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The generation of topologically non-trivial magnetic configurations has been a pivotal topic in both basic and applied nanomagnetism research. Localized non-coplanar magnetic defects such as skyrmions or merons were found to interact strongly with currents, making them interesting candidates for future spintronics applications. Here, we study a low-symmetry bcc(110) system by spin-polarized scanning tunneling microscopy and an atomistic spin model using parameters obtained from first-principles calculations. We demonstrate how a delicate balance between energy terms generates both topologically trivial and non-trivial domain walls, depending on their crystallographic direction. The topological walls consist of merons and antimerons and the topological charge amounts to about 0.2/nm wall length. The incorporation of holes in the films facilitates the transition from an in-plane ferromagnetic ground state to a spin-spiral state. Both domain walls and spirals transition into isolated elongated magnetic skyrmions in applied magnetic fields, establishing low-symmetry systems as a versatile platform for spin-texture engineering.

Materials with antiferromagnetic order have recently emerged as promising candidates in spintronics based on their beneficial characteristics such as vanishing stray fields and ultra-fast dynamics. At the same time more complex localized non-coplanar magnetic states as for instance skyrmions are in the focus of applications due to their intriguing properties such as the topological Hall effect. Recently a conceptual shift has occurred to envision the use of such magnetic defects not only in one-dimensional race track devices but to exploit their unique properties in two-dimensional networks. Here we use local strain in a collinear antiferromagnet to induce non-coplanar domain wall junctions, which connect in a very specific way to form extended networks. We combine spin-polarized scanning tunneling microscopy with density functional theory to characterize the different building blocks of the network, and unravel the origin of the handedness of triple-junctions and the size of the arising topological orbital moments., Comment: Marie Sk{\l}odowska-Curie Actions, H2020-MSCA-ITN-2020; Project acronym SPEAR; Grant Agreement No. 955671

Diffusion on surfaces is a fundamental process in surface science, governing nanostructure and film growth, molecular self-assembly, and chemical reactions. Atom motion on non-magnetic surfaces has been studied extensively both theoretically and by real-space imaging techniques. For magnetic surfaces density functional theory (DFT) calculations have predicted strong effects of the magnetic state onto adatom diffusion, but to date no corresponding experimental data exists. Here, we investigate Co and Rh atoms on a hexagonal magnetic layer, using scanning tunneling microscopy (STM) and DFT calculations. Experimentally, we "kick" atoms by local voltage pulses and thereby initiate strictly one-dimensional motion which is dictated by the row-wise antiferromagnetic (AFM) state. Our calculations show that the one-dimensional motion of Co and Rh atoms results from conserving the Co spin direction during movement and avoiding high induced Rh spin moments, respectively. These findings demonstrate that magnetism can be a means to control adatom mobility., Comment: 5 main figures, 3 extended figures

Topological orbital moments can arise in non-coplanar spin structures even in the absence of spin-orbit coupling and a net topological orbital magnetization occurs for the triple-Q state and for isolated skyrmions. For atomic-scale skyrmion lattices, a significant effect can also be expected, however, no studies have been reported yet. Here, we observe via spin-polarized scanning tunneling microscopy a non-coplanar atomic-scale spin structure with a nearly square magnetic unit cell for a pseudomorphic Fe monolayer on three atomic Ir layers on the Re(0001) surface. Employing density functional theory (DFT) calculations we consider different skyrmionic lattices to find the magnetic ground state. By mapping the DFT total energies to an atomistic spin model we demonstrate that these spin textures are stabilized by the interplay of the Dzyaloshinskii-Moriya and four-spin interactions. We evaluate the emerging phenomena of the different non-coplanar magnetic states and find significant local topological orbital moments oriented perpendicular to the surface, which order in an antiferromagnetic fashion.

Clusters supported by solid substrates are prime candidates for heterogeneous catalysis and can be prepared in various ways. While mass-selected soft-landing methods are often used for the generation of monodisperse particles, self-assembly typically leads to a range of different cluster sizes. Here we show by scanning tunneling microscopy measurements that in the initial stages of growth Mn forms trimers on a close-packed hexagonal Ir surface, providing a route for self-organized monodisperse cluster formation on an isotropic metallic surface. For an increasing amount of Mn, first a phase with reconstructed monolayer islands is formed, until at full coverage a pseudomorphic Mn phase evolves which is the most densely packed one of the three different observed Mn phases on Ir(111). The magnetic state of both the reconstructed islands and the pseudomorphic film is found to be the prototypical antiferromagnetic N\'eel state with 120{\deg} spin rotation between all nearest neighbors in the hexagonal layer., Comment: Founded by Marie Sk{\l}odowska-Curie Actions; SPEAR project, with grant number 955671

We identify the triple-Q (3Q) state as magnetic ground state in Pd/Mn and Rh/Mn bilayers on Re(0001) using spin-polarized scanning tunneling microscopy and density functional theory. An atomistic model reveals that in general the 3Q state with tetrahedral magnetic order and zero net spin moment is coupled to a hexagonal atomic lattice in a highly symmetric orientation via the anisotropic symmetric exchange interaction, whereas other spin-orbit coupling terms cancel due to symmetry. Our experiments are in agreement with the predicted orientation of the 3Q state. A distortion from the ideal tetrahedral angles leads to other orientations of the 3Q state which, however, results in a reduced topological orbital magnetization compared to the ideal 3Q state., Comment: 15 pages, 4 figures

Complex magnetic order arises due to the competition of different interactions between the magnetic moments. Recently, there has been an increased interest in such states not only to unravel the fundamental physics involved, but also with regards to applications exploiting their unique interplay with moving electrons. Whereas it is the Dzyaloshinskii-Moriya interaction (DMI) that has attracted much attention because of its nature to induce non-collinear magnetic order including magnetic-field stabilized skyrmions, it is the frustration of exchange interactions that can drive magnetic order down to the nano-scale. On top of that, interactions between multiple spins can stabilize two-dimensional magnetic textures as zero-field ground states, known as multi-Q states. Here, we introduce a two-dimensional itinerant magnet with various competing atomic-scale magnetic phases. Using spin-polarized scanning tunneling microscopy we observe several zero-field uniaxial or hexagonal nano-scale magnetic states. First-principles calculations together with an atomistic spin model reveal that these states are stabilized by the interplay of frustrated exchange and higher-order interactions while the DMI is weak. Unexpectedly, it is found that not only non-collinear magnetic states arise, but that higher-order interactions can also lead to collinear nano-scale multi-Q states., Comment: 32 pages including methods and additional information, 6 figures and 5 additional figures

Spin-polarized scanning tunneling microscopy has been applied to study non-collinear spin textures of a Mn monolayer on a four-fold symmetric W(001) substrate revealing a zero-field spin spiral ground state and two different types of rotational domain walls. With an applied magnetic field of 9 T, we observe a coexistence of the spin spiral and the skyrmion phase, even though a previous theoretical study reported that the phase transition occurs at 18 T. The skyrmions show a roughly hexagonal arrangement despite the square lattice symmetry of the W(001) substrate. Based on a reduced set of energy parameters, we are able to describe the experimental findings and to analyze the topological properties of the rotational domain walls.

We report on the structural and magnetic properties of single and double atomic layers of Mn on a clean and unreconstructed Nb(110) substrate. Low-temperature scanning tunneling spectroscopy measurements reveal a proximity-induced superconducting state in the Mn thin films, which are found to grow pseudomorphically on the Nb surface. Spin-polarized scanning tunneling microscopy measurements reveal a c(2x2) antiferromagnetic order in the Mn layers, with an out-of-plane spin-orientation. First-principles density functional theory calculations confirm the experimentally observed magnetic state, which is understood as the consequence of a strong intra- and inter-layer nearest-neighbor antiferromagnetic exchange coupling. These results are expected to be of importance for the design and the investigation of novel superconducting antiferromagnetic spintronic systems., Comment: 13 pages, 4 figures

When magnetic skyrmions are moved via currents, they do not strictly travel along the path of the current, instead their motion also gains a transverse component. This so-called skyrmion Hall effect can be detrimental in potential skyrmion devices because it drives skyrmions towards the edge of their hosting material where they face potential annihilation. Here we experimentally modify a skyrmion model system - an atomic Pd/Fe bilayer on Ir(111) - by decorating the film edge with ferromagnetic Co/Fe patches. Employing spin-polarized scanning tunneling microscopy, we demonstrate that this ferromagnetic rim prevents skyrmion annihilation at the film edge and stabilizes skyrmions and target states in zero field. Furthermore, in an external magnetic field the Co/Fe rim can give rise to skyrmions pinned to the film edge. Spin dynamics simulations reveal how a combination of different attractive and repulsive skyrmion-edge interactions can induce such an edge-pinning effect for skyrmions., Comment: 10 pages, 8 figures

We demonstrate that topological-chiral magnetic interactions can play a key role for magnetic ground states in ultrathin films at surfaces. Based on density functional theory we show that significant chiral-chiral interactions occur in hexagonal Mn monolayers due to large topological orbital moments which interact with the emergent magnetic field. Due to the competition with higher-order exchange interactions superposition states of spin spirals such as the 2Q state or a distorted 3Q state arise. Simulations of spin-polarized scanning tunneling microscopy images suggest that the distorted 3Q state could be the magnetic ground state of a Mn monolayer on Re(0001).

We investigate magnetic domain walls in a single fcc Mn layer on Re(0001) employing spin-polarized STM, atom manipulation, and spin dynamics simulations. The low symmetry of the row-wise antiferromagnetic (1Q) state leads to a new type of domain wall which connects rotational 1Q domains by a transient 2Q state with characteristic 90$^\circ$ angles between neighboring magnetic moments. The domain wall properties depend on their orientation and their width of about 2 nm essentially results from a balance of Heisenberg and higher-order exchange interactions. Atom manipulation allows domain wall imaging with atomic spin-resolution, as well as domain wall positioning, and we demonstrate that the force to move an atom is anisotropic on the 1Q domain., Comment: 6 pages, 4 figures

As heavy analog of graphene, plumbene is a two-dimensional material with strong spin-orbit coupling effects. Using scanning tunneling microscopy (STM), we observe that Pb forms a flat honeycomb lattice on an Fe monolayer on Ir(111). In contrast, without the Fe layer, a c(2x4) structure of Pb on Ir(111) is found. We use density functional theory (DFT) calculations to rationalize these findings and analyze the impact of the hybridization on the plumbene band structure. In the unoccupied states the splitting of the Dirac cone by spin-orbit interaction is clearly observed while in the occupied states of the freestanding plumbene we find a band inversion that leads to the formation of a topologically non-trivial gap. Exchange splitting as mediated by the strong hybridization with the Fe layer drives a quantum spin Hall to quantum anomalous Hall state transition., Comment: 5 pages, 5 figures

Spin-polarized scanning tunneling microscopy is used to identify the magnetic state of different thin films on a Re(0001) substrate, which becomes superconducting below 1.7 K. All magnetic films contain an Fe/Ir interface, which is known to facilitate the emergence of non-collinear magnetic order. For Fe monolayers on ultra-thin Ir films of different thickness we find several different atomic-scale magnetic states. For Pd/Fe bilayers we find nano-scale spin spirals as magnetic ground states for Ir thicknesses of three and four atomic layers. In applied magnetic fields skyrmions emerge, and in remanence non-trivial magnetic textures survive. This demonstrates the possibility to prepare skryrmion-hosting magnetic films on superconducting substrates., Comment: 7 pages, 3 figures

We experimentally verify the existence of two model-type magnetic ground states which were previously predicted but so far unobserved. We find them in Mn monolayers on the Re(0001) surface using spin-polarized scanning tunneling microscopy. For fcc stacking of Mn the collinear row-wise antiferromagnetic state occurs, whereas for hcp Mn a three-dimensional spin structure appears, which is a superposition of three row-wise antiferromagnetic states and is known as triple-Q state. Density functional theory calculations elucidate the subtle interplay of different magnetic interactions to form these spin structures and provide insight into the role played by relativistic effects., Comment: 5 pages, 4 figures

Due to their exceptional topological and dynamical properties magnetic skyrmions - localized stable spin structures on the nanometre scale - show great promise for future spintronic applications. To become technologically competitive, isolated skyrmions with diameters below 10 nm that are stable at zero magnetic field and room temperature are desired. Despite finding skyrmions in a wide spectrum of materials, the quest for a material with these envisioned properties is still ongoing. Here we report zero field isolated skyrmions with diameters smaller than 5 nm coexisting with 1 nm thin domain walls in Rh/Co atomic bilayers on the Ir(111) surface. These spin structures are characterized by spin-polarized scanning tunnelling microscopy and can also be detected using non-spin-polarized tips due to a large non-collinear magnetoresistance. We demonstrate that sub-10 nm skyrmions are stabilised in these ferromagnetic Co films at zero field due to strong frustration of exchange interaction, together with Dzyaloshinskii-Moriya interaction and a large magnetocrystalline anisotropy.

Research on magnetic systems with broken inversion symmetry has been stimulated by the experimental proof of particle-like configurations known as skyrmions, whose non-trivial topological properties make them ideal candidates for spintronic technology. This class of materials enables Dzyaloshinskii-Moriya interactions (DMI) which favor the stabilization of chiral configurations. Recent advances in material engineering have shown that in confined geometries it is possible to stabilize skyrmionic configurations at zero field. Moreover, it has been shown that in systems based on Pd/Fe bilayers on top of Ir(111) surfaces skyrmions can be as small as a few nanometres in diameter. In this work we present scanning tunneling microscopy measurements of small Pd/Fe and Pd$_2$/Fe islands on Ir(111) that exhibit a variety of different spin textures, which can be reproduced using discrete spin simulations. These configurations include skyrmions and skyrmion-like states with extra spin rotations such as the target state, which have been of interest due to their promising dynamic properties. Furthermore, using simulations we analyze the stability of these skyrmionic textures as a function of island size, applied field and boundary conditions of the system. An understanding of the parameters and conditions affecting the stability of these magnetic structures in confined geometries is crucial for the development of energetically efficient and optimally sized skyrmion-based devices., Comment: 20 pages, 13 figures, Supplemental Material 16 pages

We present a comparison of the characteristics of the magnetic domain walls in an atomic monolayer of Co on Pt(111) and a Ni/Fe atomic bilayer on Ir(111), based on spin-polarized scanning tunneling microscopy measurements. In both cases, the films exhibit a roughly triangular dislocation line pattern created by epitaxial strain relief, as well as out-of-plane ferromagnetic order. Domains with opposite magnetization are separated by domain walls with a unique rotational sense, demonstrating the important role of the Dzyaloshinskii-Moriya interaction induced by the Co/Pt and the Fe/Ir interfaces. The domain walls in Co/Pt(111) are straight and usually found in geometrical constrictions of the film, where they can minimize their length. In contrast, the domain walls in Ni/Fe/Ir(111) follow complicated paths, which can be correlated to the structural triangular pattern. The comparison between the two systems shows that the structural patterns, despite their similarity, have a different impact on the domain walls. In the Co/Pt(111) case, the magnetic state is not influenced by the dislocation line network, in contrast to the Ni/Fe/Ir(111) system in which the formation of the walls is favored at specific positions of the structural pattern.

We use spin-polarized scanning tunneling microscopy and density functional theory (DFT) to study domain walls (DWs) and the Dzyaloshinskii-Moriya interaction (DMI) in epitaxial films of Co/Ir(111) and Pt/Co/Ir(111). Our measurements reveal DWs with fixed rotational sense on one monolayer of Co on Ir, with a wall width around 2.7 nm. With Pt islands on top, we observe that the DWs occur mostly in the uncovered Co/Ir areas, suggesting that the wall energy density is higher in the Pt/Co/Ir(111). From DFT we find an interfacial DMI that stabilizes N\'{e}el-type DWs with clockwise rotational sense. The calculated DW widths are in good agreement with the experimental observations. The total DMI nearly doubles from Co/Ir(111) to Pt/Co/Ir(111), however, in the latter case the DMI is almost entirely due to the Pt with only a minor Ir contribution. Therefore a simple additive effect, where both interfaces contribute significantly to the total DMI, is not observed for one atomic Co layer., Comment: 5 pages, 4 figures, 1 table

Magnetic skyrmions are localized nanometer-sized spin configurations with particle_like properties, which are envisioned to be used as bits in next_generation information technology. An essential step towards future skyrmion-based applications is to engineer key magnetic parameters for developing and stabilizing individual magnetic skyrmions. Here we demonstrate the tuning of the non_collinear magnetic state of an Fe double layer on an Ir111 substrate by loading the sample with atomic hydrogen. By using spin_polarized scanning tunneling microscopy, we discover that the hydrogenated system supports the formation of skyrmions in external magnetic fields, while the pristine Fe double layer does not. Based on ab initio calculations, we attribute this effect to the tuning of the Heisenberg exchange and the Dzyaloshinsky_Moriya interactions due to hydrogenation. In addition to interface engineering, hydrogenation of thin magnetic films offers a unique pathway to design and optimize the skyrmionic states in low_dimensional magnetic materials.

Spin-polarized scanning tunneling microscopy investigations reveal a significant increase of the magnetic period of spin spirals in three-atomic-layer-thick Fe films on Ir(111), from about 4nm at 8K to about 65nm at room temperature. We attribute this considerable influence of temperature on the magnetic length scale of noncollinear spin states to different exchange interaction coefficients in the different Fe layers. We thus propose a classical spin model which reproduces the experimental observations and in which the crucial feature is the presence of magnetically coupled atomic layers with different interaction strengths. This model might also apply for many other systems, especially magnetic multilayers., Comment: 5 pages, 2 figures

We investigate the impact of the local spin texture on the differential conductance by scanning tunneling microscopy. In the focus is the previously found non-collinear magnetoresistance, which originates from spin mixing effects upon electron hopping between adjacent sites with canted magnetic moments. In the present work it is studied with lateral resolution both for the zero magnetic field spin spiral state as well as for individual magnetic skyrmions at different magnetic field values. We analyze in detail the response of the differential conductance and find different dependencies of peak energy and peak intensity on the local properties of the non-collinear spin texture. We find that in the center of a skyrmion the peak energy and intensity scale roughly linear with the angle between nearest neighbor moments. Elsewhere in the skyrmion, where the non-collinearity is not isotropic and the magnetization quantization axis varies, the behavior of the peak energy is more complex., Comment: 6 pages, 5 figures, no supplemental information

Using spin-polarized scanning tunneling microscopy and density functional theory we demonstrate the occurrence of a novel type of noncollinear spin structure in Rh/Fe atomic bilayers on Ir(111). We find that higher-order exchange interactions depend sensitively on the stacking sequence. For fcc-Rh/Fe/Ir(111) frustrated exchange interactions are dominant and lead to the formation of a spin spiral ground state with a period of about 1.5 nm. For hcp-Rh/Fe/Ir(111) higher-order exchange interactions favor a double-row wise antiferromagnetic or "uudd" state. However, the Dzyaloshinskii- Moriya interaction at the Fe/Ir interface leads to a small angle of about 4{\deg} between adjacent magnetic moments resulting in a canted "uudd" ground state.

The large epitaxial stress induced by the misfit between a triple atomic layer Fe film and an Ir(111) substrate is relieved by the formation of a dense dislocation line network. Spin-polarized scanning tunneling microscopy (SP-STM) investigations show that the strain is locally varying within the Fe film and that this variation affects the magnetic state of the system. Two types of dislocation line regions can be distinguished and both exhibit spin spirals with strain-dependent periods (ranging from 3 nm to 10 nm). Using a simple micromagnetic model, we attribute the changes of the period of the spin spirals to variations of the effective exchange coupling in the magnetic film. This assumption is supported by the observed dependence of the saturation magnetic field on the spin spiral period. Moreover, magnetic skyrmions appear in an external magnetic field only in one type of dislocation line area, which we impute to the different pinning properties of the dislocation lines., Comment: 7 pages, 6 figures

Spin-polarized scanning tunneling microscopy is used to investigate the magnetic state of the Fe monolayer on Re(0001). Two coexisting atomic-scale non-collinear spin textures are observed with a sharp transition between them on the order of one atomic lattice spacing. A strict position correlation between the two spin states is observed both in experiments and in Monte Carlo simulations, demonstrating their strong coupling behavior., Comment: 5 pages, 3 figures

The influence of in-plane and canted magnetic fields on spin spirals and skyrmions in atomic bilayer islands of palladium and iron on an Ir(111) substrate is investigated by scanning tunnelling microscopy at low temperatures. It is shown that the spin spiral propagation direction is determined by the island's border which can be explained by equilibrium state calculations on a triangular lattice. By application of in-plane fields, the spin spiral reorientates its propagation direction and becomes distorted, thereby allowing a proof for its cycloidal nature. Furthermore, it is demonstrated that the skyrmions' shape is distorted in canted fields which allows to determine the sense of magnetisation rotation as enforced by the interfacial Dzyaloshinskii-Moriya interaction., Comment: 14 pages, 7 figures

An understanding of the pinning of magnetic skyrmions to defects is crucial for the development of future spintronic applications. While pinning is desirable for a precise positioning of magnetic skyrmions it is detrimental when they are to be moved through a material. We use scanning tunneling microscopy to study the interaction between atomic scale defects and magnetic skyrmions that are only a few nanometers in diameter. The studied pinning centers range from single atom inlayer defects and adatoms to clusters adsorbed on the surface of our model system. We find very different pinning strengths and identify preferred positions of the skyrmion. The interaction between a cluster and a skyrmion can be sufficiently strong for the skyrmion to follow when the cluster is moved across the surface by lateral manipulation with the STM tip.

Controlling magnetism with electric fields is a key challenge to develop future energy-efficient devices, however, the switching between inversion symmetric states, e.g. magnetization up and down as used in current technology, is not straightforward, since the electric field does not break time-reversal symmetry. Here, we demonstrate that local electric fields can be used to reversibly switch between a magnetic skyrmion and the ferromagnetic state. These two states are topologically inequivalent, and we find that the direction of an electric field directly determines the final state. This observation establishes the possibility to combine energy-efficient electric field writing with the recently envisaged skyrmion racetrack-type memories., Comment: 11 pages, 4 figures, 4 supplementary figures

Magnetic skyrmions are localised non-collinear spin textures with high potential for future spintronic applications. Skyrmion phases have been discovered in a number of materials and a focus of current research is the preparation, detection, and manipulation of individual skyrmions for an implementation in devices. Local experimental characterization of skyrmions has been performed by, e.g., Lorentz microscopy or atomic-scale tunnel magnetoresistance measurements using spin-polarised scanning tunneling microscopy. Here, we report on a drastic change of the differential tunnel conductance for magnetic skyrmions arising from their non-collinearity: mixing between the spin channels locally alters the electronic structure, making a skyrmion electronically distinct from its ferromagnetic environment. We propose this non-collinear magnetoresistance (NCMR) as a reliable all-electrical detection scheme for skyrmions with an easy implementation into device architectures.

The atomic-scale spin structure of individual isolated skyrmions in an ultrathin film is investigated in real space by spin-polarized scanning tunneling microscopy. Their axial symmetry as well as their unique rotational sense is revealed by using both out-of-plane and in-plane sensitive tips. The size and shape of skyrmions change as a function of magnetic field. An analytical expression for the description of skyrmions is proposed and applied to connect the experimental data to the original theoretical model describing chiral skyrmions. Thereby, the relevant material parameters responsible for skyrmion formation can be obtained., Comment: Accepted for publication in Phys. Rev. Lett. (2015)

We demonstrate a canted magnetization of biatomic zigzag Co chains grown on the 5 x 1 reconstructed Ir(001) surface using density functional theory calculations and spin-polarized scanning tunneling microscopy (SP-STM) experiments. Biatomic Co chains grow in three different structural configurations and are all in a ferromagnetic state. Two chain types possess high symmetry due to two equivalent atomic strands and an easy magnetization direction which is along one of the principal crystallographic axes. The easy magnetization axis of the zigzag Co chains is canted away from the surface normal by an angle of 33 degrees. This giant effect is caused by the broken chain symmetry on the substrate in combination with the strong spin-orbit coupling of Ir. SP-STM measurements confirm stable ferromagnetic order of the zigzag chains with a canted magnetization., Comment: 5 pages, 5 figures

Vector spin chirality is one of the fundamental characteristics of complex magnets. For a one-dimensional spin-spiral state it can be interpreted as the handedness, or rotational sense of the spiral. Here, using spin-polarized scanning tunneling microscopy, we demonstrate the occurrence of an atomic-scale spin-spiral in finite individual bi-atomic Fe chains on the (5x1)-Ir(001) surface. We show that the broken inversion symmetry at the surface promotes one direction of the vector spin chirality, leading to a unique rotational sense of the spiral in all chains. Correspondingly, changes in the spin direction of one chain end can be probed tens of nanometers away, suggesting a new way of transmitting information about the state of magnetic objects on the nanoscale., Comment: accepted by Physical Review Letters