All-optical technique to correlate defect structure and carrier transport in transferred graphene films.

Chemical vapor deposition of graphene on copper foil is an attractive method of producing large-area graphene films, but the electronic performance is limited by defects such as creases from the film transfer process, wrinkles due to the thermal expansion coefficient mismatch, and grain boundaries from the growth process. Here we present an all-optical technique to correlate defect structure with electronic properties using spatially resolved Raman spectroscopy and transient absorption microscopy. This technique is especially attractive since it does not require any lithographic steps to probe the electronic properties of the graphene film. As a first demonstration, we focus on the effects of both wrinkles and creases while averaging over many small grains. It was found that wrinkles and creases may decrease the charge carrier diffusion coefficient by over 50% due to increased defect scattering. This technique may easily be extended to large grain graphene films in order to study the effect of different types of grain boundaries.

Luminol-labeled gold nanoparticles for ultrasensitive chemiluminescence-based chemical analyses.

We report a study on chemiluminescence-based chemical analyses using luminol molecules covalently attached to 10 nm diameter gold nanoparticles (GNPs). Chemiluminescence (CL) has been systematically studied under two schemes by varying the concentrations of luminol-labeled GNPs and [Fe(CN)6](3-) catalyst, respectively. The CL signal of luminol-labeled GNPs is enhanced by 5 to 10 times compared to the bulk luminol solutions of the same concentration. The log-log plot of the CL signal versus the number of luminol-labeled GNPs suspended in a standard 96-well plate shows two characteristic linear curves with distinct slopes across eight orders of magnitude variation in the GNP quantity (from 1.82 × 10(2) to 1.82 × 10(10) GNPs per well). The detection limit represented by the cross-point of these two curves can reach down to ~6.1 × 10(5) GNPs per well (corresponding to 1.0 × 10(-14) M GNP and 2.4 × 10(-11) M equivalent luminol concentration). The attachment of luminol molecules to GNP nano-carriers allows a large amount of luminol to be placed in a greatly reduced volume (or area) toward developing miniaturized CL sensors. We have demonstrated this by preloading dried luminol-labeled GNPs in homemade microwell arrays (with a volume of ~12 µL per well). A linear log-log curve can be obtained across the full range from 1 × 10(3) to 1 × 10(10) GNPs per microwell. The CL signal was detectable with as few as ~1000 GNPs. We have further applied this microwell method to the detection of highly diluted blood samples, in both intact and lysed forms, which releases Fe(3+)-containing hemoglobin to catalyze luminol CL. The lysed blood sample can be detected even after a 10(8) fold dilution (corresponding to ~0.18 cells per well). This ultrasensitive CL detection method may be readily adapted for developing various miniaturized multiplex biosensors for rapid chemical/biochemical analyses.

Development of nanopatterned fluorine-doped tin oxide electrodes for dye-sensitized solar cells with improved light trapping.

Transparent conductors (TCs) are an important component of optoelectronic devices and nanoscale engineering of TCs is important for optimization of the device performance through improved light trapping. In this work, patterned periodic arrays of nanopillars and nanolines of pitch size of ~700 nm were created on fluorine-doped tin oxide (FTO) using nanoimprint lithography and reactive ion etching using environmentally friendly gases. The patterned FTO exhibits enhanced light trapping as compared to the unpatterned FTO, which agrees well with simulations based on Finite-Difference Time-Domain method for up to a distance of 4 µm. Dye sensitized solar cells (DSSCs) fabricated on the patterned FTO exhibited improved performance (fill factor and power conversion efficiency), which can be attributed to enhanced light absorption in the range 400-650 nm. Further, electrochemical impedance measurements revealed lower recombination resistance for the patterned FTO/TiO(2) electrode compared to the unpatterned FTO electrode/TiO(2) electrode as a result of better light capturing properties of patterned FTO. The direct fabrication of nanopatterns on TCs developed in the present study is expected to be a viable scheme for achieving improved performance in many other optoelectronic devices.

Investigation into Photoconductivity in Single CNF/TiO(2)-Dye Core-Shell Nanowire Devices.

A vertically aligned carbon nanofiber array coated with anatase TiO(2) (CNF/TiO(2)) is an attractive possible replacement for the sintered TiO(2) nanoparticle network in the original dye-sensitized solar cell (DSSC) design due to the potential for improved charge transport and reduced charge recombination. Although the reported efficiency of 1.1% in these modified DSSC's is encouraging, the limiting factors must be identified before a higher efficiency can be obtained. This work employs a single nanowire approach to investigate the charge transport in individual CNF/TiO(2) core-shell nanowires with adsorbed N719 dye molecules in dark and under illumination. The results shed light on the role of charge traps and dye adsorption on the (photo) conductivity of nanocrystalline TiO(2) CNF's as related to dye-sensitized solar cell performance.

Novel dye-sensitized solar cell architecture using TiO2-coated vertically aligned carbon nanofiber arrays.

A novel dye-sensitized solar cell (DSSC) architecture based on vertically aligned carbon nanofibers coated with a thin nanoneedle-textured anatase TiO2 film is demonstrated. An encouraging overall conversion efficiency of approximately 1.09% and a rather high open-circuit voltage of approximately 0.64 V have been achieved. The efficient charge separation at the TiO2-CNF junction and the large outer TiO2 surface of this core-shell architecture provide new methods to tune the materials and interfaces in solar cells.