Complete set of material properties of [011](c) poled 0.24Pb(In(1/2)Nb(1/2))O(3)-0.46Pb(Mg(1/3)Nb(2/3))O(3)-0.30PbTiO(3) single crystal

A complete set of elastic, piezoelectric, and dielectric constants of [011](c) poled multidomain 0.24Pb(In(1/2)Nb(1/2))O(3)-0.46Pb(Mg(1/3)Nb(2/3))O(3)-0.30PbTiO(3) ternary single crystal has been determined using resonance and ultrasonic methods and the temperature dependence of the dielectric permittivity has been measured at 3 different frequencies. The experimental results revealed that this [011](c) poled ternary single crystal has very large transverse piezoelectric coefficient d(32) = -1693 pC/N, transverse dielectric constant ε(11)/ε(0) ~ 7400 and a high electromechanical coupling factor k(32) ~ 90%. In addition, its coercive field is 2 times of that of the corresponding binary 0.7Pb(Mg(1/3)Nb(2/3))O(3)-0.30PbTiO(3) single system with much better temperature stability. Therefore, the crystal is an excellent candidate for transverse mode electromechanical devices.     

Electrical readouts of single and few molecule systems in metal-molecule-metal device structures

Electrical conduction through molecular junctions are measured in different local environments through two test beds that are ideal for single/few molecule and molecular monolayer systems. A technique has been developed to realize Au films with approximately 1.5 A surface roughness comparable to the best available techniques and suitable for formation of patterned device structures. The technique utilizes room temperature e-beam evaporated Au films over oxidized Si substrates silanized with (3-mercaptopropyl)trimethoxysilane (MPTMS). The lateral (single/few molecule) and vertical (many molecules) device structures are both enabled by the process for realizing ultraflat Au layer. Lateral metal-molecule-metal (M-M-M) device structures are fabricated by forming pairs of Au electrodes with nanometer separation (nano-gap) through an electromigration-induced break-junction (EIBJ) technique at room temperature and conductivity measurements are carried out for dithiol functionalized single molecules. We have used the flat Au layer (using the current technique) as the bottom contact in vertical M-M-M device structures. Here, molecular self-assembly are formed on the Au surface, and patterned (20 x 20 microm2) top Au contacts were successfully transferred on to the device using a stamping technique (where the Au is deposited on a polydimethylsiloxane (PDMS) pad and following a physical contact on the thiolated Au layer). The single molecular property of XYL, a highly conductive molecule and many molecular property of HS-C9-SH, an insulating molecule in its molecular monolayer form are measured. Observation of enhanced conduction following molecular deposition, and comparison of conductance-voltage characteristics to those predicted theoretically, confirms the success of trapping single/few molecules in the nano-gap. The observed approximately 10(2) less conductance through the molecular monolayer of HS-C9-SH compared to the estimation of a linear sum of single molecule conductances over large area indicate that either all the molecules are not in physical contact with the top stamping electrode or electrode-molecule coupling has a less broadening in presence of it own environment or both.     

Single molecule microscopy: peak-frequency trajectories and linewidth distribution

Fluorescence microscopy has been adapted to cryogenic temperatures and combined with efficient image processing and analysis to observe many single molecules in parallel. The capabilities of this setup are demonstrated with the parallel recording of peak-frequency trajectories for 62 terrylene-molecules in n-hexadecane and with the measurement of 918 single molecule linewidths for terrylene in dodecane in 200 s.     

Tunable luminescence and energy transfer properties of Sr₃AlO₄F:RE³+ (RE = Tm/Tb, Eu, Ce) phosphors

Sr(3)AlO(4)F:RE(3+) (RE = Tm/Tb, Eu, Ce) phosphors were prepared by the conventional solid-state reaction. X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), photoluminescence (PL) spectra, as well as lifetimes were utilized to characterize samples. Under the excitation of UV light, Sr(3)AlO(4)F:Tm(3+), Sr(3)AlO(4)F:Tb(3+), and Sr(3)AlO(4)F:Eu(3+) exhibit the characteristic emissions of Tm(3+) ((1)D(2)→(3)F(4), blue), Tb(3+) ((5)D(4)→(7)F(5), green), and Eu(3+) ((5)D(0)→(7)F(2), red), respectively. By adjusting the doping concentration of Eu(3+) ions in Sr(3)AlO(4)F:0.10Tm(3+), 0.10Tb(3+), zEu(3+), a white emission in a single composition was obtained under the excitation of 360 nm, in which an energy transfer from Tb(3+) to Eu(3+) was observed. For Sr(3)AlO(4)F:Ce(3+),Tb(3+) samples, the energy transfer from Ce(3+) to Tb(3+) is efficient and demonstrated to be a resonant type via a dipole-quadrupole interaction by comparing the experimental data and theoretical calculation. Furthermore, the critical distance of the Ce(3+) and Tb(3+) ions has also been calculated to be 9.05 ?. The corresponding luminescence and energy transfer mechanisms have been proposed in detail. These phosphors might be promising for use in near-UV LEDs.     

Spatial periodicity in molecular switching

The ultimate miniaturization of future devices will require the use of functional molecules at the nanoscale and their integration into larger architectures. Switches represent a prototype of such functional molecules because they exhibit characteristic states of different physical/chemical properties, which can be addressed reversibly. Recently, various switching entities have been studied and switching of single molecules on surfaces has been demonstrated. However, for functional molecules to be used in a future device, it will be necessary to selectively address individual molecules, preferentially in an ordered pattern. Here, we show that azobenzene derivatives in the trans form, adsorbed in a homogeneous two-dimensional layer, can be collectively switched with spatial selectivity, thus forming a periodic pattern of cis isomers. We find that the probability of a molecule switching is not equally distributed, but is strongly dependent on both the surrounding molecules and the supporting surface, which precisely determine the switching capability of each individual molecule. Consequently, exactly the same lattices of cis isomers are created in repeated erasing and re-switching cycles. Our results demonstrate a conceptually new approach to spatially addressing single functional molecules.     

The "millipede" - nanotechnology entering data storage

Present a new scanning-probe-based data-storage concept called the "millipede" that combines ultrahigh density, terabit capacity, small form factor, and high data rate. Ultrahigh storage density has been demonstrated by a new thermomechanical local-probe technique to store, read back, and erase data in very thin polymer films. With this new technique, nanometer-sized bit indentations and pitch sizes have been made by a single cantilever/tip into thin polymer layers, resulting in a data storage densities of up to 1 Tb/in². High data rates are achieved by parallel operation of large two-dimensional (2-D) atomic force microscope (AFM) arrays that have been batch-fabricated by silicon surface-micromachining techniques. The very large-scale integration (VLSI) of micro/nanomechanical devices (cantilevers/tips) on a single chip leads to the largest and densest 2-D array of 32×32 (1024) AFM cantilevers with integrated write/read/erase storage functionality ever built. Time-multiplexed electronics control the functional storage cycles for parallel operation of the millipede array chip. Initial areal densities of 100-200 Gb/in² have been achieved with the 32×32 array chip     

Single molecule fluorescence burst detection of DNA fragments separated by capillary electrophoresis.

A method has been developed for detecting DNA separated by capillary gel electrophoresis (CGE) using single molecule photon burst counting. A confocal fluorescence microscope was used to observe the fluorescence bursts from single molecules of DNA multiply labeled with the thiazole orange derivative T06 as they passed through the approximately 2 micrometer diameter focused laser beam. Amplified photoelectron pulses from the photomultiplier are grouped into bins of 360-450 micros in duration, and the resulting histogram is stored in a computer for analysis. Solutions of M13 DNA were first flowed through the capillary at various concentrations, and the resulting data were used to optimize the parameters for digital filtering using a low-pass Fourier filter, selecting a discriminator level for peak detection, and applying a peak-calling algorithm. Statistical analyses showed that (i) the number of M13 molecules counted versus concentration was linear with slope = 1, (ii) the average burst duration was consistent with the expected transit time of a single molecule through the laser beam, and (iii) the number of detected molecules was consistent with single molecule detection. The optimized single molecule counting method was then applied to an electrophoretic separation of M13 DNA and to a separation of pBR 322 DNA from pRL 277 DNA. Clusters of discreet fluorescence bursts were observed at the expected appearance time of each DNA band. The autocorrelation function of these data indicated transit times that were consistent with the observed electrophoretic velocity. These separations were easily detected when only 50-100 molecules of DNA per band traveled through the detection region. This new detection technology should lead to the routine analysis of DNA in capillary columns with an on-column sensitivity of approximately 100 DNA molecules/band or better.     

Charge-coupled device operated in a time-delayed integration mode as an approach to high-throughput flow-based single molecule analysis

Single molecule detection (SMD) readouts are particularly attractive for assays geared toward high-throughput processing, because they can potentially reduce assay time by eliminating various processing steps. Unfortunately, most flow-based SMD experiments have generated low throughputs due primarily to the fact that they are configured in single assay formats. The use of a charge-coupled device (CCD) with flow-based SMD can image multiple single molecule assays simultaneously to realize high-throughput processing capabilities. We present, for the first time, the ability to simultaneously track and detect single molecules in multiple microfluidic channels by employing a CCD camera operated in time-delayed integration (TDI) mode as a means for increasing the throughput of any single molecule measurement. As an example of the technology, we have configured a CCD to operate in a TDI mode to detect single double-stranded DNA molecules (lambda and pBR322) labeled with an intercalating dye (TOTO-3) in a series of microfluidic channels poised on a poly(methyl methacrylate), PMMA, chip. A laser beam was launched into the side of the chip, which irradiated a series of fluidic channels (eight) with the resulting fluorescence imaged onto a CCD. Using this system, we were able to identify single DNA molecules based on the fluorescence burst intensity arising from differences in the extent of dye labeling associated with the DNA molecule length. The CCD/TDI approach allowed increasing sample throughput by a factor of 8 compared to a single-assay SMD experiment. A sampling throughput of 276 molecules s (-1) per channel and 2208 molecules s (-1) for an eight channel microfluidic system was demonstrated. Operated in its full capacity, this multichannel format was projected to yield a sample throughput of 1.7 x 10 (7) molecules s (-1), which represents a 170-fold improvement over previously reported single molecule sampling rates.     

Fragmentation of a valine molecule by electron impact

The formation of ion products of single and dissociative ionization of a valine molecule (C₅H₁₁NO₂) by high-energy (11.5 MeV) and low-energy (below 150 eV) electrons has been investigated by mass spectrometry. Mass spectra of this molecule and near-threshold functions of yield of its ion fragments, for which the magnitudes of occurrence energies are determined, have been obtained. The analysis of the changes in mass spectra of valine molecules irradiated with doses of 5 and 20 kGy in comparison with those for unirradiated molecules shows that high-energy irradiation changes irreversibly the structure of some of the initial molecules.     

Facile sonochemical synthesis of CePO(4):Tb/LaPO(4) core/shell nanorods with highly improved photoluminescent properties

A simple, efficient and quick method has been established for the synthesis of CePO(4):Tb nanorods and CePO(4):Tb/LaPO(4) core/shell nanorods via ultrasound irradiation of inorganic salt aqueous solution under ambient conditions for 2?h. The as-prepared products were characterized by means of powder x-ray diffraction (PXRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), x-ray photoelectron spectroscopy (XPS), photoluminescence (PL) spectra and lifetimes. TEM micrographs show that all of the as-prepared cerium phosphate products have rod-like shape, and have a relatively high degree of crystallinity and uniformity. HRTEM micrographs and SAED results prove that these nanorods are single crystalline in nature. The emission intensity and lifetime of the CePO(4):Tb/LaPO(4) core/shell nanorods increased significantly with respect to those of CePO(4):Tb core nanorods under the same conditions. A substantial reduction in reaction time as well as reaction temperature is observed compared with the hydrothermal process.     

Thermoluminescence response of K2YF5:Tb3+ crystals to photon radiation fields

This investigation has been performed to test the feasibility of using K2YF5:Tb3+ crystals as thermoluminescence dosemeters (TLD). K2YF5 single crystals doped with 0.2, 10.0 and 50.0 at.% of trivalent optically active Tb3+ ions as well as K2TbF5 and undoped K2YF5 crystals have been synthesized under hydrothermal conditions. Polished crystal platelets with thickness of about 1 mm have been irradiated with X and gamma rays in order to study thermoluminescent (TL) sensitivity as well as dose and energy response in terms of the Tb3+ concentration in K2YF5. Within this concentration series, K2YF5 crystals doped with 10.0 at.% Tb3+ have been found to have maximum TL response due to a broad asymmetric TL glow peak at 269 degrees C with good linearity of dose response and reproducibility of dose measurements. After deconvolution, the main dosimetric peak has been revealed to be composed of two individual peaks, both with linear TL response behaviour, centered at 210 and 269 degrees C. As it has been proved, the linear TL signal coefficient for K2Y0.9Tb0.1F5 is almost 10 times greater than that for commercial TLD-100 (LiF:Mg,Ti), irradiated with a 137Cs gamma radiation source at the same conditions. The reported results indicate that K2YF5 crystals doped with Tb3+ have potential as promising materials for radiation dosemeters.     

Intensity dependence of nonsequential double ionization of aligned asymmetric molecules

The electron correlation in nonsequential double ionization (NSDI) from aligned HeH⁺ molecules by intense laser pulses at various intensities has been investigated with the three-dimensional classical ensemble model. The results show that the correlated emission from NSDI for the parallel alignment is asymmetric. By back analysis the contribution of Coulomb focusing from H⁺ to this asymmetry has been also demonstrated besides the permanent dipole moment of the HeH²⁺ molecule. Moreover, the asymmetry of correlated emissions enhances sharply with decreasing laser intensity. This is attributed to the intensity dependence of the effects of the permanent dipole moment of the HeH²⁺ molecule and Coulomb focusing from H⁺ on the recollision dynamics. Besides the two electrons involved in NSDI of HeH⁺, molecules aligned parallel to the laser polarization are more likely to exit the molecule into the opposite hemispheres compared with the perpendicular alignment at some laser intensities, which is different from the case of symmetric molecules.     

A microfluidic system for large DNA molecule arrays

Single molecule approaches offer the promise of large, exquisitely miniature ensembles for the generation of equally large data sets. Although microfluidic devices have previously been designed to manipulate single DNA molecules, many of the functionalities they embody are not applicable to very large DNA molecules, normally extracted from cells. Importantly, such microfluidic devices must work within an integrated system to enable high-throughput biological or biochemical analysis-a key measure of any device aimed at the chemical/biological interface and required if large data sets are to be created for subsequent analysis. The challenge here was to design an integrated microfluidic device to control the deposition or elongation of large DNA molecules (up to millimeters in length), which would serve as a general platform for biological/biochemical analysis to function within an integrated system that included massively parallel data collection and analysis. The approach we took was to use replica molding to construct silastic devices to consistently deposit oriented, elongated DNA molecules onto charged surfaces, creating massive single molecule arrays, which we analyzed for both physical and biochemical insights within an integrated environment that created large data sets. The overall efficacy of this approach was demonstrated by the restriction enzyme mapping and identification of single human genomic DNA molecules.     

Biofunctionalization of CeF(3):Tb(3+) nanoparticles

CeF(3):Tb(3+) nanoparticles (short pillar-like morphology with an average length and width of 11 and 5?nm, respectively) were successfully prepared by a polyol process using diethyleneglycol (DEG) as solvent. After being functionalized with a SiO(2)-NH(2) layer, these CeF(3):Tb(3+) nanoparticles can be conjugated with biotin molecules (activated by thionyl chloride) and further with avidin. The as-formed CeF(3):Tb(3+) nanoparticles, CeF(3):Tb(3+) nanoparticles functionalized with amino groups, biotin conjugated amino-functionalized CeF(3):Tb(3+) nanoparticles and biotinylated CeF(3):Tb(3+) nanoparticles bonded with avidin were characterized by x-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier transform infrared (FT-IR), UV/vis absorption spectra and luminescence spectra, respectively. The biofunctionalization of the CeF(3):Tb(3+) nanoparticles has less effect on their luminescence properties, i.e. they still show strong green emission (from Tb(3+), with (5)D(4)-(7)F(5) at 543?nm as the most prominent group), indicative of the great potential for these CeF(3):Tb(3+) nanoparticles to be used as biological fluorescence probes.     

Molecule‐Driven Nanoenergy Generator

A large potential can be generated when one end of 1D and/or 2D semiconducting nanostructures such as zinc oxide (ZnO) and molybdenum disulfide is exposed to a wide spectrum of chemical molecules. A nanoenergy generator that comprises vertically aligned ZnO nanowires and poly(vinyl chloride‐co‐vinyl‐co‐2‐hydroxypropyl acrylate) is fabricated, and it can generate electricity from various molecules including gaseous species exhaled from human breath. The generated voltage, which depends sensitively on the molecular dipole moment of adsorbed chemical species and surface coverage, is significantly larger than the streaming or piezoelectric potentials and is powerful enough to directly drive a single carbon nanotube field‐effect transistor. It is demonstrated that the notion of voltage generation through molecule‐surface interactions bears general implications to other semiconducting materials, and has the advantages of simplicity, cost‐effectiveness, fast response to a wide range of molecules, and high power output, making our approach a promising tool for energy conversion and sensing applications.     

低电子浓度Ti-Nb-Zr合金组织及性能研究

研究了β稳定元素Nb和中性元素Zr对Ti-Nb-Zr合金的微观组织及力学性能的影响,结果显示：随着Nb和Zr含量增加,α"马氏体相和ω相两种典型亚稳相变均可被抑制,在较低电子浓度条件下获得单一β相组织,其临界电子浓度约为4.19,显著低于Ti-Nb二元合金的临界值(4.24);低电子浓度单一β相Ti-Nb-Zr合金的弹性模量较低,其强度与弹性模量比值较高,具有优于Ti-Nb二元合金的生物力学相容性。     

Polarization-dependent optical gain in crystal and glass composed of excited-state intramolecular proton transfer organic molecules

Amplified spontaneous emission (ASE) associated with excited-state intramolecular proton transfer (ESIPT) was investigated in a single crystal and a glass of acetic acid 2-{4-[2-(2-hydroxy-phenyl)-4,5-diphenyl-imidazole-1-yl]-phenyl}-ethyl ester molecules. The polarization-dependent ASE was analyzed in an effort to understand the structural evolution involved in the ESIPT photo-cycle. From the analysis of the degree of polarization in the glass sample, we observed that polarization memory has been partially lost due to the ESIPT process in the molecule. The single crystal exhibited much larger transient optical gain than the glass sample.     

Narrow-line waveguide terahertz time-domain spectroscopy of aspirin and aspirin precursors

Low frequency vibrational modes of pharmaceutical molecules are dependent on the molecule as a whole and can be used for identification purposes. However, conventional Fourier transform far-infrared spectroscopy (FT-IR) and terahertz time-domain spectroscopy (THz-TDS) often result in broad, overlapping features that are difficult to distinguish. The technique of waveguide THz-TDS has been recently developed, resulting in sharper spectral features. Waveguide THz-TDS consists of forming an ordered polycrystalline film on a metal plate and incorporating that plate in a parallel-plate waveguide, where the film is probed by THz radiation. The planar order of the film on the metal surface strongly reduces the inhomogeneous broadening, while cooling the waveguide to 77 K reduces the homogeneous broadening. This combination results in sharper absorption lines associated with the vibrational modes of the molecule. Here, this technique has been demonstrated with aspirin and its precursors, benzoic acid and salicylic acid, as well as the salicylic acid isomers 3- and 4-hydroxybenzoic acid. Linewidths as narrow as 20 GHz have been observed, rivaling single crystal measurements.     

Hierarchical Bi2S3 nanoflowers: A novel photocatalyst for enhanced photocatalytic degradation of binary mixture of Rhodamine B and Methylene blue dyes and degradation of mixture of p-nitrophenol and p-chlorophenol

Hierarchical nanostructures of bismuth sulfide (Bi₂S₃) have been synthesized by a facile hydrothermal method. The potentiality of Bi₂S₃ hierarchical nanostructures for the photocatalytic degradation of Rhodamine B (RhB), Methylene blue (MB) and the mixture of RhB-MB organic dyes have been demonstrated and compared with commercial TiO₂ (Degussa P25) sample under visible light illumination. The degradation efficiency of Bi₂S₃ and Degussa P25 is found to be higher in the single as well as in the binary dye solution for MB degradation as compared to RhB degradation. Furthermore, the degradation rate of RhB and MB is enhanced by ～8 times and ～3 times in their binary solution as compared to that in single dye solution. Whereas, Bi₂S₃ has demonstrated ～14 times higher degradation rate of both RhB and MB in their binary solution than that of Degussa P25 for RhB and MB degradation in the binary solution under visible light exposure, respectively. Interestingly, Bi₂S₃ nanostructures has exhibited larger improvement in the degradation efficiency for RhB in its binary solution which is attributed to the faster separation of photogenerated charge carriers due to the proper alignments between the molecular orbits of dyes and band level positions of Bi₂S₃ in RhB-MB-Bi₂S₃ heterogenous system. The photocatalytic degradation study of colourless contaminants, p-chlorophenol (CP), p-nitrophenol (NP) and their mixture (CP-NP) is also investigated in the presence of Bi₂S₃ nanoflowers. Among the phenolic compounds, the degradation rate of NP is observed to be highest in the single solution. However, the degradation rate of both CP and NP is found to decrease in binary mixture solution in comparison to their individual solution. A possible mechanism for the enhanced photodegradation of RhB-MB dye mixture based on the active species trapping experiment has been proposed.     

Electron-impact-induced fragmentation of proline molecule

The formation of ionized products upon single and dissociative ionization of proline (C₅H₉NO₂) molecule by electron impact at high (11.5 MeV) and low (below 150 eV) energies has been studied using mass-spectrometric techniques. The mass-spectra of proline molecule have been obtained and interpreted and the near-threshold fragment ion yields have been measured, from which the absolute values of ionization energies of the initial molecule and the appearance potentials of its main fragment ions are determined. Analysis of the influence of exposure to a high-energy beam of accelerated electrons on the resulting mass spectra of initial molecules showed that high-energy irradiation produces irreversible changes in the initial molecular structure.