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Christoph Sürgers

Publications and source records attributed to Christoph Sürgers.

At least 19 recordsLinked to original sources

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↗

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↗

High-fidelity control of a $^{13}$C nuclear spin coupled to a tin-vacancy center in diamond

Nuclear spins near group-IV defects in diamond are promising candidates for quantum memories in quantum network applications. Here, we demonstrate high-fidelity control of a single $^{13}$C nuclear spin coupled to a tin-vacancy (SnV) center in diamond. We perform a combination of optical and microwave pumping to achieve initialization into a combined electro-nuclear spin state with a fidelity of $99.74(3)\,\%$. Harnessing a superconducting waveguide for radio-frequency driving, we demonstrate precise nuclear spin control: Ramsey measurements reveal a coherence time of $T_2^* = 1.5(1)\,$milliseconds, and we use dynamical decoupling to extend it to $1.35(3)\,$seconds. We perform randomized benchmarking, yielding a single-qubit gate fidelity of $99.92(1)\,\%$. This demonstrates a coherent spin-photon system with promising properties for quantum network nodes.

quant-ph↗

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↗

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↗

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 π-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↗

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 $μ$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.

cond-mat.mes-hall↗

Lateral Mn5Ge3 spin-valve in contact with a high-mobility Ge two-dimensional hole gas

Ge two-dimensional hole gases in strained modulation-doped quantum-wells represent a promising material platform for future spintronic applications due to their excellent spin transport properties and the theoretical possibility of efficient spin manipulation. Due to the continuous development of epitaxial growth recipes extreme high hole mobilities and low effective masses can be achieved, promising an efficient spin transport. Furthermore, the Ge two-dimensional hole gas (2DHG) can be integrated in the well-established industrial complementary metal-oxide-semiconductor (CMOS) devices technology. However, efficient electrical spin injection into a Ge 2DHG - a prerequisite for the realization of spintronic devices - has not yet been demonstrated. In this work, we report the fabrication and low-temperature magnetoresistance measurements of a laterally structured Mn5Ge3/Ge 2DHG/ Mn5Ge3 device. The ferromagnetic Mn5Ge3 contacts are grown directly into the Ge quantum well by means of an interdiffusion process with a spacing of approximately 130 nm. We observe a magnetoresistance signal for temperatures below 13 K possibly arising from successful spin injection. The results represent a step forward toward the realization of CMOS compatible spintronic devices based on a 2DHG.

cond-mat.mes-hall↗

Anomalous Nernst effect in the noncollinear antiferromagnet Mn$_5$Si$_3$

Investigating the off-diagonal components of the conductivity and thermoelectric tensor of materials hosting complex antiferromagnetic structures has become a viable method to reveal the effects of topology and chirality on the electronic transport in these systems. In this respect, Mn$_5$Si$_3$ is an interesting metallic compound that exhibits several antiferromagnetic phases below 100 K with different collinear and noncollinear arrangements of Mn magnetic moments. Previous investigations have shown that the transitions between the various phases give rise to large changes of the anomalous Hall effect. Here, we report measurements of the anomalous Nernst effect of Mn$_5$Si$_3$ single crystals. Below 25 K we observe a sign change of the zero-field Nernst signal with a concomitant decrease of the Hall signal and a gradual reduction of the remanent magnetization which we attribute to a subtle rearrangement of the magnetic moment configuration at low temperatures.

cond-mat.mtrl-sci↗

Optimization of reactively sputtered Mn3GaN films based on resistivity measurements

Mn-based nitrides with antiperovskite structures have several properties that can be utilised for antiferromagnetic spintronics. Their magnetic properties depend on the structural quality, composition and doping of the cubic antiperovskite structure. Such nitride thin films are usually produced by reactive physical vapour deposition, where the deposition rate of N can only be controlled by the N2 gas flow. We show that the tuning of the N content can be optimised using low temperature resistivity measurements, which serve as an indicator of the degree of structural disorder. Several Mn3GaNx films were prepared by reactive magnetron sputtering under different N2 gas flows. Under optimised conditions, we obtain films that exhibit a metal-like temperature dependence, a vanishing logarithmic increase in resistivity towards zero, the highest resistivity ratio and a lattice contraction of 0.4 % along the growth direction when heated above that of the Néel temperature in agreement with the bulk samples.

cond-mat.mtrl-sci↗

Microwave Control of the Tin-Vacancy Spin Qubit in Diamond with a Superconducting Waveguide

Group-IV color centers in diamond are promising candidates for quantum networks due to their dominant zero-phonon line and symmetry-protected optical transitions that connect to coherent spin levels. The negatively charged tin-vacancy (SnV) center possesses long electron spin lifetimes due to its large spin-orbit splitting. However, the magnetic dipole transitions required for microwave spin control are suppressed, and strain is necessary to enable these transitions. Recent work has shown spin control of strained emitters using microwave lines that suffer from Ohmic losses, restricting coherence through heating. We utilize a superconducting coplanar waveguide to measure SnV centers subjected to strain, observing substantial improvement. A detailed analysis of the SnV center electron spin Hamiltonian based on the angle-dependent splitting of the ground and excited states is performed. We demonstrate coherent spin manipulation and obtain a Hahn echo coherence time of up to $T_2 = 430\,μ$s. With dynamical decoupling, we can prolong coherence to $T_2 = 10\,$ms, about six-fold improved compared to earlier works. We also observe a nearby coupling $^{13}\mathrm{C}$ spin which may serve as a quantum memory. This substantiates the potential of SnV centers in diamond and demonstrates the benefit of superconducting microwave structures.

quant-ph↗

Nano-assembled open quantum dot nanotube devices

A pristine suspended carbon nanotube is a near ideal environment to host long-lived quantum states. For this reason, they have been used as the core element of qubits and to explore numerous condensed matter physics phenomena. One of the most advanced technique to realize complex carbon nanotube based quantum circuits relies on a mechanical integration of the nanotube into the circuit. Despite the high-quality and complexity of the fabricated circuits, the range of possible experiments was limited to the closed quantum dot regime. Here, by engineering a transparent metal-nanotube interface, we developed a technique that overcomes this limitation. We reliably reach the open quantum dot regime as demonstrated by measurements of Fabry-Perot interferences and Kondo physics in multiple devices. A circuit-nanotube alignment precision of +/-200nm is demonstrated. Our technique allows to envision experiments requiring the combination of complex circuits and strongly coupled carbon nanotubes such as the realization of carbon nanotube superconducting qubits or flux-mediated optomechanics experiments.

physics.app-ph↗

Phase transitions associated with magnetic-field induced topological orbital momenta in a non-collinear antiferromagnet

Resistivity measurements are widely exploited to uncover electronic excitations and phase transitions in metallic solids. While single crystals are preferably studied to explore crystalline anisotropies, these usually cancel out in polycrystalline materials. Here we show that in polycrystalline Mn3Zn0.5Ge0.5N with non-collinear antiferromagnetic order, changes in the diagonal and, rather unexpected, off-diagonal components of the resistivity tensor occur at low temperatures indicating subtle transitions between magnetic phases of different symmetry. This is supported by neutron scattering and explained within a phenomenological model which suggests that the phase transitions in magnetic field are associated with field induced topological orbital momenta. The fact that we observe transitions between spin phases in a polycrystal, where effects of crystalline anisotropy are cancelled suggests that they are only controlled by exchange interactions. The observation of an off-diagonal resistivity extends the possibilities for realising antiferromagnetic spintronics with polycrystalline materials.

cond-mat.mtrl-sci↗

Onset of phase diffusion in high kinetic inductance granular aluminum micro-SQUIDs

Superconducting granular aluminum is attracting increasing interest due to its high kinetic inductance and low dissipation, favoring its use in kinetic inductance particle detectors, superconducting resonators or quantum bits. We perform switching current measurements on DC-SQUIDs, obtained by introducing two identical geometric constrictions in granular aluminum rings of various normal-state resistivities in the range from $ρ_\mathrm{n} = 250\,μΩ\mathrm{cm}$ to $5550\,μΩ\mathrm{cm}$. The relative high kinetic inductance of the SQUID loop, in the range of tens of nH, leads to a suppression of the modulation in the measured switching current versus magnetic flux, accompanied by a distortion towards a triangular shape. We observe a change in the temperature dependence of the switching current histograms with increasing normal-state film resistivity. This behavior suggests the onset of a diffusive motion of the superconducting phase across the constrictions in the two-dimensional washboard potential of the SQUIDs, which could be caused by a change of the local electromagnetic environment of films with increasing normal-state resistivities.

cond-mat.supr-con↗

Creation of equal-spin triplet superconductivity at the Al/EuS interface

In conventional superconductors, electrons of opposite spins are bound into Cooper pairs. However, when the superconductor is in contact with a non-uniformly ordered ferromagnet, an exotic type of superconductivity can appear at the interface, with electrons bound into three possible spin-triplet states. Triplet pairs with equal spin play a vital role in low-dissipation spintronics. Despite the observation of supercurrents through ferromagnets, spectroscopic evidence for the existence of equal-spin triplet pairs is still missing. Here we show a theoretical model that reveals a characteristic gap structure in the quasiparticle density of states which provides a unique signature for the presence of equal-spin triplet pairs. By scanning tunnelling spectroscopy we measure the local density of states to reveal the spin configuration of triplet pairs. We demonstrate that the Al/EuS interface causes strong and tunable spin-mixing by virtue of its spin-dependent transmission.

cond-mat.supr-con↗

Two-band superconductivity of bulk and surface states in Ag thin films on Nb

We use epitaxial strain to shift the energy of the two-dimensional Ag(111) surface states of Ag islands on Nb(110) substrates, allowing to spatially tune the bottom of the surface-state band $E_{\rm SS}$ through the Fermi level $E_{\rm F}$. Bulk and surface-state contributions to the Ag(111) local density of states (LDOS) can be separated with scanning tunneling spectroscopy. For thick islands ($\approx$\, 20 nm), the Ag surface states are decoupled from the Ag bulk states via orthogonality, and the superconductive gap induced by proximity to Nb is due to bulk states only. However, for thin islands (3-4 nm), surface-state electrons develop superconducting correlations as identified by a complete energy gap in the LDOS when $E_{\rm F}$ is smaller than but close to $E_{\rm F}$. The induced superconductivity in this case is of two-band nature and appears to occur when the surface-state wave function reaches down to the Ag/Nb interface.

cond-mat.supr-con↗

15 cm$^{-1}$ to 12000 cm$^{-1}$ spectral coverage without changing optics: diamond beam splitter adaptation of an FTIR spectrometer

In order to facilitate IR absorption measurements of mass-selected ions isolated in cryogenic matrices, we have upgraded an ion beam deposition apparatus encompassing a Bruker IFS66v/S FTIR spectrometer. A synthetic diamond beam splitter without compensator plate and UHV diamond viewports were installed. We have also modified the IR detector chamber to allow measurements with 5 different detectors. As a result we can now obtain FT absorption spectra from 12000 cm$^{-1}$ to 15 cm$^{-1}$ with the same sample held under ultrahigh vacuum conditions, simply by switching between appropriate IR detectors. We demonstrate performance of the upgraded FTIR spectrometer by presenting measurements of matrix isolated fullerene ions and an adhesive tape.

physics.ins-det↗

Signature of f-electron conductance in $α$-Ce single-atom contacts

Cerium is a fascinating element exhibiting, with its different phases, long-range magnetic order and superconductivity in bulk form. The coupling of the 4f electron to sd conduction electrons and to the lattice is responsible for unique structural and electronic properties like the isostructural first-order solid-solid transition from the cubic $γ$ phase to the cubic $α$ phase, which is accompanied by a huge volume collapse of 14 %. While the $γ- α$ phase transition has been investigated for decades, experiments aiming at disentangling the 4f contribution to the electric conductance of the different phases have not been performed. Here we report on the strongly enhanced conductance of single-atom Ce contacts. By controlling the content of $α$-Ce employing different rates of cooling, we find a strong correlation between the fraction of $α$-Ce and the magnitude of the last conductance plateau before the contact breaks. We attribute the enhanced conductance of $α$-Ce to the additional contribution of the 4f level.

cond-mat.mtrl-sci↗