Young Kuk

Bandgap modulation of carbon nanotubes by encapsulated metallofullerenes

Motivated by the technical and economic difficulties in further miniaturizing silicon-based transistors with the present fabrication technologies, there is a strong effort to develop alternative electronic devices, based, for example, on single molecules. Recently, carbon nanotubes have been successfully used for nanometre-sized devices such as diodes, transistors, and random access memory cells. Such nanotube devices are usually very long compared to silicon-based transistors. Here we report a method for dividing a semiconductor nanotube into multiple quantum dots with lengths of about 10 nm by inserting Gd@C82 endohedral fullerenes. The spatial modulation of the nanotube electronic bandgap is observed with a low-temperature scanning tunnelling microscope. We find that a bandgap of ∼0.5 eV is narrowed down to ∼0.1 eV at sites where endohedral metallofullerenes are inserted. This change in bandgap can be explained by local elastic strain and charge transfer at metallofullerene sites. This technique for fabricating an array of quantum dots could be used for nano-electronics and nano-optoelectronics.

Large-scale soft colloidal template synthesis of 1.4 nm thick CdSe nanosheets.

Two-dimensional (2D) nanocrystals have attracted tremendous attention from many researchers in various disciplines because of their unique properties. Since ways of making graphene were devised, there have been significant research efforts to synthesize free-standing 2D nanocrystals of various materials, including metals, oxides, and chalcogenides. Many of these 2D nanocrystals have been generated from exfoliation of materials with layered structures, and tiny amounts of products are generally produced. CdSe nanocrystals are among the most intensively studied nanostructured materials, owing to their many size-dependent optical and electrical characteristics and resulting exciting applications. Herein, we report on the large-scale synthesis of single-layered and lamellar-structured 2D CdSe nanocrystals with wurtzite crystal structure as thin as 1.4 nm by a soft colloidal template method. These free-standing 2D nanocrystals with insulating organic layers at the interface could find many interesting electronic and optoelectronic applications, including in quantum cascade lasers and resonant tunneling diodes utilizing their multiple quantum well structures. Compared to materials with layered crystal structures such as graphite, the synthesis of free-standing 2D nanocrystals of nonlayered materials such as CdSe is extremely challenging, because selective growth along one specific facet among several with similar energies is required. For example, in CdSe with a hexagonal wurtzite crystal structure, a (0001) facet has significantly higher surface energy than other facets, which leads to the formation of many one-dimensional nanostructures. Although there is a slight difference in the surface energies of (1120) and (1100) facets, quantum-confined thin CdSe 2D nanocrystals could not be synthesized using a conventional colloidal chemical route that employs thermal decomposition of precursors at high temperature, because the small difference in the surface energies of these two facets is negated by the high reaction temperature. Consequently, there have been only a few reports on the successful chemical synthesis of 2D CdSe nanocrystals. For example, CdSe inorganic–organic hybrid lamellar structures and CdSe nanoplatelets with zinc-blende structure were synthesized using colloidal chemical routes. However, their 2D growth mechanism has not been clearly elucidated. Furthermore, nanostructural control to form single-layered or multiple-layered nanosheets has not been demonstrated. In the current approach to creating 2D CdSe nanocrystals, we employed a soft template method, and we were able to synthesize not only free-standing single-layered CdSe nanosheets but also lamellar-structured nanosheets by controlling the interaction between organic layers in 2D templates of cadmium chloride alkyl amine complexes. It has been reported that the complex of cadmium halide and diamine can form a cadmium halide /diamine alternating layered structure through diamine bridging and hydrogen bonding between hydrogen atoms of the amine and halogen atoms. Likewise, a [CdCl2(RNH2)2] lamellar complex, which is used herein as a soft template, is expected to form lamellar structures composed of 2D arrays of CdCl2 and alkyl amine by van der Waals attraction between hydrocarbon sidechains of the alkyl amine. The small-angle X-ray scattering (SAXS) patterns of [CdCl2(RNH2)2] complexes with butylamine (BA), octylamine (OA), and dodecylamine (DA) show 00l orders of reflection, which confirms that the complexes formed typical lamellar structures (Supporting Information, Figure S1). A [CdCl2(OA)2] lamellar complex was chosen as the soft template for the synthesis of lamellarstructured CdSe nanosheets because of its optimum reactivity. [*] J. S. Son, Dr. J. Joo, K. Park, Dr. J. H. Kim, Dr. K. An, J. H. Yu, S. G. Kwon, Dr. S.-H. Choi, Prof. T. Hyeon National Creative Research Initiative Center for Oxide Nanocrystalline Materials and School of Chemical and Biological Engineering Seoul National University Seoul 151-744 (Korea) Fax: (+82)2-886-8457 E-mail: thyeon@snu.ac.kr

n-Type Nanostructured Thermoelectric Materials Prepared from Chemically Synthesized Ultrathin Bi2Te3 Nanoplates

We herein report on the large-scale synthesis of ultrathin Bi(2)Te(3) nanoplates and subsequent spark plasma sintering to fabricate n-type nanostructured bulk thermoelectric materials. Bi(2)Te(3) nanoplates were synthesized by the reaction between bismuth thiolate and tri-n-octylphosphine telluride in oleylamine. The thickness of the nanoplates was ~1 nm, which corresponds to a single layer in Bi(2)Te(3) crystals. Bi(2)Te(3) nanostructured bulk materials were prepared by sintering of surfactant-removed Bi(2)Te(3) nanoplates using spark plasma sintering. We found that the grain size and density were strongly dependent on the sintering temperature, and we investigated the effect of the sintering temperature on the thermoelectric properties of the Bi(2)Te(3) nanostructured bulk materials. The electrical conductivities increased with an increase in the sintering temperature, owing to the decreased interface density arising from the grain growth and densification. The Seebeck coefficients roughly decreased with an increase in the sintering temperature. Interestingly, the electron concentrations and mobilities strongly depended on the sintering temperature, suggesting the potential barrier scattering at interfaces and the doping effect of defects and organic residues. The thermal conductivities also increased with an increase in the sintering temperature because of grain growth and densification. The maximum thermoelectric figure-of-merit, ZT, is 0.62 at 400 K, which is one of the highest among the reported values of n-type nanostructured materials based on chemically synthesized nanoparticles. This increase in ZT shows the possibility of the preparation of highly efficient thermoelectric materials by chemical synthesis.

Experimental evidence for s-wave pairing symmetry in superconducting Cu(x)Bi2Se3 single crystals using a scanning tunneling microscope.

Topological superconductors represent a newly predicted phase of matter that is topologically distinct from conventional superconducting condensates of Cooper pairs. As a manifestation of their topological character, topological superconductors support solid-state realizations of Majorana fermions at their boundaries. The recently discovered superconductor CuxBi2Se3 has been theoretically proposed as an odd-parity superconductor in the time-reversal-invariant topological superconductor class and point-contact spectroscopy measurements have reported the observation of zero-bias conductance peaks corresponding to Majorana states in this material. Here we report scanning tunneling spectroscopy (STS) measurements of the superconducting energy gap in CuxBi2Se3 as a function of spatial position and applied magnetic field. The tunneling spectrum shows that the density of states at the Fermi level is fully gapped without any in-gap states. The spectrum is well described by the Bardeen-Cooper-Schrieffer (BCS) theory with a momentum independent order parameter, which suggests that Cu0.2Bi2Se3 is a classical s-wave superconductor contrary to previous expectations and measurements.

High-resolution tunnelling spectroscopy of a graphene quartet

Electrons in a single sheet of graphene behave quite differently from those in traditional two-dimensional electron systems. Like massless relativistic particles, they have linear dispersion and chiral eigenstates. Furthermore, two sets of electrons centred at different points in reciprocal space (‘valleys’) have this dispersion, giving rise to valley degeneracy. The symmetry between valleys, together with spin symmetry, leads to a fourfold quartet degeneracy of the Landau levels, observed as peaks in the density of states produced by an applied magnetic field. Recent electron transport measurements have observed the lifting of the fourfold degeneracy in very large applied magnetic fields, separating the quartet into integer and, more recently, fractional levels. The exact nature of the broken-symmetry states that form within the Landau levels and lift these degeneracies is unclear at present and is a topic of intense theoretical debate. Here we study the detailed features of the four quantum states that make up a degenerate graphene Landau level. We use high-resolution scanning tunnelling spectroscopy at temperatures as low as 10 mK in an applied magnetic field to study the top layer of multilayer epitaxial graphene. When the Fermi level lies inside the fourfold Landau manifold, significant electron correlation effects result in an enhanced valley splitting for even filling factors, and an enhanced electron spin splitting for odd filling factors. Most unexpectedly, we observe states with Landau level filling factors of 7/2, 9/2 and 11/2, suggestive of new many-body states in graphene.

Field ion-scanning tunneling microscopy study of C60 on the Si(100) surface

Field ion-scanning tunneling microscopy was employed to study the monolayer and multilayer adsorption behaviors of the C60 fullerene on the Si(100)2×1 surface. The C60 molecules reside stably in the trough at room temperature without rotation, encompassing the 8 neighbouring dimer-forming surface Si atoms with the nearest neighbour distance of 12 A. For the first and second layers, only local ordering of square and quasi-hexagonal patterns was observed. The orderly Stranski-Krastanov mode island formation with the hexagonal packing was observed above the third layer with its lattice constant of 10.4 A.

Real-time evolution of trapped charge in a SiO2 layer: An electrostatic force microscopy study

Time-dependent motion of localized electrons and holes trapped in a SiO2 layer is visualized with electrostatic force microscopy. Both negative and positive charges of up to ∼1010 e/cm2 are trapped at a SiO2–Si interface in ∼500-nm-diam area with a voltage stress between the tip and the sample. There is a higher probability for trapped charges to spread out in the plane direction than to de-trap toward the Si substrate. The dynamics is explained with diffusion and drift of the charges induced by Coulombic interaction.

Invited Review Article: A 10 mK scanning probe microscopy facility

We describe the design, development and performance of a scanning probe microscopy (SPM) facility operating at a base temperature of 10 mK in magnetic fields up to 15 T. The microscope is cooled by a custom designed, fully ultra-high vacuum (UHV) compatible dilution refrigerator (DR) and is capable of in situ tip and sample exchange. Subpicometer stability at the tip-sample junction is achieved through three independent vibration isolation stages and careful design of the dilution refrigerator. The system can be connected to, or disconnected from, a network of interconnected auxiliary UHV chambers, which include growth chambers for metal and semiconductor samples, a field-ion microscope for tip characterization, and a fully independent additional quick access low temperature scanning tunneling microscope (STM) and atomic force microscope (AFM) system. To characterize the system, we present the cooling performance of the DR, vibrational, tunneling current, and tip-sample displacement noise measurements. In addition, we show the spectral resolution capabilities with tunneling spectroscopy results obtained on an epitaxial graphene sample resolving the quantum Landau levels in a magnetic field, including the sublevels corresponding to the lifting of the electron spin and valley degeneracies.

Quantum Interference Channeling at Graphene Edges

Electron scattering at graphene edges is expected to make a crucial contribution to the electron transport in graphene nanodevices by producing quantum interferences. Atomic-scale scanning tunneling microscopy (STM) topographies of different edge structures of monolayer graphene show that the localization of the electronic density of states along the C-C bonds, a property unique to monolayer graphene, results in quantum interference patterns along the graphene carbon bond network, whose shapes depend only on the edge structure and not on the electron energy.

Charge trap dynamics in a SiO2 layer on Si by scanning capacitance microscopy

Trapped electrons and holes, and their dynamics, were visualized from spatially resolved capacitance–voltage (C–V) curves and dC/dV images using scanning capacitance microscopy. A trapped charge of 10−16–10−18 C, localized within 2 μm diam circular test structures, was imaged. The detrapping process of the trapped electrons can be explained with a quantum-mechanical tunneling model.