Adsorbed and free lipid bilayers at the solid-liquid interface

Single and double phosphocholine (DPPC and DSPC) bilayers adsorbed at the silicon-water interface have been prepared and characterised. The second bilayer, called “free bilayer”, is a novel highly hydrated system floating at above the first one. Robust and reproducible preparation has been possible thanks to a combination of Langmuir-Blodgett and Langmuir-Schaeffer techniques. Carefully optimised neutron reflectivity measurements have allowed a precise non-destructive characterisation of the structure, hydration and roughness of the layers. This work opens new possibilities for the investigation of the interaction between membrane lipids and soluble proteins, in particular peptides too small to be visible with other techniques. Received 17 July 1998     

Water transbilayer diffusion in macroscopically oriented lipid bilayers as studied by pulsed field gradient NMR

Water self-diffusion in lipid bilayers macroscopically oriented on glass plates was studied by pulsed field gradient¹H nuclear magnetic resonance technique. Diffusion decays were multicomponent with a distribution of diffusion coefficients ranging from about 10⁻¹⁰ to about 10⁻¹³ m²/s. A number of measurements with variations of the sample orientation, diffusion time and the distance between the glass plates showed that the “fast” component of diffusion corresponds to water in the bilayer “cracks”. The “slow” component of diffusion corresponds to transbilayer water diffusion in the long-diffusion-time regime. For a more reliable separation of parts corresponding to fast and slow diffusion of water, a “component-resolved spectroscopy” method for the global analysis of correlated spectral data (P. Stilbs, K. Paulsen, P.C. Griffiths: J. Phys. Chem. 100, 8180, 1996) was applied.     

低温生长的Ge/Si超晶格界面结构的X射线散射研究

低温下用MBE方法生长了Ge/Si超晶格,X射线反射及横向散射研究表明,Ge亚层上下表面的粗糙度呈反对称,下表面大的粗糙度来源于Ge向Si亚层中扩散形成SiGe混合组分结构,这种组分结构可以用一平均成分的SiGe合金层加以拟合,从而使得各亚层均有一个合理的粗糙度,旋转样品进行的X射线散射研究表明,这种SiGe的混合是各向同性的,这与透射电子显微镜的研究结构相一致.     

Thermal unbinding of highly oriented phospholipid membranes

We present a temperature dependent x-ray reflectivity study of highly oriented, fully hydrated multilamellar phospholipid membranes. Both the specular and diffuse (nonspecular) x-ray reflectivity were measured for dimyristoyl-sn-glycero-phosphocholine (DMPC) and oleoyl-palmitoyl-sn-glycero-phosphocholine (POPC) on silicon substrates in excess water. In this configuration the repeat distance as well as the fluctuation spectra can be determined as a function of temperature. Both model systems studied exhibit a discontinuous unbinding transition from a substrate bound, multilamellar state to a state of freely dispersed bilayers in water. In the unbound phase a single membrane remains on the substrate.     

Detecting hidden spatial and spatio-temporal structures in glasses and complex physical systems by multiresolution network clustering

We elaborate on a general method that we recently introduced for characterizing the “natural” structures in complex physical systems via multi-scale network analysis. The method is based on “community detection” wherein interacting particles are partitioned into an “ideal gas” of optimally decoupled groups of particles. Specifically, we construct a set of network representations (“replicas”) of the physical system based on interatomic potentials and apply a multiscale clustering (“multiresolution community detection”) analysis using information-based correlations among the replicas. Replicas may i) be different representations of an identical static system, ii) embody dynamics by considering replicas to be time separated snapshots of the system (with a tunable time separation), or iii) encode general correlations when different replicas correspond to different representations of the entire history of the system as it evolves in space-time. Inputs for our method are the inter-particle potentials or experimentally measured two (or higher order) particle correlations. We apply our method to computer simulations of a binary Kob-Andersen Lennard-Jones system in a mixture ratio of A₈₀B₂₀ , a ternary model system with components “A”, “B”, and “C” in ratios of A₈₈B₇C₅ (as in Al₈₈Y₇Fe₅ , and to atomic coordinates in a Zr₈₀Pt₂₀ system as gleaned by reverse Monte Carlo analysis of experimentally determined structure factors. We identify the dominant structures (disjoint or overlapping) and general length scales by analyzing extrema of the information theory measures. We speculate on possible links between i) physical transitions or crossovers and ii) changes in structures found by this method as well as phase transitions associated with the computational complexity of the community detection problem. We also briefly consider continuum approaches and discuss rigidity and the shear penetration depth in amorphous systems; this latter length scale increases as the system becomes progressively rigid.     

Magnetization Reversal Studies of Magnetic Wire Arrays by Polarized Neutron Scattering

Polarized neutron reflectivity has been used to investigate the peak pattern and the magnetization reversal process of laterally structured Fe- and CoFe-films. The peak pattern of the wire arrays was analyzed in the specular as well as in the off-specular regime. The intensities of the different cross-sections at the off-specular first-order peak were investigated as a function of external magnetic field. Magnetization reversals are discussed and compared to MOKE studies of the same system.     

Solvent Relaxation in Phospholipid Bilayers: Principles and Recent Applications

Although there exist a number of methods, such as NMR, X-ray, e.g., which explore the hydration of phospholipid bilayers, the solvent relaxation (SR) method has the advantage of simple instrumentation, easy data treatment and possibility of measuring fully hydrated samples. The main information gained from SR by the analysis of recorded “time-resolved emission spectra” (TRES) is micro-viscosity and micro-polarity of the dye microenvironment. Based on these parameters, one can draw conclusions about water structure in the bilayer. In this review, we focus on physical background of this method, on all the procedures that are needed in order to obtain relevant parameters, and on the requirements on the fluorescence dyes. Furthermore, a few recent applications (the effect of curvature, binding of antibacterial peptides and phase transition) illustrating the versatility of this method are mentioned. Moreover, limitations and potential problems are discussed.     

Hysteresis Phenomenon in Deterministic Traffic Flows

We study phase transitions of a system of particles on the one-dimensional integer lattice moving with constant acceleration, with a collision law respecting slower particles. This simple deterministic “particle-hopping” traffic flow model being a straightforward generalization to the well known Nagel–Schreckenberg model covers also a more recent slow-to-start model as a special case. The model has two distinct ergodic (unmixed) phases with two critical values. When traffic density is below the lowest critical value, the steady state of the model corresponds to the “free-flowing” (or “gaseous”) phase. When the density exceeds the second critical value the model produces large, persistent, well-defined traffic jams, which correspond to the “jammed” (or “liquid”) phase. Between the two critical values each of these phases may take place, which can be interpreted as an “overcooled gas” phase when a small perturbation can change drastically gas into liquid. Mathematical analysis is accomplished in part by the exact derivation of the life-time of individual traffic jams for a given configuration of particles. This research has been partially supported by Russian Foundation for Fundamental Research and French Ministry of Education grants.     

Implications of an extended fractal hydrodynamic model

Considering that the motions of the particles take place on continuous but non-differentiable curves, i.e. on fractals with constant fractal dimension, an extended scale relativity model in its hydrodynamic version is built. In this approach, static (particle in a box and harmonic oscillator) and time-dependent (free particle etc.) systems are analyzed. The static systems can be associated with a coherent fractal fluid (of superconductor or of super-fluid types behavior), whose particles are moving on stationary trajectories. The complex speed field of the fractal fluid proves to be essential: the zero value of the real (differentiable) part specifies the coherence of the fractal fluid, while the non-zero value of the imaginary (non-differentiable or fractal) part selects, through some “quantization” relations, the “stationary” trajectories (that may correspond to the observables from quantum mechanics) of the fractal fluid particles. Moreover, the momentum transfer in the fractal fluid is achieved only through the fractal component of the complex speed field. The free time-dependent systems can be associated with an incoherent fractal fluid, and both the differentiable and fractal components of complex speed field are inhomogeneous in fractal coordinates due to the action of a fractal potential. It exist momentum transfer on both speed components and the “observable” in the form of an uniform motion is generated through a specific mechanism of “vacuum” polarization induced by the same fractal potential. The analysis on the fractal fluid specifies conductive properties in the case of movements synchronization both on differentiable and fractal scales, and convective properties in the absence of synchronization.     

Statistical approach to finite systems of interacting particles based on the structure of haotic eigenstates

A novel approach to finite systems of interacting Fermi or Bose particles is suggested. The conditions under which such systems can be statistically described are analysed. It was, in particular, shown that even for few particles, the onset of thermalization is possible provided the interaction between particles is strong and complex enough. Presented by F.M. Izrailev at the International Conference on “Atomic Nuclei and Metallic Clusters”, Prague, September 1–5, 1997. This work was supported by the Australian Research Council.     

Optical reflectivity study of silicon ion implanted poly(methyl methacrylate)

The optical reflectivity (both specular and off-specular) of poly(methyl methacrylate) (PMMA) implanted with silicon ions (Si⁺) at energy of 50 keV, is studied in the spectral range 0.25-25 μm. The effect from the Si⁺ implantation on the reflectivity of two PMMA materials is examined in the dose range from 10¹⁴ to 10¹⁷ ions/cm² and is linked to the structure formed in this ion implanted plastic. As compared to the pristine PMMA, an enhancement of the reflectivity of Si⁺ implanted PMMA is observed, that is attributed to the modification of the subsurface region of PMMA upon the ion implantation. The ion-produced subsurface organic interface is also probed by laser-induced thermo-lens.     

Structure and morphology of Cu/Ni film grown by electrodeposition method: A study of neutron reflectivity and AFM

We present detailed study of structure and interface morphology of an electrodeposited Cu/Ni film using X-ray diffraction, X-ray reflectivity, neutron reflectivity and atomic force microscopy (AFM) techniques. The crystalline structure of the film has been determined by X-ray diffraction, which suggest polycrystalline growth of the film. The depth profile of density in the sample has been obtained from specular X-ray and neutron reflectivity measurements. AFM image of the air-film interface shows that the surface is covered by globular islands of different sizes. The AFM height distribution of the surface clearly shows two peaks and the relief structure (islands) on the surface in the film, which can be treated as a quasi-two-level random rough surface structure. We have demonstrated that the detailed morphology of air-film interfaces, the quasi-two-level surface structure as well as morphology of the buried interfaces can be obtained from off-specular neutron reflectivity data. AFM and off-specular neutron reflectivity measurements also show that the morphologies of electrodeposited surface is distinctively different as compared to that of sputter-deposited surfaces in the sample.     

Threshold reduction of stimulated Brillouin scattering (SBS) using fiber loop schemes

SBS mirrors as self-pumped and easy to handle non-linear optical devices are frequently used in high-power laser systems for improving the beam quality based on optical phase conjugation. Because of the non-linear behaviour, a certain pulse energy or power of incident light is needed to generate enough reflectivity for practical purposes. Therefore, reducing this “threshold” is still a main topic in the development of new schemes for optical phase conjugation. In addition to the taper concept reported earlier, this paper deals with loop schemes for reducing the power requirements. A reduction of the so-called “threshold” by a factor of between two and four was obtained with the schemes investigated using liquids and fibers. Received: 4 September 2001 / Revised version: 22 October 2001 / Published online: 23 November 2001     

Probing the local order of single phospholipid membranes using grazing incidence x-ray diffraction

We report the first grazing incidence x-ray diffraction measurements of a single phospholipid bilayer at the solid-liquid interface. Our grazing incidence x-ray diffraction and reflectivity measurements reveal that the lateral ordering in a supported DPPE (1, 2-Dipalmitoyl-sn-Glycero-3-Phosphoethanolamine) bilayer is significantly less than that of an equivalent monolayer at the air-liquid interface. Our findings also indicate that the leaflets of the bilayer are uncoupled in contrast to the scattering from free standing phosphatidylcholine bilayers. The methodology presented can be readily implemented to study more complicated biomembranes and their interaction with proteins.     

Effective collection of Brillouin scattered light in liquids

Devices for the collection of Brillouin scattered light in liquids are discussed. Optical systems have hitherto employed conical mirrors; their angular acceptance functions are presented. Novel devices proposed and discussed are the cylinder lens and the “scattering tube” (a cylindrical mirror). Results of applications are reported. This work was supported by the “Deutsche Forschungsgemeinschaft”.     

Retrieval of the complex reflection coefficient from nano scale thin films by using polarized neutrons and magnetic substrates

A method is proposed for overcoming the famous ‘phase problem’ in neutron specular reflectometry. It is shown that the complex reflection coefficient of any unknown non magnetic layer, with real scattering length density, can be determined by using a magnetic transmitted media and by measuring the polarization of the reflected beam relative to the incident beam. The method follows directly from a recent one which is limited to a one-dimensional neutron polarization. Here, the theory is generalized for a neutron polarization of arbitrary direction. We show that some combinations between the polarization of the incident and reflected beam must be used to determine the reflection coefficient. Also, it is shown that instead of full polarization or reflectivity analysis, some combinations between polarization and reflectivity can be used in the analysis process. The method is supplemented with a schematic example to test the method and its stability in the presence of experimental uncertainties and roughness of the interfaces. PACS 61.12.Ha; 28.20.-v     

Polarized infrared reflectivity study of an oriented ceramic of Bi 2 Sr 2 Ca 2 Cu 3 O 10 + δ (Bi-2223)

The reflectivity spectra of an oriented ceramic of Bi-2223 has been investigated by polarized infrared reflectivity spectroscopy in the energy range 0.005-2.2 eV. It is shown that the data for the polarization parallel to the c axis cannot be fitted with a one-component Drude or extended-Drude model. The conductivity spectrum is then obtained from the best fit of a “double-damping Drude” model to reflectivity spectra, itself derived from the factorized form of the dielectric function, and by a Kramers-Kronig inversion as well. The data and their analysis give a new insight of the 2D character of the system. Received 26 April 2001 and Received in final form 28 August 2001     

Specular neutron reflectivity and beyond

A polarized neutron reflectometer for vertical samples is available at Dhruva reactor guide hall, Trombay. The reflectometer has been designed for horizontal scattering vector. It uses a position-sensitive detector for obtaining the reflectivity pattern. This arrangement allows one to obtain diffuse or off-specular intensity around any specular peak at one go. We have used this instrument for studying the structure of various metal-metal and metal-semiconductor multilayers by specular reflectometry. We have also been successful in understanding interface morphology of several films through diffuse neutron reflectometry (DNR) on this reflectometer. Some of the recent results are presented in this paper to demonstrate the strength of these two techniques.      

Interface Sensitive Investigation of 57Fe/Cr Superstructure by Means of Nuclear Resonance Standing Waves in Time Scale

With synchrotron pulsed radiation we have measured the time spectra of reflectivity for several grazing angles in vicinity of the Bragg peak for a microcrystalline periodical (Fe/Cr)₂₆ multilayer. In such a way a “scan” of hyperfine field distribution over bilayer depth was performed (as follows from the concept of standing waves). Variations of the spectrum shape have revealed that the orientation of hyperfine field is different in the middle part of ⁵⁷Fe layers and in the interfaces. Besides we observed the differences of Fe/Cr and Cr/Fe interfaces. This revised version was published online in August 2006 with corrections to the Cover Date.     

Standing Wave Effects in Nuclear Resonance Bragg Reflectivity: Comparison of the Energy and Time Scales and First Experimental Results

The applicability of the concept of standing wave for the nuclear resonance Bragg reflectivity of synchrotron radiation has been tested for a microcrystalline (Fe/Cr)₂₆ multilayer. In the time domain the depth selectivity is strongly enhanced. A “scan” of hyperfine field distribution over bilayer depth was performed by a variation of the angle near the Bragg peak. In particular we observed that Fe/Cr and Cr/Fe interfaces are quite different and that the magnetic field orientation is different in the interfaces and in the central part of Fe layers. This revised version was published online in September 2006 with corrections to the Cover Date.