Tunable tunnel barriers in a semiconductor via ionization of individual atoms.

We report scanning tunneling microscopy (STM) studies of individual adatoms deposited on an InSb(110) surface. The adatoms can be reproducibly dropped off from the STM tip by voltage pulses, and impact tunneling into the surface by up to ∼100×. The spatial extent and magnitude of the tunneling effect are widely tunable by imaging conditions such as bias voltage, set current and photoillumination. We attribute the effect to occupation of a (+/0) charge transition level, and switching of the associated adatom-induced band bending. The effect in STM topographic images is well reproduced by transport modeling of filling and emptying rates as a function of the tip position. STM atomic contrast and tunneling spectra are in good agreement with density functional theory calculations for In adatoms. The adatom ionization effect can extend to distances greater than 50 nm away, which we attribute to the low concentration and low binding energy of the residual donors in the undoped InSb crystal. These studies demonstrate how individual atoms can be used to sensitively control current flow in nanoscale devices.

Image of Dynamic Local Exchange Interactions in the dc Magnetoresistance of Spin-Polarized Current through a Dopant.

We predict strong, dynamical effects in the dc magnetoresistance of current flowing from a spin-polarized electrical contact through a magnetic dopant in a nonmagnetic host. Using the stochastic Liouville formalism we calculate clearly defined resonances in the dc magnetoresistance when the applied magnetic field matches the exchange interaction with a nearby spin. At these resonances spin precession in the applied magnetic field is canceled by spin evolution in the exchange field, preserving a dynamic bottleneck for spin transport through the dopant. Similar features emerge when the dopant spin is coupled to nearby nuclei through the hyperfine interaction. These features provide a precise means of measuring exchange or hyperfine couplings between localized spins near a surface using spin-polarized scanning tunneling microscopy, without any ac electric or magnetic fields, even when the exchange or hyperfine energy is orders of magnitude smaller than the thermal energy.

Strain Effects on the Energy-Level Alignment at Metal/Organic Semiconductor Interfaces.

Flexible and wearable devices are among the upcoming trends in the opto-electronics market. Nevertheless, bendable devices should ensure the same efficiency and stability as their rigid analogs. It is well-known that the energy barriers between the metal Fermi energy and the molecular levels of organic semiconductors devoted to charge transport are key parameters in the performance of organic-based electronic devices. Therefore, it is paramount to understand how the energy barriers at metal/organic semiconductor interfaces change with bending. In this work, we experimentally measure the interface energy barriers between a metallic contact and small semiconducting molecules. The measurements are performed in operative conditions, while the samples are bent by a controlled applied mechanical strain. We determine that energy barriers are not sensitive to bending of the sample, but we observe that the hopping transport of the charges in flat molecules can be tuned by mechanical strain. The theoretical model developed for this work confirms our experimental observations.

Impact of the Synthesis Method on the Solid-State Charge Transport of Radical Polymers.

There are conflicting reports in the literature about the presence of room temperature conductivity in poly(2,2,6,6-tetramethylpiperidinyloxy methacrylate) (PTMA), a redox active polymer with radical groups pendent to an insulating backbone. To understand the variability in the findings across the literature and synthetic methods, we prepared PTMA using three living methods - anionic, ATRP and RAFT polymerization. We find that all three synthetic methods produce PTMA with radical yields of 70 - 80%, controlled molecular weight, and low dispersity. Additionally, we used on-chip EPR to probe the robustness of radical content in solid films under ambient air and light, and found negligible change in the radical content over time. Electrically, we found that PTMA is highly insulating - conductivity in the range 10-11 S/cm - regardless of the synthetic method of preparation. These findings provide greater clarity for potential applications of PTMA in energy storage.