Note:The published version in Nature Materials contains an extended manuscript and comprehensive supplementary information. . One of the primary experimental methods to reveal the mechanisms behind electronic transport through metal-molecule interfaces is the study of conductance as a function of molecule length in molecular junctions [4][5][6][7][8][9][10][11][12][13][14] . Previous studies focused on transport governed either by coherent tunneling or hopping, both at low conductance. However, the upper limit of conductance across molecular junctions has not been explored, despite the great potential for efficient information transfer, charge injection and recombination processes at high conductance. Here, we study the conductance properties of highly transmitting metal-molecule-metal interfaces, using a series of single-molecule junctions based on oligoacenes with increasing length. We find that the conductance saturates at an upper limit where it is independent of molecule length. Furthermore, we show that this upper limit can be controlled by the character of the orbital hybridization at the metal-molecule interface. Using two prototype systems, in which the molecules are contacted by either Ag or Pt electrodes, we reveal two different origins for the saturation of conductance. In the case of Ag-based molecular junctions, the conductance saturation is ascribed to a competition between energy level alignment and level broadening, while in the case of Pt-based junctions, the saturation is attributed to a band-like transport. The results are explained by an intuitive model, backed by ab-initio transport calculations. Our findings shed light on the mechanisms that constrain the conductance at the high transmission limit, providing guiding principles for the design of highly conductive metal-molecule interfaces.In order to study the conductance characteristics of highly transmitting molecular junctions, strong electronic coupling is required between the molecule and the electrodes, as well as within the molecule itself 10,11,15,16 . These conditions are achieved in this work by direct hybridization between the π-orbitals of the oligoacene molecules and the frontier orbitals of the metal electrodes, without employing anchoring groups such as thiols that can act as spacers between the orbitals of the molecular backbone and the frontier orbitals of the metal 13,15 . The oligoacenes (Fig. 1a) are linear π-conjugated molecules that can be viewed as short graphene nanoribbons 17 , whose electronic structure is subject to an ongoing research 18 . We study the evolution of conductance as a function of molecule length and compare the conductance characteristics of

Local magnetic imaging at nanoscale resolution is desirable for basic studies of magnetic materials and for magnetic logic and memories. However, such local imaging is hard to achieve by means of standard magnetic force microscopy. Other techniques require low temperatures, high vacuum, or strict limitations on the sample conditions. A simple and robust method is presented for locally resolved magnetic imaging based on short‐range spin‐exchange interactions that can be scaled down to atomic resolution. The presented method requires a conventional AFM tip functionalized with a chiral molecule. In proximity to the measured magnetic sample, charge redistribution in the chiral molecule leads to a transient spin state, caused by the chiral‐induced spin‐selectivity effect, followed by the exchange interaction with the imaged sample. While magnetic force microscopy imaging strongly depends on a large working distance, an accurate image is achieved using the molecular tip in proximity to the sample. The chiral molecules' spin‐exchange interaction is found to be 150 meV. Using the tip with the adsorbed chiral molecules, two oppositely magnetized samples are characterized, and a magnetic imaging is performed. This method is simple to perform at room temperature and does not require high‐vacuum conditions.

Hybrid ferromagnetic/superconducting systems are well known for hosting intriguing phenomena such as emergent triplet superconductivity at their interfaces and the appearance of in-gap, spin polarized Yu-Shiba-Rusinov (YSR) states bound to magnetic impurities on a superconducting surface. In this work we demonstrate that similar phenomena can be induced on a surface of a conventional superconductor by chemisorbing non-magnetic chiral molecules.Conductance spectra measured on NbSe2 flakes over which chiral alpha helix polyalanine molecules were adsorbed, exhibit, in some cases, in-gap states nearly symmetrically positioned around zero bias that shift with magnetic field, akin to YSR states, as corroborated by theoretical simulations. Other samples show evidence for a collective phenomenon of hybridized YSR-like states giving rise to unconventional, possibly triplet superconductivity, manifested in the conductance spectra by the appearance of a zero bias conductance that diminishes, but does not split, with magnetic field. The transition between these two scenarios appears to be governed by the density of adsorbed molecules.

When an electron passes through a chiral molecule, there is a high probability for correlation between the momentum and spin of the charge, thus leading to a spin polarized current. This phenomenon is known as the chiralinduced spin selectivity (CISS) effect. One of the most surprising experimental results recently demonstrated is that magnetization reversal in a ferromagnet with perpendicular anisotropy can be realized solely by chemisorbing a chiral molecular monolayer without applying any current or external magnetic field. This result raises the currently open question of whether this effect is due to the bonding event, held by the ferromagnet, or a long-time-scale effect stabilized by exchange interactions. In this work we have performed vectorial magnetic field measurements of the magnetization reorientation of a ferromagnetic layer exhibiting perpendicular anisotropy due to CISS using nitrogen-vacancy centers in diamond and followed the time dynamics of this effect. In parallel, we have measured the molecular monolayer tilt angle in order to find a correlation between the time dependence of the magnetization reorientation and the change of the tilt angle of the molecular monolayer. We have identified that changes in the magnetization direction correspond to changes of the molecular monolayer tilt angle, providing evidence for a long-time-scale characteristic of the induced magnetization reorientation. This suggests that the CISS effect has an effect over long time scales which we attribute to exchange interactions. These results offer significant insights into the fundamental processes underlying the CISS effect, contributing to the implementation of CISS in state-of-the-art applications such as spintronic and magnetic memory devices.

The spin–spin interactions between chiral molecules and ferromagnetic metals were found to be strongly affected by the chiral induced spin selectivity effect. Previous works unraveled two complementary phenomena: magnetization reorientation of ferromagnetic thin film upon adsorption of chiral molecules and different interaction rate of opposite enantiomers with a magnetic substrate. These phenomena were all observed when the easy axis of the ferromagnet was out of plane. In this work, the effects of the ferromagnetic easy axis direction, on both the chiral molecular monolayer tilt angle and the magnetization reorientation of the magnetic substrate, are studied using magnetic force microscopy. We have also studied the effect of an applied external magnetic field during the adsorption process. Our results show a clear correlation between the ferromagnetic layer easy axis direction and the tilt angle of the bonded molecules. This tilt angle was found to be larger for an in plane easy axis as compared to an out of plane easy axis. Adsorption under external magnetic field shows that magnetization reorientation occurs also after the adsorption event. These findings show that the interaction between chiral molecules and ferromagnetic layers stabilizes the magnetic reorientation, even after the adsorption, and strongly depends on the anisotropy of the magnetic substrate. This unique behavior is important for developing enantiomer separation techniques using magnetic substrates.