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.

The orbital angular moment of magnetic atoms adsorbed on surfaces is often quenched as a result of an anisotropic crystal field. Due to spin-orbit coupling, what remains of the orbital moment typically delineates the orientation of the electron spin. These two effects limit the scope of information processing based on these atoms to essentially only one magnetic degree of freedom: the spin. In this work, we gain independent access to both the spin and orbital degrees of freedom of a single atom, inciting and probing excitations of each moment. By coordinating a single Fe atom atop the nitrogen site of the Cu 2 N lattice, we realize a singleatom system with a large zero-field splitting-the largest reported for Fe atoms on surfaces-and an unquenched uniaxial orbital moment that closely approaches the free-atom value. We demonstrate a full reversal of the orbital moment through a singleelectron tunneling event between the tip and Fe atom, a process that is mediated by a charged virtual state and leaves the spin unchanged. These results, which we corroborate using density functional theory and first-principles multiplet calculations, demonstrate independent control over the spin and orbital degrees of freedom in a single-atom system.

We present controlled growth of c(2×2)N islands on the (100) surface of Cu 3 Au, which can be used as an insulating surface template for manipulation of magnetic adatoms. Compared to the commonly used Cu(100)/c(2×2)N surface, where island sizes do not exceed several nanometers due to strain limitation, the current system provides better lattice matching between metal and adsorption layer, allowing larger unstrained islands to be formed. We show that we can achieve island sizes ranging from tens to hundreds of nanometers, increasing the potential building area by a factor 10 3 . Initial manipulation attempts show no observable difference in adatom behaviour, either in manipulation or spectroscopy.

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 rolebut it's precisely the regime in which these interactions do matter where computational times lend simulations a critical advantage over numerical methods. Here, we propose a new 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 atomicallyprecise potential wells that host particle-in-a-box modes. By adjusting the shape and size 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 dependency of the electron lifetime on the properties of the underlying bulk band structure. The interplay with the bulk bands also gives rise to negative differential resistance,

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.