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Recent advances towards spin-based quantum computation have been primarily fuelled by elaborate isolation from noise sources, such as surrounding nuclear spins and spin-electric susceptibility, to extend spin coherence. In the meanwhile, addressable single-spin and spin-spin manipulations in multiple-qubit systems will necessitate sizable spin-electric coupling. Given background charge fluctuation in nanostructures, however, its compatibility with enhanced coherence should be crucially questioned. Here we realise a single-electron spin qubit with isotopically-enriched phase coherence time (20 microseconds) and fast electrical control speed (up to 30 MHz) mediated by extrinsic spin-electric coupling. Using rapid spin rotations, we reveal that the free-evolution dephasing is caused by charge (instead of conventional magnetic) noise featured by a 1/f spectrum over seven decades of frequency. The qubit nevertheless exhibits superior performance with single-qubit gate fidelities exceeding 99.9% on average. Our work strongly suggests that designing artificial spin-electric coupling with account taken of charge noise is a promising route to large-scale spin-qubit systems having fault-tolerant controllability.

Single-component azobenzene thiol (Me-SH) and two-component azobenzene dodecyl disulfide (Me-SS) have been used to understand how “space” necessary for trans ↔ cis photoisomerization, “intermolecular interactions” and “phase separation” affects the repeated photoswitching ability of azobenzene units on flat gold surfaces. Me-SH self-assembled monolayers (SAMs) with available space and π–π stacking interactions between photoswitchable azobenzene units showed ∼51% of the first trans-to-cis photoisomerization and good photoswitching performance in response to alternating irradiation with UV and visible light. On the other hand, our absorption spectral data and AFM observations suggest that each chemical component of Me-SS did not move continuously on a flat gold surface and was almost fixed after partially phase-separated SAM formation. The first trans-to-cis photoconversion of the Me-SS SAMs with additional free space arising from phase separation reached as high as 75 ± 3%. Repeated irradiation of the Me-SS SAMs with UV and visible light seems to cause (i) out-of-plane (homeotropic and/or oblique) reorientation and/or (ii) random arrangements of mixed trans- and cis-azobenzenes. Consequently, the initial excellent photoswitching ability declined gradually as the number of repeated irradiations increased. The observations indicate that a balance between space, intermolecular interactions, and phase separation plays an important role in forming repeatedly photoswitchable monolayers.