Fabrication of quantum devices by atomic-scale patterning with scanning tunneling microscopy (STM) has led to the development of single/few atom transistors, few-donor/quantum dot devices for spin manipulation, and arrayed few-donor devices for analog quantum simulation. We have developed atomic precision lithography, dopant incorporation, device encapsulation, ex situ device re-location, and contact processes to enable high-yield device fabrication. In this work, we describe a multiscale alignment strategy using Kelvin probe force microscopy to enable the alignment of buried device components to electronic support structures such as source/drain leads, in-plane and top gates, and waveguides while preserving flexibility in the placement of fabricated STM patterns. The required spatial accuracy to bridge the sub-micrometer scale central region of the device to millimeter scale large wire-bond pads is achieved through a multi-step alignment process at various stages of fabrication, including atom-scale device fabrication using STM, re-location and registration, and electron beam lithography for contact leads and pads. This alignment strategy allows imaging small device regions as well as large-scale fiducial marks, thereby bridging the gap from nanometer STM patterns to the millimeter-scale electrical contact fabrication with a 95% yield on more than 150 devices fabricated to date.

Coherent manipulation of electron spins is one of the central challenges of silicon-based quantum computing efforts. Electron spin resonance (ESR) lines, or Oersted lines, allow 10-60 GHz radio frequency (RF) pulses to induce an electromagnetic field that drives Rabi oscillations in a quantum dot interface. The frequency of these Rabi oscillations is directly proportional to the strength of the induced electromagnetic field. We outline a methodology for the design of a printed circuit board and an ESR line that is able to transmit an RF pulse in the 40 GHz regime and induce an oscillating magnetic field onto a qubit device. We propose and implement a novel design by coupling a second symmetrical Oersted line in the opposing direction of the first to act as an antenna for the purpose of monitoring power and magnetic field strength at the embedded device interface.

The doping of Si using the scanning probe hydrogen depassivation lithography technique has been shown to enable placing and positioning small numbers of P atoms with nanometer accuracy. Several groups have now used this capability to build devices that exhibit desired quantum behavior determined by their atomistic details. What remains elusive, however, is the ability to control the precise number of atoms placed at a chosen site with 100% yield, thereby limiting the complexity and degree of perfection achievable. As an important step toward precise control of dopant number, we explore the adsorption of the P precursor molecule, phosphine, into atomically perfect dangling bond patches of intentionally varied size consisting of three adjacent Si dimers along a dimer row, two adjacent dimers, and one single dimer. Using low temperature scanning tunneling microscopy, we identify the adsorption products by generating and comparing to a catalog of simulated images, explore atomic manipulation after adsorption in select cases, and follow up with incorporation of P into the substrate. For one-dimer patches, we demonstrate that manipulation of the adsorbed species leads to single P incorporation in 12 out of 12 attempts. Based on the observations made in this study, we propose this one-dimer patch method as a robust approach that can be used to fabricate devices where it is ensured that each site of interest has exactly one P atom.

The Hubbard model is an essential tool for understanding many-body physics in condensed matter systems. Artificial lattices of dopants in silicon are a promising method for the analog quantum simulation of extended Fermi-Hubbard Hamiltonians in the strong interaction regime. However, complex atom-based device fabrication requirements have meant emulating a tunable two-dimensional Fermi-Hubbard Hamiltonian in silicon has not been achieved. Here, we fabricate 3 × 3 arrays of single/few-dopant quantum dots with finite disorder and demonstrate tuning of the electron ensemble using gates and probe the many-body states using quantum transport measurements. By controlling the lattice constants, we tune the hopping amplitude and long-range interactions and observe the finite-size analogue of a transition from metallic to Mott insulating behavior. We simulate thermally activated hopping and Hubbard band formation using increased temperatures. As atomically precise fabrication continues to improve, these results enable a new class of engineered artificial lattices to simulate interactive fermionic models.

NIST is using atomically precise fabrication to develop electronic devices for use in quantum information processing and novel quantum materials. We are using hydrogen-based scanning probe lithography to enable deterministic placement of individual dopant atoms with atomically aligned contacts and gates to fabricate single atom transistors, devices for single electron spin manipulation, and arrayed devices for analog quantum simulation research. Atomic precision devices, where individual atoms or electrons fundamentally affect device performance, bring about a variety of new manufacturing and metrology challenges. Single atom defects and charge instability deeply change device performance, affecting reliable manipulation and sensing of individual electrons. Conventional metrology methods such as transmission electron and scanning electron microscopy often prove inadequate at this length scale and new, challenging electrical test methods are needed.

Scientists have long studied the physics of highly disordered conducting systems, seeking to understand the multitude of quantum phenomena that govern how electrons move through material systems. Recently, research into silicon-based quantum computing has made disordered conducting systems, such as Si:P monolayers embedded in isotopically pure Si, technically relevant. Consequently, applying and advancing the theoretical frameworks developed to describe electron behavior in disordered systems is a necessary objective in this field of research. This study investigates key components of dopant-based Si quantum computing devices: embedded regions of highly doped delta layers (delta layers). We examine the transport behavior and the electron-electron interaction (EEI) physics in embedded Si:P delta layers by means of self-consistent magnetotransport measurements. Parameters associated with the electronic transport offer a meaningful quantitative characterization of delta-layer quality and dopant diffusion. In addition, by examining EEI behaviors in a set of samples with embedded Si:P delta layers produced with different PH3 exposure procedures prior to Si encapsulation, we show how details of material synthesis affect the dimensionality of charge carrier interactions in embedded Si:P delta layers. The relationship between delta-layer confinement and EEI screening lengths is established here. This understanding will help validate important models used for device simulation and design and lead to improvements in the control of electrostatic gating of and tunneling transport through Si:P single atom transistors.

The transfer of charge carriers across the optically excited hetero-interface of graphene and semiconducting transition metal dichalcogenides (TMDCs) is the key to convert light to electricity, although the intermediate steps from the creation of excitons in TMDC to the collection of free carriers in the graphene layer are not fully understood. Here, we investigate photo-induced charge transport across graphene–MoS2 and graphene–WSe2 hetero-interfaces using time-dependent photoresistance relaxation with varying temperature, wavelength, and gate voltage. In both types of heterostructures, we observe an unprecedented resonance in the inter-layer charge transfer rate as the Fermi energy (EF) of the graphene layer is tuned externally with a global back gate. We attribute this to a resonant quantum tunneling from the excitonic state of the TMDC to EF of the graphene layer and outline a new method to estimate the excitonic binding energies (Eb) in the TMDCs, which are found to be 400 meV and 460 meV in MoS2 and WSe2 layers, respectively. The gate tunability of the inter-layer charge transfer timescales may allow precise engineering and readout of the optically excited electronic states at graphene–TMDC interfaces.

Atomically precise donor-based quantum devices are a promising candidate for solid-state quantum computing and analog quantum simulations. However, critical challenges in atomically precise fabrication have meant systematic, atomic scale control of the tunneling rates and tunnel coupling has not been demonstrated. Here using a room temperature grown locking layer and precise control over the entire fabrication process, we reduce unintentional dopant movement while achieving high quality epitaxy in scanning tunnelling microscope (STM)-patterned devices. Using the Si(100)2 × 1 surface reconstruction as an atomically-precise ruler to characterize the tunnel gap in precision-patterned single electron transistors, we demonstrate the exponential scaling of the tunneling resistance on the tunnel gap as it is varied from 7 dimer rows to 16 dimer rows. We demonstrate the capability to reproducibly pattern devices with atomic precision and a donor-based fabrication process where atomic scale changes in the patterned tunnel gap result in the expected changes in the tunneling rates.

Atomically precise fabrication has an important role to play in developing atom‐based electronic devices for use in quantum information processing, quantum materials research, and quantum sensing. Atom‐by‐atom fabrication has the potential to enable precise control over tunnel coupling, exchange coupling, on‐site charging energies, and other key properties of basic devices needed for solid‐state quantum computing and analog quantum simulation. Using hydrogen‐based scanning probe lithography, individual dopant atoms are deterministically placed relative to atomically aligned contacts and gates to build single electron transistors, single atom transistors, and gate‐controlled quantum sensing devices. The key steps required to fabricate and demonstrate the essential building blocks needed for spin selective initialization/readout and coherent quantum manipulation are described.

Scanning tunneling microscopy (STM) enables the fabrication of two-dimensional δ-doped structures in Si with atomistic precision, with applications from tunnel field-effect transistors to qubits. The combination of a very small contact area and the restrictive thermal budget necessary to maintain the integrity of the δ layer make developing a robust electrical contact method a significant challenge to realizing the potential of atomically precise devices. We demonstrate a method for electrical contact using Pd2Si formed at the temperature of silicon overgrowth (250 °C), minimizing the diffusive impact on the δ layer. We use the transfer length method to show our Pd2Si contacts have very high yield (99.7% +0.2% -1.5%) and low resistivity (272±41Ωμm) in contacting mesa-etched Si:P δ layers. We also present three terminal measurements of low contact resistance (<1 kΩ) to devices written by STM hydrogen depassivation lithography with similarly high yield (100% +0% -3.2%).

Atomically precise donor-based quantum devices are a promising candidate for scalable solid-state quantum computing. Atomically precise design and implementation of the tunnel coupling in these devices is essential to realize gate-tunable exchange coupling, and electron spin initialization and readout. Current efforts in atomically precise lithography have enabled deterministic placement of single dopant atoms into the Si lattice with sub-nm precision. However, critical challenges in atomically precise fabrication have meant systematic, atomic-scale control of the tunneling coupling has not been demonstrated. Here using a room-temperature grown locking layer and precise control over the entire atomic-scale fabrication process, we demonstrate atomic-scale control of the tunnel coupling in atomically precise single-electron transistors (SETs). Using the naturally occurring Si (100) 2x1 surface reconstruction lattice as an atomically-precise ruler, we systematically vary the number of lattice counts within the tunnel junction gaps and demonstrate exponential scaling of the tunneling resistance at the atomic limit. Using low-temperature transport measurements, we characterize the tunnel coupling asymmetry in a pair of nominally identical tunnel gaps that results from atomic-scale variation in the tunnel junction and show a resistance difference of four that corresponds to half a dimer row pitch difference in the effective tunnel gap distances - the intrinsic limit of hydrogen lithography precision on Si (100) 2x1 surfaces. Our results demonstrate the key capability to do atom-scale design and engineering of the tunnel coupling necessary for solid-state quantum computing and analog quantum simulation.

Hydrogen atoms on a silicon surface, H-Si (100), behave as a resist that can be patterned with perfect atomic precision using a scanning tunneling microscope. When a hydrogen atom is removed in this manner, the underlying silicon presents a chemically active site, commonly referred to as a dangling bond. It has been predicted that individual dangling bonds function as artificial atoms, which, if grouped together, can form designer molecules on the H-Si (100) surface. Here, we present an artificial ring structure molecule spanning three dimer rows, constructed from dangling bonds, and verified by spectroscopic measurement of its molecular orbitals. We found that removing 8 hydrogen atoms resulted in a molecular analog to 1,4-disilylene-hexasilabenzene (Si8H8). Scanning tunneling spectroscopic measurements reveal molecular π and π* orbitals that agree with those expected for the same molecule in a vacuum; this is validated by density functional theory calculations of the dangling bond system on a silicon slab that show direct links both to the experimental results and to calculations for the isolated molecule. We believe the unique electronic structure of artificial molecules constructed in this manner can be engineered to enable future molecule-based electronics, surface catalytic functionality, and templating for subsequent site-selective deposition.

Van der Waals hybrids of graphene and transition metal dichalcogenides exhibit an extremely large response to optical excitation, yet counting of photons with single‐photon resolution is not achieved. Here, a dual‐gated bilayer graphene (BLG) and molybdenum disulphide (MoS 2 ) hybrid are demonstrated, where opening a band gap in the BLG allows extremely low channel (receiver) noise and large optical gain (≈10 10 ) simultaneously. The resulting device is capable of unambiguous determination of the Poissonian emission statistics of an optical source with single‐photon resolution at an operating temperature of 80 K, dark count rate 0.07 Hz, and linear dynamic range of ≈40 dB. Single‐shot number‐resolved single‐photon detection with van der Waals heterostructures may impact multiple technologies, including the linear optical quantum computation.