Dissipative curvature fluctuations in bilayer vesicles: Coexistence of pure-bending and hybrid curvature-compression modes

We have studied the relaxation dynamics of shape fluctuations in unilamellar lipid vesicles by neutron spin echo (NSE). The presence of a hybrid curvature-compression mode coexisting with the usual bending one has been revealed in the experimental relaxation functions at high q . Differently to the conventional relaxation ∼ q ³ typical for bending modes, the hybrid mode was found to relax as ∼ q ² , which is compatible with a dissipation mechanism arising from intermonolayer friction. Complementary data obtained from flickering spectroscopy (FS) in giant unilamellar vesicles confirm the existence of both modes coexisting together. By combining NSE and FS data we have depicted the experimental bimodal dispersion diagram, which is found compatible with theoretical predictions for reliable values of the material parameters. From the present data two conventional dynamical methods (NSE and FS) have been shown to be suitable for measuring intermonolayer friction coefficients in bilayer vesicles.     

Concentration-independent spontaneously forming biomimetric vesicles

In this Letter we present small-angle neutron scattering data from a biomimetic system composed of the phospholipids dimyristoyl and dihexanoyl phosphorylcholine (DMPC and DHPC, respectively). Doping DMPC-DHPC multilamellar vesicles with either the negatively charged lipid dimyristoyl phosphorylglycerol (DMPG, net charge -1) or the divalent cation, calcium (Ca2+), leads to the spontaneous formation of energetically stabilized monodisperse unilamellar vesicles whose radii are concentration independent and in contrast with previous experimental observations.     

Transition from unilamellar to bilamellar vesicles induced by an amphiphilic biopolymer

We report some unusual structural transitions upon the addition of an amphiphilic biopolymer to unilamellar surfactant vesicles. The polymer is a hydrophobically modified chitosan and it embeds its hydrophobes in vesicle bilayers. We study vesicle-polymer mixtures using small-angle neutron scattering (SANS) and cryotransmission electron microscopy (cryo-TEM). When low amounts of the polymer are added to unilamellar vesicles of ca. 120 nm diameter, the vesicle size decreases by about 50%. Upon further addition of polymer, lamellar peaks are observed in the SANS spectra at high scattering vectors. We show that these spectra correspond to a co-existence of unilamellar and bilamellar vesicles. The transition to bilamellar vesicles as well as the changes in unilamellar vesicle size are further confirmed by cryo-TEM. A mechanism for the polymer-induced transitions in vesicle morphology is proposed.     

Phosphatidylcholine Membrane Fusion Induced by Dimethyl Sulfoxide and Diethyl Sulfoxide

The kinetics of unilamellar vesicle fusion induced by the addition of dimethyl sulfoxide (DMSO) and diethyl sulfoxide (DESO) with mole fractions of 0.1 and 0.2 is studied in the liquid-crystal phase using small-angle neutron scattering. Multilamellar vesicles formed due to the partial fusion of unilamellar vesicles of 1,2-dimyristoyl-sn-glycero-3-phosphadylcholine (DMPC) with the addition of DMSO (Х_DMSO = 0.1, 0.2) and DESO (Х_DESO = 0.2) are stable for a long time. The cooling–heating process does not affect the stability of the formed systems. The presence of DMSO and DESO with a mole fraction of 0.2 leads to disappearance of the ripple phase. The addition of DESO to the unilamellar vesicles of DMPC in D₂O with a mole fraction of 0.1 does not affect the structure of unilamellar vesicles for 5–15 minutes after adding the sulfoxide in the liquid-crystal phase. Three hours later, a stable system consisting of unilamellar vesicles with a lipid bilayer thickness of 27.3(2) Å and multilamellar vesicles with a repeat distance of d = 43.6(2) Å is formed. During cooling, multilamellar vesicles are destroyed in the region of the main phase transition (T'_m = 24.8(9)°C for the investigated system) and unilamellar vesicles are formed.     

Regulation of the intermittent release of giant unilamellar vesicles under osmotic pressure

Osmotic pressure can break the fluid balance between intracellular and extracellular solutions. In hypo-osmotic solution, water molecules, which transfer into the cell and burst, are driven by the concentration difference of solute across the semi-permeable membrane. The complicated dynamic processes of intermittent bursts have been previously observed. However, the underlying physical mechanism has yet to be thoroughly explored and analyzed. Here, the intermittent release of inclusion in giant unilamellar vesicles was investigated quantitatively, applying the combination of experimental and theoretical methods in the hypo-osmotic medium. Experimentally, we adopted a highly sensitive electron multiplying charge-coupled device to acquire intermittent dynamic images. Notably, the component of the vesicle phospholipids affected the stretch velocity, and the prepared solution of vesicles adjusted the release time. Theoretically, we chose equations and numerical simulations to quantify the dynamic process in phases and explored the influences of physical parameters such as bilayer permeability and solution viscosity on the process. It was concluded that the time taken to achieve the balance of giant unilamellar vesicles was highly dependent on the molecular structure of the lipid. The pore lifetime was strongly related to the internal solution environment of giant unilamellar vesicles. The vesicles prepared in viscous solution were able to visualize long-lived pores. Furthermore, the line tension was measured quantitatively by the release velocity of inclusion, which was of the same order of magnitude as the theoretical simulation. In all, the experimental values well matched the theoretical values. Our investigation clarified the physical regulatory mechanism of intermittent pore formation and inclusion release, which provides an important reference for the development of novel technologies such as gene therapy based on transmembrane transport as well as controlled drug delivery based on liposomes.     

Dynamics of the self-assembly of unilamellar vesicles

We have studied the transient stages in the formation of unilamellar vesicles with millisecond time resolution. The self-assembly was initiated by rapid mixing of equimolar amounts of anionic and zwitterionic micelles and the transient micellar entities were probed by time-resolved small-angle x-ray scattering. Within the mixing time, original micelles transformed to disklike micelles which evolved further to a critical size and then closed to form monodisperse unilamellar vesicles within a second. Subsequent growth led to an unexpected broadening of the vesicle size distribution.     

Lattice dynamics of Nb3Sn at 300 K

The phonon dispersion curves have been calculated from a microscopic model for Nb₃Sn at 300 K and are in good agreement with the available inelastic neutron scattering data. The calculated phonon density of states exhibits the essential features of the experimental results obtained by incoherent inelastic neutron scattering.     

Detection of submicron-sized raft-like domains in membranes by small-angle neutron scattering

Using coarse grained models of heterogeneous vesicles we demonstrate the potential for small-angle neutron scattering (SANS) to detect and distinguish between two different categories of lateral segregation: 1) unilamellar vesicles (ULV) containing a single domain and 2) the formation of several small domains or “clusters” (~10 nm in radius) on a ULV. Exploiting the unique sensitivity of neutron scattering to differences between hydrogen and deuterium, we show that the liquid ordered (lo) DPPC-rich phase can be selectively labeled using chain deuterated dipalymitoyl phosphatidylcholine (dDPPC), which greatly facilitates the use of SANS to detect membrane domains. SANS experiments are then performed in order to detect and characterize, on nanometer length scales, lateral heterogeneities, or so-called “rafts”, in ~30 nm radius low polydispersity ULV made up of ternary mixtures of phospholipids and cholesterol. For 1:1:1 DOPC:DPPC:cholesterol (DDC) ULV we find evidence for the formation of lateral heterogeneities on cooling below 30 °C. These heterogeneities do not appear when DOPC is replaced by SOPC. Fits to the experimental data using coarse grained models show that, at room temperature, DDC ULV each exhibit approximately 30 domains with average radii of ~10 nm.     

Determination of nanostructure of liposomes containing two model drugs by X‐ray scattering from a synchrotron source

Small‐angle X‐ray scattering has been employed to study how the introduction of paracetamol and acetylsalicylic acid into a liposome bilayer system affects the system's nanostructure. An X‐ray scattering model, developed for multilamellar liposome systems [Pabst et al. (2000), Phys. Rev. E, 62 , 4000–4009], has been used to fit the experimental data and to extract information on how structural parameters, such as the number and thickness of the bilayers of the liposomes, thickness of the water layer in between the bilayers, size and volume of the head and tail groups, are affected by the drugs and their concentration. Even though the experimental data reveal a complicated picture of the drug–bilayer interaction, they clearly show a correlation between nanostructure, drug and concentration in some aspects. The localization of the drugs in the bilayers is discussed.     

Transition from small to big charged unilamellar vesicles

The transition from small to big unilamellar vesicles predicted by a Poisson-Boltzmann Cell Model for the thermodynamics of a dilute phase of unilamellar charged vesicles is characterized. The radius as a function of experimental parameters is calculated and the coexistence region of small and big vesicles is identified. We further investigate the physical meaning in terms of simplified models, which allow for an identification of the role of parameters like the surface charge density or the Debye-length. Connections to experiments are discussed. Received: 20 October 1997 / Received in final form: 9 February 1998 / Accepted: 9 March 1998     

Optical studies of lecithin-membrane melting

The two-dimensional phase transition of some lecithin membranes forming large vesicles was observed under a phase contrast microscope. The transition temperatures were found to depend on membrane thickness. This seems to offer a convenient means to discern unilamellar vesicles, i.e., those surrounded by a single bilayer.     

Nano-meter-sized domain formation in lipid membranes observed by small angle neutron scattering

Using a contrast matching technique of small angle neutron scattering (SANS), we have investigated a phase separation to liquid-disordered and liquid-ordered phases on ternary small unilamellar vesicles (SUVs) composed of deuterated-saturated, hydrogenated-unsaturated phosphatidylcholine lipids and cholesterol, where the equilibrium size of these domains is constrained to less than 10nm by the system size. Below a miscibility temperature, we observed characteristic scattering profiles with a maximum, indicating the formation of nano-meter-sized domains on the SUVs. The observed profiles can be described by a multi-domain model rather than a mono-domain model. The nano-meter-sized domain is agitated by thermal fluctuations and eventually ruptured, which may result in the multi-domain state. The kinetically trapped nano-meter-sized domains grow to a mono-domain state by decreasing temperature. Furthermore, between the miscibility and disorder-order transition temperature of saturated lipid, the integrated SANS intensity increased slightly, indicating the formation of nano-meter-sized heterogeneity prior to the domain nucleation.     

Further Analysis of Neutron Double-Differential Cross Section of n ＋ ^16O at 14.1 MeV and 18 MeV

By using a new reaction model for light nuclei, the double-differential cross section of total outgoing neutron with LUNF code for n＋^16O reactions at En=14.1 MeV and 18 MeV have been calculated and analyzed. In this paper the opened reaction channels, which have contribution to emitting the neutrons, are listed in detail. To improve the fitting results the direct inelastic scattering mechanism is involved. The calculating results agree fairly well with the experimental data at E,~ = 14.1 MeV and the deviation from calculated results and experimental data in low energy region at En= 18 MeV has been analyzed. Since the possibility of 5He has been affirmed theoretically [J.S. Zhang, Sci. Chin. G 47 （2004） 137], so 5He emission from n＋ ^16O reaction is taken into account, which plays an important role at the region of the outgoing neutron energy εn〈3 MeV in total outgoing neutron energy-angular spectrum. The calculated results indicate that the pre-equilibrium mechanism dominates the whole reaction processes, and the recoil effect in light nuclear reactions is essentially important.     

密闭实验大厅内散射中子注量的模拟研究

为能够快速评判实验测试方案和预估实验结果,建立了中子体通量的快速估算模型。理论上,封闭空间中子平均体通量与特征长度的平方成反比,且中子体通量的大小能反映散射中子注量强弱。采用蒙特卡罗模拟方法,计算得到了密闭实验大厅内中子的体通量,以及不同位置处的散射中子注量,并将模拟得到的体通量和散射中子注量拟合成便于工程实践中应用的解析表达式,拟合结果与模拟结果的相对偏差小于10%。研究结果表明,球形空间内中子的体通量与球半径的1.905次方成反比;密闭实验大厅的中子体通量与大厅横截面宽度的1.948次方成反比,与长宽比的0.775次方成反比;球形空间结构内,每个源中子的平均径迹长度约为半径的5.4倍,而长方体密闭实验大厅内,单个源中子的平均径迹长度为大厅特征尺度的2~3倍。     

Structure and phase transitions of DMPC multilamellar vesicles in the presence of Ca<Superscript>2+</Superscript> ions

Results obtained via small-angle neutron scattering studies of the influence of calcium ions on the structure and phase transitions of phospholipid membranes are presented. The main phase transition temperature of 1,2-dimyristoyl-sn-glycero-3-phosphatidylcholine (1 wt %) multilamellar vesicles is demonstrated to increase by more than 1°C even when the calcium-ion content of the solution is low (0.1 mM). Detailed analysis of the multilamellar vesicles transition between “bound” and “unbound” state indicates the continuous character of the investigated process in both liquid and gel phases. The critical Ca²⁺ ion concentrations which initiate the destruction of the multilamellar structures and the formation of unilamellar vesicles are found to be ~0.3 mM in the gel and ~0.4–0.5 mM in the liquid-crystal phases during heating and ~0.5 mM in the phases under study upon cooling.     

中子辐射俘获反应机制的质量能量相关性研究

对A?<10?0核质量区内的核素,研究中子辐射俘获反应中不同反应机制对辐射俘获截面的贡献随靶核质量数和中子入射能量变化的规律.所考虑的反应机制有复合核统计过程和复合核弹性散射道中的辐射俘获及形状弹性散射道中的直接–半直接辐射俘获两种非统计过程.在中子入射能量0.1—20MeV区间,给出了²⁷Al,⁴⁰Ca,⁶³Cu和⁹³Nb的理论计算结果及与实验数据的比较,并对呈现的变化规律进行了分析讨论     

Influence of lipid composition and membrane curvature on fluorescence and solvent relaxation kinetics in unilamellar vesicles

Time-resolved fluorescence on unilamellar vesicles shows that increasing amounts of anionic, natural lipid lead to a larger increase in polarity close to the headgroups than in the hydrophobic core of the bilayer. The region close to the headgroups is less polar in vesicles containing phosphatic acid rather than phosphatidylserine. A greater membrane curvature increases the mobility of the hydrated headgroups.     

Neutron-Proton Ratio at Different Atmospheric Depths and Sea Level Neutron Spectrum Derived from the Primary Nucleon Spectrum

The differential neutron spectrum at sea level has been calculated using the conventional phenomenological model after ASHTON. The energy dependence of nucleon-air nucleus inelastic interaction cross section is assumed in these calculations. The derived sea level neutron spectrum from the satellite measured primary nucleon spectrum of GRIGOROV et al. fits well the experimental neutron spectrum of ASHTON and COATS. The neutron-proton ratios calculated for different atmospheric depths is in accord with the measured data (AGUIRRE).