Imaging nanomagnetism and magnetic phase transitions in atomically thin CrSBr.

Since their first observation in 2017, atomically thin van der Waals (vdW) magnets have attracted significant fundamental, and application-driven attention. However, their low ordering temperatures, Tc, sensitivity to atmospheric conditions and difficulties in preparing clean large-area samples still present major limitations to further progress, especially amongst van der Waals magnetic semiconductors. The remarkably stable, high-Tc vdW magnet CrSBr has the potential to overcome these key shortcomings, but its nanoscale properties and rich magnetic phase diagram remain poorly understood. Here we use single spin magnetometry to quantitatively characterise saturation magnetization, magnetic anisotropy constants, and magnetic phase transitions in few-layer CrSBr by direct magnetic imaging. We show pristine magnetic phases, devoid of defects on micron length-scales, and demonstrate remarkable air-stability down the monolayer limit. We furthermore address the spin-flip transition in bilayer CrSBr by imaging the phase-coexistence of regions of antiferromagnetically (AFM) ordered and fully aligned spins. Our work will enable the engineering of exotic electronic and magnetic phases in CrSBr and the realization of novel nanomagnetic devices based on this highly promising vdW magnet.

Scanning Nitrogen-Vacancy Magnetometry of Focused-Electron-Beam-Deposited Cobalt Nanomagnets.

Focused-electron-beam-induced deposition is a promising technique for patterning nanomagnets in a single step. We fabricate cobalt nanomagnets in such a process and characterize their content, saturation magnetization, and stray magnetic field profiles by using a combination of transmission electron microscopy and scanning nitrogen-vacancy (NV) magnetometry. We find agreement between the measured stray field profiles and saturation magnetization with micromagnetic simulations. We further characterize magnetic domains and grainy stray magnetic fields in the nanomagnets and their halo side-deposits. This work may aid in the evaluation of Co nanomagnets produced through focused electron-beam-induced deposition for applications in spin qubits, magnetic field sensing, and magnetic logic.

Adsorption of squaraine molecules to Au(111) and Ag(001) surfaces.

The adsorption of anilino squaraines, an important chromophore for the use in organic solar cells, to Ag(001) and Au(111) has been studied with scanning tunneling microscopy. Self-assembly into square building blocks with eight molecules per unit cell is revealed on the Ag surface, while no ordering effects occur on gold. The squaraine-silver interaction is mediated by the carbonyl and hydroxyl oxygens located in the center of the molecule. The intermolecular coupling, on the other hand, is governed by hydrogen bonds formed between the terminal isobutyl groups and oxygen species of adjacent molecules. The latter gets maximized by rotating the molecules by a few degrees against a perfect square alignment. A similar molecular pattern does not form on Au(111) due to symmetry mismatch. Moreover, the high electronegativity of gold reduces the directing effect of oxygen-metal bonds that trigger the ordering process on silver. As a consequence, only frustrated three-fold symmetric units that do not expand into an ordered molecular network are present on the gold surface.

Incorrect DFT-GGA predictions of the stability of non-stoichiometric/polar dielectric surfaces: the case of Cu2O(111).

Scanning tunneling microscopy (STM) and hybrid density functional theory (DFT) have been used to study the stability and electronic characteristics of the Cu2O(111) surface. We challenge previous interpretations of its structure and composition and show that only appropriate (hybrid) calculations can correctly account for the relative thermodynamic stability of stoichiometric versus Cu-deficient terminations. Our theoretical finding of the stoichiometric surface to be most stable at oxygen-lean conditions is confirmed by an excellent matching between STM spectroscopy data and the calculated surface electronic structure. Beyond the specific case of the Cu2O(111) surface, and beyond the known deficiencies of GGA-based approaches in the description of oxide electronic structures, our work highlights the risk of an erroneous evaluation of the surface stability, in cases where the energetics and electronic characteristics are strongly coupled, as in a wide class of polar and/or non-stoichiometric oxide surfaces.