Langmuir膜及LB膜中的金属参与

本文主要介绍了金属离子与Langmuir膜及LB膜相互作用中静电、配位等作用方式及其对膜相态和分子二维排列的影响。在此基础上探讨了Langmuir膜对金属离子的识别与传感。以Langmuir膜和LB膜为二维模板诱导无机盐定向生长作为金属/单分子膜结合的重要应用在文中也进行了讨论。通过举例展示了金属离子参与的Langmuir膜和LB膜催化有机反应的特点。最后对金属参与的Langmuir膜和LB膜在功能化和器件化等方面的研究也作了论述， 并通过介绍金属螯合类脂分子的Langmuir膜在蛋白质等生物大分子界面定向聚集研究中的应用表明了金属参与的Langmuir膜及LB 膜在生命科学研究中的意义。全文贯穿了金属结合调节Langmuir膜和LB膜组装结构以及通过金属结合导入功能基团进行有序组装的思想。     

Langmuir-Blodgett films of a Mo-blue nanoring [Mo(142)O(429)H(10)(H(2)O)(49)(CH(3)CO(2))(5)(CH(3)CH(2)CO(2))](30)(-) (Mo(142)) by the semiamphiphilic method

Langmuir monolayers and LB films of the ring-shaped mixed-valence polyoxomolybdate [Mo142O429H10(H2O)49(CH3CO2)5(CH3CH2CO2)](30-) (Mo142) dissolved in the aqueous subphase have been successfully fabricated by using the adsorption properties of a DODA monolayer. Infrared and ultraviolet-visible spectroscopy of the LB films indicates that Mo142 and DODA molecules are incorporated within these LB films. X-ray reflectivity experiments indicate that the LB films exhibit a well-defined lamellar structure formed by bilayers of DODA molecules alternating with monolayers of Mo142. Using behenic acid-modified hydrophobic quartz substrate is critical for the formation of the well-defined lamellar structure. From the values of the periodicity obtained by these experiments it is clear that the Mo142 clusters lie flat along the charged organic layers. AFM images also showed the flat and homogeneous films on the quartz substrates treated with behenic acid. Cyclic voltammograms of Mo142-LB films deposited on ITO substrates showed quasi-reversible oxidation/reduction waves with positive shift of the potential compared to the case of solution.     

Interaction of small amounts of bovine serum albumin with phospholipid monolayers investigated by surface pressure and atomic force microscopy

The influence of small amounts of bovine serum albumin (BSA) (nM concentration) on the lateral organization of phospholipid monolayers at the air-water interface and transferred onto solid substrates as one-layer Langmuir-Blodgett (LB) films was investigated. The kinetics of adsorption of BSA onto the phospholipid monolayers was monitored with surface pressure isotherms in a Langmuir trough, for the zwitterionic dipalmitoylphosphatidyl ethanolamine (N,N-dimethyl-PE) and the anionic dimyristoylphosphatidic acid (DMPA). A monolayer of N,N-dimethyl-PE or DMPA incorporating BSA was transferred onto a solid substrate using the Langmuir-Blodgett technique. Atomic force microscopy (AFM) images of one-layer LB films displayed protein-phospholipid domains, whose morphology was characterized using dynamic scaling theories to calculate roughness exponents. For DMPA-BSA films the surface is characteristic of self-affine fractals, which may be described with the Kardar-Parisi-Zhang (KPZ) equation. On the other hand, for N,N-dimethyl-PE-BSA films, the results indicate a relatively flat surface within the globule. The height profile and the number and size of globules varied with the type of phospholipid. The overall results, from kinetics of adsorption on Langmuir monolayers and surface morphology in LB films, could be interpreted in terms of the higher affinity of BSA to the anionic DMPA than to the zwitterionic N,N-dimethyl-PE. Furthermore, the effects from such small amounts of BSA in the monolayer point to a cooperative response of DMPA and N,N-dimethyl-PE monolayers to the protein.     

Influence of ion transfer kinetics on the composition of langmuir-blodgett films

The effect of ion transfer kinetics on the ionic composition of Langmuir-Blodgett (LB) films formed by charged monolayers is analyzed. The dynamic regimes of the LB deposition are considered by taking into account the competitive adsorption of several counterions having different diffusivities, valences, binding constants, and bulk concentrations. It is shown that the composition of deposited films should change with the deposition rate. At lower deposition rates, the ion with higher binding constant is more represented within the deposited monolayer in comparison to the higher deposition rates. At low deposition rates, the ratio of counterion amounts within the LB films is the same as that within the floating monolayer excluding the ions within the diffuse layer. At high deposition rates, the ratio of the counterion amounts is the same as that within the floating monolayer when the potential-determining counterions within the diffuse layer are taken into account.     

Effect of thickness and monolayer location on thermostability of metal stearate LB films studied by FT-IR reflection—absorption spectroscopy

LB films of Cd and Ca stearates with 1, 3, 9, and 21 monolayers were fabricated on silver-coated glass slides. 9-Monolayer LB films of Cd and Ca salts of deuterated stearic acid, in which the 1st, 5th, or 9th layer was replaced by 1 monolayer of undeuterated analogues, were also prepared on the above substrates. Temperature dependences of Fourier transform infrared (FT-IR) reflection—absorption (RA) spectra were examined for these LB films in the range 31–140°C. At room temperature, the hydrocarbon chains in these LB films were in a well-ordered state with a high degree of perpendicular orientation to the substrate. However, they became disordered at elevated temperatures. These order-disorder phase transition temperatures were dependent on the film thickness, to a small degree in the Cd stearate LB film (102–108°C), but to a large degree in the Ca stearate LB film (103–129°C). In the latter LB film, the effect of dehydration was inferred. The degree of disorder at high temperatures was dependent on the film thickness and the location of monolayer in the 9-monolayer LB films. This result is discussed in terms of the internal pressure within the LB film.     

Surface enhanced resonance Raman scattering imaging of Langmuir-Blodgett monolayers of bis (benzimidazo) thioperylene.

The synthesis, spectroscopic characterization and surface-enhanced spectroscopy of a new electro active organic material bis (benzimidazo) thioperylene (Monothio BZP) are reported. Langmuir monolayers of Monothio BZP were successfully formed on water subphase and characterized by the pi-A surface-pressure area isotherm. Langmuir-Blodgett (LB) monomolecular layers of Monothio BZP were fabricated onto glass substrates and onto silver island films for surface-enhanced spectroscopic studies. The results of surface-enhanced resonance Raman scattering (SERRS), SERRS imaging and surface-enhanced fluorescence (SEF) studies for Monothio BZP LB monolayers are reported. Raman imaging (global imaging and point-by-point mapping) of the SERRS signal for a single monomolecular layer on silver islands were obtained using the 514.5 nm laser line. The SERRS imaging permits a visualization of the variation of the SERRS intensity across of the rough metal surface. The SEF was recorded for the excimer emission of aggregates in the LB film. The distance dependence and the enhancement factor of SEF were determined using fatty acid spacing layers. A temperature dependence study of the LB monolayer SERRS and SEF spectra was carried out between -190 degrees and + 200 degrees C confirming the thermal stability of the LB monolayer on silver. The specificity and the sensitivity of SERRS signal on metal island films was probed using mixed LB films with 0.01% molecular ratio of Monothio BZP in Arachidic Acid (AA). The micro-Raman SERRS spectra from ca. 10(-3) attomole of the dye were recorded.     

Structuring of tricarbocyanine dye molecules in Langmuir-Blodgett films

The problems of formation of stable Langmuir monolayers containingN-sulfopropyl substituted thiatricarbocyanine dyes are considered: the effects of the composition of the mixture applied on the surface of an aqueous subphase and of the extent of compression of the monolayer on processes of ordering of molecular structure. Dyes are introduced into complex monolayers at the water-air interface and then are transferred on solid substrates as multilayered Langmuir-Blodgett (LB) films. For the first time the formation of J-aggregates has been observed for two tricarbocyanine dyes. The structure of J-aggregates depends on the composition of the mixture and the value of the constant pressure at which the transfer occurs. LB films of J-aggregated dyes are optically anisotropic, which is related to the fact that they are formed in the monolayer on the surface and there is no interlayer aggregation during the transfer to substrates. Heterodimers are formed in complex monolayers containing oppositely charged ions of dyes.Translated fromIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 7, pp. 1278–1283, July, 1995.The work was partially financially supported by the Foundation for Basic Research of the State Committee on Science and Technologies of the Ukraine (Project No. 2.2/48 Normal').     

Langmuir and Langmuir-Blodgett films of N-(4-octadecyloxy-2-hydroxybenzylidene) derivatives of amino acids

Langmuir and Langmuir-Blodgett monolayers of N-(4-octadecyloxy-2-hydroxybenzylidene) derivatives of glycine, tyrosine, and phenylalanine were studied using pi-A isotherms and photoelastic modulated FTIR (PEM-FTIR). Based on compression modulus and interaction parameters, mixed monolayers of these compounds with stearylamine (SAM) showed well-organized monolayers compared to mixed systems with stearic acid (SA) and stearyl alcohol (SAL). The pure amphiphiles exhibited fairly well-ordered packing in the films, and in the mixtures, the ordering increased and showed a triclinic packing arrangement. For the phenylalanine amphiphile the packing showed slight disorder compared to the other two compounds. Surface properties of the LB films of these compounds on solid substrates were analyzed using static and dynamic contact angles of a series of liquids. The surface tension of coated substrates reflected clearly the highly acidic character. Fluidlike monolayers having a molecularly rough surface indicated high wettability for n-alkanes. In contrast, the monolayer containing well-ordered, well-packed alkyl chains indicated low wettability and small hysteresis.     

A comparative Langmuir-Blodgett study on a set of covalently linked porphyrin-based amphiphiles: a detailed atomic force microscopic study

A set of covalently linked phenyl-amidophenyl-substituted porphyrin amphiphiles with n-C15H31 tails have been synthesized and completely characterized. These amphiphiles form good Langmuir-Blodgett (LB) films at the air/water interface. Mean molecular areas for the series were measured from the isotherms and found to increase as the number of aliphatic chains increased from one to four. No influence of the subphase pH was observed on the isotherms. LB films can be transferred successfully onto different solid surfaces. The LB films were characterized using tapping mode atomic force microscopy (AFM). Bis-, tris-, and tetra-substituted porphyrins were found to be fairly good film-forming amphiphiles, whereas irregular aggregates were seen in the case of the monosubstituted porphyrin amphiphile. Multilayers were also formed with tetra-substituted amphiphiles on mica. Detailed AFM studies of tetra-substituted amphiphiles have been carried out to investigate the effect of preparation procedure and solid substrates on film formation and transfer. The absorption and fluorescence spectra for the amphiphiles in solution and LB films deposited onto mica and glass were recorded, which demonstrated the successful transfer of LB films onto the substrates and provided more information about the arrangement of porphyrin molecules within the LB films. For comparison, self-assembled monolayers (SAMs) and the cast thin films of the amphiphiles were prepared and characterized.     

Effect of Metal Ions on the Formation and Properties of Monolayers and Nanosized Langmuir-Blodgett Films Based on Diphilic Aminomethylated Calix[4]resorcinarenes

The behavior of the monolayers of three diphilic aminomethylated calix[4]resorcinarene (CRA) derivatives on the surface of a pure aqueous subphase and subphase containing copper(II), nickel(II), europium(III), terbium(III), and lanthanum(III) ions was investigated. The monolayer transfer to the quartz and single-crystal silicon substrates was accomplished by the Langmuir-Blodgett (LB) technique. The films were studied by ellipsometry and mass-spectrometry. Metal ions were found to exert effect on the limit area per one CRA molecule in the monolayer, on the surface collapse pressure and transfer coefficient of monolayer, and on the thickness and refractive index of the CRA-based LB films.     

Assembly of oriented zeolite monolayers and thin films on polymeric surfaces via hydrogen bonding

The b-oriented monolayers of microsized silicalite-1 crystals have been manually assembled on glass plate supported poly(ethylene oxide) (PEO), poly(vinyl alcohol) (PVA), chitosan, and poly(methyl methacrylate) (PMMA) thin films via hydrogen bonding with much enhanced binding strength and satisfactory degrees of coverage and close packing. The exerted pressure and rubbing time in the manual assembly do not affect the binding strength of the silicalite-1 monolayer on the glass plate supported polymeric film. This manual assembly has been further applied to fabricate zeolite monolayers on commercially available Plexiglas surfaces and b-oriented multilayered films of silicalite-1 crystals on glass plates. The assembly method established in this study provides a feasible way to produce zeolite monolayers on polymer-modified solid substrates and Plexiglas and to fabricate zeolite-polymer composite membranes by means of the layer-by-layer technique.     

Molecular recognition of cytosine- and guanine-functionalized nucleolipids in the mixed monolayers at the air-water interface and Langmuir-Blodgett films

Molecular recognition of mixed nucleolipids of 1-(2-octadecyloxycarbonylethyl)cytosine and 7-(2-octadecyloxycarbonylethyl)guanine in the monolayers at the air-water interface and Langmuir-Blodgett (LB) films has been investigated in detail using surface pressure/potential-area isotherms, infrared reflection-absorption spectroscopy (IRRAS), and Fourier transform infrared (FTIR) transmission spectroscopy, respectively. Prior to molecular recognition, the cytosine moieties in the monolayer were hydrogen bonded with an almost flat-on orientation, the alkyl chains were uniaxially oriented with respect to the film normal, the guanine moieties in the monolayer were stacked probably through pi-pi interaction with an end-on orientation, and the C-C-C planes of the alkyl chains were preferentially oriented parallel to the water surface. In the monolayer of equimolar mixture, molecular recognition between the cytosine and guanine moieties occurred together with the ring planes of base pairing and the C-C-C planes of the alkyl chains favorably oriented parallel to the water surface. The guanine moieties underwent an orientation change from an end-on mode before molecular recognition to a flat-on one after molecular recognition. The base pairing between the cytosine and guanine moieties in the monolayers was achieved since the N7-substituted guanine derivatives suppressed the formation of guanine tetramers. Both the IRRAS spectra of the monolayers and the FTIR spectra of the LB films presented the exact sites in the cytosine and guanine moieties for the formation of triple hydrogen bonds. The base pairing resulted in a change in molecular orientation and interaction, and the corresponding LB film exhibited a different phase transition behavior from a typical crystal transition for the cytosine-functionalized nucleolipids and an analogous glass transition for the guanine-functionalized nucleolipids. The thermal stability of the mixed LB film was improved in comparison to the LB films of pure components.     

In situ observation of gamma-Fe2O3 nanoparticle adsorption under different monolayers at the air/water interface

We studied the adsorption of gamma-Fe 2O 3 nanoparticles from an aqueous solution under different charged Langmuir monolayers (stearic acid, stearyl alcohol, and stearyl amine). The aqueous subphase was composed of a colloidal suspension of gamma-Fe 2O 3 nanoparticles. The average hydrodynamic diameter of the nanoparticles measured by dynamic light scattering measurements was 16 nm. The observed zeta potential of +40 mV (at pH 4) results in a long-term stability of the colloidal dispersion. The behavior of the different monolayer/nanoparticle composites were studied with surface pressure/area (pi/ A) isotherms. The adsorption of the nanoparticles under the different monolayers induced an expansion of the monolayers. These phenomena depended on the charge of the monolayers. After the Langmuir/Blodgett transfer on glass substrates, the nanoparticle/monolayer composite films were studied by means of UV-vis spectroscopy. The spectra pointed to increasing adsorption of the nanoparticles with increasing electronegativity of the monolayers. On the basis of these results, we studied the in situ adsorption of nanoparticles under the different monolayers by X-ray reflectivity measurements. Electron density profiles of the liquid/gas interfaces were obtained from the X-ray reflectivity data. The results gave clear evidence for the presence of electrostatic interaction between the differently charged monolayers and the positively charged nanoparticles. While the adsorption process was favored by the negatively charged stearic acid monolayer, the positively charged layer of stearyl amine prevented the formation of ultrathin nanoparticle layers.     

Langmuir-Blodgett-Kuhn and self-assembled films of asymmetrically substituted poly(paraphenylene)

Asymmetrically substituted poly(paraphenylene) (PhPPP) with hydrophilic and hydrophobic side chains was investigated. The polymer behavior at the air-water interface was studied on the basis of surface pressure-area (pi-A) isotherms and compression/expansion hysteresis measurements. PhPPP can form stable monolayers with an area per repeat unit of A=0.20+/-0.02 nm2 and a collapse pressure in the range of pi=25 mN/m. Then, Langmuir-Blodgett-Kuhn (LBK) films of PhPPP were prepared by horizontally and vertically transferring the Langmuir monolayers onto hydrophilic solid substrates at pi=12 mN/m. Cross-section analysis of the AFM tapping-mode topography images of a single transferred monolayer reveals a thickness of d0=0.9+/-0.1 nm. Taking into account the obtained monolayer thickness, curve-fitting calculations of angular scan data of LB monolayers measured using surface plasmon resonance (SPR) spectroscopy lead to a value for the refractive index of n=1.78+/-0.02 at lambda=632.8 nm. Next, the spontaneous formation of a PhPPP monolayer by adsorption from solution was studied ex situ by atomic force microscopy and UV-vis spectroscopy and in situ by using SPR spectroscopy. Stable self-assembled monolayers of PhPPP can be formed on hydrophilic surfaces with a thickness similar to that of the monolayer obtained using the LB method. The characterization results confirmed the amphiphilic character and the self-assembly properties of PhPPP, as well as the possibility of preparing homogeneous monolayer and multilayer films.     

Aggregation and photoisomerization of amphiphilic crown-ether styryl dye in monolayers at the interface

The molecules oftrans-isomer of styryl dye1a, containing the benzo-18-crown-6 moiety and the methoxybenzothiazole residue with theN-octadecyl substituent, were shown to form stable, highly ordered monolayers at the water/air interface. Increasing the surface pressure of the monolayer results in the formation of the H-aggregated molecules of compound1a. The H-aggregates tend to dissociate to the monomerictrans-form, when the monolayer forms in the Langmuir-Blodgett film (LB film). The light irradiation of the LB films leads to the partially reversibletrans-cis-photoisomerization of compound1a, whose efficiency is much lower than that observed in an acetonitrile solution of1a. The aggregation of cis-1a isomers in the LB film is suggested to hamper the reversecis-trans-isomerization. The aggregation oftrans-1a molecules in the LB films does not occur in air, but, after dipping in an aqueous solution, molecules of the LB film slowly form J-aggregates. A model of the structural organization oftrans-1a molecules in the LB films was proposed.Translated fromIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 10, pp. 2490–2496, October, 1996.     

Resorcinol calixarenes (resorcarenes): Langmuir-Blodgett films and optical properties

Specially synthesized amphiphilic resorcinol calixarene (resorcarene 2) molecules have been deposited as Langmuir-Blodgett (LB) films on a variety of substrates including hydrophobically treated glass slides, silicon and gold-coated glass slides. A value of 1.9 nm² is obtained for the area per molecule from measurements of pressure/area isotherms of the floating layer. Optical absorption studies within the ultraviolet-visible frequency region have been performed on these molecules in both LB films and in solution of resorcarene 2 in chloroform, containing 10% ethanol. Molecular aggregation in the form of dimerization is believed to take place during film formation. Further analysis has been carried out for Langmuir-Blodgett films of resorcarene 2 by using Fourier transform infra-red spectroscopy, low-angle X-ray diffraction and surface plasmon resonance (SPR) techniques. The monolayer thickness of 1.6 nm found from SPR measurements is consistent with that from other experimental observations.     

Acidichromism in the Mixed Langmuir—Blodgett Films of Stearic Acid with a Carbazole—containing Schiff Base

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Thermodynamic characteristics and Langmuir-Blodgett deposition behavior of mixed DPPA/DPPC monolayers at air/liquid interfaces

The role of dipalmitoylphosphatic acid (DPPA) as a transfer promoter to enhance the Langmuir-Blodgett (LB) deposition of a dipalmitoylphosphatidylcholine (DPPC) monolayer at air/liquid interfaces was investigated, and the effects of Ca2+ ions in the subphase were discussed. The miscibility of the two components at air/liquid interfaces was evaluated by surface pressure-area per molecule isotherms, thermodynamic analysis, and by the direct observation of Brewster angle microscopy (BAM). Multilayer LB deposition behavior of the mixed DPPA/DPPC monolayers was then studied by transferring the monolayers onto hydrophilic glass plates at a surface pressure of 30 mN/m. The results showed that the two components, DPPA and DPPC, were miscible in a monolayer on both subphases of pure water and 0.2 mM CaCl2 solution. However, an exception occurs between X(DPPA)=0.2 and 0.5 at air/CaCl2-solution interface, where a partially miscible monolayer with phase separation may occur. Negative deviations in the excess area analysis were found for the mixed monolayer system, indicating the existence of attractive interactions between DPPA and DPPC molecules in the monolayers. The monolayers were stable at the surface pressure of 30 mN/m for the following LB deposition as evaluated from the area relaxation behavior. It was found that the presence of Ca2+ ions had a stabilization effect for DPPA-rich monolayers, probably due to the association of negatively charged DPPA molecules with Ca2+ ions. Moreover, the Ca2+ ions may enhance the adhesion of DPPA polar groups to a glass surface and the interactions between DPPA polar groups in the multilayer LB film structure. As a result, Y-type multilayer LB films containing DPPC could be fabricated from the mixed DPPA/DPPC monolayers with the presence of Ca2+ ions.     

Two-dimensional arrays of amphiphilic Zn2+-cyclens for guided molecular recognition at interfaces

The sterically guided molecular recognition of nucleobases, phosphates, adenosine, and uridine nucleotides on Langmuir monolayers and Langmuir-Blodgett monolayers of amphiphilic mono- or bis(Zn2+-cyclen)s assembled on thiolated surfaces was investigated. The stepwise selective binding of metal ions, uracil, or phosphate by dicetyl cyclen monolayers with variously tuned structures at the air/water interface was corroborated by the measurements of the corresponding LB films deposited onto quartz crystals. Two types of recognition surfaces were fabricated from Zn2+-dicetyl cyclen. The surface covered with a complex preformed in the Langmuir monolayer was capable both of imide and of phosphate binding. The similar complex formed directly in an LB film on thiolated gold was inactive with respect to imide. The surface plasmon resonance measurements evidenced the stepwise assembly of complementary nucleotides on SAM/LB templates through consecutive phosphate-Zn2+-cyclen coordination. Base pairing between nucleotides resulted in a formation of A-U bilayers comprising two complementary monolayers. Finally, we report on SAM/LB patterns designed for divalent molecular recognition of uridine phosphate by amphiphilic bis(Zn2+-cyclen).     

Equilibrium structure and dynamics of (2R, 3R)-(+)-bis(decyloxy)succinic acid at the air-water interface

A twin-tailed, twin-chiral fatty acid, (2R,3R)-(+)-bis(decyloxy)succinic acid was synthesized and its two dimensional behavior at the air-water interface was examined. The pH of the subphase had a profound effect on the monolayer formation. On acidic subphase, stable monolayers with increased area per molecule due to hydrogen bonding and bilayers at collapse pressures were observed. Highly compressible films were formed at 40 degrees C, while stable monolayers with increased area were observed at sub-room temperatures. Langmuir monolayers formed on subphases containing 1 mM ZnCl2 and CaCl2 revealed two dimensional metal complex formation with Zn2+ forming a chelate-type complex, while Ca2+ formed an ionic-type complex. Monolayers transferred from the condensed phase onto hydrophilic Si(100) and quartz substrates revealed the formation of bilayers through transfer-induced monolayer buckling. Compression induced crystallites in 2D from monolayers and vesicle-like supramolecular structures from multilayers were the noted LB film characteristics, adopting optical imaging and electron microscopy. The interfacial monolayer structure studied through molecular dynamics simulation revealed the order and packing at a molecular level; monolayers adsorbed at various simulated specific areas of the molecule corroborated the (pi-A) isotherm and the formation of a hexagonal lattice at the air-water interface.