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Applied Physics Letters

Quantifying the number of color centers in single fluorescent nanodiamonds by photon correlation spectroscopy and Monte Carlo simulation

Yuen Yung Hui, Yi-Ren Chang, Tsong‐Shin Lim, Hsu-Yang Lee, Wunshain S. Fann, Huan‐Cheng Chang

Published Jan 5, 2009• 27 citations
Publisher

Abstract

The number of negatively charged nitrogen-vacancy centers (N-V)− in fluorescent nanodiamond (FND) has been determined by photon correlation spectroscopy and Monte Carlo simulations at the single particle level. By taking account of the random dipole orientation of the multiple (N-V)− fluorophores and simulating the probability distribution of their effective numbers (Ne), we found that the actual number (Na) of the fluorophores is in linear correlation with Ne, with correction factors of 1.8 and 1.2 in measurements using linearly and circularly polarized lights, respectively. We determined Na=8±1 for 28 nm FND particles prepared by 3 MeV proton irradiation.

DOI
10.1063/1.3067867

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Measuring the number of (N-V)^− centers in single fluorescent nanodiamonds in the presence of quenching effects

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Quenching effects, including graphite-shell quenching and impurity quenching, on negatively charged nitrogen-vacancy (N-V)− centers in fluorescent nanodiamonds (FNDs) can reduce the fluorescence quantum yield and bring about multiexponential decay fluorescence to FNDs. This causes the number of (N-V)− centers to be underestimated when using the photon correlation method, which presumes identical emitters. This study proposes a method that combines time-resolved spectroscopy and photon correlation spectroscopy to modify the number measurement with the photon correlation method. The average number of (N-V)− centers in 35 nm FNDs was corrected from 7.6 with the unmodified method to 11.96 with the modified method.

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Monitoring Dark-State Dynamics of a Single Nitrogen-Vacancy Center in Nanodiamond by Auto-Correlation Spectroscopy: Photonionization and Recharging

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In this letter, the photon-induced charge conversion dynamics of a single Nitrogen-Vacancy (NV) center in nanodiamond between two charge states, negative (NV−) and neutral (NV0), is studied by the auto-correlation function. It is observed that the ionization of NV− converts to NV0, which is regarded as the dark state of the NV−, leading to fluorescence intermittency in single NV centers. A new method, based on the auto-correlation calculation of the time-course fluorescence intensity from NV centers, was developed to quantify the transition kinetics and yielded the calculation of transition rates from NV− to NV0 (ionization) and from NV0 to NV− (recharging). Based on our experimental investigation, we found that the NV−-NV0 transition is wavelength-dependent, and more frequent transitions were observed when short-wavelength illumination was used. From the analysis of the auto-correlation curve, it is found that the transition time of NV− to NV0 (ionization) is around 0.1 μs, but the transition time of NV0 to NV− (recharging) is around 20 ms. Power-dependent measurements reveal that the ionization rate increases linearly with the laser power, while the recharging rate has a quadratic increase with the laser power. This difference suggests that the ionization in the NV center is a one-photon process, while the recharging of NV0 to NV− is a two-photon process. This work, which offers theoretical and experimental explanations of the emission property of a single NV center, is expected to help the utilization of the NV center for quantum information science, quantum communication, and quantum bioimaging.

Nanomaterials•Apr 10, 2021•3 citations
The number of negatively charged nitrogen-vacancy centers (N-V)− in fluorescent nanodiamond (FND) has been determined by photon correlation spectroscopy and Monte Carlo simulations at the single particle level. By taking account of the random dipole orientation of the multiple (N-V)− fluorophores and simulating the probability distribution of their effective numbers (Ne), we found that the actual number (Na) of the fluorophores is in linear correlation with Ne, with correction factors of 1.8 and 1.2 in measurements using linearly and circularly polarized lights, respectively. We determined Na=8±1 for 28 nm FND particles prepared by 3 MeV proton irradiation.
Quenching effects, including graphite-shell quenching and impurity quenching, on negatively charged nitrogen-vacancy (N-V)− centers in fluorescent nanodiamonds (FNDs) can reduce the fluorescence quantum yield and bring about multiexponential decay fluorescence to FNDs. This causes the number of (N-V)− centers to be underestimated when using the photon correlation method, which presumes identical emitters. This study proposes a method that combines time-resolved spectroscopy and photon correlation spectroscopy to modify the number measurement with the photon correlation method. The average number of (N-V)− centers in 35 nm FNDs was corrected from 7.6 with the unmodified method to 11.96 with the modified method.
Abstract Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV − ) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV − to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV − charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower N s 0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T 1 spin relaxation times of 3.2 ± 0.7 ms and 4.7 ± 1.6 ms, respectively, compared to 0.17 ± 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T 1 spin relaxation properties.
Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV-) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV- to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV- charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower Ns0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T1 spin relaxation times of 3.2 ±\pm± 0.7 ms and 4.7 ±\pm± 1.6 ms, respectively, compared to 0.17 ±\pm± 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T1 spin relaxation properties.
Diamond nanocrystals containing highly photoluminescent color centers are attractive, nonclassical, and near-field light sources. For near-field applications, the size of the nanocrystal is crucial, since it defines the optical resolution. Nitrogen-vacancy (NV) color centers are efficiently created by proton irradiation and annealing of a nanodiamond powder. Using near-field microscopy and photon statistics measurements, we show that nanodiamonds with sizes down to 25 nm can hold a single NV color center with bright and stable photoluminescence.
Abstract We report on the characterization of the angular-dependent emission of single-photon emitters based on single nitrogen-vacancy (NV-) centers in nanodiamond at room temperature. A theoretical model for the calculation of the angular emission patterns of such an NV-center at a dielectric interface will be presented. For the first time, the orientation of the NV-centers in nanodiamond was determined from back focal plane images of NV-centers and by comparison of the theoretical and experimental angular emission pattern. Furthermore, the orientation of the NV-centers was also obtained from measurements of the fluorescence intensity in dependence on the polarization angle of the linearly polarized excitation laser. The results of these measurements are in good agreement. Moreover, the collection efficiency in this setup was calculated to be higher than 80% using the model of the angular emission of the NV-centers.
In this letter, the photon-induced charge conversion dynamics of a single Nitrogen-Vacancy (NV) center in nanodiamond between two charge states, negative (NV−) and neutral (NV0), is studied by the auto-correlation function. It is observed that the ionization of NV− converts to NV0, which is regarded as the dark state of the NV−, leading to fluorescence intermittency in single NV centers. A new method, based on the auto-correlation calculation of the time-course fluorescence intensity from NV centers, was developed to quantify the transition kinetics and yielded the calculation of transition rates from NV− to NV0 (ionization) and from NV0 to NV− (recharging). Based on our experimental investigation, we found that the NV−-NV0 transition is wavelength-dependent, and more frequent transitions were observed when short-wavelength illumination was used. From the analysis of the auto-correlation curve, it is found that the transition time of NV− to NV0 (ionization) is around 0.1 μs, but the transition time of NV0 to NV− (recharging) is around 20 ms. Power-dependent measurements reveal that the ionization rate increases linearly with the laser power, while the recharging rate has a quadratic increase with the laser power. This difference suggests that the ionization in the NV center is a one-photon process, while the recharging of NV0 to NV− is a two-photon process. This work, which offers theoretical and experimental explanations of the emission property of a single NV center, is expected to help the utilization of the NV center for quantum information science, quantum communication, and quantum bioimaging.