Conformations and charge transport characteristics of biphenyldithiol self-assembled-monolayer molecular electronic devices: A multiscale computational study

We report a computational study of conformations and charge transport characteristics of biphenyldithiol (BPDT) monolayers in the (sqrt(3)×sqrt(3))R30° packing ratio sandwiched between Au(111) electrodes. From force-field molecular-dynamics and annealing simulations of BPDT self-assembled monolayers (SAMs) with up to 100 molecules on a Au(111) substrate, we identify an energetically favorable herringbone-type SAM packing configuration and a less-stable parallel packing configuration. Both SAMs are described by the (2sqrt(3)×sqrt(3))R30° unit cell including two molecules. With subsequent density-functional theory calculations of one unit cell of the (i) herringbone SAM with the molecular tilt angle theta[approximate]15°, (ii) herringbone SAM with theta[approximate]30°, and (iii) parallel SAM with theta[approximate]30°, we confirm that the herringbone packing configuration is more stable than the parallel one but find that the energy variation with respect to the molecule tilting within the herringbone packing is very small. Next, by capping these SAMs with the top Au(111) electrode, we prepare three molecular electronic device models and calculate their coherent charge transport properties within the matrix Green's function approach. Current–voltage (I–V) curves are then obtained via the Landauer–Büttiker formula. We find that at low-bias voltages (|V|~0.5 V), the I–V characteristics of the three models show noticeable differences due to different phenyl band structures. We thus conclude that the BPDT SAM I–V characteristics in the low-bias voltage region are mainly determined by the Si–Au interaction within the individual molecule-electrode contact, while both intramolecular conformation and intermolecular interaction can affect the BPDT SAM I–V characteristics in the high-bias voltage region

Possible performance improvement in [2]catenane molecular electronic switches

Mechanically interlocked bistable supramolecular complexes are promising candidates of molecular electronics. Applying a multiscale computational approach, here we study the coherent charge transport properties of catenane monolayers sandwiched between Cu(111) electrodes. We demonstrate the robust nature of electrical switching behavior with respect to the variations in the monolayer packing density and the type of electrodes, as well as the thermal fluctuations of the molecules. We propose that the asymmetry of molecule-electrode barriers can be utilized to improve the switching ratio

Two-dimensional heterogeneous photonic bandedge laser

We proposed and realized a two-dimensional (2D) photonic bandedge laser surrounded by the photonic bandgap. The heterogeneous photonic crystal structure consists of two triangular lattices of the same lattice constant with different air hole radii. The photonic crystal laser was realized by room-temperature optical pumping of air-bridge slabs of InGaAsP quantum wells emitting at 1.55 micrometer. The lasing mode was identified from its spectral positions and polarization directions. A low threshold incident pump power of 0.24mW was achieved. The measured characteristics of the photonic crystal lasers closely agree with the results of real space and Fourier space calculations based on the finite-difference time-domain method.Comment: 14 pages, 4 figure

First-principles study of the switching mechanism of [2]catenane molecular electronic devices

We present a first-principles study of the coherent charge transport properties of bistable [2]catenane molecular monolayers sandwiched between Au(111) electrodes. We find that conduction channels around the Fermi level are dominated by the two highest occupied molecular orbital levels from tetrathiafulvalene (TTF) and dioxynaphthalene (DNP) and the two lowest unoccupied molecular orbital levels from tetracationic cyclophane (CBPQT(4+)), and the OFF to ON switching results from the energetic shifts of these orbitals as CBPQT(4+) moves from TTF to DNP. We show that the superposition principle can be adopted for predicting the function of the composite device