Si1-xGex anode synthesis on plastic films for flexible rechargeable batteries.

SiGe is a promising anode material for replacing graphite in next generation thin-film batteries owing to its high theoretical charge/discharge capacity. Metal-induced layer exchange (LE) is a unique technique used for the low-temperature synthesis of SiGe layers on arbitrary substrates. Here, we demonstrate the synthesis of Si1-xGex (x = 0-1) layers on plastic films using Al-induced LE. The resulting SiGe layers exhibited high electrical conductivity (up to 1200 S cm-1), reflecting the self-organized doping effect of LE. Moreover, the Si1-xGex layer synthesized by the same process was adopted as the anode for the lithium-ion battery. All Si1-xGex anodes showed clear charge/discharge operation and high coulombic efficiency (≥ 97%) after 100 cycles. While the discharge capacities almost reflected the theoretical values at each x at 0.1 C, the capacity degradation with increasing current rate strongly depended on x. Si-rich samples exhibited high initial capacity and low capacity retention, while Ge-rich samples showed contrasting characteristics. In particular, the Si1-xGex layers with x ≥ 0.8 showed excellent current rate performance owing to their high electrical conductivity and low volume expansion, maintaining a high capacity (> 500 mAh g-1) even at a high current rate (10 C). Thus, we revealed the relationship between SiGe composition and anode characteristics for the SiGe layers formed by LE at low temperatures. These results will pave the way for the next generation of flexible batteries based on SiGe anodes.

Grain size dependent photoresponsivity in GaAs films formed on glass with Ge seed layers.

The strong correlation between grain size and photoresponsivity in polycrystalline GaAs films on glass was experimentally demonstrated using Ge seed layers with a wide range of grain sizes (1‒330 µm). The crystal evaluations using Raman spectroscopy, scanning electron microscopy, electron backscatter diffraction, and transmission electron microscopy revealed that 500-nm-thick GaAs films epitaxially grown from the Ge seed layers at 550 °C inherited the grain boundaries and crystal orientations in Ge. With increasing grain size, the photoresponsivity corresponding to GaAs increased from 0.01 to 3 A W-1 under a bias voltage of 0.3 V. The maximum value approached that of the GaAs film formed simultaneously on a single-crystal Ge wafer, indicating the high potential of the large-grained GaAs film. Knowledge gained from this study will be essential for designing advanced solar cells based on polycrystalline III-V compound semiconductors using inexpensive substrates.

High-electron-mobility (370 cm2/Vs) polycrystalline Ge on an insulator formed by As-doped solid-phase crystallization.

High-electron-mobility polycrystalline Ge (poly-Ge) thin films are difficult to form because of their poor crystallinity, defect-induced acceptors and low solid solubility of n-type dopants. Here, we found that As doping into amorphous Ge significantly influenced the subsequent solid-phase crystallization. Although excessive As doping degraded the crystallinity of the poly-Ge, the appropriate amount of As (~1020 cm-3) promoted lateral growth and increased the Ge grain size to approximately 20 µm at a growth temperature of 375 °C. Moreover, neutral As atoms in poly-Ge reduced the trap-state density and energy barrier height of the grain boundaries. These properties reduced grain boundary scattering and allowed for an electron mobility of 370 cm2/Vs at an electron concentration of 5 × 1018 cm-3 after post annealing at 500 °C. The electron mobility further exceeds that of any other n-type poly-Ge layers and even that of single-crystal Si wafers with n ≥ 1018 cm-3. The low-temperature synthesis of high-mobility Ge on insulators will provide a pathway for the monolithic integration of high-performance Ge-CMOS onto Si-LSIs and flat-panel displays.

Fabrication of SrGe2 thin films on Ge (100), (110), and (111) substrates.

Semiconductor strontium digermanide (SrGe2) has a large absorption coefficient in the near-infrared light region and is expected to be useful for multijunction solar cells. This study firstly demonstrates the formation of SrGe2 thin films via a reactive deposition epitaxy on Ge substrates. The growth morphology of SrGe2 dramatically changed depending on the growth temperature (300-700 °C) and the crystal orientation of the Ge substrate. We succeeded in obtaining single-oriented SrGe2 using a Ge (110) substrate at 500 °C. Development on Si or glass substrates will lead to the application of SrGe2 to high-efficiency thin-film solar cells.

Early Gravi-Electrical Responses in Bean Epicotyls.

The relationship between gravitropism and surface electrical potentials was studied using etiolated epicotyls of adzuki bean (Phaseolus angularis). Early downward curvature (or transient positive gravitropic response) was observed about 1 min after gravistimulation. The downward curvature was closely related to the speed of the subsequent upward curvature. Surface electrical potentials decreased cooperatively in a limited region on the upper side within only 0.5 to 2 min. This is the earliest event found so far to follow gravistimulation of intact epicotyls. The rapid change in the potential had a high correlation with the early downward curvature and also the subsequent negative gravitropism. It is suggested that the rapid potential change plays an important role in gravity perception.

Electronic tongue.

A taste sensor with global selectivity is composed of several kinds of lipid/polymer membranes for transforming information of taste substances into an electric signal. The output of this electronic tongue shows different patterns for chemical substances which have different taste qualities, such as saltiness and sourness. Amino acids can be classified into several groups according to their own tastes from sensor outputs. The taste of foodstuffs such as beer, sake, coffee, mineral water, milk and vegetables can be discussed quantitatively using the electronic tongue, which provides the objective scale for the human sensory expression.

Multichannel taste sensor using electric potential changes in lipid membranes.

A taste sensor with a multichannel electrode was developed by using lipid membranes as a transducer of taste substances. The sensor can detect the taste in a similar manner to the human gustatory sensation by response patterns of electric potential to taste substances. The sensitivity, reproducibility and durability were superior to those of humans. The same taste as that elicited by some commercial aqueous drink was reproduced by making aqueous solution mixed from four kinds of basic taste substances, the concentrations of which were determined so that the electric-potential pattern of this mixed solution could agree well with the pattern by the drink. Different brands of beer were easily distinguished by the electric-potential patterns.

Antitumor activity and low intestinal toxicity of S-1, a new formulation of oral tegafur, in experimental tumor models in rats.

S-1, a new oral antitumor agent, is composed of 1-(2-tetrahydrofuryl)-5-fluorouracil (Tegafur, FT), 5-chloro-2,4-dihydroxypyridine (CDHP) and potassium oxonate (Oxo) in a molar ratio of 1:0.4:1. FT which is a masked compound of 5-fluorouracil (5-FU) acts as an effector, while both CDHP and Oxo which do not have antitumor activity themselves act as modulators. In this study, the antitumor activity and intestinal toxicity of S-1 were investigated using experimental tumor models in rats, and compared with those of other oral fluoropyrimidines, namely 5-FU, FT, FCD (1 M FT/0.4 M CDHP) and UFT (combination of FT and uracil). In rats bearing subcutaneous Yoshida sarcoma, S-1 inhibited tumor growth at the lowest dose (ED50 value: S-1 5, UFT 22, FT 82, FCD 5, and 5-FU 19 mg/kg per day), and induced the least host body weight suppression, leading to the highest therapeutic index (TI) (S-1 4.5, UFT 1.4, FT 1.8, FCD 2.0, and 5-FU 1.4). S-1 also showed a higher therapeutic effect than UFT against AH-130 and Sato lung carcinoma. After administration of S-1 and UFT at equitoxic doses, S-1 showed a higher and more prolonged concentration of 5-FU than UFT both in plasma (AUC0-infinity: S-1 28 nmolh/ml, UFT 15 nmol.h/ml) and in tumor tissue (AUC0-infinity: S-1 95 nmolh/g tissue, UFT 52 nmolh/g tissue), leading to a higher 5-FU level incorporated into the RNA fraction (F-RNA level) in tumor tissue (AUC0-24: S-1 7.0 nmolh/mg RNA, UFT 4.3 nmolh/mg RNA) and 5-8% higher thymidylate synthase (TS) inhibition in tumor tissue at every time-point through 24 h. Compared with other oral fluoropyrimidines after administration of the maximal tolerable dose (MTD), S-1 caused the lowest rates of intestinal toxicities, such as diarrhea and occult blood in feces. S-1 also showed a higher antitumor effect on Yoshida sarcoma implanted intracolonically than UFT at an equitoxic dose (tumor weight: S-1 64 +/- 30 mg, UFT 133 +/- 52 mg; P < 0.05). These results suggest that CDHP, which is a potent inhibitor of 5-FU degradation, increases the antitumor activity of FT, and that Oxo, which is an inhibitor of 5-FU phosphorylation, locally protects the gastrointestinal tract from 5-FU-induced toxicity without decreasing the antitumor activity.

Theory of electric characteristics of the lipid/PVC/DOPP membrane and PVC/DOPP membrane in response to taste stimuli.

Electric characteristics of two kinds of membranes in response to NaCl and quinine were theoretically studied; one membrane composed of polyvinyl chloride (PVC) and dioctylphenylphosphonate (DOPP), and the other a lipid/PVC/DOPP membrane containing PVC, DOPP and a negatively charged lipid. We develop a theory by taking into account both the surface electric potential and the diffusion potential within the membrane and succeed in interpreting the observed data. On increasing the NaCl concentration, the lipid/PVC/DOPP membrane changes from weakly charged state to fully charged state by dissociation of H+ from the lipids. The hydrophobic interaction between quinine and the PVC/DOPP membrane was strong enough to overcome the electric repulsion.

Stabilization effect of protons and divalent cations on membrane structures of lipids.

Ordered-fluid phase transitions of methylphosphatidic and phosphatidic acid bilayers are discussed theoretically to explain comprehensively various observed data in the presence of Ca2+ or protons. It is shown that the observed data can be explained reasonably by taking account of the interaction among neighboring head-groups with the aid of Ca2+ or protons. As a result, a quantitative explanation is given for the dependence of the phase-transition temperature on pH as well as Ca2+ concentration with the coexistence of monovalent cations. The dependence of the cooperativity of the transition on pH and monovalent cation concentration is also well explained. It is also pointed out that in the ordered-fluid phase transitions, a hysteresis metastable state and phase separation can be expected to appear under some conditions.

Electric oscillation in an excitable model membrane impregnated with lipid analogues.

A model membrane constructed from a Millipore filter, whose pores were impregnated with dioleyl phosphate, exhibited an electric self-oscillation under nonequilibrium conditions. The membrane interposed between two solutions with the same KCl concentrations showed no temporal change in membrane potential. However, the potential became oscillatory on application of an electric current to the membrane. The frequency was proportional to the magnitude of the electric current. When both KCl solutions were replaced by NaCl solutions, a similar trend was observed, although the oscillation was not as regular as in the case of KCl. A membrane placed between equimolar solutions of KCl and NaCl, on the other hand, gave rise to an oscillation even without current application. When a membrane was placed between 5 mM KCl and 100 mM KCl, it was found that NaCl added to the 5 mM KCl side had a pronounced effect on the membrane with respect to the frequency response of the oscillation. These results indicate that the dioleyl phosphate membrane discriminates Na+ from K+.

Band structure of surface electric potential in growing roots.

For growing roots of azuki bean (Phaseolus chrysanthos), an electric potential is measured minutely along the surface of the root, together with the surface pH. It was found that the root begins to display a band-type pattern of potential with a spatial period of about 2 cm in a mature region as soon as it grows to about 10 cm in root length, while the surface potential shows only one convex peak around a position 5-20 mm behind a root tip and a succeeding concave peak around 20-35 mm, providing the length of root is shorter than about 10 cm. Since the surface potential takes a relatively positive value on average at the side of the root base compared with that in an elongation zone near the tip, electric current is supposed to flow into the elongation zone, accompanied by some local current loops in the mature region. The present band-type pattern observed first in multi-cell systems seems to be a kind of dissipative structure appearing far from equilibrium, and hence its relationship to growth is discussed.

Self-sustained oscillations of electric potential in a model membrane.

A model membrane constructed from a Millipore filter, whose pores are filled with dioleyl phosphate molecules, exhibits a self-oscillation of the electric potential with a period of about a few seconds in the presence of a salt-concentration difference, pressure difference and/or electric current across the filter. In this paper, the effects of chemicals such as KCl, CaCl2, pH and sucrose on the self-oscillation are investigated experimentally. These chemical substances are shown to alter the characteristic properties as the frequency of oscillation. Theoretical consideration of electrochemical interaction between these substances and DOPH molecules gives a fairly good explanation of the observed results.

Electric inhomogeneity in membranes of Characean internode influenced by light/dark transition, O2, N2, CO2-free air and extracellular pH.

The electric membrane potential as functions of position and time of Characean internode has been studied using a modified water-film electrode technique. Between the low-conductance hyperpolarized region (called the H-region or acidic region) and the high-conductance depolarized region (D-region), there is a difference in the direction of responses to light-off and -on stimulations. In darkness the membrane potential becomes hyperpolarized in the D-region, whereas it is depolarized in the H-region at the steady state. The potential difference between D- and H-regions, delta Vm, is increased by exposure to pure O2, N2, or CO2-free air. When the amount of water surrounding the internode is limited, the formation of an electric pattern occurs rapidly. In contrast, the recovery is delayed. The membrane potential of the D-region is sometimes hyperpolarized significantly with lowering of the extracellular pH to 7.5, while the potential of the H-region is slightly depolarized. This seems to be an all-or-none type response. However, the electric profile is always homogenized with the pH of 6.8. Thus, the pH around 7.5 may be a threshold level to open/close putative OH- (or H+) channels of the D-region.

Change in electric characteristics of membranes in response to taste stimuli with increasing amount of lipids in membrane matrix of PVC and plasticizer.

Changes in membrane electric potential in response to taste substances were studied for membranes containing differing amounts of negatively charged lipids in the membrane matrix of polyvinyl chloride and plasticizer. Responses to quinine showing bitterness decreased systematically with increasing the quantity of charged lipids contained in the membrane, whereas the response did not depend on differences in the hydrocarbon chains of lipids. The mechanism is discussed qualitatively in terms of hydrophobicity and hydrophilicity of the membranes.

Current-voltage characteristics and self-sustained oscillations in dioleyl phosphate-millipore membranes.

For an artificial membrane prepared by infiltrating dioleyl phosphate (DOPH) into pores of a Millipore filter, we propose a theoretical model for explaining observed data on electric behavior, such as d.c. current-voltage characteristics and self-sustained oscillations of the electric potential. The model consists of a simple electric circuit composed of electric resistances and capacitances as given functions of internal variables which represent conformational states of DOPH molecules and salt concentration inside the pore concerned. The kinetic equations for these variables are the same as those presented previously for describing a phase transition of DOPH. except for a slight modification taking account of effects of salt accumulation inside the pore. The present theory can describe well the I-V hysteresis and various features of spike-like oscillations with long periods of up to a few hours in the absence of external force and also short-period oscillations with periods of the order of 1 s under pressure difference.

Dynamic property of membrane formation in a protoplasmic droplet of Nitella.

A theory is presented to explain the dynamic characteristics of an electric potential and the resistance of a surface membrane during the formation of a protoplasmic droplet isolated from Nitella. Basic equations are coupled ones for describing ion concentrations near the surface of the droplet, active and passive ion fluxes on the surface, and kinetics of membrane-constituting molecules diffusing from the inside of the protoplasm. The present results give a good explanation of the observed kinetics of electric properties throughout the formative process of surface membranes after the ion concentrations are replaced by lower ones. The results can also explain well the observed data on the steady state. Oscillatory changes in the membrane potential induced by ions strongly adsorbed on the surface membrane are discussed in relation to growth and regeneration phenomena in biological systems such as bean roots and Acetabularia.

Theory of electric dissipative structure in Characean internode.

A band-type alternating pattern of acidic and alkaline regions formed along the Characean cell wall is discussed theoretically. The model system is constructed from linear diffusion equations for the concentration of H+ outside the internode and in the protoplasm. The plasmalemma is taken as a boundary transporting H+ under energy supply by light. The sizes of the protoplasm and extracellular water phase are taken into account explicitly in the present model system to reproduce qualitatively the characteristics observed in various types of experiments. Theoretical analysis shows that the band pattern belongs to dissipative structures emerging far from equilibrium, and is stabilized through the electric current loops produced by locally activated electrogenic H+ pumps and spatially separated passive H+ influx (or OH- efflux) across the membrane. Both the numerical calculation and the theoretical analysis using a generalized time-dependent Ginzburg-Landau equation reveal the following points: (i) the intemodal cell with a larger vacuole in a smaller size of the extracellular water phase tends to exhibit a clearer band pattern; (ii) the increase in viscosity of the external aqueous medium makes the bands appear more easily and, furthermore, distinctly; (iii) the change in size of the extracellular water phase significantly affects the kinetics of the pattern- formation process. These results are interpreted reasonably by taking account of the electric current circulating between the acidic and alkaline regions.

On the oscillatory phenomenon in an oil/water interface.

A simple theoretical model is presented for simulating the self-sustained oscillations of electric potential and pH at an oil/water interface appearing in a two-phase system composed of 2-nitropropane solution containing picrate acid and an aqueous solution of cetyltrimethylammonium bromide. In the present model, a well-known condition necessary for the occurrence of self-sustained oscillations, i.e., the presence of a positive feedback process far from equilibrium, is taken into account in a set of kinetic equations to describe simplified characters of the following two processes: (i) a cooperative formation of ion pair complexes at the interface, and (ii) supply of picrate anions and cetyltrimethylammonium cations to the interface accompanied by release of ion pair complexes to the organic phase. The numerical solutions of the present equations are shown to reproduce fairly well the characteristic properties of the oscillation of electric potential and pH such as wave forms and frequencies.

Electrical characteristics in an excitable element of lipid membrane.

Electrical characteristics in a membrane constructed from a porous filter adsorbed with a lipid analogue, dioleoyl phosphate (DOPH), were investigated in a situation interposed between 100 mM NaCl + 3 mM CaCl2 and 100 mM KCl. Calcium ions affected significantly the membrane characteristics. The membrane potential was negative on the KCl side, which implies the higher permeability to K+ than Na+; this tendency was increased by a tiny amount of Ca2+. While the membrane showed a low electrical resistance of several k omega . cm2 under K+/Na+ gradient, it showed several M omega . cm2 by Ca2+. The surface structure of the membrane exhibited many voids in the low-resistance state, but the surface was covered by oil droplets in the high-resistance state. Oscillations of the membrane potential appeared spontaneously with application of the electrical current from the KCl side to the NaCl + CaCl2 side. The frequency was increased with the electrical current. All these results were explained comprehensively using an electrochemical kinetic model taking account of the Ca2+ binding effect, where DOPH assemblies make a phase transition between oil droplets due to Ca2+ and multi-bilayers with excess K+. The oscillation arises from coupling of the phase transition to accumulation and release of K+ or Ca2+. This membrane can be used as an excitable element regulated by Ca2+ in neuro-computer devices.