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Register a new userSurface-induced charge state conversion of nitrogen-vacancy defects in nanodiamonds
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We present a study of the charge state conversion of single nitrogen-vacancy (NV) defects hosted in nanodiamonds (NDs). We first show that the proportion of negatively-charged NV$^{-}$ defects, with respect to its neutral counterpart NV$^{0}$, decreases with the size of the ND. We then propose a simple model based on a layer of electron traps located at the ND surface which is in good agreement with the recorded statistics. By using thermal oxidation to remove the shell of amorphous carbon around the NDs, we demonstrate a significant increase of the proportion of NV$^{-}$ defects in 10-nm NDs. These results are invaluable for further understanding, control and use of the unique properties of negatively-charged NV defects in diamond
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We introduce a microwave-assisted spectroscopy technique to determine the relative concentrations of nitrogen vacancy (NV) centers in diamond that are negatively-charged (NV${}^-$) and neutrally-charged (NV${}^0$), and present its application to studying spin-dependent ionization in NV ensembles and enhancing NV-magnetometer sensitivity. Our technique is based on selectively modulating the NV${}^-$ fluorescence with a spin-state-resonant microwave drive to isolate, in-situ, the spectral shape of the NV${}^-$ and NV${}^0$ contributions to an NV-ensemble samples fluorescence. As well as serving as a reliable means to characterize charge state ratio, the method can be used as a tool to study spin-dependent ionization in NV ensembles. As an example, we applied the microwave technique to a high-NV-density diamond sample and found evidence for a new spin-dependent ionization pathway, which we present here alongside a rate-equation model of the data. We further show that our method can be used to enhance the contrast of optically-detected magnetic resonance (ODMR) on NV ensembles and may lead to significant sensitivity gains in NV magnetometers dominated by technical noise sources, especially where the NV${}^0$ population is large. With the high-NV-density diamond sample investigated here, we demonstrate up to a 4.8-fold enhancement in ODMR contrast. The techniques presented here may also be applied to other solid-state defects whose fluorescence can be selectively modulated by means of a microwave drive. We demonstrate this utility by applying our method to isolate room-temperature spectral signatures of the V2-type silicon vacancy from an ensemble of V1 and V2 silicon vacancies in 4H silicon carbide.
The photophysics and charge state dynamics of the nitrogen vacancy (NV) center in diamond has been extensively investigated but is still not fully understood. In contrast to previous work, we find that NV$^{0}$ converts to NV$^{-}$ under excitation with low power near-infrared (1064 nm) light, resulting in $increased$ photoluminescence from the NV$^{-}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that NV$^{0}$ converts to NV$^{-}$ via absorption of 1064 nm photons from the valence band of diamond. We report fast quenching and recovery of the photoluminescence from $both$ charge states of the NV center under low power 1064 nm laser excitation, which has not been previously observed. We also find, using optically detected magnetic resonance experiments, that the charge transfer process mediated by the 1064 nm laser is spin-dependent.
We report on sensing stability of nanodiamond (ND) quantum sensors in various pH aqueous buffer solutions for the two detection schemes of quantum decoherence spectroscopy and thermometry. The electron spin properties of single nitrogen-vacancy (NV) centers in 25-nm-sized NDs have been characterized by a spin-measurement compatible perfusion (SMCP) chamber where observing the same individual NDs in different buffer solutions is possible. With this system, we have determined the stability of the NV quantum sensors during the pH change from 4 to 11 as the fluctuations of +- 12% and +- 0.2 MHz for the spin coherence time ($T_2$) and the resonance frequency ($omega_0$) of their mean values, which are comparable to the instrumental error of the measurement system. Here, we discuss the importance of characterizing the sensing stability during pH changes and how the present observations affect ND-based NV quantum sensing.
We show a marked reduction in the emission from nitrogen-vacancy (NV) color centers in single crystal diamond due to exposure of the diamond to hydrogen plasmas ranging from 700{deg}C to 1000{deg}C. Significant fluorescence reduction was observed beneath the exposed surface to at least 80mm depth after ~10 minutes, and did not recover after post-annealing in vacuum for seven hours at 1100{deg}C. We attribute the fluorescence reduction to the formation of NVH centers by the plasma induced diffusion of hydrogen. These results have important implications for the formation of nitrogen-vacancy centers for quantum applications, and inform our understanding of the conversion of nitrogen-vacancy to NVH, whilst also providing the first experimental evidence of long range hydrogen diffusion through intrinsic high-purity diamond material.
Nitrogen-vacancy (NV) centers in diamonds are interesting due to their remarkable characteristics that are well suited to applications in quantum-information processing and magnetic field sensing, as well as representing stable fluorescent sources. Multiple NV centers in nanodiamonds (NDs) are especially useful as biological fluorophores due to their chemical neutrality, brightness and room-temperature photostability. Furthermore, NDs containing multiple NV centers also have potential in high-precision magnetic field and temperature sensing. Coupling NV centers to propagating surface plasmon polariton (SPP) modes gives a base for lab-on-a-chip sensing devices, allows enhanced fluorescence emission and collection which can further enhance the precision of NV-based sensors. Here, we investigate coupling of multiple NV centers in individual NDs to the SPP modes supported by silver surfaces protected by thin dielectric layers and by gold V-grooves (VGs) produced via the self-terminated silicon etching. In the first case, we concentrate on monitoring differences in fluorescence spectra obtained from a source ND, which is illuminated by a pump laser, and from a scattering ND illuminated only by the fluorescence-excited SPP radiation. In the second case, we observe changes in the average NV lifetime when the same ND is characterized outside and inside a VG. Fluorescence emission from the VG terminations is also observed, which confirms the NV coupling to the VG-supported SPP modes.
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