Nuclear Electric Resonance for Spatially-Resolved Spin Control via Pulsed Optical Excitation in the UV-Visible Spectrum
arXiv:2501.17575 · doi:10.1103/PhysRevA.108.053110
Abstract
Nuclear electric resonance (NER) spectroscopy is currently experiencing a revival as a tool for nuclear spin-based quantum computing. Compared to magnetic or electric fields, local electron density fluctuations caused by changes in the atomic environment provide a much higher spatial resolution for the addressing of nuclear spins in qubit registers or within a single molecule. In this article, we investigate the possibility of coherent spin control in atoms or molecules via nuclear quadrupole resonance from first principles. An abstract, time-dependent description is provided which entails and reflects on commonly applied approximations. This formalism is then used to propose a new method we refer to as `optical' nuclear electric resonance (ONER). It employs pulsed optical excitations in the UV-visible light spectrum to modulate the electric field gradient at the position of a specific nucleus of interest by periodic changes of the surrounding electron density. Possible realizations and limitations of ONER for atomically resolved spin manipulation are discussed and tested on Be as an atomic benchmark system via electronic structure theory.
Author accepted version of the manuscript published in Phys. Rev. A 108, 053110 (2023). The published version is available at https://doi.org/10.1103/PhysRevA.108.053110
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