Direct Measurement of Water-Assisted Ion Desorption and Solvation on Isolated Carbon Nanotubes.

We have investigated the change in mean residence time of gaseous ions adsorbed on the surface of suspended carbon nanotube field-effect transistors (CNT-FETs) with and without native surface water layers that exists in atmospheric conditions. Devices were characterized electrically before and after dehydration by thermal, dry gas, and vacuum desiccation and in each scenario were found to have substantially higher mean ion residence times. It is proposed that water molecules native to the CNT surface in ambient conditions provide a reduction pathway for incoming gaseous ions, yielding hydronium ions (H3O+). This is supported by the appearance of frequent clustered readsorption events in the presence of surface water, caused by the rapid hopping of H+ between the device surface and the lowest water layer, which are not present in data collected from desiccated devices. After desiccation of the device, a thermal trial was conducted to determine the adsorption energy of N2+ ions on the CNT surface. This work has profound implications for our understanding of wetting in one-dimensional systems and the chemistry of ion chemisorption and solvation on the surfaces of materials in general.

Formation of Brightly Luminescent MoS2 Nanoislands from Multilayer Flakes via Plasma Treatment and Laser Exposure.

A robust and reliable method for enhancing the photoluminescence (PL) of multilayer MoS2 is demonstrated using an oxygen plasma treatment process followed by laser exposure. Here, the plasma and laser treatments result in an indirect-to-direct band gap transition. The oxygen plasma creates a slight decoupling of the layers and converts some of the MoS2 to MoO3. Subsequent laser irradiation further oxidizes the MoS2 to MoO3, as confirmed via X-ray photoelectron spectroscopy, and results in localized regions of brightly luminescent MoS2 monolayer triangular islands as seen in high-resolution transmission electron microscopy images. The PL lifetimes are found to decrease from 494 to 190 ps after plasma and laser treatment, reflecting the smaller size of the MoS2 grains/regions. Atomic force microscopic imaging shows a 2 nm increase in thickness of the laser-irradiated regions, which provides further evidence of the MoS2 being converted to MoO3.

Single-ion adsorption and switching in carbon nanotubes.

Single-ion detection has, for many years, been the domain of large devices such as the Geiger counter, and studies on interactions of ionized gasses with materials have been limited to large systems. To date, there have been no reports on single gaseous ion interaction with microelectronic devices, and single neutral atom detection techniques have shown only small, barely detectable responses. Here we report the observation of single gaseous ion adsorption on individual carbon nanotubes (CNTs), which, because of the severely restricted one-dimensional current path, experience discrete, quantized resistance increases of over two orders of magnitude. Only positive ions cause changes, by the mechanism of ion potential-induced carrier depletion, which is supported by density functional and Landauer transport theory. Our observations reveal a new single-ion/CNT heterostructure with novel electronic properties, and demonstrate that as electronics are ultimately scaled towards the one-dimensional limit, atomic-scale effects become increasingly important.

Thermoacoustic transduction in individual suspended carbon nanotubes.

We report an experimental measurement of the acoustic signal emitted from an individual suspended carbon nanotube (CNT) approximate 2 µm in length, 1 nm in diameter, and 10(-21) kg in mass. This system represents the smallest thermoacoustic system studied to date. By applying an AC voltage of 1.4 V at 8 kHz to the suspended CNT, we are able to detect the acoustic signal using a commercial microphone. The acoustic power detected is found to span a range from 0.1 to 2.4 attoWatts or 0.2 to 1 µPa of sound pressure. This corresponds to thermoacoustic efficiencies ranging from 0.007 to 0.6 Pa/W for the seven devices that were measured in this study. Here, the small lateral dimensions of these devices cause large heat losses due to thermal conduction, which result in the relatively small observed thermoacoustic efficiencies.

Electrical and optical characterization of surface passivation in GaAs nanowires.

We report a systematic study of carrier dynamics in Al(x)Ga(1-x)As-passivated GaAs nanowires. With passivation, the minority carrier diffusion length (L(diff)) increases from 30 to 180 nm, as measured by electron beam induced current (EBIC) mapping, and the photoluminescence (PL) lifetime increases from sub-60 ps to 1.3 ns. A 48-fold enhancement in the continuous-wave PL intensity is observed on the same individual nanowire with and without the Al(x)Ga(1-x)As passivation layer, indicating a significant reduction in surface recombination. These results indicate that, in passivated nanowires, the minority carrier lifetime is not limited by twin stacking faults. From the PL lifetime and minority carrier diffusion length, we estimate the surface recombination velocity (SRV) to range from 1.7 × 10(3) to 1.1 × 10(4) cm·s(-1), and the minority carrier mobility µ is estimated to lie in the range from 10.3 to 67.5 cm(2) V(-1) s(-1) for the passivated nanowires.

Large modulations in the intensity of Raman-scattered light from pristine carbon nanotubes.

Large modulations of up to 2 orders of magnitude are observed in the Raman intensity of pristine, suspended, quasimetallic, single-walled carbon nanotubes in response to applied gate potentials. No change in the resonance condition is observed, and all Raman bands exhibit the same changes in intensity, regardless of phonon energy or laser excitation energy. The effect is not observed in semiconducting nanotubes. The electronic energy gaps correlate with the drop in the Raman intensity, and the recently observed Mott insulating behavior is suggested as a possible explanation for this effect.

Gate voltage controllable non-equilibrium and non-ohmic behavior in suspended carbon nanotubes.

In this work, we measure the electrical conductance and temperature of individual, suspended quasi-metallic single-walled carbon nanotubes under high voltage biases using Raman spectroscopy, while varying the doping conditions with an applied gate voltage. By applying a gate voltage, the high-bias conductance can be switched dramatically between linear (Ohmic) behavior and nonlinear behavior exhibiting negative differential conductance (NDC). Phonon populations are observed to be in thermal equilibrium under Ohmic conditions but switch to nonequilibrium under NDC conditions. A typical Landauer transport model assuming zero bandgap is found to be inadequate to describe the experimental data. A more detailed model is presented, which incorporates the doping dependence in order to fit this data.

Spatially resolved temperature measurements of electrically heated carbon nanotubes.

Spatially resolved Raman spectra of individual pristine suspended carbon nanotubes are observed under electrical heating. The Raman G+ and G- bands show unequal temperature profiles. The preferential heating is more pronounced in short nanotubes (2 microm) than in long nanotubes (5 microm). These results are understood in terms of the decay and thermalization of nonequilibrium phonons, revealing the mechanism of thermal transport in these devices. The measurements also enable a direct estimate of thermal contact resistances and the spatial variation of thermal conductivity.

Direct observation of Born-Oppenheimer approximation breakdown in carbon nanotubes.

Raman spectra and electrical conductance of individual, pristine, suspended, metallic single-walled carbon nanotubes are measured under applied gate potentials. The G(-) band is observed to downshift with small applied gate voltages, with the minima occurring at E(F) = +/-(1)/(2)E(phonon), contrary to adiabatic predictions. A subsequent upshift in the Raman frequency at higher gate voltages results in a "W"-shaped Raman shift profile that agrees well with a nonadiabatic phonon renormalization model. This behavior constitutes the first experimental confirmation of the theoretically predicted breakdown of the Born-Oppenheimer approximation in individual single-walled carbon nanotubes.

Direct observation of mode selective electron-phonon coupling in suspended carbon nanotubes.

Raman spectra of individual pristine suspended single-walled carbon nanotubes are observed under high electrical bias. The LO and TO modes of the G band behave differently with respect to voltage bias, indicating preferential electron-phonon coupling and nonequilibrium phonon populations, which cause negative differential conductance in suspended devices. By correlating the electron resistivity to the optically measured phonon population, the data are fit using a Landauer model to determine the key scattering parameters.