Quantifying the Variation in the Number of Donors in Quantum Dots Created Using Atomic Precision Advanced Manufacturing

• Published in: Journal of physical chemistry. C 2023-03, Vol.127 (12), p.6071-6079
• Main Authors: Campbell, Quinn T., Koepke, Justine C., Ivie, Jeffrey A., Mounce, Andrew M., Ward, Daniel R., Carroll, Malcolm S., Misra, Shashank, Baczewski, Andrew D., Bussmann, Ezra
• Format: Article
• Language: English
• Subjects: C: Physical Properties of Materials and Interfaces; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; kinetic modeling; mathematical methods; oligomers; scanning tunneling microscopy; silicon
• ISSN: 1932-7447; 1932-7455
• DOI: 10.1021/acs.jpcc.3c00479

Atomic-precision advanced manufacturing enables unique silicon quantum electronics built on quantum dots fabricated from small numbers of phosphorus dopants. The number of dopant atoms comprising a dot plays a central role in determining the behavior of charge and spin confined to the dots and thus overall device performance. In this work, we use both theoretical and experimental techniques to explore the combined impact of lithographic variation and stochastic kinetics on the number of P incorporations in quantum dots made using these techniques and how this variation changes as a function of the size of the dot. Using a kinetic model of PH3 dissociation augmented with novel reaction barriers, we demonstrate that for a 2 × 3 silicon dimer window the probability that no donor incorporates goes to zero, allowing for certainty in the placement of at least one donor. However, this still comes with some uncertainty in the precise number of incorporated donors (either one or two), and this variability may still impact certain applications. We also examine the impact of the size of the initial lithographic window, finding that the incorporation fraction saturates to δ-layer-like coverage as the circumference-to-area ratio decreases. We predict that this incorporation fraction depends strongly on the dosage of the precursor and that the standard deviation of the number of incorporations scales as ∼√n, as would be expected for a sequence of largely independent incorporation events. Finally, we characterize an array of 36 experimentally prepared multidonor 3 × 3 nm lithographic windows with scanning tunneling microscopy, measuring the fidelity of the lithography to the desired array and the final location of PH x fragments within these lithographic windows. We use our kinetic model to examine the expected variability due to the observed lithographic error, predicting a negligible impact on incorporation statistics. We find good agreement between our model and the inferred incorporation locations in these windows from scanning tunneling microscope measurements.