Comment on “Microhydration of Biomolecules: Revealing the Native Structures by Cold Ion IR Spectroscopy”
This paper presents a re-examination of the conclusions of a study reported in The Journal of Physical Chemistry Letters (Saparbaev et al., 2021, 12, 907) that compared the structure of microsolvated ions formed by electrospray ionization to those formed in the gas-phase via a previously published cryogenic ion trap approach. We conducted additional experiments that clearly show that most of the observed differences in the IR spectra can be accounted for by considering the different spectroscopic action schemes used to obtain them. In particular, the presence of the D2-tag induces shifts in some of the N-H and O-H peaks which need to be carefully considered before comparing spectra. Furthermore, once these spectral effects are taken into account, we show that both clustering approaches yields similar clusters structures for the small GlyH+(H2O)n species. Using unimolecular reaction rate theory, we also show that for the small complexes considered here, only the gas-phase equilibrium distribution of conformers should be expected in both experimental approaches. In addition, the barrier heights necessary to kinetically trap high-energy conformers at 298K is explored using a series of model polyalanine chains.
- Research Organization:
- Univ. of Wisconsin, Madison, WI (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Grant/Contract Number:
- SC0018902
- OSTI ID:
- 1864741
- Journal Information:
- Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 8 Vol. 13; ISSN 1948-7185
- Publisher:
- American Chemical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Similar Records
Competition between Solvation and Intramolecular Hydrogen-Bonding in Microsolvated Protonated Glycine and β-Alanine
Microhydrated dihydrogen phosphate clusters probed by gas phase vibrational spectroscopy and first principles calculations