Sebastian Sorgenfrei

Boron nitride substrates for high-quality graphene electronics

Graphene devices on standard SiO(2) substrates are highly disordered, exhibiting characteristics that are far inferior to the expected intrinsic properties of graphene. Although suspending the graphene above the substrate leads to a substantial improvement in device quality, this geometry imposes severe limitations on device architecture and functionality. There is a growing need, therefore, to identify dielectrics that allow a substrate-supported geometry while retaining the quality achieved with a suspended sample. Hexagonal boron nitride (h-BN) is an appealing substrate, because it has an atomically smooth surface that is relatively free of dangling bonds and charge traps. It also has a lattice constant similar to that of graphite, and has large optical phonon modes and a large electrical bandgap. Here we report the fabrication and characterization of high-quality exfoliated mono- and bilayer graphene devices on single-crystal h-BN substrates, by using a mechanical transfer process. Graphene devices on h-BN substrates have mobilities and carrier inhomogeneities that are almost an order of magnitude better than devices on SiO(2). These devices also show reduced roughness, intrinsic doping and chemical reactivity. The ability to assemble crystalline layered materials in a controlled way permits the fabrication of graphene devices on other promising dielectrics and allows for the realization of more complex graphene heterostructures.

Label-free single-molecule detection of DNA-hybridization kinetics with a carbon nanotube field-effect transistor

Single-molecule measurements of biomolecules can provide information about the molecular interactions and kinetics that are hidden in ensemble measurements. However, there is a requirement for techniques with improved sensitivity and time resolution for use in exploring biomolecular systems with fast dynamics. Here, we report the detection of DNA hybridization at the single-molecule level using a carbon nanotube field-effect transistor. By covalently attaching a single-stranded probe DNA sequence to a point defect in a carbon nanotube, we are able to measure two-level fluctuations in the conductance of the nanotube in the presence of a complementary DNA target. The kinetics of the system are studied as a function of temperature, allowing the measurement of rate constants, melting curves and activation energies for different sequences and target concentrations. The kinetics demonstrate non-Arrhenius behaviour, in agreement with DNA hybridization experiments using fluorescence correlation spectroscopy. This technique is label-free and could be used to probe single-molecule dynamics at microsecond timescales.

Electronic compressibility of layer-polarized bilayer graphene

We report on a capacitance study of dual gated bilayer graphene. The measured capacitance allows us to probe the electronic compressibility as a function of carrier density, temperature, and applied perpendicular electrical displacement D. As a band gap is induced with increasing D, the compressibility minimum at charge neutrality becomes deeper but remains finite, suggesting the presence of localized states within the energy gap. Temperature dependent capacitance measurements show that compressibility is sensitive to the intrinsic band gap. For large displacements, an additional peak appears in the compressibility as a function of density, corresponding to the presence of a 1-dimensional van Hove singularity (vHs) at the band edge arising from the quartic bilayer graphene band structure. For D > 0, the additional peak is observed only for electrons, while D < 0 the peak appears only for holes. This asymmetry that can be understood in terms of the finite interlayer separation and may be useful as a direct probe of the layer polarization.

Debye Screening in Single-Molecule Carbon Nanotube Field-Effect Sensors

Point-functionalized carbon nanotube field-effect transistors can serve as highly sensitive detectors for biomolecules. With a probe molecule covalently bound to a defect in the nanotube sidewall, two-level random telegraph noise (RTN) in the conductance of the device is observed as a result of a charged target biomolecule binding and unbinding at the defect site. Charge in proximity to the defect modulates the potential (and transmission) of the conductance-limiting barrier created by the defect. In this Letter, we study how these single-molecule electronic sensors are affected by ionic screening. Both charge in proximity to the defect site and buffer concentration are found to affect RTN amplitude in a manner that follows from simple Debye length considerations. RTN amplitude is also dependent on the potential of the electrolyte gate as applied to the reference electrode; at high enough gate potentials, the target DNA is completely repelled and RTN is suppressed.

A 0.18-

This paper describes the design of an active, integrated CMOS sensor array for fluorescence applications which enables time-gated, time-resolved fluorescence spectroscopy. The 64-by-64 array is sensitive to photon densities as low as 8.8 times 106 photons/cm2 with 64-point averaging and, through a differential pixel design, has a measured impulse response of better than 800 ps. Applications include both active microarrays and high-frame-rate imagers for fluorescence lifetime imaging microscopy.

\mu

We investigate dielectrophoretic deposition of single-walled carbon nanotubes using an in situ detection system. Pairs of electrodes are stimulated with a small-amplitude, low-frequency voltage superimposed on a large-amplitude, high-frequency dielectrophoretic voltage. Measuring the magnitude of the current both at dc (Idc) and at the low frequency (Iac) through a digital lock-in technique allows us to determine when a nanotube has made electrical contact and to halt the dielectrophoretic process. Because Idc is determined by nonlinearities in the device current-voltage characteristic, measurement of the Idc/Iac ratio allows the real-time determination of whether the deposited nanotube is metallic or semiconducting.

m CMOS Array Sensor for Integrated Time-Resolved Fluorescence Detection

This paper describes the design of an active CMOS sensor array for fluorescence applications which enables time-gated, time-resolved fluorescence spectroscopy. The 64 times 64 array is sensitive to photon densities as low as 8 times 106 photons/cm with 64-point averaging and, through a differential pixel design, has a measured impulse response of better than 800 ps. Applications include both active microarrays and high-frame-rate imagers for fluorescence lifetime imaging microscopy.

Controlled dielectrophoretic assembly of carbon nanotubes using real-time electrical detection

Traditionally, biomolecular systems have been studied in ensemble. While much can be determined with ensemble measurements, scientific and technological interest is rapidly moving to single-molecule techniques, which rely primarily on fluorescent markers and advanced microscopy techniques. In this paper, we describe recent work using nanoscale transistors based on carbon nanotubes as charge-sensitive detectors. We show carbon nanotubes can be used for ensemble studies through sidewall adsorption. Sensitivity can be greatly enhanced though an engineered defect in the nanotube. Biomolecular interactions are characterized by random-telegraph-noise response, which can be analyzed to study single-molecule kinetics and thermodynamics.

A CMOS Array Sensor for Sub-800-ps Time-Resolved Fluorescence Detection

Technological advances in fluorescent probes, solid-state imagers, and microscopy techniques have enabled biomolecular studies at the single-molecule level. Fluorescent techniques are highly specific but their bandwidth is fundamentally limited by the number of photons that can be collected. New electronic sensors including nanopores and nanotube field-effect transistors offer different tradeoffs between bandwidth and noise levels. Here, we discuss the performance of these direct solid-state interfaces and their potential for sensing single-molecule dynamics at shorter timescales.

Single-molecule electronic detection using nanoscale field-effect devices

We present a label-free single-molecule based sensing platform using a carbon nanotube field-effect transistor. By point functionalizing a carbon nanotube through an electrochemical oxidation reaction, the conductance becomes sensitive and chemically reactive at a single point to which we can covalently attach a probe DNA molecule. Two-level fluctuations appear in the conductance of the carbon nanotube when it is immersed in a liquid buffer solution containing complementary target DNA. We show that the autocorrelation of the conductance can be used to extract DNN hybridization kinetics. The results are comparable to the one extracted through a hidden Markov model.