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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

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 towards 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 3 adjacent Si dimers along a dimer row, 2 adjacent dimers, and 1 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 1-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 1-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 one of the primary models for understanding the essential many-body physics in condensed matter systems such as Mott insulators and cuprate high-Tc superconductors. Recent advances in atomically precise fabrication in silicon using scanning tunneling microscopy (STM) have made possible atom-by-atom fabrication of single and few-dopant quantum dots and atomic-scale control of tunneling in dopant-based devices. However, the complex fabrication requirements of multi-component devices have meant that emulating two-dimensional (2D) Fermi-Hubbard physics using these systems has not been demonstrated. Here, we overcome these challenges by integrating the latest developments in atomic fabrication and demonstrate the analog quantum simulation of a 2D extended Fermi-Hubbard Hamiltonian using STM-fabricated 3x3 arrays of single/few-dopant quantum dots. We demonstrate low-temperature quantum transport and tuning of the electron ensemble using in-plane gates as efficient probes to characterize the many-body properties, such as charge addition, tunnel coupling, and the impact of disorder within the array. By controlling the array lattice constants with sub-nm precision, we demonstrate tuning of the hopping amplitude and long-range interactions and observe the finite-size analogue of a transition from Mott insulating to metallic behavior in the array. By increasing the measurement temperature, we simulate the effect of thermally activated hopping and Hubbard band formation in transport spectroscopy. We compare the analog quantum simulations with numerically simulated results to help understand the energy spectrum and resonant tunneling within the array. The results demonstrated in this study serve as a launching point for a new class of engineered artificial lattices to simulate the extended Fermi-Hubbard model of strongly correlated materials.

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.

Advanced hydrogen lithography techniques and low-temperature epitaxial overgrowth enable patterning of highly phosphorus-doped silicon (Si:P) monolayers (ML) with atomic precision. This approach to device fabrication has made Si:P monolayer systems a testbed for multiqubit quantum computing architectures and atomically precise 2-D superlattice designs whose behaviors are directly tied to the deterministic placement of single dopants. However, dopant segregation, diffusion, surface roughening, and defect formation during the encapsulation overgrowth introduce large uncertainties to the exact dopant placement and activation ratio. In this study, we develop a unique method by combining dopant segregation/diffusion models with sputter profiling simulation to monitor and control, at the atomic scale, dopant movement using room-temperature grown locking layers (LL). We explore the impact of LL growth rate, thickness, rapid thermal anneal, surface accumulation, and growth front roughness on dopant confinement, local crystalline quality, and electrical activation within Si:P 2-D systems. We demonstrate that dopant movement can be more efficiently suppressed by increasing the LL growth rate than by increasing LL thickness. We find that the dopant segregation length can be suppressed below a single Si lattice constant by increasing LL growth rates at room temperature while maintaining epitaxy. Although dopant diffusivity within the LL is found to remain high even below the hydrogen desorption temperature, we demonstrate that exceptionally sharp dopant confinement with high electrical quality within Si:P monolayers can be achieved by combining a high LL growth rate with a low-temperature LL rapid thermal anneal.