Isotopic enrichment of silicon by high fluence 28 Si − ion implantation

Spins in the ``semiconductor vacuum'' of silicon-28 ($^{28}\mathrm{Si}$) are suitable qubit candidates due to their long coherence times. An isotopically purified substrate or epilayer of $^{28}\mathrm{Si}$ is required to limit the decoherence pathway caused by magnetic perturbations from surrounding $^{29}\mathrm{Si}$ nuclear spins ($I=1/2$), present in natural Si ($^{\text{nat}}\mathrm{Si}$) at an abundance of 4.67%. We isotopically enrich surface layers of $^{\text{nat}}\mathrm{Si}$ by sputtering using high fluence ${}^{28}{\text{Si}}^{\ensuremath{-}}$ implantation. Phosphorus (P) donors implanted into one such $^{28}\mathrm{Si}$ layer with $\ensuremath{\sim}3000$ ppm $^{29}\mathrm{Si}$, produced by implanting 30 keV ${}^{28}{\text{Si}}^{\ensuremath{-}}$ ions at a fluence of $4\ifmmode\times\else\texttimes\fi{}{10}^{18}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$, were measured with pulsed electron spin resonance, confirming successful donor activation upon annealing. The monoexponential decay of the Hahn echo signal indicates a depletion of $^{29}\mathrm{Si}$. A coherence time of ${T}_{2}=285\ifmmode\pm\else\textpm\fi{}14\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{s}$ is extracted, which is longer than that obtained in ${}^{\text{nat}}\text{Si}$ for similar doping concentrations and can be increased by reducing the P concentration in the future. Guided by simulations, the isotopic enrichment was improved by employing one-for-one ion sputtering using 45 keV ${}^{28}{\text{Si}}^{\ensuremath{-}}$ implanted with a fluence of $2.63\ifmmode\times\else\texttimes\fi{}{10}^{18}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$ into ${}^{\text{nat}}\text{Si}$. This resulted in an isotopically enriched surface layer $\ensuremath{\sim}100$ nm thick, suitable for providing a sufficient volume of $^{28}\mathrm{Si}$ for donor qubits implanted into the near-surface region. We observe a depletion of $^{29}\mathrm{Si}$ to 250 ppm as measured by secondary ion mass spectrometry. The impurity content and the crystallization kinetics via solid phase epitaxy are discussed. The $^{28}\mathrm{Si}$ layer is confirmed to be a single crystal using transmission electron microscopy. This method of Si isotopic enrichment shows promise for incorporation into the fabrication process flow of Si spin-qubit devices.