Erika Penzo

Long-range charge transport in single G-quadruplex DNA molecules

DNA and DNA-based polymers are of interest in molecular electronics because of their versatile and programmable structures. However, transport measurements have produced a range of seemingly contradictory results due to differences in the measured molecules and experimental set-ups, and transporting significant current through individual DNA-based molecules remains a considerable challenge. Here, we report reproducible charge transport in guanine-quadruplex (G4) DNA molecules adsorbed on a mica substrate. Currents ranging from tens of picoamperes to more than 100 pA were measured in the G4-DNA over distances ranging from tens of nanometres to more than 100 nm. Our experimental results, combined with theoretical modelling, suggest that transport occurs via a thermally activated long-range hopping between multi-tetrad segments of DNA. These results could re-ignite interest in DNA-based wires and devices, and in the use of such systems in the development of programmable circuits.

Selective Biomolecular Nanoarrays for Parallel Single-Molecule Investigations

The ability to direct the self-assembly of biomolecules on surfaces with true nanoscale control is key for the creation of functional substrates. Herein we report the fabrication of nanoscale biomolecular arrays via selective self-assembly on nanopatterned surfaces and minimized nonspecific adsorption. We demonstrate that the platform developed allows for the simultaneous screening of specific protein-DNA binding events at the single-molecule level. The strategy presented here is generally applicable and enables high-throughput monitoring of biological activity in real time and with single-molecule resolution.

Directed Assembly of Single Wall Carbon Nanotube Field Effect Transistors

The outstanding electronic properties of single wall carbon nanotubes (SWCNTs) have made them prime candidates for future nanoelectronics technologies. One of the main obstacles to the implementation of advanced SWCNT electronics to date is the inability to arrange them in a manner suitable for complex circuits. Directed assembly of SWCNT segments onto lithographically patterned and chemically functionalized substrates is a promising way to organize SWCNTs in topologies that are amenable to integration for advanced applications, but the placement and orientational control required have not yet been demonstrated. We have developed a technique for assembling length sorted and chirality monodisperse DNA-wrapped SWCNT segments on hydrophilic lines patterned on a passivated oxidized silicon substrate. Placement of individual SWCNT segments at predetermined locations was achieved with nanometer accuracy. Three terminal electronic devices, consisting of a single SWCNT segment placed either beneath or on top of metallic source/drain electrodes were fabricated. Devices made with semiconducting nanotubes behaved as typical p-type field effect transistors (FETs), whereas devices made with metallic nanotubes had a finite resistance with little or no gate modulation. This scalable, high resolution approach represents an important step forward toward the potential implementation of complex SWCNT devices and circuits.

Controlled Formation of Carbon Nanotube Junctions via Linker-Induced Assembly in Aqueous Solution

Here we present a simple approach for the controlled formation of one-dimensional and multiterminal nanotube junctions. We describe a facile bottom-up strategy for joining the ends of single-walled carbon nanotubes. The geometry of the junctions can be varied and controlled by linker-induced assembly of DNA-wrapped nanotubes.

Selective placement of DNA origami on substrates patterned by nanoimprint lithography

Self-assembled DNA nanostructures can be used as scaffolds to organize small functional nanocomponents. In order to build working devices—electronic circuits, biochips, optical/photonics devices—controlled placement of DNA nanostructures on substrates must be achieved. Here we present a nanoimprint lithography-based process to create chemically patterned templates, rendering them capable of selectively binding DNA origami. Hexamethyldisilazane (HMDS) is used as a passivating layer on silicon dioxide substrates, which prevents DNA attachment. Hydrophilic areas, patterned by nanoimprint lithography with the same size and shape of the origami, are formed by selective removal of the HMDS, enabling the assembly of the origami scaffolds in the patterned areas. The use of nanoimprint lithography, a low cost, high throughput patterning technique, enables high precision positioning and orientation of DNA nanostructures on a surface over large areas.

Directed Assembly of End-Functionalized Single Wall Carbon Nanotube Segments

A key impediment to the implementation of a nanoelectronics technology based on single wall carbon nanotubes (SWCNTs) is the inability to arrange them in a manner suitable for integration into complex circuits. As a step toward addressing this problem, we explore the binding of fixed-length, end-functionalized SWCNT segments to lithographically defined nanoscale anchors, such that individual SWCNTs can be placed with control over position and orientation. Both monovalent and bivalent bindings are explored using covalent and noncovalent binding chemistries. Placement efficiency is assessed in terms of overall yield of SWCNT binding, as well as binding specificity and the degree of nonspecific binding. Placement yields as high as 93% and 79% are achieved, respectively, for covalent binding and for binding through DNA hybridization. Orientational control of the SWCNT segments is achieved with 95% and 51% efficiency for monovalent and bivalent bindings, respectively. This represents a new approach that could pave the way toward complex SWCNT devices and circuits.

Lithographically directed assembly of one-dimensional DNA nanostructures via bivalent binding interactions

AbstractIn order to exploit the outstanding physical properties of one-dimensional (1D) nanostructures such as carbon nanotubes and semiconducting nanowires and nanorods in future technological applications, it will be necessary to organize them on surfaces with precise control over both position and orientation. Here, we use a 1D rigid DNA motif as a model for studying directed assembly at the molecular scale to lithographically patterned nanodot anchors. By matching the inter-nanodot spacing to the length of the DNA nanostructure, we are able to achieve nearly 100% placement yield. By varying the length of single-stranded DNA linkers bound covalently to the nanodots, we are able to study the binding selectivity as a function of the strength of the binding interactions. We analyze the binding in terms of a thermodynamic model which provides insight into the bivalent nature of the binding, a scheme that has general applicability for the controlled assembly of a broad range of functional nanostructures.

Tunable Anisotropic Photon Emission from Self-Organized CsPbBr3 Perovskite Nanocrystals

We report controllable anisotropic light emission of photons originating from vertically aligned transition dipole moments in spun-cast films of CsPbBr3 nanocubes. By depositing films of nanocrystals on precoated substrates we can control the packing density and resultant radiation pattern of the emitted photons. We develop a technical framework to calculate the average orientation of light emitters, i.e., the angle between the transition dipole moment vector (TDM) and the substrate. This model is applicable to any emissive material with a known refractive index. Theoretical modeling indicates that oriented emission originates from an anisotropic alignment of the valence band and conduction band edge states on the ionic crystal lattice and demonstrates a general path to model the experimentally less accessible internal electric field of a nanosystem from the photoluminescent anisotropy. The uniquely accessible surface of the perovskite nanoparticles allows for perturbation of the normally isotropic emissive transition. The reported sensitive and tunable TDM orientation and control of emitted light will allow for applications of perovskite nanocrystals in a wide range of photonic technologies inaccessible to traditional light emitters.

Optical biosensors based on photonic crystals supporting bound states in the continuum

A novel optical label-free bio-sensing platform based on a new class of resonances supported in a photonic crystal metasurface is reported herein. Molecular binding is detected as a shift in the resonant wavelength of the bound states in the continuum of radiation modes. The new configuration is applied to the recognition of the interaction between protein p53 and its protein regulatory partner murine double minute 2 (MDM2). A detection limit of 66 nM for the protein p53 is found. The device provides an excellent interrogation stability and loss-free operation, requires minimal optical interrogation equipment and can be easily optimized to work in a wide wavelength range.

Patterning of electrically tunable light-emitting photonic structures demonstrating bound states in the continuum

The authors report a scalable process to fabricate electrically tunable light-emitting photonic structures made of optically active and electrically conductive erbium-doped zinc oxide (Er:ZnO) deposited by magnetron sputtering. Such structures are expected to produce a dramatic amplification of the erbium fluorescence due to enhanced light-matter coupling at topologically protected states called bound states in the continuum (BIC). Our patterning approach circumvents roughening of the Er:ZnO during plasma etching by employing a metallic mask and a lift-off process. Etching with a polymer mask resulted in an unacceptable increase of the surface roughness, from a root mean square (RMS) roughness of 0.5 nm for the as-deposited sample to a RMS roughness of 25 nm after etching. Such surface roughness proves detrimental to the photonic crystal resonances and to the BIC mode in particular. Using a metallic mask instead allowed for the etching of Er:ZnO with a modest roughness increase (RMS value 4.1 nm). This pa...