Designing Optically Addressable Nitrogen-Vacancy Centers in Ultra-Small Nanodiamonds: Insights from First-Principles Calculations

TL;DR

This study uses first-principles calculations to explore how surface termination affects the optical and charge stability of nitrogen-vacancy centers in ultrasmall nanodiamonds, with implications for quantum sensing and bio-labeling.

Contribution

It provides new insights into stabilizing NV- centers in USNDs through surface chemistry and array configurations, combining electronic structure and vibronic effects.

Findings

Fluorine, hydroxyl, and ether terminations stabilize NV- in USNDs.

Hydroxyl and ether are advantageous for quantum sensing.

Array configurations with larger inter-particle separations enhance charge stability.

Abstract

Ultrasmall nanodiamonds (USNDs) are promising platforms for fluorescent and quantum sensing applications. Here we present first-principles electronic structure calculations of color centers in USNDs, specifically the nitrogen-vacancy (NV-) and we investigate their optical addressability as a function of the surface termination. We consider both isolated nanoparticles and arrays of USNDs with different degrees of packing, and we include quantum vibronic effects in our analysis, using stochastic methods. We find that the NV in USNDs can be stabilized in a negative charge state if the nanoparticles are terminated by fluorine, hydroxyl, and ether. While fluorine terminations can be used for fluorescent bio-tags, we suggest that hydroxyl and ether terminations are beneficial for quantum sensing applications. We also find that the NV- can be stabilized in arrays of USNDs when inter-particle separations are larger than the diameter of the nanoparticle. Interestingly, the phonon renormalizations of single-particle energy levels found in arrays contribute to the charge stability of negatively charged NV centers.