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PubMed2005

Separation and preconcentration phenomena in internally heated poly(dimethylsilicone) capillaries: preliminary modelling and demonstration studies.

The concept of achieving low-resolution separations in internally heated capillary membranes is discussed in terms of controlling the diffusion coefficients of volatile organic compounds in poly(dimethylsilicone) membranes in space and time. The behaviour of 1,1,1-trichloroethane in polydimethylsilicone was used in conjunction with a mixed-physics finite element model, incorporating second order partial differential equations, to describe time and spatial variations of mass-flux, membrane temperature and diffusion coefficients. The model, coded with Femlab, predicted highly non-linear diffusion coefficient profiles resulting from temperature programming a 500 [micro sign]m thick membrane, with an increase in the diffusion coefficient of approximately 30% in the last 30% of the membrane thickness. Simulations of sampling hypothetical analytes, with disparate temperature dependent diffusion coefficient relationships, predicted distinct thermal desorption profiles with selectivities that reflected the extent of diffusion through the membrane. The predicted desorption profiles of these analytes also indicated that low resolution separations were possible. An internally heated poly(dimethylsilicone) capillary membrane was constructed from a 10 cm long, 1.5 mm od capillary with 0.5 mm thick walls. Thirteen aqueous standards of volatile organic compounds of environmental significance were studied, and low-resolution separations were indicated, with temperature programming of the membrane enabling desorption profiles to be differentiated. Further, analytically useful relationships in the [micro sign]g cm(-3) concentration range were demonstrated with correlation coefficients >0.96 observed for linear regressions of desorption profile intensities to analyte concentrations.

Journal Article↗
PubMed2005

Surface diffusion: the low activation energy path for nanotube growth.

We present the temperature dependence of the growth rate of carbon nanofibers by plasma-enhanced chemical vapor deposition with Ni, Co, and Fe catalysts. We extrapolate a common low activation energy of 0.23-0.4 eV, much lower than for thermal deposition. The carbon diffusion on the catalyst surface and the stability of the precursor molecules, C2H2 or CH4, are investigated by ab initio plane wave density functional calculations. We find a low activation energy of 0.4 eV for carbon surface diffusion on Ni and Co (111) planes, much lower than for bulk diffusion. The energy barrier for C2H2 and CH4 dissociation is at least 1.3 eV and 0.9 eV, respectively, on Ni(111) planes or step edges. Hence, the rate-limiting step for plasma-enhanced growth is carbon diffusion on the catalyst surface, while an extra barrier is present for thermal growth due to gas decomposition.

Journal Article↗
PubMed2005

Diffusion-weighted 19F-MRI of lung periphery: Influence of pressure and air-SF6 composition on apparent diffusion coefficients.

Lung functional magnetic resonance imaging (MRI) has become a reality using different inert hyperpolarized gases, such as 3He and 129Xe, which have provided an extraordinary boost in lung imaging and has also attracted interest to other chemically inert gaseous contrast agents. In this context, we have recently demonstrated the first diffusion-weighted images using thermally polarized inhaled sulfur hexafluoride (SF6) in small animals. The aim of this study was to evaluate whether or not the diffusion coefficient of this fluorinated gas is sensitive to pulmonary structure, gas concentration and air pressure in the airways. Diffusion coefficients of SF6 (both pure and in air mixtures) measured in vitro at different pressures and 20 degrees C showed an excellent agreement with theoretical values. Measurements of diffusion coefficients were also performed in vivo and post-mortem on healthy rats, achieving satisfactory signal-to-noise ratios (SNRs), and SF6 gas was found to be in an almost completely restricted diffusion regime in the lung, i.e., the transport by molecular diffusion is delayed by collisions with barriers such as the alveolar septa. This observed low diffusivity means that this gas will be less sensitive to structural changes in the lungs than other magnetic resonance sensitive gas such as 3He, particularly at human scale. However, it is still possible that SF6 plays a role since it opens a new structural window. Thus, the interest of researchers in delimiting the important limiting technical factors that makes this process very challenging is obvious. Among them, T2 relaxation is very fast, so gradient systems with very fast switching rate and probably large radiofrequency (RF) power and high field systems will be needed for hexafluoride to be used in human studies.

Animals↗
PubMed2005

Comparison of 24 h averaged VOC monitoring results for residential indoor and outdoor air using Carbopack X-filled diffusive samplers and active sampling--a pilot study.

Analytical results obtained by thermal desorption GC/MS for 24 h diffusive sampling of 11 volatile organic compounds (VOCs) are compared with results of time-averaged active sampling at a known constant flow rate. Air samples were collected with co-located duplicate diffusive sampling tubes and one passivated canister. A total of eight multiple-component sampling events took place at fixed positions inside and outside three private homes. Subsequently, a known amount of sample air was transferred from the canister to an adsorbent tube for analysis by thermal desorption GC/MS. Results for the 11 most prevalent compounds--Freon 11, 1,3-butadiene, benzene, toluene, tetrachloroethene, ethylbenzene, m,p-xylene, o-xylene, 4-ethyltoluene, 1,3,5-trimethylbenzene, and p-dichlorobenzene--show that the ratio of average study values (diffusive sampling to active sampling) is 0.92 with 0.70 and 1.14 extreme ratios. Absolute percent difference for duplicate samples using diffusive sampling was <10% for the four most prevalent compounds. Agreement between the two sampling approaches indicates that the prediction of approximately constant diffusive sampling rates based on previous laboratory studies is valid under the field conditions.

Air Pollutants↗
PubMed1998

Interpreting the equatorial diffraction pattern of collagenous tissues in the light of molecular motion.

The equatorial diffraction pattern associated with collagenous tissues, particularly type I collagen, is diffuse and clearly unlike that from crystals. Hukins and Woodhead-Galloway proposed a statistical model that they termed a "liquid crystal" for collagen fibers in tendons. Fratzl et al. applied this model to both unmineralized and mineralized turkey leg tendon, a model that ignores the organization imposed by the well-known cross-linking. The justification for adopting this model is that the curve fits the data. It is shown that the data can be equally well matched by fitting a least-squares curve consisting of a second-order polynomial plus a Gaussian. The peak of the Gaussian is taken as the equatorial spacing of the collagen. A physical explanation for this model is given, as is a reason for the changes in the spacing with changes in water content of the tissue. The diffusion is attributed to thermally driven agitation of the molecules, in accordance with the Debye-Waller theory including the Gaussian distribution. The remainder of the diffusion is attributed to other scattering sources like the mineral crystallites.

Animals↗
PubMed2005

Breather-induced anomalous charge diffusion.

We present results on the diffusive motion of a charge interacting with the nonlinear dynamics of a thermalized underlying lattice. Signatures of anomalous diffusive properties are found at relatively high temperatures, where highly nonlinear excitations are present. A sublinear diffusion and a plateau appear before the standard long-time diffusion during the evolution of the mean-squared displacement and a significant degree of heterogeneity is exhibited among individual trajectories. Both properties are connected with the existence of vibrational hot spots (breather or multibreather excitations). Transport parameters of the charge are strongly affected in this case, as can be exemplified by the significant suppression of the diffusion coefficient D. The variation of D with temperature follows a stretched exponential law. The results are contrasted with those of the linearized case, in the absence of breathers. Such anomalous diffusion of a charge coupled to a thermalized lattice may be relevant in low-dimensional soft materials with strong anharmonicities, such as biomolecules, conducting polymers, etc.

Biopolymers↗
PubMed2005

Acceleration of diffusion in randomly switching potential with supersymmetry.

We investigate the overdamped Brownian motion in a supersymmetric periodic potential switched by Markovian dichotomous noise between two configurations. The two configurations differ from each other by a shift of one-half period. The calculation of the effective diffusion coefficient is reduced to the mean first passage time problem. We derive general equations to calculate the effective diffusion coefficient of Brownian particles moving in arbitrary supersymmetric potential. For the sawtooth potential, we obtain the exact expression for the effective diffusion coefficient, which is valid for the arbitrary mean rate of potential switchings and arbitrary intensity of white Gaussian noise. We find the acceleration of diffusion in comparison with the free diffusion case and a finite net diffusion in the absence of thermal noise. Such a potential could be used to enhance the diffusion over its free value by an appropriate choice of parameters.

Journal Article↗
PubMed2006

Full q-space analysis of x-ray scattering of multilamellar membranes at liquid-solid interfaces.

A method for analyzing the x-ray scattering of a stack of phospholipid membranes at the solid-liquid interface in excess water is presented. It is argued that bilayers near the substrate fluctuate less significantly than the ones away from it and, therefore, make a larger contribution to the specular reflection at the low index Bragg peaks. But the diffuse scattering due to thermal fluctuations corrupts the Bragg peaks at high angles so that the specular contribution is not clearly observable. In the midst the specular reflection and the diffuse scattering cannot be separated easily and must be analyzed simultaneously. The height-difference correlation function derived from a modified Caillé theory enables one to simulate the longitudinal and the transverse scans in the same theoretical framework to yield more reliable structural parameters. The theoretical apparatus is successfully applied to the experimental data on DOPC membranes.

Algorithms↗
PubMed1999

Contribution of vaporization and boiling to thermal-spike sputtering by ions or laser pulses.

Here we consider what, in our terminology, we designate as normal vaporization, normal boiling, and phase explosion. In the case of vaporization, one is dealing with the emission of particles (atoms or molecules) from the extreme outer surface of either a solid or liquid for any temperature exceeding 0 K. In the case of boiling, one is (at least ideally) dealing with heterogeneously nucleated bubbles which diffuse to the outer surface of a liquid or solid and then escape, the latter being possible for temperatures equal to or exceeding the boiling temperature (T(b)). In the case of phase explosion one is dealing with the consequences of what happens when a liquid approaches the thermodynamic critical temperature (T(tc) or T(c)), and massive homogeneous nucleation takes place. Although these three mechanisms have been reviewed in reasonable detail in recent work, we will here present evidence, apparently not previously considered, that boiling, whether the distance scale is atomically small (5-15 nm, as for laser-pulse impact on a metal in the absence of thermal diffusion) or much larger, has a prohibitive kinetic obstacle because it requires bubble diffusion if the bubbles are formed other than at the outer surface. That is to say, boiling will never be a significant process whether with ion or laser-pulse impact. This leaves vaporization and phase explosion as the only possible thermal-spike processes capable of expelling material from an ion- or laser-pulse bombarded surface in a significant quantity. But even with vaporization it can be shown that a kinetic obstacle, although not as severe as for boiling, will enter. The final result is that only phase explosion will normally be relevant for sufficiently short time scales.

Journal Article↗
PubMed1982

Lateral diffusion of epidermal growth factor complexed to its surface receptors does not account for the thermal sensitivity of patch formation and endocytosis.

The patching and endocytosis of EGF (epidermal growth factor) bound to A-431 cells (a human epidermoid carcinoma line) are temperature-sensitive processes which are completely inhibited at 4 degrees C. Receptor-mediated endocytosis generally occurs through coated regions, and EGF bound to its membrane receptor must diffuse laterally to these points of internalization. In this work we investigated the thermal sensitivity of the lateral diffusion of EGF receptor complexes and the thermal sensitivity of the patching and endocytosis of the hormone receptor complexes. Using the fluorescence photobleach recovery technique, we measured the lateral diffusion coefficients of a fluorescent derivative of EGF as a function of temperature. The lateral diffusion coefficient (D) increased gradually from 2.8 X 10(-10) cm2/s at 5 degrees C to 8.5 X 10(-10) cm2/s at 37 degrees C, and no phase transition was detected. Neither was a phase transition detected when we measured the diffusion coefficient of fluorescent lipid probes over this temperature range. From a calculation of the collision frequency of the occupied EGF receptors with coated regions using our measured values of D at 5 and 37 degrees C, we conclude that diffusion is not the rate-limiting step for either endocytosis or patching.

Animals↗
PubMed1996

Anomalous diffusion due to binding: a Monte Carlo study.

In classical diffusion, the mean-square displacement increases linearly with time. But in the presence of obstacles or binding sites, anomalous diffusion may occur, in which the mean-square displacement is proportional to a nonintegral power of time for some or all times. Anomalous diffusion is discussed for various models of binding, including an obstruction/binding model in which immobile membrane proteins are represented by obstacles that bind diffusing particles in nearest-neighbor sites. The classification of binding models is considered, including the distinction between valley and mountain models and the distinction between singular and nonsingular distributions of binding energies. Anomalous diffusion is sensitive to the initial conditions of the measurement. In valley models, diffusion is anomalous if the diffusing particles start at random positions but normal if the particles start at thermal equilibrium positions. Thermal equilibration leads to normal diffusion, or to diffusion as normal as the obstacles allow.

Animals↗
PubMed2002

Microsurgical DREZotomy for pain of spinal cord and Cauda equina injury origin: clinical characteristics of pain and implications for surgery in a series of 26 patients.

The result of the DREZotomy procedure used for the treatment of chronic intractable neuropathic pain caused by injuries at the T9-L4 spine level in 26 patients has been reported. For the purpose of identifying the most favorable pain pattern for DREZ surgery we retrospectively analyzed the effectiveness of surgical treatment on different forms of pain in the follow-up period of 13-50 months, 37 months on average. All pain forms were classified according to subjective sensory pain expression including the rhythm and topography of the pain. Three groups of pain were formed according to subjective sensory equivalents: pain of thermal quality (burning, boiling, baking, warm etc.), pain of mechanical-nonthermal quality (shooting, cutting, stabbing, sharp, incisive, cramping, constriction, distraction, throbbing etc.). The third group was the combination of the previous two. Success in pain relief has been defined as a 50% or greater reduction in pain after surgery such that pain no longer interferes with patient activities of daily living and sleeping pattern and no longer requires routine analgesic pain medication. Our results revealed that the pain of mechanical-nonthermal nature and intermittent rhythm, confined to segmental topography was the most responsive to the DREZ surgical treatment so that 90% patients suffering from this pain pattern experienced a good long-term pain relief (70% had complete long term pain relief). Neuropathic pain of thermal quality with the diffuse infralesional distribution and steady rhythm was the most resistant to the DREZ surgical treatment: neither patient had long-term relief of this pain pattern. In the group of patients suffering from pain consisting of combined mechanical and thermal sensory components with confined pain territory, 75% experienced a good long-term pain relief (50% had complete long-term pain relief). Immediate pain relief was obtained in 88% of patients and was long lasting in 69% of the total series. Our results pointed to confined territory, intermittent rhythm and mechanical nature of the pain as the most relevant predictors of the expected pain relief achieved by the DREZ surgery.

Adult↗
PubMed1987

Modeling optical and thermal distributions in tissue during laser irradiation.

The propagation of light energy in tissues is an important problem in phototherapy, especially with the increased use of lasers as light sources. Often a slight difference in delivered energy separates a useless, efficacious, or disastrous treatment. Methods are presented for experimental characterization of the optical properties of a tissue and computational prediction of the distribution of light energy within a tissue. A standard integrating sphere spectrophotometer measured the total transmission, Tt, total reflectance, Rt, and the on-axis transmission, Ta, for incident collimated light that propagated through the dermis of albino mouse skin, over the visible spectrum. The diffusion approximation solution to the one-dimensional (1-D) optical transport equation computed the expected Tt and Rt for different combinations of absorbance, k, scattering, s, and anisotropy, g, and by iterative comparison of the measured and computed Tt and Rt values converged to the intrinsic tissue parameters. For example, mouse dermis presented optical parameters of 2.8 cm-1, 239 cm-1, and 0.74 for k, s, and g, respectively, at 488 nm wavelength. These values were used in the model to simulate the optical propagation of the 488-nm line of an argon laser through mouse skin in vivo. A 1-D Green's function thermal diffusion model computed the temperature distribution within the tissue at different times during laser irradiation. In vitro experiments showed that the threshold temperature range for coagulation was 60 degrees-70 degrees C, and the kinetics were first order, with a temperature-dependent rate constant that obeyed an Arrhenius relation (molar entropy 276 cal/mol-degrees K, molar enthalpy 102 kcal/mol). The model simulation agreed with the corresponding in vivo experiment that a 2-s pulse at 55 W/cm2 irradiance will achieve coagulation of the skin.

Animals↗
PubMed2002

Modeling of drug release from collagen matrices.

Drug release from collagen matrices is in most cases governed by diffusion from swollen matrices but also enzymatic matrix degradation or hydrophobic drug/collagen interactions may contribute. To reduce water uptake and to prolong the release, insoluble collagen matrices have been chemically or dehydrothermally crosslinked. Assuming Fickian diffusion a one-dimensional model was developed and tested that allows description of water penetration, swelling and drug release and that may be expanded considering a subsequent erosion process or interactions. Swelling is described by a volume balance. For dry collagen matrices crosslinked by thermal treatment the existence of a moving front separating the polymer from a gel phase was considered, and a convective term induced by the volume expansion was incorporated. The resulting moving boundary problem was solved using a method based on biquadratic finite elements in both space and time that is stable, shows high accuracy, and is suitable for solving problems with a singularity at the initial time point. The model was verified for insoluble collagen matrices at different crosslinking degrees for both chemical and thermal treatment. For constant diffusion coefficients a close form of the solution was derived yielding equivalent results to the numerical approach.

Animals↗
PubMedDate not supplied

In vivo assessment of thermal damage in the liver using optical spectroscopy.

Resection is not a viable treatment option for the majority of liver cancer patients. Alternatives to resection include thermotherapies such as radio-frequency ablation; however, these therapies lack adequate intraoperative feedback regarding the degree and margins of tissue thermal damage. In this proof of principle study, we test the ability of fluorescence and diffuse reflectance spectroscopy to assess local thermal damage in vivo. Spectra were acquired in vivo from healthy canine liver tissue undergoing radio-frequency ablation using a portable fiber-optic-based spectroscopic system. The major observed spectral alterations on thermal coagulation were a red shift in the fluorescence emission peak at 480 nm, a decrease in the overall fluorescence intensity, and an increase in the diffuse reflectance from 450 to 750 nm. Spectral changes were quantified and correlated to tissue histology. We found a good correlation between the proposed spectral correlates of thermal damage and histology. The results of this study suggest that fluorescence and diffuse reflectance spectroscopy show strong potential as tools to monitor liver tissue thermal damage intraoperatively.

Animals↗
PubMed2005

Temperature dependence of interfacial fluctuations of polymerized fatty acid salt multilayers.

X-ray scattering was used to study the temperature dependence of the profile structure of polymerized 10,12-tricosadiynoic acid salt multilayers. The stacking periodicity of the multilayers was found to decrease with increasing temperature due to the conformational changes of the alkyl chains. When the samples were fully hydrated in water, the reflectivity measurement showed that the thermal fluctuations of the interfaces are enhanced with temperature, resulting in reduced ordering. Meanwhile, the diffuse scattering indicated that the thermal fluctuations renormalize the elasticity of the multilayers; both the bending and the compression moduli are reduced. Similar measurements performed in air, however, do not show this thermal enhancement although the stacking periodicity decreases in the same manner. It is implied that water might weaken the interaction between the carboxyl groups and the metal ions so that the polymerized bilayers are softened in water.

Journal Article↗
PubMed1984

Transport properties of polymer solutions. A comparative approach.

A variety of transport properties have been measured for solutions of the water soluble polymer poly(ethylene oxide)(PEO) with molecular weights ranging from 200 to 14,000, and volume fractions ranging from 0-80%. The transport properties are thermal conductivity, electrical conductivity at audio frequencies (in solutions containing dilute electrolyte), and water self-diffusion. These data, together with dielectric relaxation data previously reported, are amenable to analysis by the same mixture theory. The ionic conductivity and water self-diffusion coefficient, but not the thermal conductivity, are substantially smaller than predicted by the Maxwell and Hanai mixture relations, calculated using the known transport properties of pure liquid water. A 25% (by volume) solution of PEO exhibits an average dielectric relaxation frequency of the suspending water of one half that of pure water, with clear evidence of a distribution of relaxation times present. The limits of the cumulative distribution of dielectric relaxation times that are consistent with the data are obtained using a linear programming technique. The application of simple mixture theory, under appropriate limiting conditions, yields hydration values for the more dilute polymer solutions that are somewhat larger than values obtained from thermodynamic measurements.

Biological Transport↗