Optical characterization of ultrasmall Si nanoparticles prepared through electrochemical dispersion of bulk Si

Studying the properties and stability of silicon nanoparticles (Si-np) in aqueous environments may lead to novel applications in biological systems. In this work, we use absorption and photoluminescence (PL) spectroscopy to characterize ultrasmall Si-np prepared through anodic etching and ultrasonic fractionation of a crystalline Si wafer. Their behavior is studied over time in 2-propanol and during treatments with water, NaOH, HCl, and H(2)O(2). The observed population is divided into two types of material: bright species consisting of well-etched Si-np, approximately 1 nm in diameter, and dark species derived from partially etched or aggregated Si structures. The dark material is seen by its scattering in the 2-propanol and water solutions and is largely removed via precipitation with the NaOH or HCl treatment. The bright material includes three distinct species with their respective emissions in the UV-B, UV-A, and hard-blue regions of the spectrum. The hard-blue PL is shown to have a simple pH dependence with a pK(a) approximately 3, providing an important insight into its chemical origin and signaling for possible application of Si-np as environmental probes. Our results offer some potential for tailoring the PL properties of ultrasmall Si-np through control of their surface chemistry.     

Direct imaging of Cu dimer formation, motion, and interaction with Cu atoms on Ag(111)

We have investigated the formation and motion of copper adatoms and addimers on Ag(111) between 6 and 25 K with low-temperature scanning tunneling microscopy. The presence of atoms and dimers alters the motion of atoms and dimers via the long-range interaction mediated by the electrons in the two-dimensional surface state band. Above 16 K, dimers show quantum rotor behavior with altered rotational behavior in the presence of an additional adatom. The most favorable diffusional motion of the dimer is identified in combination with molecular dynamics calculations to be a zigzag out-of-cell motion starting above 24 K.     

Controlled low-temperature molecular manipulation of sexiphenyl molecules on Ag111 using scanning tunneling microscopy

A novel scanning tunneling microscope manipulation scheme for a controlled molecular transport of weakly adsorbed molecules is demonstrated. Single sexiphenyl molecules adsorbed on a Ag(111) surface at 6 K are shot towards single silver atoms by excitation with the tip. To achieve atomically straight shooting paths, an electron resonator consisting of linear standing-wave fronts is constructed. The sexiphenyl manipulation signals reveal a pi ring flipping as the molecule moves from the hcp to fcc site. Ab initio calculations show an incorporation of the Ag atom below the center of a pi ring.     

Probing molecular free energy landscapes by periodic loading

Single molecule pulling experiments provide information about interactions in biomolecules that cannot be obtained by any other method. However, the reconstruction of the molecule's free energy profile from the experimental data is still a challenge, in particular, for the unstable barrier regions. We propose a new method for obtaining the full profile by introducing a periodic ramp and using Jarzynski's relation for obtaining equilibrium quantities from nonequilibrium data. Our simulated experiments show that this method delivers significant more accurate data than previous methods, under the constraint of equal experimental effort.     

Two-dimensional coarsening kinetics of reconstruction domains: GaAs(001)-beta(2 x 4)

We study the nonconserved coarsening kinetics of a reconstructed semiconductor surface. The domain size evolution is obtained in situ by time-resolved surface x-ray diffraction. The system exhibits four equivalent domain types with two nonequivalent types of domain boundaries. Small domains are prepared by molecular beam epitaxy deposition of one GaAs layer. We find the correlation lengths of the domain size distribution to depend on time as l is proportional to t(0.42+/-0.05) in the half-order reflections and l is proportional to t(0.22+/-0.05) in the quarter-order reflections. The fraction of the higher energy domain boundaries increases as lnt.     

Dissection of heteronuclear NMR experiments for studies of magnetization transfer efficiencies

Modern NMR experiments for applications with biological macromolecules in solution typically include multiple magnetization transfer steps. When working with large structures, a significant fraction of the magnetization is lost during these transfers. For the design and optimization of complex experimental schemes, the magnetization transfer efficiencies have therefore commonly been calculated from the spin relaxation times. This paper now suggests a new method for measurement of individual transfer efficiencies directly with the system of interest, using short, reliable experiments. Initial applications of this approach with a 110,000 Da protein indicate that there is a wide range of transfer efficiencies among individual spin pairs in a structure of this size, which leads to a correspondingly large variation of the individual signal intensities and the need for techniques to enhance the weak signals.     

Fast voltage transients in capacitive silicon-to-cell stimulation detected with a luminescent molecular electronic probe

The capacitive stimulation of nerve cells from semiconductor chips is a prerequisite for the development of neuroelectronic devices. We report on the primary response of a cell membrane to a voltage step applied to oxidized silicon. It is observed with a luminescent voltage-sensitive dye. We find exponential voltage transients with a time constant of 1-5 micros. We assign the short response to an electrical decoupling by a thin film of electrolyte between oxide and membrane. The high-pass filtering of stimulation is a crucial constraint for the development of silicon-to-neuron interfaces.     

Homoclinic bifurcation in a Hodgkin-Huxley model of thermally sensitive neurons

We study global bifurcations of the chaotic attractor in a modified Hodgkin-Huxley model of thermally sensitive neurons. The control parameter for this model is the temperature. The chaotic behavior is realized over a wide range of temperatures and is visualized using interspike intervals. We observe an abrupt increase of the interspike intervals in a certain temperature region. We identify this as a homoclinic bifurcation of a saddle-focus fixed point which is embedded in the chaotic attractors. The transition is accompanied by intermittency, which obeys a universal scaling law for the average length of trajectory segments exhibiting only short interspike intervals with the distance from the onset of intermittency. We also present experimental results of interspike interval measurements taken from the crayfish caudal photoreceptor, which qualitatively demonstrate the same bifurcation structure. (c) 2000 American Institute of Physics.     

QCD sum rules in exclusive kinematics and pion wave function

We suggest a modification of the QCD sum rules for three-point correlation functions that relates hadron expectation values of an operator of interest to properties of the QCD vacuum in alternating external fields. A new sum rule is obtained for the nucleon magnetic moments. Relations are found between the couplings g_πNN , g_ρωπ and the value of the pion wave function at the point with equal momentum carried by the quark and the antiquark. Our results seem to exclude the possibility of having a pronounced dip in the pion wave function in the middle point, as has been assumed on the evidence of a large value of the second moment.