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Optics Letters

Stimulated fluorescence quenching in nitrogen–vacancy centers of diamond: temperature effects

Sean M. Blakley, Andrei B. Fedotov, J. Becker, Narangerel Altangerel, И. В. Федотов, Philip Hemmer, Marlan O. Scully, Aleksei M. Zheltikov

Published Apr 25, 2016• 21 citations
Publisher

Abstract

Laser-induced fluorescence quenching in nitrogen-vacancy (NV) centers in diamond is studied simultaneously with in situ measurements of the heating-induced shift of the electron spin resonance of NV centers in the presence of a microwave field. These experiments reveal a strong correlation between fluorescence suppression in NV centers and the rise of the local temperature inside the diamond crystal. This finding sheds light on quantum pathways behind stimulated fluorescence quenching in NV centers of diamond and may imply significant limitations on the applications of this effect as a method of superresolving imaging in biological systems.

DOI
10.1364/ol.41.002077

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Laser-induced fluorescence quenching in nitrogen-vacancy (NV) centers in diamond is studied simultaneously with in situ measurements of the heating-induced shift of the electron spin resonance of NV centers in the presence of a microwave field. These experiments reveal a strong correlation between fluorescence suppression in NV centers and the rise of the local temperature inside the diamond crystal. This finding sheds light on quantum pathways behind stimulated fluorescence quenching in NV centers of diamond and may imply significant limitations on the applications of this effect as a method of superresolving imaging in biological systems.
Among quantum sensors, the single nitrogen-vacancy (NV) defect in diamond has the highest sensitivity-to-size factor. For instance, a single-NV spin when used as a magnetometer could achieve sensitivities of the order of nT/Hz, while the dimensions of the sensor are merely atomic in size. The sensitivity is limited only by the photon shot noise. One method to boost the magnetometer sensitivity to pico-tesla scales is to use many NV defect centers as an ensemble sensor [Phys. Rev. X5, 041001 (2015)PRXHAE2160-330810.1103/PhysRevX.5.041001]. However, during the absorption-emission (fluorescence) optical cycles, the NV centers transfer a portion of the irradiation laser energy into phonons and heat the diamond matrix. This results in unintended fluorescence decrease, spin resonance lines shifts, and fluctuations. Hence, the advantages gained by packing a high density of NV centers are significantly reduced. Here we investigate the heat generation of ensemble NV centers in micrometer-sized diamond under 532 nm laser irradiation and its effects pertaining to sensing applications. These investigations help us to find strategies that mitigate the detrimental effects of heating and yet permits the use of ensemble NV defects for improved metrology applications.
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.
Magnetic resonance and fluorescence spectra of nitrogen-vacancy (NV) color centers ensemble in high purity diamond sample were measured, with temperature ranging from 5.6 K to 295 K. Both microwave and optical transition energies have similar nonlinear temperature dependent changes, which might mainly originate from the local thermal expansion. As the frequency shifts will reduce the fidelity of resonant quantum control, the present results demonstrate the necessity of taking temperature fluctuation into consideration. For temperature below 100 K, the transition energies show tendencies to be constant, which indicate higher stability and performance in applications with NV centers.
Diamond samples of defects with negative charged nitrogen-vacancy (NV) centers are promising solid state spin sensors suitable for quantum information processing, high sensitive measurements of magnetic, electric and thermal fields in nanoscale. The diamond defect with a NV center is unique for its robust temperature-dependent zero field splitting Dgs of the triplet ground state. This property enables optical readout of electron spin states through manipulation of the ground triplet state using microwave resonance with Dgs from 100 K to about 600 K. Thus, prohibiting Dgs from unwanted external thermal disturbances is crucial for an accurate measurement using diamond NV sensors. Our observation demonstrates the existence of a prominent microwave heating effect on the diamond samples of NV centers. The effect is inevitable to shift Dgs and cause measurement errors. The temperature increment caused by the effect monotonically depends on the power and the duration of microwave irradiation. The effect is obvious with the microwave irradiation in the continuous mode and some pulse sequence modes, but is neglectable for the quantum lock-in XY8-N method.
The nitrogen vacancy (NV) center in diamond is the most widely studied color center in diamond for its wide range of applications in both physics and biology. The negatively charged state ${\mathrm{NV}}^{\ensuremath{-}}$ is often favored for its better spin-optical properties, whereas the presence of the neutral charge state NV0{\mathrm{NV}}^{0}NV0 is often minimized or neglected by using a single optimized excitation wavelength. In many cases, the use of additional laser wavelengths has an important impact on the NV optical properties and can lead to a dramatically quenched fluorescence. Through measurements of the photophysics of the NV center we show in this work that this quenching mechanism is mediated by charge state interconversion providing additional channels for nonradiative decay. Our results show that this mechanism is also sensitive to the spin state of the ${\mathrm{NV}}^{\ensuremath{-}}$. A better understanding of this physical mechanism will help mitigate the spin and charge state depolarization effects that are detrimental for quantum technology applications.
Abstract A novel creation procedure for the nitrogen-vacancy (NV) center in diamond is investigated. After shallow nitrogen implantation, a continuous-wave laser is used to induce NV formation, while simultaneously exciting fluorescence to enable live observation. Our investigations imply that a different mechanism than heat induced vacancy diffusion causes the formation of NV centers with this method and we suggest possible alternative pathways which could be responsible, based on the observed properties. Furthermore, we test the procedure for its capabilities for the controlled creation of single centers and show that the emergence of individual centers can be tracked, while achieving sub-micrometer spatial precision.