Hong En Lim

Growth of carbon nanotubes via twisted graphene nanoribbons.

Carbon nanotubes have long been described as rolled-up graphene sheets. It is only fairly recently observed that longitudinal cleavage of carbon nanotubes, using chemical, catalytical and electrical approaches, unzips them into thin graphene strips of various widths, the so-called graphene nanoribbons. In contrast, rolling up these flimsy ribbons into tubes in a real experiment has not been possible. Theoretical studies conducted by Kit et al. recently demonstrated the tube formation through twisting of graphene nanoribbon, an idea very different from the rolling-up postulation. Here we report the first experimental evidence of a thermally induced self-intertwining of graphene nanoribbons for the preferential synthesis of (7, 2) and (8, 1) tubes within parent-tube templates. Through the tailoring of ribbon’s width and edge, the present finding adds a radically new aspect to the understanding of carbon nanotube formation, shedding much light on not only the future chirality tuning, but also contemporary nanomaterials engineering.

Short channel field-effect transistors from highly enriched semiconducting carbon nanotubes

AbstractSemiconducting single-walled carbon nanotubes (s-SWNTs) with a purity of ∼98% have been obtained by gel filtration of arc-discharge grown SWNTs with diameters in the range 1.2–1.6 nm. Multi-laser Raman spectroscopy confirmed the presence of less than 2% of metallic SWNTs (m-SWNTs) in the s-SWNT enriched sample. Measurement of ∼50 individual tubes in Pd-contacted devices with channel length 200 nm showed on/off ratios of >104, conductances of 1.38–5.8 μS, and mobilities in the range 40–150 cm2·V/s. Short channel multi-tube devices with ∼100 tubes showed lower on/off ratios due to residual m-SWNTs, although the on-current was greatly increased relative to the devices made from individual tubes.

Anisotropic optical and electronic properties of two-dimensional layered germanium sulfide

Two-dimensional (2D) layered materials, transition-metal dichalcogenides, and black phosphorus have attracted considerable interest from the viewpoints of fundamental physics and device applications. The establishment of new functionalities in anisotropic layered 2D materials is a challenging but rewarding frontier, owing to the remarkable optical properties of these materials and their prospects for new devices. Herein, we report the anisotropic and thickness-dependent optical properties of a 2D layered monochalcogenide of germanium sulfide (GeS). Three Raman-scattering peaks corresponding to the B3g, Ag1, and Ag2 modes with a strong polarization dependence are demonstrated in the GeS flakes, which validates polarized Raman spectroscopy as an effective method for identifying the crystal orientation of anisotropic layered GeS. Photoluminescence (PL) is observed with a peak at ~1.66 eV that originates from the direct optical transition in GeS at room temperature. The polarization-dependent characteristics of the PL, which are revealed for the first time, along with the demonstration of anisotropic absorption, indicate an obvious anisotropic optical transition near the band edge of GeS, which is supported by density functional theory calculations. The significantly thickness-dependent PL is observed and discussed. This anisotropic layered GeS presents opportunities for the discovery of new physical phenomena and will find applications that exploit its anisotropic properties, such as polarization-sensitive photodetectors.

Fabrication and Optical Probing of Highly Extended, Ultrathin Graphene Nanoribbons in Carbon Nanotubes

Nanotemplated growth of graphene nanoribbons (GNRs) inside carbon nanotubes is a promising mean to fabricate ultrathin ribbons with desired side edge configuration. We report the optical properties of the GNRs formed in single-wall carbon nanotubes. When coronene is used as the precursor, extended GNRs are grown via a high-temperature annealing at 700 °C. Their optical responses are probed through the diazonium-based side-wall functionalization, which effectively suppresses the excitonic absorption peaks of the nanotubes without damaging the inner GNRs. Differential absorption spectra clearly show two distinct peaks around 1.5 and 3.4 eV. These peaks are assigned to the optical transitions between the van Hove singularities in the density of state of the GNRs in qualitative agreement with the first-principles calculations. Resonance Raman spectra and transmission electron microscope observations also support the formation of long GNRs.

Purity-enhanced bulk synthesis of thin single-wall carbon nanotubes using iron–copper catalysts

We report high purity and high yield synthesis of single-wall carbon nanotubes (SWCNTs) of narrow diameter from iron-copper bimetal catalysts. The SWCNTs with diameter of 0.8-1.2 nm are synthesized using the zeolite-supported alcohol chemical vapour deposition method. Single metal and bimetal catalysts are systematically investigated to achieve both the enhancement of SWCNT yield and the suppression of the undesired formation of graphitic impurities. The relative yield and purity of SWCNTs are quantified using optical absorption spectroscopy with an ultracentrifuge-based purification technique. For the single metal catalyst, iron shows the highest catalytic activity compared with the other metals such as cobalt, nickel, molybdenum, copper, and platinum. It has been found that the addition of copper to iron results in the suppression of carbonaceous impurity formation without decreasing the SWCNT yield. The purity-enhanced SWCNT shows fairly low sheet resistance due to the improvement of inter-nanotube contacts. This scalable design of SWCNT synthesis with enhanced purity is therefore a promising tool for shaping future high performance devices.

Carrier Transport and Photoresponse in GeSe/MoS2 Heterojunction p–n Diodes

Simple stacking of thin van der Waals 2D materials with different physical properties enables one to create heterojunctions (HJs) with novel functionalities and new potential applications. Here, a 2D material p-n HJ of GeSe/MoS2 is fabricated and its vertical and horizontal carrier transport and photoresponse properties are studied. Substantial rectification with a very high contrast (>104 ) through the potential barrier in the vertical-direction tunneling of HJs is observed. The negative differential transconductance with high peak-to-valley ratio (>105 ) due to the series resistance change of GeSe, MoS2 , and HJs at different gate voltages is observed. Moreover, strong and broad-band photoresponse via the photoconductive effect are also demonstrated. The explored multifunctional properties of the GeSe/MoS2 HJs are expected to be important for understanding the carrier transport and photoresponse of 2D-material HJs for achieving their use in various new applications in the electronics and optoelectronics fields.

Long radiative lifetimes of excitons in monolayer transition-metal dichalcogenides MX 2 (M = Mo, W; X = S, Se)

We studied the effective exciton radiative lifetimes of monolayer two-dimensional transition-metal dichalcogenides MX 2 (M = Mo, W; X = S, Se). The photoluminescence (PL) quantum yield and PL decay time were measured for monolayer MoS2, MoSe2, WS2, and WSe2 at room temperature. Effective exciton radiative lifetimes of >10 ns were determined from the PL quantum yield of 10−2 to 10−3 and the PL decay time of several hundred picoseconds. The results are explained on the basis of the long radiative lifetime of bright excitons at a low temperature limit, a finite exciton coherence area of several square nanometers, and the population of dark exciton states.

Photoluminescence quantum yields for atomically thin-layered ReS2: Identification of indirect-bandgap semiconductors

Rhenium dichalcogenides have attracted considerable attention as new members of group VII layered semiconductor transition-metal dichalcogenides (TMDs) with respect to fundamental physics and potential applications. In this study, room-temperature photoluminescence (PL) spectra, as well as PL quantum yields (QYs) of thin-layer rhenium disulfide (ReS2), were evaluated. Low PL QYs of ∼10–4 were determined from a monolayer thickness to seven layers (1–7L) of ReS2 regardless of the layer number. These low PL QYs strongly suggest that the ReS2 is an indirect-bandgap semiconductor from a monolayer limit to the bulk, which is in contrast to those observed for group VI TMDs (MX2: M = Mo and W; X = S and Se). Our experimental findings will provide valuable information for the electronic and optical device applications in atomically thin-layered ReS2.Rhenium dichalcogenides have attracted considerable attention as new members of group VII layered semiconductor transition-metal dichalcogenides (TMDs) with respect to fundamental physics and potential applications. In this study, room-temperature photoluminescence (PL) spectra, as well as PL quantum yields (QYs) of thin-layer rhenium disulfide (ReS2), were evaluated. Low PL QYs of ∼10–4 were determined from a monolayer thickness to seven layers (1–7L) of ReS2 regardless of the layer number. These low PL QYs strongly suggest that the ReS2 is an indirect-bandgap semiconductor from a monolayer limit to the bulk, which is in contrast to those observed for group VI TMDs (MX2: M = Mo and W; X = S and Se). Our experimental findings will provide valuable information for the electronic and optical device applications in atomically thin-layered ReS2.

Photoluminescence quantum yield and long exciton radiative lifetime in monolayer two-dimensional transition metal dichalcogenides

Semiconducting transition metal dichalcogenides (TMDs) have attracted great research interests due to both from fundamental physics and their interesting potential applications of optoelectronic devices. It is very crucial to know its photoluminescence (PL) quantum yield, concurrently with the radiative lifetimes of its elementary excitation, exciton (electron-hole pair). We have experimentally evaluated intrinsic exciton radiative lifetime of 2D (two-dimensional) semiconductor TMDs of monolayer WSe2 from static and time-resolved PL spectroscopy at room temperature. In order to calculate the radiative lifetime, we also employed PL quantum yield measurements using relative method with standard reference fluorescent dye. The exciton radiative lifetime of ~40 ns was evaluated from PL quantum yield of ~1 % and PL decay time of several hundred ps. This value of radiative lifetime of several tenth ns suggests the contribution of dark states and finite exciton coherence length (area) of several nm.