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 moveable 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.The prospect of atom scale computing was initially indicated by "molecular cascades"where sequentially toppling molecules were arranged in precise configurations to achieve binary logic functions 1 . Many notable approaches toward molecular electronics 2-7 , atomic electronics 8,9 , and quantum-dot-based electronics 10-15 have also been explored.The quantum dot based approaches [16][17][18][19][20] are particularly attractive, as they provide a low power yet fast basis 21 to go beyond today's CMOS technology 22 . These approaches, however, require cryogenic temperatures to minimize the population of thermally-excited states and achieve the desired functionality. Variability among quantum dots and sensitivity to uncontrolled fields are
At the atomic scale, there has always been a trade-off between the ease of fabrication of structures and their thermal stability. Complex structures that are created effortlessly often disorder above cryogenic conditions. Conversely, systems with high thermal stability do not generally permit the same degree of complex manipulations. Here, we report scanning tunneling microscope (STM) techniques to substantially improve automated hydrogen lithography (HL) on silicon, and to transform state-of-the-art hydrogen repassivation into an efficient, accessible error correction/editing tool relative to existing chemical and mechanical methods. These techniques are readily adapted to many STMs, together enabling fabrication of error-free, room-temperature stable structures of unprecedented size. We created two rewriteable atomic memories (1.1 petabits per in2), storing the alphabet letter-by-letter in 8 bits and a piece of music in 192 bits. With HL no longer faced with this trade-off, practical silicon-based atomic-scale devices are poised to make rapid advances towards their full potential.
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.
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 highlydoped 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
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.
The origin of bond-resolved atomic force microscope images remains controversial. Moreover, most work to date has involved planar, conjugated hydrocarbon molecules on a metal substrate thereby limiting knowledge of the generality of findings made about the imaging mechanism. Here we report the study of a very different sample; a hydrogen-terminated silicon surface. A procedure to obtain a passivated hydrogen-functionalized tip is defined and evolution of atomic force microscopy images at different tip elevations are shown. At relatively large tip-sample distances, the topmost atoms appear as distinct protrusions. However, on decreasing the tip-sample distance, features consistent with the silicon covalent bonds of the surface emerge. Using a density functional tight-binding-based method to simulate atomic force microscopy images, we reproduce the experimental results. The role of the tip flexibility and the nature of bonds and false bond-like features are discussed.
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 combination of scanning tunnelling microscopy (STM) and non-contact atomic force microscopy (nc-AFM) allows enhanced extraction and correlation of properties not readily available via a single imaging mode. We demonstrate this through the characterization and classification of several commonly found defects of the hydrogen-terminated silicon (100)-2 × 1 surface (H–Si(100)-2 × 1) by using six unique imaging modes. The H–Si surface was chosen as it provides a promising platform for the development of atom scale devices, with recent work showing their creation through precise desorption or placement of surface hydrogen atoms. While samples with relatively large areas of the H–Si surface are routinely created using an in situ methodology, surface defects are inevitably formed reducing the area available for patterning. By probing the surface using the different interactivity afforded by either hydrogen- or silicon-terminated tips, we are able to extract new insights regarding the atomic and electronic structure of these defects. This allows for the confirmation of literature assignments of several commonly found defects, as well as proposed classifications of previously unreported and unassigned defects. By combining insights from multiple imaging modes, better understanding of their successes and shortcomings in identifying defect structures and origins is achieved. With this, we take the first steps toward enabling the creation of superior H–Si surfaces through an improved understanding of surface defects, ultimately leading to more consistent and reliable fabrication of atom scale devices.
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