Biomolecular recognition of antigens and epitopes by antibodies is a fundamental event in the initiation of immune response and plays a central role in a variety of biochemical processes. Peptide binding requires, in many cases, presentation of the peptides at interfaces, such as protein surfaces, cellular membranes, and synthetic polymer surfaces. We describe a novel molecular system in which interactions between antibodies and peptide epitopes displayed at a biomimetic membrane interface can be detected through induction of visible, rapid color transitions. The colorimetric assembly consists of a phospholipid/polydiacetylene matrix anchoring a hydrophobic peptide displaying the epitope at its N-terminus. The colorimetric transitions observed in the assembly, corresponding to perturbation of the polydiacetylene framework, are induced only upon recognition of the displayed epitope by its specific antibody present in the aqueous solution. Significantly, the color changes occur after a single mixing step, without further chemical reactions or enzymatic processing. The new molecular system could be utilized for studying antigen-antibody interactions and peptide-protein recognition, epitope mapping, and rapid screening of biological and chemical libraries.
Non-covalent compositional assemblies, made of monomeric mutually catalytic molecules, constitute an alternative to alphabet-based informational biopolymers as a mechanism of primordial inheritance. Such assemblies appear implicitly in many "Metabolism First" origin of life scenarios, and more explicitly in the Graded Autocatalysis Replication Domain (GARD) model [Segréet al. (2000). Proc. Natl Acad. Sci. U.S.A.97, 4112-4117]. In the present work, we provide a detailed analysis of the quantitative molecular roots of such behavior. It is demonstrated that the fidelity of reproduction provided by a newly defined heritability measure eta(*)(s), strongly depends on the values of molecular recognition parameters and on assembly size. We find that if the catalytic rate acceleration coefficients are distributed normally, transfer of compositional information becomes impossible, due to frequent "compositional error catastrophes". In contrast, if the catalytic acceleration rates obey a lognormal distribution, as actually predicted by a statistical formalism for molecular repertoires, high reproduction fidelity is obtained. There is also a clear dependence on assembly size N, whereby maximal eta is seen in a narrow range around N approximately 3.5 N(G)/lambda, where N(G)is the size of the primordial molecular repertoire and lambda is a molecular interaction statistical parameter. Such relationships help define the physicochemical conditions that could underlie the early steps in pre-biotic evolution.
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