Probing Solvation-Induced Structural Changes in Conformationally Flexible Peptides: IR Spectroscopy of Gly3H+•(H2O)

Fischer, Kaitlyn C.; Voss, Jonathan M.; Zhou, Jia; Garand, Etienne

doi:10.1021/acs.jpca.8b07546

Title: Probing Solvation-Induced Structural Changes in Conformationally Flexible Peptides: IR Spectroscopy of Gly₃H⁺•(H₂O)

Journal Article · Fri Sep 21 00:00:00 EDT 2018 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.8b07546· OSTI ID:1513761

Fischer, Kaitlyn C. ^[1]; Voss, Jonathan M. ^[1]; Zhou, Jia ^[1];

^[1]

Univ. of Wisconsin-Madison, Madison, WI (United States)

IR predissociation spectroscopy of the Gly₃H⁺(H₂O) complex formed inside of a cryogenic ion trap reveals how the flexible model peptide structurally responds to solvation by a single water molecule. The resulting one-laser spectrum is quite congested, and the spectral analyses were assisted by both H₂O/D₂O substitution and IR–IR double resonance spectroscopy, revealing the presence of two contributing isomers and extensive anharmonic features. Comparisons to structures found via a systematic computational search identified the geometries of these two isomers. The major isomer, with all trans amide bonds and protonation on the terminal amine, represents ~90% of the overall population. It noticeably differs from the unsolvated Gly₃H⁺, which exists in two isomeric forms: one with a cis amide bond and the other with protonation on an amide C=O. These results indicate that interactions with just one water molecule can induce significant structural changes, i.e., cis–trans amide bond rotation and proton migration, even as the clustering occurs within an 80 K cryogenic ion trap. In conclusion, calculations of the isomerization pathways further reveal that the binding energy of the water molecule provides sufficient internal energy to overcome the barriers for the observed structural changes, and the minor solvation isomer results from a small fraction of the ions being kinetically trapped along one of the pathways.

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Research Organization:: Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0010326

OSTI ID:: 1513761

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 122, Issue 41; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 11 works

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Title: Probing Solvation-Induced Structural Changes in Conformationally Flexible Peptides: IR Spectroscopy of Gly₃H⁺•(H₂O)