Scanning Tunneling Microscope Lithography Research Articles

Machine Learning-Assisted Precision Manufacturing of Atom Qubits in Silicon.

Donor-based qubits in silicon, manufactured using scanning tunneling microscope (STM) lithography, provide a promising route to realizing full-scale quantum computing architectures. This is due to the precision of donor placement, long coherence times, and scalability of the silicon material platform. The properties of multiatom quantum dot qubits, however, depend on the exact number and location of the donor atoms within the quantum dots. In this work, we develop machine learning techniques that allow accurate and real-time prediction of the donor number at the qubit site during STM patterning. Machine learning image recognition is used to determine the probability distribution of donor numbers at the qubit site directly from STM images during device manufacturing. Models in excess of 90% accuracy are found to be consistently achieved by mitigating overfitting through reduced model complexity, image preprocessing, data augmentation, and examination of the intermediate layers of the convolutional neural networks. The results presented in this paper constitute an important milestone in automating the manufacture of atom-based qubits for computation and sensing applications.

Multi‐Scale Modeling of Tunneling in Nanoscale Atomically Precise Si:P Tunnel Junctions

AbstractControlling electron tunneling is of fundamental importance in the design and operation of semiconductor nanostructures such as field effect transistors (FETs) and quantum computing device architectures. The exponential sensitivity of tunneling with distance requires precise fabrication techniques to engineer the desired device dimensions to achieve the appropriate tunneling resistances/tunnel rates. This is particularly important for high fidelity spin readout and qubit exchange in quantum computing architectures. Here, it is shown by combining precision fabrication techniques with accurate atomistic modeling, predictive device design criteria are achieved at atomic length scales. Such a tool is useful when devices become more complex or have arbitrary shapes/geometries. In particular, in this study, atomic precision patterning of monolayer degenerately phosphorus‐doped silicon tunnel junctions patterned by scanning tunnelling microscopy lithography and tight‐binding non‐equilibrium Green's function (TB‐NEGF) modeling is combined to describe the dependence of tunnel junction resistance RT on junction length. An agreement with experiment to within a factor of 2 over 4 orders of magnitude in RT is found, and this model allows to accurately determine the barrier height V0 = 57.5 ± 1 meV and lateral seam sxy = 0.39 ± 0.01 nm in these nanoscale junctions. This study confirms the use of the TB‐NEGF formalism to accurately model highly doped atomically precise tunnel junctions in silicon. Further applications of this model will enable improved device performance at the nanoscale.

Atomic-resolution lithography with an on-chip scanning tunneling microscope

In this work, atomic-resolution lithography with a Microelectromechanical-System (MEMS) based Scanning Tunneling Microscope (STM) is demonstrated for the first time. The microscope consists of a commercial UltraHigh-Vacuum (UHV) STM whose regular tip is replaced with a 1-Degree-of-Freedom (1-DOF) MEMS nanopositioner. This results in a hybrid STM system where XY-plane motions are provided by the piezotube of the original system and Z-axis motion by the MEMS with a higher bandwidth. Sharp tips made of Pt or W are added to the MEMS devices with postfabrication techniques. With this hybrid system, STM-based lithography is demonstrated on an H-passivated Si (100)-2×1 sample under UHV condition. Results prove the capability of the hybrid STM system for atomic-scale lithography. This capability, paired with the small footprint of the MEMS device, makes this approach a candidate for building a high-throughput parallel STM lithography platform by incorporating an array of 1-DOF MEMS devices that perform lithography in parallel.

Impact of Incorporation Kinetics on Device Fabrication with Atomic Precision

Scanning tunneling microscope lithography can be used to create nanoelectronic devices in which dopant atoms are precisely positioned in a $\mathrm{Si}$ lattice within approximately $1$ nm of a target position. This exquisite precision is promising for realizing various quantum technologies. However, a potentially impactful form of disorder is due to incorporation kinetics, in which the number of P atoms that incorporate into a single lithographic window is manifestly uncertain. We present experimental results indicating that the likelihood of incorporating into an ideally written three-dimer single-donor window is $63\ifmmode\pm\else\textpm\fi{}10\mathrm{%}$ for room-temperature dosing, and corroborate these results with a model for the incorporation kinetics. Nevertheless, further analysis of this model suggests conditions that might raise the incorporation rate to near-deterministic levels. We simulate bias spectroscopy on a chain of comparable dimensions to the array in our yield study, indicating that such an experiment may help confirm the inferred incorporation rate.

Ohmic Contact to Two-Dimensional Nanofabricated Silicon Structures with a Two-Probe Scanning Tunneling Microscope.

We used multiprobe scanning tunneling microscope (STM) to fabricate and electrically characterize nanostructures on Si surfaces. We overcame resistive contacts by using field evaporation to clean tip apexes in order to create Ohmic contact with the Si surface states on a Si substrate. A two-probe (2P-) STM with Ohmic contact allowed for measurement at very low bias, limiting conduction through space-charge layer and bulk states. The Ohmic 2P-STM measurement clarified the surface conductivity of the Si(111)-(7 × 7) surface. We also confirmed that Ohmic 2P-STM can be replaced with more convenient Ohmic one-probe STM for the conductance measurements on the Si surface. We prepared nanostructures using STM lithography to define electronically isolated two-dimensional (2D) regions with various aspect ratios. Their surface conduction properties are described well by the conventional sheet model, proving the diffusive 2D conduction on the Si surface. Constrictions and breaks in 2D structures were also evaluated. Ohmic 2P-STM will be helpful for the investigation of exploratory atomic-scale circuitry or cutting-edge materials sciences.

STM-Induced Desorption and Lithographic Patterning of Cl-Si(100)-(2 × 1).

A scanning tunneling microscope (STM) was used to investigate tip-induced chlorine desorption and lithographic patterning of Cl-terminated Si(100)-(2 × 1) surfaces from 4 to 600 K in ultrahigh vacuum. Until now, STM lithography has exclusively focused on hydrogen-based chemistry for donor device fabrication. As the initial step in developing halogen-based chemistries for STM fabrication of acceptor-based devices, we substituted the hydrogen resist with chlorine. We found that chlorine can be selectively desorbed by the STM tip using both electron and hole injection. Observations show that targeted chlorine was not driven into the surface but desorbed completely as both individual and pairs of atoms. Chlorine depassivation lithography is demonstrated using both field-emission patterning to desorb chlorine from large areas with high efficiency (0.83(1)) and atomic-precision patterning to desorb one to two dimer rows at a time, resulting in 1.5 nm wide lines. Further, varying the experimental parameters for lithography revealed a positive correlation between pattern line widths and both positive sample bias voltage (1.7(2) nm/V) and total electron dose (0.15(2) nm/(mC/cm)), demonstrating that the energy and total number of electrons play a role in desorption from multiple sites.

Ab Initio Study of the Early Stage of Si Epitaxy on the Chlorinated Si(100) Surface

The homoepitaxial growth of Si on Si(100) covered by a resist mask is a necessary technological step for the fabrication of donor-based quantum devices with scanning tunneling microscope lithography. In the present work, the chlorine monolayer is selected as the resist. Using density functional theory, we investigated the adsorption of a single silicon atom on Si(100)-2$\times$1-Cl as the starting process of Si epitaxy. The incorporation of a silicon atom under a Cl monolayer proved to be the most energetically favorable process. Our results show that chlorine segregates on the surface during Si deposition and does not incorporate into homoepitaxial layers. In addition, we found that SiCl$_2^{\ast}$, SiCl$_3^{\ast}$, and SiCl$_4^{\ast}$ clusters can be formed above a Si(100)-2$\times$1-Cl surface while Si is adsorbed. SiCl$_2^{\ast}$ clusters are bound weakly to the substrate, and their desorption leaves the silicon surface free of chlorine. To check whether the Si epitaxy is possible on the chlorine resist, we compare our results with the well-studied case of a hydrogen resist. We find the two processes to be similar; moreover, epitaxy on chlorine resist appears to have an advantage.

Characterization of a Scalable Donor-Based Singlet-Triplet Qubit Architecture in Silicon.

We present a donor-based quadruple-quantum-dot device, designed to host two singlet-triplet qubits fabricated by scanning tunnelling microscope lithography, with just two leads per qubit. The design is geometrically compact, with each pair of dots independently controlled via one gate and one reservoir. The reservoirs both supply electrons for the dots and measure the singlet-triplet state of each qubit via dispersive sensing. We verify the locations of the four phosphorus donor dots via an electrostatic model of the device. We study one of the observed singlet-triplet states with a tunnel coupling of 39 GHz and a S0-to- T- decay of 2 ms at zero detuning. We measure a 5 GHz electrostatic interaction between two pairs of dots separated by 65 nm. The results outline a low-gate-density pathway to a scalable 1D building block of atomic-precision singlet-triplet qubits using donors with dispersive readout.

Charge sensing of a few-donor double quantum dot in silicon

We demonstrate the charge sensing of a few-donor double quantum dot precision placed with atomic resolution scanning tunnelling microscope lithography. We show that a tunnel-coupled single electron transistor (SET) can be used to detect electron transitions on both dots as well as inter-dot transitions. We demonstrate that we can control the tunnel times of the second dot to the SET island by ∼4 orders of magnitude by detuning its energy with respect to the first dot.

Imaging of buried phosphorus nanostructures in silicon using scanning tunneling microscopy

We demonstrate the locating and imaging of single phosphorus atoms and phosphorus dopant nanostructures, buried beneath the Si(001) surface using scanning tunneling microscopy. The buried dopant nanostructures have been fabricated in a bottom-up approach using scanning tunneling microscope lithography on Si(001). We find that current imaging tunneling spectroscopy is suited to locate and image buried nanostructures at room temperature and with residual surface roughness present. From these studies, we can place an upper limit on the lateral diffusion during encapsulation with low-temperature Si molecular beam epitaxy.

Transport in Asymmetrically Coupled Donor-Based Silicon Triple Quantum Dots

We demonstrate serial electron transport through a donor-based triple quantum dot in silicon fabricated with nanoscale precision by scanning tunnelling microscopy lithography. From an equivalent circuit model, we calculate the electrochemical potentials of the dots allowing us to identify ground and excited states in finite bias transport. Significantly, we show that using a scanning tunnelling microscope, we can directly demonstrate that a ∼1 nm difference in interdot distance dramatically affects transport pathways between the three dots.

Tunneling electron induced chemisorption of copper phthalocyanine molecules on the Cu(111) surface

The adsorption of up to one monolayer (ML) of copper phthalocyanine (CuPc) molecules on a room temperature Cu(111) surface has been studied using scanning tunneling microscopy (STM). Below 1 ML the molecules are in a fluid state and are highly mobile on the surface. At 1 ML coverage the molecules coalesce into a highly ordered 2D crystal phase. At sub-ML coverages, chemisorption of individual CuPc molecules can be induced through exposure to tunneling electrons at a tunneling bias voltage exceeding a threshold value. This tunneling electron induced effect has been exploited to perform molecular STM lithography.

Graphene nanoribbons with zigzag and armchair edges prepared by scanning tunneling microscope lithography on gold substrates

The properties of graphene nanoribbons are dependent on both the nanoribbon width and the crystallographic orientation of the edges. Scanning tunneling microscope lithography is a method which is able to create graphene nanoribbons with well defined edge orientation, having a width of a few nanometers. However, it has only been demonstrated on the top layer of graphite. In order to allow practical applications of this powerful lithography technique, it needs to be implemented on single layer graphene. We demonstrate the preparation of graphene nanoribbons with well defined crystallographic orientation on top of gold substrates. Our transfer and lithography approach brings one step closer the preparation of well defined graphene nanoribbons on arbitrary substrates for nanoelectronic applications.

Ab initio calculation of valley splitting in monolayer δ-doped phosphorus in silicon.

The differences in energy between electronic bands due to valley splitting are of paramount importance in interpreting transport spectroscopy experiments on state-of-the-art quantum devices defined by scanning tunnelling microscope lithography. Using vasp, we develop a plane-wave density functional theory description of systems which is size limited due to computational tractability. Nonetheless, we provide valuable data for the benchmarking of empirical modelling techniques more capable of extending this discussion to confined disordered systems or actual devices. We then develop a less resource-intensive alternative via localised basis functions in siesta, retaining the physics of the plane-wave description, and extend this model beyond the capability of plane-wave methods to determine the ab initio valley splitting of well-isolated δ-layers. In obtaining an agreement between plane-wave and localised methods, we show that valley splitting has been overestimated in previous ab initio calculations by more than 50%.

Atomistic modeling of metallic nanowires in silicon

Scanning tunneling microscope (STM) lithography has recently demonstrated the ultimate in device scaling with buried, conducting nanowires just a few atoms wide and the realization of single atom transistors, where a single P atom has been placed inside a transistor architecture with atomic precision accuracy. Despite the dimensions of the critical parts of these devices being defined by a small number of P atoms, the device electronic properties are influenced by the surrounding 10(4) to 10(6) Si atoms. Such effects are hard to capture with most modeling approaches, and prior to this work no theory existed that could explore the realistic size of the complete device in which both dopant disorder and placement are important. This work presents a comprehensive study of the electronic and transport properties of ultra-thin (<10 nm wide) monolayer highly P δ-doped Si (Si:P) nanowires in a fully atomistic self-consistent tight-binding approach. This atomistic approach covering large device volumes allows for a systematic study of disorder on the physical properties of the nanowires. Excellent quantitative agreement is observed with recent resistance measurements of STM-patterned nanowires [Weber et al., Science, 2012, 335, 64], confirming the presence of metallic behavior at the scaling limit. At high doping densities the channel resistance is shown to be insensitive to the exact channel dopant placement highlighting their future use as metallic interconnects. This work presents the first theoretical study of Si:P nanowires that are realistically extended and disordered, providing a strong theoretical foundation for the design and understanding of atomic-scale electronics.

New avenues to an old material: controlled nanoscale doping of germanium

We review our recent research into n-type doping of Ge for nanoelectronics and integrated photonics. We demonstrate a doping method in ultra-high vacuum to achieve high electron concentrations in Ge while maintaining atomic-level control of the doping process. We integrated this doping technique with ultra-high vacuum scanning tunneling microscope lithography and femtosecond laser ablation micron-scale lithography, and demonstrated basic components of donor-based nanoelectronic circuitry such as wires and tunnel gaps. By repetition of controlled doping cycles we have shown that stacking of multiple Ge:P two-dimensional electron gases results in high electron densities in Ge (>10(20) cm(-3)). Because of the strong vertical electron confinement, closely stacked 2D layers - although interacting - maintain their individuality in terms of electron transport. These results bode well towards the realization of nanoscale 3D epitaxial circuits in Ge comprising stacked 2DEGs and/or atomic-scale Ge:P devices with confinement in more dimensions.

Nanometer wide ribbons and triangles by STM lithography of graphene

In this article, we present a method, which is suitable for the realization of graphene-based nanostructures by scanning tunneling microscopy lithography. Graphene nanoribbons (GNRs) and other more complicated nanoarchitectures like: GNR networks, triangular quantum-billiards, etc. can be created with controlled shape and crystallographic orientation. The cutting process operates with nanometer accuracy. After the lithography process the same STM tip is suitable for acquiring atomic resolution images on the nanoarchitectures created by STM lithography. The experimental observation of long range electronic superstructures indicates the long phase coherence length in graphene nanostructures even at room temperature.

Electronic structure of realistically extended atomistically resolved disordered Si:Pδ-doped layers

The emergence of scanning tunneling microscope (STM) lithography and low temperature molecular beam epitaxy (MBE) opens the possibility of creating scalable donor based quantum computing architectures. In particular, atomically precise Si:P monolayer structures ($\ensuremath{\delta}$-doped layers) serve as crucial contact regions and in-plane gates in single impurity devices. In this paper we study highly confined $\ensuremath{\delta}$-doped layers to explain the disorder in the P dopant placements in realistically extended systems. The band structure is computed using the tight-binding formalism and charge-potential self-consistency. The exchange-correlation corrected impurity potential pulls down subbands below the silicon valley minima to create impurity bands. Our methodology is benchmarked and validated against other theoretical methods for small ordered systems. The doping density is shown to linearly control the impurity bands. Disorder within the Si:P $\ensuremath{\delta}$-doped layer is examined using an extended domain to describe the effects of experimentally unavoidable randomness through explicitly disordered dopant placement. Disorder in the $\ensuremath{\delta}$-doped layer breaks the symmetry in the supercell and creates band splitting in every subband. Vertical segregation of dopants is shown to dramatically reduce valley splitting (VS). Such VS can be used as a measure of ideality of the fabricated Si:P $\ensuremath{\delta}$-doped layer. Although the resulting disorder induces density of states fluctuations, this theoretical analysis shows that $\ensuremath{\delta}$-doped layers can serve as quasimetallic 2D electron sources even in the presence of strong nonidealities.

Charge Sensing of Precisely Positioned P Donors in Si

Real-time sensing of (spin-dependent) single-electron tunneling is fundamental to electrical readout of qubit states in spin quantum computing. Here, we demonstrate the feasibility of detecting such single-electron tunneling events using an atomically planar charge sensing layout, which can be readily integrated in scalable quantum computing architectures with phosphorus-donor-based spin qubits in silicon (Si:P). Using scanning tunneling microscopy (STM) lithography on a Si(001) surface, we patterned a single-electron transistor (SET), both tunnel and electrostatically coupled to a coplanar ultrasmall quantum dot, the latter consisting of approximately four P donors. Charge transitions of the quantum dot could be detected both in time-averaged and single-shot current response of the SET. Single electron tunneling between the quantum dot and the SET island on a time-scale (τ ∼ ms) two-orders-of-magnitude faster than the spin-lattice relaxation time of a P donor in Si makes this device geometry suitable for projective readout of Si:P spin qubits. Crucial to scalability is the ability to reproducibly achieve sufficient electron tunnel rates and charge sensitivity of the SET. The inherent atomic-scale control of STM lithography bodes extremely well to precisely optimize both of these parameters.

A Complete Fabrication Route for Atomic-Scale, Donor-Based Devices in Single-Crystal Germanium

Despite the rapidly growing interest in Ge for ultrascaled classical transistors and innovative quantum devices, the field of Ge nanoelectronics is still in its infancy. One major hurdle has been electron confinement since fast dopant diffusion occurs when traditional Si CMOS fabrication processes are applied to Ge. We demonstrate a complete fabrication route for atomic-scale, donor-based devices in single-crystal Ge using a combination of scanning tunneling microscope lithography and high-quality crystal growth. The cornerstone of this fabrication process is an innovative lithographic procedure based on direct laser patterning of the semiconductor surface, allowing the gap between atomic-scale STM-patterned structures and the outside world to be bridged. Using this fabrication process, we show electron confinement in a 5 nm wide phosphorus-doped nanowire in single-crystal Ge. At cryogenic temperatures, Ohmic behavior is observed and a low planar resistivity of 8.3 kΩ/□ is measured.