Kondo Resonances in Molecular Devices

Molecular electronic devices currently serve as a platform for studying a variety of physical phenomena only accessible at the nanometer scale. One such phenomenon is the highly correlated electronic state responsible for the Kondo effect, manifested here as a "Kondo resonance" in the conductance. Because the Kondo effect results from strong electron-electron interactions, it is not captured by the usual quantum chemistry approaches traditionally applied to understand chemical electron transfer. In this review we will discuss the origins and phenomenology of Kondo resonances observed in single molecule devices, focusing primarily on the spin-1/2 Kondo state arising from a single unpaired electron. We explore the rich physical system of a single-molecule device, which offers a unique spectroscopic tool for investigating the interplay of emergent Kondo behavior and such properties as molecular orbital transitions and vibrational modes. We will additionally address more exotic systems, such as higher spin states in the Kondo regime, and we will review recent experimental advances in the ability to manipulate and exert control over these nanoscale devices.Comment: 19 Pages, 17 Figure

Temperature-dependent contact resistances in high-quality polymer field-effect transistors

Contact resistances between organic semiconductors and metals can dominate the transport properties of electronic devices incorporating such materials. We report measurements of the parasitic contact resistance and the true channel resistance in bottom contact poly(3-hexylthiophene) (P3HT) field-effect transistors with channel lengths from 400 nm up to 40 $\mu$m, from room temperature down to 77 K. For fixed gate voltage, the ratio of contact to channel resistance decreases with decreasing temperature. We compare this result with a recent model for metal-organic semiconductor contacts. Mobilities corrected for this contact resistance can approach 1 cm$^{2}$/Vs at room temperature and high gate voltages.Comment: 10 pages, 4 figures, accepted to Appl. Phys. Let

Transport in organic semiconductors in large electric fields: From thermal activation to field emission

Understanding charge transport in organic semiconductors in large electric fields is relevant to many applications. We present transport measurements in organic field-effect transistors based on poly(3-hexylthiophene) and 6,13-bis(triisopropyl-silylethynyl) pentacene with short channels, from room temperature down to 4.2 K. Near 300 K transport in both systems is well described by thermally assisted hopping with Poole-Frenkel-like enhancement of the mobility. At low temperatures and large gate voltages, transport in both materials becomes nearly temperature independent, crossing over into field-driven tunneling. These data, particularly in TIPS-pentacene, show that great caution must be exercised when considering more exotic (e.g., Tomonaga-Luttinger Liquid) interpretations of transport.Comment: 3.5 pages, 3 figures. Corrected legend in Fig.

Zero-bias anomalies in electrochemically fabricated nanojunctions

A streamlined technique for the electrochemical fabrication of metal nanojunctions (MNJs) between lithographically defined electrodes is presented. The first low-temperature transport measurements in such structures reveal suppression of the conductance near zero-bias. The size of the zero-bias anomaly (ZBA) depends strongly on the fabrication electrochemistry and the dimensions of the resulting MNJ. We present evidence that the nonperturbative ZBA in atomic-scale junctions is due to a density of states suppression in the leads.Comment: 4 pages, 4 figure

Etching-dependent reproducible memory switching in vertical SiO2 structures

Vertical structures of SiO$_{2}$ sandwiched between a top tungsten electrode and conducting non-metal substrate were fabricated by dry and wet etching methods. Both structures exhibit similar voltage-controlled memory behaviors, in which short voltage pulses (1 $\mu$s) can switch the devices between high- and low-impedance states. Through the comparison of current-voltage characteristics in structures made by different methods, filamentary conduction at the etched oxide edges is most consistent with the results, providing insights into similar behaviors in metal/SiO/metal systems. High ON/OFF ratios of over 10$^{4}$ were demonstrated.Comment: 6 pages, 3 figures + 2 suppl. figure

Doping dependent charge injection and band alignment in organic field-effect transistors

We have studied metal/organic semiconductor charge injection in poly(3-hexylthiophene) (P3HT) field-effect transistors with Pt and Au electrodes as a function of annealing in vacuum. At low impurity dopant densities, Au/P3HT contact resistances increase and become nonohmic. In contrast, Pt/P3HT contacts remain ohmic even at far lower doping. Ultraviolet photoemission spectroscopy (UPS) reveals that metal/P3HT band alignment shifts dramatically as samples are dedoped, leading to an increased injection barrier for holes, with a greater shift for Au/P3HT. These results demonstrate that doping can drastically alter band alignment and the charge injection process at metal/organic interfaces.Comment: 5 pages, 4 figure

Nonlinear charge injection in organic field-effect transistors

Transport properties of a series of poly(3-hexylthiophene) organic field effect transistors with Cr, Cu and Au source/drain electrodes were examined over a broad temperature range. The current-voltage characteristics of the injecting contacts are extracted from the dependence of conductance on channel length. With reasonable parameters, a model of hopping injection into a disordered density of localized states, with emphasis on the primary injection event, agrees well with the field and the temperature dependence of the data over a broad range of temperatures and gate voltages.Comment: 7 pages, 7 figures, sub. to J. Appl. Phy

Mesoscopic conductance effects in InMnAs structures

Quantum corrections to the electrical conduction of magnetic semiconductors are comparatively unexplored. We report measurements of time-dependent universal conductance fluctuations (TDUCF) and magnetic field dependent universal conductance fluctuations (MFUCF) in micron-scale structures fabricated from two different In$_{1-x}$Mn$_{x}$As thin films. TDUCF and MFUCF increasing in magnitude with decreasing temperature are observed. At 4 K and below, TDUCF are suppressed at finite magnetic fields independent of field orientation.Comment: 5 pages, 3+2 figures, 1 table; Appl. Phys. Lett. (in press