The nuclear spin is a prime candidate for quantum information applications due to its weak coupling to the environment and inherently long coherence times. However, this weak coupling also challenges the addressability of the nuclear spin. Here we demonstrate nuclear magnetic resonance (NMR) on a single on-surface atom using a local scanning probe. We employ an electron-nuclear double resonance measurement scheme and resolve nuclear spin transitions of a single 47Ti isotope with a nuclear spin of I = 5/2. The quadrupole interaction enables to resolve multiple NMR transitions, which are consistent with our eigenenergy calculations. Our experimental results indicate that the nuclear spin can be driven efficiently irrespective of its hybridization with the electron spin, which is required for direct control of the nuclear spin in the long-lifetime regime. This investigation of NMR on a single atom in a platform with atomic-scale control is a valuable development for other platforms deploying nuclear spins for characterization techniques or quantum information technology.
The nuclear spin is a prime candidate for quantum information applications due to its weak coupling to the environment and inherently long coherence times. However, this weak coupling also challenges the addressability of the nuclear spin. Here we demonstrate nuclear magnetic resonance (NMR) on a single on-surface atom using a local scanning probe. We employ an electron-nuclear double resonance measurement scheme and resolve nuclear spin transitions of a single 47Ti isotope with a nuclear spin of I = 5/2. The quadrupole interaction enables to resolve multiple NMR transitions, which are consistent with our eigenenergy calculations. Our experimental results indicate that the nuclear spin can be driven efficiently irrespective of its hybridization with the electron spin, which is required for direct control of the nuclear spin in the long-lifetime regime. This investigation of NMR on a single atom in a platform with atomic-scale control is a valuable development for other platforms deploying nuclear spins for characterization techniques or quantum information technology.
Solid-state nuclear magnetic resonance (NMR) has emerged as an important technique for material characterization, finding extensive applications across a diverse range of disciplines including physics, materials science, chemistry, and biology. Its utility stems from the ability to probe the local atomic environments and molecular dynamics within solid materials, which provides information on the composition of the material. In recent years, the scope of solid-state NMR has expanded into the realm of quantum information science and technology, where its abundant many-body interactions pulse control methodologies make it have significant research value and application potential. This paper offers a comprehensive overview of the research objects and theoretical underpinnings of solid-state NMR, delving into the critical nuclear spin interaction mechanisms and their corresponding Hamiltonian forms. These interactions, which include dipolar coupling, chemical shift anisotropy, and quadrupolar interactions, are fundamental to the interpretation of NMR spectra and the understanding of material properties at the atomic level. Moreover, the paper introduces typical dynamical control methods employed in the manipulation of solid-state nuclear spins. Techniques such as dynamical decoupling, which mitigates the effects of spin-spin interactions to extend coherence times, and magic-angle spinning, which averages out anisotropic interactions to yield high-resolution spectra. These methods are essential for enhancing the sensitivity and resolution of NMR experiments, enabling the extraction of detailed structural and dynamic information from complex materials. Then we introduce some recent advancements in quantum control based on solid-state NMR, such as nuclear spin polarization enhancement techniques, which include dynamic nuclear polarization (DNP) and cross polarization (CP), significantly boost the sensitivity of NMR measurements. Additionally, the control techniques of Floquet average Hamiltonians are mentioned, showcasing their role in the precise manipulation of quantum states and the realization of quantum dynamics. Finally, the paper presents a series of seminal research works that illustrate the application of solid-state NMR quantum control technologies in the field of quantum simulation. These studies demonstrate how solid-state NMR can be leveraged to simulate and investigate quantum many-body systems, providing valuable insights into quantum phase transitions, entanglement dynamics, and other phenomena relevant to quantum information science. By bridging the gap between fundamental research and practical applications, solid-state NMR continues to play a crucial role in advancing our understanding of quantum materials and technologies.
Electron spin resonance in scanning tunneling microscopy enabled the study of electronic transitions of magnetic impurities on surfaces at the atomic scale. This ESR-STM technique allows to spectroscopically probe and coherently manipulate spins using an all-electrical method without oscillating external magnetic driving fields. Here, we aim to review recent advancements in ESR-STM. We will discuss possible fundamental mechanisms by which the electric field drives spin resonance based on Heisenberg exchange, Kondo scattering, and Anderson impurity models. We validate theoretical predictions against experimental observations, to understand how electronic correlations, spin exchange, and many-body effects manifest in ESR-STM signals. After reviewing coherent spin control in the STM junction, we discuss potential applications of the ESR-STM method for coherent multi-spin control which enables multiple-qubit operations. Finally, we address recent developments in coupled electron-nuclear spin systems, including hyperfine-resolved ESR spectroscopy, and the driving and polarization of nuclear spins in ESR-STM.
The goal of this project was to improve our control over nuclear spins in the solid state, and to extend this control to coupled electron-nuclear spins. Our key results are summarized below. 1. We extended the control techniques developed in liquid state NMR quantum information processing to the control of a three-qubit solid state NMR quantum information processor. 2. To explore multi-body spin dynamics and their sensitivity to decoherence, we have measured the decay of NMR multiple quantum coherence intensities in the presence and absence of the dipolar Hamiltonian, in a cubic and a one-dimensional spin system. 3. We also studied the transport of polarization in the one-dimensional fluoroapatite system, both experimentally and theoretically, and created special states in which the polarization is localized to the ends of the chain. This enables both universal Quantum Computing and Quantum Simulation in 1-D systems. 4. We devised a novel scheme for electron-nuclear quantum information processing that exploits the anisotropic hyperfine coupling. This scheme enables universal control over a 1-electron, N-nuclear spin system, addressing only a single electron spin transition. Not having to address the nuclear spins directly significantly speeds up the control. We designed and fabricated a pulsed electron spin resonance spectrometer, along with a cryogenic probe which we used to experimentally implement this scheme on a single crystal sample of irradiated malonic acid. 5. We demonstrated the role of nuclear spin dipolar diffusion in dynamic nuclear polarization (DNP) experiments, in dielectric samples with abundant nuclear spins. We achieved a 29Si polarization of 8.3% at 66 GHz and 1.1 K in single crystal P-doped, the highest ever reported, using DNP.
Rapid developments in quantum information processing have been made, and remarkable achievements have been obtained in recent years, both in theory and experiments. Coherent control of nuclear spin dynamics is a powerful tool for the experimental implementation of quantum schemes in liquid and solid nuclear magnetic resonance (NMR) system, especially in liquid-state NMR. Compared with other quantum information processing systems, the NMR platform has the advantages such as the long coherence time, the precise manipulation, and well-developed quantum control techniques, which make it possible to accurately control a quantum system with up to 12-qubits. Extensive applications of liquid-state NMR spectroscopy in quantum information processing such as quantum communication, quantum computing, and quantum simulation have been thoroughly studied over half a century. This article introduces the general principles of NMR quantum information processing, and reviews the new-developed techniques. The review will also include the recent achievements of the experimental realization of quantum algorithms for machine learning, quantum simulations for high energy physics, and topological order in NMR. We also discuss the limitation and prospect of liquid-state NMR spectroscopy and the solid-state NMR systems as quantum computing in the article.
The ability to coherently control and read out qubits with long coherence times in a scalable system is a crucial requirement for any quantum processor. Nuclear spins in the solid state have shown great promise as long-lived qubits. Control and readout of individual nuclear spin qubit registers has made major progress in the recent years using individual electron spin ancilla addressed either electrically or optically. Here, we present a new platform for quantum information processing, consisting of 183W nuclear spin qubits adjacent to an Er3+ impurity in a CaWO4 crystal, interfaced via a superconducting resonator and detected using a microwave photon counter at 10mK. We study two nuclear spin qubits with T2∗ of 0.8(2)s and 1.2(3)s, T2 of 3.4(4)s and 4.4(6) s, respectively. We demonstrate single-shot quantum non-demolition readout of each nuclear spin qubit using the Er3+ spin as an ancilla. We introduce a new scheme for all-microwave single- and two-qubit gates, based on stimulated Raman driving of the coupled electron-nuclear spin system. We realize single- and two-qubit gates on a timescale of a few milliseconds, and prepare a decoherence-protected Bell state with 88% fidelity and T2∗ of 1.7(2)s. Our results are a proof-of-principle demonstrating the potential of solid-state nuclear spin qubits as a promising platform for quantum information processing. With the potential to scale to tens or hundreds of qubits, this platform has prospects for the development of scalable quantum processors with long-lived qubits.
Spin is a quantum mechanical property that describes the magnetic orientation of elementary and composite particles such as electrons and nuclei. For spin-half particles placed in a magnetic field, two states with differing energies are defined. Proposals exist for developing a revolutionary kind of computer that encodes bits of information on the states of a simple quantum two-level system - like those of a spin in a magnetic field. These quantum computers exploit the fundamental principles of quantum mechanics in order to perform certain calculations exponentially faster than their classical counterparts. Key to the development of such a device is the identification of potential systems that are suitable for employment as a quantum bit (qubit). This thesis explores quantum bits constructed from the spin states of single atoms hosted in silicon semiconductor devices. Silicon is an exceptional platform for spin-based quantum computing - in addition to being the dominant material in the microelectronic industry, it is also predominantly composed of nuclear spin-zero isotopes, providing very little background magnetic disturbance. The donor-atom phosphorus (31P) is investigated here. It possesses a nucleus that binds an additional electron to its positive charge, providing two distinct spin qubits. Here, several world-first experimental milestones in spin-based quantum information processing are reported. First, the readout of the electron spin is demonstrated in single-shot, using a silicon device which combines implanted phosphorus donors with a sensitive nanoscale electrometer. Then, the electron spin is coherently operated as a qubit by delivering on-chip microwave excitations. Combining the electron spin detection and control capabilities enables a quantum non-demolition measurement of the single 31P nuclear spin. Experiments yield exceptional nuclear readout fidelities - the highest for any solid-state qubit. Through an application of nuclear magnetic resonance, high-fidelity quantum control of the nuclear spin qubit is demonstrated. Finally, a single spin-bearing silicon nucleus (29Si) coupled to the electron spin is detected in single-shot and operated as a qubit. These results, along with the clear pathways identified for improving device performance, illustrate that single-atom electron and nuclear spin qubits in silicon constitute an excellent basis on which to construct a quantum computer.