arXiv subjects

Paul Greule

Publications and source records attributed to Paul Greule.

7 recordsLinked to original sources

arXiv2026

Electrical Spin Pumping in Exchange-coupled Molecules

Electron spins in single molecules are a promising platform for quantum information processing. However, their practical implementation as qubits requires reliable control at the single-entity level, including an efficient state initialization. Here, we demonstrate the remote, all-electrical initialization of the electron spin in single molecules: Using electron spin resonance scanning tunneling microscopy, we investigate coupled pairs of S=1/2 molecules (Fe-FePc), where one molecule serves as a readout and pumping unit for the neighboring one. We show that the exchange interaction between them enables angular momentum transfer, which allows for the control of the remote spin state via the direction and magnitude of the spin-polarized tunneling current and the exchange coupling strength. These results establish a general, all-electrical approach for remote spin initialization that is readily transferable to a wide range of spin-based quantum architectures.

cond-mat.mes-hall↗

arXiv2026

On the interpretation of Hahn echo measurements in electron spin resonance scanning tunneling microscopy

Electron spin resonance scanning tunneling microscopy (ESR-STM) has become a powerful tool for probing spin dynamics and coherence of individual atoms and molecules on surfaces. In this work, we perform Rabi oscillation and Hahn echo pulse protocols on individual iron phthalocyanine (FePc) molecules on MgO/Ag(001) using ESR-STM. While Hahn echo protocols are widely used to extract spin coherence times, we show that in ESR-STM they are particularly susceptible to misinterpretation due to tunneling electrons generated by the applied radio-frequency (RF) voltage. The RF voltage not only drives the spin, but simultaneously probes and relaxes it, which consequently leads to an exponential decay that reflects spin relaxation rather than intrinsic phase coherence. We moreover show that varying both delay times in the refocusing pulse sequence is a reliable way to ensure a coherent nature of the echo signal. The extracted decay for the latter protocol suggests that T2 is approximately 30 ns and is thus closer to the decoherence time observed in Rabi oscillation measurements. This is significantly shorter than values reported in previous echo measurements. Our findings underscore the need for caution in interpreting T2 times from Hahn echo and Carr-Purcell protocols in ESR-STM and provide practical criteria for distinguishing true spin echoes from tunneling-induced relaxometry signals.

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arXiv2026

Atomic-Scale Quantum Control of Single Spin Defects in a Two-Dimensional Semiconductor

Individual spin defects in solids are promising building blocks for quantum technologies, but their deterministic creation, individual addressability, and operation near surfaces remain major challenges. Two-dimensional materials provide an attractive alternative, as their single-layer thickness enables direct atomic-scale access to defect states. Here, we demonstrate single-spin control of solid-state defects in a two-dimensional semiconductor by a combination of scanning tunneling microscopy and electron spin resonance. We create and manipulate individual sulfur vacancies and carbon substitution defects in monolayer molybdenum disulfide and characterize their spin dynamics, including coherent control, at the single-defect level. Using atomic manipulation, we further engineer and probe spin-spin interactions between defect pairs. Our results demonstrate deterministic creation, addressability, coherent manipulation, and controlled coupling of individual spin defects within a single experimental platform. This establishes atomically engineered spin defects in two-dimensional semiconductors as a versatile class of controllable solid-state quantum systems and opens a route towards tailored quantum sensing experiments.

cond-mat.mes-hall↗

arXiv2025

Spin-Electric Control of Individual Molecules on Surfaces

Individual magnetic molecules are promising building blocks for quantum technologies because of their chemical tunability, nanoscale dimensions, and ability to self-assemble into ordered arrays. However, harnessing their properties in quantum information processing requires precise local control of their spin properties. In this work, we present spin-electric coupling (SEC) for two molecular spin systems, iron phthalocyanine (FePc) and Fe-FePc complexes, adsorbed on a surface. We use electron spin resonance combined with scanning tunnelling microscopy (ESR-STM) to locally address them with the STM tip and electrically tune them using the applied bias voltage. These measurements reveal a pronounced nonlinear voltage dependence of the resonance frequency, linked to the energic onset of other molecular orbitals. We attribute this effect to a transport-mediated exchange field from the magnetic tip, providing a large, highly localized, and broadly applicable SEC mechanism. Finally, we demonstrate that the SEC enables all-electrical coherent spin control: In Rabi oscillation measurements of both single and coupled Fe-FePc complexes we show that the spin dynamics can be tuned, demonstrating a pathway towards electrically controlled quantum operation.

cond-mat.mes-hall↗

arXiv2025

An electrically controlled single molecule spin switch

Precise control of spin states and spin-spin interactions in atomic-scale magnetic structures is crucial for spin-based quantum technologies. A promising architecture is molecular spin systems, which offer chemical tunability and scalability for larger structures. An essential component, in addition to the qubits themselves, is switchable qubit-qubit interactions that can be individually addressed. In this study, we present an electrically controlled single-molecule spin switch based on a bistable complex adsorbed on an insulating magnesium oxide film. The complex, which consists of an Fe adatom coupled to an iron phthalocyanine (FePc) molecule, can be reversibly switched between two stable states using voltage pulses locally via the tip of a scanning tunnelling microscope (STM). Inelastic electron tunnelling spectroscopy (IETS) measurements and density functional theory (DFT) calculations reveal a distinct change between a paramagnetic and a non-magnetic spin configuration. Lastly, we demonstrate the functionality of this molecular spin switch by using it to modify the electron spin resonance (ESR) frequency of a nearby target FePc spin within a spin-spin coupled structure. Thus, we showcase how individual molecular machines can be utilized to create scalable and tunable quantum devices.

cond-mat.mes-hall↗

arXiv2025

Probing Magnetism in Self-Assembled Organometallic Complexes using Kondo Spectroscopy

Control of individual spins at the atomic level holds great promise for miniaturized spintronics, quantum sensing, and quantum information processing. Both single atomic and molecular spin centers are prime candidates for these applications and are often individually addressed and manipulated using scanning tunneling microscopy (STM). In this work, we present a hybrid approach and demonstrate a robust method for self-assembly of magnetic organometallic complexes consisting of individual iron (Fe) atoms and molecules on a silver substrate using STM. We employ two types of molecules, bis(dibenzoylmethane) copper(II) [Cu(dbm)2] and iron phthalocyanine (FePc). We show that in both cases the Fe atoms preferentially attach underneath the benzene ring ligand of the molecules, effectively forming an organometallic half-sandwich arene complex, Fe(C6H6), that is akin to the properties of metallocenes. In both situations, a molecule can be combined with up to two Fe atoms. In addition, we observe a change in the magnetic properties of the attached Fe atoms in scanning tunneling spectroscopy, revealing a distinct Kondo signature at the Fe sites. We explain the latter using density functional theory calculations, and find that the bond formation between the Fe 3d-orbitals and the benzene {\pi}-molecular orbitals creates a favorable situation for Kondo screening of the d_xz- and d_yz-like orbitals. Thus, this work establishes a reliable design principle for forming hybrid organometallic complexes and simultaneous tuning of their atomic spin states.

cond-mat.mes-hall↗

arXiv2024

Quantum Spin-Engineering in On-Surface Molecular Ferrimagnets

The design and control of atomic-scale spin structures constitute major challenges for spin-based quantum technology platforms, including quantum dots, color centers, and molecular spins. Here, we showcase a strategy for designing the quantum properties of molecular spin qubits by combining tip-assisted on-surface assembly with electron spin resonance scanning tunneling microscopy (ESR-STM): We fabricate magnetic dimer complexes that consist of an iron phthalocyanine (FePc) molecule and an organometallic half-sandwich complex formed by the FePc ligand and an attached iron atom, Fe(C6H6). The total complex forms a mixed-spin (1/2,1) quantum ferrimagnet with a well-separated correlated ground state doublet, which we utilize for coherent control. As a result of the correlation, the quantum ferrimagnet shows an improved spin lifetime (>1.5 ${\mu}$s) as it is partially protected against inelastic electron scattering. Lastly, the ferrimagnet units also enable intermolecular coupling, that can be used to realize both ferromagnetic or antiferromagnetic structures. Thus, quantum ferrimagnets provide a versatile platform to improve coherent control in general and to study complex magnetic interactions.

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