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

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

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.Comment: 16 pages, 5 figure

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

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

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.Comment: Accepted manuscrip

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

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