Spin-polarized Scanning Tunneling Microscopy Research Articles

Atomic-scale visualization of a cascade of magnetic orders in the layered antiferromagnet GdTe3

GdTe3 is a layered antiferromagnet which has attracted attention due to its exceptionally high mobility, distinctive unidirectional incommensurate charge density wave (CDW), superconductivity under pressure, and a cascade of magnetic transitions between 7 and 12 K, with as yet unknown order parameters. Here, we use spin-polarized scanning tunneling microscopy to directly image the charge and magnetic orders in GdTe3. Below 7 K, we find a striped antiferromagnetic phase with twice the periodicity of the Gd lattice and perpendicular to the CDW. As we heat the sample, we discover a spin density wave with the same periodicity as the CDW between 7 and 12 K; the viability of this phase is supported by our Landau free energy model. Our work reveals the order parameters of the magnetic phases in GdTe3 and shows how the interplay between charge and spin can generate a cascade of magnetic orders.

Evidence of Ferromagnetism and Ultrafast Dynamics of Demagnetization in an Epitaxial FeCl2 Monolayer.

The development of two-dimensional (2D) magnetism is driven not only by the interest of low-dimensional physics but also by potential applications in high-density miniaturized spintronic devices. However, 2D materials possessing a ferromagnetic order with a relatively high Curie temperature (Tc) are rare. In this paper, the evidence of ferromagnetism in monolayer FeCl2 on Au(111) surfaces, as well as the interlayer antiferromagnetic coupling of bilayer FeCl2, is characterized by using spin-polarized scanning tunneling microscopy. A Curie temperature (Tc) of ∼147 K is revealed for monolayer FeCl2, based on our static magneto-optical Kerr effect measurements. Furthermore, temperature-dependent magnetization dynamics is investigated by the time-resolved magneto-optical Kerr effect. A transition from one- to two-step demagnetization occurs as the lattice temperature approaches Tc, which supports the Elliott-Yafet spin relaxation mechanism. The findings contribute to a deeper understanding of the underlying mechanisms governing ultrafast magnetization in 2D ferromagnetic materials.

Hidden non-collinear spin-order induced topological surface states

Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2 K below the Néel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism.

Growth and surface magnetism of ultrathin Cr(001) films

We investigate the growth of ultrathin Cr films on a Au(001) surface and observe that the growth of 1.5 nm thick Cr layers at 290 K, followed by post-annealing at 520 K, results in high-quality epitaxial Cr(001) films with atomically flat large terraces and distinct surface states. Subsequently, these optimized growth conditions are successfully applied to the growth of 1 nm and 3 nm thick Cr films. Magnetic imaging of 1 and 1.5 nm thick Cr(001) films prepared under the optimized growth conditions is performed using spin-polarized scanning tunneling microscopy. Distinct magnetic contrasts featuring a topological antiferromagnetic (TAF) order are observed in both films; however, spin frustration originating from the density of screw dislocations for both films shows a significant difference. The 1.0 nm thick Cr film, which exhibits a clear TAF order with the suppression of a large spin-frustrated area, is suitable for application to spin-electronic devices.

Probing Spin-Dependent Ballistic Charge Transport at Single-Nanometer Length Scales.

The coherent transport of charge and spin is a key requirement of future devices for quantum computing and communication. Scattering at defects or impurities may significantly reduce the coherence of quantum-mechanical states, thereby affecting the device functionality. While numerous methods exist to experimentally assess charge transport, the real-space detection of a material's ballistic spin transport properties with nanometer resolution remains a challenge. Here we report on a novel approach that utilizes a combination of spin-polarized scanning tunneling microscopy (SP-STM) and the recently introduced molecular nanoprobe (MONA) technique. It relies on the local injection of spin-polarized charge carriers from a magnetic STM tip and their detection by a single surface-deposited phthalocyanine molecule via reversible electron-induced tautomerization events. Based on the particular electronic structure of the Rashba alloy BiAg2, which is governed by a spin-momentum-locked surface state, we prove that the current direction inverses upon tip magnetization reversal.

Spin-Selective Electron Transport Through Single Chiral Molecules.

The interplay between chirality and magnetism is a source of fascination among scientists for over a century. In recent years, chirality-induced spin selectivity (CISS) has attracted renewed interest. It is observed that electron transport through layers of homochiral molecules leads to a significant spin polarization of several tens of percent. Despite the abundant experimental evidence gathered through mesoscopic transport measurements, the exact mechanism behind CISS remains elusive. This study reports spin-selective electron transport through single helical aromatic hydrocarbons that are sublimed in vacuo onto ferromagnetic cobalt surfaces and examined with spin-polarized scanning tunneling microscopy (SP-STM) at a temperature of 5K. Direct comparison of two enantiomers under otherwise identical conditions revealed magnetochiral conductance asymmetries of up to 50% when either the molecular handedness is exchanged or the magnetization direction of the STM tip or Co substrate is reversed. Importantly, the results rule out electron-phonon coupling and ensemble effects as primary mechanisms responsible forCISS.

Hanle effect in transport through single atoms in spin-polarized STM

Following recent achievements in quantum-coherent manipulation and detection of individual atomic spins with the use of spin-polarized scanning tunneling microscope, we propose how to observe and utilize the Hanle effect in electronic transport in such setups. We show that the Hanle experiment can be used to observe the single spin precession driven by the intrinsic exchange field. This field is a result of virtual particle exchange processes, and its magnitude and sign can be controlled electrically. We also show that from detailed analysis of the Hanle resonance curve one can determine the spin relaxation time from dc current measurements.

Detecting the spin-polarization of edge states in graphene nanoribbons

Low dimensional carbon-based materials can show intrinsic magnetism associated to p-electrons in open-shell π-conjugated systems. Chemical design provides atomically precise control of the π-electron cloud, which makes them promising for nanoscale magnetic devices. However, direct verification of their spatially resolved spin-moment remains elusive. Here, we report the spin-polarization of chiral graphene nanoribbons (one-dimensional strips of graphene with alternating zig-zag and arm-chair boundaries), obtained by means of spin-polarized scanning tunnelling microscopy. We extract the energy-dependent spin-moment distribution of spatially extended edge states with π-orbital character, thus beyond localized magnetic moments at radical or defective carbon sites. Guided by mean-field Hubbard calculations, we demonstrate that electron correlations are responsible for the spin-splitting of the electronic structure. Our versatile platform utilizes a ferromagnetic substrate that stabilizes the organic magnetic moments against thermal and quantum fluctuations, while being fully compatible with on-surface synthesis of the rapidly growing class of nanographenes.

Evidence for a conical spin spiral state in the Mn triple layer on W(001): Spin-polarized scanning tunneling microscopy and first-principles calculations

Evidence for a conical spin spiral state in the Mn triple layer on W(001): Spin-polarized scanning tunneling microscopy and first-principles calculations

Fe-induced Kondo peak splitting in tip-functionalized scanning tunneling spectroscopy: A first-principles-based simulation

The spin-polarized scanning tunneling microscope (SP-STM) has been employed to enhance its capabilities of detecting the electronic and magnetic properties of organometallic molecules. Using a tip functionalized with a cobaltocene (Cc) molecule, recent SP-STM experiment performed on the Cu-tip/Cc/Fe/Cu(100) composite junction revealed an asymmetric Kondo resonance splitting in the differential conductance (dI/dV) spectrum. However, a systematic theoretical simulation of such system is lacking, and the important roles of the substrate spin-polarization and the Fe adatom still remain to be elucidated. In this work, by combining density functional theory and the hierarchical equations of motion methods, we achieve first-principles-based simulations of the tip control process of the Cu-tip/Cc/Fe/Cu(100) junction. We correctly reproduce the experimental results and demonstrate the influences of the Fe adatom on the spin-polarization of the substrate and on the Kondo resonance splitting in the dI/dV spectra.

Observation of skyrmion bubbles in multilayer [Pt/Co/Cu]n using spin-polarized STM

Magnetic multilayers are a promising platform for storage and logic devices based on skyrmion spin textures, due to the large materials phase space for tuning properties. Epitaxial superlattice structures of [Pt/Co/Cu]n thin films were grown by molecular beam epitaxy at room temperature. Spin-polarized scanning tunneling microscopy (SP-STM) of these samples was used to probe the connection between surface structure and skyrmion morphology with nanoscale spatial resolution. Irregular-shaped skyrmion bubbles were observed, with effective diameters from 20 to 200 nm that are much larger than the nanoscale grain structure of the surface topography. Nucleation, annihilation, and motion of skyrmion bubbles could be driven using the stray field of the ferromagnetic tip in repeated imaging, and spin-polarized current/voltage pulses. Our detailed comparison of STM topography and differential conductance images shows that there are no surface defects or inhomogeneities at length scales that could account for the range in skyrmion bubble size or shape observed in the measurements.

Optimizing tip-surface interactions in ESR-STM experiments

Electron-spin resonance carried out with scanning tunneling microscopes (ESR-STM) is a recently developed experimental technique that is attracting enormous interest on account of its potential to carry out single-spin on-surface resonance with subatomic resolution. Here we carry out a theoretical study of the role of tip-adatom interactions and provide guidelines for choosing the experimental parameters in order to optimize spin resonance measurements. We consider the case of the Fe adatom on a MgO surface and its interaction with the spin-polarized STM tip. We address three problems: first, how to optimize the tip-sample distance to cancel the effective magnetic field created by the tip on the surface spin, in order to carry out proper magnetic field sensing. Second, how to reduce the voltage dependence of the surface-spin resonant frequency, in order to minimize tip-induced decoherence due to voltage noise. Third, we propose an experimental protocol to infer the detuning angle between the applied field and the tip magnetization, which plays a crucial role in the modeling of the experimental results.

Single-Atomic-Layer Stanene on Ferromagnetic Co Nanoislands with Topological Band Structures.

Introducing magnetism to two-dimensional topological insulators is a central issue in the pursuit of magnetic topological materials in low dimensionality. By means of low-temperature growth at 80 K, we succeeded in fabricating a monolayer stanene on Co/Cu(111) and resolving ferromagnetic spin contrast by field-dependent spin-polarized scanning tunneling microscopy (SP-STM). Increases of both remanence to saturation magnetization ratio (Mr/Ms) and coercive field (Hc) due to an enhanced perpendicular magnetic anisotropy (PMA) are further identified by out-of-plane magneto-optical Kerr effect (MOKE). In addition to ultraflat stanene fully relaxed on bilayer Co/Cu(111) from density functional theory (DFT), characteristic topological properties including an in-plane s-p band inversion and a spin-orbit coupling (SOC) induced gap about 0.25 eV at the Γ̅ point have also been verified in the Sn-projected band structure. Interfacial coupling of single-atomic-layer stanene with ferromagnetic Co biatomic layers allows topological band features to coexist with ferromagnetism, facilitating a conceptual design of atomically thin magnetic topological heterostructures.

The influence of adatom diffusion on the formation of skyrmion lattice in sub-monolayer Fe on Ir(111)

Room temperature grown Fe monolayer (ML) on the Ir(111) single crystal substrate has attracted great research interests as nano-skyrmion lattice can form under proper growth conditions. The formation of the nanoscale skyrmion, however, appears to be greatly affected by the diffusion length of the Fe adatoms on the Ir(111) surface. We made this observation by employing spin-polarized scanning tunneling microscopy to study skyrmion formation upon systematically changing the impurity density on the substrate surface prior to Fe deposition. Since the substrate surface impurities serve as pinning centers for Fe adatoms, the eventual size and shape of the Fe islands exhibit a direct correlation with the impurity density, which in turn determines whether skyrmion can be formed. Our observation indicates that skyrmion only forms when the impurity density is below 0.006/nm2, i.e., 12 nm averaged spacing between the neighboring defects. We verify the significance of Fe diffusion length by growing Fe on clean Ir(111) substrate at low temperature of 30 K, where no skyrmion was observed to form. Our findings signify the importance of diffusion of Fe atoms on the Ir(111) substrate, which affects the size, shape and lattice perfection of the Fe islands and thus the formation of skyrmion lattice.

Antiferromagnetic domain formation and spin frustration induced by adjacent paired screw dislocations in 10 monolayer-thick Cr(001) films

We investigated the growth and surface morphology of 10 monolayer (ML)-thick Cr(001) films on clean Au(001) surfaces. High quality epitaxial Cr(001) films with large atomically flat terraces and distinct surface states were successfully fabricated through growth at 300 K and subsequent post-annealing at 520 K. At 300 K, spin-polarized scanning tunneling microscopy images of both the topological and magnetic structures of this Cr film were obtained. The magnetic images exhibited the following features: (1) The layered antiferromagnetic (AF) order appeared in adjacent terraces and one ML-depth shallow hole in the terraces; (2) significant spin frustrations induced by adjacent paired screw dislocations caused the AF domain formation with 90 degrees quantum axis rotation and a large spin frustration area, not always limited in the vicinity of screw dislocations. The feature (2) was qualitatively reproduced by the micromagnetic simulation. These findings may be essential for the further development of spin-electronics utilizing thin AF films.

Pair-Density-Wave and Chiral Superconductivity in Twisted Bilayer Transition Metal Dichalcogenides.

We theoretically explore possible orders induced by weak repulsive interactions in twisted bilayer transition metal dichalcogenides (e.g., WSe_{2}) in the presence of an out-of-plane electric field. Using renormalization group analysis, we show that superconductivity survives even with the conventional van Hove singularities. We find that topological chiral superconducting states with Chern number N=1, 2, 4 (namely, p+ip, d+id, and g+ig) appear over a large parameter region with a moiré filling factor around n=1. At some special values of applied electric field and in the presence of a weak out-of-plane Zeeman field, spin-polarized pair-density-wave (PDW) superconductivity can emerge. This spin-polarized PDW state can be probed by experiments such as spin-polarized STM measuring spin-resolved pairing gap and quasiparticle interference. Moreover, the spin-polarized PDW could lead to a spin-polarized superconducting diode effect.

Spin-Resolved Imaging of Antiferromagnetic Order in Fe4 Se5 Ultrathin Films on SrTiO3.

Unraveling the magnetic order in iron chalcogenides and pnictides at atomic scale is pivotal for understanding their unconventional superconducting pairing mechanism, but is experimentally challenging. Here, by utilizing spin-polarized scanning tunneling microscopy, real-space spin contrasts are successfully resolved to exhibit atomically unidirectional stripes in Fe4 Se5 ultrathin films, the plausible closely related compound of bulk FeSe with ordered Fe-vacancies, which are grown by molecular beam epitaxy. As is substantiated by the first-principles electronic structure calculations, the spin contrast originates from a pair-checkerboard antiferromagnetic ground state with in-plane magnetization, which is modulated by a spin-lattice coupling. These measurements further identify three types of nanoscale antiferromagnetic domains with distinguishable spin contrasts, which are subject to thermal fluctuations into short-ranged patches at elevated temperatures. This work provides promising opportunities in understanding the emergent magnetic order and the electronic phase diagram for FeSe-derived superconductors.

Valence Orbitals Driving the Spin Dynamics in a Rare-Earth Single-Atom Magnet.

We combine spin-polarized scanning tunneling microscopy with quantum master equation analysis to investigate the spin dynamics of the single atom magnet Dy on graphene/Ir(111). By performing reading and writing experiments, we show that the strongly spin polarized 5d6s valence shells, as well as their intra-atomic exchange coupling to the 4f shell, determine the pathways for magnetization relaxation and thus the spin dynamics. The good quantum number that determines which states are stable and which mechanisms for reversal exist in a given crystal field is the atomic total angular momentum J_{z}^{tot} and not the commonly considered J_{z}^{4f} of the 4f shell only.

Structure-property relationship of reversible magnetic chirality tuning

The Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction mediates collinear magnetic interactions via the conduction electrons of a nonmagnetic spacer, resulting in a ferro- or antiferromagnetic magnetization in magnetic multilayers. Recently it has been discovered that heavy nonmagnetic spacers are able to mediate an indirect magnetic coupling that is noncollinear and chiral. This Dzyaloshinskii-Moriya-enhanced RKKY interaction causes the emergence of a variety of interesting magnetic structures, such as skyrmions and spin spirals. Here, we show by spin-polarized scanning tunneling microscopy that the interchain coupling between manganese oxide chains on Ir(001) can reproducibly be switched from chiral to collinear antiferromagnetic by increasing the oxidation state of ${\mathrm{MnO}}_{2}$, while the reverse process can be induced by thermal reduction. The underlying structure--property relationship is revealed by low-energy electron diffraction intensity analysis. Density functional theory calculations suggest that the magnetic transition may be caused by a significant increase of the Heisenberg exchange which overrides the Dzyaloshinskii-Moriya interaction upon oxidation.

Tweezer-like magnetic tip control of the local spin state in the FeOEP/Pb(111) adsorption system: a preliminary exploration based on first-principles calculations.

The magnetic interactions between the spin-polarized scanning tunnelling microscopy (SP-STM) tip and the localized spin impurities lead to various forms of the Kondo effect. Although these intriguing phenomena enrich Kondo physics, detailed theoretical simulations and explanations are still lacking due to the rather complex formation mechanisms. Here, by combining density functional theory (DFT), complete active space self-consistent field (CASSCF) theory, and hierarchical equations of motion (HEOM) methods, we perform first-principles-based simulation to elaborate the regulation process of the magnetic Co-tip on the spin state and transport behaviour of FeOEP/Pb(111) system. Compared with the non-magnetic tip, the stronger interaction between the magnetic tip and FeOEP molecule results in a more drastic deformation of the molecular structure with more electron transfer from the local environment to Fe-3d orbitals. The magnetic anisotropy of FeOEP changes very drastically from positive values in the tunnelling region to negative values in the contact region. The ferromagnetic electron correlation between the magnetic tip and the molecule induces an asymmetric Kondo line-shape near the Fermi level. This work highlights that the DFT + CASSCF + HEOM approach can not only predict complex quantum phenomena and explain underlying physical mechanisms, but also facilitate the design of more fascinating quantum control experiments.