Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

arXiv:2109.11170 · Nature Communications

Quantum nonlinear spectroscopy of single nuclear spins

Jonas Meinel, Vadim Vorobyov, Ping Wang, Boris V. Yavkin, Matthias Pfender, Hitoshi Sumiya, Shinobu Onoda, Junichi Isoya, Ren‐Bao Liu, Jörg Wrachtrup

Published Sep 9, 2022• 22 citations
arXivHTMLPDF

Abstract

Conventional nonlinear spectroscopy, which use classical probes, can only access a limited set of correlations in a quantum system. Here we demonstrate that quantum nonlinear spectroscopy, in which a quantum sensor and a quantum object are first entangled and the sensor is measured along a chosen basis, can extract arbitrary types and orders of correlations in a quantum system. We measured fourth-order correlations of single nuclear spins that cannot be measured in conventional nonlinear spectroscopy, using sequential weak measurement via a nitrogen-vacancy center in diamond. The quantum nonlinear spectroscopy provides fingerprint features to identify different types of objects, such as Gaussian noises, random-phased AC fields, and quantum spins, which would be indistinguishable in second-order correlations. This work constitutes an initial step toward the application of higher-order correlations to quantum sensing, to examining the quantum foundation (by, e.g., higher-order Leggett-Garg inequality), and to studying quantum many-body physics.

DOI
10.1038/s41467-022-32610-8

Related papers

Quantum Nonlinear Spectroscopy via Correlations of Weak Faraday‐Rotation Measurements

Brian Chung Hang Cheung, Ren‐Bao Liu

Abstract The correlations of fluctuations are key to studying fundamental quantum physics and quantum many‐body dynamics. They are also useful information for understanding and combating decoherence in quantum technology. Nonlinear spectroscopy and noise spectroscopy are powerful tools to characterize fluctuations, but they can access only very few among the many types of higher‐order correlations. A systematic quantum sensing approach, called quantum nonlinear spectroscopy (QNS), is recently proposed for extracting arbitrary types and orders of time‐ordered correlations, using sequential weak measurement via a spin quantum sensor. However, the requirement of a central spin as the quantum sensor limits the versatility of the QNS since usually a central spin interacts only with a small number of particles in proximity and the measurement of single spins needs stringent conditions. Here, the aim is to employ the polarization (a pseudo‐spin) of a coherent light beam as a quantum sensor for QNS. After interacting with a target system (such as a transparent magnetic material), the small Faraday rotation of the linearly polarized light can be measured, which constitutes a weak measurement of the magnetization in the target system. Using a Mach–Zehnder interferometer with a designed phase shift, one can post‐select the effects of the light–material interaction to be either a quantum evolution or a quantum measurement of the material magnetization. This way, the correlated difference photon counts of a certain number of measurement shots, each with a designated interference phase, can be made proportional to a certain type and order of correlations of the magnetic fluctuations in the material. The analysis of the signal‐to‐noise ratios shows that the second‐order correlations are detectable in general under realistic conditions and higher‐order correlations are significant when the correlation lengths of the fluctuations are comparable to the laser spot size (such as in systems near the critical points). Since the photon sensor can interact simultaneously with many particles and interferometry is a standard technique, this protocol of QNS is advantageous for studying quantum many‐body systems.

arXiv:2309.00207•Advanced Quantum Technologies•Jun 16, 2024•3 citations

Gaussian-to-Non-Gaussian Transition of a Quantum Spin Bath Revealed by Fourth-Order Correlation

Fan Xia, S. Li, Xinyu Pan +2 more

Non-Gaussian fluctuations are one of the essential properties of quantum systems. However, the direct detection of non-Gaussian fluctuations has not yet been achieved in experiments since the specific order of correlation has to be isolated from the complex dynamics of the whole system. In this Letter, we measure the second- and fourth-order correlations of ^{13}C nuclear spins around a nitrogen vacancy center in diamond, using the recently developed quantum nonlinear spectroscopy. By adjusting the detection window and the spectral resolution, we observe the Gaussian to non-Gaussian transition of the multispin system. We find that the fourth-order correlation provides a fingerprint signal that can be used to identify individual spins with the same precession frequency, suggesting that Gaussianity is a potential quantum resource for quantum sensing. Our results shed light on the study of nonequilibrium quantum many-body dynamics and quantum materials at the nanoscale.

Physical Review Letters•May 27, 2025•3 citations

Detection of arbitrary quantum correlations via synthesized quantum channels

Ze Wu, Ping Wang, Tianyun Wang +6 more

Quantum correlations are key information about the structures and dynamics of quantum many-body systems. There are many types of high-order quantum correlations with different time orderings, but only a few of them are accessible to the existing detection methods. Recently, a quantum-sensing approach based on sequential weak measurement was proposed to selectively extract arbitrary types of correlations. However, its experimental implementation is still elusive. Here we demonstrate the extraction of arbitrary types of quantum correlations. We generalized the original weak measurement scheme to a protocol using synthesized quantum channels, which can be applied to more universal scenarios including both single and ensemble quantum systems. In this quantum channel method, various controls on the sensors are superimposed to select the sensor-target evolution along a specific path for measuring a desired quantum correlation. Using the versatility of nuclear magnetic resonance techniques, we successfully extract the second- and fourth-order correlations of a nuclear-spin target by another nuclear-spin sensor. The full characterization of quantum correlations provides a new tool for understanding quantum many-body systems, exploring fundamental quantum physics, and developing quantum technologies.

arXiv:2206.05883•Jun 13, 2022•0 citations

Quantum interpolation for high-resolution sensing

Ashok Ajoy, Yi-Xiang Liu, Kasturi Saha +4 more

Recent advances in engineering and control of nanoscale quantum sensors have opened new paradigms in precision metrology. Unfortunately, hardware restrictions often limit the sensor performance. In nanoscale magnetic resonance probes, for instance, finite sampling times greatly limit the achievable sensitivity and spectral resolution. Here we introduce a technique for coherent quantum interpolation that can overcome these problems. Using a quantum sensor associated with the nitrogen vacancy center in diamond, we experimentally demonstrate that quantum interpolation can achieve spectroscopy of classical magnetic fields and individual quantum spins with orders of magnitude finer frequency resolution than conventionally possible. Not only is quantum interpolation an enabling technique to extract structural and chemical information from single biomolecules, but it can be directly applied to other quantum systems for superresolution quantum spectroscopy.

arXiv:1604.01677•Proceedings of the National Academy of Sciences•Feb 14, 2017•37 citations

Optical readout of single spins for quantum computing and magnetic sensing

Rolf Simon Schoenfeld

The ability to measure and manipulate the quantum state of a single spin in a solid state system opens up a broad range of powerful applications ranging from nano probes to quantum information processing. Over the past few years, a number of ground breaking experiments have been conducted on paramagnetic nitrogen vacancy defect centers in diamond, including up to 3-qubit entanglement, single-shot-readout of a nuclear spin, selective access of two coupled centers and magnetic, electric and thermographic sensing at the nanoscale with promising properties in some cases exceeding most currently known techniques. Yet, almost all of the experiments conducted so far focus on centers deeply buried in the diamond, which is undesirable especially for sensing applications, but also in terms of scalability and electronic access to the information. In this work we focus on the spin physics of centers only few nanometers below the surface, where the unique properties of the center are strongly influenced by the external environment. We coherently manipulated and detected single spins at ambient temperature by combining optically detected magnetic resonance with single molecule spectroscopy using a confocal microscope. We measured the spin dephasing behavior and the phase relaxation time and examined the primary sources of decoherence. Furthermore, we observed effects of water, atmosphere and paramagnetic molecules on the coherence and readability of spins in nanodiamonds and demonstrated ways to preserve the coherence using external magnetic fields and a number of different dynamic decoupling pulse sequences. In addition, we measured couplings to proximal nuclear spins by continuous wave spectroscopy and to molecules on the surface by double electron electron resonance. Also, we demonstrate execution of the refined Deutsch-Jozsa algorithm on a nitrogen vacancy center in a nanodiamond. Finally, we propose new technological approach for realtime measurements of magnetic fields using a single spin in diamond. In test measurements using external fields and spatially resolved measurements of the field from a magnetic microwire a sensitivity of a few uT / sqrt(Hz) was achieved.

•Jan 1, 2011•3 citations

Nanoscale Detection of Many-Body Entanglement via Multidimensional Correlation Imprinting

T.Y. Zhang, Wentao Ji, Yuhang Guo +6 more

Understanding the nonequilibrium dynamics of isolated quantum many-body systems is a central goal of modern physics. Measuring genuine many-body correlations in quantum systems is central to this aim, while it remains a fundamental challenge for systems lacking individual addressability. We introduce a multidimensional correlation imprinting technique that encodes the structure of a many-body state into the temporal fluctuation spectrum of a local quantum probe. This allows direct measurement of arbitrary-order correlations in nonequilibrium quantum states. Using a nitrogen-vacancy center in diamond coupled to a ^{13}C nuclear spin bath, we experimentally reconstruct many-body correlation landscape to third order. Furthermore, by analyzing the spectral structure of correlation cumulants, we directly visualize the dynamics of quantum entanglement. Our Letter establishes a general approach to probing complex nonequilibrium phenomena and entanglement in quantum many-body systems at the nanoscale.

Physical Review Letters•Nov 19, 2025•1 citation
Conventional nonlinear spectroscopy, which use classical probes, can only access a limited set of correlations in a quantum system. Here we demonstrate that quantum nonlinear spectroscopy, in which a quantum sensor and a quantum object are first entangled and the sensor is measured along a chosen basis, can extract arbitrary types and orders of correlations in a quantum system. We measured fourth-order correlations of single nuclear spins that cannot be measured in conventional nonlinear spectroscopy, using sequential weak measurement via a nitrogen-vacancy center in diamond. The quantum nonlinear spectroscopy provides fingerprint features to identify different types of objects, such as Gaussian noises, random-phased AC fields, and quantum spins, which would be indistinguishable in second-order correlations. This work constitutes an initial step toward the application of higher-order correlations to quantum sensing, to examining the quantum foundation (by, e.g., higher-order Leggett-Garg inequality), and to studying quantum many-body physics.
Abstract The correlations of fluctuations are key to studying fundamental quantum physics and quantum many‐body dynamics. They are also useful information for understanding and combating decoherence in quantum technology. Nonlinear spectroscopy and noise spectroscopy are powerful tools to characterize fluctuations, but they can access only very few among the many types of higher‐order correlations. A systematic quantum sensing approach, called quantum nonlinear spectroscopy (QNS), is recently proposed for extracting arbitrary types and orders of time‐ordered correlations, using sequential weak measurement via a spin quantum sensor. However, the requirement of a central spin as the quantum sensor limits the versatility of the QNS since usually a central spin interacts only with a small number of particles in proximity and the measurement of single spins needs stringent conditions. Here, the aim is to employ the polarization (a pseudo‐spin) of a coherent light beam as a quantum sensor for QNS. After interacting with a target system (such as a transparent magnetic material), the small Faraday rotation of the linearly polarized light can be measured, which constitutes a weak measurement of the magnetization in the target system. Using a Mach–Zehnder interferometer with a designed phase shift, one can post‐select the effects of the light–material interaction to be either a quantum evolution or a quantum measurement of the material magnetization. This way, the correlated difference photon counts of a certain number of measurement shots, each with a designated interference phase, can be made proportional to a certain type and order of correlations of the magnetic fluctuations in the material. The analysis of the signal‐to‐noise ratios shows that the second‐order correlations are detectable in general under realistic conditions and higher‐order correlations are significant when the correlation lengths of the fluctuations are comparable to the laser spot size (such as in systems near the critical points). Since the photon sensor can interact simultaneously with many particles and interferometry is a standard technique, this protocol of QNS is advantageous for studying quantum many‐body systems.
Non-Gaussian fluctuations are one of the essential properties of quantum systems. However, the direct detection of non-Gaussian fluctuations has not yet been achieved in experiments since the specific order of correlation has to be isolated from the complex dynamics of the whole system. In this Letter, we measure the second- and fourth-order correlations of ^{13}C nuclear spins around a nitrogen vacancy center in diamond, using the recently developed quantum nonlinear spectroscopy. By adjusting the detection window and the spectral resolution, we observe the Gaussian to non-Gaussian transition of the multispin system. We find that the fourth-order correlation provides a fingerprint signal that can be used to identify individual spins with the same precession frequency, suggesting that Gaussianity is a potential quantum resource for quantum sensing. Our results shed light on the study of nonequilibrium quantum many-body dynamics and quantum materials at the nanoscale.
Quantum correlations are key information about the structures and dynamics of quantum many-body systems. There are many types of high-order quantum correlations with different time orderings, but only a few of them are accessible to the existing detection methods. Recently, a quantum-sensing approach based on sequential weak measurement was proposed to selectively extract arbitrary types of correlations. However, its experimental implementation is still elusive. Here we demonstrate the extraction of arbitrary types of quantum correlations. We generalized the original weak measurement scheme to a protocol using synthesized quantum channels, which can be applied to more universal scenarios including both single and ensemble quantum systems. In this quantum channel method, various controls on the sensors are superimposed to select the sensor-target evolution along a specific path for measuring a desired quantum correlation. Using the versatility of nuclear magnetic resonance techniques, we successfully extract the second- and fourth-order correlations of a nuclear-spin target by another nuclear-spin sensor. The full characterization of quantum correlations provides a new tool for understanding quantum many-body systems, exploring fundamental quantum physics, and developing quantum technologies.
Recent advances in engineering and control of nanoscale quantum sensors have opened new paradigms in precision metrology. Unfortunately, hardware restrictions often limit the sensor performance. In nanoscale magnetic resonance probes, for instance, finite sampling times greatly limit the achievable sensitivity and spectral resolution. Here we introduce a technique for coherent quantum interpolation that can overcome these problems. Using a quantum sensor associated with the nitrogen vacancy center in diamond, we experimentally demonstrate that quantum interpolation can achieve spectroscopy of classical magnetic fields and individual quantum spins with orders of magnitude finer frequency resolution than conventionally possible. Not only is quantum interpolation an enabling technique to extract structural and chemical information from single biomolecules, but it can be directly applied to other quantum systems for superresolution quantum spectroscopy.
The ability to measure and manipulate the quantum state of a single spin in a solid state system opens up a broad range of powerful applications ranging from nano probes to quantum information processing. Over the past few years, a number of ground breaking experiments have been conducted on paramagnetic nitrogen vacancy defect centers in diamond, including up to 3-qubit entanglement, single-shot-readout of a nuclear spin, selective access of two coupled centers and magnetic, electric and thermographic sensing at the nanoscale with promising properties in some cases exceeding most currently known techniques. Yet, almost all of the experiments conducted so far focus on centers deeply buried in the diamond, which is undesirable especially for sensing applications, but also in terms of scalability and electronic access to the information. In this work we focus on the spin physics of centers only few nanometers below the surface, where the unique properties of the center are strongly influenced by the external environment. We coherently manipulated and detected single spins at ambient temperature by combining optically detected magnetic resonance with single molecule spectroscopy using a confocal microscope. We measured the spin dephasing behavior and the phase relaxation time and examined the primary sources of decoherence. Furthermore, we observed effects of water, atmosphere and paramagnetic molecules on the coherence and readability of spins in nanodiamonds and demonstrated ways to preserve the coherence using external magnetic fields and a number of different dynamic decoupling pulse sequences. In addition, we measured couplings to proximal nuclear spins by continuous wave spectroscopy and to molecules on the surface by double electron electron resonance. Also, we demonstrate execution of the refined Deutsch-Jozsa algorithm on a nitrogen vacancy center in a nanodiamond. Finally, we propose new technological approach for realtime measurements of magnetic fields using a single spin in diamond. In test measurements using external fields and spatially resolved measurements of the field from a magnetic microwire a sensitivity of a few uT / sqrt(Hz) was achieved.
Understanding the nonequilibrium dynamics of isolated quantum many-body systems is a central goal of modern physics. Measuring genuine many-body correlations in quantum systems is central to this aim, while it remains a fundamental challenge for systems lacking individual addressability. We introduce a multidimensional correlation imprinting technique that encodes the structure of a many-body state into the temporal fluctuation spectrum of a local quantum probe. This allows direct measurement of arbitrary-order correlations in nonequilibrium quantum states. Using a nitrogen-vacancy center in diamond coupled to a ^{13}C nuclear spin bath, we experimentally reconstruct many-body correlation landscape to third order. Furthermore, by analyzing the spectral structure of correlation cumulants, we directly visualize the dynamics of quantum entanglement. Our Letter establishes a general approach to probing complex nonequilibrium phenomena and entanglement in quantum many-body systems at the nanoscale.