arXiv subjects

Fazhan Shi

Publications and source records attributed to Fazhan Shi.

At least 19 recordsLinked to original sources

arXiv2026

Molecular chiral discrimination through symmetry-breaking spin dynamics

Molecular chirality plays a crucial role in physics, chemistry, life sciences and pharmacology. Nowadays, the chiral discrimination and control at the single-molecule level is urgently needed to reveal the origin of the chirality-relevant phenomena by recovering the information disturbed by the ensemble averaging. The method of magnetic resonance (MR), as one of powerful tools for structure analysis, is blind to the molecular chirality in the absence of a chiral reagent. Here we propose and experimentally demonstrate a direct MR-based method for determining the chirality at the single-molecule level through constructing the symmetry-breaking dynamics of nearby nuclear spins. In principle, the mirror asymmetry of two enantiomers in real space is manifested by breaking the joint symmetry of the mirror reflection and time reversal in spin space under spin dynamics. Experimentally, two enantiomers are indistinguishable from the dynamics of strongly-coupled but unpolarized nuclear spins, but diverge evidently in the dynamical results that break the field-inversion symmetry after spins are polarized. Our method and results will benefit the study of chirality-induced properties in the fields of chemistry and biology.

quant-ph↗

arXiv2026

Removing inhomogeneous broadening in cross-relaxation spectra via hole burning

Quantum relaxometry based on nitrogen-vacancy (NV) centers in diamond is an easy-to-use technique that detects magnetic noise by measuring the longitudinal relaxation of NV centers. It is favored in chemical and biological applications due to the robustness against imperfect spin control. By tuning the energy level, NV relaxometry can detect magnetic noise generated by other spins and obtain magnetic resonance spectra through cross relaxation. However, the inhomogeneous broadening of NV centers greatly limits the spectral resolution of cross-relaxation spectra. Here we demonstrate a hole-burning technique to remove the inhomogeneous broadening. We utilize a weak pump field to deplete specific NV centers during the relaxation measurement, which contribute a reverse signal in the cross-relaxation spectra with a much narrower linewidth. Our method retains the convenience and sensitivity of NV relaxometry, opening up new avenues for high-resolution magnetic resonance spectroscopy in complex scenarios.

quant-ph↗

arXiv2026

Spin-based magnetic detection of optically trapped single cell in microfluidic channel

Combining optical tweezers with fluorescence microscopy is a powerful tool for single-cell analysis, playing a pivotal role in disease diagnosis, cell sorting, and the investigation of cellular dynamics. However, fluorescence detection faces challenges such as blinking, photobleaching and autofluorescence in biotissues. To address these limitations, we developed a magnetic detection strategy by integrating quantum magnetometry using nitrogen-vacancy centers into optical tweezers, demonstrating precise trapping and manipulation of individual cells in microfluidic environment. We detected a magnetic signal of 89 {\mu}T from a single cell labeled with magnetic nanoparticles, compared to a noise floor of 3.9 {\mu}T observed in unlabeled cells. This platform provides a promising approach for high-precision single-cell analysis and holds significant potential for probing cellular activities within biological microenvironments.

physics.optics↗

arXiv2026

Sub-nanometer resolution of the nitrogen-vacancy center by Fourier magnetic imaging

Solid-state spins in diamond are promising building blocks for quantum computing and quantum sensing, both of which require precise nanoscale addressing of individual spins. To explore the resolution limit of this approach, we demonstrate Fourier magnetic imaging of nitrogen-vacancy centers in diamond under state-of-the-art conditions. We constructed a highly compact experimental platform featuring thermal drift compensation under ambient conditions and generated a pulsed magnetic field gradient of up to 13.5 G/$\mu$m. By implementing the Fourier magnetic imaging protocol, we achieved localization of a single nitrogen-vacancy center with a spatial resolution of 0.28 $\pm$ 0.10 nm and a magnetic field measurement deviation of 9 nT. This technique holds potential for applications such as localizing spins within proteins and cells.

quant-ph↗

arXiv2025

Quantum Noise Spectroscopy of Nanoscale Charge Defects in Silicon Carbide at Room Temperature

The nanoscale charge environment critically influences semiconductor physics and device performance. While conventional bulk characterization techniques provide volume-averaged defect properties, they lack the spatial resolution to resolve nanoscale charge heterogeneity and identify microscopic noise sources. Here, we utilize single PL5 centers in 4H-SiC as room-temperature broadband quantum sensors to fill in the gap. We report the first real-time, nanoscale observation of singlecharge tunneling dynamics in a commercial semiconductor at room temperature, by monitoring the random telegraph noise using optically detected magnetic resonance (ODMR). This capability enables an electrical noise imaging technique, showing distinct noise variations across different wafer substrates. By employing dynamical decoupling, we extend noise spectroscopy from near-DC to MHz frequencies, uncovering significant noise spectral density correlations across frequency bands. Finally, we probe MHz-GHz noise and identify its origin via T1 relaxation spectroscopy, obtaining the first nanoscale electron paramagnetic resonance (EPR) spectroscopic fingerprint of charge defects in SiC. These techniques open avenues for characterizing noise environments in semiconductor devices, providing critical insights for optimizing SiC fabrication processes, defect control, and advancing quantum technologies.

quant-ph↗

arXiv2025

Double-Layered Silica-Engineered Fluorescent Nanodiamonds for Catalytic Generation and Quantum Sensing of Active Radicals

Fluorescent nanodiamonds (FNDs) hosting nitrogen-vacancy (NV) centers have attracted considerable attention for quantum sensing applications, particularly owing to notable advancements achieved in the field of weak magnetic signal detection in recent years. Here, we report a practical quantum-sensing platform for the controlled production and real-time monitoring of ultra-short-lived reactive free radicals using a double-layered silica modification strategy. An inner dense silica layer preserves the intrinsic properties of NV centers, while an outer porous silica layer facilitates efficient adsorption and stabilization of hydroxyl radicals and their precursor reactants. By doping this mesoporous shell with gadolinium (III) catalysts, we achieve sustained, light-free generation of hydroxyl radicals via catalytic water splitting, eliminating reliance on external precursors. The mechanism underlying this efficient radical generation is discussed in detail. The radical production is monitored in real time and in situ through spin-dependent T1 relaxometry of the NV centers, demonstrating stable and tunable radical fluxes, with concentration tunable across a continuous range from approximately 100 mM to molar levels by adjusting the catalyst condition. This study extends the technical application of nanodiamonds from relaxation sensing to the controlled synthesis of reactive free radicals, thereby providing robust experimental evidence to support the advancement of quantum sensing systems in intelligent manufacturing.

quant-ph↗

arXiv2025

Single-molecule Scale Nuclear Magnetic Resonance Spectroscopy using a Robust Near-Infrared Spin Sensor

Nuclear magnetic resonance (NMR) at the single-molecule level with atomic resolution holds transformative potential for structural biology and surface chemistry. Near-surface solid-state spin sensors with optical readout ability offer a promising pathway toward this goal. However, their extreme proximity to target molecules demands exceptional robustness against surface-induced perturbations. Furthermore, life science applications require these sensors to operate in biocompatible spectral ranges that minimize photodamage. In this work, we demonstrate that the PL6 quantum defect in 4H silicon carbide (4H-SiC) can serve as a robust near-infrared spin sensor. This sensor operates at tissue-transparent wavelengths and exhibits exceptional near-surface stability even at depth of 2 nm. Using shallow PL6 centers, we achieve nanoscale NMR detection of proton ($\mathrm{^{1}H}$) spins in immersion oil and fluorine ($\mathrm{^{19}F}$) spins in Fomblin, attaining a detection volume of $\mathrm{(3~nm)^3}$ and a sensitivity reaching the requirement for single-proton spin detection. This work establishes 4H-SiC quantum sensors as a compelling platform for nanoscale magnetic resonance, with promising applications in probing low-dimensional water phases, protein folding dynamics, and molecular interactions.

quant-ph↗

arXiv2025

Quantum relaxometry for detecting biomolecular interactions with single NV centers

The investigation of biomolecular interactions at the single-molecule level has emerged as a pivotal research area in life science, particularly through optical, mechanical, and electrochemical approaches. Spins existing widely in biological systems, offer a unique degree of freedom for detecting such interactions. However, most previous studies have been largely confined to ensemble-level detection in the spin degree. Here, we developed a molecular interaction analysis method approaching single-molecule level based on relaxometry using the quantum sensor, nitrogen-vacancy (NV) center in diamond. Experiments utilized an optimized diamond surface functionalized with a polyethylenimine nanogel layer, achieving $\sim$10 nm average protein distance and mitigating interfacial steric hindrance. Then we measured the strong interaction between streptavidin and spin-labeled biotin complexes, as well as the weak interaction between bovine serum albumin and biotin complexes, at both the micrometer scale and nanoscale. For the micrometer-scale measurements using ensemble NV centers, we re-examined the often-neglected fast relaxation component and proposed a relaxation rate evaluation method, substantially enhancing the measurement sensitivity. Furthermore, we achieved nanoscale detection approaching single-molecule level using single NV centers. This methodology holds promise for applications in molecular screening, identification and kinetic studies at the single-molecule level, offering critical insights into molecular function and activity mechanisms.

quant-ph↗

arXiv2025

Subcellular Metabolic Tracking Using Fluorescent Nanodiamonds Relaxometry

Fluorescent nanodiamonds (FNDs) relaxometry holds promising future for advancement of high spatiotemporal resolution metabolic imaging technology. In this study, we demonstrate a simultaneous integration of spatial position tracking with FND relaxometry to characterize the temporal dynamics of metabolic processes, thereby enhancing the capability to monitor cellular activities over time. To enable targeted metabolic probing in living cells, FNDs were surface-functionalized to achieve specific localization within key organelles, including the nucleus and mitochondria. This strategy not only facilitates subcellular-level metabolic monitoring but also allows for direct comparison between intra- and extranuclear microenvironments within the same living cell, offering substantial potential for elucidating the spatial and functional heterogeneity of cellular metabolism.

physics.bio-ph↗

arXiv2025

Parallel accelerated electron paramagnetic resonance spectroscopy using diamond sensors

The nitrogen-vacancy (NV) center can serve as a magnetic sensor for electron paramagnetic resonance (EPR) measurements. Benefiting from its atomic size, the diamond chip can integrate a tremendous amount of NV centers to improve the magnetic-field sensitivity. However, EPR spectroscopy using NV ensembles is less efficient due to inhomogeneities in both sensors and targets. Spectral line broadening induced by ensemble averaging is even detrimental to spectroscopy. Here we show a kind of cross-relaxation EPR spectroscopy at zero field, where the sensor is tuned by an amplitude-modulated control field to match the target. The modulation makes detection robust to the sensor's inhomogeneity, while zero-field EPR is naturally robust to the target's inhomogeneity. We demonstrate an efficient EPR measurement on an ensemble of roughly 30000 NV centers. Our method shows the ability to not only acquire unambiguous EPR spectra of free radicals, but also monitor their spectroscopic dynamics in real time.

quant-ph↗

arXiv2025

Single-cell identification with quantum-enhanced nuclear magnetic resonance

Identification of individual cells within heterogeneous populations is essential for biomedical research and clinical diagnostics. Conventional labeling-based sorting methods, such as fluorescence-activated cell sorting and magnetic-activated cell sorting, enable precise sorting when reliable markers are available. However, their applicability is limited in cells lacking defined markers or sensitive to labeling, as labeling can compromise cellular viability and function. We present a single-cell identification approach using quantum-enhanced NMR with diamond nitrogen-vacancy centers for label-free detection of intracellular proton ($^1$H) signals. Using this method, we distinguish two human tumor cell lines by their proton spin-lattice ($T_1$) relaxation times, which serve as a cell-intrinsic physicochemical signature. It lays the groundwork for label-free sorting applications in rare cell analysis, personalized medicine, and single-cell diagnostics.

quant-ph↗

arXiv2025

Scalable quantum error mitigation for dynamical decoupling

Quantum coherence remains a fundamental challenge for advancing quantum technologies. Although dynamical decoupling can suppress decoherence noise, it frequently misestimates decoherence times due to control errors -- a previously underappreciated issue. Here, we present Hadamard phase cycling, a scalable non-Markovian quantum error mitigation method using group-structured phase configurations to filter spurious dynamics. Validated across molecular electron spins, nitrogen-vacancy centers in diamond, nuclear spins, trapped ions, and superconducting qubits, this technique enables accurate decoherence time characterization and enhanced state fidelity with linear complexity. Our results indicate that many reported ultralong decoherence times stem from artifacts like coherence-population mixing rather than genuine noise suppression. By ensuring dynamical authenticity, Hadamard phase cycling establishes a robust framework for reliable quantum control, paving the way for reassessment and advancement of coherence benchmarks in the NISQ era.

quant-ph↗

arXiv2025

Entanglement-Enhanced Nanoscale Single-Spin Sensing

Detecting individual spins--including stable and metastable states--represents a fundamental challenge in quantum sensing with broad applications across condensed matter physics, quantum chemistry, and single-molecule magnetic resonance imaging. While nitrogen-vacancy (NV) centers in diamond have emerged as powerful nanoscale sensors, their performance for single-spin detection remains constrained by substantial environmental noise and restricted sensing volume. Here, we propose and demonstrate an entanglement-enhanced sensing protocol that overcomes these limitations through the strategic use of entangled NV pairs. Our approach achieves a 3.4-fold enhancement in sensitivity and a 1.6-fold reduction in spatial resolution relative to single NV centers under ambient conditions. The protocol employs carefully engineered entangled states that amplify target spin signals through quantum interference while suppressing environmental noise. Crucially, we extend these capabilities to resolve metastable single-spin dynamics, directly observing stochastic transitions between different spin states by identifying state-dependent coupling strengths. This dual functionality enables simultaneous detection of static and dynamic spin species for studying complex quantum systems. The achieved performance establishes entanglement-enhanced sensing as a viable pathway toward atomic-scale characterization of quantum materials and interface.

quant-ph↗

arXiv2025

Room-temperature hybrid 2D-3D quantum spin system for enhanced magnetic sensing and many-body dynamics

Advances in hybrid quantum systems and their precise control are pivotal for developing advanced quantum technologies. Two-dimensional (2D) materials with optically accessible spin defects have emerged as a promising platform for building integrated quantum spin systems due to their exceptional flexibility and scalability. However, experimentally realizing such systems and demonstrating their superiority remains challenging. Here, we present a hybrid spin system operating under ambient conditions, integrating boron vacancy (V_B^-) spins in 2D hexagonal boron nitride flakes with a single nitrogen vacancy (NV) center in 3D single-crystal diamonds. This combined system achieves full controllability and exhibits enhanced performance for nanoscale magnetic sensing, including an improved dynamic range. Moreover, we investigate the rich many-body spin dynamics within the hybrid system, which enables us to estimate the concentration of V_B^- spins. This work provides a critical foundation for advancing the development of 2D-3D integrated quantum spin systems.

quant-ph↗

arXiv2025

Oxygen-vacancy quantum spin defects in silicon carbide

Optically addressable spin defects in wide-bandgap semiconductors are promising building blocks for quantum sensing and quantum networks. Establishing their atomic structure is essential for understanding functionality and enabling controlled engineering. In 4H-SiC, the PL5 and PL6 centers have long been recognized for their exceptional charge stability and room-temperature optically detected magnetic resonance (ODMR) performance, but their structural origin has remained elusive for over a decade. Here, we provide direct evidence for their oxygen-vacancy (${\rm O_C V_{Si}}$) origins through a combined chemical and isotopic control strategy. Under oxygen ion implantation, we observe over tenfold enhancement in the yield of PL5 and PL6 compared to nitrogen ion implantation. Furthermore, implantation with $^{17}{\rm O}$ ions produces PL5 and PL6 defects that exhibit a characteristic six-fold $^{17}{\rm O}$ hyperfine splitting in their ODMR spectra. These results affirm PL6 as the ${\rm O_C V_{Si}}$ defect in the $hh$ configuration. For PL5, the oxygen-related evidence, together with \textit{ab initio} calculations and additional measurements of the zero-field splitting and hyperfine structure, establishes it as the ${\rm O_C V_{Si}}$ defect in the $kh$ configuration. This unambiguous structural identification, achieved through materials-level chemical control, provides the microscopic foundation for deterministic engineering of these defects, paving the way for scalable photonic devices and high-sensitivity ensemble quantum sensors based on oxygen-vacancy centers.

cond-mat.mtrl-sci↗

arXiv2025

Single-molecule Scale Magnetic Resonance Spectroscopy using Nitrogen-Vacancy Centers in Diamond

Single-molecule technology stands as a powerful tool, enabling the characterization of intricate structural and dynamic information that would otherwise remain concealed within the averaged behaviors of numerous molecules. This technology finds extensive application across diverse fields including physics, chemistry, biology, and medicine. Quantum sensing, particularly leveraging nitrogen-vacancy (NV) centers within diamond structures, presents a promising avenue for single-molecule magnetic resonance, offering prospects for sensing and imaging technology at the single-molecule level. Notably, while significant strides have been made in single-molecule scale magnetic resonance using NV centers over the past two decades, current approaches still exhibit limitations in magnetic sensitivity, spectral resolution, and spatial resolution. Particularly, the full reconstruction of three-dimensional positions of nuclear spins within single molecules remains an unattained goal. This review provides a comprehensive overview of the current state-of-the-art in single-molecule scale magnetic resonance, encompassing an analysis of various relevant techniques involving NV centers. Additionally, it explores the optimization of technical parameters associated with these methods. This detailed analysis serves as a foundation for the development of new technologies and the exploration of potential applications.

quant-ph↗

arXiv2024

Discovery of an anomalous non-evaporating sub-nanometre water layer in open environment

Water exhibits complex behaviors as a result of hydrogen bonding, and low-dimensional confined water plays a key role in material science, geology, and biology science. Conventional techniques like STM, TEM, and AFM enable atomic-scale observations but face limitations under ambient conditions and surface topographies. NV center magnetic resonance technology provides an opportunity to overcome these limitations, offering non-contact atomic-scale measurements with chemical resolution capability. In this study, a nanoscale layer dissection method was developed utilizing NV center technology to analyze water layers with diverse physicochemical properties. It unveiled the presence of a non-evaporating sub-nanometer water layer on a diamond surface under ambient conditions. This layer demonstrated impervious to atmospheric water vapor and exhibited unique electronic transport mediated via hydrogen bonding. These findings provide new perspectives and a platform for studying the structure and behavior of low-dimensional water, as well as the surface properties influenced by adsorbed water under native conditions.

cond-mat.mtrl-sci↗

arXiv2024

Spin-wave frequency multiplication by magnetic vortex cores

Frequency multiplication involves generating harmonics from an input frequency, a technique particularly useful for integrating spin-wave devices operating at different frequencies. While topological magnetic textures offer distinct advantages in spin-wave applications, frequency multiplication has not yet been observed in these structures. Here, we study the magnetization dynamics of magnetic vortices formed in micron-sized disks and squares via wide-field magnetic imaging. We found the occurrence of coherent spin-wave harmonics arising from the gyration of vortex cores driven by microwave fields. This phenomenon reveals a universal mechanism where the periodical motion of delta function-like objects such as vortex cores gives rise to a frequency comb. Our results pave the way for creating nanoscale, tunable spin-based frequency multipliers and open new possibilities for frequency comb generation in a variety of systems.

cond-mat.mes-hall↗