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arXiv:1410.4668 · Light Science & Applications

Subdiffraction optical manipulation of the charge state of nitrogen vacancy center in diamond

Xiang-Dong Chen, Chang‐Ling Zou, Zhao-Jun Gong, Chun‐Hua Dong, Guang‐Can Guo, Fang‐Wen Sun

Published Jan 2, 2015• 128 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/lsa.2015.3

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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.
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.
Two-photon charge state conversion has been utilized to improve the spatial resolution of the sensing and imaging with the nitrogen vacancy (NV) center in diamonds. Here, we studied the charge state conversion of the NV center under picosecond pulsed laser excitation. With the same average power, the charge state conversion rate can be improved approximately 24 times by reducing the repetition rate of the laser pulse from 80 to 1 MHz. Subsequently, a pulsed laser with a low repetition rate was applied for the super-resolution charge state depletion microscopy of the NV center. The average power of the depletion laser was reduced approximately 5 times. It can decrease the optical heating, which affects the accuracy and sensitivity of sensing. With the assistance of an additional near-infrared laser, a resolution of 12 nm was obtained with 1 mW depletion laser power. Combined with spin manipulation, we expect our results can be used for the development of a diffraction-unlimited NV center sensing.
The conversion between two nitrogen vacancy (NV) center charge states (NV0 and NV−) was experimentally studied with laser in the range from 378 to 492 nm. The wavelength and power dependent charge state conversion was proved to be single-photon process at short wavelength and two-photon process at long wavelength. Also, the presence of metastable state in NV− significantly affected the conversion process, which can be used to increase NV− population from 72.5% to 80.5% by applying a magnetic field under 532 nm excitation. The method can be used for improving the fidelity of charge state polarization and subsequently optimizing the quantum control with NV center and resolution in the magnetometric and biological sensoring.
Wide-field quantum sensing and imaging with solid-state spins has attracted wide interest for its ability to detect relative physical quantities with high sensitivity at nanoscale. However, the optical diffraction limit hinders the improvement in spatial resolution. In this work, we utilize blind structured illumination microscopy to perform wide-field quantum sensing with nitrogen-vacancy (NV) center in diamond. Without the requirement of prior knowledge of excitation light field, the spatial resolution of NV centers imaging is enhanced by 1.8-fold in comparison with conventional microscopy. Combined with spin manipulation and detection, super-resolution NV center sensing is subsequently performed to reveal the optical and electrical properties of nanodevice. The high spatial resolution and feasibility of this work will promote the applications of quantum sensing in nanoscience.
Nitrogen-vacancy (NV) centers in diamond have been exploited as reliable single-photon emitters, with applications in quantum technologies and metrology. Two charge states are known for NV centers: NV0 and NV–, with the latter being mostly studied due to its long electron spin coherence time. Therefore, control over the charge state of the NV centers is essential. However, the understanding of the dynamics between the different states still remains challenging. Here we show that electron excitation induces the conversion from NV– to NV0 through electron-induced carrier generation. We present for the first time ultrafast pump-probe cathodoluminescence spectroscopy, with electron pulses as pump, and laser pulses as probe, to prepare and read out the NV states. The experimental data is explained with a model considering carrier dynamics (0.8 ns), NV0 spontaneous emission (20 ns) and NV0NV– back transfer (500 ms). Our results provide new insights into the NV–NV0 conversion dynamics, and into the use of pump-probe cathodoluminescence as a nanoscale NV characterization tool.