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arXiv:1207.5276 · New Journal of Physics

Nanoscale magnetometry through quantum control of nitrogen–vacancy centres in rotationally diffusing nanodiamonds

Dougal Maclaurin, Liam T. Hall, A. Martin, Lloyd C. L. Hollenberg

Published Jan 17, 2013• 33 citations
arXivHTMLPDF

Abstract

The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen–vacancy centre in diamond—a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen–vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of nitrogen–vacancy magnetometry are developed for a randomly diffusing diamond nanocrystal. We find that the accumulation of geometric phases, due to the rotation of the nanodiamond plays a crucial role in the application of a diffusing nanodiamond as a bio-label and magnetometer. Specifically, we show that a freely diffusing nanodiamond can offer real-time information about local magnetic fields and its own rotational behaviour, beyond continuous optically detected magnetic resonance monitoring, in parallel with operation as a fluorescent biomarker.

DOI
10.1088/1367-2630/15/1/013041

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The confluence of quantum physics and biology is driving a new generation of quantum-based sensing and imaging technology capable of harnessing the power of quantum effects to provide tools to understand the fundamental processes of life. One of the most promising systems in this area is the nitrogen–vacancy centre in diamond—a natural spin qubit which remarkably has all the right attributes for nanoscale sensing in ambient biological conditions. Typically the nitrogen–vacancy qubits are fixed in tightly controlled/isolated experimental conditions. In this work quantum control principles of nitrogen–vacancy magnetometry are developed for a randomly diffusing diamond nanocrystal. We find that the accumulation of geometric phases, due to the rotation of the nanodiamond plays a crucial role in the application of a diffusing nanodiamond as a bio-label and magnetometer. Specifically, we show that a freely diffusing nanodiamond can offer real-time information about local magnetic fields and its own rotational behaviour, beyond continuous optically detected magnetic resonance monitoring, in parallel with operation as a fluorescent biomarker.
Quantum sensing using nitrogen-vacancy (NV) centers in diamond has emerged as a powerful platform for detecting ultra-low magnetic fields under ambient conditions. Owing to their long spin coherence times, optical addressability, and compatibility with aqueous environments, it has found widespread applications in biosensing and bio-imaging. This review presents the fundamental principles and recent advances in NV-based quantum magnetometry for biosensing applications, with a particular focus on measurements in aqueous medium and at cellular and molecular length scales. We discuss the underlying spin physics of NV centers and highlight two primary detection modalities: optically detected magnetic resonance (ODMR) and T1 relaxometry-based sensing and how these approaches aids in the detection of both static magnetic fields and dynamic magnetic noise arising from biological processes. The review explores key application areas, including nanoscale nuclear magnetic resonance (NMR), monitoring of neural activity, detection of abnormal or rogue cells using NV-based platforms etc. In addition, strategies for enhancing sensitivity, such as surface functionalization of nanodiamonds, femtosecond (fs) laser-written photonic structures, and integration with microfluidic and lab-on-chip systems have also been discussed in depth. We also address the critical challenges, including surface-induced decoherence, charge-state instability, and signal-to-noise limitations in biofluids associated with NV-based biosensing applications. Finally, we outline future prospects, highlighting how NV-based magnetic biosensing provides a promising pathway for translating quantum sensing technologies into practical biomedical applications.
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This thesis represents several steps in the development of Nitrogen-Vacancy Nanodiamond as an effective optical label for biological measurements and as a tool for nanometry and quantum information techniques. In this thesis I cover concrete progress in many areas of nanodiamond research, demonstrating that optical interactions alone can be used to control NV spin polarisation and measure NV temperature. I develop a method for high-contrast imaging of NV centres using magnetic modulation, and also show a method for measuring the Raman scattering of water to an unprecedented level of accuracy. This thesis also contains the outlines of two more experiments: one aimed at measuring NV concentration in aqueous nanodiamond suspensions, and another whose aim is to use multiple NV centres in a single nanodiamond to measure the orientation and strength of an external magnetic field.
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.
A controlled qubit in a rotating frame opens new opportunities to probe fundamental quantum physics, such as geometric phases in physically rotating frames, and can potentially enhance detection of magnetic fields. Realising a single qubit that can be measured and controlled during physical rotation is experimentally challenging. In this work, we demonstrate quantum control of a single nitrogen-vacancy (NV) centre within a diamond rotated at 200,000rpm, a rotational period comparable to the NV spin coherence time T2T_2T2​. We stroboscopically image individual NV centres that execute rapid circular motion in addition to rotation, and demonstrate preparation, control and readout of the qubit quantum state with lasers and microwaves. Using spin-echo interferometry of the rotating qubit, we are able to detect modulation of the NV Zeeman shift arising from the rotating NV axis and an external DC magnetic field. Our work establishes single NV qubits in diamond as quantum sensors in the physically rotating frame, and paves the way for the realisation of single-qubit diamond-based rotation sensors.
The nitrogen-vacancy (NV) centre in diamond gained popularity as a probe for nanoscale sensing applications in research thanks to the array of sensing modalities available and the bio-compatibility of the material itself, however the utility of NV sensing is limited by the lack of suitable strategies to control them spatially. By confining single nanodiamonds using an optical tweezers (OT) we are able to combine the sensing opportunities of the NV centre with the precision control of position and orientation afforded by OT. This work is an investigation of the interaction of the trapping laser with the spin-based photoluminescence of the NV centre, further it is a demonstration of an all-optical sensing protocol which eliminates the spin depolarisation effects of the trapping laser and allows for NV spin relaxometry in an optically trapped nanodiamond. This relaxometry protocol can determine spin lattice relaxation times on the order of ms and requires relatively low trapping powers < 50 mW, making it particularly applicable to biological systems.