Student Publications

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NanoJapan IREU: Student Peer-Reviewed Publications

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Excitonic effects on coherent phonon dynamics in single-wall carbon nanotubes
(The American Physical Society, 2013) Nugraha, A.R.T.; Rosenthal, E.I.; Hasdeo, E.H.; Sanders, G.D.; Stanton, C.J.; Dresselhaus, M.S.; Saito, R.
We discuss how excitons can affect the generation of coherent radial breathing modes in the ultrafast spectroscopy of single-wall carbon nanotubes. Photoexcited excitons can be localized spatially and give rise to a spatially distributed driving force in real space which involves many phonon wave vectors of the exciton-phonon interaction. The equation of motion for the coherent phonons is modeled phenomenologically by the Klein-Gordon equation, which we solve for the oscillation amplitudes as a function of space and time. By averaging the calculated amplitudes per nanotube length, we obtain time-dependent coherent phonon amplitudes that resemble the homogeneous oscillations that are observed in some pump-probe experiments. We interpret this result to mean that the experiments are only able to see a spatial average of coherent phonon oscillations over the wavelength of light in carbon nanotubes and the microscopic details are averaged out. Our interpretation is justified by calculating the time-dependent absorption spectra resulting from the macroscopic atomic displacements induced by the coherent phonon oscillations. The calculated coherent phonon spectra including excitonic effects show the experimentally observed symmetric peaks at the nanotube transition energies, in contrast to the asymmetric peaks that would be obtained if excitonic effects were not included.
Collective antenna effects in the terahertz and infrared response of highly aligned carbon nanotube arrays
(The American Physical Society, 2013) Ren, L.; Zhang, Q.; Pint, C.L.; Wójcik, A.K.; Bunney, M. Jr; Arikawa, T.; Kawayama, I.; Tonouchi, M.; Hauge, R.H.; Belyanin, A.A.; Kono, J.
We study macroscopically aligned single-wall carbon nanotube arrays with uniform lengths via polarization-dependent terahertz and infrared transmission spectroscopy. Polarization anisotropy is extreme at frequencies less than ∼100 cm−1 with no sign of attenuation when the polarization is perpendicular to the alignment direction. The attenuation for both parallel and perpendicular polarizations increases with increasing frequency, exhibiting a pronounced and broad peak around 450 cm−1 in the parallel case. We model the electromagnetic response of the sample by taking into account both radiative scattering and absorption losses. We show that our sample acts as an effective antenna due to the high degree of alignment, exhibiting much larger radiative scattering than absorption in the mid/far-infrared range. Our calculated attenuation spectrum clearly shows a non-Drude peak at ∼450 cm−1 in agreement with the experiment.
Photoluminescence sidebands of carbon nanotubes below the bright singlet excitonic levels
(The American Physical Society, 2009) Murakami, Yoichi; Lu, Benjamin; Kazaoui, Said; Minami, Nobutsugu; Okubo, Tatsuya; Maruyama, Shigeo
We performed detailed photoluminescence (PL) spectroscopy studies of three different types of single-walled carbon nanotubes (SWNTs) by using samples that contain essentially only one chiral type of SWNT, (6,5), (7,5), or (10,5). The observed PL spectra unambiguously show the existence of an emission sideband at ∼140 meV below the lowest singlet excitonic (E11) level, whose identity and origin are now under debate. We find that the energy separation between the E11 level and the sideband is independent of the SWNT diameter within our experimental certainty. Based on this, we ascribe the origin of the observed sideband to coupling between K-point phonons and dipole-forbidden dark excitons, as recently suggested based on the measurement of (6,5) SWNTs.
GR-FET application for high-frequency detection device
(Springer, 2013) Mahjoub, Akram M.; Nicol, Alec; Abe, Takuto; Ouchi, Takahiro; Iso, Yuhei; Kida, Michio; Aoki, Noboyuki; Miyamoto, Katsuhiko; Omatsu, Takashige; Bird, Jonathan P.; Ferry, David K.; Ishibashi, Koji; Ochiai, Yuichi
A small forbidden gap matched to low-energy photons (meV) and a quasi-Dirac electron system are both definitive characteristics of bilayer graphene (GR) that has gained it considerable interest in realizing a broadly tunable sensor for application in the microwave region around gigahertz (GHz) and terahertz (THz) regimes. In this work, a systematic study is presented which explores the GHz/THz detection limit of both bilayer and single-layer graphene field-effect transistor (GR-FET) devices. Several major improvements to the wiring setup, insulation architecture, graphite source, and bolometric heating of the GR-FET sensor were made in order to extend microwave photoresponse past previous reports of 40 GHz and to further improve THz detection.
Imaging molecular adsorption and desorption dynamics on graphene using terahertz emission spectroscopy
(Nature Publishing Group, 2014) Ajayan, P.M.; Kono, J.; Tonouchi, M.
Being an atomically thin material, graphene is known to be extremely susceptible to its environment, including defects and phonons in the substrate on which it is placed as well as gas molecules that surround it. Thus, any device design using graphene has to take into consideration all surrounding components, and device performance needs to be evaluated in terms of environmental influence. However, no methods have been established to date to readily measure the density and distribution of external perturbations in a quantitative and non-destructive manner. Here, we present a rapid and non-contact method for visualizing the distribution of molecular adsorbates on graphene semi-quantitatively using terahertz time-domain spectroscopy and imaging. We found that the waveform of terahertz bursts emitted from graphene-coated InP sensitively changes with the type of atmospheric gas, laser irradiation time, and ultraviolet light illumination. The terahertz waveform change is explained through band structure modifications in the InP surface depletion layer due to the presence of localized electric dipoles induced by adsorbed oxygen. These results demonstrate that terahertz emission serves as a local probe for monitoring adsorption and desorption processes on graphene films and devices, suggesting a novel two-dimensional sensor for detecting local chemical reactions.
Macroscopic Ensembles of Aligned Carbon Nanotubes in Bubble Imprints Studied by Polarized Raman Microscopy
(Hindawi Publishing Corporation, 2014) Ushiba, Shota; Hoyt, Jordan; Masui, Kyoko; Kono, Junichiro; Kawata, Satoshi; Shoji, Satoru; NanoJapan Program
We study the alignment of single-wall carbon nanotubes (SWCNTs) in bubble imprints through polarized Raman microscopy. A hemispherical bubble containing SWCNTs is pressed against a glass substrate, resulting in an imprint of the bubble membrane with a coffee ring on the substrate. We find that macroscopic ensembles of aligned SWCNTs are obtained in the imprints, in which there are three patterns of orientations: (i) azimuthal alignment on the coffee ring, (ii) radial alignment at the edge of the membrane, and (iii) random orientation at the center of the membrane. We also find that the alignment of SWCNTs in the imprints can be manipulated by spinning bubbles. The orientation of SWCNTs on the coffee ring is directed radially, which is orthogonal to the case of unspun bubbles. This approach enables one to align SWCNTs in large quantities and in a short time, potentially opening up a wide range of CNT-based electronic and optical applications.

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