The study of open quantum systems, quantum thermodynamics and quantum many-body spin physics in realistic solid-state platforms, has been a long-standing goal in quantum and condensed-matter physics. In this talk I will address these topics through the platform of nitrogen-vacancy (NV) spins in diamond, in the context of purification (or cooling) of a spin bath as a quantum resource and for enhanced metrology. I will first describe a general theoretical framework we developed for Hamiltonian engineering in an interacting spin system [1]. I will then extend this framework to coupling of the spin ensemble to a spin bath, including both coherent and dissipative dynamics [2]. Using these tools I will present a scheme for efficient purification of the spin bath, surpassing the current state-of-the-art and providing a path toward applications in quantum technologies, such as enhanced MRI sensing.
The study of open quantum systems, quantum thermodynamics and quantum many-body spin physics in realistic solid-state platforms, has been a long-standing goal in quantum and condensed-matter physics. In this talk I will address these topics through the platform of nitrogen-vacancy (NV) spins in diamond, in the context of purification (or cooling) of a spin bath as a quantum resource and for enhanced metrology. I will first describe a general theoretical framework we developed for Hamiltonian engineering in an interacting spin system [1]. I will then extend this framework to coupling of the spin ensemble to a spin bath, including both coherent and dissipative dynamics [2]. Using these tools I will present a scheme for efficient purification of the spin bath, surpassing the current state-of-the-art and providing a path toward applications in quantum technologies, such as enhanced MRI sensing.
The study of quantum many-body spin physics in realistic solid-state platforms has been a long-standing goal in quantum and condensed-matter physics. We demonstrate separate steps required to reach this goal using nitrogen-vacancy (NV) centers in diamond. First, standard (TEM) electron irradiation is used for the enhancement of N to NV conversion efficiencies by over an order-of-magnitude. Second, robust pulsed and continuous dynamical decoupling (DD) techniques enable the preservation of arbitrary states of the ensemble. These combined efforts could lead to the desired interaction-dominated regime. Finally, we simulate the effects of continuous and pulsed microwave (MW) control on the resulting NV-NV many body dynamics in a realistic spin-bath environment. We emphasize that dominant interaction sources could be identified and decoupled by the application of proper pulse sequences, and the modification of such sequences could lead to the creation engineered interaction Hamiltonians. Such interaction Hamiltonians could pave the way toward the creation of non-classical states, e.g. spin-squeezed states, which were not yet demonstrated in the solid-state, and could eventually lead to magnetic sensing beyond the standard quantum limit (SQL).
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.
Improved control and manipulation of quantum systems lies at the heart of modern quantum science and technology, with broad applications ranging from quantum metrology to quantum information science and many-body physics. In this thesis, I will introduce a novel framework for robust Hamiltonian engineering in interacting spin systems, which enables the efficient design of Floquet engineering pulse sequences for qubit and qudit systems that out-perform state-of-the-art control methods by orders of magnitude. As applications of this framework, we utilize a high density ensemble of nitrogen vacancy (NV) centers in diamond, and demonstrate significantly improved control over the disordered, interacting many-body spin system. This enabled the first solid state spin ensemble quantum sensor operating beyond the sensitivity limit imposed by interactions between sensing particles, as well as the observation and understanding of novel dynamical many-body phenomena, including discrete time crystalline order and thermalization dynamics in long-range interacting XXZ spin models.
The studies of many-body dynamics of interacting spin ensembles, as well as quantum sensing in solid state systems, are often limited by the need for high spin concentrations, along with efficient decoupling of the spin ensemble from its environment. In particular, for an ensemble of nitrogen-vacancy (NV) centers in diamond, high conversion efficiencies between nitrogen (P1) defects and NV centers are essential while maintaining long coherence times of an NV ensemble. In this work, we study the effect of electron irradiation on the conversion efficiency and the coherence time of various types of diamond samples with different initial nitrogen concentrations. The samples were irradiated using a 200 keV transmission electron microscope. Our study reveals that the efficiency of NV creation strongly depends on the initial conversion efficiency and on the initial nitrogen concentration. The irradiation of the examined samples exhibits an order of magnitude improvement in the NV concentration (up to ∼1011 NV/cm2), without degradation in their coherence time of ∼180 μs. We address the potential of this technique toward the study of many-body physics of NV ensembles and the creation of non-classical spin states for quantum sensing.
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.
This dissertation investigates applications of the Nitrogen vacancy in diamond (NV). The NV is a unique quantum system allowing for optical polarization and read out even at ambient conditions. Its electron spin (S=1) has coherence times in the order of milliseconds and is therefore an ideal candidate to investigate the foundations of quantum mechanics as well as exploiting quantum effects in metrology and information processing applications. To utilize the NV for quantum technologies, first the interaction of the NV with its surroundings has to be investigated and controlled. Here dynamical decoupling sequences (CPMG) could be utilized to extend the NV coherence time to a few milliseconds by decoupling the NV from its surrounding spin bath (given by the 13C isotope, natural abundance 1.1%). But not only decoupling sequences can be used to suppress the spin bath interaction, also eigen state tailoring can suppress the bath interaction. As long as strain is the dominant interaction, the NV eigen energies are not susceptible to small magnetic field changes. Therefore the magnetic dipole interaction with the spin bath is suppressed. But the spin bath is not only a nuisance limiting NV coherence times, but also a potential resource for quantum technologies. In order to harness the individual 13C nuclear spins, their interaction with the NV and among themselves has to be investigated. To not be limited by the NV coherence times, a new spectroscopy method, only limited by the NV lifetime, was developed. This can in principle be extended to the second range by using a nuclear spin memory. First advances in quantum technology were demonstrated in the field of metrology, where the Zeeman effect of the NV center allowed for precise nanoscale measurement of magnetic fields. Here this concept was extended to us the Stark effect to detect electric fields. A sensitivity of η=142.6±3.6 V/(cmHz1/2) was demonstrated. This is equivalent to the detection of a single elemental charge at a distance of 150 nm in one second. By using two NVs with a distance of less then 20 nm, a demonstration of nanoscale single fundamental charge detection was feasible. Here one NV was used as a controllable fundamental charge while the other NV was used as sensor NV, detecting the electric field of the fundamental charge. This allowed for the detection of a single electronic charge at ambient conditions. Another keystone of quantum technology is the reliable on demand or heralded creation of entanglement. In this dissertation, the successful entanglement of two electron spins in solid state at ambient conditions is demonstrated. The fundamental interaction used to create an entangled state was dipolar coupling between the two electron spins. In order to be able to harness weaker coupling strengths, an entanglement protocol based on dynamical decoupling was developed. A fidelity of F=0.67±0.04 was demonstrated. By using the intrinsic nuclear spins of the nitrogen it was possible to store the entangled state on the millisecond time scale. However, the theoretical limit for the fidelity given by the polarization and the coherence times is F=0.849. The discrepancy can be explained by pulse errors. These can be avoided by using optimal control yielding a fidelity of F=0.824±0.015. Also optimal control allowed for nuclear spin entanglement by storing the electron spin entanglement on the nitrogen nuclear spins. These experiments are first steps towards a room temperature quantum register, where the electron spins are used as bus to transport information and the nuclear spins act as a memory.