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The nitrogen-vacancy (NV) centre in diamond is a promising candidate for a solid-state qubit. However, its charge state is known to be unstable, discharging from the qubit state NV(-) into the neutral state NV(0) under various circumstances. Here we demonstrate that the charge state can be controlled by an electrolytic gate electrode. This way, single centres can be switched from an unknown non-fluorescent state into the neutral charge state NV(0), and the population of an ensemble of centres can be shifted from NV(0) to NV(-). Numerical simulations confirm the manipulation of the charge state to be induced by the gate-controlled shift of the Fermi level at the diamond surface. This result opens the way to a dynamic control of transitions between charge states and to explore hitherto inaccessible states, such as NV(+).

The hydrophobic interaction of surfaces with water is a well-known phenomenon, but experimental evidence of its influence on biosensor devices has been lacking. In this work we investigate diamond field-effect devices, reporting on Hall effect experiments and complementary simulations of the interfacial potential at the hydrogen-terminated diamond/aqueous electrolyte interface. The interfacial capacitance, derived from the gate-dependent Hall carrier concentration, can be modeled only when considering the hydrophobic nature of this surface and its influence on the structure of interfacial water. Our work demonstrates how profoundly the performance of potentiometric biosensor devices can be affected by their surfaces' hydrophobicity.

We investigate the origin of the surface conductivity of H-terminated diamond films immersed in aqueous electrolyte. We demonstrate that in contrast to the in air situation, charge transfer across the diamond interface does not govern the surface conductivity in aqueous electrolyte when a gate electrode controls the diamond/electrolyte interfacial potential. Instead, this almost ideally polarizable interface allows the capacitive charging of the surface. This description resolves the observed disagreement of the pH sensitivity of the diamond surface conductivity in air and in aqueous electrolyte.