C. C. Ahn

Hydrogen adsorption and cohesive energy of single-walled carbon nanotubes

Hydrogen adsorption on crystalline ropes of carbon single-walled nanotubes (SWNT) was found to exceed 8 wt.%, which is the highest capacity of any carbon material. Hydrogen is first adsorbed on the outer surfaces of the crystalline ropes. At pressures higher than about 40 bar at 80 K, however, a phase transition occurs where there is a separation of the individual SWNTs, and hydrogen is physisorbed on their exposed surfaces. The pressure of this phase transition provides a tube-tube cohesive energy for much of the material of 5 meV/C atom. This small cohesive energy is affected strongly by the quality of crystalline order in the ropes.

Highly Reversible Lithium Storage in Nanostructured Silicon

Anode materials of nanostructured silicon have been prepared by physical vapor deposition and characterized using electrochemical methods. The electrodes were prepared in thin-film form as nanocrystalline particles (12 nm mean diameter) and as continuous amorphous thin films (100 nm thick). The nanocrystalline silicon exhibited specific capacities of around 1100 mAh/g with a 50% capacity retention after 50 cycles. The amorphous thin-film electrodes exhibited initial capacities of 3500 mAh/g with a stable capacity of 2000 mAh/g over 50 cycles. We suggest that the nanoscale dimensions of the silicon circumvents conventional mechanisms of mechanical deterioration, permitting good cycle life.

Nanocrystalline and thin film germanium electrodes with high lithium capacity and high rate capabilities

Germanium nanocrystals (12 nm mean diam) and amorphous thin films (60-250 nm thick) were prepared as anodes for lithium secondary cells. Amorphous thin film electrodes prepared on planar nickel substrates showed stable capacities of 1700 mAh/g over 60 cycles. Germanium nanocrystals showed reversible gravimetric capacities of up to 1400 mAh/g with 60% capacity retention after 50 cycles. Both electrodes were found to be crystalline in the fully lithiated state. The enhanced capacity, rate capability (1000C), and cycle life of nanophase germanium over bulk crystalline germanium is attributed to the high surface area and short diffusion lengths of the active material and the absence of defects in nanophase materials.

Irreversible Capacities of Graphite in Low‐Temperature Electrolytes for Lithium‐Ion Batteries

Carbonaceous anode materials in lithium-ion rechargeable cells exhibit irreversible capacity, mainly due to reaction of lithium during the formation of passive surface films. The stability and kinetics of lithium intercalation into the carbon anodes are determined by these films. The nature, thickness, and morphology of these films are in turn affected by the electrolyte components, primarily the solvent constituents. In this work, the films formed on graphite anodes in low-temperature electrolytes, i.e., solutions with different mixtures of alkyl carbonates and low-viscosity solvent additives, are examined using electrochemical impedance spectroscopy (EIS) and solid-state ^(7)Li nuclear magnetic resonance techniques. In addition, other ex situ studies such as X-ray diffraction, transmission electron microscopy, and electron energy loss spectroscopy were carried out on the graphite anodes to understand their microstructures.

Measurements of 3d state occupancy in transition metals using electron energy loss spectrometry

We report a linear correlation between the total intensities of the L2,3 white lines in electron energy loss spectra and the number of unoccupied 3d states in 3d transition metals. We show that this correlation can be used to obtain quantitative information about electronic changes during alloying and during solid‐state phase transformations.

Electron energy-loss spectrometry on lithiated graphite

Transmission electron energy-loss spectrometry was used to investigate the electronic states of metallic Li and LiC6, which is the Li-intercalated graphite used in Li-ion batteries. The Li K edges of metallic Li and LiC6 were nearly identical, and the C K edges were only weakly affected by the presence of Li. These results suggest only a small charge transfer from Li to C in LiC6, contrary to prior results from surface spectra obtained by x-ray photoelectron spectroscopy. Effects of radiation damage and sample oxidation in the transmission electron microscopy are also reported.

Ge layer transfer to Si for photovoltaic applications

Abstract We have successfully used hydrophobic direct-wafer bonding, along with H-induced layer splitting of Ge, to transfer 700-nm-thick, single-crystal Ge (100) films to Si (100) substrates without using a metallic bonding layer. The metal-free nature of the bond makes the bonded wafers suitable for subsequent epitaxial growth of triple-junction GaInP/GaAs/Ge solar cell structures at high temperatures, without concern about metal contamination of the active region of the device. Contact-mode atomic force microscopy images of the transferred Ge surface generated by hydrogen-induced layer-splitting reveals root mean square (rms) surface roughness of between 10 and 23 nm. Electrical measurements indicate ohmic I – V characteristics for as-bonded Ge layers bonded to silicon substrates with ∼400 Ω cm −2 resistance at the interface. Triple-junction solar cell structures grown on these Ge/Si heterostructure templates by metal–organic chemical vapor deposition show comparable photoluminescence intensity and minority carrier lifetime to a control structure grown on bulk Ge. An epitaxial Ge buffer layer is grown to smooth the cleaved surface of the Ge heterostructure and reduces the rms surface roughness from ∼11 to as low as 1.5 nm, with a mesa-like morphology that has a top surface roughness of under 1.0 nm, providing a promising surface for improved GaAs growth.

Hydrogen adsorption and phase transitions in fullerite

Hydrogen desorption and adsorption properties of the fullerene materials C60, C70, and fullerite (a mixture of C60 and C70) were measured volumetrically using a Sieverts apparatus. Over several cycles of isotherm measurements at 77 K, the hydrogen storage capacities of one of the fullerite samples increased from an initial value of 0.4 wt % for the first cycle to a capacity of 4.4 wt % for the fourth cycle. Correspondingly, the surface area of this sample increased from 0.9 to 11 m^2/g, and there were changes in its x-ray powder diffraction pattern. In comparison, two other fullerite samples, prepared by a different procedure showed no such behavior. Pure C60 and pure C70 were also cycled and exhibited small and constant capacities of 0.7 and 0.33 wt %, respectively, as a function of number of cycles. The enhanced storage capacity of fullerite material is tentatively attributed to the presence of C60 oxide.

Wafer bonding and layer transfer processes for 4-junction high efficiency solar cells

A four-junction cell design consisting of InGaAs, InGaAsP, GaAs, and Ga/sub 0.5/In/sub 0.5/P subcells could reach 1/spl times/AM0 efficiencies of 35.4%, but relies on the integration of non-lattice-matched materials. Wafer bonding and layer transfer processes show promise in the fabrication of InP/Si epitaxial templates for growth of the bottom InGaAs and InGaAsP subcells on a Si support substrate. Subsequent wafer bonding and layer transfer of a thin Ge layer onto the lower subcell stack can serve as an epitaxial template for GaAs and Ga/sub 0.5/In/sub 0.5/P subcells. Present results indicate that optically active III/V compound semiconductors can be grown on both Ge/Si and InP/Si heterostructures. Current voltage electrical characterization of the interfaces of these structures indicates that both InP/Si and Ge/Si interfaces have specific resistances lower than 0.1 /spl Omega/ cm/sup 2/ for heavily doped wafer bonded interfaces, enabling back surface power extraction from the finished cell structure.

Band offsets in Si/Si1–x–yGexCy heterojunctions measured by admittance spectroscopy

We have used admittance spectroscopy to measure conduction-band and valence-band offsets in Si/Si1–xGex and Si/Si1–x–yGexCy heterostructures grown by solid-source molecular-beam epitaxy. Valence-band offsets measured for Si/Si1–xGex heterojunctions were in excellent agreement with previously reported values. Incorporation of C into Si1–x–yGexCy lowers the valence- and conduction-band-edge energies compared to those in Si1–xGex with the same Ge concentration. Comparison of our measured band offsets with previously reported measurements of energy band gaps in Si1–x–yGexCy and Si1–yCy alloy layers indicate that the band alignment is Type I for the compositions we have studied and that our measured band offsets are in quantitative agreement with these previously reported results.