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Acta Physica Sinica

Quantum sensing based on strongly interacting nuclear spin systems

Qing Li, Yunlan Ji, Ran LIU, Dieter Suter, Min Jiang, Xinhua Peng

Published Jan 1, 2025• 1 citation
Publisher

Abstract

Quantum sensing utilizes the quantum resources of well-controlled quantum systems to measure small signals with high sensitivity, and has great potential in both fundamental science and concrete applications. Interacting quantum systems have attracted increasing interest in the field of precise measurements, owing to their potential to generate quantum-correlated states and exhibit rich many-body dynamics. These features provide a novel avenue for exploiting quantum resources in sensing applications. Although previous studies have shown that using such systems can improve sensitivity, they mainly focused on measuring individual physical quantities. In experiment, the challenge of using interacting quantum systems to achieve high-precision measurements of multiple physical parameters simultaneously has not been explored to a large extent. In this study, we demonstrate a first realisation of interaction-based multiparameter sensing by using strongly interacting nuclear spins under ultra-low magnetic field conditions. We find that, as the interaction strength among nuclear spins becomes significantly larger than their Larmor frequencies, a different regime emerges where the strongly interacting spins can be simultaneously sensitive to all components of a multidimensional field, such as a three-dimensional magnetic field. Moreover, we observe that the strong interactions between nuclear spins can increase their quantum coherence times to as long as several seconds, thereby improving measurement precision. Our sensor successfully achieves precision measurement of three-dimensional vector magnetic fields with a field sensitivity reaching the order of 10–11 T and an angular resolution as high as 0.2 rad. Importantly, this approach eliminates the need for external reference fields, thereby avoiding calibration errors and technical noise commonly encountered in traditional magnetometry. Experimentally optimized protocol further enhances the sensitivity of the interacting spin-based sensor by up to five orders of magnitude compared with non-interacting or classical schemes. These results demonstrate the enormous potential of interacting spin systems as a powerful platform for high-precision multi-parameter quantum sensing. The techniques developed here pave the way for a new generation of quantum sensors that use intrinsic spin interactions to exceed the traditional sensitivity limits, presenting a promising route toward ultra-sensitive, calibration-free magnetometry in complex environments.

DOI
10.7498/aps.74.20250271

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Quantum sensing utilizes the quantum resources of well-controlled quantum systems to measure small signals with high sensitivity, and has great potential in both fundamental science and concrete applications. Interacting quantum systems have attracted increasing interest in the field of precise measurements, owing to their potential to generate quantum-correlated states and exhibit rich many-body dynamics. These features provide a novel avenue for exploiting quantum resources in sensing applications. Although previous studies have shown that using such systems can improve sensitivity, they mainly focused on measuring individual physical quantities. In experiment, the challenge of using interacting quantum systems to achieve high-precision measurements of multiple physical parameters simultaneously has not been explored to a large extent. In this study, we demonstrate a first realisation of interaction-based multiparameter sensing by using strongly interacting nuclear spins under ultra-low magnetic field conditions. We find that, as the interaction strength among nuclear spins becomes significantly larger than their Larmor frequencies, a different regime emerges where the strongly interacting spins can be simultaneously sensitive to all components of a multidimensional field, such as a three-dimensional magnetic field. Moreover, we observe that the strong interactions between nuclear spins can increase their quantum coherence times to as long as several seconds, thereby improving measurement precision. Our sensor successfully achieves precision measurement of three-dimensional vector magnetic fields with a field sensitivity reaching the order of 10–11 T and an angular resolution as high as 0.2 rad. Importantly, this approach eliminates the need for external reference fields, thereby avoiding calibration errors and technical noise commonly encountered in traditional magnetometry. Experimentally optimized protocol further enhances the sensitivity of the interacting spin-based sensor by up to five orders of magnitude compared with non-interacting or classical schemes. These results demonstrate the enormous potential of interacting spin systems as a powerful platform for high-precision multi-parameter quantum sensing. The techniques developed here pave the way for a new generation of quantum sensors that use intrinsic spin interactions to exceed the traditional sensitivity limits, presenting a promising route toward ultra-sensitive, calibration-free magnetometry in complex environments.
Interacting quantum systems are attracting increasing interest for developing precise metrology. In particular, the realisation that quantum-correlated states and the dynamics of interacting systems can lead to entirely new and unexpected phenomena have initiated an intense research effort to explore interaction-based metrology both theoretically and experimentally. However, the current framework of interaction-based metrology mainly focuses on single-parameter estimations, a demonstration of multiparameter metrology using interactions as a resource was heretofore lacking. Here we demonstrate an interaction-based multiparameter metrology with strongly interacting nuclear spins. We show that the interacting spins become intrinsically sensitive to all components of a multidimensional field when their interactions are significantly larger than their Larmor frequencies. Using liquid-state molecules containing strongly interacting nuclear spins, we demonstrate the proof-of-principle estimation of all three components of an unknown magnetic field and inertial rotation. In contrast to existing approaches, the present interaction-based multiparameter sensing does not require external reference fields and opens a path to develop an entirely new class of multiparameter quantum sensors.
The use of nuclear spins as physical sensing systems is disadvantaged by their low signal responsivity, particularly when compared to sensing techniques based on electron spins. This primarily results from the small nuclear gyromagnetic ratio and the difficulties in achieving high spin polarization. Here we develop a new approach to investigating the response of hyperpolarized molecular nuclear spins to magnetic fields and demonstrate orders-of-magnitude enhanced magnetic responsivity over state-of-the-art proton and Overhauser magnetometers. Using hyperpolarized molecules with proton spins, we report the realization of magnetic amplification in linear and nonlinear types. We further extend this amplification to hyperpolarized scalar-coupled multi-spin molecules and observe substantial magnetic amplification exceeding 10%. Moreover, we observe an anomalous amplification with dispersive frequency dependence that originates from magnetic interference effects. Our work highlights the potential of hyperpolarized molecular nuclear spins for use in a new class of quantum sensors, with promising applications in both applied and fundamental physics, including highly accurate absolute magnetometry and the exploration of axion-nucleon exotic interactions.
Quantum sensing has witnessed rapid development and transition from laboratories to practical applications in the past decade. Applications of quantum sensors, ranging from nanotechnologies to biosensing, are expected to benefit from quantum sensors' unprecedented spatial resolution and sensitivity. Solid-state spin systems are particularly attractive platforms for quantum sensing technologies because room temperature operation is viable while reaching the quantum limits of sensitivity. Among various solid-state spin systems, nitrogen-vacancy (NV) centers in diamond demonstrated high-fidelity initialization, coherent control, and high contrast readout of the electron spin state. However, electron spin coherence due to noise from the surrounding spin bath and this environment effect limits the sensitivity of NV centers. Thus, a critical task in NV center-based quantum sensing is sensitivity enhancement through coherence protection. Several strategies, such as dynamical decoupling techniques, feedback control, and nuclear spin-assisted sensing protocols, have been developed and realized for this task. Among these strategies, nuclear spin-assisted protocols have demonstrated greater enhancement of electron spin coherence. In addition, the electron and nuclear spin pair of an NV center in diamond naturally allows the application of the nuclear spin-assisted sensitivity enhancement protocol. Owing to long nuclear coherence times, further enhancement of sensitivity can be achieved by exploiting active nuclear spins (e.g., 14N, 13C) in the proximity of an NV center as memory ancillas when coupled with the NV center. Here, we review the spin properties of NV centers, mechanisms of the nuclear spin-assisted protocol and its gate variation, and the status of quantum sensing applications in high-resolution nuclear spin spectroscopy, atomic imaging, and magnetic field sensing. We discuss the potential for commercialization, current challenges in sensitivity enhancement, and conclude with future research directions for promoting the development of nuclear spin-assisted protocol and its integration into industrial applications.
In modern-day quantum metrology, quantum sensors are widely employed to detect weak magnetic fields or nanoscale signals. Quantum devices, exploiting quantum coherence, are inevitably connected to physical constants and can achieve accuracy, repeatability, and precision approaching fundamental limits. As a result, these sensors have shown utility in a wide range of research domains spanning both science and technology. A rapidly emerging quantum sensing platform employs atomic-scale defects in crystals. In particular, magnetometry using nitrogen-vacancy (NV) color centers in diamond has garnered increasing interest. NV systems possess a combination of remarkable properties, optical addressability, long coherence times, and biocompatibility. Sensors based on NV centers excel in spatial resolution and magnetic sensitivity. These diamond-based sensors promise comparable combination of high spatial resolution and magnetic sensitivity without cryogenic operation. The above properties of NV magnetometers promise increasingly integrated quantum measurement technology, as a result, they have been extensively developed with various protocols and find use in numerous applications spanning materials characterization, nuclear magnetic resonance (NMR), condensed matter physics, paleomagnetism, neuroscience and living systems biology, and industrial vector magnetometry. In this chapter, NV centers are explored for magnetic sensing in a number of contexts. In general, we introduce novel regimes for magnetic-field probes with NV ensembles. Specifically, NV centers are developed for sensitive magnetometers for applications where microwaves (MWs) are prohibitively invasive and operations need to be carried out under zero ambient magnetic field. The primary goal of our discussion is to improve the utility of these NV center-based magnetometers.
The recent decade has witnessed exciting developments in quantum science and technology. Quantum sensing is a rapidly growing branch, which exploits the fragility of quantum systems to detect small external signals. The extreme control at the single-atom level and the remarkably long coherence time of engineered quantum systems enable unprecedented sensitivity and precision, beating the performance of classical techniques. The nitrogen-vacancy (NV) center in diamond is one of the most promising quantum sensors. Its unique advantages have attracted considerable attention, including a long spin coherence time throughout a broad temperature range, nanoscale resolution limited by the sensor-sample distance, convenient optical control of its spin states and remarkably versatile sensing capabilities. Its properties are well studied under a bias magnetic field oriented along its quantization axis. However, its sensing capabilities in the presence of an off-axis magnetic field are much less explored. My research aims to unlock the full potential of NV quantum sensor by developing new sensing modalities under a magnetic field acting perpendicular to the NV axis, and furthermore, integrating them into a scanning probe microscope. In this dissertation, I will report our progress toward building a scanning NV multimodal quantum imaging platform, which will open up exciting opportunities in measuring nanoscale phenomena. The first chapter provides an introduction to the background of quantum sensing with NV centers, followed by a discussion on its basic properties and established sensing techniques. The second and third chapters are dedicated to two experiments performed under a perpendicular magnetic field where traditional NV magnetometry based on the Zeeman effect fails. In the second chapter, I will introduce a new sensing strategy that uses the entanglement between the electron and nuclear spins to restore the magnetic field sensitivity under this unfavored condition. This allows us to sense small changes in the magnetic field angle relative to the NV axis, and to detect anisotropic magnetic noise in the local environment. In the third chapter, I will present our latest development of scanning NV electrometry, where a single NV at the apex of a diamond scanning probe images external alternating (AC) and direct (DC) electric fields with sub-100 nm resolution. In the last chapter, I will discuss our efforts on four experiments that were left unfinished. I will present the results we have achieved, analyze the challenges that we faced and propose potential solutions to overcome them.
Abstract Solid state spins have demonstrated significant potential in quantum sensing with applications including fundamental science, medical diagnostics and navigation. The quantum sensing schemes showing best performance under ambient conditions all utilize microwave or radio-frequency driving, which poses a significant limitation for miniaturization, energy efficiency, and non-invasiveness of quantum sensors. We overcome this limitation by demonstrating a purely optical approach to coherent quantum sensing. Our scheme involves the 15N nuclear spin of the Nitrogen-Vacancy (NV) center in diamond as a sensing resource, and exploits NV spin dynamics in oblique magnetic fields near the NV’s excited state level anti-crossing to optically pump the nuclear spin into a quantum superposition state. We demonstrate all-optical free-induction decay measurements—the key protocol for low-frequency quantum sensing—both on single spins and spin ensembles. Our results pave the way for highly compact quantum sensors to be employed for magnetometry or gyroscopy applications in challenging environments.