Mario G. Ancona

High-mobility Carbon-nanotube Thin-film Transistors on a Polymeric Substrate

We report the development of high-mobility carbon-nanotube thin-film transistors fabricated on a polymeric substrate. The active semiconducting channel in the devices is composed of a random two-dimensional network of single-walled carbon nanotubes (SWNTs). The devices exhibit a field-effect mobility of 150cm2∕Vs and a normalized transconductance of 0.5mS∕mm. The ratio of on-current (Ion) to off-current (Ioff) is ∼100 and is limited by metallic SWNTs in the network. With electronic purification of the SWNTs and improved gate capacitance we project that the transconductance can be increased to ∼10–100mS∕mm with a significantly higher value of Ion∕Ioff, thus approaching crystalline semiconductor-like performance on polymeric substrates.

Lateral distribution of hot-carrier-induced interface traps in MOSFETs

The spatial profiles of hot-carrier-induced interface traps in MOSFETs with abrupt arsenic junctions and oxide thickness of 10-38 nm are determined using charge pumping both in the conventional manner and with a modified constant-field approach. For the thinnest oxides the damage is highly localized in a very sharp peak that is located inside the drain at the point of maximum lateral electric field. In thicker oxides, the damage peak is broader and is shifted toward the edge of the drain junction. Two-dimensional device simulations using the measured profiles are in qualitative agreement with measured I-V characteristics after degradation. However, the magnitude of the predicted degradation is underestimated, suggesting that significant electron trapping occurs also. >

Quantum Dot DNA Bioconjugates: Attachment Chemistry Strongly Influences the Resulting Composite Architecture

The unique properties provided by hybrid semiconductor quantum dot (QD) bioconjugates continue to stimulate interest for many applications ranging from biosensing to energy harvesting. Understanding both the structure and function of these composite materials is an important component in their development. Here, we compare the architecture that results from using two common self-assembly chemistries to attach DNA to QDs. DNA modified to display either a terminal biotin or an oligohistidine peptidyl sequence was assembled to streptavidin/amphiphilic polymer- or PEG-functionalized QDs, respectively. A series of complementary acceptor dye-labeled DNA were hybridized to different positions on the DNA in each QD configuration and the separation distances between the QD donor and each dye-acceptor probed with Förster resonance energy transfer (FRET). The polyhistidine self-assembly yielded QD-DNA bioconjugates where predicted and experimental separation distances matched reasonably well. Although displaying efficient FRET, data from QD-DNA bioconjugates assembled using biotin-streptavidin chemistry did not match any predicted separation distances. Modeling based upon known QD and DNA structures along with the linkage chemistry and FRET-derived distances was used to simulate each QD-DNA structure and provide insight into the underlying architecture. Although displaying some rotational freedom, the DNA modified with the polyhistidine assembles to the QD with its structure extended out from the QD-PEG surface as predicted. In contrast, the random orientation of streptavidin on the QD surface resulted in DNA with a wide variety of possible orientations relative to the QD which cannot be controlled during assembly. These results suggest that if a particular QD biocomposite structure is desired, for example, random versus oriented, the type of bioconjugation chemistry utilized will be a key influencing factor.

Self-Assembled Quantum Dot-Sensitized Multivalent DNA Photonic Wires

Combining the inherent scaffolding provided by DNA structure with spatial control over fluorophore positioning allows the creation of DNA-based photonic wires with the capacity to transfer excitation energy over distances greater than 150 Å. We demonstrate hybrid multifluorophore DNA-photonic wires that both self-assemble around semiconductor quantum dots (QDs) and exploit their unique photophysical properties. In this architecture, the QDs function as both central nanoscaffolds and ultraviolet energy harvesting donors that drive Förster resonance energy transfer (FRET) cascades through the DNA wires with emissions that approach the near-infrared. To assemble the wires, DNA fragments labeled with a series of increasingly red-shifted acceptor-dyes were hybridized in a predetermined linear arrangement to a complementary DNA template that was chemoselectively modified with a hexahistidine-appended peptide. The peptide portion facilitated metal-affinity coordination of multiple hybridized DNA-dye structures to a central QD completing the final nanocrystal-DNA photonic wire structure. We assembled several such hybrid structures where labeled-acceptor dyes were excited by the QDs and arranged to interact with each other via consecutive FRET processes. The inherently facile reconfiguration properties of this design allowed testing of alternate formats including the addition of an intercalating dye located in the template DNA or placement of multiple identical dye acceptors that engaged in homoFRET. Lastly, a photonic structure linking the central QD with multiple copies of DNA hybridized with 4-sequentially arranged acceptor dyes and demonstrating 4-consecutive energy transfer steps was examined. Step-by-step monitoring of energy transfer with both steady-state and time-resolved spectroscopy allowed efficiencies to be tracked through the structures and suggested that acceptor dye quantum yields are the predominant limiting factor. Integrating such DNA-based photonic structures with QDs can help create a new generation of biophotonic wire assemblies with widespread potential in nanotechnology.

Mobility enhancement in strained p-InGaSb quantum wells

Quantum wells of InGaSb clad by AlGaSb were grown by molecular beam epitaxy. The InGaSb is in compressive strain, resulting in a splitting of the heavy- and light-hole valence bands and an enhancement of the mobility. The mobility was found to increase with increasing InSb mole fraction for values of strain up to 2%. Room-temperature mobilities as high as 1500cm2∕Vs were reached for 7.5nm channels of In0.40Ga0.60Sb. These results are an important step toward the goal of high-performance p-channel field-effect transistors for complementary circuits operating at extremely low power.

Determination of interface trap capture cross sections using three-level charge pumping

A modified three-voltage-level charge pumping (CP) technique is described for measuring interface trap parameters in MOSFETs. Charge pumping (CP) is a technique for studying traps at the Si-SiO/sub 2/ interface in MOS transistors. In the CP technique, a pulse is applied to the gate of the MOSFET which alternately fills the traps with electrons and holes, thereby causing a recombination current I/sub cp/ to flow in the substrate. With this technique, interface trap capture cross sections for both electrons and holes may be determined as a function of trap energy in a single device. It is demonstrated that a modified three-level charge pumping method may be used to determine not only interface trap densities but also to capture cross sections as a function of trap energy. The trap parameters are obtained for both electrons and holes using a single MOSFET.

Enhanced plasmon coupling in crossed dielectric/metal nanowire composite geometries and applications to surface-enhanced Raman spectroscopy

Surface-enhanced Raman spectroscopy (SERS) was performed on Ga2O3∕Ag and ZnO∕Ag nanowires, which were arranged in either a crossover or noncrossing geometry. Results indicate a high SERS sensitivity (near 0.2pg) for nanowires arranged in a crossing geometry. It is suggested that this is due to the dielectric core/metal shell structure, as well as to the nanowire crossings, which are regions of very high electric fields. Finite element simulations of the electric field near two crossed wires confirm an enhanced plasmon resonance in the vicinity of the crossing, which extends spatially in the crossings and around the nanowires.

Density-gradient analysis of MOS tunneling

The density-gradient description of quantum transport is applied to the analysis of tunneling phenomena in ultrathin (<25 /spl Aring/) oxide MOS capacitors. Both electron and hole tunneling are included in the one-dimensional (1-D) analysis and two new refinements to density-gradient theory are introduced, one relating to the treatment of Shockley-Read-Hall recombination and the other a modification of the tunneling boundary conditions to account for the semiconductor bandgap. Detailed comparisons are made with experimental current-voltage (I-V) data for samples with both n/sup +/ and p/sup +/ polysilicon gates and all of the features of the data are found to be understandable within the density-gradient framework. Besides providing new understanding of these experiments, these results show that the density-gradient approach can be of great value for engineering-oriented device analysis in quantum regimes.

Complex Logic Functions Implemented with Quantum Dot Bionanophotonic Circuits

We combine quantum dots (QDs) with long-lifetime terbium complexes (Tb), a near-IR Alexa Fluor dye (A647), and self-assembling peptides to demonstrate combinatorial and sequential bionanophotonic logic devices that function by time-gated Förster resonance energy transfer (FRET). Upon excitation, the Tb-QD-A647 FRET-complex produces time-dependent photoluminescent signatures from multi-FRET pathways enabled by the capacitor-like behavior of the Tb. The unique photoluminescent signatures are manipulated by ratiometrically varying dye/Tb inputs and collection time. Fluorescent output is converted into Boolean logic states to create complex arithmetic circuits including the half-adder/half-subtractor, 2:1 multiplexer/1:2 demultiplexer, and a 3-digit, 16-combination keypad lock.

Assembling programmable FRET-based photonic networks using designer DNA scaffolds

DNA demonstrates a remarkable capacity for creating designer nanostructures and devices. A growing number of these structures utilize Förster resonance energy transfer (FRET) as part of the devices functionality, readout or characterization, and, as device sophistication increases so do the concomitant FRET requirements. Here we create multi-dye FRET cascades and assess how well DNA can marshal organic dyes into nanoantennae that focus excitonic energy. We evaluate 36 increasingly complex designs including linear, bifurcated, Holliday junction, 8-arm star and dendrimers involving up to five different dyes engaging in four-consecutive FRET steps, while systematically varying fluorophore spacing by Förster distance (R0). Decreasing R0 while augmenting cross-sectional collection area with multiple donors significantly increases terminal exciton delivery efficiency within dendrimers compared with the first linear constructs. Förster modelling confirms that best results are obtained when there are multiple interacting FRET pathways rather than independent channels by which excitons travel from initial donor(s) to final acceptor.