measurement. It covers the quest to create a silicon-based quantum computer and expands to include diverse material systems and fabrication techniques, highlighting the potential for a broad range of semiconductor quantum technological applications. Key developments include phosphorus in silicon devices such as single-atom transistors, arrayed few-donor devices, one- and two-qubit gates, three-dimensional architectures, and the development of a toolbox for future quantum integrated circuits. The roadmap also explores new impurity species like arsenic and antimony for enhanced scalability and higher-dimensional spin systems, new chemistry for dopant precursors and lithographic resists, and the potential for germanium-based devices. Emerging methods, such as photon-based lithography and electron beam manipulation, are discussed for their disruptive potential. This roadmap charts the path toward scalable quantum computing and advanced semiconductor quantum technologies, emphasising the critical intersections of experiment, technological development, and theory., Comment: 94 pages

Bare silicon dimers on hydrogen-terminated Si(100) have two dangling bonds. These are atomically localized regions of high state density near to and within the bulk silicon band gap. We studied bare silicon dimers as monomeric units. Silicon dimer wires are much more stable than wires composed of individual dangling bonds. Dimer wires composed of 1 to 5 dimers were intentionally fabricated and characterised by STM techniques combined with density functional theory to provide detailed insights into geometric and electronic structure. Structural and dynamic qualities displayed by short wires were shown to be similar to the characteristics of a relatively long 37 dimer wire. Rather than adding two states into the band gap, experiment and theory reveal that each dimer adds one empty state into the gap and one filled state into the valence bands. Coupling among these states provides a conduction pathway with small bulk coupling., Comment: 14 pages, 5 figures

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.

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.

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.

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 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

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.

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

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

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