Engineering and Probing a One-Dimensional Dipolar Spin Ensemble in Diamond
Lingjie Chen, Shreyas Parthasarathy, Simon A. Meynell, Lillian B. Hughes Wyatt, Eveline Postelnicu, Haopu Yang, Zilin Wang, Weijie Wu, Winston V. Peloso, Casey K. Kim, Chris R. Laumann, Kunal Mukherjee, Norman Y. Yao, Ania C. Bleszynski Jayich
quant-phcond-mat.mes-hallcond-mat.mtrl-sciSubmitted Sep 16, 2026• Announced Sep 18, 2026• 0 citations
Dimensionality plays a central role in determining the collective behavior of interacting quantum systems. Engineering strongly interacting ensembles of solid-state spin defects in reduced dimensions remains a significant challenge at the interface between the applied and fundamental sciences. Here, we create and characterize a positionally disordered, quasi-one-dimensional spin chain in diamond, consisting of optically dark substitutional nitrogen defects (P1 centers) and optically addressable probe nitrogen-vacancy (NV) centers. Our approach exploits the preferential incorporation of nitrogen along step bunches formed during chemical vapor deposition to achieve both lateral and vertical confinement. Combining spatially resolved materials characterization with nanoscale quantum sensing, we establish the one-dimensional character of the optically dark, unpolarized P1 spin ensemble. We then use correlation spectroscopy to probe local spin autocorrelations and investigate infinite-temperature dipolar spin transport. Our results establish a materials-based route for engineering low-dimensional quantum spin systems.
Dimensionality plays a central role in determining the collective behavior of interacting quantum systems. Engineering strongly interacting ensembles of solid-state spin defects in reduced dimensions remains a significant challenge at the interface between the applied and fundamental sciences. Here, we create and characterize a positionally disordered, quasi-one-dimensional spin chain in diamond, consisting of optically dark substitutional nitrogen defects (P1 centers) and optically addressable probe nitrogen-vacancy (NV) centers. Our approach exploits the preferential incorporation of nitrogen along step bunches formed during chemical vapor deposition to achieve both lateral and vertical confinement. Combining spatially resolved materials characterization with nanoscale quantum sensing, we establish the one-dimensional character of the optically dark, unpolarized P1 spin ensemble. We then use correlation spectroscopy to probe local spin autocorrelations and investigate infinite-temperature dipolar spin transport. Our results establish a materials-based route for engineering low-dimensional quantum spin systems.
Systems of spins engineered with tunable density and reduced dimensionality enable a number of advancements in quantum sensing and simulation. Defects in diamond, such as nitrogen-vacancy (NV) centers and substitutional nitrogen (P1 centers), are particularly promising solid-state platforms to explore. However, the ability to controllably create coherent, two-dimensional spin systems and characterize their properties, such as density, depth confinement, and coherence, is an outstanding materials challenge. We present a refined approach to engineer dense (≳1 ppm ⋅ nm), 2D nitrogen, and NV layers in diamond using delta-doping during plasma-enhanced chemical vapor deposition epitaxial growth. We employ both traditional materials techniques, e.g., secondary ion mass spectrometry, alongside NV spin decoherence-based measurements to characterize the density and dimensionality of the P1 and NV layers. We find P1 densities of 5–10 ppm ⋅ nm, NV densities between 1 and 3.5 ppm ⋅ nm tuned via electron irradiation dosage, and depth confinement of the spin layer down to 1.6 nm. We also observe high (up to 0.74) ratios of NV to P1 centers and reproducibly long NV coherence times, dominated by dipolar interactions with the engineered P1 and NV spin baths.
Harnessing dipolar spin environments as controllable quantum resources is a central challenge in solid-state quantum technologies. Here, we report the observation of a coherent mesoscopic spin state in a disordered ensemble of substitutional nitrogen (P1) centers in diamond. An iterative Hartmann-Hahn protocol transfers polarization from dense nitrogen-vacancy (NV) centers to a P1 ensemble, yielding a 740-fold enhancement over room-temperature thermal equilibrium as revealed by differential readout. The resulting mesoscopic P1 spin ensemble exhibits collective Rabi oscillations and long-lived spin-lock and Hahn-echo coherences. We identify a crossover in the saturation polarization arising from the competition between coherent driving and local disorder, providing a quantitative measure of the system's intrinsic disorder. These results establish a foundation for utilizing dark electron spin ensembles as robust resources for quantum sensing and quantum many-body simulation.
The most direct approach for characterizing the quantum dynamics of a strongly-interacting system is to measure the time-evolution of its full many-body state. Despite the conceptual simplicity of this approach, it quickly becomes intractable as the system size grows. An alternate framework is to think of the many-body dynamics as generating noise, which can be measured by the decoherence of a probe qubit. Our work centers on the following question: What can the decoherence dynamics of such a probe tell us about the many-body system? In particular, we utilize optically addressable probe spins to experimentally characterize both static and dynamical properties of strongly-interacting magnetic dipoles. Our experimental platform consists of two types of spin defects in diamond: nitrogen-vacancy (NV) color centers (probe spins) and substitutional nitrogen impurities (many-body system). We demonstrate that signatures of the many-body system's dimensionality, dynamics, and disorder are naturally encoded in the functional form of the NV's decoherence profile. Leveraging these insights, we directly characterize the two-dimensional nature of a nitrogen delta-doped diamond sample. In addition, we explore two distinct facets of the many-body dynamics: First, we address a persistent debate about the microscopic nature of spin dynamics in strongly-interacting dipolar systems. Second, we demonstrate direct control over the spectral properties of the many-body system, including its correlation time. Our work opens the door to new directions in both quantum sensing and simulation.
Solid-state spin defects, particularly the nitrogen-vacancy (NV) center in diamond, have emerged as powerful platforms for exploring quantum many-body physics and quantum metrology. Their exceptional coherence properties and strong dipolar interactions offer unique opportunities to simulate complex quantum dynamics and engineer entangled states for enhanced sensing beyond the standard quantum limit. However, achieving scalable entanglement in these systems is notoriously difficult due to intrinsic disorder and the complex nature of long-range dipole-dipole interactions. This thesis presents both theoretical and experimental advancements in harnessing quantum dynamics in interacting spin ensembles for quantum-enhanced metrology. A central result is the experimental realization of spin squeezing in a dense ensemble of NV centers, demonstrating a clear path toward overcoming classical limits in solid-state platforms. To further formalize and scale these phenomena, this work develops theoretical frameworks for generating robust spin squeezing under realistic experimental conditions. We show that finite-temperature easy-plane magnetism can be actively leveraged to create scalable squeezed states for the dipolar spin systems on regular lattices. Building upon this, we further extend the result to spatially disordered quantum dipoles. We demonstrate that strongly coupled spin pairs suppress squeezing through dynamical heating, and we propose a selective shelving protocol to mitigate this problem. Furthermore, we also propose a universal protocol for quantum-enhanced sensing that exploits information scrambling, utilizing the natural, scrambling dynamics of strongly interacting many-body systems to effectively amplify weak external signals. Together, the findings detailed in this thesis establish a foundational paradigm for controlling and utilizing solid-state spin ensembles, paving the way for entanglement-enhanced quantum sensors.
Ensembles of nitrogen-vacancy (NV) centers in diamond are versatile quantum sensors with broad applications in the physical and life sciences. The concentration of neutral substitutional nitrogen ( [ N s 0 ]) strongly influences NV electronic spin coherence times, sensitivity, and optimal sensing strategies. Diamonds with [ N s 0 ] ∼ 1–10 ppm are a focus of recent material engineering efforts, with higher concentrations being favorable for continuous-wave optically detected magnetic resonance (CW-ODMR) and lower concentrations expected to benefit pulsed magnetometry techniques through extended NV spin coherence times and improved sensing duty cycles. In this work, we synthesize and characterize low- [ N s 0 ] ( ∼ 0.8 ppm), NV-enriched diamond material, engineered through low-strain chemical vapor deposition (CVD) growth on high-quality substrates, 12 C isotopic purification, and controlled electron irradiation and annealing. Our results demonstrate good strain homogeneity in diamonds grown on CVD substrates and spin-bath-limited NV dephasing times. By measuring NV spin and charge properties across a wide range of optical NV excitation intensity, we provide direct comparisons of photon-shot-noise-limited magnetic field sensitivity between the current low- [ N s 0 ] and previously studied higher- [ N s 0 ] ( ∼ 14 ppm) NV-diamond sensors. We show that low- [ N s 0 ] diamond can outperform higher- [ N s 0 ] diamond at moderate and low optical NV excitation intensity. Our results provide practical benchmarks and guidance for selecting NV-diamond sensors tailored to specific experimental constraints and sensing requirements.
The most direct approach for characterizing the quantum dynamics of a strongly interacting system is to measure the time evolution of its full many-body state. Despite the conceptual simplicity of this approach, it quickly becomes intractable as the system size grows. An alternate approach is to think of the many-body dynamics as generating noise, which can be measured by the decoherence of a probe qubit. Here we investigate what the decoherence dynamics of such a probe tells us about the many-body system. In particular, we utilize optically addressable probe spins to experimentally characterize both static and dynamical properties of strongly interacting magnetic dipoles. Our experimental platform consists of two types of spin defects in nitrogen delta-doped diamond: nitrogen-vacancy colour centres, which we use as probe spins, and a many-body ensemble of substitutional nitrogen impurities. We demonstrate that the many-body system's dimensionality, dynamics and disorder are naturally encoded in the probe spins' decoherence profile. Furthermore, we obtain direct control over the spectral properties of the many-body system, with potential applications in quantum sensing and simulation.