Individual Suspended Carbon Nanotubes Research Articles

(Invited) Broadband Electroluminescence from Reverse Breakdown in Individual Suspended Carbon Nanotube Pn-Junctions

There are various mechanisms of light emission in carbon nanotubes (CNTs), which give rise to a wide range of spectral emission characteristics that provide important information regarding the underlying physical processes that lead to photon emission. Here, we report spectra obtained from individual suspended CNT dual-gate field effect transistor (FET) devices under different gate and bias conditions. By applying opposite voltages to the gate electrodes (i.e., Vg1 = –Vg2), we are able to create a pn-junction within the suspended region of the CNT. Under forward bias conditions, the spectra exhibit a peak corresponding to E11 exciton emission via thermal (i.e., blackbody) emission occurring at electrical powers around 8 μW, which corresponds to a power density of approximately 0.5 MW/cm2. On the other hand, the spectra observed under reverse bias correspond to impact ionization and avalanche emission, which occurs at electrical powers of ~ 10 nW and exhibits a featureless flat spectrum extending from 1,600 nm to shorter wavelengths up to 600 nm. Here, the hot electrons generated by the high electric fields (~ 0.5 MV/cm) are able to produce high energy photons far above the E11 (ground state) energy. It is somewhat surprising that these devices do not exhibit light emission by the annihilation of electrons and holes under forward bias, as in a light emitting diode (LED). Possible reasons for this are discussed, including Auger recombination.DOI: 10.1007/s12274-020-2941-3 Figure 1

Fast In-Situ Optical Visualization of Carbon Nanotubes Assisted by Smoke.

The fast visualization and manipulation of individual carbon nanotubes (CNTs) has always been a significant technology for their fundamental research. Here, a fast and facile approach is proposed to realize the optical observation of individual suspended CNTs and CNT networks under conventional optical microscopes with the assistance of tar nanodroplets from smoke. The nanodroplets deposited on CNTs render them with strong light scattering to visible light, thus making the CNTs visible under optical microscopes. This visualization method is controllable, environmentally friendly, low-cost, and can be completed in just a few seconds in ambient conditions. Besides, the tar nanodroplets can be easily removed from the CNTs by laser irradiation. More importantly, the smoke sources are widely available and there are no strict requirements for operating conditions. This smoke-assisted visualization method shows great potential in the fundamental research of CNTs.

Optical Phonon Scattering Dominated Transport in Individual Suspended Carbon Nanotubes

Optical Phonon Scattering Dominated Transport in Individual Suspended Carbon Nanotubes

Broadband electroluminescence from reverse breakdown in individual suspended carbon nanotube pn-junctions

There are various mechanisms of light emission in carbon nanotubes (CNTs), which give rise to a wide range of spectral emission characteristics that provide important information regarding the underlying physical processes that lead to photon emission. Here, we report spectra obtained from individual suspended CNT dual-gate field effect transistor (FET) devices under different gate and bias conditions. By applying opposite voltages to the gate electrodes (i.e., Vg1 = −Vg2), we are able to create a pn-junction within the suspended region of the CNT. Under forward bias conditions, the spectra exhibit a peak corresponding to E11 exciton emission via thermal (i.e., blackbody) emission occurring at electrical powers around 8 µW, which corresponds to a power density of approximately 0.5 MW/cm2. On the other hand, the spectra observed under reverse bias correspond to impact ionization and avalanche emission, which occurs at electrical powers of ~10 nW and exhibits a featureless flat spectrum extending from 1,600 nm to shorter wavelengths up to 600 nm. Here, the hot electrons generated by the high electric fields (~0.5 MV/cm) are able to produce high energy photons far above the E11 (ground state) energy. It is somewhat surprising that these devices do not exhibit light emission by the annihilation of electrons and holes under forward bias, as in a light emitting diode (LED). Possible reasons for this are discussed, including Auger recombination.

Optical Phonon Scattering Dominated Transport in Individual Suspended Carbon Nanotubes

The transport property of six types of individual carbon nanotubes (CNT) with specified chiral indices at high temperature is investigated on a home‐made apparatus. It is found that the resistivity of all individual CNTs increases with temperature monotonically, whereas the mobility decreases with temperature and follows different laws in different temperature ranges. The carrier concentration increases exponentially with −1/T. The mobility of CNT deviates from traditional trends with temperature, T−β, at high temperature (1070–1728 K). This deviation is attributed to scattering with optical phonons at high temperature. The data show that the electron‐optical phonon interaction becomes dominant in the temperature range of 1070–1362 K for all measured CNTs. Finally, result within a polaron model is discussed.

The Influence of Carbon Nanotube's Conductivity and Diameter on Its Thermionic Electron Emission

High‐temperature thermionic electron emission from different types of individual suspended carbon nanotubes (CNTs) in a homemade chip is studied. When collecting emission electrons with an external electrode, it is found that the collecting electric field influence the transport current in the CNTs, and the thermionic electron emission deviated from the traditional thermionic electron emission model and cannot reach “saturation”. This effect is analyzed for single‐walled, double‐walled, multiwalled‐CNT and CNT bundles. It is found that this effect show correlation with the conductivity and diameter of the CNT. With the increase in metallicity, the influence of collecting electrode is gradually weakened. Also, the effect shows a negative correlation with the diameter of CNTs. An equation is proposed to describe the measured thermionic emission curve and determine the “effective” work function of the CNT.

Spectroscopic signatures of spin-orbit coupling and free excitons in individual suspended carbon nanotubes

We investigate the intrinsic magneto-optical properties of suspended single-walled carbon nanotubes of various chiralities, using a combination of spectrally and time-resolved spectroscopy of individual nanotubes at low temperature. This study elucidates the population and relaxation dynamics of the lowest-energy bright and dark singlet excitons that are mixed with the Aharonov-Bohm effect. The high-quality emission spectra reveal the residual oscillator strength of the dark exciton in zero field, as an optical signature of spin-orbit coupling. They also unveil an asymmetry in the bright exciton recombination line, attributed to the free nature of excitons in these unperturbed nanotubes.

Defect-Induced Photoluminescence Enhancement and Corresponding Transport Degradation in Individual Suspended Carbon Nanotubes

Defect-Induced Photoluminescence Enhancement and Corresponding Transport Degradation in Individual Suspended Carbon Nanotubes

Photocurrent Quantum Yield in Suspended Carbon Nanotube p-n Junctions.

We study photocurrent generation in individual suspended carbon nanotube p-n junctions using spectrally resolved scanning photocurrent microscopy. Spatial maps of the photocurrent allow us to determine the length of the p-n junction intrinsic region, as well as the role of the n-type Schottky barrier. We show that reverse-bias operation eliminates complications caused by the n-type Schottky barrier and increases the length of the intrinsic region. The absorption cross-section of the CNT is calculated using an empirically verified model, and the effect of substrate reflection is determined using FDTD simulations. We find that the room temperature photocurrent quantum yield is approximately 30% when exciting the carbon nanotube at the S44 and S55 excitonic transitions. The quantum yield value is an order of magnitude larger than previous estimates.

(Invited) Exciton Dissociation and Trion Generation in Individual Carbon Nanotubes

Screening is limited in single-walled carbon nanotubes because of their one-dimensional nature, and the strong Coulomb interactions result in optical spectra dominated by excitons with binding energies lager than half an eV. Also because of the limited screening, a charged carrier can be bound to an exciton to form a trion that is stable at room temperature. Here we discuss experiments aimed at highlighting the behaviors of excitons and trions under electric fields. Microspectroscopy measurements are performed on individual suspended carbon nanotubes integrated into field-effect devices. Simultaneous photoluminescence and photoconductivity spectroscopy show evidences for spontaneous dissociation [1], despite the expectation that free carrier generation from such a tightly-bound state would be difficult. As the field is increased, we observe an emergence of new absorption peaks in the excitation spectra, which can be explained by electrical activation of dark excited states [2]. Although trion formation has been thought to be difficult in suspended nanotubes due to low exciton-carrier scattering rates, we have succeeded in identifying trion emission under an application of gate voltages [3]. Work supported by KAKENHI, The Canon Foundation, The Asahi Glass Foundation, and the Photon Frontier Network Program of MEXT, Japan. [1] Y. Kumamoto, M. Yoshida, A. Ishii, A. Yokoyama, T. Shimada, Y. K. Kato, Phys. Rev. Lett. 112, 117401 (2014).[2] T. Uda, M. Yoshida, A. Ishii, Y. K. Kato, submitted.[3] M. Yoshida, A. Popert, Y. K. Kato, arXiv:1510.08996.

Tunable electronic correlation effects in nanotube-light interactions

Electronic many-body correlation effects in one-dimensional (1D) systems such as carbon nanotubes have been predicted to strongly modify the nature of photoexcited states. Here we directly probe this effect using broadband elastic light scattering from individual suspended carbon nanotubes under electrostatic gating conditions. We observe significant shifts in optical transition energies, as well as line broadening, as the carrier density is increased. The results demonstrate the role of screening of many-body electronic interactions on the different length scales, a feature inherent to quasi-1D systems. Our findings further demonstrate the possibility of electrical tuning of optical transitions and provide a basis for understanding of various optical phenomena in carbon nanotubes and other quasi-1D systems in the presence of charge carrier doping.

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.

(Invited) Optoelectronic Properties and Electromechanical Resonance Behavior in Individual Suspended Carbon Nanotube Pn-Junctions and Devices

In carbon nanotubes pn-junctions, we observe Zener tunneling behavior and photocurrent generation in quasi-metallic nanotubes1, 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. We also explore the role of weak clamping forces, typically assumed to be infinite, in the electromechanical resonance behavior of these suspended carbon nanotubes.2 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. 1. Amer, M.R., S.-W. Chang, R. Dhall, J. Qiu and S. Cronin, “Zener Tunneling and Photocurrent Generation in Quasi-Metallic Carbon Nanotube pn-Devices” Nano Letters, 13, 5129 (2013). 2. Mehmet Aykol, Bingya Hou, Rohan Dhall, Shun-Wen Chang, William Branham, Jing Qiu, and Stephen Cronin, "Clamping Instability and van der Waals Forces in Carbon Nanotube Mechanical Resonators" Nano Letters, 14, 2426 (2014). 3. Shun-Wen Chang, Kevin Bergemann, Rohan Dhall, Jeramy Zimmerman, Stephen Forrest, Stephen Cronin, "Non-ideal Diode Behavior and Band Gap Renormalization in Carbon Nanotube P-N Junctions" IEEE Transactions on Nanotechnology, 13, 41 (2014).

Bright, long-lived and coherent excitons in carbon nanotube quantum dots

Carbon nanotubes exhibit a wealth of unique physical properties. By virtue of their exceptionally low mass and extreme stiffness they provide ultrahigh-quality mechanical resonances, promise long electron spin coherence times in a nuclear-spin free lattice for quantum information processing and spintronics, and feature unprecedented tunability of optical transitions for optoelectronic applications. Excitons in semiconducting single-walled carbon nanotubes could facilitate the upconversion of spin, mechanical or hybrid spin-mechanical degrees of freedom to optical frequencies for efficient manipulation and detection. However, successful implementation of such schemes with carbon nanotubes has been impeded by rapid exciton decoherence at non-radiative quenching sites, environmental dephasing and emission intermittence. Here we demonstrate that these limitations may be overcome by exciton localization in suspended carbon nanotubes. For excitons localized in nanotube quantum dots we found narrow optical lines free of spectral wandering, radiative exciton lifetimes and effectively suppressed blinking. Our findings identify the great potential of localized excitons for efficient and spectrally precise interfacing of photons, phonons and spins in novel carbon nanotube-based quantum devices.

Pointwise Plucking of Suspended Carbon Nanotubes

Vibration of nanotubes/wires is significant for fundamental and applied researches. However, it remains challenging to control the vibration with point-level precision. Herein, individual suspended carbon nanotubes are plucked point by point to vibrate in scanning electron microscope with the electron beam as a nanoscale pointer. The vibration is directly imaged, and its images fit well with simulations from the plucking mechanism. This demonstrates a new way to manipulate the nanotube vibration with unprecedented precision.

Direct observation of heat dissipation in individual suspended carbon nanotubes using a two-laser technique

A two-laser technique is used to investigate heat spreading along individual single walled carbon nanotube (SWCNT) bundles in vacuum and air environments. A 532 nm laser focused on the center of a suspended SWCNT bundle is used as a local heat source, and a 633 nm laser is used to measure the spatial temperature profile along the SWCNT bundle by monitoring the G band downshifts in the Raman spectra. A constant temperature gradient is observed when the SWCNT bundle is irradiated in vacuum, giving direct evidence of diffusive transport of the phonons probed by the Raman laser. In air, however, we observe an exponentially decaying temperature profile with a decay length of about 7 μm, due to heat dissipation from the SWCNT bundle to the surrounding gas molecules. The thermal conductivity of the suspended carbon nanotube (CNT) is determined from its electrical heating temperature profile as measured in vacuum and the nanotube bundle diameter measured via transmission electron microscopy. Based on the exponential decay curves measured in three different CNTs in air, the heat transfer coefficient between the SWCNTs and the surrounding air molecules is found to range from 1.5 × 103 to 7.9 × 104 W/m2 K, which is smaller than the 1 × 105 W/m2 K thermal boundary conductance value calculated using the kinetic theory of gases. This measurement is insensitive to the thermal contact resistance, as no temperature drops occur at the ends of the nanotube. It is also insensitive to errors in the calibration of the G band temperature coefficient. The optical absorption is also obtained from these results and is on the order of 10−5.

Thermal Emission Spectra from Individual Suspended Carbon Nanotubes

We study the thermal emission spectra of individual suspended carbon nanotubes induced by electrical heating. Semiconducting and metallic devices exhibit different spectra, based on their distinctive band structures. These spectra are compared with the ideal blackbody emission spectrum. In the visible wavelength range, the thermal emission spectra of semiconducting devices agree well with Planck's law, while the spectra of metallic devices show an additional peak between 1.5 and 1.9 eV. In the near-infrared wavelength range, the semiconducting nanotubes exhibit a peak around 1 eV. These additional peaks are attributed to the E11M and E22SC transitions that are thermally driven under these high applied bias voltages. These peaks show a strong polarization dependence, while the blackbody tail is unpolarized, which provides further evidence for electron-hole recombination in thermal emission. For semiconducting devices, the temperature of the nanotube is fit to Planck's law and compared with the temperatures obtained from the G band and 2D band Raman downshifts, as well as the anti-Stokes/Stokes intensity ratio. For devices showing thermal non-equilibrium, the electron temperature agrees well with G+ downshift but deviates from G_ downshift.

(Invited) Individual Suspended Carbon Nanotubes under Applied Gate and Bias Potentials

not Available.

Optical Absorption and Thermal Transport of Individual Suspended Carbon Nanotube Bundles

A focused laser beam is used to heat individual single-walled carbon nanotube bundles bridging two suspended microthermometers. By measurement of the temperature rise of the two thermometers, the optical absorption of 7.4-10.3 nm diameter bundles is found to be between 0.03 and 0.44% of the incident photons in the 0.4 microm diameter laser spot. The thermal conductance of the bundle is obtained with the additional measurement of the temperature rise of the nanotubes in the laser spot from shifts in the Raman G band frequency. According to the nanotube bundle diameter determined by transmission electron microscopy, the thermal conductivity is obtained.