Designing and characterizing the many-body behaviors of quantum materials represents a prominent challenge for understanding strongly correlated physics and quantum information processing. We constructed artificial quantum magnets on a surface by using spin-1/2 atoms in a scanning tunneling microscope (STM). These coupled spins feature strong quantum fluctuations due to antiferromagnetic exchange interactions between neighboring atoms. To characterize the resulting collective magnetic states and their energy levels, we performed electron spin resonance on individual atoms within each quantum magnet. This gives atomic-scale access to properties of the exotic quantum many-body states, such as a finite-size realization of a resonating valence bond state. The tunable atomic-scale magnetic field from the STM tip allows us to further characterize and engineer the quantum states. These results open a new avenue to designing and exploring quantum magnets at the atomic scale for applications in spintronics and quantum simulations.
Designing and characterizing the many-body behaviors of quantum materials represents a prominent challenge for understanding strongly correlated physics and quantum information processing. We constructed artificial quantum magnets on a surface by using spin-1/2 atoms in a scanning tunneling microscope (STM). These coupled spins feature strong quantum fluctuations due to antiferromagnetic exchange interactions between neighboring atoms. To characterize the resulting collective magnetic states and their energy levels, we performed electron spin resonance on individual atoms within each quantum magnet. This gives atomic-scale access to properties of the exotic quantum many-body states, such as a finite-size realization of a resonating valence bond state. The tunable atomic-scale magnetic field from the STM tip allows us to further characterize and engineer the quantum states. These results open a new avenue to designing and exploring quantum magnets at the atomic scale for applications in spintronics and quantum simulations.
Achieving time-domain control of quantum states with atomic-scale spatial resolution in nanostructures is a long-term goal in quantum nanoscience and spintronics. Here, we demonstrate coherent spin rotations of individual atoms on a surface at the nanosecond time scale, using an all-electric scheme in a scanning tunneling microscope (STM). By modulating the atomically confined magnetic interaction between the STM tip and surface atoms, we drive quantum Rabi oscillations between spin-up and spin-down states in as little as ~20 nanoseconds. Ramsey fringes and spin echo signals allow us to understand and improve quantum coherence. We further demonstrate coherent operations on engineered atomic dimers. The coherent control of spins arranged with atomic precision provides a solid-state platform for quantum-state engineering and simulation of many-body systems.
Physics at the level of an atom is dominated by laws of quantum mechanics. Often, this is entangled with a high complexity in behavior of the systems at that length scale. Unravelling the properties of a material at the atomic level is, therefore, a challenging task that easily supersedes current computational capabilities. A route to circumvent this problem is found in physical realization of simpler quantum systems that are representative of the complex quantum systems one is interested in. These simpler physical systems, unlike their more complex counterparts, can actually be measured and information about the complex system, otherwise inaccessible, gained. This thesis describes experimental work focusing mainly on the property of magnetism in spin chains. To mimic these complex systems, we employ a scanning tunneling microscope (STM) to build atomic chains on solid state surfaces and probe their magnetic properties. The intrinsic strength of STM in building and testing structures with single atom precision makes STM a great candidate for simulation of complex quantum systems. In addition to STM having a role of a quantum simulator, I present work supporting STM as a control device determining the very existence of the magnetic excitations of the atom it measures. Finally, I present experimental findings that suggest we are able to probe the magnetic excitations of the atom with subatomic resolution. In summary, this thesis work presents STM as a powerful probing and control tool for studies on quantum magnetism at the level of a single atom.
Quantum entanglement permeates the complex ground states of correlated electron materials defying single-particle descriptions. Coupled magnetic atoms have potential as model systems for entanglement in condensed matter giving the opportunity to create artificial many-body states which can be controlled by tuning the underlying interactions. They provide an avenue to unravel the complexities of correlated-electron materials. Here we use low temperature scanning tunnelling microscopy (STM) and atomic manipulation to tune entanglement in chains of magnetic atoms. We find that a Kondo singlet state can emerge from this entanglement. The many electron Kondo state is based on the screening of the entangled spin ground state of the chain by substrate electrons and can be engineered to envelop at least ten magnetic atoms. The concomitant Kondo resonance measured in the differential conductance enables the electric read-out of entanglement. By tuning composition and coupling strength within atomic chains it is possible to create model spin chains with defined entanglement. This lays the foundation for a new class of experiments to construct exotic correlated-electron materials atom by atom.
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.
Quantum-mechanical correlations of interacting fermions result in the emergence of exotic phases.Magnetic phases naturally arise in the Mott-insulator regime of the Fermi-Hubbard model, where charges are localized and the spin degree of freedom remains.In this regime, the occurrence of phenomena such as resonating valence bonds, frustrated magnetism, and spin liquids is predicted.Quantum systems with engineered Hamiltonians can be used as simulators of such spin physics to provide insights beyond the capabilities of analytical methods and classical computers.To be useful, methods for the preparation of intricate many-body spin states and access to relevant observables are required.Here, we show the quantum simulation of magnetism in the Mott-insulator regime with a linear quantum-dot array.We characterize the energy spectrum for a Heisenberg spin chain, from which we can identify when the conditions for homogeneous exchange couplings are met.Next, we study the multispin coherence with global exchange oscillations in both the singlet and triplet subspace of the Heisenberg Hamiltonian.Last, we adiabatically prepare the low-energy global singlet of the homogeneous spin chain and probe it with two-spin singlettriplet measurements on each nearest-neighbor pair and the correlations therein.The methods and control presented here open new opportunities for the simulation of quantum magnetism benefiting from the flexibility in tuning and layout of gate-defined quantum-dot arrays.
Individual spin defects in solids are promising building blocks for quantum technologies, but their deterministic creation, individual addressability, and operation near surfaces remain major challenges. Two-dimensional materials provide an attractive alternative, as their single-layer thickness enables direct atomic-scale access to defect states. Here, we demonstrate single-spin control of solid-state defects in a two-dimensional semiconductor by a combination of scanning tunneling microscopy and electron spin resonance. We create and manipulate individual sulfur vacancies and carbon substitution defects in monolayer molybdenum disulfide and characterize their spin dynamics, including coherent control, at the single-defect level. Using atomic manipulation, we further engineer and probe spin-spin interactions between defect pairs. Our results demonstrate deterministic creation, addressability, coherent manipulation, and controlled coupling of individual spin defects within a single experimental platform. This establishes atomically engineered spin defects in two-dimensional semiconductors as a versatile class of controllable solid-state quantum systems and opens a route towards tailored quantum sensing experiments.