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.
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.
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.
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.
Abstract Nitrogen-vacancy (NV) centers in diamond have been developed into essential hardware units for a wide range of solid-state-based quantum technology applications. While such applications require the long spin coherence times of the NV centers, they are often limited due to decoherence. In this study, we theoretically investigate the decoherence of NV-spin ensembles induced by nitrogen impurities (P1 centers), which are one of the most dominant and inevitable magnetic field noise sources in diamond. We combined cluster correlation expansion and density functional theory to compute the Hahn-echo spin-coherence time of the NV centers for a broad range of P1 concentrations. Results indicate a clear linear dependence of T2 on P1 concentrations on a log scale with a slope of −1.06, which is in excellent agreement with previous experimental results. The interplay between the Jahn–Teller effect and the hyperfine interaction in the P1 center plays a critical role in determining the bath dynamics and the resulting NV decoherence. Our results provide a theoretical upper bound for the NV-spin T2 over a wide range of P1 densities, serving as a key reference for materials optimization and spin bath characterization to develop highly coherent NV-based devices for quantum information technology.
Under ambient conditions, spin impurities in solid-state systems are found in thermally mixed states and are optically "dark"; i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright"; i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a scheme to resonantly couple bright NV electronic spins to dark substitutional-nitrogen (P1) electronic spins by dressing their spin states with oscillating magnetic fields. This resonant coupling mechanism can be used to transfer spin polarization from NV spins to nearby dark spins and could be used to cool a mesoscopic bath of dark spins to near-zero temperature, thus providing a resource for quantum information and sensing, and aiding studies of quantum effects in many-body spin systems.
Under ambient conditions, spin impurities in solid-state systems are found in thermally-mixed states and are optically "dark", i.e., the spin states cannot be optically controlled. Nitrogen-vacancy (NV) centers in diamond are an exception in that the electronic spin states are "bright", i.e., they can be polarized by optical pumping, coherently manipulated with spin-resonance techniques, and read out optically, all at room temperature. Here we demonstrate a dressed-state, double-resonance scheme to transfer polarization from bright NV electronic spins to dark substitutional-Nitrogen (P1) electronic spins in diamond. This polarization-transfer mechanism could be used to cool a mesoscopic bath of dark spins to near-zero temperature, thus providing a resource for quantum information and sensing, and aiding studies of quantum effects in many-body 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.