Suitability of nanodiamond NV centers for spontaneous emission control experiments

TL;DR

This study experimentally investigates the emission properties of NV centers in diamond nanocrystals, revealing their insensitivity to local density of states variations and wide quantum efficiency distribution, impacting their use in photonic applications.

Contribution

First calibration of quantum efficiencies of NV centers in nanodiamonds, showing wide distribution and independence from LDOS variations, informing future photonic device integration.

Findings

NV centers in 25 nm nanocrystals are insensitive to LDOS changes.

Quantum efficiencies in nanocrystals range widely from 0% to 20%.

Decays in 100 nm nanocrystals can be reversibly controlled by a scanning mirror.

Abstract

NV centers in diamond are generally recognized as highly promising as indefinitely stable highly efficient single-photon sources. We report an experimental quantification of the brightness, radiative decay rate, nonradiative decay rate and quantum efficiency of single NV centers in diamond nanocrystals. Our experiments show that the commonly observed large spread in fluorescence decay rates of NV centers in nanodiamond is inconsistent with the common explanation of large nanophotonic mode-density variations in the ultra-small high-index crystals at near-unity quantum efficiency. We report that NV centers in 25 nm nanocrystals are essentially insensitive to local density of states (LDOS) variations that we induce at a dielectric interface by using liquids to vary the refractive index, and propose that quantum efficiencies in such nanocrystals are widely distributed between 0% and 20%. For single NV centers in larger 100 nm nanocrystals, we show that decay rate changes can be reversibly induced by nanomechanically approaching a mirror to change the LDOS. Using this scanning mirror method, for the first time we report calibrated quantum efficiencies of NV centers, and show that different but nominally identical nanocrystals have widely distributed quantum efficiencies between 10% and 90%. Our measurements imply that nanocrystals that are to be assembled into hybrid photonic structures for cavity QED should first be individually screened to assess fluorescence properties in detail.