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Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI3. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI3, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI3 layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI3 tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing., Comment: 23 pages, 4 figures

CrBr$_{3}$ is a layered van der Waals material with magnetic ordering down to the 2D limit. For decades, based on optical measurements, it is believed that the energy gap of CrBr$_{3}$ is in the range of 1.68-2.1 eV. However, controversial results have indicated that the band gap of CrBr$_{3}$ is possibly smaller than that. An unambiguous determination of the energy gap is critical to the correct interpretations of the experimental results of CrBr$_{3}$. Here, we present the scanning tunneling microscopy and spectroscopy (STM/S) results of CrBr$_{3}$ thin and thick flakes exfoliated onto pyropytic graphite (HOPG) surfaces and density functional theory (DFT) calculations to reveal the small energy gap (peak-to-peak energy gap to be 0.57 eV $\pm$ 0.04 eV; or the onset signal energy gap to be 0.29 $\pm$ 0.05 eV from dI/dV spectra). Atomic resolution topography images show the defect-free crystal structure and the dI/dV spectra exhibit multiple peak features measured at 77 K. The conduction band - valence band peak pairs in the multi-peak dI/dV spectrum agree very well with all reported optical transitions. STM topography images of mono- and bi-layer CrBr$_{3}$ flakes exhibit edge degradation due to short air exposure (~15 min) during sample transfer. The unambiguously determined small energy gap settles the controversy and is the key in better understanding CrBr$_{3}$ and similar materials.

Materials' microstructure strongly influences its performance and is thus a critical aspect in design of functional materials. Previous efforts on microstructure mediated design mostly assume isotropy, which is not ideal when material performance is dependent on an underlying transport phenomenon. In this article, we propose an anisotropic microstructure design strategy that leverages Spectral Density Function (SDF) for rapid reconstruction of high resolution, two phase, isotropic or anisotropic microstructures in 2D and 3D. We demonstrate that SDF microstructure representation provides an intuitive method for quantifying anisotropy through a dimensionless scalar variable termed anisotropy index. The computational efficiency and low dimensional microstructure representation enabled by our method is demonstrated through an active layer design case study for Bulk Heterojunction Organic Photovoltaic Cells (OPVCs). Results indicate that optimized design, exhibiting strong anisotropy, outperforms isotropic active layer designs. Further, we show that Cross-sectional Scanning Tunneling Microscopy and Spectroscopy (XSTM/S) is as an effective tool for characterization of anisotropic microstructures.

The effects of the electric-field-assisted annealing on the bulk heterojunction nano-morphology in the P3HT/PCBM active layer of the organic photovoltaic cells (OPVCs) are presented here. It was widely accepted that the electric-field-assisted annealing will facilitate the P3HT, the polar polymer, to be better crystalline to enhance the charge mobility, hence the improvement of the OPVC performance. The influences on the nano-morphology of the electron donor and accepter domains are not well understood. Here, using the cross-sectional scanning tunneling microscopy and spectroscopy (XSTM/S), the electric-field-assisted annealing treatment is found to influence the molecular domains to be elongated with the orientation near the direction of the external electric field. The elongation of the molecular domains is believed to facilitate the domain percolation, which causes higher charge mobility, hence the higher short-circuit current density (Jsc). On the other hand, it was also observed that the electronic properties of the P3HT-rich and PCBM-rich domains in the electric-field-assisted annealed samples showed smaller energy band gaps and smaller molecular orbital offset between the two domains, which is argued to decrease the open circuit voltage (Voc) and negatively impact the OPVC performance. Based on the X-ray diffraction (XRD) and small angle X-ray scattering (SAXS) results, the altered electronic properties are argued to be due to the molecular intermixing induced doping effects. These results point out competing factors affecting the OPVC performance with the electric-field-assisted annealing treatment.

Cross-sectional scanning tunnelling microscopy and spectroscopy (XSTM/S) were used to map out the band alignment across the complex oxide interface of La$_{2/3}$Ca$_{1/3}$MnO$_{3}$/Nb-doped SrTiO$_{3}$. By a controlled cross-sectional fracturing procedure, unit-cell high steps persist near the interface between the thin film and the substrate in the non-cleavable perovskite materials. The abrupt changes of the mechanical and electronic properties were visualized directly by XSTM/S. Using changes in the DOS as probe by STM, the electronic band alignment across the heterointerface was mapped out providing a new approach to directly measure the electronic properties at complex oxide interfaces., Comment: 15 pages, 4 figures

Cross-sectional scanning tunneling microscopy was utilized to study fractured perovskie oxide surfaces. It was found for the non-cleavable perovskite oxide, SrTiO$_{3}$, that atomically flat terraces could be routinely created with a controlled fracturing procedure. Optical and scanning electron microscopy as well as a profilometer were used to obtain the information from sub-millimeter to sub-micrometer scales of the fractured surface topography., Comment: 9 pages, 4 figures