Nuclear spins owe their long-lived magnetic states to their excellent isolation from the environment. At the same time, a finite degree of interaction with their surroundings is necessary for reading and writing the spin state. Therefore, detailed knowledge of and control over the atomic environment of a nuclear spin is key to optimizing conditions for quantum information applications. While various platforms enabled single-shot readout of nuclear spins, their direct environments were either unknown or impossible to controllably modify on the atomic scale. Scanning tunneling microscopy (STM), combined with electron spin resonance (ESR), provides atomic-scale information of individual nuclear spins via the hyperfine interaction. Here, we demonstrate single-shot readout of an individual ⁴⁹Ti nuclear spin with an STM. Employing a pulsed measurement scheme, we find its lifetime to be in the order of seconds. Furthermore, we shed light on the pumping and relaxation mechanisms of the nuclear spin by investigating its response to both ESR driving and tunneling current, which is supported by model calculations. These findings give an atomic-scale insight into the nature of nuclear spin relaxation and are relevant for the development of atomically assembled qubit platforms.

Atomically engineered artificial lattices are a useful tool for simulating complex quantum phenomena, but have so far been limited to the study of Hamiltonians where electron-electron interactions do not play a role. However, it is precisely the regime in which these interactions do matter where computational times lend simulations a critical advantage over numerical methods. Here, we propose a platform for constructing artificial matter that relies on the confinement of field-emission resonances, a class of vacuum-localized discretized electronic states. We use atom manipulation of surface vacancies in a chlorine-terminated Cu(100) surface to reveal square patches of the underlying metal, thereby creating atomically precise potential wells that host particle-in-a-box modes. By adjusting the dimensions of the confining potential, we can access states with different quantum numbers, making these patches attractive candidates as quantum dots or artificial atoms. We demonstrate that the lifetime of electrons in these engineered states can be extended and tuned through modification of the confining potential, either via atomic assembly or by changing the tip-sample distance. We also demonstrate control over a finite range of state filling, a parameter which plays a key role in the evolution of quantum many-body states. We model the transport through the localized state to disentangle and quantify the lifetime-limiting processes, illustrating the critical dependence of the electron lifetime on the properties of the underlying bulk band structure. The interplay with the bulk bands gives rise to negative differential resistance, leading to possible applications in engineering custom atomic-scale resonant tunnelling diodes, which exhibit similar current-voltage characteristics.

Full insight into the dynamics of a coupled quantum system depends on the ability to follow the effect of a local excitation in real-time. Here, we trace the free coherent evolution of a pair of coupled atomic spins by means of scanning tunneling microscopy. Rather than using microwave pulses, we use a direct-current pump-probe scheme to detect the local magnetization after a current-induced excitation performed on one of the spins. By making use of magnetic interaction with the probe tip, we are able to tune the relative precession of the spins. We show that only if their Larmor frequencies match, the two spins can entangle, causing angular momentum to be swapped back and forth. These results provide insight into the locality of electron spin scattering and set the stage for controlled migration of a quantum state through an extended spin lattice.