本研究探討由合成或天然之聚電解質(polyelectrolytes)與具相反電荷之單鏈界劑分子，於空氣-溶液界面上所形成的吸附膜，並藉由改變聚電解質及界劑之性質，進而探討吸附膜之形成機制、流變性質和表面型態等。
本研究首先以聚丙烯酸(polyacrylic acid)與直鏈烷基三甲基溴化胺(alkyltri-methylammonium bromides)之混合溶液，探討界劑分子之疏水性質對吸附行為及吸附膜之流變性質的影響。實驗結果顯示，界劑之碳氫鏈越長，表面彈性(surface elasticity)也越高；且當界劑濃度接近臨界微胞濃度時，表面彈性曲線有兩個區域最大值，分別是因為於表面形成聚電解質及界劑分子之聚集體，及多層聚集體於氣-液界面形成之結果。
因聚電解質及界劑分子溶液中靜電之吸附能障，使界劑較慢吸附至氣-液界面。因此，本研究嘗試以聚二丙烯基二甲基氯化銨(poly(diallyldimethylammonium chloride))及十二烷基硫酸鈉(sodium dodecyl sulfate)之氯化鈉水溶液探討溶液離子強度對吸附行為的影響。當溶液的離子強度增強，因為吸附速率的增加，也使得吸附層的結構及流變性質產生很大的改變。當溶液接近電中性時，表面流變性質主要會受到存在於吸附層的微聚集體所影響；故我們以三種不同的溶液型態，藉由壓縮及擴張氣-液界面，以所得之表面張力進行探討。實驗結果發現，均勻溶液所得之表面張力為正弦震盪，其餘兩溶液之結果則偏離了正弦震盪，並可以總諧波失真參數(total harmonic distortion parameter)來表示。
本研究依據合成聚電解質及界劑溶液所得之理論及實驗結果後，進而探討較為複雜的天然聚電解質及界劑溶液之系統；由於DNA為具有特殊之雙螺旋結構的去氧核醣核酸，故為本研究天然聚電解質的最佳選擇，且DNA及界劑溶液系統之研究也將為本論文的核心。
首先，本研究必須先了解線性之小牛胸腺DNA與十六烷基三甲基溴化胺於溶液表面之相互作用，並藉由改變不同之DNA或界劑濃度，探討其吸附動力學。實驗結果顯示，當DNA濃度較低時，由動態表面張力曲線可發現有相轉換的現象，即在某張力值有一兩相共存區，並藉由其他量測方法可知，形成吸附層之機制大約可分為四個階段。
由線性DNA及不同鏈長之界劑的實驗結果分析發現，DNA及界劑分子之複合體的形成不只是因為兩分子間的靜電吸引力，也包含了界劑疏水基及DNA鹼基對間的相互作用力。
最後，為了解DNA結構與DNA/界劑吸附層之流變性質的關係，本研究以線性及質體DNA之溶液進行探討。DNA分子的大小、結構及有效電荷會促使其生成不同表面活性的DNA/界劑複合體，並對吸附層的流變性質產生很大的改變。

This dissertation focusses on two general systems of interest – adsorption films formed by synthetic and natural polyelectrolytes with oppositely charged single chained surfactants at the liquid/gas interface. The surface properties of these polyelectrolyte/surfactant adsorption films were studied by several experimental techniques in order to investigate the mechanism of adsorption layer formation, its rheological properties, and morphology depending on various system parameters, such as surfactant hydrophobicity, solution ionic strength, bulk and surface composition, nature and molecular structure of polyelectrolyte.
First, the influence of surfactant hydrophobicity on the adsorption kinetics and rheological properties of mixed solutions of polyacrylic acid and alkyltrimethylammonium bromides was examined. It was found that the dynamic surface elasticity exhibited non-monotonic behaviour for all the investigated solutions and displayed two local maxima at surfactant concentrations close to the critical micelle concentration. The first maximum was connected with the aggregate formation in the surface layer while the second maximum occurred simultaneously with a multilayer formation at the gas-liquid interface. The increase of the surfactant hydrocarbon chain length caused the formation of a more rigid adsorption layer, characterized by a higher surface elasticity.
The slow adsorption kinetics, typically observed for oppositely charged polyelectrolyte/surfactant systems due to the electrostatic adsorption barrier, urged us to investigate the impact of the solution ionic strength using as an example solutions of poly(diallyldimethylammonium chloride) with sodium dodecyl sulfate in presence of sodium chloride. The increase of the solution ionic strength resulted in strong changes of the surface dilatational rheological properties and, thereby, of the interfacial layer structure due to the large increase of the adsorption rate. Close to the charge neutralization point, however, the surface rheological properties were mainly influenced by the presence of micro-aggregates embedded in the adsorption layer. In this case, the effects of changing of the sample history on the rheological behavior and heterogeneity of the interface were further investigated. The appearance of non-linear effects and deviation from pure sinusoidal oscillations of the surface tension was quantitatively characterized by the total harmonic distortion parameter.
Relying on the body of theoretical and experimental results regarding to a relatively simple model system of synthetic polyelectrolyte/surfactant solutions, the further study was devoted to a more complex system, containing a natural polyelectrolyte of special importance. Due to its specific double-helix structure deoxyribonucleic acid proved to be an excellent candidate for our purpose. The results obtained for DNA/surfactant solutions are discussed in details and form a core of this thesis.
First, the main attention was paid to the interaction of linear calf thymus DNA with oppositely charged cethyltrimetylammonium bromide at the solution surface. Measurements of the kinetic dependencies of the surface properties as a function of DNA and surfactant concentration gave a possibility to discover the time intervals corresponding to coexistence of two-dimensional phases in the surface layer, which has not been detected previously for polyelectrolyte/surfactant solutions. The multi-technique approach together with the calculations of the adsorption kinetics allowed elucidation of the nature of coexisting surface phases and distinguishing four main steps of the adsorption layer formation mechanism.
Afterward, the results obtained for linear DNA and surfactants with different chain lengths were analyzed, providing a strong support to the idea that the formation of the DNA/surfactant complexes is caused by not only electrostatic attractions but also hydrophobic interactions between hydrophobic surfactant tail and nucleobases of DNA exposed in the major groove of the double helix.
Finally, in order to investigate the correlation between the DNA molecular structure and the rheological behavior of DNA/surfactant adsorption layers, measurements of the dynamic surface properties of the solutions containing linear and plasmid DNA were carried out. The significant difference in the size of macromolecules, their conformation, and thereby their effective charge led to the formation of DNA/surfactant complexes of different surface activity and caused drastic changes in the rheology of the adsorption layer.

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