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Structure and Dynamics of Oligonucleotides in the Gas Phase
Author(s) -
Arcella Annalisa,
Dreyer Jens,
Ippoliti Emiliano,
Ivani Ivan,
Portella Guillem,
Gabelica Valérie,
Carloni Paolo,
Orozco Modesto
Publication year - 2015
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201406910
Subject(s) - oligonucleotide , millisecond , molecular dynamics , vaporization , nanosecond , picosecond , chemical physics , chemistry , gas phase , ionization , mass spectrometry , electrospray ionization , ion , ab initio , nucleic acid , computational chemistry , physics , quantum mechanics , dna , laser , biochemistry , organic chemistry , chromatography
By combining ion‐mobility mass spectrometry experiments with sub‐millisecond classical and ab initio molecular dynamics we fully characterized, for the first time, the dynamic ensemble of a model nucleic acid in the gas phase under electrospray ionization conditions. The studied oligonucleotide unfolds upon vaporization, loses memory of the solution structure, and explores true gas‐phase conformational space. Contrary to our original expectations, the oligonucleotide shows very rich dynamics in three different timescales (multi‐picosecond, nanosecond, and sub‐millisecond). The shorter timescale dynamics has a quantum mechanical nature and leads to changes in the covalent structure, whereas the other two are of classical origin. Overall, this study suggests that a re‐evaluation on our view of the physics of nucleic acids upon vaporization is needed.