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arXiv:1809.01668 · Physical Review Letters

Imaging the Local Charge Environment of Nitrogen-Vacancy Centers in Diamond

Thomas Mittiga, Satcher Hsieh, Chong Zu, Bryce Kobrin, Francisco Machado, Prabudhya Bhattacharyya, Nicholas Z. Rui, Andrey Jarmola, Soonwon Choi, Dmitry Budker, Norman Y. Yao

Published Dec 12, 2018• 170 citations
arXivHTMLPDF

Abstract

Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields, and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at a low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning more than two orders of magnitude. Motivated by this understanding, we propose and implement a novel method for the nanoscale localization of individual charges within the diamond lattice; our approach relies upon the fact that the charge induces a NV dark state which depends on the electric field orientation.

DOI
10.1103/physrevlett.121.246402

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Characterizing the local internal environment surrounding solid-state spin defects is crucial to harnessing them as nanoscale sensors of external fields. This is especially germane to the case of defect ensembles which can exhibit a complex interplay between interactions, internal fields, and lattice strain. Working with the nitrogen-vacancy (NV) center in diamond, we demonstrate that local electric fields dominate the magnetic resonance behavior of NV ensembles at a low magnetic field. We introduce a simple microscopic model that quantitatively captures the observed spectra for samples with NV concentrations spanning more than two orders of magnitude. Motivated by this understanding, we propose and implement a novel method for the nanoscale localization of individual charges within the diamond lattice; our approach relies upon the fact that the charge induces a NV dark state which depends on the electric field orientation.
We report measurements of optically detected magnetic resonance spectra of ensembles of negatively charged nitrogen-vacancy (NV) centers in diamonds in the presence of strain and DC external electric fields. The Stark shift of the spectral lines is stronger when the axial magnetic field along the NV centers quantization axis is minimized. The shift is also enhanced at avoided crossings between the hyperfine levels at an axial field of 77 uT. Since the intrinsic strain in the diamond also induces a Stark shift, we are able to calculate the magnitude and direction of the strain within the crystal. We also use the Stark effect to map the electric field in the diamond volume between patterned electrodes.
The NV defect center in diamond forms a pseudo-atomic quantum system with discreet optically excitable transitions between ground and excited states in the gap between valence and conduction bands, making the NV center a deep-level defect center in diamond. For the negatively charged NV center (NV-), both the ground and excited states are spin triplets (S=1) and coupling between optical and spin states provides unique opportunities for optical detection of magnetic resonance (ODMR) and quantum metrology under ambient conditions. As an atomically sized point defect that is stable in single nanodiamonds as small as a few nanometers, the NV center enables spin based imaging of temperature, electric fields, magnetic fields and mechanical strain with nanoscale spatial resolution. Made of carbon, nanodiamonds are also ideal nanoparticles for use in biological systems, exhibiting extremely low cytotoxicity, no photo bleaching and exceptional contrast in transmission electron and light microscopy. With the ability to act as both a passive, non perturbing sensor (e.g. a diamagnetic material used for sensing magnetic fields) and a connection point for two way, direct coupling of far field optics to NV−^-− spins and indirectly to the highly localized neighborhood of atoms, electronic states and phonon modes in the local vicinity, NV diamond provides a route to nanoscale field sensing and spin based optical microscopy. These sensors are also stable in nanodiamonds. For nanoparticles, the reduction in particle diameter dramatically enhances the proportion of the material that is surface exposed, enhancing any surface related properties. Nitrogen Vacancy centers in nanodiamonds provide another example of material properties that vary with particle size. In chapter 5, evidence that modulation of nanodiamonds fluorescent emissions by electrical perturbations in their surrouding environment allows transduction of local electrodynamics into a far field optical signal capable of mapping action potentials in cardiomyocytes in presented. The unifying theme for all of the work presented in this dissertation is to enable the use of magnetic resonance signals and interactions for imaging and sensing in previously inaccessible regimes. The specific focus is on methods and techniques to enable nanoscale physical sensing and functional imaging in live tissues, with the ultimate aim to lay the predicate for the combination of both without compromise.
Ensembles of nitrogen-vacancy (N-VVV) centers in diamond show promise as versatile electric field sensors, but are limited by noise from an inhomogeneous internal charge environment. Here researchers develop a scheme for optically enhanced electrometry that improves N-VVV sensitivity to external electric fields, especially at low temperatures. They also implement a complementary method for experimentally extracting the color center's excited-state electric field susceptibilities, and they provide a simple scaling theory for optimizing the density of N-VVV defects in electrometry applications.
Nitrogen-Vacancy (NV) centers in diamond have been established as exceptionally versatile probes for quantum technologies from sensing to simulation.Owing to the versatility of diamond fabrication, NVs can be integrated into probes with nanoscale resolution and superb sensitivity.\nHowever, because the diamond is host to many other types of defects, the local environment of the NV is unique for each NV, which poses challenges for any devices instrumenting NVs.\nThis thesis contributes to the future of NV technologies along two essential directions.\nFirst, we work towards a more complete understanding of the local charge and strain environments of the NV.\nIn addition to permitting the calibration of these effects for NV probes, we suggest potential uses for the local charges and strain that had previously been considered hindrances.\nSecond, we develop new technologies for NV sensing and simulation.\nOur work integrating NVs into diamond anvil cells opens the door to detecting high pressure phenomena using the NVs as all-in-one sensors.\nFinally, our study of the coherence regimes of the local defect environment of the NV is a step towards versatile quantum simulation in dimensions lower than three.
Nitrogen-vacancy (NV) centers in nanodiamonds have emerged as a promising quantum sensing platform for biomedical imaging applications, yet random orientations of individual particles present significant challenges in large-scale sensor calibration. In this study, we demonstrate a novel approach to simultaneously determine each particle's crystallographic axes and the surrounding local vector magnetic field. Specifically, a minimum of four distinct bias fields is required to unambiguously extract both the orientation and the local field. We validate our method experimentally using NV centers in two scenarios: (1) in a bulk diamond with known crystal orientation as a proof of concept, and (2) on various single nanodiamonds to mimic real-world applications. Our work represents a crucial step towards unlocking the full potential of nanodiamonds for advanced applications such as in-situ biomedical imaging and nanoscale sensing in complex environments.
Control over the charge states of color centers in solids is necessary to fully utilize them in quantum technologies. However, the microscopic charge dynamics of deep defects in wide-band-gap semiconductors are complex, and much remains unknown. We utilize a single-shot charge-state readout of an individual nitrogen-vacancy (NV) center to probe the charge dynamics of the surrounding defects in diamond. We show that the NV center charge state can be converted through the capture of holes produced by optical illumination of defects many micrometers away. With this method, we study the optical charge conversion of silicon-vacancy (SiV) centers and provide evidence that the dark state of the SiV center under optical illumination is SiV 2– . These measurements illustrate that charge carrier generation, transport, and capture are important considerations in the design and implementation of quantum devices with color centers and provide a novel way to probe and control charge dynamics in diamond.