Differential conductance spectroscopy performed in the high bias regime - in which the applied voltage exceeds the sample work function - is a suboptimal measure of the local density of states due to the effects of the changing tunnel barrier. Additionally, the large applied voltage oftentimes makes constant-height measurement experimentally impractical, lending constant-current spectroscopy an advantageous edge; but the differential conductance in that case is even further removed from the local density of states due to the changing tip height. Here, we present a normalization scheme for extracting the local density of states from high bias scanning tunneling spectroscopy, obtained in either constant-current or constant-height mode. We extend this model to account for the effects of the in-plane momentum of the probed states to the overall current. We demonstrate the validity of the proposed scheme by applying it to laterally confined field-emission resonances, which appear as peak-shaped spectroscopic features with a well-defined in-plane momentum.

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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.

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This thesis focuses on possible platforms for a bottom-up approach towards realizing and characterizing atomically assembled magnetic and electronic artificial lattices. For this, we make use of the scanning tunneling microscope (STM), which provides a local probe of the magnetic and electronic properties of the sample and allows for the atom-by-atom construction of extended lattices. On the one hand, to address avenues for constructing extended spin lattices, we study single Fe atoms coordinated on the four-fold symmetric nitrogen binding site of the Cu2N/Cu3Au surface—a system which permits large-scale atomic assembly, and allows for independent access to both the orbital and spin degrees of freedom. On the other hand, we investigate the viability of laterally confined vacuum resonances on the chlorinated Cu(100) surface as a basis for constructing electronic lattices. We atomically assemble dimers and trimers of various geometries to determine the tight-binding parameters, and as a proof of concept, experimentally realize a looped Su-Schrieffer–Heeger chain using this platform. These studies are made possible by means of a low-temperature, ultra-high vacuum STM, which allows for atom manipulation and, via spectroscopic techniques, permits us to locally probe the sample density of states and detect inelastic excitations of the spin and orbital angular momentum.@en

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.

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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 Cu₂N lattice, we realize a single-atom 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 single-electron 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.

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