Understanding Surface-Induced Decoherence of NV Centers in Diamond

TL;DR

This study uses atomistic modeling and decoherence calculations to understand how surface properties of diamond affect the coherence times of NV centers, providing guidelines for surface engineering to improve quantum sensor performance.

Contribution

It introduces a detailed atomistic and decoherence modeling approach to quantify surface effects on NV center coherence, emphasizing the role of surface spin hopping and orientation.

Findings

Surface orientation and functionalization significantly influence NV coherence times.

A crossover depth exists where surface noise effects diminish, restoring bulk-like coherence.

Surface spin hopping is crucial for accurately modeling NV decoherence behavior.

Abstract

Nitrogen vacancy centers (NV) in proximity to diamond surfaces are promising nanoscale quantum sensors. However, their coherence properties are negatively affected by magnetic and electric surface noise, whose origin and detailed impact have remained elusive. Using atomistic models of diamond surfaces derived with density functional theory, together with decoherence time calculations with cluster correlation expansion methods, we quantify the effects of surface crystallographic orientation and functionalization, and of the density of unpaired electrons on the NV Hahn-echo time $T_2$. We determine a crossover depth at which $T_2$ ceases to be limited by surface nuclear spins and recovers the bulk-limited value. We find that for static surface-electron baths, the ratio between the NV depth and the separation between surface electron spins determines a transition from fast-fluctuating to quasi-static noise, leading to a dependence of $T_2$ on orientation for specific surfaces. We also find that the modulation of $T_2$ by spin-phonon relaxations leads to motional-narrowing at sub-microsecond relaxation times. Importantly, our calculations show that it is only when accounting for surface-spin in-sequence hopping that measured $T_2$ values as a function of depth can be reproduced, thus highlighting the importance of hopping-mediated models to describe the surface spin noise affecting NV sensors. Overall, our work provides clear guidelines for engineering diamond surfaces to achieve enhanced NV coherence for quantum sensing and information processing applications.