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Unraveling the spectroscopy of coupled intramolecular tunneling modes: A study of double proton transfer in the formic-acetic acid complex.
MedLine Citation:
PMID:  21303129     Owner:  NLM     Status:  In-Data-Review    
Abstract/OtherAbstract:
The rotational spectrum of the hetero dimer comprising doubly hydrogen-bonded formic acid and acetic acid has been recorded between 4 and 18 GHz using a pulsed-nozzle Fourier transform microwave spectrometer. Each rigid-molecule rotational transition is split into four as a result of two concurrently ongoing tunneling motions, one being proton transfer between the two acid molecules, and the other the torsion/rotation of the methyl group within the acetyl part. We present a full assignment of the spectrum J = 1 to J = 6 for the ground vibronic states. The transitions are fitted to within a few kilohertz of the observed frequencies using a molecule-fixed effective rotational Hamiltonian for the separate A and E vibrational species of the G(12) permutation-inversion symmetry group. Interpretation of the motion problem uses an internal-vibration and overall-rotation angular momentum coupling scheme and full sets of rotational and centrifugal distortion constants are determined. The tunneling frequencies of the proton-transfer motion are measured for the ground A and E methyl rotation states as 250.4442(12) and -136.1673(30) MHz, respectively. The slight deviation of the latter tunneling frequency from being one half of the former, as simple theory otherwise predicts, is due to different degrees of mixing in wavefunctions between the ground and excited states.
Authors:
Michael C D Tayler; Bin Ouyang; Brian J Howard
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Publication Detail:
Type:  Journal Article    
Journal Detail:
Title:  The Journal of chemical physics     Volume:  134     ISSN:  1089-7690     ISO Abbreviation:  J Chem Phys     Publication Date:  2011 Feb 
Date Detail:
Created Date:  2011-02-09     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  0375360     Medline TA:  J Chem Phys     Country:  United States    
Other Details:
Languages:  eng     Pagination:  054316     Citation Subset:  IM    
Affiliation:
Physical and Theoretical Chemistry Laboratory, South Parks Road, Oxford OX1 3QZ, United Kingdom.
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