Key spin transport phenomena, including magnetoresistance and spin transfer torque, cannot be activated without spin-polarized currents, in which one electron spin is dominant. At the nanoscale, the relevant length-scale for modern spintronics, spin current generation is rather limited due to unwanted contributions from poorly spin-polarized frontier states in ferromagnetic electrodes, or too short length-scales for efficient spin splitting by spin-orbit interaction and magnetic fields. Here, we show that spin-polarized currents can be generated in silver-vanadocene-silver single molecule junctions without magnetic components or magnetic fields. In some cases, the measured spin currents approach the limit of ideal ballistic spin transport. Comparison between conductance and shot-noise measurements to detailed calculations reveals a mechanism based on spin-dependent quantum interference that yields very efficient spin filtering. Our findings pave the way for nanoscale spintronics based on quantum interference, with the advantages of low sensitivity to decoherence effects and the freedom to use non-magnetic materials.
Photoluminescence (PL) of CdSe nanocrystals (NCs) is known to be quenched when the NCs are capped with dithiols, because the redox levels of dithiols are located above the valence band edge of the NCs and thereby trap photogenerated holes. We locate the conduction and valence-band edges of the NCs and determine the redox levels via scanning tunneling spectroscopy (STS) studies to provide direct evidence of hole trapping and thereby PL quenching. In this regard, we have varied the chain length of dithiol ligands and also considered a range of diameters of CdSe NCs. We also characterized CdTe NCs that even after dithiol capping are known to yield PL emission. The STS studies provided band edges of the NCs and redox levels of the stabilizers in relation to PL quenching/emission in the dithiol-capped CdSe and CdTe NCs.
We have grown gold (Au) and copper-zinc-tin-sulfide (CZTS) nanocrystals and Au-CZTS core-shell nanostructures, with gold in the core and the semiconductor in the shell layer, through a high-temperature colloidal synthetic approach. Following usual characterization, we formed ultrathin layers of these in order to characterize the nanostructures in an ultrahigh-vacuum scanning tunneling microscope. Scanning tunneling spectroscopy of individual nanostructures showed the memristor effect or resistive switching from a low- to a high-conducting state upon application of a suitable voltage pulse. The Au-CZTS core-shell nanostructures also show a multilevel memristor effect with the nanostructures undergoing two transitions in conductance at two magnitudes of voltage pulse. We have studied the reproducibility, reversibility, and retentivity of the multilevel memristors. From the normalized density of states (NDOS), we infer that the memristor effect is correlated to a decrease in the transport gap of the nanostructures. We also infer that the memristor effect occurs in the nanostructures due to an increase in the density of available states upon application of a voltage pulse.
Core-shell nanocrystals having a type-I band-alignment confine charge carriers to the core. In this work, we choose CdSe/CdS core-shell nano-heterostructures that evidence confinement of holes only. Such a selective confinement occurs in the core-shell nanocrystals due to a low energy-offset of conduction band (CB) edges resulting in delocalization of electrons and thus a decrease in the conduction band-edge. Since the delocalization occurs through a thermal assistance, we study temperature dependence of selective delocalization process through scanning tunneling spectroscopy. From the density of states (DOS), we observe that the electrons are confined to the core at low temperatures. Above a certain temperature, they become delocalized up to the shell leading to a decrease in the CB of the core-shell system due to widening of quantum confinement effect. With holes remaining confined to the core due to a large offset in the valence band (VB), we record the topography of the core-shell nanocrystals by probing their CB and VB edges separately. The topographies recorded at different temperatures representing wave-functions of electrons and holes corresponded to the results obtained from the DOS spectra. The results evidence temperature-dependent wave-function delocalization of one-type of carriers up to the shell layer in core-shell nano-heterostructures.
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