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Journal of the Optical Society of America B

Fluorescence modulation of the nitrogen-vacancy center with competition between charge-state conversion and stimulated emission

Bo Du, Xiang-Dong Chen, Shao-Chun Zhang, Yang Dong, Cuihong Li, Guang‐Can Guo, Fang‐Wen Sun

Published Mar 26, 2020• 9 citations
Publisher

Abstract

The nitrogen-vacancy (NV) center in diamond has been widely used for quantum information processing, nanophotonics, and biological imaging. In this work, we experimentally studied the charge-state conversion and stimulated emission of the NV center with a near-infrared (NIR) pumping laser. The competition between these two processes resulted in a nonmonotonic dependence of the NV center’s fluorescence intensity on the NIR laser power. Fluorescence enhancement was observed with a weak NIR laser, while fluorescence depletion was observed with a high-power NIR laser. It led to the nonmonotonic change of the spatial resolution with stimulated emission depletion microscopy, which has been used for subdiffraction imaging of the NV center. Our work can help to further understand the optical mechanism and extend the applications of the NV center.

DOI
10.1364/josab.390157

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The nitrogen-vacancy (NV) center in diamond has been widely used for quantum information processing, nanophotonics, and biological imaging. In this work, we experimentally studied the charge-state conversion and stimulated emission of the NV center with a near-infrared (NIR) pumping laser. The competition between these two processes resulted in a nonmonotonic dependence of the NV center’s fluorescence intensity on the NIR laser power. Fluorescence enhancement was observed with a weak NIR laser, while fluorescence depletion was observed with a high-power NIR laser. It led to the nonmonotonic change of the spatial resolution with stimulated emission depletion microscopy, which has been used for subdiffraction imaging of the NV center. Our work can help to further understand the optical mechanism and extend the applications of the NV center.
As a potential candidate for quantum computation and metrology, the nitrogen vacancy (NV) center in diamond presents both challenges and opportunities resulting from charge-state conversion. By utilizing different lasers for the photon-induced charge-state conversion, we achieved subdiffraction charge-state manipulation. The charge-state depletion (CSD) microscopy resolution was improved to 4.1 nm by optimizing the laser pulse sequences. Subsequently, the electron spin-state dynamics of adjacent NV centers were selectively detected via the CSD. The experimental results demonstrated that the CSD can improve the spatial resolution of the measurement of NV centers for nanoscale sensing and quantum information. The nitrogen vacancy (NV) in diamond is useful for quantum optics and spintronics due to the long coherence time of its electron spin state. Scientists in China have now used the techniques of super-resolution microscopy to optically control the charge state of an NV defect with a subdiffraction spatial resolution of 4.1 nm. Xiangdong Chen and co-workers from the University of Science and Technology of China in Hefei used a green (532 nm) laser beam to switch the charge state of the defect between NV0 and NV–. They achieved this manipulation on a subdiffraction scale by using specially shaped doughnut laser beams, in common with the principles of super-resolution stimulated emission depletion microscopy. This achievement represents a significant step towards nanoscale sensing and quantum information processing.
Charged nitrogen-vacancy (NV) color centers in diamond are excellent luminescence sources for far-field fluorescence nanoscopy by stimulated emission depletion (STED). Here we show that these photostable color centers can be visualized by STED using simple continuous-wave or high repetition pulsed lasers (76 MHz) at wavelengths >700 nm for STED. Furthermore, we show that NV centers can be imaged in three dimensions (3D) inside the diamond crystal and present single-photon signatures of single color centers recorded in high density samples, demonstrating a new recording scheme for STED and related far-field nanoscopy approaches. Finally, we exemplify the potential of using nanodiamonds containing NV centers as luminescence tags in STED microscopy. Our results offer new experimental avenues in nanooptics, nanotechnology, and the life sciences.
The charge-state dynamics of the nitrogen-vacancy (NV) center in diamond play a key role in a wide range of applications, yet remain imperfectly understood. Using single picosecond pulses and pulse pairs, we quantitatively investigate the charge dynamics associated with excitation and fluorescence depletion of a single NV center. Our pulsed excitation approach permits significant modeling simplifications and allows us to extract relative rates of excitation, stimulated emission, ionization, and recombination under 531 and 766 nm illumination. By varying the duration between paired pulses, we can also investigate ionization and recombination out of metastable states. Our results are directly applicable to experiments employing stimulated emission-depletion imaging and can be used to predict optimal operating regimes where excitation and stimulated emission are maximized relative to charge-state-switching processes.
The nitrogen-vacancy (NV) center in nanodiamonds has emerged as an excellent platform in quantum technologies due to its applications in spin manipulation and nanoscale sensing. However, their use is limited by the unavoidable charge-state conversion under optical pumping. In this study, we investigate the control of charge-state conversion in NV centers using an engineered photonic environment and thus change the available local density of optical states (LDOS). The spectral- and pump-dependent decay rate measurements are performed to study the redistribution of emission rates due to the change in LDOS and their effect on charge-state conversion. We have achieved an 8% enhancement of emission rate at the zero phonon line which is accompanied with a 10% suppression in the phonon sideband emission rate in the low-pump-power regime. In the high-pump-power regime, the charge-state conversion becomes inevitable and leads to the deterioration of LDOS-induced modification in the NV center emission lifetimes. The results are useful for efficient NV center spin readout and charge-state depletion microscopy utilizing reversible charge-state conversion.
The spatial resolution and fluorescence signal amplitude in stimulated emission depletion (STED) microscopy is limited by the photostability of available fluorophores. Here, we show that negatively-charged silicon vacancy (SiV) centers in diamond are promising fluorophores for STED microscopy, owing to their photostable, near-infrared emission and favorable photophysical properties. A home-built pulsed STED microscope was used to image shallow implanted SiV centers in bulk diamond at room temperature. The SiV stimulated emission cross section for 765-800 nm light is found to be (4.0 ± 0.3)×10^−17 cm^2, which is approximately 2-4 times larger than that of the negatively-charged diamond nitrogen vacancy center and approaches that of commonly-used organic dye molecules. We performed STED microscopy on isolated SiV centers and observed a lateral full-width-at-half- maximum spot size of 89 ± 2 nm, limited by the low available STED laser pulse energy (0.4 nJ). For a pulse energy of 5 nJ, the resolution is expected to be ∼20 nm. We show that the present microscope can resolve SiV centers separated by �� < 150 nm that cannot be resolved by confocal microscopy.
The spatial resolution and fluorescence signal amplitude in stimulated emission depletion (STED) microscopy is limited by the photostability of available fluorophores. Here, we show that negatively charged silicon vacancy (SiV) centers in diamond are promising fluorophores for STED microscopy, owing to their photostable, near-infrared emission and favorable photophysical properties. A home-built pulsed STED microscope was used to image shallow implanted SiV centers in bulk diamond at room temperature. The SiV stimulated emission cross section for 765–800 nm light is found to be (4.0 ± 0.3) × 10 –17 cm 2, which is approximately 2–4 times larger than that of the negatively charged diamond nitrogen vacancy center and approaches that of commonly used organic dye molecules. We performed STED microscopy on isolated SiV centers and observed a lateral full-width-at-half-maximum spot size of 89 ± 2 nm, limited by the low available STED laser pulse energy (0.4 nJ). For a pulse energy of 5 nJ, the resolution is expected to be ∼20 nm. We show that the present microscope can resolve SiV centers separated by ≲150 nm that cannot be resolved by confocal microscopy.