The induction of unconventional superconductivity by twisting two layers of graphene a small angle was groundbreaking1, and since then has attracted widespread attention to novel phenomena caused by lattice or angle mismatch between two-dimensional (2D) materials2. While many studies address the influence of angle mismatch between layered 2D materials3-5 , the impact of the absorption alignment on the physical properties of planar molecules on 2D substrates has not been studied in detail. Using scanning probe microscopy (SPM) we show that individual cobalt phthalocyanine (CoPc) molecules adsorbed on the layered superconductor 2H-NbSe2 change drastically their charge and spin state when the symmetry axes of the molecule and the substrate are twisted with respect to each other. The CoPc changes from an effective spin-1/2 as found in gas-phase6 to a molecule with non-magnetic ground-state. On the latter we observe a singlet-triplet transition originating from an antiferromagnetic interaction between the central-ion spin and a distributed magnetic moment on the molecular ligands. Because the Ising superconductor 2H-NbSe2 lacks inversion symmetry and has large spin-orbit coupling7 this intramolecular magnetic exchange has significant non-collinear Dzyaloshinskii-Moriya (DM)8, 9 contribution.
The quantum anomalous Hall (QAH) effect - a macroscopic manifestation of chiral band topology at zero magnetic field - has only been experimentally realized by magnetic doping of topological insulators (1 - 3) and delicate design of Moire heterostructures (4 - 8). However, the seemingly simple bilayer graphene without magnetic doping or Moire engineering has long been predicted to host competing ordered states with QAH effects (9 - 11). Here, we explore states in bilayer graphene with conductance of 2 e2/h that not only survive down to anomalously small magnetic fields and up to temperatures o…
We have performed density functional theory calculations of graphene decorated with carbon adatoms, which bind at the bridge site of a C--C bond. Earlier studies have shown that the C adatoms have magnetic moments and have suggested the possibility of ferromagnetism with high Curie temperature. Here we propose to use a gate voltage to fine tune the magnetic moments from zero to 1$μ_B$ while changing the magnetic coupling from antiferromagnetism to ferromagnetism and again to antiferromagnetism. These results are rationalized within the Stoner and RKKY models. When the SCAN meta-GGA correction …
Controlling magnetic order in magnetic topological insulators (MTIs) is a key to developing spintronic applications with MTIs, and is commonly achieved by changing the magnetic doping concentration, which inevitably affects spin-orbit-coupling strength and the very topological properties. Here, we demonstrate tunable magnetic properties in topological heterostructures over a wide range, from a ferromagnetic phase with Curie temperature of around 100 K all the way to a paramagnetic phase, while keeping the overall chemical composition the same, by controlling the thickness of non-magnetic space…
The heat capacity of conduction electrons obtained from the Sommerfeld expansion is shown to be tunable via the Rashba and Dresselhaus spin-orbit coupling parameters. Using an AlInSb/InSb/AlInSb as a representative heterostructure with alterable well and asymmetric barrier regions, the heat capacity is found to be higher for the spin-down electrons and suffers a reduction for wider wells. A further lowering is obtained through the application of an uniaxial strain. Finally, we suggest a method to determine the spin lifetimes for spins relaxing via the D'yakonov-Perel' mechanism from experiment…
Magnetism is a prototypical phenomenon of quantum collective state, and has found ubiquitous applications in semiconductor technologies such as dynamic random access memory (DRAM). In conventional materials, it typically arises from the strong exchange interaction among the magnetic moments of d- or f-shell electrons. Magnetism, however, can also emerge in perfect lattices from non-magnetic elements. For instance, flat band systems with high density of states (DOS) may develop spontaneous magnetic ordering, as exemplified by the Stoner criterion. Here we report tunable magnetism in rhombohedra…
Engineered substrates offer a promising avenue towards graphene devices having tunable properties. In particular, topographically patterned substrates can expose unique behavior due to their ability to induce local variations in strain and electrostatic doping. However, to explore the range of possible science and applications, it is important to create topographic substrates which both have tunable features and are suitable for transport measurements. In this Letter we describe the fabrication of tunable, topographically patterned substrates suitable for transport measurements. We report both…
Emergence of $π$-magnetism in open-shell nanographenes has been theoretically predicted decades ago but their experimental characterization was elusive due to the strong chemical reactivity that makes their synthesis and stabilization difficult. In recent years, on-surface synthesis under vacuum conditions has provided unprecedented opportunities for atomically precise engineering of nanographenes, which in combination with scanning probe techniques have led to a substantial progress in our capabilities to realize localized electron spin states and to control electron spin interactions at the …
We present a density functional theory study of the carrier-density and strain dependence of magnetic order in two-dimensional (2D) MAX$_3$ (M= V, Cr, Mn, Fe, Co, Ni; A= Si, Ge, Sn, and X= S, Se, Te) transition metal trichalcogenides. Our {\em ab initio} calculations show that this class of compounds includes wide and narrow gap semiconductors and metals and half-metals, and that most of these compounds are magnetic. Although antiferromagnetic order is most common, ferromagnetism is predicted in MSiSe$_3$ for M= Mn, Ni, in MSiTe$_3$ for M= V, Ni, in MnGeSe$_3$, in MGeTe$_3$ for M=Cr, Mn, Ni, i…
Removing a single-carbon vacancy introduces (quasi-)localized states for both and electrons in graphene. Interactions between the localized dangling bond and quasilocalized electrons of a single-carbon vacancy in graphene are predicted to control its magnetism. However, experimentally confirming this prediction through manipulating the interactions between the and electrons remains an outstanding challenge. Here we report the manipulation of magnetism of individual single-carbon vacancy in graphene by using a scanning tunnelling microscopy (STM) tip. Our spin-polarized STM measurements, comple…
Magnetic carbon nanostructures are currently under scrutiny for a wide spectrum of applications. Here, we theoretically investigate armchair graphene nanoribbons patterned with asymmetric edge extensions consisting of laterally fused naphtho groups, as recently fabricated via on-surface synthesis. We show that an individual edge extension acts as a spin-$\frac{1}{2}$ center and develops a sizable spin-polarization of the conductance around the band edges. The Heisenberg exchange coupling between a pair of edge extensions is dictated by the position of the second naphtho group in the carbon bac…
Graphene is a nonmagnetic semimetal and cannot be directly used as electronic or spintronic devices. We demonstrate that graphene quantum dots (GQDs) can exhibit strong edge magnetism and tunable energy gaps due to the presence of localized edge states. By using large-scale first principle density functional theory (DFT) calculations and detailed analysis based on model Hamiltonians, we can show that the zigzag edge states in GQDs become much stronger and more localized as the system size increases. The enhanced edge states induce strong electron-electron interactions along the edges of GQDs, …
Artificial spin ice systems have opened experimental windows into a range of model magnetic systems through the control of interactions among nanomagnet moments. This control has previously been enabled by altering the nanomagnet size and the geometry of their placement. Here we demonstrate that the interactions in artificial spin ice can be further controlled by including a soft ferromagnetic underlayer below the moments. Such a substrate also breaks the symmetry in the array when magnetized, introducing a directional component to the correlations. Using spatially resolved magneto-optical Ker…
The discovery of archetypal two-dimensional (2D) materials provides enormous opportunities in both fundamental breakthroughs and device applications, as evident by the research booming in graphene, atomically thin transition-metal chalcogenides, and few-layer black phosphorous in the past decade. Here, we report a new, large family of semiconducting dialkali-metal monochalcogenides (DMMCs) with an inherent A$_{2}$X monolayer structure, in which two alkali sub-monolayers form hexagonal close packing and sandwich the triangular chalcogen atomic plane. Such unique lattice structure leads to extra…
Inducing magnetism in graphene holds great promises, such as controlling the exchange interaction with a gate electrode and generating exotic magnetic phases. Coating graphene with magnetic molecules or atoms has so far mostly lead to decreased graphene mobility. In the present work, we show that Pt-porphyrins adsorbed on graphene lead to an enhanced mobility and to gate-dependent magnetism. We report that porphyrins can be donor or acceptor, depending on graphene s initial doping. The porphyrins transfer charge and ionize around the charged impurities on graphene, decreasing the graphene dopi…
Twisted graphene bilayers provide a versatile platform to engineer metamaterials with novel emergent properties by exploiting the resulting geometric moiré superlattice. Such superlattices are known to host bulk valley currents at tiny angles ($α\approx 0.3 ^\circ$) and flat bands at magic angles ($α\approx 1^\circ$). We show that tuning the twist angle to $α^*\approx 0.8^\circ$ generates flat bands away from charge neutrality with a triangular superlattice periodicity. When doped with $\pm 6$ electrons per moiré cell, these bands are half-filled and electronic interactions produce a symmetry-…
We report on a theoretical study of electronic and magnetic properties of hydrogen-saturated InSe nanoribbons (H-ZISNs). Based on hybrid-functional first-principles calculations, we find that H-ZISNs exhibit tunable half-metallicity and short-range ferromagnetic order. We first show that p-type doping turns narrow H-ZISNs from semimetal to half-metal with spin-polarization along In-terminated edge. This behavior is further analyzed in terms of a two-band tight-binding model, which provides a tractable description of the H-ZISN electronic structure, and serves as a starting point for the determ…
We present a comprehensive theoretical study of the static spin response in HgTe quantum wells, revealing distinctive behavior for the topologically nontrivial inverted structure. Most strikingly, the q=0 (long-wave-length) spin susceptibility of the undoped topological-insulator system is constant and equal to the value found for the gapless Dirac-like structure, whereas the same quantity shows the typical decrease with increasing band gap in the normal-insulator regime. We discuss ramifications for the ordering of localized magnetic moments present in the quantum well, both in the insulating…
Lieb lattice, a two-dimensional edge-depleted square lattice, has been predicted to host various exotic electronic properties due to its unusual band structure, i.e., Dirac cone intersected by a flat band (Dirac-flat bands). Until now, although a few artificial Lieb lattices have been discovered in experiments, the realization of a Lieb lattice in a real material is still unachievable. In this article, based on tight-binding modeling and first-principles calculations, we predict that the two covalent organic frameworks (COFs), i.e., sp2C-COF and sp2N-COF, which have been synthesized in the rec…
The possible realization of dissipationless chiral edge current in a topological insulator / magnetic insulator heterostructure is based on the condition that the magnetic proximity exchange coupling at the interface is dominated by the Dirac surface states of the topological insulator. Here we report a polarized neutron reflectometry observation of Dirac electrons mediated magnetic proximity effect in a bulk-insulating topological insulator (Bi$_{0.2}$Sb$_{0.8}$)$_{2}$Te$_{3}$ / magnetic insulator EuS heterostructure. We are able to maximize the proximity induced magnetism by applying an elec…
Diverse interlayer tunability of physical properties of two-dimensional layers mostly lies in the covalent-like quasi-bonding that is significant in electronic structures but rather weak for energetics. Such characteristics result in various stacking orders that are energetically comparable but may significantly differ in terms of electronic structures, e.g. magnetism. Inspired by several recent experiments showing interlayer anti-ferromagnetically coupled CrI3 bilayers, we carried out first-principles calculations for CrI3 bilayers. We found that the anti-ferromagnetic coupling results from a…
Zigzag nanoribbons of monolayer graphene-like two-dimensional materials host spontaneous edge magnetism at the zigzag terminations, whose configuration controls the band gap. In this article, the edge magnetism of zigzag nanoribbons of bilayer hexagonal crystals are studied. The specific models of bilayer graphene and bilayer silicene are both studied. As the gated voltage increases, the total energy level, magnetic structure and band structures of the ground state and the first quasi-stable excited state are tuned. For certain region of the gated voltage, the band gaps of spin up and down are…
The study of novel 2D platforms implementing magnetism in tunable van der Waals (vdW) homo- and hetero-structures paves the way to innovative spintronics and magnetic devices. In this study, we unravel the intriguing properties of few-layer Nb$_3$I$_8$ vdW nanofilms from first principles, showing how and to what extent specific magnetic orderings can be tuned using several degrees of freedom, such as film thickness, stacking geometry, and strain or even a combination of them. All these aspects are explored here, giving a comprehensive view of this novel and promising magnetic material.
We investigate superconducting interference device (SQUID) with two asymmetric Josephson junctions coupled to a mechanical resonator embedded in the loop of the SQUID. We quantize this system in the case when the frequency of the mechanical resonator is much lower than the cavity frequency of the SQUID and in the case when they are comparable. In the first case, the radiation pressure and cross-Kerr type interactions arise and are modified by asymmetry. Cross-Kerr type coupling is the leading term at the extremum points where radiation pressure is zero. In the second case, the main interaction…
We study the spin relaxation in graphene due to magnetic moments induced by defects. We propose and employ in our studies a microscopic model that describes magnetic impurity scattering processes mediated by charge puddles. This model incorporates the spin texture related to the defect-induced state. We calibrate our model parameters using experimentally-inferred values. The results we obtain for the spin relaxation times are in very good agreement with experimental findings. Our study leads to a comprehensive explanation for the short spin relaxation times reported in the experimental literat…
We propose a realization of mechanically tunable Ruderman-Kittel-Kasuya-Yosida interaction in a double quantum dot nanoelectromechanical device. The coupling between spins of two quantum dots suspended above a metallic plate is mediated by conduction electrons. We show that the spin-mechanical interaction can be driven by a slow modulation of charge density in the metallic plate. We propose to use Stuckelberg oscillations as a sensitive tool for detection of the spin and charge states of the coupled quantum dots. Theory of mechanical back action induced by a dynamical spin-spin interaction is …
Van der Waals heterostructures combining two-dimensional magnetic and semiconducting layers constitute a promising platform for interfacing magnetism, electronics, and optics. Here, we use resonant optical reflection spectroscopy to the observe magnetic proximity effect in a gate-tunable MoSe$_2$/CrBr$_3$ heterostructure. High quality of the interface leads to a giant zero-field splitting of the K and K' valley excitons in MoSe$_2$, equivalent to an external magnetic field of 12 T, with a weak but distinct electric field dependence that hints at potential for electrical control of magnetizatio…
