arXiv subjects

Manuel Steinbrecher

Publications and source records attributed to Manuel Steinbrecher.

14 recordsLinked to original sources

arXiv2024

Quantifying the quantum nature of high spin YSR excitations in transverse magnetic field

Excitations of individual and coupled spins on superconductors provide a platform to study quantum spin impurity models as well as a pathway toward realizing topological quantum computing. Here, we characterize, using ultra-low temperature scanning tunneling microscopy/spectroscopy, the Yu-Shiba-Rusinov (YSR) states of individual manganese phthalocyanine molecules with high spin character on the surface of an ultra-thin lead film in variable transverse magnetic field. We observe two types of YSR excitations, depending on the adsorption geometry of the molecule. Using a zero-bandwidth model, we detail the role of the magnetic anisotropy, spin-spin exchange, and Kondo exchange. We illustrate that one molecular type can be treated as an individual spin akin to an isolated spin on the metal center, whereas the other molecular type invokes a coupled spin system represented by a spin on the center and the ligand. Using the field-dependent evolution of the YSR excitations and comparisons to modeling, we describe the quantum phase of each of the molecules. These results provide an insight into the quantum nature of YSR excitations in magnetic field, and a platform to study spin impurity models on superconductors in magnetic field.

cond-mat.supr-con↗

arXiv2024

Activating the fluorescence of a Ni(II) complex by energy transfer

Luminescence of open-shell 3d metal complexes is often quenched due to ultrafast intersystem crossing (ISC) and cooling into a dark metal-centered excited state. We demonstrate successful activation of fluorescence from individual nickel phthalocyanine (NiPc) molecules in the junction of a scanning tunneling microscope (STM) by resonant energy transfer from other metal phthalocyanines at low temperature. By combining STM, scanning tunneling spectroscopy, STM- induced luminescence, and photoluminescence experiments as well as time-dependent density functional theory, we provide evidence that there is an activation barrier for the ISC, which in most experimental conditions is overcome. We show that this is also the case in an electroluminescent tunnel junction where individual NiPc molecules adsorbed on an ultrathin NaCl decoupling film on a Ag(111) substrate are probed. However, when placing an MPc (M = Zn, Pd, Pt) molecule close to NiPc by means of STM atomic manipulation, resonant energy transfer can excite NiPc without overcoming the ISC activation barrier, leading to Q-band fluorescence. This work demonstrates that the thermally activated population of dark metal-centered states can be avoided by a designed local environment at low temperatures paired with a directed molecular excitation into vibrationally cold electronic states. Thus, we can envisage the use of luminophores based on more abundant transition metal complexes that do not rely on Pt or Ir.

cond-mat.mes-hall↗

arXiv2022

Threefold enhancement of superconductivity and the role of field-induced odd-frequency pairing in epitaxial aluminum films near the 2D limit

BCS theory has been widely successful at describing elemental bulk superconductors. Yet, as the length scales of such superconductors approach the atomic limit, dimensionality as well as the environment of the superconductor can lead to drastically different and unpredictable superconducting behavior. Here, we report a threefold enhancement of the superconducting critical temperature and gap size in ultrathin epitaxial Al films on Si(111), when approaching the 2D limit, based on high-resolution scanning tunneling microscopy/spectroscopy (STM/STS) measurements. In magnetic field, the Al films show type II behavior and the Meservey-Tedrow-Fulde (MTF) effect for in-plane magnetic fields. Using spatially resolved spectroscopy, we characterize the vortex structure in the MTF regime and find strong deviations from the typical Abrikosov vortex. We corroborate these findings with calculations that unveil the role of odd-frequency pairing and a paramagnetic Meissner effect. These results illustrate two striking influences of reduced dimensionality on a BCS superconductor and present a new platform to study BCS superconductivity in large magnetic fields.

cond-mat.supr-con↗

arXiv2021

Anisotropic superconductivity induced at a hybrid superconducting-semiconducting interface

Epitaxial semiconductor-superconductor heterostructures are promising as a platform for gate-tunable superconducting electronics. Thus far, the superconducting properties in such hybrid systems have been predicted based on simplified hybridization models which neglect the electronic structure that can arise at the interface. Here, we demonstrate that the hybrid electronic structure derived at the interface between semiconducting black phosphorus and atomically thin films of lead can drastically modify the superconducting properties of the thin metallic film. Using ultra-low temperature scanning tunneling microscopy and spectroscopy, we ascertain the moiré structure driven by the interface, and observe a strongly anisotropic renormalization of the superconducting gap and vortex structure of the lead film. Based on density functional theory, we attribute the renormalization of the superconductivity to weak hybridization at the interface where the anisotropic characteristics of the semiconductor band structure is imprinted on the Fermi surface of the superconductor. Based on a hybrid two-band model, we link this hybridization-driven renormalization to a weighting of the superconducting order parameter that quantitatively reproduces the measured spectra. These results illustrate the effect of interfacial hybridization at superconductor-semiconductor heterostructures, and pathways for engineering quantum technologies based on gate-tunable superconducting electronics.

cond-mat.supr-con↗

arXiv2021

Quantifying the interplay between fine structure and geometry of an individual molecule on a surface

The pathway toward the tailored synthesis of materials starts with precise characterization of the conformational properties and dynamics of individual molecules. Electron spin resonance based scanning tunneling microscopy can potentially address molecular structure with unprecedented resolution. Here, we determine the fine structure and geometry of an individual TiH molecule, utilizing a combination of a newly developed mK ESR-STM in a vector magnetic field and ab initio approaches. We demonstrate a strikingly large anisotropy of the g-tensor unusual for a spin doublet ground state, resulting from a non-trivial orbital angular momentum stemming from the molecular ground state. We quantify the relationship between the resultant fine structure, hindered rotational modes, and orbital excitations. Our model system provides new avenues to determine the structure and dynamics of individual molecules.

cond-mat.mes-hall↗

arXiv2020

A scanning tunneling microscope capable of electron spin resonance and pump-probe spectroscopy at mK temperature and in vector magnetic field

In the last decade, detecting spin dynamics at the atomic scale has been enabled by combining techniques like electron spin resonance (ESR) or pump-probe spectroscopy with scanning tunneling microscopy (STM). Here, we demonstrate an ultra-high vacuum (UHV) STM operational at milliKelvin (mK) and in a vector magnetic field capable of both ESR and pump-probe spectroscopy. By implementing GHz compatible cabling, we achieve appreciable RF amplitudes at the junction while maintaining mK base temperature. We demonstrate the successful operation of our setup by utilizing two experimental ESR modes (frequency sweep and magnetic field sweep) on an individual TiH molecule on MgO/Ag(100) and extract the effective g-factor. We trace the ESR transitions down to MHz into an unprecedented low frequency band enabled by the mK base temperature. We also implement an all-electrical pump-probe scheme based on waveform sequencing suited for studying dynamics down to the nanoseconds range. We benchmark our system by detecting the spin relaxation time T1 of individual Fe atoms on MgO/Ag(100) and note a field strength and orientation dependent relaxation time.

cond-mat.mes-hall↗

arXiv2020

Self-induced spin glass state in elemental and crystalline neodymium

Spin glasses are a highly complex magnetic state of matter, intricately linked to spin frustration and structural disorder. They exhibit no long-range order and exude aging phenomena, distinguishing them from quantum spin liquids. We report a new type of spin glass state, the spin-Q glass, observable in bulk-like crystalline metallic neodymium thick films. Using spin-polarized scanning tunneling microscopy combined with ab initio calculations and atomistic spin-dynamics simulations, we visualize the variations in atomic-scale non-collinear order and its response to magnetic field and temperature. We quantify the aging phenomena relating the glassiness to crystalline symmetry and the energy landscape. This result not only resolves the long-standing debate of the magnetism of neodymium, but also suggests that glassiness may arise in other magnetic solids lacking extrinsic disorder.

cond-mat.mtrl-sci↗

arXiv2020

Controlling in-gap end states by linking nonmagnetic atoms and artificially-constructed spin chains on superconductors

Chains of magnetic atoms with either strong spin-orbit coupling or spiral magnetic order which are proximity-coupled to superconducting substrates can host topologically non-trivial Majorana bound states. The experimental signature of these states consists of spectral weight at the Fermi energy and spatially localized near the ends of the chain. However, topologically trivial Yu-Shiba-Rusinov in-gap states localized near the ends of the chain can lead to similar spectra. Here, we explore a protocol to disentangle these contributions by artificially augmenting a candidate Majorana spin chain with orbitally-compatible nonmagnetic atoms. Combining scanning tunneling spectroscopy with ab-initio and tight-binding calculations, we realize a sharp spatial transition between the proximity-coupled spiral magnetic order and the non-magnetic superconducting wire termination, with persistent zero-energy spectral weight localized at either end of the magnetic spiral. Our findings open a new path towards the control of the spatial position of in-gap end states, trivial or Majorana, via different chain terminations, and the realization of designer Majorana chain networks for demonstrating topological quantum computation.

cond-mat.supr-con↗

arXiv2019

Magnetism and in-gap states of 3d transition metal atoms on superconducting Re

Magnetic atoms on heavy-element superconducting substrates are potential building blocks for realizing topological superconductivity in one- and two-dimensional atomic arrays. Their localized magnetic moments induce so-called Yu-Shiba-Rusinov (YSR) states inside the energy gap of the substrate. In the dilute limit, where the electronic states of the array atoms are only weakly coupled, proximity of the YSR states to the Fermi energy is essential for the formation of topological superconductivity in the band of YSR states. Here, we reveal via scanning tunnel spectroscopy and ab initio calculations of a series of 3d transition metal atoms (Mn, Fe, Co) adsorbed on the heavy-element superconductor Re that the increase of the Kondo coupling and sign change in magnetic anisotropy with d-state filling is accompanied by a shift of the YSR states through the energy gap of the substrate and a crossing of the Fermi level. The uncovered systematic trends enable the identification of the most promising candidates for the realization of topological superconductivity in arrays of similar systems.

cond-mat.supr-con↗

arXiv2018

Stabilizing spin systems via symmetrically tailored RKKY interactions

The spin of a single atom adsorbed on a substrate is a promising building block for future spintronics and quantum computation schemes. To process spin information and also for increased magnetic stability, these building blocks have to be coupled. For a single atom, a high symmetry of the environment is known to lead to increased spin stability. However, little is known about the role of the nature and symmetry of the magnetic couplings. Here, we study arrays of atomic spins coupled via the ubiquitous Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction, focusing on its two anisotropic parts: the Dzyaloshinskii-Moriya (DM) and the symmetric anisotropic exchange interactions. First, we show that the high spin stability of an iron trimer can be remotely detected by a nearby iron atom, and how the DM interaction can lead to its destabilization. Second, we find that adding more nearby iron atoms almost always leads to a destabilization of the trimer, due to a non-local effective transverse anisotropy originating in the symmetric anisotropic exchange interaction. This transverse anisotropy can be quenched only for highly symmetric structures, for which the spin lifetime of the array is increased by orders of magnitude.

cond-mat.mes-hall↗

arXiv2018

Non-collinear spin states in bottom-up fabricated atomic chains

Non-collinear spin states with unique rotational sense, such as chiral spin-spirals, are recently heavily investigated because of advantages for future applications in spintronics and information technology and as potential hosts for Majorana Fermions when coupled to a superconductor. Tuning the properties of such spin states, e.g., the rotational period and sense, is a highly desirable yet difficult task. Here, we experimentally demonstrate the bottom-up assembly of a spin-spiral derived from a chain of Fe atoms on a Pt substrate using the magnetic tip of a scanning tunneling microscope as a tool. We show that the spin-spiral is induced by the interplay of the Heisenberg and Dzyaloshinskii-Moriya components of the Ruderman-Kittel-Kasuya-Yosida interaction between the Fe atoms. The relative strengths and signs of these two components can be adjusted by the interatomic Fe distance, which enables tailoring of the rotational period and sense of the spin-spiral.

cond-mat.mes-hall↗

arXiv2017

Long spin relaxation times in a transition metal atom in direct contact to a metal substrate

Long spin relaxation times are a prerequisite for the use of spins in data storage or nanospintronics technologies. An atomic-scale solid-state realization of such a system is the spin of a transition metal atom adsorbed on a suitable substrate. For the case of a metallic substrate, which enables directly addressing the spin by conduction electrons, the experimentally measured lifetimes reported to date are on the order of only hundreds of femtoseconds. Here, we show that the spin states of iron atoms adsorbed directly on a conductive platinum substrate have an astonishingly long spin relaxation time in the nanosecond regime, which is comparable to that of a transition metal atom decoupled from the substrate electrons by a thin decoupling layer. The combination of long spin relaxation times and strong coupling to conduction electrons implies the possibility to use flexible coupling schemes in order to process the spin-information.

cond-mat.mes-hall↗

arXiv2013

Spin excitations of individual Fe atoms on Pt(111): impact of the site-dependent giant substrate polarization

We demonstrate using inelastic scanning tunneling spectroscopy (ISTS) and simulations based on density functional theory that the amplitude and sign of the magnetic anisotropy energy for a single Fe atom adsorbed onto the Pt(111) surface can be manipulated by modifying the adatom binding site. Since the magnitude of the measured anisotropy is remarkably small, up to an order of magnitude smaller than previously reported, electron-hole excitations are weak and thus the spin-excitation exhibits long lived precessional lifetimes compared to the values found for the same adatom on noble metal surfaces.

cond-mat.mes-hall↗

arXiv2013

Finding the Rashba-type spin-splitting from interband scattering in quasiparticle interference maps

We have studied the BiCu$_2$/Cu(111) surface alloy using low-temperature scanning tunneling microscopy and spectroscopy. We observed standing waves caused by scattering off defects and step edges. Different from previous studies on similar Rashba-type surfaces, we identified multiple scattering vectors that originate from various intraband as well as interband scattering processes. A detailed energy-dependent analysis of the standing-wave patterns enables a quantitative determination of band dispersions, including the Rashba splitting. The results are in good agreement with ARPES data and demonstrate the usefulness of this strategy to determine the band structure of Rashba systems. The lack of other possible scattering channels will be discussed in terms of spin conservation and hybridization effects. The results open new possibilities to study spin-dependent scattering on complex spin-orbit coupled surfaces.

cond-mat.mtrl-sci↗