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PubMed2004

Imaging phase separation near the Mott boundary of the correlated organic superconductors kappa-(BEDT-TTF)2X.

Electronic phase separation consisting of the metallic and insulating domains with 50-100 microm in diameter is found in the organic Mott system kappa-[(h8-BEDT-TTF)(1-x)(d8-BEDT-TTF)x]2Cu[N(CN)2]Br by means of scanning microregion infrared spectroscopy using the synchrotron radiation. The phase separation appears below the critical end temperature 35-40 K of the first-order Mott transition. The observation of the macroscopic size of the domains indicates a different class of the intrinsic electronic inhomogeneity from the nanoscale one reported in the inorganic Mott systems such as high-Tc copper and manganese oxides.

Journal Article↗

PubMed2004

Drug release characteristics of phase separation pHEMA sponge materials.

A number of phase separation pHEMA sponge hydrogels have been prepared based on variations in monomer contents, concentration of cross-linking agent, solvent mixture and temperature of polymerization. The loading levels and release profiles of the anti-inflammatory drug prednisolone were examined for each of the pHEMA sponge materials. An effective diffusion coefficient determined by an optimization approach based on the experimental data was used to measure their release characteristics. The effect of morphological variations, revealed by the environmental scanning electron microscopy, and polymer/solvent volume fractions on these properties were discussed.

Adhesives↗

PubMed2002

Phase separation due to quantum mechanical correlations.

Can phase separation be induced by strong electron correlations? We present a theorem that affirmatively answers this question in the Falicov-Kimball model away from half filling, for any dimension. In the ground state the itinerant electrons are spatially separated from the classical particles.

Journal Article↗

PubMed1993

The effect of phase separation on biphasic waveform defibrillation.

It has been hypothesized that the defibrillation efficacy of a biphasic shock is caused by the large change in voltage between the two phases. This study examined the effects of separating the two phases in time thus splitting in half the rapid voltage change at phase reversal. The study was performed in three parts each using six dogs. Part I determined defibrillation thresholds (DFTs) for two exponentially truncated biphasic waveforms (3.5/2 msec and 6/6 msec) with interphase time delays of 0, 1, 2, 3, 4, 6, 8, and 10 msec. In Part II, probability of success curves were generated using an up down method with 15 shocks for each delay for the 3.5/2 msec biphasic waveform with interphase delays of 0, 2, 3, 4, and 5 msec. In Part III, DFTs were determined using a 3.5/2 msec and 6/6 msec biphasic as well as a third waveform that consisted of two sequential 6-msec pulses of the same polarity with interphase delays of 0, 5, 10, 15, 20, 25, 50, and 100 msec. In all three parts the defibrillating cathode was a 6.17 cm2 transvenous spring electrode positioned in the RV apex and the anode was a 113 cm2 cutaneous left chest wall electrode patch. With all waveforms, the trailing edge voltage of the first phase was equal to the negative of the leading edge voltage of the second phase. There was no statistical difference in DFTs or in 50% successful defibrillation points for phase separations from 0 to 6 msec and 0 to 5 msec for Parts I and II, respectively. In Part I there was a significant increase in DFTs for phase separations of 8 and 10 msec compared to a phase separation of 0 msec. In Part III there was no significant difference for separations of 0 and 5 msec; however, there was a significant increase in DFT requirements for separations from 5 to 50 msec, which then decreased with a separation of 100 msec for all three waveforms tested. In conclusion, defibrillation efficacy was unchanged with phase separations up to 6 msec. With phase separation, the rapid voltage change during phase reversal is split in half and, thus, cannot explain the improved efficacy of biphasic waveforms.

Animals↗

PubMed2005

Kinetics of phase separation in thin films: simulations for the diffusive case.

We study the diffusion-driven kinetics of phase separation of a symmetric binary mixture (AB), confined in a thin-film geometry between two parallel walls. We consider cases where (i) both walls preferentially attract the same component (A), and (ii) one wall attracts and the other wall attracts (with the same strength). We focus on the interplay of phase separation and wetting at the walls, which is referred to as surface-directed spinodal decomposition (SDSD). The formation of SDSD waves at the two surfaces, with wave vectors oriented perpendicular to them, often results in a metastable layered state (also referred to as "stratified morphology"). This state is reminiscent of the situation where the thin film is still in the one-phase region but the surfaces are completely wet, and hence coated with thick wetting layers. This metastable state decays by spinodal fluctuations and crosses over to an asymptotic growth regime characterized by the lateral coarsening of pancakelike domains. These pancakes may or may not be coated by precursors of wetting layers. We use Langevin simulations to study this crossover and the growth kinetics in the asymptotic coarsening regime.

Journal Article↗

PubMed2002

Dynamic phase separation of fluid membranes with rigid inclusions.

Membrane shape fluctuations induce attractive interactions between rigid inclusions. Previous analytical studies showed that the fluctuation-induced pair interactions are rather small compared to thermal energies, but also that multibody interactions cannot be neglected. In this paper, it is shown numerically that shape fluctuations indeed lead to the dynamic separation of the membrane into phases with different inclusion concentrations. The tendency of lateral phase separation strongly increases with the inclusion size. Large inclusions aggregate at very small inclusion concentrations and for relatively small values of the inclusions' elastic modulus.

Journal Article↗

PubMed2005

Phase separation and an upper bound for a generalized superfluid gap for cold fermi fluids in the unitary regime.

An upper bound is derived for Delta for a cold dilute fluid of equal amounts of two species of fermion in the unitary limit k(f)a--> infinity (where k(f) is the Fermi momentum, a is the scattering length, and Delta is a pairing energy: the difference in energy per particle between adding to the system a macroscopic number (but infinitesimal fraction) of particles of one species compared to adding equal numbers of both. The bound is delta < or =5/3 [2(2xi)(2/5)-(2xi)] where xi=epsilon/epsilon(FG), delta=2Delta/epsilon(FG); epsilon is the energy per particle and epsilon(FG) is the energy per particle of a noninteracting Fermi gas. If the bound is saturated, then systems with unequal densities of the two species will separate spatially into a superfluid phase with equal numbers of the two species and a normal phase with the excess. If the bound is not saturated, then Delta is the usual superfluid gap. If the superfluid gap exceeds the maximum allowed by the inequality, phase separation occurs.

Journal Article↗

PubMed2006

The performance of a phase separated granular bed bioreactor treating brewery wastewater.

This study presents the performance characteristics of a plug flow phase separated anaerobic granular bed baffled reactor (GRABBR) fed with brewery wastewater at various operating conditions. The reactor achieved chemical oxygen demand (COD) removal of 93-96% with high methane production when operated at organic loading rates (OLRs) of 2.16-13.38kg COD m(-3)d(-1). The reactor configuration and microbial environment encouraged the acidogenic dominant zone to produce intermediate products suitable for degradation in the predominantly methanogenic zone. Noticeable phase separation between acidogenesis and methanogenesis mainly occurred at high OLR, involving a greater number of compartments to contribute to wastewater treatment. The highly active nature and good settling characteristics of methanogenic granular sludge offered high biomass retention and enhanced methanogenic activities within the system. The granular structure in the acidogenic dominant zone of the GRABBR was susceptible to disintegration and flotation. Methanogenic granular sludge was a multi-layered structure with Methanosaeta-like organisms dominant in the core.

Bacteria, Anaerobic↗

PubMed1975

Chemically induced lipid phase separation in model membranes containing charged lipids: a spin label study.

The lipid distribution in binary mixed membranes containing charged and uncharged lipids and the effect of Ca2+ and polylysine on the lipid organization was studied by the spin label technique. Dipalmitoyl phosphatidic acid was the charged, and spin labelled dipalmitoyl lecithin was the uncharged (zwitterionic) component. The ESR spectra were analyzed in terms of the spin exchange frequency, Wex. By measuring Wex as a function of the molar percentage of labelled lecithin a distinction between a random and a heterogeneous lipid distribution could be made. It is established that mixed lecithin-phosphatidic acid membranes exhibit lipid segregation (or a miscibility gap) in the fluid state. Comparative experiments with bilayer and monolayer membranes strongly suggest a lateral lipid segregation. At low lecithin concentration, aggregates containing between 25% and 40% lecithin are formed in the fluid phosphatidic acid membrane. This phase separation in membranes containing charged lipids is understandable on the basis of the Gouy-Chapman theory of electric double layers. In dipalmitoyl lecithin and in dimyristoyl phosphatidylethanolamine membranes the labelled lecithin is randomly distributed above the phase transition and has a coefficient of lateral diffusion of D = 2.8-10(-8) cm2/s at 59 degrees C. Addition of Ca2+ dramatically increases the extent of phase separation in lecithin-phosphatidic acid membranes. This chemically (and isothermally) induced phase separation is caused by the formation of crystalline patches of the Ca2+-bound phosphatidic acid. Lecithin is squeezed out from these patches of rigid lipid. The observed dependence of Wex on the Ca2+ concentration could be interpreted quantitatively on the basis of a two-cluster model. At low lecithin and Ca2+ concentration clusters containing about 30 mol % lecithin are formed. At high lecithin or Ca2+ concentrations a second type of precipitation containing 100% lecithin starts to form in addition. A one-to-one binding of divalent ions and phosphatidic acid at pH 9 was assumed. Such a one-to-one binding at pH 9 was established for the case of Mn2+ using ESR spectroscopy. Polylysine leads to the same strong increase in the lecithin segregation as Ca2+. The transition of the phosphatidic acid bound by the polypeptide is shifted from Tt = 47.5 degrees to Tt = 62 degrees C. This finding suggests the possibility of cooperative conformational changes in the lipid matrix and in the surface proteins in biological membranes.

Calcium↗

PubMed2005

Oxidized phospholipids induce phase separation in lipid vesicles.

The thermal behaviour of phospholipid multilamellar vesicles (MLV) made of various molar percentages of DPPC and LPPC, containing also oxidized LPPC (LPPCox), was studied by use of EPR spectroscopy and n-DSPC spin label in order to determine variations in the membrane fluidity brought about by lipid oxidation. Experimental variables were temperature, ranging from 4 to 44 degrees C, and molar percentage composition of DPPC/LPPC/LPPCox ternary mixture. We found that the presence of LPPCox in a percentage higher than both normal phospholipids' heavily hindered membrane formation, while lower percentage of the oxidized lipid with higher DPPC percentages yielded two-components EPR spectra, showing the presence of two different fluidity domains, indicative of membrane phase separation. When LPPC was the dominant lipid in the ternary mixture, simple EPR spectra were observed, indicating homogeneity of MLV membranes. Phase separation observed in the presence of LPPCox was better visible at lower temperature (12 degrees C or less), and almost disappeared with increasing temperature (36 degrees C or more). Furthermore, the correlation time of 16-DSPC in ternary mixture MLVs with higher LPPC percentage (homogeneous membranes) was not affected by the presence of LPPCox, while it normally increased upon DPPC percentage increase, as readily calculated from the EPR spectra featuring simple bands at 24 degrees C. It is concluded that oxidized lipid induces phase separation in more rigid DPPC-rich membranes, while leaving fluidity unaffected in more fluid LPPC-rich membranes, and at higher temperature.

1,2-Dipalmitoylphosphatidylcholine↗

PubMed1996

Effect of electrostatic interaction on phase separation behaviour of chitin crystallite suspensions.

Optical and electron microscopy were used to observe the dynamics of the phase separation in aqueous chitin suspensions prepared by HCl hydrolysis of crab chitin. Freeze-fracture transmission electron microscopy reveals that chitin crystallites are partially aggregated in the suspension and have an average length of 200 nm and an average width of 8 nm. They exhibit a positive surface charge of approximately 0.5 e/nm2 when fully protonated. The liquid crystal-forming aqueous suspensions of such crystallites are investigated through phase diagrams and Zeta potential measurements for different ionic strength. Exposure of the suspension to a low concentration of univalent electrolyte has a negligible effect on phase separation because of the contribution of the charged crystallites themselves to the ionic strength. The thickness of the effective repulsive layer is estimated both from the phase diagrams according to Onsager's theory and from the computed interaction energy derived from the Poisson-Boltzmann equation using the experimental Zeta potential as surface potential. When the contribution of crystallites to the ionic strength is taken into account and an hypothetical linear charge density close to the Manning limit is assumed, there is good agreement with the Debye length.

Animals↗

PubMed2006

Comment on "Pairing and phase separation in a polarized Fermi gas".

Partridge et al. (Reports, 27 January 2006, p. 503) reported pairing and phase separation in a polarized Fermi gas. We argue that it is not possible to distinguish the superfluid from the normal regimes in the presented data, or to discern which clouds were phase-separated. Some of the reported conclusions are inconsistent with recent experiments.

Comment↗

PubMed2005

Smoothed particle hydrodynamics model for phase separating fluid mixtures. II. Diffusion in a binary mixture.

A previously formulated smoothed particle hydrodynamics model for a phase separating mixture is tested for the case when viscous processes are negligible and only mass and energy diffusive processes take place. We restrict ourselves to the case of a binary mixture that can exhibit liquid-liquid phase separation. The thermodynamic consistency of the model is assessed and the potential of the model to study complex pattern formation in the presence of various thermal boundaries is illustrated.

Journal Article↗

PubMed1986

Fractionation of detergent lysates of cells by ammonium sulphate-induced phase separation.

A procedure is described for fractionating detergent lysates of cells based on the ability of (NH4)2SO4 to induce phase separation of detergents such as Triton X-100, sodium deoxycholate, and sodium cholate, into detergent-rich and detergent-depleted phases. An analysis of six murine lymphocyte cell surface molecules revealed that the partitioning in Triton X-100 of each molecule was highly dependent upon the (NH4)2SO4 concentration, each antigen partitioning into the detergent-rich phase at a defined salt concentration. In contrast, none of the six molecules appeared in the detergent-rich phase of a Triton X-114 phase separation, even though two of the molecules, namely Ly-2/3 and L3T4, are well-characterized integral membrane proteins. It was also observed that (NH4)2SO4 resulted in the partitioning of many nonmembrane proteins into the detergent-rich phase, indicating that the procedure can be used to fractionate all cellular proteins. By judicious choice of (NH4)2SO4 concentrations, precipitation of cellular proteins at two different (NH4)2SO4 concentrations, and combining the method with subcellular fractionation prior to detergent solubilization, substantial enrichment and concentration of particular cellular proteins could be achieved.

Ammonium Sulfate↗

PubMed2000

Forming supramolecular networks from nanoscale rods in binary, phase-separating mixtures

Simulations show that when low-volume fractions of nanoscale rods are immersed in a binary, phase-separating blend, the rods self-assemble into needle-like, percolating networks. The interconnected network arises through the dynamic interplay of phase-separation between the fluids, through preferential adsorption of the minority component onto the mobile rods, and through rod-rod repulsion. Such cooperative effects provide a means of manipulating the motion of nanoscopic objects and directing their association into supramolecular structures. Increasing the rod concentration beyond the effective percolation threshold drives the system to self-assemble into a lamellar morphology, with layers of wetted rods alternating with layers of the majority-component fluid. This approach can potentially yield organic/inorganic composites that are ordered on nanometer scales and exhibit electrical or structural integrity.

Journal Article↗

PubMed2004

A two-dimensional liquid-phase separation method coupled with mass spectrometry for proteomic studies of breast cancer and biomarker identification.

A two-dimensional liquid-phase separation scheme coupled with mass spectrometry (MS) is presented for proteomic analysis of cell lysates from normal and malignant breast epithelial cell lines. Liquid-phase separations consist of isoelectric focusing as the first dimension and nonporous silica reverse-phase high-performance liquid chromatography (NPS-RP-HPLC) as the second dimension. Protein quantitation and mass measurement are performed using electrospray ionization-time of flight MS (ESI-TOF MS). Proteins are identified by peptide mass fingerprinting using matrix-assisted laser desorption ionization-time of flight MS (MALDI-TOF MS) and MALDI-quadrupole time of flight (QTOF)-tandem mass spectrometry (MS/MS). Two pH regions with 50-60 unique proteins in each pH range were chosen for analysis. Mass maps were created that allowed visualization of protein quantitation differences between normal and malignant breast epithelial cells. Of the approximately 110 unique proteins observed from mass mapping experiments over the limited pH range, 40 (36%) were positively identified by peptide mass fingerprinting and assigned to bands in the mass maps. Of these 40 proteins, 22 were more highly expressed in one or more of the malignant cell lines. These proteins represent potential breast cancer biomarkers that could aid in diagnosis, therapy, or drug development.

Biomarkers, Tumor↗

PubMed2006

Selective protein adsorption on a phase-separated solvent-cast polymer blend.

Polymer-based biomedical devices are growing increasingly sophisticated as compositions evolve toward copolymers and blends in order to satisfy complex design criteria. Such polymers afford opportunities for both micro- and macrophase separation at nano- and micro-length scales and raise questions concerning the role of heterogeneous surface morphology on protein adsorption. Adsorbed protein layers play a critical role in mediating the interaction of cells with polymer surfaces, and both understanding and controlling protein adsorption is assuming greater significance in the development of surfaces with enhanced physiological compatibility. Here we study the short-time adsorption of ferritin, a model protein highly resistant to denaturation and easily imaged in the transmission electron microscope (TEM), onto a phase-separated homopolymer blend of polycaprolactone (PCL) and a polycarbonate derived from desaminotyrosyl-tyrosine dodecyl ester (PDTD). At physiological pH, ferritin selectively adsorbs onto the PDTD phase at a surface density approximately three times greater than that on the PCL phase. By decreasing the pH below ferritin's isoelectric point so its average charge becomes positive, the selective adsorption disappears and the surface density of adsorbed ferritin becomes independent of the phase separation. We attribute the selectivity to the electrostatic repulsion between ferritin and hydrolytically charged PCL, both of which will have a net negative charge at physiological pH. To perform these experiments, we solvent-cast ultrathin polymer films onto dissolvable salt substrates, and we characterize the morphology by TEM imaging and quantitative spatially resolved electron energy-loss spectroscopy (EELS). We find that the film morphology depends strongly on such processing-related variables as the solvent evaporation rate and the nature of the surface in contact with the polymer film during casting. The adsorption of ferritin depends on whether the film is phase-separated as well as to which surface of the film the protein solution is exposed, and these findings suggest that seemingly small variations in polymer processing that influence both the bulk and surface morphology can have a profound effect on the short-time protein adsorption.

Adsorption↗

PubMed1983

Phase separation in rat lenses cultured in low glucose media.

Experimental evidence that indicates the nuclear opacity that develops in the hypoglycemic cataract in rat lenses is the result of a phase separation of the lens cytoplasm is presented. Phase diagrams of the cytoplasm of organ-cultured lenses were constructed for a series of incubation times in normal and hypoglycemic media. In normal media, the maximum phase separation temperature, Tmax, of the lens cytoplasm decreases with time. In hypoglycemic media, Tmax increases with time and exceeds 37 C after 24 hrs. The increase in Tmax can be stopped and reversed if the lens is returned to normal media within 8 hrs; in good agreement with an earlier biochemical analysis of the kinetics of hypoglycemic cataract formation.

Animals↗