Shun-Wen Chang

Enhanced photocurrent and photoluminescence spectra in MoS2 under ionic liquid gating

We report substantial improvements and modulation in the photocurrent (PC) and photoluminescence (PL) spectra of monolayer MoS2 recorded under electrostatic and ionic liquid gating conditions. The photocurrent and photoluminescence spectra show good agreement with a dominant peak at 1.85 eV. The magnitude of the photoluminescence can be increased 300% by ionic liquid gating due to the passivation of surface states and trapped charges that act as recombination centers. The photocurrent also doubles when passivated by the ionic liquid. Interestingly, a significant shift of the PL peak position is observed under electrostatic (14 meV) and ionic liquid (30 meV) gating, as a result of passivation. The ionic liquid provides significant screening without any externally applied voltage, indicating that these surface recombination centers have net charge. The acute sensitivity of monolayer MoS2 to ionic liquid gating and passivation arises because of its high surface-to-volume ratio, which makes it especially sensitive to trapped charge and surface states. These results reveal that, in order for efficient optoelectronic devices to be made from monolayer MoS2, some passivation strategy must be employed to mitigate the issues associated with surface recombination.

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.

Clamping instability and van der Waals forces in carbon nanotube mechanical resonators.

We investigate the role of weak clamping forces, typically assumed to be infinite, in carbon nanotube mechanical resonators. Due to these forces, we observe a hysteretic clamping and unclamping of the nanotube device that results in a discrete drop in the mechanical resonance frequency on the order of 5-20 MHz, when the temperature is cycled between 340 and 375 K. This instability in the resonant frequency results from the nanotube unpinning from the electrode/trench sidewall where it is bound weakly by van der Waals forces. Interestingly, this unpinning does not affect the Q-factor of the resonance, since the clamping is still governed by van der Waals forces above and below the unpinning. For a 1 μm device, the drop observed in resonance frequency corresponds to a change in nanotube length of approximately 50-65 nm. On the basis of these findings, we introduce a new model, which includes a finite tension around zero gate voltage due to van der Waals forces and shows better agreement with the experimental data than the perfect clamping model. From the gate dependence of the mechanical resonance frequency, we extract the van der Waals clamping force to be 1.8 pN. The mechanical resonance frequency exhibits a striking temperature dependence below 200 K attributed to a temperature-dependent slack arising from the competition between the van der Waals force and the thermal fluctuations in the suspended nanotube.

A Comparison of Photocurrent Mechanisms in Quasi-Metallic and Semiconducting Carbon Nanotube pn-Junctions.

We present a comparative study of quasi-metallic (Eg ∼ 100 meV) and semiconducting (Eg ∼ 1 eV) suspended carbon nanotube pn-junctions introduced by electrostatic gating. While the built-in fields of the quasi-metallic carbon nanotubes (CNTs) are 1-2 orders of magnitude smaller than those of the semiconducting CNTs, their photocurrent is 2 orders of magnitude higher than the corresponding semiconducting CNT devices under the same experimental conditions. Here, the large exciton binding energy in semiconducting nanotubes (∼400 meV) makes it difficult for excitons to dissociate into free carriers that can contribute to an externally measured photocurent. As such, semiconducting nanotubes require a phonon to assist in the exciton dissociation process, in order to produce a finite photocurrent, while quasi-metallic nanotubes do not. The quasi-metallic nanotubes have much lower exciton binding energies (∼50 meV) as well as a continuum of electronic states to decay into and, therefore, do not require the absorption of a phonon in order to dissociate, making it much easier for these excitons to produce a photocurrent. We performed detailed simulations of the band energies in quasi-metallic and semiconducting nanotube devices in order to obtain the electric field profiles along the lengths of the nanotubes. These simulations predict maximum built-in electric field strengths of 2.3 V/μm for semiconducting and 0.032-0.22 V/μm for quasi-metallic nanotubes under the applied gate voltages used in this study.

Zener tunneling and photocurrent generation in quasi-metallic carbon nanotube pn-devices.

We investigate the electronic and optoelectronic properties of quasi-metallic nanotube pn-devices, which have smaller band gaps than most known bulk semiconductors. These carbon nanotube-based devices deviate from conventional bulk semiconductor device behavior due to their low-dimensional nature. We observe rectifying behavior based on Zener tunneling of ballistic carriers instead of ideal diode behavior, as limited by the diffusive transport of carriers. We observe substantial photocurrents at room temperature, suggesting that these quasi-metallic pn-devices may have a broader impact in optoelectronic devices. A new technique based on photocurrent spectroscopy is presented to identify the unique chirality of nanotubes in a functional device. This chirality information is crucial in obtaining a theoretical understanding of the underlying device physics that depends sensitively on nanotube chirality, as is the case for quasi-metallic nanotube devices. A detailed model is developed to fit the observed I-V characteristics, which enables us to verify the band gap from these measurements as well as the dimensions of the insulating tunneling barrier region.

Photocurrent spectroscopy of exciton and free particle optical transitions in suspended carbon nanotube pn-junctions

We study photocurrent generation in individual, suspended carbon nanotube pn-junction diodes formed by electrostatic doping using two gate electrodes. Photocurrent spectra collected under various electrostatic doping concentrations reveal distinctive behaviors for free particle optical transitions and excitonic transitions. In particular, the photocurrent generated by excitonic transitions exhibits a strong gate doping dependence, while that of the free particle transitions is gate independent. Here, the built-in potential of the pn-junction is required to separate the strongly bound electron-hole pairs of the excitons, while free particle excitations do not require this field-assisted charge separation. We observe a sharp, well defined E11 free particle interband transition in contrast with previous photocurrent studies. Several steps are taken to ensure that the active charge separating region of these pn-junctions is suspended off the substrate in a suspended region that is substantially longer than th...

Competing Photocurrent Mechanisms in Quasi‐Metallic Carbon Nanotube pn Devices

Photodetectors based on quasi-metallic carbon nanotubes exhibit unique optoelectronic properties. Due to their small bandgap, photocurrent generation is possible at room temperature. The origin of this photocurrent is investigated to determine the underlying mechanism, which can be photothermoelectric effect or photovoltaic effect, depending on the bandgap magnitude of the quasi-metallic nanotube.

Evidence for structural phase transitions and large effective band gaps in quasi-metallic ultra-clean suspended carbon nanotubes

AbstractWe report evidence for a structural phase transition in individual suspended metallic carbon nanotubes by examining their Raman spectra and electron transport under electrostatic gate potentials. The current-gate voltage characteristics reveal anomalously large quasi-metallic band gaps as high as 240 meV, the largest reported to date. For nanotubes with band gaps larger than 200 meV, we observe a pronounced M-shape profile in the gate dependence of the 2D band (or G’ band) Raman frequency. The pronounced dip (or softening) of the phonon mode near zero gate voltage can be attributed to a structural phase transition (SPT) that occurs at the charge neutrality point (CNP). The 2D band Raman intensity also changes abruptly near the CNP, providing further evidence for a change in the lattice symmetry and a possible SPT. Pronounced non-adiabatic effects are observed in the gate dependence of the G band Raman mode, however, this behavior deviates from non-adiabatic theory near the CNP. For nanotubes with band gaps larger than 200 meV, non-adiabatic effects should be largely suppressed, which is not observed experimentally. This data suggests that these large effective band gaps are primarily caused by a SPT to an insulating state, which causes the large modulation observed in the conductance around the CNP. Possible mechanisms for this SPT are discussed, including electron-electron (e.g., Mott) and electron-phonon (e.g., Peierls) driven transitions.

Determination of free carrier concentration profiles and the valence‐band discontinuity energy of Hg0.7Cd0.3Te/Cd(4% Zn)Te heterojunctions using organic semiconductor layers

Capacitance‐voltage data are utilized to obtain the free‐carrier concentration in n‐ and p‐type Hg1−yCdyTe layers, and to measure the valence‐band discontinuity energy of a p‐type Hg0.7Cd0.3Te/Cd(4% Zn)Te isotype heterojunction. To facilitate measurement, rectifying contact was made to the Hg1−yCdyTe layers using one of two organic materials—metal‐free phthalocyanine and copper phthalocyanine. Contrary to previous results with this heterojunction system, we find that holes are accumulated near the Cd(4% Zn)Te side (rather than Hg1−yCdyTe side). We obtain a valence band discontinuity energy (ΔEv ) equal to (110±20) meV, and a fixed interface charge density of σ=−(5.9±0.3)×1010 cm−2.

Electromechanical resonance behavior of suspended single-walled carbon nanotubes under high bias voltages

We characterize the nanoelectromechanical response of suspended individual carbon nanotubes under high voltage biases. An abrupt upshift in the mechanical resonance frequency of approximately 3 MHz is observed at high bias. While several possible mechanisms are discussed, this upshift is attributed to the onset of optical phonon emission, which results in a sudden contraction of the nanotube due to its negative thermal expansion coefficient. This, in turn, causes an increase in the tension in the suspended nanotube, which upshifts its mechanical resonance frequency. This upshift is consistent with Raman spectral measurements, which show a sudden downshift of the optical phonon modes at high bias voltages. Using a simple model for oscillations on a string, we estimate the effective change in the length of the nanotube to be ΔL/L ≈ −2 × 10−5 at a bias voltage of 1 V.