This thesis describes atomic spin chains subject to magnetic anisotropy. Such chains, assembled through means of scanning tunneling microscopy (STM), can be home to a plethora of magnetic states and spin physics. This includes quantum tunneling of magnetization, the injection and delocalization of magnons and, for single atoms, the application of electron spin resonance (ESR). Each phenomenon happens at their own timescale which is dependent on the isolation of the spin chain from the environment, ranging from seconds to picoseconds.@en

Recent advances in improving the spectroscopic energy resolution in scanning tunneling microscopy (STM) have been achieved by integrating electron spin resonance (ESR) with STM. Here, we demonstrate the design and performance of a homebuilt STM capable of ESR at temperatures ranging from 1 to 10 K. The STM is incorporated with a homebuilt Joule-Thomson refrigerator and a two-axis vector magnet. Our STM design allows for the deposition of atoms and molecules directly into the cold STM, eliminating the need to extract the sample for deposition. In addition, we adopt two methods to apply radio-frequency (RF) voltages to the tunnel junction: the early design of wiring to the STM tip directly and a more recent idea to use an RF antenna. Direct comparisons of ESR results measured using the two methods and simulations of electric field distribution around the tunnel junction show that, despite their different designs and capacitive coupling to the tunnel junction, there is no discernible difference in the driving and detection of ESR. Furthermore, at a magnetic field of ∼1.6 T, we observe ESR signals (near 40 GHz) sustained up to 10 K, which is the highest temperature for ESR-STM measurement reported to date, to the best of our knowledge. Although the ESR intensity exponentially decreases with increasing temperature, our ESR-STM system with low noise at the tunnel junction allows us to measure weak ESR signals with intensities of a few fA. Our new design of an ESR-STM system, which is operational in a large frequency and temperature range, can broaden the use of ESR spectroscopy in STM and enable the simple modification of existing STM systems, which will hopefully accelerate a generalized use of ESR-STM.@en

Atomic spin structures assembled by means of scanning tunneling microscopy (STM) provide valuable insight into the understanding of atomic-scale magnetism. Among the major challenges are the detection and subsequent read-out of ultrafast spin dynamics due to a dichotomy in travel speed of these dynamics and the probe tip. Here, we present a device composed of individual Fe atoms that allows for remote detection of spin dynamics. We have characterized the device and used it to detect the presence of spin waves originating from an excitation induced by the STM tip several nanometres away; this may be extended to much longer distances. The device contains a memory element that can be consulted seconds after detection, similar in functionality to e.g. a single photon detector. We performed statistical analysis of the responsiveness to remote spin excitations and corroborated the results using basic calculations of the free evolution of coupled quantum spins.@en