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Physical Review A

Charge-state conversion in nitrogen-vacancy centers mediated by an engineered photonic environment

Sachin Kumar Sharma, Rajesh V. Nair

Published Apr 27, 2020• 6 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.101.043420

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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.
We study the effect of charge state conversion of nitrogen vacancy (NV) centers on the local density of states (LDOS) induced modifications in emission lifetime. The pump-dependent decay rates reveal two power regimes according to the dominance of photoionization of NV centers or the effect of LDOS. The extent of lifetime modification is achieved at low pump power, whereby the emission rate of zero phonon line is enhanced and the rate of phonon sideband emission is suppressed. At high pump power, the effect of modified emission rate is demeaned due to increased photoionization of NV centers.
Abstract The nitrogen-vacancy (NV) center is one of the most prominent candidates for quantum technologies, and its efficient utilization requires control over its spontaneous emission rate. Here, we report the wavelength-selective enhancement and suppression of NV center emission lifetime at room temperature by modifying the local density of optical states (LDOS) around them. The results are explained using the Barnett–Loudon sum rule and also supported by the LDOS calculations. Two complementary measurement geometries are employed to study the direction-dependent emission behavior from the nanodiamonds decorated on the top of photonic crystals. The lifetime distributions are compared with a proper reference sample using the Kolmogorov–Smirnov test to verify the distinct nature of lifetime distributions. The wavelength-selective enhancement or suppression of emission rates would be useful for NV center-based high-resolution imaging and effective readout of its charge states.
Nitrogen–vacancy (NV) centers in diamond are generally recognized as highly promising as indefinitely stable highly efficient single-photon sources. We report an experimental quantification of the brightness, radiative decay rate, nonradiative decay rate and quantum efficiency of single NV centers in diamond nanocrystals. Our experiments show that the commonly observed large spread in fluorescence decay rates of NV centers in nanodiamond is inconsistent with the common explanation of large nanophotonic mode-density variations in the ultra-small high-index crystals at near-unity quantum efficiency. We report that NV centers in 25 nm nanocrystals are essentially insensitive to local density of optical states (LDOS) variations that we induce at a dielectric interface by using liquids to vary the refractive index, and propose that quantum efficiencies in such nanocrystals are widely distributed between 0 and 20%. For single NV centers in larger 100 nm nanocrystals, we show that decay rate changes can be reversibly induced by nanomechanically approaching a mirror to change the LDOS. Using this scanning mirror method, for the first time we report calibrated quantum efficiencies of NV centers, and show that different but nominally identical nanocrystals have widely distributed quantum efficiencies between 10 and 90%. Our measurements imply that nanocrystals that are to be assembled into hybrid photonic structures for cavity QED should first be individually screened to assess fluorescence properties in detail.
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 manipulation of the charge states of nitrogen-vacancy (NV) centers in diamond is a prerequisite for next-generation quantum sensing, communication, and computing. Here, we use phonon-assisted anti-Stokes excitation to realize the reversible conversion between the NV 0 and NV – states. In this case, we observe two decay processes of NV – centers with lifetimes as long as tens of seconds. By studying the kinetics of spectral structure evolution of NV – states, we find that the spectral structure of the NV – center is modulated by the charge state transition process under anti-Stokes excitation. We propose that the main reason is the local electric field generated by the ionization of the NV –, which changes the radiation environment of the color centers. Our results might provide an alternative method to control the charge states of nitrogen-vacancy centers.
Recently, the nitrogen vacancy (NV) center has emerged as a deterministic single-photon source at room temperature. However, the presence of phonon sideband emission limits the use of NV centers in various quantum optical applications. Here we report a novel way to suppress the phonon sideband emission of NV centers aided with the enhancement of zero phonon line intensity using photonic crystals at room temperature. We study the photonic stop gap mediated charge state conversion in NV centers. The enhancement of phonon sideband emission from the same structures by implementing a different measurement geometry is also discussed. The studies open new avenues in studying the NV center-based quantum nanophotonics and biophotonics.