NV- - N+ pair centre in 1b diamond

TL;DR

This paper investigates how nitrogen concentration and optical excitation influence the spin polarization and charge dynamics of NV$^-$ centers in 1b diamond, revealing the impact of NV$^-$ - N$^+$ pair separation on their properties.

Contribution

It provides a detailed spectroscopic analysis linking NV$^-$ center behavior to nitrogen concentration and excitation wavelength, highlighting charge tunneling effects and their influence on spin polarization.

Findings

Spin polarization decreases with decreasing NV$^-$ - N$^+$ separation.

Charge tunneling affects emission, lifetime, and spin coherence times.

Optical excitation modifies charge dynamics and induces Stark shifts.

Abstract

The study establishes that the degree of optically induced spin polarization that can be achieved for NV$^- $in 1b diamond is limited by the concentration of single substitutional nitrogen, N$^0$ . The polarization of the individual NV centres in the diamond is dependent on the separation of the NV$^-$ and the nitrogen donor. When the NV$^-$ - N$^+$ pair separation is large the properties of the pair will be as for single sites and a high degree of spin polarization attainable. When the separation decreases the emission is reduced, the lifetime shortened and the spin polarization downgraded. The deterioration occurs as a consequence of electron tunneling in the excited state from NV$^-$ to N$^+$ and results in an optical cycle that includes NV$^0$. The tunneling process is linear in optical excitation and more prevalent the closer the N$^+$ is to the NV$^-$ centre. However, the separation between the NV$^-$ and its donor N$^+$ can be effected by light through the excitation of NV$^-$ and/or ionization of N$^0$. The optical excitation that creates the spin polarization can also modify the sample properties and during excitation creates charge dynamics. The consequence is that the magnitude of spin polarization, the spin relaxation and coherence times T$_1$ and T$_2$ have a dependence on the nitrogen concentration and on the excitation wavelength. The adjacent N$^+$ gives an electric field that Stark shifts the NV$^-$ transitions and for an ensemble results in line broadening. It is observation of changes of these Stark induced effects that allow the variation in NV$^-$ - N$^+$ separation to be monitored. Spectroscopic measurements including that of the varying line widths are central to the study. They are made at low temperatures and include extensive measurements of the NV$^-$ optical transition at 637 nm, the infrared transition at 1042 nm and ODMR at 2.87 GHz.