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Proceedings of the National Academy of Sciences

Toward quantum sensing of electron beams using solid-state spins

Jakob Grzesik, Dominic Catanzaro, Charles Roques‐Carmes, Eric I. Rosenthal, G. L. van de Stolpe, Aviv Karnieli, Giovanni Scuri, Souvik Biswas, Kenneth J. Leedle, Dylan S. Black, Robert L. Byer, Ido E. Kaminer, R. J. England, Shanhui Fan, Olav Solgaard, Jelena Vuckovic A

Published Jun 12, 2026• 0 citations
Publisher

Abstract

Scattering experiments with energetic particles, such as free electrons, have been historically used to reveal the quantum structure of matter. However, realizing coherent interactions between free-electron beams and solid-state quantum systems has remained out of reach, owing to their intrinsically weak coupling. Realizing such coherent control would open up opportunities for hybrid quantum platforms combining free electrons and solid-state qubits for coincident quantum information processing and nanoscale sensing. Here, we present a framework that employs negatively charged nitrogen-vacancy centers (NV − ) in diamond as quantum sensors of a bunched electron beam. We develop a Lindblad master equation description of the magnetic free-electron–qubit interactions and identify spin relaxometry as a sensitive probe of the interaction. Experimentally, we integrate a confocal fluorescence microscopy setup into a microwave-bunched electron beam line. We monitor charge-state dynamics and assess their impact on key sensing performance metrics (such as spin readout contrast), defining safe operating parameters for quantum sensing experiments. By performing T 1 relaxometry under controlled electron beam exposure, we do not resolve a measurable reduction in T 1 within experimental uncertainty, and instead establish an upper bound on the free-electron–spin coupling strength. Our results establish NV − centers as quantitative probes of free electrons, providing a metrological benchmark for free-electron–qubit coupling under realistic conditions, and chart a route toward solid-state quantum control with electron beams.

DOI
10.1073/pnas.2531808123

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Scattering experiments with energetic particles, such as free electrons, have been historically used to reveal the quantum structure of matter. However, realizing coherent interactions between free-electron beams and solid-state quantum systems has remained out of reach, owing to their intrinsically weak coupling. Realizing such coherent control would open up opportunities for hybrid quantum platforms combining free electrons and solid-state qubits for coincident quantum information processing and nanoscale sensing. Here, we present a framework that employs negatively charged nitrogen-vacancy centers (NV − ) in diamond as quantum sensors of a bunched electron beam. We develop a Lindblad master equation description of the magnetic free-electron–qubit interactions and identify spin relaxometry as a sensitive probe of the interaction. Experimentally, we integrate a confocal fluorescence microscopy setup into a microwave-bunched electron beam line. We monitor charge-state dynamics and assess their impact on key sensing performance metrics (such as spin readout contrast), defining safe operating parameters for quantum sensing experiments. By performing T 1 relaxometry under controlled electron beam exposure, we do not resolve a measurable reduction in T 1 within experimental uncertainty, and instead establish an upper bound on the free-electron–spin coupling strength. Our results establish NV − centers as quantitative probes of free electrons, providing a metrological benchmark for free-electron–qubit coupling under realistic conditions, and chart a route toward solid-state quantum control with electron beams.
Scattering experiments with energetic particles, such as free electrons, have been historically used to reveal the quantum structure of matter. However, realizing coherent interactions between free-electron beams and solid-state quantum systems has remained out of reach, owing to their intrinsically weak coupling. Realizing such coherent control would open up opportunities for hybrid quantum platforms combining free electrons and solid-state qubits for coincident quantum information processing and nanoscale sensing. Here, we present a framework that employs negatively charged nitrogen-vacancy centers (NV-) in diamond as quantum sensors of a bunched electron beam. We develop a Lindblad master equation description of the magnetic free-electron--qubit interactions and identify spin relaxometry as a sensitive probe of the interaction. Experimentally, we integrate a confocal fluorescence microscopy setup into a microwave-bunched electron beam line. We monitor charge-state dynamics and assess their impact on key sensing performance metrics (such as spin readout contrast), defining safe operating parameters for quantum sensing experiments. By performing T1T_1T1​ relaxometry under controlled electron beam exposure, we establish an upper bound on the free-electron--spin coupling strength. Our results establish NV- centers as quantitative probes of free electrons, providing a metrological benchmark for free-electron--qubit coupling under realistic conditions, and chart a route toward solid-state quantum control with electron beams.
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.
Quantum sensors encompass a diverse class of devices that exploit quantum coherence to detect weak or nanoscale signals. As their behavior is tied to physical constants, quantum sensors can achieve accuracy, repeatability, and precision approaching fundamental limits [1, 2]. As a result, these sensors have shown utility in a wide range of applications in both science and engineering leading to innovations. Among many solid-state spin systems, nitrogen-vacancy (NV) centers in diamonds have attracted considerable attention as a leading platform in many fields of quantum technologies, from quantum sensing to information processing and communication applications. They have superior physical properties, and their quantum coherence is preserved even at room temperature. The energy levels of NV centers are sensitive to magnetic fields, electric fields, strain, and temperature, and the spatial resolution is scalable from nanometers to millimeters. Therefore, diamond quantum sensors are distinctive sensors with multimodality and span scalable application fields. To realize an ideal quantum sensor for applications, the technical challenges in the sensor materials and the quantum control techniques, such as coherent microwave spin manipulation, effective optical spin-state initialization, and readout, have been developed. This chapter briefly explains the sensing principle using NV centers and then introduces sensor systems for biomedical applications, and monitoring of batteries for electric vehicles and internal power devices.
This thesis investigates the theoretical foundations, material properties, and experimental realization of quantum sensors based on the Nitrogen-Vacancy (NV) centers in diamond, a solid-state system that combines quantum coherence with room-temperature operability. The first chapter introduces the principles of quantum sensing, outlining the fundamental definitions, operating protocols, and physical processes underlying the quantum measurement paradigm. Emphasis is placed on the quantum sensing Hamiltonian and the distinction between various classes of quantum sensors. The second chapter focuses on diamond as a host material and on the NV center as a quantum defect. The electronic structure, optical transitions, and spin properties of the NV center are analyzed in detail. Several techniques of NV-based magnetometry are presented, including continuouswave and pulsed optically detected magnetic resonance (ODMR). The discussion also addresses coherence times (T1, T2, and T∗2 ) and methods of diamond synthesis together with NV-center generation through irradiation and annealing. Chapter three develops the physical theory describing the NV center. The Hamiltonian formalism includes spin-spin, hyperfine, and quadrupolar interactions, as well as couplings to external magnetic fields. The chapter further introduces the Bloch sphere representation, magnetic resonance phenomena, and models of lightmatter interaction, ranging from the semiclassical to the fully quantum Rabi framework. A seven-level rate-equation model is proposed to capture the spin dynamics and optical cycling processes of the NV center. The fourth chapter reports the experimental results. After describing materials and methods, several ODMR-based vector magnetometry experiments are presented, highlighting different spectral regimes and the dependence of resonance features on the external magnetic field geometry. Additional studies demonstrate temperature sensing and microwave-free magnetometry techniques for mapping magnetic field distributions. Sensitivity analysis and calibration procedures are also discussed.
As a demand from developing nanotechnology and quantum information technology based on mesoscopic material, quantum sensors with better spatial resolution and sensitivity are required. \n \nHowever, few material meets the requirements of nanoscale sensors including stability and small size. Single spin of Nitrogen-Vacancy(NV) centers in diamond crystal is one kind of the ideal quantum sensors for magnetometry that has been investigated in recent years. It provides a potential way to study the dynamics in a mesoscopic system with high sensitivity at room temperature. This thesis proposes a theoretical method to realize spin interaction detection based on NV centers on an atomic force-microscopy(AFM) tip. To realize this method, a robust control on NV centers and target electron spins at zero magnetic field is necessary. A pulse control technique for NV centers is proposed to realize transitions between two degenerate states at zero magnetic field, which is an important part of the sensing method. The key to realizing this transition is a circularly polarized microwave pulse generated by two parallel wires. Combined with optimal control techniques, this pulse can achieve a gate fidelity over 99.95% theoretically.