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arXiv:2604.25660

Nanoscale Sensing of Solid-State Samples with High Frequency Resolution

P. Alsina-Bolívar, I. Iriarte-Zendoia, D. B. Bucher, J. Casanova

quant-phSubmitted Apr 28, 2026• Announced Apr 29, 2026• 0 citations• Revised Apr 29, 2026 (v2)
v1 · Apr 28, 2026v2 · Apr 29, 2026
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Abstract

To meet the growing demand for nanoscale surface analysis, nitrogen-vacancy (NV) centers offer a high-sensitivity alternative by leveraging their ability to operate in immediate proximity to the sample. In this work, we propose a quantum control protocol designed to overcome the inherent challenges of solid-state environments, specifically by mitigating anisotropy and strong dipole-dipole interactions to enable the detection of isotropic chemical shifts at the nanoscale. To achieve this, our scheme synchronizes a slowly rotating magnetic field with tailored RF decoupling and MW control of the NV sensors. We provide an analytical mapping that explicitly links the measured spectrum to the control sequence features and the underlying system parameters, enabling a straightforward characterization of the sample.

Comments
4 pages, 2 figures + Appendices

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To meet the growing demand for nanoscale surface analysis, nitrogen-vacancy (NV) centers offer a high-sensitivity alternative by leveraging their ability to operate in immediate proximity to the sample. In this work, we propose a quantum control protocol designed to overcome the inherent challenges of solid-state environments, specifically by mitigating anisotropy and strong dipole-dipole interactions to enable the detection of isotropic chemical shifts at the nanoscale. To achieve this, our scheme synchronizes a slowly rotating magnetic field with tailored RF decoupling and MW control of the NV sensors. We provide an analytical mapping that explicitly links the measured spectrum to the control sequence features and the underlying system parameters, enabling a straightforward characterization of the sample.
Magnetic field fluctuations on nanometer length scales manifest in a diverse range of phenomena -- electron and spin dynamics in materials and devices, quantum many-body systems, and molecular chemistry. Measuring these phenomena requires sensors with a challenging combination of broad spectral bandwidth, high sensitivity, and nanoscale spatial resolution. Nitrogen-vacancy (NV) centers, atom-like quantum sensors in diamond, possess the requisite sensitivity and nanoscale sensing volume, but are typically limited in bandwidth by the practical speed of the applied quantum control sequence. Here, we overcome this limitation by exposing the NV qubit to a microwave dressing field during a dynamical decoupling sequence, which both amplifies and frequency-mixes target signals at arbitrary frequencies into the detection band of the dynamical decoupling protocol. We demonstrate this approach by using NV centers to detect both coherent and noisy nanoscale spin wave dynamics in a magnetic yttrium-iron-garnet (YIG) thin film over a broad frequency range. Our technique generalizes to other qubit platforms, providing a versatile framework for nanoscale spectroscopy across diverse physical and chemical systems.
Diamond-based quantum sensors have enabled high-resolution NMR spectroscopy at the microscale in scenarios where fast molecular motion averages out dipolar interactions among target nuclei. However, in samples with low-diffusion, ubiquitous dipolar couplings challenge the extraction of relevant spectroscopic information. In this work we present a protocol that enables the scanning of nuclear spins in dipolarly-coupled samples at high magnetic fields with a sensor based on nitrogen vacancy (NV) ensembles. Our protocol is based on the synchronized delivery of radio frequency (RF) and microwave (MW) radiation to eliminate couplings among nuclei in the scanned sample and to efficiently extract target energy-shifts from the sample's magnetization dynamics. In addition, the method is designed to operate at high magnetic fields leading to a larger sample thermal polarization, thus to an increased NMR signal. The precision of our method is ultimately limited by the coherence time of the sample, allowing for accurate identification of relevant energy shifts in solid-state systems.
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.
We present a method relying on shortcuts to adiabaticity to achieve quantum detection of high-frequency signals at the nanoscale in a robust manner. More specifically, our protocol delivers tailored amplitudes and frequencies for control fields that, firstly, enable the coupling of the sensor with high-frequency signals and, secondly, minimize errors that would otherwise spoil the detection process. To exemplify the method, we particularize to detection of signals emitted by fast-rotating nuclear spins with nitrogen-vacancy-center quantum sensors. However, our protocol is straightforwardly applicable to other quantum devices such as silicon-vacancy centers, germanium-vacancy centers, or divacancies in silicon carbide.
Nitrogen vacancy (NV) centers in diamond are widely deployed as local magnetic sensors, using coherent, single qubit control to measure both time-averaged fields and noise with nanoscale spatial resolution. Moving beyond single qubits to multi-qubit control enables new sensing modalities such as measuring nonlocal spatiotemporal correlators, or using entangled states to improve measurement sensitivity. Here, we describe protocols to use optically unresolved NV center pairs and nuclear spins as multi-qubit sensors for measuring correlated noise, enabling covariance magnetometry at nanometer length scales. For NV centers that are optically unresolved but have spectrally resolved spin transitions, we implement a phase-cycling protocol that disambiguates magnetic correlations from variance fluctuations by alternating the relative spin orientations of the two NV centers. For NV centers that are both optically and spectrally unresolved, we leverage the presence of a third qubit, a 13C nucleus that is strongly coupled to one of the NV centers, to effect coherent single-NV spin flips and enable a similar phase-cycling protocol. For length scales around 10 nm, we create maximally entangled Bell states through dipole-dipole coupling between two NV centers, and use these entangled states to directly read out the magnetic field correlation, rather than reconstructing it from independent measurements of unentangled NV centers. Importantly, this changes the scaling of sensitivity with readout noise from quadratic to linear. For conventional off-resonant readout of the NV center spin state (for which the readout noise is roughly 30 times the quantum projection limit), this results in a dramatic sensitivity improvement. Finally, we demonstrate methods for the detection of high spatial- and temporal-resolution correlators with pairs of strongly interacting NV centers.
High spatial resolution quantum sensing of near-surface nitrogen vacancy (NV) centers in diamond has enabled detection of magnetic, electrical, and thermal signals at the nanoscale. At depths of just a few nanometers, NV centers serve as localized quantum probes for external spins or low-dimensional materials, but their proximity to the surface also enhances decoherence caused by fluctuating nuclear spins. While advances in surface engineering have stabilized the charge state of NV centers at depths of tens of nanometers, achieving both ultra-shallow implantation (0.5-2 nm) and long-term spin coherence remains a central challenge. In this work, we show using first-principles modeling that, by exploiting the interaction of surface-induced strain and weak dc magnetic fields, the spin coherence times of 1-nm-deep NV centers can be greatly improved near the spin-phonon-confined regime at room temperature in 12C-rich diamonds. We also demonstrate that this protocol benefits ~ 10-nm-deep NV centers in natural diamond, enabling vector magnetometry at the nanoscale. Shallow NV centers in diamond are advantageous for quantum sensing but suffer from surface magnetic noise. Using first-principles simulations supported by experiments, the authors show that a combination of small magnetic fields and surface strain can significantly enhance spin coherence of 1 nm-deep NV centers.