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Applied Physics Letters

Optical manipulation of the charge state of nitrogen-vacancy center in diamond

Xiang-Dong Chen, Chang‐Ling Zou, Fang‐Wen Sun, Guang‐Can Guo

Published Jul 1, 2013• 73 citations
Publisher

Abstract

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.

DOI
10.1063/1.4813120

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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.
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.
Ultrafast conversion dynamics between the NV 0 and NV – charge states in diamond is crucial for spin-state manipulation and readout. However, the underlying mechanism of the conversion, including the effective excitation wavelength, the time scales of the conversion, and the influencing factors, is still unclear. Here, we proposed a method to probe the ultrafast conversion of the two charge states via two-photon excitation with femtosecond laser pulses separated by 12.5 ns. We found that the highest conversion efficiency occurs at the excitation wavelength of around 532 nm, and the efficiency increases with temperature as well. The conversion time from NV 0 to NV – is obtained to be around 75 ps at 300 K. These findings advance the understanding of NV center charge-state dynamics and provide insights for high-speed spin readout in quantum information applications.
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 electron spin of the negatively charged the nitrogen vacancy center $({\mathrm{NV}}^{\ensuremath{-}}$) in diamond can be optically polarized through intersystem crossing, which enables the defect to be used for quantum computation and metrology. In this work, we studied the electron spin depolarization effect of the NV center induced by charge state conversion, which was proven to be a spin-independent process. The spin-state initialization fidelity was largely affected by the charge state conversion process. As a result, the optical polarization of the electron spin decreased about 1414%(31%14) with a high-power continuous-wave (pulsed) green laser. Moreover, the undefined fluorescence anomalous saturation effect of the NV center was analyzed and explained in detail based on the spin depolarization. The results demonstrated that a weak laser should be used for initialization of the NV center. In addition, the power and polarization of a laser for NV spin detection should be carefully adjusted to obtain the highest fluorescence signal. Our work also provided information that can increase the understanding of the charge state conversion and spin polarization processes of the NV center for quantum information and sensing.
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.
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 NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ under excitation with low power near-infrared (1064-nm) light, resulting in increased photoluminescence from the ${\mathrm{NV}}^{\ensuremath{-}}$ state. We used a combination of spectral and time-resolved photoluminescence experiments and rate-equation modeling to conclude that NV0{\mathrm{NV}}^{0}NV0 converts to ${\mathrm{NV}}^{\ensuremath{-}}$ 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.