Transport Studies of Isolated Molecular Wires in Self-Assembled Monolayer Devices

We have fabricated a variety of novel molecular diodes based on self-assembled-monolayers (SAM) of solid-state mixture of molecular wires (1,4 benzene-dimethane-thiol), and molecular insulator spacers (1-pentanethiol) with different concentration ratios r of wires/spacers, which were sandwiched between two gold (Au) electrodes. We introduce two new methods borrowed from Surface Science to (i) confirm the connectivity between the benzene-dimethane-thiol molecules with the upper Au electrode, and (ii) count the number of isolated molecular wires in the devices. The electrical transport properties of the SAM diodes were studied at different temperatures via the conductance and differential conductance spectra. We found that a potential barrier caused by the spatial connectivity gap between the pentanethiol molecules and the upper Au electrode dominates the transport properties of the pure pentanethiol SAM diode (r = 0). The transport properties of molecular diodes with low r-values are dominated by the conductance of the isolated benzene-dimethane-thiol molecules in the device. We found that the temperature dependence of the molecular diodes is much weaker than that of the pure pentanethiol device indicating the importance of the benzene-dimethane-thiol simultaneous bonding to the two Au electrodes that facilitate electrical transport. From the differential conductance spectra we also found that the energy difference, Delta between the Au electrode Fermi-level and the benzene-dimethane-thiol HOMO (or LUMO) level is ~1.5 eV; whereas it is ~2.5 eV for the pentanethiol molecule. The weak temperature dependent transport that we obtained for the SSM diodes reflects the weak temperature dependence of Delta.Comment: 38 p 8 Fi

Comment on Frequency response and origin of the spin-1/2 photolumines-cence-detected magnetic resonance in a pi-conjugated polymer

In a recent paper Segal et al. [1] attempted to explain the dynamics of spin 1/2 photoluminescence detected magnetic resonance (PLDMR) in films of a pi-conjugated polymer, namely a soluble de-rivative of poly(phenylene-vinylene) [MEH-PPV] using a model (dubbed TPQ), in which the PLDMR is due to spin dependent triplet-polaron interactions that reduce the polarons density and consequent quenching of singlet excitons. We studied the full PLDMR and photoinduced ab-sorption (PA) dynamics of MEH-PPV films as a function of microwave power at various tempera-tures. We show, firstly, that the TPQ model is incompatible with the full frequency dependent spin 1/2 PLDMR response; secondly, it is not in agreement with the spin-1 PLDMR temperature dependence; thirdly, it predicts a much shorter triplet exciton lifetime than that obtained experimentally; and fourthly, that is in contradiction with the temperature dependencies of spin 1/2 PLDMR and triplet exciton PA. In contrast, an alternative model, namely the spin dependent re-combination of polarons, is capable of explaining the whole body of experimental results, and in particular the PLDMR dynamics.Comment: 7 pages, 3 figure

Ultrafast response of surface electromagnetic waves in an aluminum film perforated with subwavelength hole arrays

The ultrafast dynamics of surface electromagnetic waves photogenerated on aluminum film perforated with subwavelength holes array was studied in the visible spectral range by the technique of transient photomodulation with 100 fs time resolution. We observed a pronounced blueshift of the resonant transmission band that reveals the important role of plasma attenuation in the optical response of nanohole arrays. The blueshift is inconsistent with plasmonic mechanism of extraordinary transmission and points to the crucial role of interference in the formation of transmission bands. The transient photomodulation spectra were successfully modeled within the Boltzmann equation approach for the electron-phonon relaxation dynamics, involving non-equilibrium hot electrons and quasi-equilibrium phonons.Comment: 4 pages, 3 figure

Organic spin-valves: physics and applications

Journal ArticleSpin-valve devices of organic semiconductors in the vertical configuration using a variety of exotic and regular ferromagnetic electrodes were fabricated and studied as a function of applied magnetic field, temperature and applied bias voltage. These devices show that spin polarized carriers can be injected from ferromagnetic electrodes into organic semiconductors and diffuse without loss of spin polarization for distances of the order of 100 nm at low temperatures