title: Pressure modulates the self-cleavage step of the hairpin ribozyme.
abstract: The ability of certain RNAs, denoted as ribozymes, to not only store genetic information but also catalyse chemical reactions gave support to the RNA world hypothesis as a putative step in the development of early life on Earth. This, however, might have evolved under extreme environmental conditions, including the deep sea with pressures in the kbar regime. Here we study pressure-induced effects on the self-cleavage of hairpin ribozyme by following structural changes in real-time. Our results suggest that compression of the ribozyme leads to an accelerated transesterification reaction, being the self-cleavage step, although the overall process is retarded in the high-pressure regime. The results reveal that favourable interactions between the reaction site and neighbouring nucleobases are strengthened under pressure, resulting therefore in an accelerated self-cleavage step upon compression. These results suggest that properly engineered ribozymes may also act as piezophilic biocatalysts in addition to their hitherto known properties.
authors.affiliation: Physikalische Chemie I-Biophysikalische Chemie, Fakultät für Chemie und Chemische Biologie, TU Dortmund, Otto-Hahn-Strasse 4a, Dortmund 44227, Germany.
authors.forename: Caroline
authors.initials: C
authors.lastname: Schuabb
authors.affiliation: Lehrstuhl für Theoretische Chemie, Ruhr-Universität Bochum, Bochum 44780, Germany.
authors.forename: Narendra
authors.initials: N
authors.lastname: Kumar
authors.affiliation: Physikalische Chemie I-Biophysikalische Chemie, Fakultät für Chemie und Chemische Biologie, TU Dortmund, Otto-Hahn-Strasse 4a, Dortmund 44227, Germany.
authors.forename: Salome
authors.initials: S
authors.lastname: Pataraia
authors.affiliation: Lehrstuhl für Theoretische Chemie, Ruhr-Universität Bochum, Bochum 44780, Germany.
authors.forename: Dominik
authors.initials: D
authors.lastname: Marx
authors.affiliation: Physikalische Chemie I-Biophysikalische Chemie, Fakultät für Chemie und Chemische Biologie, TU Dortmund, Otto-Hahn-Strasse 4a, Dortmund 44227, Germany.
authors.forename: Roland
authors.identifier: 0000-0002-3512-6928
authors.initials: R
authors.lastname: Winter
mesh_terms: D001483:Base Sequence; D055162:Biocatalysis; D031541:Fluorescence Resonance Energy Transfer; D006860:Hydrogen Bonding; D062105:Molecular Docking Simulation; D009690:Nucleic Acid Conformation; D011312:Pressure; D011336:Probability; D016337:RNA, Catalytic / Q000737:chemistry / Q000378:metabolism*; D013816:Thermodynamics
chemical_list: D016337:RNA, Catalytic; C418481:hairpin ribozyme