Atomic scale engineering of magnetic fields is a key ingredient for miniaturizing quantum devices and precision control of quantum systems. This requires a unique combination of magnetic stability and spin-manipulation capabilities. Surface-supported single atom magnets offer such possibilities, where long temporal and thermal stability of the magnetic states can be achieved by maximizing the magnet/ic anisotropy energy (MAE) and by minimizing quantum tunnelling of the magnetization. Here, we show that dysprosium (Dy) atoms on magnesium oxide (MgO) have a giant MAE of 250 meV, currently the highest among all surface spins. Using a variety of scanning tunnelling microscopy (STM) techniques including single atom electron spin resonance (ESR), we confirm no spontaneous spin-switching in Dy over days at ≈ 1 K under low and even vanishing magnetic field. We utilize these robust Dy single atom magnets to engineer magnetic nanostructures, demonstrating unique control of magnetic fields with atomic scale tunability.
Electron spin resonance (ESR) spectroscopy is a crucial tool in investigations of the chemical structure of materials, and of the electronic structure of materials associated with unpaired spins, through spin-labelling. ESR spectra measured in molecular systems, however, are established on large ensembles of spins and usually require complicated structural analysis. Recently, the combination of scanning tunneling microscopy (STM) with ESR has proven to be a powerful tool to image and coherently control individual atomic spins on surfaces. Here, we extend this technique single coordination complexes -iron phthalocyanines (FePc) -and investigate the magnetic interactions between their molecular spin with either another molecular spin (in FePc-FePc dimers) or an atomic spin (in FePc-Ti pairs). We show that the molecular spin density of 2 FePc is both localized at the central Fe atom and also distributed to the outer ligands, yielding a strongly molecular, geometry-dependent exchange coupling.
Control of single electron spins constitutes one of the most promising platforms for spintronics, quantum sensing, and quantum information processing. Utilizing single molecular magnets as their hosts establishes an interesting framework since their molecular structure is highly flexible and chemistry-based large-scale synthesis directly provides a way toward scalability. Here, we demonstrate coherent spin manipulation of single molecules on a surface, which we control individually using a scanning tunneling microscope in combination with electron spin resonance. We previously found that iron phthalocyanine (FePc) molecules form a spin-1/2 system when placed on an insulating thin film of magnesium oxide (MgO). Performing Rabi oscillation and Hahn echo measurements, we show that the FePc spin can be coherently manipulated with a phase coherence time T 2 Echo of several hundreds of nanoseconds. Tunneling current-dependent measurements demonstrate that interaction with the tunneling electrons is the dominating source of decoherence. In addition, we perform Hahn echo measurements on small self-assembled arrays of FePc molecules. We show that, despite additional intermolecular magnetic coupling, spin resonance and T 2 Echo are much less perturbed by T 1 spin flip events of neighboring spins than by the tunneling current. This will potentially allow for individual addressable molecular spins in self-assemblies and with application for quantum information processing.
Electron spin resonance with a scanning tunneling microscope (ESR-STM) combines the high energy resolution of spin resonance spectroscopy with the atomic scale control and spatial resolution of STM. Here we describe the upgrade of a helium-3 STM with a 2D vector-field magnet (Bz = 8.0 T, Bx = 0.8 T) to an ESR-STM. The system is capable of delivering radio frequency (RF) power to the tunnel junction at frequencies up to 30 GHz. We demonstrate magnetic field-sweep ESR for the model system TiH/MgO/Ag(100) and find a magnetic moment of (1.004 ± 0.001) B. Our upgrade enables to toggle between a DC mode, where the STM is operated with the regular control electronics, and an ultrafast-pulsed mode that uses an arbitrary waveform generator for pump-probe spectroscopy or reading of spin-states. Both modes allow for simultaneous radiofrequency excitation, which we add via a resistive pick-off tee to the bias voltage path. The RF cabling from room temperature to the 350 mK stage has an average attenuation of 18 dB between 5 and 25 GHz. The cable segment between the 350 mK stage and the STM tip presently attenuates an additional 34+5−3 dB from 10 to 26 GHz and 38+3−2 dB between 20 and 30 GHz. We discuss our transmission losses and indicate ways to reduce this attenuation. We finally demonstrate how to synchronize the arrival times of RF and DC pulses coming from different paths to the STM junction, a prerequisite for future pulsed ESR experiments.
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